TID-4067 

Isotopes Development Programs 

Research 

and 

Development 

1971 

ttsraffiUTRW OF mis mmm is um.mm 
DISCLAIMER 

This report was prepared as an account of work sponsored by an 

agency of the United States Government. Neither the United States 

Government nor any agency Thereof, nor any of their employees, 

makes any warranty, express or implied, or assumes any legal 

liability or responsibility for the accuracy, completeness, or 

usefulness of any information, apparatus, product, or process 

disclosed, or represents that its use would not infringe privately 

owned rights. Reference herein to any specific commercial product, 

process, or service by trade name, trademark, manufacturer, or 

otherwise does not necessarily constitute or imply its endorsement, 

recommendation, or favoring by the United States Government or any 

agency thereof. The views and opinions of authors expressed herein 

do not necessarily state or reflect those of the United States 

Government or any agency thereof. 
DISCLAIMER 

Portions of this document may be illegible in 

electronic image products. Images are produced 

from the best available original document. 
NOTIC E 

This report was prepared as an account of work sponsored by the United States 

Government. Neither the United States nor the United States Atomic Energy Commission, 

nor any of their employees, nor any of their contractors, subcontractors, or their 

employees, makes any warranty, express or implied, or assumes any legal liability or 

responsibility for the accuracy, completeness or usefulness of any information, apparatus, 

product or process disclosed, or represents that its use would not infringe privately owned 

rights. 

Available from the National Technical Information Service, U. S. Department of 

Commerce, Springfield, Virginia 22151 . 

Price: Paper Copy $3.00 

Microfiche $0.95. 

Pfinitd in iht Unitid Slatci ol lkn«iiea 

U&AEC TKtwilc-l InFarnKX.Dn Cm'*'. Ook Rirfgc, T.n 
RADIOISOTOPE AND RADIATION APPLICATIONS TID-4067 

ISOTOPES DEVELOPMENT PROGRAMS 

RESEARCH AND DEVELOPMENT: 1971 

Progress Reports on Sponsored Work 

-NOTICEThis report was prepared as an account of work 

sponsored by the United States Government. Neither 

the United States nor the United States Atomic Energy 

Commission, nor any of their employees, nor any of 

their contractors, subcontractors, or their employees, 

makes any warranty, express or implied, or assumes any 

legal liability or responsibility for the accuracy, completeness or usefulness of any information, apparatus, 

product or process disclosed, or represents that its use 

would not infringe privately owned rights. 

Issued: February 1972 

Division of Applied Technology 

United States Atomic Energy Commission 

Washington, D. C. 20545 

KTMiUTWi Of T«IS ii€UKiT IS UiLMlW 

'i0\ 
Isotopes Deveiopment Programs 

— NOTICEThis report was prepare prepared as an account of work 

sponsored by the United States Government. Neither 

the United States nor the United States Atomic Energy 

Commission, nor any of their employees, nor any of 

their contractors, subcontractors, or their employees, 

makes any warranty, express or implied, or assumes any 

legal liability or responsibility for the accuracy, completeness or usefulness of any information, apparatus, 

product or process disclosed, or represents that its use 

would not infringe privately owned rights. 

Research 

and 

Development 

1971 

•si^i * m IB ^smm is umMiwm 
FOREWORD 

Isotopes are contributing to the advancement of 

science and technology and human betterment to an 

extent equaled by few discoveries or inventions m 

history Their use spans the whole ot our scientific 

disciplines, and many of them are being brought to bear 

on urgent human problems and national rcquiiements 

In some areas, such as medicine and industry this new 

technology is now well established and its benefits are 

very significant In others, such as pollution i ontrol and 

forensic analysis its potential is just beginning to be 

realized Through its Isotopes Development Program 

the Atomic Energy Commission is endeavoring to 

establish the basic technology necessary for realization 

of these values, the specific objectives of this program 

are to 

Bring about productive utilization of radioisotopes 

and radiation, important to the national economy 

and welfare through research and development and 

demonstration programs and to assist in the intro 

duction of this technology into wide scale use 

Develop technology tor the production separation 

purification and encapsulation of radioisotopes 

utilizing resources of both the Atomic Energy 

Commission and industry 

Ensure that national requirements for the produc 

tion and distribution of radioisotopes aie satisfied 

by the AtC or by private industry and that current 

AEC activities in this area are transferred to private 

industry in keeping with the best interest of the 

public 

To achieve these objectives the Atomic Energy 

Commission sponsois research and development at its 

laboratories and plants such as Oak Ridgc National 

Laboidtory and Brookhaven National Labor itory ^ nd 

at various industrial and academic facilities Major 

technical program areas and goals are 

Radioisotope Production and Materials to improve 

methods for the production of radionuclides 

Thermal Apphcations to develop applications using 

the thermal energy generated by radioisotope decay as a 

heat souice oi for conversion to mechanical ptiwer 

Environmental and Ocean Sciences to develop i idio 

isotope techniques to aid m environmental problem^ 

such as pollution and water management and to assist ui 

the exploration and economic development of the 

oceans 

Radiation Analysis and Control to dtvtlop basK 

technology and instrumentation for detection and 

measurement of radioisotopes and to appl> the tech 

nology to current problems 

Process Radiation to develop melliods for the piod ic 

tion of chemicals and other materials using large sources 

of radiation and to develop efficient safe radiation 

sources for process radiation 

Radiation Preservation of Foods to develop a low 

dose radiation processing method to extend marketing 

times and reduce spoilage of selected foods 

Technology Analysis and Utiluation to eviluate 

Program requirements obfeetives and outputs and to 

expedite the wide scale use of technology developed 

under the Program 

This report is the fifth edition of ihe Isotopes 

Devek>pment Program Project Summaries It present a 

short summary of objectives results and future plans 

for each research or development project within the 

program areas described above 

Assistant Diiector 

lor Isotopes Development 

Division of Applied f eehnologv 

U S Atomic Energv Commission 
The project summaries m this report were prepared by the contractors who 

are performing the work and were collected and edited for technical content b\ 

members of the technical staff of the Isotopes Development Branch*, Division 

of Applied Technology, USAEC Final editing and preparation for publication 

was done by the staff of the Isotopes Information Center, Oak Ridge National 

Laboratory 

*Formerl> Division of Isotopes Deveiopment Since the reeirganization of the ALC 

occurred subsequent to the editing of the draft of this report, changes could not be made in 

the text to reflect the new organizational structure Hence the divisions referred to are those 

as they existed prior to December 7, 1971 
CONTENTS 

TECHNOLOGY UTILIZATION 

Isotopes Information Center (ORNL) 

RADIOISOTOPE PRODUCTION AND MATERIALS 

ORNL Fission Product Development Program (ORNL) 

Krypton-85 Enrichment (ORNL) 

Cesium-137 Chloride Process Improvement and Source Characterization — Chemical Proce 

Improvement (ORNL) 

Cesium-137 Chloride Process Improvement and Source Characterization — Effect of KCl 

on Physical Properties of Cs(137)Cl Source (ORNL) 

Isotope Production Evaluations (PNL) 

Low-Cost Cesium and Strontium Sources (PNL) 

Hanford Fission Product Production Capabilities (ARHCO) 

Fission Product Rhodium, Palladium, Ruthenium, and Technetium Research (PNL) 

Evaluation of Large-Scale Uses for Purified Fission Product Xenon (PNL) 

Promethium-146 Reduction (PNL) 

Fission Products Development Laboratory (ORNL) 

ORNL Reactor Produced Radioisotopes Program (ORNL) 

Potassium-43 (ORNL) 

Phosphorus 33 (ORNL) 

Silicon-32 (ORNL) 

Thulium 170 (ORNL) 

Platinum-195m (ORNL) 

BNL Accelerator Products Development (BNL) 

The Brookhaven Linac Isotope Producer (BLIP) (BNL) 

BNL Cyclotron Product Development (BNL) 

Dysprosium-157 (BNL) 

Auxiliary Cyclotron Beam Monitor Development (BNL) 

Van de Graaff Generator Technology (BNL) 

Xenon-127 (BNL) 

Bismuth-204 (BNL) 

ORNL Accelerator-Produced Radioisotopes Program (ORNL) 

Gallium-67 (ORNL) 

Indium-Ul (ORNL) 

Barium-133m (ORNL) 

Bismuth-206 (ORNL) 

Lead-203 (ORNL) 

BNL Biomedical Products Development (BNL) 

Chemical Studies of Technetium 99m (BNL) 

Instant Tc-99m Compounds (BNL) 

v 
Technetium-99m Labeled Red Blood Cells (BNL) 37 

New Cesium-137 Source Compounds Development and Evaluation (ORNL) 38 

Strontium Silicate Beta Source Development (ORNL) 39 

Low-Energy Photon Radiation Sources (ORNL) 40 

Advanced Source Development (PNL) 41 

Nondestructive Testing Technology in Support of DID Capsule Development Activities and 

Radiation Source Programs (PNL) 42 

Shipping Cask Design and Evaluation (ORNL) 44 

Radioisotope Safety Testing (ORNL) 45 

Radioisotope Characterization, Quality Control, and Standards (ORNL) 46 

THERMAL APPLICATIONS 49 

Evaluation of Practicability of a Radioisotope Thermal Converter 

for an Artificial Heart Device (Westmghouse Electric Corp ) 53 

Preparation and Evaluation of Plutonium-238 Radioisotopic Heat Sources (LASL) 55 

Evaluation of Practicability of a Radioisotope Thermal Converter 

for an Artificial Heart Device (TRW Systems Group) 56 

Recipient Radiation Exposure and Radiological Engineering Studies Relating 

to Circulatory Support Systems (PNL) 58 

Population Radiation Exposure from Heart Device (PNL) 60 

Artificial Heart Program (Monsanto Research Corp ) 61 

Integrated Waste Management — Water System Using Radioisotopes for Thermal Energy 

(General Electric Co ) 61 

Integrated Waste Management Program [Radioisotopes for Thermal Energy (RITE) Heat Source] 

(Monsanto Research Corp ) 62 

Biomedical Engineering Support (University of Utah) 63 

Radioisotope Heater Development Program — Phase II (McDonnell Douglas Astronautics Co ) 63 

Development of Cobalt-60 Heat Sources (SRL) 65 

Cobalt-60 Heat Source Demonstration Program (Westmghouse Electric Corp ) 66 

Pioneer Radioisotope Heater Unit (PRHU) Program (Monsanto Research Corp ) 67 

A Review and Evaluation of TRW Safety Analysis Report, Volumes I and II, for the 

Pioneer Radioisotope Heater Unit (Werner Associates, Inc ) 68 

ENVIRONMENTAL AND OCEAN SCIENCES 69 

Atmospheric Diagnostics Program (BNL) 73 

Measurement of Sulfur Dioxide in Stack Gases (Industrial Nucleonics Corp ) 74 

Snow-Management Research (U S Forest Service) 75 

Telemetered Profiling Isotopic Snow Gage (Aerojet Nuclear Co ) 77 

Role of Paper Mill Additives as Potential Stream Pollutants Development of 

Nuclear Analytical Techniques (Washington State University) 77 

Development of Nuclear Analytical Techniques for Oil-Slick Identification (Gulf Radiation Technology) 78 

Radioisotopic Sediment Tracing (RIST) Study Synoptic Study of Sediment Transport 

(U S Army Coastal Engineering Research Center) 79 

Radioisotopic Sediment Tracing (RIST) Study Fundamental Studies of Sand Transport and 

Equipment Design (ORNL) 79 

Evaluation of Treatment Plants by Tracer Methods (Georgia Institute of Technology) 80 

Nuclear Techniques for Seabed Mineral Exploration (PNL) 81 

Radioisotope Density Gage for the Deep-Ocean Sediment Probe (University of Rhode Island and 

Navy Underwater Sound Lab ) 82 
RADIATION ANALYSIS AND CONTROL 

Research on Single-Crystal Semi-lnsulatmg Cadmium Tellunde as a Gamma-Ray Spectrometer 

(Hughes Research Labs) 87 

Cadmium Tellunde Detectors (Tyco Corp ) 88 

Evaluation of Cadmium Tellunde for Radiation Detectors (Emory University) 90 

Low-Noise Field-Effect Transistors (BNL) 92 

New Research Applications of Cerenkov Radiation (ORNL) 94 

Evaluation of the 200-mCi Iron 55 X-ray Diffraction Source m Focusing and Debye Scherrer 

Analytical Applications (Edsel B Ford Institute for Medical Research) 95 

Gamma-Ray Spectrometry of Neutron-Deficient Nuclides (Aerojet Nuclear Co ) 96 

Apphcation of Nuclear Technology to Art-Identification Problems (Carnegie-Mellon University) 98 

Study of Tooth-Enamel Density (University of Chicago and General Electric Co ) 99 

Radioisotopic X-ray Fluorescence Spectrometry for Multielement Analysis of 

Air Pollutants (Columbia Scientific Industries) 100 

Portable Radioisotopic X-ray Fluorescence Detector of Bullet Holes 

(Dade County, Fla , Public Safety Department) 102 

X-ray Fluorescence Analysis System for Lead in Blood (New York University Medical Center) 103 

Kryptonates for the Analysis of Automobile Exhausts (Panametncs, Inc ) 105 

Nuclear Instrument Landing System (TRW Systems) 107 

Neutron Radiography with Californium-252 (PNL) 108 

Indwelling Intracranial Pressure Sensor (Hittman Associates, Inc ) 110 

PROCESS RADIATION 113 

Concrete-Polymer Materials (BNL) 117 

Development of Concrete—Polymer Materials (U S Bureau of Reclamation) 118 

Radiation Chemical Engineering (BNL) 119 

Survey Experiments Application of Isotopic Radiation for Chemical Processing (BNL) 120 

Composite Materials (BNL) 121 

Basic and Engineering Studies of Radiation Induced Reactions in the Liquid Phase 

(North Carolina State University) 123 

Radiation-Induced Chain Reactions in Heterogeneous Systems (University of Maryland) 124 

Influence of Radiation upon Heterogeneous Catalytic Selectivity (University of Notre Dame) 125 

Radiation Cross-Linking of Polymers with Segregated Metallic Particles (Drexei Institute of Technology) 126 

Electron and X and Gamma-Ray Research for Radiation Processing (NBS) 128 

High Intensity Radiation Development Laboratory Operations (BNL) 130 

Radiation Source Development, Testing, and Evaluation (BNL) 130 

Dosimetry and Dosimeter Development (BNL) 132 

Portable Irradiator Support (BNL) 133 

General Engineering and Technical Assistance (BNL) 134 

Field Dosimetry Standardization (BNL) 135 

Patent Review — Process Radiation Development (ORNL) 136 

RADIATION PRESERVATION OF FOODS 137 

Marine Products Development Irradiator Program (National Marine Fisheries Service) 141 

Radiation Pasteurization of Fresh Meats and Poultry (Michigan State University) 141 

A Study of Control of Public Health Problems Using Irradiation (University of Nebraska) 142 

Radiation Technology in Conjunction with Post Harvest Procedures as a Means of Extending the 

Shelf Life of Fruits and Vegetables (University of California, Davis) 143 

Hawaii Food Irradiation Program Study of Dosimetry, Tolerance, and Shelf Life Extension Related to 

Disinfestation of Fruits and Vegetables (State of Hawaii, Dept of Agriculture) 145 

Loan of 50,000 Curies of Co-60 for Use m Radiation Facility for Research m Foods 

(University of Massachusetts) 146 

V l l 
AUTHOR INDEX 147 

CORPORATE AUTHOR INDEX 149 

SUBJECT INDEX 150 

viii 
TECHNOLOGY UTILIZATION, ISOTOPES 

INFORMATION CENTER* 

Objective of Work 

The project objective is to collect, evaluate, and 

disseminate information as reported in world literature 

— primardy on the production and uses of radioisotopes 

in industry, medicine, and research. The Center also 

maintains a current awareness of uses of isotopes m 

biology, agriculture, education, forensics, and the military. 

Progress and Results 

During the current period, the first of a number of 

"Radioisotope Briefings for Industry" was completed 

These consist of annotated bibliographies covering 

specific aieas of isotope applications - e.g., "Nonferrous Metals." These are to be available as handouts 

to interested users and will be submitted to appropriate 

trade journals for publicity. 

The Center's total of indexed documents is now 

nearly 23 thousand. The information contained in these 

documents was used by membeis of the Center for the 

following purposes. 

To write four issues of the quarterly technical 

progress review. Isotopes and Radiation Technology, for publication by the Division of Technical 

Information (This review is available from Superintendent of Documents, U. S. Government Printing 

Office, Washmgton, DC 20402, subscription $2.50 

per year, $0 70 for individual issues, non-U.S. 

subscriptions S3.25 per year, $0.90 for individual 

issues.) 

*P S Baker, Oak Ridge National Laboratory, P O Box X, 

Oak Ridge, TN 37830, Contract W-7405-eng-26. 

To answer about 350 requests for specific information and to fill over 850 individual requests for 

about 2500 copies of IIC publications. The information requests came from industry (30%), Government (12%), educational institutions and research 

institutes (30%), individuals, no affiliation indicated 

(13%), and miscellaneous sources (15%). 

To provide information - chiefly in the form of 

bibhographies — needed by personnel of DID to 

evaluate research proposals. 

To provide information for DID personnel for 

inclusion m reports and for presentation at meetings 

and to help prepare tire Annual Summaries of DID's 

Research and Development Projects. 

To prepare a number of summary review articles 

and other special reports and bibliogiaphies. These 

reports are listed under Reports Published 

The previously reported (1969) Isotope User's Guide 

continued to be a very popular item and a reprinting 

was necessary. 

More than one hundred persons visited the Center 

during the year. 

Plan for Next Period 

The continuing program of the Center comprises all 

of the above activities, with increased emphasis on 

providing for the preparation of more summaiy leview 

articles and on extending and piomotmg the interplay 

between the IIC and industry so as to improve the 

technology utilization aspects of DID's programs 

Reports Published 

P S Baker, A F. Rupp, and Associates, Isotopes and 

Radiation Technology, Volumes 8(3), 8(4), 9(1), 

and 9(2). 

1 
2 

Ruth Curl, Comp , List of AEC Radioisotope Customers with Summary of Radioisotope Shipments, 

FY 1970, USAEC Report ORNL-nC-32, February 

1971 

R E Greene, H S Warren, and P S Baker, Patent 

Literature on Process Radiation and Irradiator 

Design Part 1 U S Patents 1950 Through 1968, 

USAEC Report ORNL-IlC-34, June 1971 

R Shor, R H Lafferty, and P S Baker, Comps, 

Strontium-90 Heat Sources, USAEC Report ORNLIIC-36,May 1971 

Martha Gerrard and P S Baker, Selected Abstracts of 

World Literature on Production and Industrial Uses 

of Radioisotopes, USAEC Reports ORNL-lIC-30 

(Part 3) December 1970, ORNL-IIC-30 (Part 4) 

April 1971, ORNL-IIC-37 (Part I) m press 

IIC Staff, Eds, Division of Isotopes Development 

Research and Development Projects, 1970, USAEC 

Report TID-4066, February 1971 

Estimated Date of Final Report 

Continuing project 
RADIOISOTOPE PRODUCTION 

AND MATERIALS 

BLIP target. 

HAPO I cask arriving at 

ORNL's FPDL from Hanfotd. 

Radioisotope Production and Materials 

The radioisotope production and materials development work has been concerned with meeting isotope 

requirements in four principal areas' (a) diagnostic and 

therapeutic medicine, (b) analysis and controls, (c) 

process radiation, and (d) thermal energy As a result of 

the AEC's program, radioisotopes are now firmly 

established as essential mateiials m medicine and in 

analysis and controls. In addition, considerable progress 

has been made toward establishing the oppoitunity for 

economical use of large quantities of the radioactive 

nuclides for process radiation and thermal power 

applications This effort also includes the pilot production of radioisotope pioducts, unique to AEC capabilities, as part of the program to develop radioisotope 

applications for the national benefit. 

The Fis'iion Product Studies represent continuing 

efforts at Oak Ridge National Laboiatory (ORNL) and 

Pacific Northwest Laboratory (PNL) to develop production technology and to characterize products. Also 

supported is a small effort at Atlantic Richfield 

Hanford Company on fission product availability from 

Hanford reactor wastes. Fission products, particularly 

from power reactors, represent a potentially valuable 

source of long-lived radioisotopes including Sr-90, 

Cs-137, Kr-85 and Pm-147. Work at ORNL is principally on enrichment of Kr-85, preparation of Cs-137 

sources for optimized process radiation applications, 

and development of encapsulation technology foi Sr-90 

sources. In addition, pilot plant operations at ORNL 

supply Sr-90, Cs-137, and Kr-85 along with a broad 

spectrum of shorter-lived fission products for applications development. The PNL studies include Pm-147, 

Sr-90, and Cs-137 and the stable fission products 

rhodium, palladium, and xenon. In addition, studies are 

made of piojected isotope availability based on power 

reactor operations Pilot production operations provide 

Pin-147 for applications development. 

The Reactor Product Studies involve work at ORNL 

and the Savannah River Laboratory. The studies at 

ORNL employ two high flux reactors in the development of new products primarily for medical applications Specific products investigated include P-33, 

CI-36, K-43, Ru-97, La-137, Ba-]35m, Gd-153, 

Tm-170, Pt-195m, and Rh-105 

The Accelerator Product Studies at Brookhaven 

National Laboratory (BNL) and ORNL are continuing, 

with emphasis on research and medical products. In 

these studies, the 86-inch cyclotron at Oak Ridge along 

with the 60-inch cyclotron and Van de Graaff machines 

at Brookhaven are used In addition, facilities are being 

established to use the Linear Accelerator Injector of the 

Brookhaven Alternating Gradient Synchrotron in 1972 

for spallation reaction studies. Specific product studies 

include Ga-67, In-Ill, Rb-83, Nd-140, F-l8, Cs-129, 

Ba-133m, Tm-167, and Pb-203. General technology 

studies include radionuclide recoil labeling 

The Apphcations and Technology Support Studies 

include work principally at BNL, ORNL, and PNL. 

Both Brookhaven and Oak Ridge have major supporting 

activities in the radiopharmaceutical area. Studies involving radiation sources, standards, and regulatory 

questions are earned out at ORNL. At PNL research on 

nondestructive testing is m progress 

5 

7 

ORNL FISSION PRODUCT 

DEVELOPMENT PROGRAM" 

Objective of Work 

The objective of the ORNL fission product develop 

ment piogram is to support development activities in 

the areas of thermal and radiation applications Radio 

isotopes that result from the fission process are the 

most abundant sources of unique energy forms In 

addition, technical support is provided for the Fission 

Products Development Laboratory (FPDL) and the 

short lived fission product processing unit Specific 

areas of application include (1) materials sterilization, 

(2) food preservation, (3) radiation stimulated chemical 

processing (4) pollution abatement, (5) extrateirestrial, 

terrestrial and oceanographic thermal control and (6) 

medical research 

Progress and Results 

The usefulness of Kr 85 can be increased by removing 

from It the nomadioactive krypton isotopes thus 

increasing the specific activity of the product The 

technique of thermal diffusion enrichment is being 

applied to isotopic enrichment of Kr-85 Progress in the 

development of this technique is reported in a separate 

summary Cesium-137 chloride process improvement 

and source characterization studies were continued with 

emphasis on (1) chemical process improvement and (2) 

the effect of KCl on the physical properties of 

Cs(137)Cl sources Both items are reported in individual 

summaries Alternative Cs-137 compounds to Cs(137)CI 

were prepared and evaluated on the basis of technical 

feasibility and economic potential Progress in the 

examination of niobates tantalates, and silicates is 

reported in a separate summary 

The preparation of fission-product xenon highly 

purified and decontaminated from Kr-85 was continued 

in order to supply Battelle Northwest Laboratory with 

material for evaluation of apphcations in medicine A 

separate technical summary describes this work 

Plan for Next Period 

See summaries of individual projects 

Reports Published 

See summaries of individual projects 

*T A Butler Oak Ridge National Laboratory, P O Box X 

Oak Ridge, TN 37830 Contract W 7405 eng 26 

Estimated Date of Final Report 

Continuing Project 

KRYPTON-85 ENRICHMENT* 

Objective of Work 

The objective of the Kr 85 enrichment program is to 

provide krypton gas containing a higher concentiation 

of radioactive mass 85 isotope than the approximately 

5% that IS found in normal tission product krypton 

The minimal biological hazard and ease of handling of 

the inert gas krypton are desirable features of this 

radioisotope Fission krypton has been used in such 

applications as beta thickness gages, wireless emergency 

exit and highway signs, and kryptonated metal parts foi 

wear and temperature measurements The availability of 

krypton with an increased specific activity has improved the effectiveness of most of these applications 

and may open new uses, such as in isotopic power 

sources 

Progress and Results 

The thermal diffusion pilot plant constructed to 

provide operational experience, is routinely producing 

approximately 1200 Ci/year of material containing 

greater than 1 5% Kr 85 (214 Ci/liter) and has produced 

material containing as much as 43 8% (625 Ci/litei) 

Kr-85, representing an enrichment factor of neaily 12 

times the specific activity of the starting feed gas The 

present system has been in operation for more than two 

years vvith remarkably few operational difficulties or 

maintenance problems The only major repairs needed 

during this period involved replacing several manual 

valves ir one cell containing three therma' diffusion 

units 

One of the six column bundles has been used to 

demonstrate a method for decontaminating fission 

xenon to a low Kr-85 level so that the xenon could be 

used m unregulated apphcations, such as in light bulbs 

or as an anesthetic Fission xenon which had been 

decontaminated to a Kr-85 activity level of 0 4 juCi/ml 

by chromatographic methods was further decontami 

nated to an activity level of 0 002 ^tCi/ml by thermal 

diffusion Twenty days of column operating time was 

required to reach this activity level 

*W R Rathkamp Oak Ridge National Laboratory, P O Box 

X, Oak Ridge TN 37830, Contract W-7405 eng 26 
Plan for Next Period 

Operation of the pilot plant will continue, with 

emphasis on producing material enriched to greatei 

than 43.8% of Kr-85. 

Reports Published 

None. 

Estimated Date of Final Report 

Continuing project. 

CESlUM-137 CHLORIDE 

PROCESS IMPROVEMENT AND 

SOURCE CHARACTERIZATION -

CHEMICAL PROCESS IMPROVEMENT* 

Objective of Work 

The objectives of this project are (1) to develop an 

improved process to replace the one in use at the 

Fission Products Development Laboratory (FPDL) for 

conversion of cesium eluted from the inorganic ion 

exchanger shipping cask to Cs(137)Cl and (2) to carry 

out experimental studies on technical feasibility of the 

selected processes 

Progress and Results 

A preliminary evaluation of fixed capital costs (relative figures) based on a generalized semi-empirical 

equation has been earned out for five processes under 

consideration for purification and conversion of the 

Cs-137 feed from an inorganic ion exchanger into 

Cs(137)CI. Conceptual process flow diagrams and estimated values of various parameters were used in the 

computation. The result, summarized in the table, 

indicates that Process 1 (NH4CI eluant) is economically 

the most attractive from the viewpoint of the fixed 

capital costs. Process 4 (HCl eluant) requires the second 

lowest fixed capital costs, but experimental results 

revealed that the elution efficiency of the acid-type 

eluant is appreciably lower than that of the ammonium 

salt type. A similar statement is applicable to Process 5 

(HNO3 eluant). For these reasons. Processes 1, 2, and 3 

are preferred to Processes 4 and 5 

In progress is the study on the corrosion of materials 

for construction of processing vessels (several grades of 

stainless steel) by NH4CI and (NH4)2C03-NH4 0H 

solutions The initial examination of the test specimens 

Comparison of Fixed Capital Costs for Various 

Conceptual Cs(137)Cl Processes 

Eluant 

NH4CI 

(NH4)2C03-NH40H 

(NH4)2S04 

HCl 

HNO3 

Fixed Capital Costs" 

(Relative Figure) 

14 9 K 

26 2 K 

33 4 K 

23.7 K 

30 9 K 

''K = CP"(1/1), where C is a constant, P is the production 

capacity (Ci/yr), n is a tactor derived from a statistical 

correlation between F and P, and I and I are construction-cost 

indices K is assumed to be common to all the processes 

exposed to the solutions circulating at ~75°C under 

Cs(137)Cl radiation showed almost negligible attack in 

all cases after about two months. Furthei studies are 

required before any interpretation and conclusion can 

be made m regard to the compatibility of the eluant 

solutions with the structural materials. 

Plan for Next Period 

Experimental studies will be continued to confirm 

technical feasibility of the selected Cs(137)Cl piocesses. 

The experimental data obtained will be used as the basis 

for the preliminary process design and economic evaluation of commercial-scale plants 

Reports Published 

None. 

Estimated Date of Final Report 

Continuing project 

CESIUM-137 CHLORIDE PROCESS 

IMPROVEMENT AND SOURCE 

CHARACTERIZATION - EFFECT OF KCl 

ON PHYSICAL PROPERTIES 

OF Cs(137)a SOURCE* 

Objective of Work 

The objectives of this project are (1) to investigate 

how presence of the KCl impurity m Cs(137)Cl gamma 

sources influences dimensional stability of the source 

compound and (2) to determine the limits of application conditions based on the study. 

*K H. Lin, Oak Ridge National Laboratory. P O Box X, Oak 

Ridge, TN 37830, Contract W-7405-eng-26 

*K H Lin and D N. Braski, Oak Ridge National Laboratory, 

P O Box X, Oak Ridge, TN 37830, Contraet W-7405-eng-26 
Progress and Results 

Further studies on the effect of KCl on the dimensional stability of CsCl have been carried out using 

dilatometry and high-temperature x-ray diffractometry 

Emphasis was placed on elucidating the solid phase 

transformations as related to the thermal expansion as a 

function of several variables Both equilibrium and 

kinetic effect were investigated 

The data obtained from previously reported differ 

ential thermal analysis (DTA) studies were combined 

with the dilatometry and x-ray diffractometry data to 

estabhsh a clear understanding of the equilibrium phase 

diagram for the sohd phase region Previous DTA data 

were inadequate for this purpose due to small energies 

of the transformations The DTA data did indicate, 

however, that kinetic effects are very significant factors 

The addition of KCl (up to 2 mole%, 0 9 wt%) does not 

significantly alter the phases present at equilibrium The 

addition of 2 mole% KCl does significantly alter the 

kinetics of the sohd—solid phase transformation For 

example (see the figure) 

The solid—solid phase change from |3 to a at 

approximately 460°C takes place very slowly m 2 

mole% KCl—CsCl mixture, whereas in pure CsCl the 

transformation at this temperature is rapid both on 

heating and on coohng 

The linear coefficient of thermal expansion of the 

high-temperature form (j3 phase) is much less than 

for pure CsCl The linear coefficient of thermal 

expansion of pure CsCl in the high-temperature form 

(above 465°C) is 22 to 44 times that of the 

low-temperature form (below 465°C) When 2 

mole% KCl is added to CsCl the relative expansion is 

reduced by a factor of about 2 

The residual expansion of pure CsCl when repeatedly cycled about the solid—solid transformation point IS about 10% When 2 mole% KCl is 

present, the residual expansion is about 6 5% The 

addition of an amount of KCl greater than the 2 

mole% alters significantly the phases present as a 

function of temperature In addition severe kinetic 

effects are encountered, especially m samples not 

exposed to ambient air 

i M 

MO 

o 

s. 

a 

MO 

MO 

I I I 

"TO" 

a Solid solution of KCl in CsCl 

(CsCl structure) 

1^2 Solid solution of KCl and CsCl —4. 

(NaCI structure) (3^ and (Jg 

differ only in composition and 

lattice parameter , 

0 \ LJII J L 

WOZCiCI 

10 w" 30 M 60 

^^1£%(KCI) 

70 •0 »0 100 

Phase diagram for CsCl-KCl system. 
10 

Based on the findings described above, the following 

recommendations are made m regard to the limits of 

application conditions 

1 For a conservative design of the source capsule, a 

sufficient volume should be allowed for thermal 

expansion based on pure CsCl, although the presence 

of a small amount of KCl tends to reduce the extent 

of such expansion 

2 Thermal cycling through the sohd-phase transformation temperature (depends on KCl content) should 

be minimized because it tends to increase the 

amount of residual expansion of the salt 

Plan for Next Period 

This phase of the project has been completed 

Reports Published 

None 

Estimated Date for Final Report 

Second quarter of 1972 

ISOTOPE PRODUCTION EVALUATIONS* 

Objective of Work 

The objective of this project is to evaluate major 

aspects of isotope production, including (1) economic 

evaluations of isotope production by target irradiation 

or recovery from fuel reprocessing waste, (2) preparation of isotope availability projections, and (3) development of a computerized isotope data system 

Progress and Results 

The study to define the time and circumstances as to 

when recovery of fission product cesium and strontium 

might be attractive to the nuclear fuel reprocessing 

industry was completed Initial results are described in 

the 1970 report (TID-4066) 

An important aspect of this study was determination 

of the value of cesium recovered from power reactors 

and from Hanford Waste Management Program (HWMF) 

relative to Co-60 The value of power reactor cesium as 

a gamma radiation source is enhanced by the larger 

gamma energy contribution of the contained Cs-134 

(~2 5 wt%), while the value of HWMP cesium is 

reduced by the large self-absorption effect in the 2 6-in 

*R W McKee, Battelle, Pacific Northwest Laboratory, 

Richland, WA 99352, Contract AT(45-1)-1830 

dia capsules The values relative to Co-60 at $0 40/Ci 

and based on a discounted cash flow analysis were 

found to be in the range of $0 25 to $0 30/Ci Cs-137 

for power reactor cesium and $0 07 to $0 09/Ci Cs-137 

for the HWMP cesium 

The computer program mentioned in TlD-4066 was 

designed to calculate price requirements for a profitable 

venture This computer program was modified to 

include more realistic market projection options as well 

as market sharing options This permits examination of 

the gamma-radiation source market as a whole with a 

suitable apportionment of the market between Co-60, 

power reactor cesium, and HWMF cesium For different 

source materials, the different initial and replenishment 

requirements result in quite different annual curie 

requirements for the same basic market 

Using this computer program, a series of cases was 

prepared which simulated the development of a Cs-137 

and Sr-90 recovery industry The gradually developing 

market is first supphed from HWMP cesium and 

strontium resources, and when the market has grown 

large enough to justify the large investment required, a 

private reprocessor begins operations The results of 

these calculations indicated that this kind of two-phase 

market evolution could result in feasible private recovery operations in the late 1970's or early 1980's 

Results for the base-case assumptions are shown in the 

first table 

Target irradiation capabilities of a pressurized water 

reactor (1975-startup design) were calculated using the 

2DB and ALTHAEA computer codes It was assumed 

that targets could be inserted m unused rod cluster 

control assembly locations Results are summarized in 

the second table for 11-month irradiations (one refueling cycle) 

Revised projections of isotope availabihty from power 

reactor spent fuel processing were developed following 

the procedures outlined in BNWL-716 (July 1968) A 

slower rate of nuclear plant startups and lower capacity 

factors have reduced projected quantities relative to 

those in BNWL-716 The difference was large in the 

early 1970's but amounted to only a one-year offset m 

the 1980's 

A computerized isotope data system was developed 

and tested on a sample data file of 50 nuclides The 

system was designed for remote accessing via a teletype 

terminal with queries in the English language All design 

options were tested and found operable 

The system permits searching the data file with up to 

50 constraints imposed on items to be reported For 

example, maximum or minimum constraints can be 

specified for half-life, gamma energies or abundances. 
11 

Market Projection 

HWMR Sales 

Phaseout 

Startup of 

Power Reactor 

Cs Recovery 

Pnce Required 

^/CiCsl37 

Price Requirements for Base Case Power Reactor-Cesium Recovery 

tf/Ci Cs-137) 

I 

Gradual 

Low 

_ 1 _ 

Medium High 

Abrupt Gradual Abrupt Gradual 

1977 1977 

1980 

1977 

19 

1977 

1980 

1977 

1980 

1982 1982 1982 

64 57 53 50 38 35 45 40 36 36 

1982 

27 25 36 

Abrupt 

1977 

1980 

1982 

29 25 

1980 

1982 

29 20 18 

Note Feasible prices enclosed m rectangles 

Target Irradiation Capabilities of a Power Reactor (PWR) 

Target 

Np-237 

(oxide) 

Am (50/50) 

241 & 243 

(oxide) 

Cobalt 

Thulium 

(TmjOa) 

Bismuth 

Nitrogen 

(Be3N2) 

Lithium 

(LijO) 

Phosphorus 

(P2O5) 

Sulfur 

Tellurium 

* Based on 

Reaction 

n,7 

n,7 

n,7 

n,7 

n,7 

n,p 

n,a 

n,7 

n,7 

n,7 

Product 

Pu-238 

Cm-242 

Pu-238 

Cm-244 

Co-60 

Tml7 0 

Po-210 

C 14 

H-3 

P-32 

S-35 

1-131 

1-127 

1-129 

Target 

cone 

g/cm^ 

0 5 

0 25 

(20 g/ft) 

0 5 

9 8 

0 8 

0 1 

1 0 

19 

5 7 

Enrichment 

required 

m assembly, 

% U-235* 

4 09 

4 24 

3 99 

3 80 

3 30 

3 43 

3 87 

3 40 

3 41 

4 14 

enrichment without target = 3 3% U-235 

beta energies, cross sections. etc , and 

Product Yields (no loss basis) 

g/g 

0 193 

0 115 

0 106 

0 113 

0 028 

0 108 

1 6 X 10"^ 

1 3 X 10"^ 

0 262 

1 6 X 10"^ 

1 6 X lO""* 

2 6 X 10'* 

1 6 X lO'"* 

1 4 X 10"'' 

kg/assembly 

0 05 

0 150 

0 138 

0 147 

0 134 

0 280 

7 2 x 10"* 

5 5 x 10 ^ 

0 136 

8 0 X 10"^ 

16 X 10"^ 

7 6 X 10"^ 

only data on Plan for Next Period 

isotopes satisfying these constraints will be reported 

Results can be reported m tabular form in one to ten ^ ° ^"'"*^'' ^^^"""^ '^ 

evenly spaced columns, with 

increasing or decreasing order 

Items sorted in eithe '^ Reports Published 

None 

Maximum 

kWper 

1000 MWe 

per year 

32 1 

2050 

8 8 

47 

500 

12 

0 9 X 10 ^ 

5 6 

875 

2 5 

3 6 

anticipated 

Maximum 

kCi per 

1000 MWe 

per year 

17,300 

194,000 

370 

2 8 

150,000 

260,000 

7,600 

1,100 

Product 

activity, 

Ci per 

gram of 

element 

315 

650 

4490 

4 5 

9690 

440 

6 7 

1040 

The Nuclide Data File (2000 nuchdes) was completely revised and updated and the file is ready for 

loading into the data system 

Estimated Date of Final Report 

None planned 
12 

LOW-COST CESIUM AND 

STRONTIUM SOURCES* 

Obj'ective of Work 

The objective of this program is to provide technology for the production of inexpensive cesium and 

strontium sources by using the purified compounds 

generated m the Hanford Waste Management Program 

(HWMF) Large scale use of these radioisotopes will 

require an assessment of the capabilities of HWMF for 

producing suitable radiation and heat sources, acceptance of the HWMP product by the customer, licensing 

of the sources, and market development activities 

Progress and Results 

Construction has been started by Atlantic Richfield 

Hanford Company (ARHCO) on the encapsulation 

portion of the Waste Management Plant The facility is 

expected to be ready for cold testing m 1973, and for 

full hot operation m January 1974 Ion-exchange 

purification equipment for cesium is being installed, 

and final purification of cesium is expected to start m 

FY-1972 Purified strontium is currently being accumulated One of the strontium product tanks contains 

about 12 MCi of strontium of 95% chemical purit> The 

Sr-90 content is 53 7 wt% based on total cation 

content 

At the present processing rate, the waste storage tanks 

will have been completely processed m about 1976 A 

few additional years will be required for conversion to 

solids and encapsulation 

Container sizes for both cesium and strontium were 

recently changed by HWMP to provide easier handling, 

welding, and nondestructive testing (NOT), however, 

the amount of material per container was not changed 

In each case new dimensions are 2 625-in o d for the 

outer capsule and 2 500-in o d for the inner capsule 

The total wall thickness for the cesium capsule was 

reduced slightly to 0 179 m The utility of each type of 

capsule for radioisotope applications is not affected 

appreciably 

The work described above was funded by the Division 

of Production, but the status is described here because 

of the strong interaction with the Division of Isotopes 

Development program described below 

The process for encapsulation of Cs-137 m the HWMP 

involves casting of molten CsCl into a series of nine 

containers Optimization of radiation sources will require the ability to transfer the molten CsCl through 

*H H Van Tuyl, Battelle Pacific Northwest Laboratory, 

Richland, WA 99352, Contract AT(45-1)-1830 

small diameter lines into a series of 1 in o d capsules a 

size that would be attractive as a radiation source 

A device for loading a series of ten 1-in o d b> 18 m 

long capsules with 0 035-m wall was fabricated for 

testing Each capsule was mated and sealed to a transfer 

head that contained *;4"in lines for conducting the 

molten salt to and from each capsule m series Molten 

CsCi was transferred into the series of ten capsules 

without difficulty The density ot the CsCl was 2 68 

gjcmr' (~78% theoretical density) A uniform cylinder 

of CsCl was produced with only slight (~V2 m) 

depression of the top surface caused by cooling This 

demonstrates that HWMP could load the small diameter 

capsules without adjusting the batch size normally used 

m the Waste Management Plant 

A study of technical feasibility and cost has shown 

that multimegacurie amounts of strontium as the 

fluoride, titanate, or oxide can be encapsulated by 

HWMP Low costs are possible due to low waste 

disposal costs, a large amount of available hot-cell 

space, large-scale equipment, and a large enough workload to permit optimum assignment of personnel 

Analyses of selected samples of the strontium product 

showed about 10 mole% calcium and less than 1 mole% 

of any other single cation The flowsheet for isolation 

of the strontium from Purex high level waste uses 

several cycles of solvent extraction to concentrate the 

product from very large volumes of waste and effect a 

gross separation from the major contaminants The 

product from solvent extraction is purified from calcium using a sulfate purification step Except for the 

rare earth and lead, this material meets the requirements for encapsulation Adjusting to a pH of 10 and 

filtering should remove these elements from solution 

Compatibility of strontium fluoride with container 

materials was reviewed The strontium purity being 

achieved by HWMP is adequate for storage, but may not 

be adequate for use in heat sources The presence of 

trace impurities such as sulfate, phosphate, lead, managanese, and sodium may have a deleterious effect on 

the high temperature compatibility of the fluoride with 

materials of containment This, in turn, can endanger 

the long-term mteguty of the strontium fluoride 

package Elimination of traces of water m the final 

encapsulated package could require modifications to 

the proposed installation Additional data on strontium 

fluoride compatibihty are necessary to determine the 

required purity for heat source uses 

Phase diagrams including strontium fluoride as one of 

the components were reviewed Sodium fluoride and 

strontium fluoride do not form a solid solution under 

any conditions, but they do form an equimolar eutectic 
13 

with a melting point of about 850°C Thus, the theimal 

equilibrium composition expected m HWMP strontium 

product IS a bulk phase consisting of alkahne earth 

fluorides and a small amount of a second phase 

containing alkali—alkaline earth fluoride eutectic The 

properties of the bulk phase can be evaluated with 

sufficient accuracy from existing data The properties 

of the impurity phase cannot be evaluated adequately 

from existing data 

As decay of the strontium proceeds, ZrF2 is created 

m the lattice This rather unstable molecule has been 

reported and its properties are said to be those of group 

IV-A difluondes Disproportionation would be expected to occur when a sample of old encapsulated 

SrFa IS brought to 800°C for the first time This would 

probably mean a decrease m melting point as the ZrF4 

is formed and makes eutectic mixtures with other 

fluorides 

Plan for Next Penod 

Progress of the HWMP will be followed by close 

coordination with ARHCO and Division of Production 

Changes in process and encapsulation equipment will be 

recommended when necessary to permit commericai 

utilization of the HWMF products 

Equipment similar to that used for producing non 

radioactive cesium sources wdl be acquired and used for 

fabrication of fully radioactive sources Prototype 

sources will be evaluated for licensing and suitabihty tor 

commercial use 

Process technology tor preparing strontium com 

pounds other than the fluoride in HWMP will be 

developed Accumulation of currently available data for 

licensing strontium fluoride will be completed and 

additional data will be developed 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

HANFORD FISSION PRODUCT 

PRODUCTION CAPABILITIES* 

Objective of Work 

The objective of this project is to evaluate the 

production of heat and radiation sources to customer 

*D J Larkin and 1 D Moore Atlantic Richfield Hanford 

Co , Richland, WA 99352, Contract AT(45 1) 2130 

specification, using the fission products separated as 

part of the Hanford Waste Management Program 

(HWMP) Construction of a plant for the encapsulation 

of CsCl and of SrF2 is m progress and startup is 

scheduled for 1974 

Progress aod Results 

Three separate studies were undertaken to evaluate 

the production of special Sr-90 and Cs-137 sources In 

the first study, the capability of the encapsulation plant 

to produce up to 5 megacunes annually as doubly clad 

Sr90 sources (as SrF2, SrO, or SrTiOs) m capsules 

ranging from 1 to 4 in in dia and having thermal output 

of from 20 to 2000 W each was evaluated Encapsulation plant equipment additions modifications and 

development work costs were estimated 

In the second study, information regarding the 

production of special Cs-137 radiation sources and 

encapsulation plant operating cost was developed 

Production of 10 and 100 CsCl sources similar m 

design to the HWMP capsule but containing inert partial 

inserts was found feasible This work could be per 

formed without modification to the existing equipment 

and with a minimal capital expenditure The number of 

capsules per year and the insert diameters are listed 

below for production of this type of source 

Number of Capsules per Year Insert Diameter 

10 1 m 

10 1*72 m 

100 1 m 

100 1V2 m 

Evaluation of other capsule sizes indicated that 

production of forty l-m dia sources without the inserts 

IS feasible with the work force presently planned If 400 

of these capsules were to be produced annually, the 

staff would have to be increased by ~30% 

Plan for Next Period 

A report will be issued annually, giving a current 

assessment of Hanford's fission product production 

capabilities Included will be information on plant flow 

sheets, operating costs, production rates and schedules, 

existing plant facilities, and isotope supplies and purities 

Reports Published 

None 
14 

Estimated Date of Final Report 

July 1, 1972 (Annual Report) 

FISSION PRODUCT RHODIUM, 

PALLADIUM, RUTHENIUM, AND 

TECHNETIUM RESEARCH* 

Objective of Work 

The initial objective of this program was to measure 

the radiation characteristics of the fission product 

rhodium and palladium produced in power reactors, 

and to study ways of recovery of these two elements 

from the fuels reprocessing wastes The program has 

been expanded to include ruthenium and technetium, 

and the emphasis of the goals has been placed on the 

practical aspects of the safe use of these four elements 

The expanded program has five tasks 

1 Evaluation of rhodium and palladium produced in 

power reactors 

2 Technology for recovery of Rh, Pd, Tc, and Ru 

*P P Roberts, J C Sheppard, and R S Kemper, Battelle, 

Pacific Northwest Laboratory, Richland, WA 99352, Contract 

AT(45-1)-1830 

3 Market analysis of Rh, Pd, Tc, and Ru 

4 Economic analysis of Rh, Pd, Tc, and Ru production 

from nuclear wastes 

5 Fabrication process development for nuclear source 

Rh, Pd, Tc, and Ru 

The overall program is designed to establish whether or 

not any of these fission products are candidates for 

industrial apphcation The desirability of use of each of 

these elements must be based on future requirements, 

economic feasibility, and the degree of the radiological 

hazards inherent m their use 

Progress and Results 

The principal radiation characteristics of the rhodium 

and palladium formed in power reactors have been 

established Palladium-103 and Rh-102m are the radioactive isotopes which will be important m defining 

restrictions placed on the use of these two fission 

products Ruthenium has two radioactive isotopes with 

significantly long half-lives, Ru-103 and Ru-106 The 

Ru-106 will be the hmiting radioactivity Technetium 

from fission is essentially 100% Tc-99 The radiation 

characteristics of these fission products are given in the 

table 

Radiation Characteristics of Rh, Pd, Ru, and Tc Isotopes 

Isotope Half-hfe Decay mode 

Maximum beta Gamma energies. 

energy, MeV MeV 

Specific 

activity,'' 

MCl/g 

Rh-102 

Rh-102m 

Pd-107 

Ru-103 

Ru-106 

Tc-99 

206 d 

3 38y 

7 X lO' 

39 6 d 

368 d 

2 12x 

' y 

l oS 

Beta 

Positron 

EC 

EC 

Beta 

Beta 

Beta 

Beta 

1 29 

none 

0 04 

0 70 

3 54" 

0 292 

0 475(57%) 

0 511(25%) 

0 632(54%) 

0 698(41%) 

1 110(22%) 

0 418(13%) 

0 475(95%) 

0 632(54%) 

0 768(30%) 

1 050(41%) 

1 110(22%) 

none 

0 497(88%) 

0 610(6%) 

0 512(21%)* 

0 622(11%) 

1 050(1 5%) 

1 130(0 5%) 

1 550(0 2%) 

none 

1900 

290 

90 

5X10 « 

5 X 10** 

1 71 X 10'* 

"The specific activities are for the fission product mixture The values for ruthenium are the 

"worst case" and are probably too high 

^These include the daughter radiations from Ru-106 
15 

The half-life of Rh-102m has been determined Its 

value IS 3 38 ± 0 05 yr The precise value of this half-life 

is important in projecting the specific activity of a 

fission product at various cooling times The specific 

activity of rhodium from a typical power reactor was 

found to be 290 ^tCi/g at discharge 

The dose rate from fission product palladium has 

been measured Surface dose rates from unshielded 

slabs IS 0 83 rad/hr, but with 7 mg/cm^ shielding (this is 

the thickness of the human skin) the dose rate is 

essentially zero 

An examination of the supply—demand relationships 

for Rh, Ru, Pd, and Tc was made Recent geological 

data indicate that the world's platinum metal reserves 

are well established and that major discoveries are 

unlikely Bureau of Mines data and calculations using a 

logistical growth model indicate expanded use of the 

platinum metals and a resource deficit after 1980 

Breeder reactors, such as the LMFBR, may be a 

significant source of light platinum metals if these 

reactors are built in projected numbers 

The future use of these fission-produced elements is 

contingent on establishment of their radiological haz 

ards The control potential of these radioactive plati 

num metals was investigated in terms of environmental 

dispersion and mixing with nonradioactive platinum 

metals Vaporization appears to be the primary dispersion mode for palladium, largely used for switching 

contacts, and rhodium, used m the catalytic production 

of nitric acid There are sufficient thermodynamic and 

experimental data available to make qualitative esti 

mates of these losses 

Analysis of potential radiological hazards of fissionproduced palladium suggests that internal doses are very 

small and that the skm-contact dose may be biologically 

insignificant More work should be done to confirm 

these conclusions before radio-palladium is used in large 

amounts 

Rhodium and ruthenium produced by nuclear re 

actors are radioactive enough to represent a present 

hazard and should be stored 20 to 40 yr before use as 

substitutes for nonradioactive material When considered m terms of future resource scarcity, there may 

be justification for the separation and storage of these 

fission-produced platinum metals 

Plan for Next Period 

The radiation characteristics of the fission products 

Rh, Pd, Ru, and Tc are now sufficiently well defined to 

permit analyses of the hazards associated with their use 

No further studies are planned at this time A report 

summarizing all of the data obtained will be issued 

during the coming period 

Further studies on the technology for recovery of the 

fission products Rh, Pd, Ru, and Tc from nuclear fuels 

reprocessing wastes will be carried out The objective is 

to find a simple economical process for isolating Rh, 

Pd, Ru, and Tc from the other fission products 

The market and safety analysis will be completed and 

a report will be issued 

The economic analysis to determine the feasibility of 

recovery and use of the fission products Rh, Pd, Ru, 

and Tc will be completed Efforts will be initiated to 

develop fabrication processes for the fission products 

Rh, Pd, Ru, and Tc 

Reports Published 

R G Nelson and D P O'Keefe, A Study of TungstenTechnetium Alloys - Concluding Progress Report 

October 1, 1966 - August 1, 1968, USAEC Report 

BNWL-865, Battelle-Northwest, 1968 

C A Calvin, Recovery of Palladium from Nuclear 

Waste Solutions Using a Packed Column of Tricapyrl Monomethyl Ammonium Chloride on an 

Inert Support, USAEC Report ARH-1346, 1969 

J V Panesko, Recovery of Rhodium, Palladium, and 

Technetium on Strongly Basic Anion Exchange 

Resin, USAEC Report ARH-1279, 1969 

J V Panesko, Process for Recovery of Rhodium, 

Palladium, and Technetium from Aged Reprocessing Wastes at Hanford, USAEC Report ARH-733, 

1968 

F F Roberts, Fission Product Rhodium and Palladium, 

USAEC Report BNWL-CC-2239, Battelle-Northwest, 1969 

Estimated Date of Final Report 

The next major report will be issued in January 1972 

EVALUATION OF LARGE-SCALE USES 

FOR PURIFIED FISSION PRODUCT 

XENON* 

Objective of Work 

The objectives of this work are to reprocess existing 

stocks of crude fission product xenon to such a purity 

(low Kr-85 content) that specimens can be offered to 

interested large scale users m exchange for the results of 

*C A Rohrmann, Battelle, Pacific Northwest Laboratory, 

Richland, WA 99352, Contract AT(45 1) 1830 
16 

their evaluation of the product in their various applica 

tions 

Progress and Results 

Purification of the first volume (approximately 900 

liters, STF) of fission product xenon was completed at 

ORNL The composition and quality of this material 

was as follows 

Xenon: 99.93% 

Kr-85 less than 1 (one) microcurie per liter (STP) xenon 

Isotopic Composition 

Xe-124 

126 

128 

129 

130 

131 

132 

134 

136 

Other Gases 

F P Xe 

0 01% 

0.08 

0 04 

10 34 

16 61 

29.21 

43 70 

Atmospheric Xe 

0 096 

0.090 

1.92 

26 44 

4 08 

21 18 

26 89 

10.44 

8 87 

CO None Hj Less than 200 ppm (0 02%) 

CH4 None N2 Less than 300 ppm 

Hydrocarbons None O2 Less than 200 ppm 

H2O None CO2 Less than 200 ppm 

Ar Less than 200 ppm 

These figures for other gases are the limits of 

detection by the ORNL methods used. From the xenon 

purity figure it is concluded that the actual concentration of these other gases is far below the indicated 

numbers. It is also concluded that the sum of the 

concentrations of all such contaminant gases could not 

reach 700 ppM. 

Contacts with prospective evaluators 01 users of this 

material were continued. The progress of the project 

was also reviewed with visitors 

Plan for Next Period 

Formal announcement of the quahty and availability 

of the existing stock of punfied gas will be made to a 

variety of producers, users, and nuclear fuel processors 

with the expectation that some requests for the 

material will be received. Purification of the remaining 

stock of available crude fission product xenon will be 

completed to yield a total of about double the piesent 

volume of pure material Progress being made by those 

who will be provided with material for test or evaluation will be followed. 

Reports Published 

C A Rohrmann, Fission Product Xenon and Krypton 

- An Opportunity for Large Scale Utilization, 

Isotop Radiat Technol, 8(3) 253-260 (Spring 

1971) 

Estimated Date of Final Report 

The next major report on this program will probably 

be the Annual Report for FY-1972, which will be 

issued early in FY-1973 

PROMETHIUM-146 REDUCTION* 

Objective of Work 

The objective of the Pm-146 burnout program is to 

demonstrate the technical feasibility of reducing the 

Pm-146 content m power source promethium to less 

than 0 1 ppM by neutron capture Such a reduction of 

the Pm-146 content would substantially lower the 

radiation level of promethium and enhance its value for 

biomedical apphcations 

Progress and Results 

Previous Pm-146 burnout experiments in Hanford and 

Savannah River reactors did not reduce the Pm-146 

level in promethium to the desired level of less than 0.1 

ppM Analysis of these experiments and those related to 

the production of Fu-238 heat source material containing low Pu-236 concentrations indicated the importance 

of the Pm-147(n,2n)Pm-146 and Fm-147(7,n)Pm-146 

back reactions. Additional analysis showed that, m 

addition to the high Pm-146 cross section of 3500 

barns, the extent of Pm-146 burnout is determined by 

the following factors (1) Structural members of reactors containing iron, chromium, and nickel are 

important sources of high energy gammas capable of 

inducing the Pm-147(7,n)Pm-146 reaction and should 

be avoided (2) Promethium target matrix and cladding 

materials can be important sources of the 

Pm-147(7,n)Pm-146 reaction Aluminum may be an 

important high energy gamma source and should be 

avoided Impurity levels of iron, nickel, and chromium 

may be important contributors to the 

Pm-147(7,n)Pm-146 back reaction Zirconium, beryllium, tantalum, and graphite are desirable cladding and 

matrix materials (3) Location of the promethium 

target element m a well moderated region of a reactor 

*J C Sheppard, Battelle, Pacific Northwest Laboratory, 

Richland, WA 99352, Contract AT(45-1)-1830 
17 

can significantly reduce the contribution of the 

Pm-147(n,2n)Pm-146 back reaction 

Analysis has shown that the Pm-146 content m 

promethium can be successfully reduced to 0 1 ppM or 

below by neutron irradiation, provided that the 

contributions of the Fm-147(7,n)Pm-146 and 

Fm-147(n,2n)Pm-146 back reactions are carefully minimized Other data indicate that such irradiation conditions are attainable in the HFIR, ORR, Savannah River 

Cf-252, and Hanford N reactors 

Plan for Next Period 

This program was terminated at the end of FY-1971 

Reports Published 

None 

Estimated Date of Final Report 

Results of this program were reported in 

BNWL-1308-7, Pacific Northwest Laboratory, Division 

of Isotopes Development Programs Quarterly Report 

May-July 1971, August 1971 

FISSION PRODUCTS 

DEVELOPMENT LABORATORY* 

Objective of Work 

The Fission Products Development Laboratory provides Sr-90 and Cs-137 products on the megacurie level 

of annual production Feed material is received from 

Aflantic Richfield Hanford Corporation (ARHCO) as 

purified Sr(90)CO3 and crude Cs-137 sorbed on an 

inorganic ion exchanger The Sr-90 is converted to 

strontium titanate or strontium oxide, densified by hot 

pressing, and encapsulated as heat sources The Cs-137 

IS purified by alum crystallizations, converted to 

Cs(137)Cl, and encapsulated as radiation sources or 

shipped as powder Pilot plant testing of chemical 

process and mechanical fabrication techniques and 

production are accomphshed simultaneously 

Progress and Results 

Shipments of fission product feed material from 

ARHCO included two shipments of Sr-90 totaling 1 

million Ci and one shipment of Cs-137 containing 400 

thousand Ci An improved Cs-137 shipping cask design 

and improvements m the cask elution process resulted 

*R W Schaich, Oak Ridge National Laboratory, P O Box X, 

Oak Ridge, TN 37830, Contract No W-7405 eng 26 

in a ten-fold increase in Cs-137 concentration in the 

process equipment with corresponding savings in processing costs Detailed cost records for one process cycle 

resulting m 70 thousand Ci of Cs(137)Cl product 

revealec a basic product cost of $0 14 per curie A total 

of 19 Sr-90 sources containing 1 065 million Ci and 41 

Cs-137 sources containing 47 thousand Ci were fabricated 

One shipment of Sr-90 from ARHCO contained 

unusually high (3 4 mole%) stable rare-earth content 

that would dimmish the power density of the product 

fuel form A separation process was developed and used 

to give 63% removal of the rare earths by an oxalate 

precipitation technique 

Hot pressing of the strontium titanate fuel form is 

used to provide the high power density pellets required 

for isotopic power generators Improvements in hot 

press operating efficiency resulted from the design 

improvements m vacuum-atmosphere—resistance heated 

and inert-atmosphere—mduction-heated hot presses Die 

body hfe was prolonged by using carbon filament 

reinforced strength members 

Test pressings of stable strontium titanate powder are 

being made to define the optimum process conditions 

A problem strontium titanate composition, Sr3Ti2 07, 

that results in low pellet density was defined by x-ray 

diffraction analysis of test pellets A procedure utilizing 

calorimetric analysis of Sr(90)CO3 followed by dry 

mixing with T1O2 was developed to provide closer 

control of product composition 

Containment of strontium titanate fuel forms is 

usually provided by Hastelloy—C-276 capsules which 

are sealed by mert-gas, tungsten-arc welding to provide 

0 055-in penetration Small variations in alloy formulation or in fit between the cap and capsule body can 

cause welds of insufficient penetration A remote 

plasma arc weld technique was developed to provide 

greater than 0 080-in penetration in capsule seal welds 

Plan for Next Period 

Several of the operating cells need refurbishing to 

correct equipment failures which have occurred over 

the past several years that the equipment has been in 

use Work will continue to improve the fuel forms 

which affect hot-pressed pellet integrity 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 
18 

ORNL REACTOR-PRODUCED 

RADIOISOTOPES PROGRAM* 

Objective of Work 

The principal objective of the ORNL reactorproduced radioisotopes program is the development of 

new and improved techniques and procedures to prepare, characterize, and support the use of radioisotopes 

produced by neutron irradiation Improved or previously unavadable research materials for use in medical, biological, and physical sciences are provided 

Experimental irradiations are performed in the HFIR 

(see figure) and other AEC research or production 

reactors in order to obtain very high neutron fluxes 

*T A Butler, Oak Ridge National Laboratory, P O Box X, 

Oak Ridge, TN 37830, Contract W-7405-eng-26 

(>10'^ n/cm^-sec) and desired neutron energy spectra 

for the reactions being investigated 

The program objective is accomplished by (1) examination of the principal modes of neutron interaction 

[(n,a;), (n,p), and (n,7)] with naturally occurring or 

enriched isotope targets, (2) development of appropriate chemical or physical processes to recover and purify 

the desired radioisotope, (3) characterization of the 

product purity and determination of unknown or 

uncertain nuclear properties such as half-hfe and decay 

scheme, and (4) establishment of cooperative programs 

with research groups to promote the beneficial apphcations of these radioisotopes 

Progress and Results 

The preparation of radioisotopes for use in the 

development of medical diagnostic procedures and 

REACTOR PRESSURE 

VESSEL 

HB-4 

HB-3 

Plan view of Hi ^ Flux isotope Reactor (HFIR) core. 
clinical apphcations through cooperative programs was 

emphasized as part of our special research materials 

interests Cooperative research studies demonstrated the 

value of K 43 in imaging the myocardium and quan 

tizmg infarction An appropriate increase in the ORNL 

pilot production effort was made in order to supply the 

increasing demand for K 43 for use in chnical evalua 

tion studies Cerium 141 m the form of high specific 

activity wafers of Ce( 141)02 was supphed as a special 

research material to the Los Alamos Scientific Labora 

tory 

Separate project summaries describe work on K43, 

P 33, Si 32, Tm 170, and Ft 195m 

Plan for Next Period 

This continuing project will emphasize the use of 

reactor produced radioisotopes by continuing to de 

velop special research materials for cooperative pro 

grams with pubhcly or privately funded research groups 

and to improve the quality of the radioisotope prepara 

tions 

Reports Published 

See summaries of individual projects 

Estimated Date of Final Report 

Continuing project 

Anterior and left anterior oblique gamma camera images of 

POTASSIUM-43* 

Objective of Work 

The objectives of this project are to prepare K 43 by 

the Ca-43(n,p)K-43 reaction, using isotopically enriched 

Ca(43)0 targets, in quantities sufficient for medical and 

biological experiments, to define a method for sepa 

rating K 43 from the target m a purity suitable for 

medical use, and to establish cooperative programs with 

medical institutions interested in evaluating its useful 

ness Potassium 43, with a half hfe of 22 5 hr and 

gamma ray emissions of 0 373 and 0 617 MeV, is 

potentially useful for metabolic and chnical studies of 

blood flow, rejection of transplanted organs, and 

kidney function because the dose rate would permit 

multiple doses 

Progress and Results 

About 20 targets of enriched Ca(43)0 were irradiated 

in a fast neutron flux of ~1 X 10' ^ n/cm^ s) to deliver 

over 150 mCi K43 Most of the activity was supphed 

for evaluation under medical cooperative programs to 

the University of Mississippi Medical Center, Peter Bent 

Brigham Hospital in Boston, the Johns Hopkins Medical 

Institutions in Baltimore the University Hospitals of 

Cleveland and V A Hospital, Durham, NC These 

cooperative research studies have demonstrated the 

value of K 43 in imaging the myocardium and quan 

tizmg infarction (see figures) 

*J K Poggenburg Oak Ridge National Laboratory P O Box 

X Oak Ridge TN 37830 Contract W 7405 eng 26 

patient with extensive anterior and inferior myocardial infarction 
20 

The effectiveness of the calcium recovery process and 

the abihty of the ion-exchange procedure to pioduce a 

product acceptable for human use have been demonstrated The recovered calcium target shows no degradation of enrichment after a year of use Radioactivities 

other than K-42 m the product aie usually at a level less 

than 10 nanocuries/ml The K-42 is about 12% of the 

activity at delivery 

The physical decay properties of K-43 have been 

studied and evaluated 

Plan for Next Period 

Efforts at process improvement will continue to 

shorten the calcium recovery procedure and maintain 

reliability in processing larger batches Improvements m 

labeling and handhng of the product will be effected 

The study of the decay properties and production 

technique will be pubhshed in reports 

Reports Published 

P J Hurley, M Cooper, R C Reba, J K Poggenburg, 

and H N Wagner, Jr, "^^KCl A New Radiopharmaceutical for Imaging the Heart, / Nucl 

Med, 12 516(1971) 

B L Holman, J K Poggenburg, D F Adams, P Eldh, 

and S J Adelstein, Assessment of Myocardial 

Perfusion and Viabihty with K-43, / Nucl Med, 

12 366 (1971) (Abstract) 

R O Smith, F H Lehan, H K Hellems, and J K 

Poggenburg, Limitation of the Bolus Isotope Infustion for Myocardial Scanning — A Possible Solution, 

J Nucl Med, n 394 (1971) (Abstract) 

J K Poggenburg, K-43 The Reactor Production, 

Physical Properties, and Potential Availability of a 

Useful Radioisotope, / Nucl Med ,12 457 (1971) 

(Abstract) 

K O Smith, P H Lehan, H K Hellems, and J K 

Poggenburg, Scatter Problem When Counting the 

Lower Energies of K-43, / Nucl Med, 12 464 

(1971) (Abstract) 

Estimated Date of Final Report 

1972 

PHOSPHORUS-33* 

Objective of Work 

The purpose of this project is to develop methods of 

preparing hundred-milhcune quantities of carrier-free 

*J K Poggenburg, Oak Ridge National Laboratory, P O Box 

X, Oak Ridge, TN 37830, Contract W-7405-eng-26 

F-33 containing <5% P-32 The two methods of 

producing P-33 being evaluated are based on the 

irradiation of highly enriched targets of S 33 (>92 at %) 

or CI 36 (~69 at %), in a fast neutron flux Phos 

phorus-33 (25 2 d, 0 248-MeV iS^^^) has both a longer 

half life and a lower energy beta than F-32 (14 3 d, 

1 709-MeV l^j^^^), which makes it advantageous for 

autoradiography, ecological and agricultural studies, 

synthesis of tagged complex organophosphorus compounds, and double labeling experiments 

The HFIR is utihzed for quantity production of high 

quahty P 33 at reasonable cost for utilization by 

commercial vendors in providing tagged compounds and 

specialized preparations 

Progress and Results 

The Cl-36(n,a!)P-33 reaction has been determined to 

be the most practical method for large-scale production, 

but the available (>92%) enriched K2S(33)04 was also 

used to produce over 4 Ci of F-33 product The 

recycled KC1(36) target has attained an enrichment of 

69% Cl-36 with Cl-35 depleted to 3% The P-32 content 

in a product produced from this target is <1% at 

processing within one week after reactor discharge The 

capability of routinely producing curie batches of F 33 

has been demonstrated Efforts have been directed at 

building up an inventory of KC1(36) of intermediate 

enrichment for further irradiation enrichment and 

blending into existing target material 

Process improvements include the addition of a 

solvent extraction step using methyl isobutyl ketone to 

remove the bulk of the iron used as a phosphate carrier 

This step was found to remove concomitantly the traces 

of antimony activity leached from the quartz target 

ampules A small cation exchange column is used as a 

final cleanup step A procedure was developed for 

removing casual Cr-51 activity from the product The 

Cr-51 IS usually in the Cr04^ " form and is reduced to 

Cr' * with SOj gas so it can be removed on a cation 

exchange column 

Plan for Next Penod 

Efforts wiU continue towards process and target 

recovery improvements The problem of long-term 

buildup of Cs-134 activity by activation of cesium 

impurity m the targets will be studied and a method for 

its removal will be devised Buildup of enriched target 

will continue 

Reports Published 

L C Brown, Determination of P-32 and P-33 in 

Aqueous Solution, Anal Chem , 43 1326 (1971) 
21 

Estimated Date of Final Report 

Continuing project 

SILICON-32* 

Objective of Work 

The objective of this project is to develop the reactor 

technology for the preparation of microcune quantities 

of Si-32 (~650 y) Silicon-32 exhibits many desirable 

physical decay characteristics that make it an interesting and attractive radionuchde for a variety of 

uses (1) as the only long-lived radionuchde of silicon 

for use in agriculture, geology, sohd-state physics, etc , 

(2) as a parent for a Si-32—F-32 generator system which 

would offer a constant supply of P-32, and (3) as a 

long-lived counting standard for F-32 determinations 

Progress and Results 

Three multiple-neutron-capture reaction paths have 

been considered for the production of microcune 

quantities of Si-32 in the HFIR Two of these reaction 

paths which should yield carrier-free Si-32 were selected 

for investigation [P-31(n,7)P-32(n,p)Si-32 and 

S-34(n,7) S-35(n,Q:)Si-32] A short irradiation of a small 

AIFO4 target has been performed to produce a tracer 

level sample for chemical process and separations 

development Larger targets of AIPO4 and K2^'*S04 

have been fabricated and inserted for extended irradiation, le , >6 to 12 months, at high thermal and fast 

neutron fluxes for microcune production 

Plan for Next Period 

Process development will be undertaken using the 

tracer level sample mentioned above while larger production targets are irradiated Production samples will 

be processed as the irradiations are completed Measurements of the Si-32 half-life will be made and P-32 

burnup cross section will also be determined in the 

course of this work 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

*L C Brown and J K Poggenburg, Oak Ridge National 

Laboratory, P O Box X, Oak Ridge, TN 37830, Contract 

W-7405-eng 26 

THULIUM-170* 

Objective of Work 

The objectives of this research are to provide sufficient data on Tm-170 to permit reasonable assessment 

of Its potential apphcation, to permit preliminary 

engineering design of power sources, and to develop 

data for safety analysis It has been proposed as an 

isotopic power source for short-duration missions The 

economics for reactor production of Tm-170 (1285 

days, 0 32 MeV j3^y) from natural Tm-169 are favorable 

and the sesquioxide (Tm2 03) offers a promising fuel 

compound, having a practical specific power of approximately 2 W/g and a power density of approximately 16 

W/cm' The study includes measurements of thermal 

conductivity, leach rates, high-temperature compatibility with suitable containment metals, vapor pressure, 

and fuel-form densification 

Progress and Results 

The effusion method, using two Knudsen cells of 

different sizes, was employed in the determination of 

rates of effusion and partial and total pressures of 

various vapor species above solid Tm203 and Yb203 

(both nonradioactive) Two Tm2 03—Yb2 03 mixtures 

(l7 wt% and 28 wt% Yb2 03) have been prepared by 

the coprecipitation method for this work The selection 

of the first Yb203-Tm203 mixture (17 wt% Yb203) 

IS based on the typical initial composition of the 

thulium(170) sesquioxide fuel source The second 

mixture is chosen to represent the composition of the 

fuel source after a period of one half-life (128 days) 

which was assumed to be the maximum mission life of a 

thulium(170) sesquioxide source 

Values of the apparent vapor pressure of Tm2 03 

(sum of the partial pressures of vapor species above 

solid Tm2 03) thus obtained at 1990°C ranged from 

2 38 X lO"'' to 3 25 X 10"'' atm The apparent vapor 

pressure of Yb2 03 at 1990°Cis2 22X 10"" atm 

In the thulium(170) sesquioxide—refractory metal 

compatibility studies, 16 compatibility couples have 

completed exposure runs at 1600°C Of these, the 

exposure time for 8 couples was 2500 hr, and that for 

the other 8 was 5000 hr The potential capsule 

materials tested included TZM, Ta-10% W, T-111, and 

tungsten Two thuhum(170) sesquioxide-tungsten 

couples were exposed at 2000°C for 500 hr The results 

*K H Lin and J K Poggenburg Oak Ridge National 

Laboratory, P O Box X, Oak Ridge, TN 37830, 

W-7405-eng-26 
22 

of the examination of the radioactive samples will be 

compared with the data from a similar study using 

nonradioactive Tm2 03 and YbjOs to determine 

whether there was any effect attributable to radioactivity 

Plan for Next Period 

Further experiments will be earned out to complete 

the vapor pressure data for Tm2 03, Yb2 03, 17 wt% 

Yb2 03-Tm2 03, and 28 wt% Yb2 03-Tm2 03 m the 

temperature range from 1800 to 2300°C The compatibility study will emphasize examination of the exposed 

compatibility couples and assessment of the results of 

examination 

A final summary report of all AEC-sponsored research 

on thuhum oxide properties will be completed 

Report Published 

None 

Estimated Date of Final Report 

1972 

PLATINUM-195m* 

Objective of Woik 

The objectives of this work are to develop methods 

for preparing platinum isotopes suitable for whole-body 

scanning m biological and medical experiments and to 

establish cooperative programs with medical research 

groups interested m evaluating their usefulness 

Recent medical research has shown that certain 

platinum compounds act as chemical therapeutic agents 

towards certain tumors There is need for platinum 

radioisotopes as tools for investigating the therapeutic 

mechanism involved Platinum-195m (4 1 d) has gamma 

emissions of 99 keV (12%) and 129 keV (3%) which 

make it suitable for whole-body scanning 

Progress and Results 

Several reactor irradiations of 57% enriched Pt-194 

were made and a cooperative research program was 

estabhshed with Michigan State University to test the 

radioisotope in their antitumor studies The Pt-195m 

was supphed in an aqua regia solution from which both 

the CIS- and trans- dichloro-diammine Pt(ll) compound 

was synthesized and administered mtraperitoneally to 

tumor-infected mice 

*J K Poggenburg, Oak Ridge National Laboratory, P, 0 Box 

X, Oak Ridge, TN 37830, Contract W-7405-eng-26 

The irradiations identified several problems with the 

Ft-195m The best enrichment of Pt-194, the 57% 

target used, contains 8% Ft-196 and 0 4% Ft-198 

Because of the larger capture cross sections of Ft-196 

and Ft-198, the irradiated target contains much more 

Ft-197 (20 hr) and Au-199 (from Ft-199 (5' Au-199) 

activity than Ft-195m activity The gold activity can be 

completely removed by two extractions with methyl 

isobutyl ketone The presence of Ft-197 requires an 

additional correction m the whole-body counting procedure and requires the use of a silicon or germanium 

detector to assay both the Ft-195m and Pt-197 which 

have photon energies too close to be adequately 

resolved with Nal The results of a 10-day irradiation 

suggest that the activation cross section to produce 

Ft-195m may be an order of magnitude less than the 

0 09 barn quoted in BNL-325 

Plan for Next Period 

Platinum-195m will continue to be supplied for 

cooperative research Other platinum isotopes will be 

investigated Experiments will be directed toward establishing the production cross sections for Pt-195m 

Reports published 

None 

Estimated Date of Final Report 

1973 

BNL ACCELERATOR 

PRODUCTS DEVELOPMENT* 

Objective of Woik 

The overall objective of the BNL accelerator products 

development program is to increase the use of radionuchdes and techniques involving their use in medicine, 

industry, and research The program is designed to 

make maximum use of the unique accelerator capabilities avadable at Brookhaven, including a new highenergy proton linear accelerator presently under construction, as an injector for the Alternating Gradient 

Synchrotron as well as the rebuilt 60-m cyclotron and 

two Van de Graaff generators The work is primarily 

exploratory in nature and involves determining the 

feasibility of radionuchde production by new technqiues or improving existing methods Goals of this 

*P Richards, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-1)-16 
23 

program are the development of new radionuclides as 

well as increasing the quantities, improving the 

purity, and reducing the cost for existing nuclides The 

effort also entails the development of technology 

required for radionuclide preparation in existing and 

planned medical and commercial cyclotrons and the 

supplying of special radioisotopes for the collaborative 

BNL biomedical radioisotope program and collaborative 

programs with other institutions The potentialities of 

high- (spallation) and low-energy proton or triton 

reactions and the use of on-machine recoil labeling 

techniques are being evaluated for product development The program is divided into three categories (1) 

the BNL Linac Isotope Producer (BLIP), (2) cyclotron 

products, and (3) Van de Graaff generator technology 

Progress and Results 

See summaries of individual projects 

Plan for Next Period 

See summaries of individual projects 

Reports Published 

See summaries of individual projects 

Estimated Date of Final Report 

Continuing project 

THE BROOKHAVEN LINAC 

ISOTOPE PRODUCER (BLIP)* 

Objective of Work 

The objective of BLIP project is to explore the 

capabilities of a high-energy proton linear accelerator 

for the production of a large variety of radionuchdes by 

spallation reactions as well as by low-energy proton 

reactions 

The construction of a 200-MeV proton Lmac is 

presently nearing completion at Brookhaven National 

Laboratory to inject high-intensity pulses of protons 

into the Alternating Gradient Synchrotron (AGS), a 

machine used for high-energy physics research Excess 

beam capacity of the Lmac (average current of ~ 180 

/uA), required for beam monitoring and maintenance of 

equipment stabihty, is available for radionuchde production studies in a beam-stop facility where targets 

*L G Stang, Jr , P Richards, and E Lebowitz, Brookhaven 

National Laboratory, Upton, NY 11973, Contract AT(30 1)-16 

may be placed to intercept the beam Such a facility 

will have unique potential for isotope production for 

two reasons (1) the high proton energy combined with 

a relatively high beam intensity and (2) the continuous 

mode of operation High incident particle energy will 

allow the bombardment of multiple independently 

interchangeable targets simultaneously while continuous operation will make long term irradiations of 

targets feasible 

The BLIP project is designed to evaluate a number of 

unexplored capabilities in isotope preparation, including (1) the production of short- and long-lived 

activities by both fast and slow reactions simultaneously, (2) the discovery of new nuchdes, (3) the 

preparation of both neutron rich and neutron deficient 

products, (4) greatly increased quantities or improved 

purity of certain existing nuchdes with important 

apphcation potential, and (5) the production of milhgram quantities of long-lived materials presently available only in minute amounts Part of the beam time is 

expected to be available for service irradiations 

Progress and Results 

Since BLIP incorporates the first high-energy accelerator to be used for isotope development and production, 

much original effort has been required to realize the full 

capability of this unique machine The design of a 

facihty for utilization of the beam has been completed 

and construction should be nearly complete by the end 

of 1971 Work is being coordinated with the start-up of 

the Linac which is currently in preliminary operation 

but will not require beam dumping until early m 1972 

The water tank beam stop was fabncated and 

installed A 32-ft depth of water will serve as a 

transparent, flexible shield against the high-energy 

neutrons generated during operation A prefabricated 

operations building has been constructed over the beam 

stop tank The remote target manipulation system has 

been fabricated and installed in the tank This will allow 

the insertion into or removal from the beam of a 

number of individual targets, each with its own cooling 

system 

A standard target holder assembly has been developed 

and is shown in the figure Preliminary studies of target 

processing, equipment development, and the modification of existing processing facilities have been started 

Work has been started on several products, including 

Fe-52, 1-123, Xe-127, and Ta-179 Several low-mtensity 

bombardments have been earned out on target materials in the Lmac tunnel to verify heat transfer 

calculations 
24 

#####• 

BLIP target assembly. From left to right: 1. Target holder with inlet and outlet coohng water connections. 2. Two typical 

metalhc targets. 3. Metal 0-ring. 4. 0.005-in. stainless-steel window. 5. Retaining flange. 

Plan for Next Period 

Deflection of the 200-MeV proton beam into BLIP 

should start by the beginning of 1972. The facility, 

including the target handling equipment and target 

cooling system, should be completed and in operation 

early in the year. Experimental studies of radiation 

damage, heat transfer, and target manipulation problems will be undertaken. 

Preliminary production parameters for certain nuclides will be evaluated for comparison with previously 

calculated data. The development of chemical processes 

for specific products will be under way and exploratory 

production should start during 1972. Some of the 

typical products to be investigated initially include (1) 

1-123 (half-life, 13 hr), which has the best physical 

properties of all iodine isotopes for medical diagnostic 

scanning; (2) Fe-52 (half-life, 8 hr), which is the only 

isotope of iron suitable for chnical diagnostics and is 

expected to find use in studying the distribution of 

functioning bone marrow in various diseased states; (3) 

Ta-179 (half-life, 1.6 yr), which decays by electron 

capture, emits 55-keV x rays and should find important 

uses in radiography, transmission scanning, and as a 

source for gaging instruments; and (4) Xe-127 (half-life, 

36 d), which, with its higher energy photons, appears to 

be superior to the presently used Xe-133 for studies of 

lung perfusion and ventilation. 

Some irradiations of special targets for outside interests should also take place during 1972. 
25 

Reports Pubhshed 

None 

Estimated Date of Final Report 

Continuing project 

BNL CYCLOTRON PRODUCT 

DEVELOPMENT* 

Objective of Work 

The objectives of the BNL cyclotron program are 

twofold (1) to develop production technologies for 

radionuchdes for potential apphcation in collaborative 

studies with the BNL Medical Research Center and for 

cooperative programs with other institutions and (2) to 

develop production information useful to both medical 

and commericai cyclotrons, existing and planned The 

BNL 60-in cyclotron can accelerate protons to 40 

MeV, deuterons to 20 MeV, He-3 to 60 MeV, and He-4 

to 40 MeV Because of its relatively high energy and its 

ability to accelerate both hydrogen and helium isotopes, this machine has unique capabilities both to 

produce useful quantities of biomedically useful radionuclides and to develop production parameters for use 

on other machines with lesser capabilities The program 

IS also involved in areas of target development and 

materials, chemical processing, and purification procedures 

Plan for Next Period 

See summaries of individual projects 

Reports Published 

E Lebowitz, M W Greene, M Kinsley, and P 

Richards, The Development of New and Improved 

Isotopes for Nuclear Medicine with the Brookhaven 

Cyclotron - Dy-I57 and Bi-204, / Nucl Med , 

12(6) 376-7(1971) 

Estimated Date of Final Report 

Continuing project 

*P Richards, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30 1) 16 

DYSPROSIUM-157* 

Objective of Work 

Hydioxyethylethylenediaminetriacetic acid (HEDTA) 

complexes of many rare-earth nuclides are good bone 

seekers, while many of the rare-earth colloids locahze m 

bone marrow Dysprosium-157 has excellent physical 

characteristics (half-hfe, 8 2 hr, photon energy, 326 

kilovolts m 91% abundance) The objective of this 

study is to develop the necessary production technology and produce sufficient Dy-157 for evaluation as 

a bone and bone marrow scanning agent This work is 

being carried out in cooperation with Dr John McAfee 

of the State University of New York at Syracuse 

Progress and Results 

A method has been developed for producing and 

separating by ion exchange Dy-157 m high yield (~30 

mCi/iuAh), high-specific activity (~100 Mg of rare-earth 

material m sample), high radiopurity (<10"'* radiocontammants), and high chemical purity In addition, 

the excitation function has been measured and evaluation of methods of production earned out to assist 

potential producers of Dy-157 

Good results have been obtained at the Upstate 

Medical Center in Syracuse, using Dy-157 for both bone 

and bone marrow imaging depending on the chemical 

form m which the nuclide is administered 

The excitation function for the reaction 

Tb-159(p,3n)Dy-157 was determined by irradiation of a 

stack of terbium foils and subsequent assay of the 

Dy-157 activity with a Ge(Li) detector Copper flux 

monitors were included m each stack of foils to 

determine the proton beam current 

In the production method, a terbium foil (825 

mg/cm^) is irradiated with 33-MeV protons m the 

external cyclotron beam After bombardment and 

target dissolution the carrier-free Dy-157 is separated 

from the terbium target material by ion exchange 

chromatography on AG 50W—X12 resin with elution 

by a-hydroxyisobutyric acid (HIBA) Optimum conditions for the separation have been determined and 

Dy-157 of excellent purity has been achieved The 

product activity is converted to the desired chemical 

form for administration 

This work has shown that, although very high yields 

are obtained at higher energy protons, the 22- and 

26-MeV commercial cyclotrons can still produce practical quantities of Dy-157 

*E Lebowitz, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-l)-16 
26 

Plan for Next Period 

More full-scale production runs will be carried out to 

supply coOaborating institutions with Dy-157 for clinical evaluation 

Reports Published 

G Subramanian, J G McAfee, R J Blair, R E 

O'Mara, M W Greene, and E Lebowitz, Dysprosium-157-HEDT A for Skeletal Imaging, / Nucl 

Med , 12 558-61 (1971) 

G Subramanian, J G McAfee, M Rosenstreich, A 

Mehter, M W Greene, and E Lebowitz, Dysprosium-157 Gluconate A New Radiopharmaceutical 

for Bone Marrow Imaging, / Nucl Med , 12(6) 

400(1971) 

Estimated Date of Final Report 

July 1972 

AUXILIARY CYCLOTRON BEAM 

MONITOR DEVELOPMENT* 

Objective of Work 

The objective of this project is to develop methods to 

accurately measure the amount of a cyclotron beam 

that IS actuahy striking the target Some causes of the 

uncertainty in this measurement may be the use of a 

target smaller than the beam, a misahgned beam, or 

measurement by the target current monitor of secondary particles introduced into the beam by its 

passage through a window or air gap A simple 

technique to check the beam current consists m 

simultaneously irradiating a copper foil with an identically shaped target The cross section for the production in copper of the measured reaction product must 

be known If a Ge(Li) detector is used for the 

radioisotope assay, no chemistry is required and the 

beam current is calculated from the assay and cross 

section data 

Progress and Results 

In the previous report (TID-4066) an auxihary cyclotron beam monitor for use with He-3 and He-4 beams 

was described A similar technique for monitoring 

proton beams using cross sections reported m the 

hterature gave serious discrepancies between the 60-m 

*E Lebowitz, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-1)-16 

0 10 20 30 

PROTON ENERGY MeV 

Excitation function for the reaction Cu-63(p,2n)Zn-62. 

Present work indicated by error bars and compared with other 

hterature values 

BNL cyclotron monitoring system and the foil monitors Therefore, independent measurements of proton 

cross sections on copper were made Polyethylene foils 

were bombarded as a check of the cyclotron beam 

integration system by using the very accurately measured (±3%) cross sections for the C-12(p,pn)C-ll 

reaction to determine beam current Reasonable agreement with the cyclotron beam integration system was 

obtained Our results are shown in the figures 

This auxihary beam monitoring system offers a 

simple, rapid, and accurate method to cyclotron users 

for determinmg the beam current striking a target 
27 

0 10 2 0 3 0 

PROTON ENERGY M9V 

Excitation function for the reaction Cu-65(p,n)Zn-65. Present 

work mdicated by error bars and compared with other literature 

values 

Reports Published 

E Lebowitz and M Greene, An Auxihary Cyclotron 

Beam Monitor, Int J Appl Radiat Isotop , 21 

625(1970) 

Estimated Date of Final Report 

Continuing project 

VAN DE GRAAFF GENERATOR 

TECHNOLOGY* 

Objective of Work 

The development of methods for the production of 

Mg-28 and F-18 by the bombardment of targets with 

tntons accelerated m a Van de Graaff generator was 

described in a previous edition of this report 

(TID-4066) 

A study IS currently under way to determine the 

feasibihty of labeling potentiahy useful biological compounds wath F-18, a 1 lO-mm positron emitter, by recoil 

techniques The method involves bombarding of a neon 

gas target m a container, whose wahs are coated with a 

compound to be labeled, with deuterons accelerated in 

the Van de Graaff generator The F-18 atoms produced 

by the reaction Ne-20(d,a)F-18 recoil to the target 

waUs and react with the compound to be labeled 

Process and Results 

The targetry and separation technology have been 

developed and a study is presently under way to 

determine the feasibihty of labehng uracil by this 

technique Colhmation of the deuteron beam prevents 

It from hitting and destroying the compound to be 

labeled and the neon target gas is recirculated through a 

hquid nitrogen trap to cool the window and target By 

having the compound to be labeled m the solid phase 

rather than as a gas, higher yields are achieved and the 

radiation damage done to the target compound and 

product compound is minimized The Ne-20(d,ct)F-18 

reaction is advantageous for F-18 recoil labehng because 

the target gas is inert and because the a-recoil energy 

gives the F-18 much initial kinetic energy 

After the deuteron irradiation, the compound coating 

the walls and the fluorine-labeled product are dissolved 

in distilled water and passed through a SrF2 column to 

Plan for Next Period 

Other foil monitors will be developed as the need for 

them arises in the accelerator program 

*E Lebowitz, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-1)-16 
28 

Separation of 1 mg of 5-fluorouracil from 300 mg of uracil. 

remove F" ions (decontamination factor >10'*) The 

effluent of the SrF2 column is then eluted through an 

Amberhte CG-50 (200 to 400 mesh) cation exchange 

column (95 cm X 255 cm at 54°C) to separate the F-18 

labeled compound from the unlabeled compound and 

degradation products (see figure) Since the amount of 

carrier fluoro-compound can be as small as desired, very 

high specific activity material can be produced 

The processing time is approximately two hours from 

the end of bombardment until the final product is 

ready for medical use 

The effect of the filhng target gas pressure on the 

percentage of the F-18 produced which is in the form 

of 5-fluorouracil is shown m the figure Fluorine 

labeling of uracil at other positions of the ring leads to 

an unstable molecule. 

Since the yield stays approximately constant well 

beyond pressures corresponding to the F-18 recoil 

reaching the walls at higher than thermal velocity, the 

labehng is not done by fluorine of high kinetic energy 

It would be expected ihat a mixture of neutral species 

and electronically excited species contribute lO the 

labeling yield. The very low labehng yield obtained at 1 

1.0 

0.5 

n 

1 

1 

1 1 1 1 1 

^ y ^ 3 4 MeV DEUTERONS 

til l 

-

10 15 20 25 

INCHES OF VAC (Hg) 

30 

Yield of F-lS-uiacil as a function of target gas pressure. 

atm indicates that the kinetically deexcited fluorine 

reactive species will become unreactive if enough 

collisions (which could lead, for example, to chemical 

reactions with impurities) are made before it reaches 

the labeling compound 

Plan for Next Period 

Some prehminary measurements have been made 

which indicate that substantially more F-18 activity 

could be produced with higher energy deuterons (~7 

MeV) to which we presently do not have access When a 

higher energy deuteron beam becomes available next 

year on the Brookhaven Radiobiology Van de Graaff, 

we estimate that enough activity could be produced for 

clinical studies 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

XENON-127* 

Objective of Work 

The objective of this study is to develop the production technology as well as to produce Xe-127 for 

clinical evaluation Thirty-six-day Xe-127 with its 

higher energy photons (172 and 203 keV), lack of 

particle emission, and longer shelf hfe, should be 

superior to the presently used 5-day Xe-133 with its 

low-energy photons (which are heavily scattered) for 

*E Lebowitz, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30 l)-16 
29 

studies of lung perfusion and ventilation Initial development of the chemical processing and preliminary 

clinical evaluations will utilize the BNL 60-in cyclotron 

for production of Xe-127 Then large-scale production 

and clinical evaluation will be carried out on BLIP, 

based on the cyclotron results 

Progress and Results 

A study has been initiated to develop the necessary 

technology for the production and separation of 

Xe-127 and to make the isotope available for medical 

evaluation The chemical processing consists of melting 

the salt target (CsCl) and sweeping out the xenon with a 

stream of helium The gas stream flows through a dry 

ice trap to remove any iodine activity and then through 

a liquid nitrogen cooled trap which catches the xenon 

This xenon product can then be used as a gas for 

ventilation studies or can be dissolved m saline for 

perfusion and ventilation studies 

Plan for Next Period 

The optimum technology for the production, separation, and chnical use of Xe-127 will be developed 

Clinical studies with this isotope will be performed at 

the BNL Medical Research Center 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

BISMUTH-204* 

Objective of Work 

The objective of this work is to study the feasibihty 

of producing Bi-204 on the BNL cyclotron for medical 

evaluation studies It has been reported that bismuth 

locahzes m certain types of tumors with a relatively 

high tumor-to-nontumor ratio, suggesting its use m 

nuclear medicine for tumor diagnosis Unfortunately, 

none of the radioisotopes of bismuth have very good 

physical properties for use as a scanning agent Bismuth-204 appears to have the most potential This 

study IS being carried out m a cooperative program with 

Dr Richard E Peterson, University of Iowa Hospitals, 

Iowa City 

*E Lebowitz, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-l) 16 

Progress and Results 

The preferred method for Bi-204 production is via the 

Pb-206(p,3n)Bi-204 reaction Because of radiation dose 

considerations, the Pb target thickness and incident 

proton energy must be carefully controlled to maintain 

high radioisotopic purity of the Bi-204 A metallic Fb 

target has been developed which allows the water to 

impmge directly on the Pb, thereby allowing the use of 

relatively high proton beam currents This method of 

production gives a yield of a few mCi/juAh and high 

product punty (<1% Bi-205, <10% Bi 203) A rapid 

elcctrol>sis method has been developed to separate 

carrier-free Bi-204 in high yield from the Pb-206 target 

and also allow satisfactory recovery of the enriched lead 

for reuse The figure shows the electrolysis ng After 

electrolysis, the bismuth is leached off the platinum 

cathode The following table gives the chemical analysis 

of a typical Bi-204 product solution 

B 

Pb 

Sl 

Cu 

Fe 

Ag 

Mg 

Bi 

Hg 

Sb 

As 

Mn 

Mg 

0 1 

0 5 

~3 

0 5 

0 3 

0 5 

<0 01 

<1 

<1 

<0 1 

<1 

<0 0l 

Cr 

Sn 

Ni 

Mo 

Ge 

Zr 

Be 

Ti 

Nb 

Pb 

Ir 

Mg 

<0 1 

<0 1 

<0 1 

<0 1 

<1 

<0 1 

<0 01 

<0 1 

<0 1 

<0 1 

<1 

Hf 

Ga 

In 

Os 

Pd 

Rh 

Ru 

Co 

Bi 

Al 

Cd 

Mg 

<1 

<0 1 

<0 1 

<1 

<0 1 

<1 

<1 

<0 1 

<0 1 

<0 1 

<1 

— 

ta 

c 

S H 

— 

p 

) 

„ 

« 

^ 

-

Apparatus for electrolytic separation of B-204 from Pb target. 

1 Screw hnk 2 50 ml beaker 3 Pt foil 0 39 mm, 19 mm dia 

connected with 0 4 mm Pt wire 4 Magnetic stirrer 5 

Electrolyte 6 Pyrex pipe 8 mm dia with fine frit 7 Teflon 

plug 8 Pt wffe 0 5 mm dia 
30 

Clinical evaluations are under way at the University of 

Iowa 

Plan for Next Period 

Several full-scale production runs wdl be carried out 

to verify the production method and to continue 

clinical evaluations of Bi-204 for tumor diagnosis 

Reports Published 

None 

Estimated Date of Final Report 

June 1972 

ORNL ACCELERATOR-PRODUCED 

RADIOISOTOPES PROGRAM* 

Objective of Work 

The objective of this work is the development of 

improved targets and target materials, of separationprocess chemistry, and of recovery techniques for target 

materials for the production of isotopes in the ORNL 

86-in cyclotron 

Cyclotron production offers a broad range of available radionuchdes of any element and in some cases 

offers the only practical radionuclide for a given 

element The principal areas of apphcation of neutrondeficient radionuchdes have been radiobiology, nuclear 

medicine, chemistry, metallurgy, and physics A primary source of carrier-free, neutron-deficient radioisotopes continues to be the ORNL 86-m cyclotron 

Progress and Results 

A number of cooperative programs were estabhshed, 

or continued, to assist cooperative participants to fill 

specialized requirements for specific radionuchdes not 

usuaMy available A considerable increase in the Ga-67 

pilot production operations was necessitated by product requirements for an Oak Ridge Associated Universities sponsored cooperative group study of the apphcations of Ga-67 in medicine Indium-111 pilot 

production was also increased in response to growing 

mterest m its medical apphcations 

Development work on Rb-83 and Rb-84 was completed during the previous reporting period with the 

exception of a new half-hfe determination of 86 2 days 

*T A Butler, Oak Ridge National Laboratory, P O Box X, 

Oak Ridge, TN 37830, Contract W-7405-eng-26 

for Rb-83 New development was initiated on the 

production of Cs-129 by proton reaction on enriched 

Xe-129 Considerable interest has been evidenced m 

evaluation of this radionuchde for heart studies 

Separate project summary reports describe the development activities for Ga-67, In 111, Ba-133m, 

Bi-206, and Fb 203 

Plan for Next Period 

See summaries of individual radionuclides 

Reports Published 

See summaries of mdividual radionuclides 

Estimated Date of Final Report 

Continuing project 

GALLIUM-67* 

Objective of Work 

The objective of this program is to determine the 

optimal proton production parameters, e g, target 

configuration, chemical processing, etc , for the preparation of carrier-free Ga-67 (78 2 hr) in acceptable 

punty and quantity for chnical apphcafions research 

and development Interest m this isotope has been 

spurred by evidence of a high uptake of carrier-free 

Ga-67 by lymphoid tumors in both animals and 

humans This discovery was made during the evaluation 

of carrier-free Ga-67 as a bone-scanning agent for a 

patient with Hodgkin's disease and has since been 

successfuUy extended to chnical studies of several types 

of malignant neoplasms 

Progress and Results 

The chemical processing development stage, le , 

separation and purification of the product, has been 

completed and reported The natural-isotopicabundance zinc tube target (0 375 m OD X 0 020 in 

wall thickness) has been tested extensively and found 

acceptable for moderate-scale production (200 to 300 

usable mCi/target) This target configuration has been 

used to produce more than 25 Ci of Ga-67 (leference 

time end of bombardment) during the past year for 

distribution through cooperative programs and for sale 

as an experimental product 

*L C Brown, Oak Ridge National Laboratory, P O Box X, 

Oak Ridge TN 37830, Contract W-7405-eng-26 
31 

Plan for Next Period 

The current zinc tube target design also yields Ga-66 

(9 5 hrj that is produced concurrently by the 

Zn-67(p,2n)Ga-66 reaction This activity must be allowed to decay, usually 3 to 4 days, before the Ga-67 

product can be used Further effort will be apphed to 

develop enriched Zn-68 targets for increased Ga-67 

yields and minimum Ga-66 contamination, thereby 

reducing the required decay time Pilot production will 

be continued to supply Ga-67 to cooperative participants and as an experimental product for research and 

development evaluation 

Reports Published 

L C Brown, Chemical Processing of CyclotronProduced Ga-67, Int J Appl Radiat Isotop , 22 , 

710-13(1971) 

Estimated Date of Final Report 

Continuing project 

INDIUM-111* 

Objective of Work 

The initial objectives of this program were to define 

and optimize the pertinent production parameters for 

the economical preparation of In-Ill of satisfactory 

quahty for radiopharmaceutical manufacture The current objectives are to obtain practical operating experience of the procedures developed for pilot production 

and to provide this radionuclide to interested users as a 

special research material for their evaluation and apphcation. Indium-111 has been either used for or suggested for such studies as spinal-cerebral cisternography, 

aerosol lung studies, delayed brain scanning, visuahzation of the lymphatic system, metabohc studies of 

indmm-labeled macroaggregates and colloids, and tumor 

locahzation Indium-111 has gamma emissions of 171 

keV (89%) and 245 keV (94%) - ideally suited for 

external detection — and an optimal half-hfe (2 82 d) 

for labehng and distribution studies which must be 

carried out over 24 hr or longer 

Progress and Results 

Development of the large-scale cyclotron production 

of In-111 by the Cd-11 ](p,n)In-l 11 reaction path and 

*L C Brown, Oak Ridge National Laboratory, P O Box X, 

Oak Ridge, TN 37830, Contract W 7405-eng-26 

of the associated chemical processing, i.e., separation 

and purification of the product, has been completed 

and reported The product has a radionuchde purity of 

>99 9% and contains <20 Mg Cd and <5 ng Fe per ml 

of solution. Additional operating experience has been 

obtained from pilot production during the past year 

that has shown that the process consistently yields a 

pyrogen-free, high-purity product acceptable for human 

use More than 3 Ci of In-111 has been produced during 

this period for distribution as a special research 

material 

Plan for Next Period 

Pilot production will continue to supply In-111 as a 

special research material in batch lots to customers 

interested in its use and evaluation 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

BARIUM-133m* 

Objective of Work 

The medium to heavy alkaline earths (i e , Ca, Sr, and 

Ba) have been used extensively as bone-scannmg agents 

Due to the high toxicity of barium, the preparation of 

low-dose, carrier-free Ba-133m by the Cs133(p,n)Ba-133m reaction has been initiated as a 

possible alternative to lower specific activity, neutronproduced Ba-135m (28 7 hr) Banum-133m has a single 

prominent gamma ray of suitable energy (276 keV) and 

intensity (17%) for scanning Production of Ba-133m 

would be possible with conventional low-energy cyclotrons, whereas preparation of high specific activity 

Ba-135m requires a high-flux reactor 

Progress and Results 

Two prehminary irradiations have been completed, 

with one product being retained for characterization 

and one being distributed to cooperative participants 

for evaluation Thick-target production rates of ~350 

mCi/mA-hr with >99 9% Ba-133m radionuchdic punty 

(le , <0 1% Ba-133) have been achieved for short 

*L C Brown, Oak Ridge National Laboratory, P O Box X, 

Oak Ridge, TN 37830, Contract W-7405-eng-26 
32 

irradiations of a CsCl target Attempts to extend this 

target configuration to longer irradiation times resulted 

m premature target failure, presumably due to the 

~15% volume expansion of CsCl at 496°C resulting 

from a change m crystal structure 

A preliminary ion-exchange separation scheme has 

been devised and initial testing begun with good results 

Banum-133m is separated from a dilute HCl solution of 

the cesium target material by passage through a strong 

cation exchanger The ion-exchange resin is then 

washed with IM HCl to remove any remaining cesium 

ions and cobalt and strontium radionuchdic impurities 

before removal of the product with 4M HCl The 

preliminary evaluation of this isotope by cooperating 

participants indicates that it is comparable to Ba-135m 

Plan for Next Period 

Work Will be continued on target design, chemical 

processing, and product characterization Developmental production runs will be performed to verify 

production parameters and product punty, and to 

supply cooperating participants with material for product evaluation 

Reports Published 

None 

Estimated Date of Final Report 

1972 

BISMUTH-206* 

Objective of Work 

The objectives of this program are to evaluate the 

pertinent production parameters and to provide 

6 24-day Bi-206 for evaluation as a diagnostic radionuchde m medicine Bismuth-206 has been used to 

delineate brain tumors m patients with known brain 

tumors which are poorly visualized by more common 

radionuclides Even though very favorable tumor-tobackground activity ratio has been obtained by earlier 

workers, the lack of an appropriate scanning system 

suitable for the high-energy emissions of this nuclide 

[803 keV (99%), 880 keV (72%), 895 keV (19%), et 

al ] has retarded the evaluation of the isotope A 

cooperative program for the evaluation of Bi-206 as a 

diagnostic radionuchde using a high-energy photon 

*L C Brown, Oak Ridge National Laboratory, P O Box X, 

Odk Ridge, TN 37830, Contract W-7405-eng-26 

scanning system has been undertaken as part of this 

program with Vanderbilt University 

Progress and Results 

Bismuth-206 has been prepared by both the 

Pb-207(p,2n)Bi-206 and Fb-206(p,n)Bi-206 reactions 

using isotopically ennched targets The Bi-205 contaminafion levels of punfied bismuth products obtained 

from these two production paths have been determined 

to be 1 1 and 12 1% for the (p,2n) and (p,n) reactions, 

respectively The patient radiation dose from Bi-205, 

which IS produced from proton-induced reactions on 

isotopic impurities m the ennched targets, is estimated 

to be •~2-V2 times that from Bi-206 As a result of these 

findings, development of the (p,2n) production path 

will be pursued to provide a lower dose product 

Excitation functions shown in the literature indicate 

that the (p,2n) production path should also offer larger 

production rates than the (p,n) path for the proton 

energies available, that is, <22 MeV Prehminary work 

has begun on a PbCl2 precipitation—cation exchange 

separation procedure to separate lead and bismuth 

Preliminary data indicate greater than 95% bismuth 

recovery 

Plan for Next Period 

Development of a high current, high yield, enriched 

Fb-207 cyclotron target will be pursued Process development has been only prehminary and will be 

continued to obtain a rapid and efficient process which 

yields a product suitable for human use Product 

characterization and specifications will also be determined concurrent to process development 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

LEAD-203* 

Objective of Work 

The objective of this work is to investigate the proton 

production parameters of high-purity Pb-203 suitable 

for human use Lead-203 (52 1 hr) has been suggested 

*L C Brown, Oak Ridge National Laboratory, P O Box X, 

Oak Ridge, TN 37830, Contract W-7405-eng-26 
33 

as a possible bone-scanning agent with an acceptable 

half-hfe for production and shipment and with low 

radiation dose decay characteristics (i e , it decays 

solely by electron capture with the emission of two 

main gamma rays of 279 and 401 keV with intensities 

of 81% and 5%, respectively) Three medical cooperative programs have been estabhshed to perform the 

apphcations evaluation of this nuclide 

Progress and Results 

Lead-203 can be produced with <22-MeV protons by 

two different reaction paths (1) Tl-203(p,n)Pb-203 or 

(2) Pb-204(p,2n)Bi-203 -ECiS" -^Pb-203 Prehminary 

experiments utihzing the first reaction path have been 

undertaken for the initial investigation due to the ready 

availabihty of a cyclotron target holder design and the 

lower cost of the enriched target material. A prehminary irradiation has been carried out, and the Pb-203 

produced supphed to a cooperating participant for 

evaluation. A prehminary separation procedure based 

on the extraction of Tl(III) from a 2M HBr—Br2 

solution into isopropyl ether, followed by a cation 

exchange chromatographic separation of Pb-203 from 

the aqueous raffmate, has been employed A 94% 

chemical yield with >99 9% radiochemical purity was 

obtained from this process Additional chemical process 

development is indicated by a high total sohds content 

of the first experimental product 

Plan for Next Period 

Additional target design and chemical process development Will be undertaken The relative economics of 

reaction paths (1) and (2) will be evaluated to determine whether increases in cyclotron yield will offset the 

added cost of the more expensive Pb-204 target 

material Full-scale irradiations will be performed and 

the Pb-203 produced distributed to cooperating participants for apphcations evaluation 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

BNL BIOMEDICAL 

PRODUCTS DEVELOPMENT* 

Objective of Work 

The primary objective of the BNL biomedical development program is to increase the use and usefulness of 

radionuclides m biomedical apphcations Technology 

resulting from this program is used to develop new 

materials for biomedical research and to improve 

diagnostic tracers for many hospitals while furnishing 

technology useful to the commercial radioisotope industry Areas of work include (1) the incorporation of 

suitable existing radionuchdes, as well as of new 

radioisotopes resulting from developments m the BNL 

accelerator development program, into special chemical 

forms for use in new or improved biomedical apphcations and (2) the development or improvement of 

radioisotope generator systems and their evaluation 

This program is carried on in collaboration with 

members of the staff of the BNL Medical Research 

Center as well as m cooperation with other medical 

institutions 

At the present time, major emphasis is being placed 

on the continued development of Tc-99m, as it is 

considered to be the best radionuchde for use in most 

radioisotope procedures because of its ideal physical 

properties and its general widespread availabihty Technetium-99m studies relating to its use m nuclear 

medicine are being carried out on a broad front 

including technetium chemistry, technetium-labelmg 

techniques, and the improvement and simplification of 

existing technetium procedures The development of 

analytical techniques can also be expected to play a 

greater role This work will later be expanded to include 

other radionuchdes appearing to have potential use m 

biomedical apphcations 

Plan for Next Period 

See summaries of individual projects 

Reports Published 

H L Atkins, K. G Cardmale, W C. Eckelman, W 

Hauser, J F Klopper, and F Richards, Evaluation 

of Tc-99m-DTPA Prepared by Three Different 

Methods, Radiology,98 674 (1971) 

*P Richards, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-1)-16 
34 

H L Atkins W C Eckelman, W Hauser, J F Hopper, 

and P Richards Evaluation of Glomerular Filtra 

tion Rate with Tc 99m-DTPA, / Nucl Med , 

12(6) 338(1971) 

Estimated Date of Final Report 

Continuing project 

CHEMICAL STUDIES OF 

TECHNETIUM-99m* 

Objective of Work 

The objectives of this project are to obtain a more 

thorough understanding of the chemistry of technetium 

in some of the presently used technetium labeled 

compounds and to develop information useful m the 

labeling of other potentially useful biological materials 

Progress and Results 

A number of analytical methods have been surveyed 

to determine if equihbnum constants can be obtained 

for technetium biomedical products Various methods 

using spectroscopy were not successful because the 

technetium chelates studied did not have a strong 

absorption either in the visible or near ultraviolet 

region 

Fotentiometric determination of the equihbnum con 

slant was not possible because of the interaction of the 

chelates with the titrating solutions Ceric ions were 

used to fitrate the reduced states of technetium 

produced by stannous ion and ferrous ion However, 

when chelate was added, the cenc ion oxidized the 

chelate and no equilibrium values could be obtained 

The reversibility of the reactions taking place with 

technetium is also questionable, and therefore this 

approach was not carried further 

Another method used to determine equihbnum constants IS that of partition chromatography Solutions of 

various technetium—chelating agent ratios were eluted 

across Sephadex G25 and the partition of technetium 

was used to calculate equihbnum values Studies at 

various pH values and concentration ranges were undertaken These studies have the advantage that they can 

be performed with carrier-free technetium whereas 

spectroscopic methods require large amounts of carrier 

technetium However, the analysis of the data showed 

that the system did not involve a simple equilibrium 

*W Eckelman, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-1)-16 

between one technetium species and the chelating 

agent The use of concentrated HCl to leduce the 

technetium resulted in a system which was comphcated 

by slow hydrolysis of the reactive technetium species 

and by a possibihty of mixed valence states in addition 

to the desired reaction Attempts to reduce technetium 

by stronger reducing agents such as stannous ion 

ehminated the mixed oxidation state comphcation, but 

the system was apparently still susceptible to irreversi 

ble hydrolysis reactions which prevent the elucidation 

of equihbnum expressions 

Another area of work concerned with the chemical 

state of technetium involves the development of analytical techniques that can accurately idenfify various 

components m these products Work here and at other 

laboratories has shown that technetium activity is 

associated with several components following the chemical manipulations commonly used in preparing labeled 

compounds Technetium—HSA, for example, usually 

contains varying amounts of technetium activity as a 

chelate, as unreacted pertechnetate, and as a hydrolyzed form as well as that which is bound to HSA 

The recent hterature contains much misleading analytical data concerning the identification of these 

various technetium components in biomedical products 

Inasmuch as the different forms of technetium have 

different biological behavior, failure to identify and 

quantify them can result m misuse of the compound or 

give incorrect internal dose calculations This study has 

compared various analytical methods now m use to 

determine the advantages and disadvantages of each 

method Commonly used technefium-labeled compounds were analyzed by anion exchange chromatography, by paper chromatography with both 85% methanol and sahne as solvents, and by gel chromatography 

(Sephadex G25) 

Results show that the most widely used techniques, 

ion exchange and paper chromatography with methanol, give the least discriminating analysis Ion exchange 

on anion resins will separate pertechnetate from the 

other components but does not identify other fractions 

Paper chromatography with saline solvent gives somewhat better identification of components but there 

appears to be some oxidation or breakdown on the 

paper because of the small sample size Gel chromatography, with nitrogen-purged sahne as eluant, will 

separate and identify technetium4abeled proteins, 

chelates, hydrolysis products, and pertechnetate Gel 

chromatography seems to be the single analytical 

method of choice but nevertheless it seems advantageous to use more than one analytical method whenever 

possible 
35 

Plan for Next Period 

Fuither etforts wiU be made to determine the 

oxidation state and physical constants of Tc-99m in 

biomedical products Additional work is also required 

to improve analytical techniques for Tc-99m biomedical 

products 

Reports Published 

W Eckelman, G Memken, and P Richards, The 

Chemical State of Tc-99m in Biomedical Products, 

/ Nucl Med , 12 596(1971) 

Estimated Date of Final Report 

Continuing project 

INSTANT Tc-99m COMPOUNDS* 

Objective of Work 

One of the present goals of the Biomedical Development Program at BNL is to prepare technetium compounds which contain a single component, as demonstrated by various analytical techniques, and which can 

be easily prepared, ideally by adding pertechnetate to a 

prepared solution Such a one-step, single-component 

product would enable the widespread use of this 

compound, especially if it were commercially available 

to those hospitals and clinics that have limited radiopharmaceutical facilities Such a system would also 

enable sterihty and pyrogemcity to be determined 

before use 

During the development of a red blood cell labeling 

procedure, the effectiveness of stannous ion in carrying 

out the above mentioned objectives was noted Therefore, single-component one-step products are being 

formulated using stannous ion as the reducing agent 

Progress and Results 

An instant procedure foi the preparation of the 

chelate TcDTFA (diethylenetriaminepentaacetic acid) 

has been reported previously (TID-4066) This instant 

compound has been used successfully in single injection 

methods for determining renal clearance rates Infusion 

techniques are usually thought to yield more reliable 

clearance values because equilibrium of the infused 

substance is achieved between the plasma and the 

extravascular space 

*W Eckelman, Brookhaven National Laboratory Upton, NY 

11973, Contract AT(30-1)-16 

To perform constant infusion studies, large volumes 

of instant TcDTPA are required Therefore, a study was 

initiated to determine the factors involved in the use of 

500-ml volumes of TcDTPA The use of large volumes 

of stock SnDTPA did not seem advisable because of the 

toxicity of the stannous ion Therefore, a minimum 

amount of stock solution (5 ml) was used to retain 

reducing power, and the overall stability of the 

TcDTPA was maintained by adding DTPA to maintain 

constant molarity This combination of factors resulted 

m a solution of 500 ml of TcDTPA which showed a 

yield of 95% for a period of 5 hr as measured by gel 

chromatography 

Samples of urme and plasma from the infused dogs 

were assayed by gel chromatography to determine the 

stabihty of the chelate Technetium was excreted in the 

urme exclusively as TcDTPA The plasma samples 

contained a plateau value of 10 to 15% protein bound 

technetium as a result of breakdown of the constantly 

infused TcDTPA The protein binding in a single 

injection of TcDTPA is ~5% as determined by gel 

chromatography After correction for protein binding 

of the infused TcDTPA, the renal clearance values 

indicate that the TcDTPA is filtered exclusively by the 

glomeruh and not readsorbed by the tubules 

The second instant procedure developed was that for 

TcHSA (human serum albumin) The approach was 

similar to that used in TcDTPA Stannous HSA chelate 

was prepared at various pH values However, unlike the 

DTPA case, the majority of the tin could not be 

chelated with up to 250 mg HSA (~3 micromoles) This 

presented problems because colloidal tin could compete 

with the HSA for the technetium The elimination of 

this competitive binder effect was achieved with varying 

success by (1) using less initial stannous ion, (2) 

removing the tin colloid before addition of pertechnetate, and (3) adding the technetium at a pH sufficiently low to prevent tin hydrolysis The procedures 

incorporating these three approaches are given m the 

first table Both of the procedures which incorporate 

stock solutions at pH 6 give relatively high yields, but 

both were more variable and not as high as the low pH 

method In this procedure, the technetium is added to a 

solution of SnCl2 •2H2O and HSA at pH 2, which was 

determined to be the binding pH giving the highest 

yield This preparation gives TcHSA of >95% yield and 

high reproducibihty It is not a one-step procedure, 

since the tm HSA cannot be stored at pH 1 because of 

gel formation and because the pH must be raised aftei 

pertechnetate addition However, the manipulations 

necessary to add HSA, pertechnetate, and buffer are 
36 

LowpH Method 

Instant Procedures 

Excess Tin Not Removed Excess Tm Removed 

1 ml of 250 mg/ml HSA 

IS added to 0 5 ml of 

2mg/mlSnCl2-2H20* 

0 l-2ml««'"TcOi-is 

added 

The solution is mixed 

for one minute 

The pH of the solution 

IS raised to 6 with 

IMNaOH** 

Terminal dilution up to 

20 ml total can be made 

if lower HSA concentration 

is desired 

4 ml of 250 mg/ml HSA 

IS added to 2 ml of 

1 mg/ml SnCl2-2H20* 

The pH of the solution 

IS raised to 6 with 

IMNaOH** 

0 l-lml'*'"TcOi*is 

added per ml stock solution 

as needed** 

Terminal dilution up to 

20 ml total can be made 

if lower HSA concentration 

IS desired*** 

4 ml of 250 mg/ml HSA 

IS added to 2 ml of 

1 mg/ml SnCl2*2H20* 

The pH of the solution 

IS raised to 6 with 

lAfNaOH** 

The entire solution is 

eluted across a 35 cm 

Sephadex G25 column 

with saline eluant 

The protein fractions are 

collected and the solution 

assayed for HSA 

concentration 

0 1 1 m mii 1CU4 «""TcO^ : IS 

added per ml stock solution 

as needed*** 

*Preparation of SnCl2*2H20 solution The appropriate amount of SnCl2*2H20 is dissolved m 2 5 ml concentrated 

HCl with heat The solution is then diluted to 25 ml with N2 purged distilled water 

**NaOH solution of <M NaOH should be used to neutralize the solution to prevent localized concentrations of 

strong base which lead to formation of hydrolyzed technetium 

***A11 stock solutions are stored under nitrogen 

Variation of pH for 

pH Tc HSA 

0 9 63 

2 2 80 

3 3 59 

15-•mm mix 

Tc hydride 

37 

20 

31 

Yield of ' 

pH 

2 4 

2 9 

3 5 

39mJ^. Hs ^ ^g Function of pH and Time 

Variation of pH 

TcHSA 

96 

91 

82 

for 30 mm mix 

Tc hydride 

4 

9 

18 

Mm 

5 

15 

30 

Variation of time at 

TcHSA 

82 

87 

96 

p H 2 5 

Tc hydride 

18 

13 

4 

Reaction of 1 ml of TCO4 with 25 mg HSA and 250 Mg SnCl2'2H20 in appropriate solution of HCl Final pH of 6 1 achieved 

with 0 15 ml 0 8M NaH2P04 Analysis performed on Sephadex G25 

well worth the increased yield and rehability obtained 

as compared to the two one-step instant procedures 

The critical variables were also determined for production of high specific activity HSA using 25 to 50 mg 

HSA instead of the 250 mg used in the original low pH 

procedure The results of these experiments are given m 

the second table The maximum yield seems to be 

obtained at pH 2 0 to 2 5, as in the case of 250 mg 

HSA As expected, the labehng of HSA using 25 mg 

HSA was slower than the labehng using 250 mg HSA 

Whereas the 250 mg HSA produces yields of >95% with 

one-minute mixing at low pH, the 25 mg HSA 

procedure requires 30-min mixing at low pH to achieve 

comparable yields Use of 50 mg HSA did not increase 

the yields significantly and 30 mm was still required to 

achieve yields of >95% 

Plan for Next Period 

It appears that development of kits for other biologically interesting compounds may be possible using 

similar procedures The major emphasis will be on lung, 

kidney, and bone scanning agents 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 
37 

TECHNETIUM-99m LABELED Red Cell Filterability Studies 

RED BLOOD CELLS* 

Obj"ective of Work 

The objective of this work is to develop an improved 

method for labeling red blood cells with Tc-99m This 

product IS valuable for spleen scanning and for blood 

pool studies Chromium-51, presently used to label 

cells, does not have the favorable decay characteristics 

that technetium does 

Progress and Results 

The development of methods for the labehng of red 

blood cells with Tc-99m and then altering the cells for 

use in visualization of the spleen has been previously 

reported Further work m this area included additional 

studies of both the labehng procedure and the altera 

tion or damaging procedure The original labehng 

procedure, as a result, has been shortened substantially, 

and the abbreviated method makes Tc-99m labehng 

competitive with the more commonly used Cr-51 

procedure Studies of the glucose levels and fluoride 

exchange reactions using F-18 tracer indicate that the 

mechanism of labehng involves pertechnetate crossing 

the membrane by passive diffusion The pertechnetate 

is then reduced by the stannous ion and bound 

mtercellularly Approximately 30% of the technetium 

appears to be associated with the hemoglobin whereas 

the remaining technetium is reduced and bound to a 

low molecular weight species as yet unidentified There 

does not seem to be any alteration of the transport 

properties of the cell but rather simple diffusion of 

pertechnetate with subsequent chemical binding to the 

intracellular components 

A second aspect of the work involves alteration or 

damaging of the cells so that they will be removed by 

the capillary system of the spleen thus enabling the 

physician to visualize the spleen The measurement of 

the osmotic fragihty of the cells as a means of 

determining the degree of alteration indicated that 

increasing amounts of stannous citrate made the cells 

more fragile Measurement of filterability of the red 

cells, perhaps a closer analogy to the action of the 

spleen m removing altered red cells, was also undertaken A Milhpore filter of 5 micron pore size was used 

to filter the cells altered to various degrees by the use of 

different amounts of stannous citrate and citrate alone 

The results of this study are given m the table From 

these results, animal experiments were set up Increas-

*W Eckelman, Brookhaven National Laboratory, Upton NY 

11973, Contract AT(30-1) 16 

ml of 1 mg/ml SnCl2 •2H2O* Flow rate at 4 in Hg 

m ACD (ml/min) 

0 0 033 

0 1 0 033 

2 0 027(81%) 

3 0 027 

*Added to 4 ml packed red blood cells 

mg amounts of splenic uptake were observed, respectively, with the use of 2 ml of stannous citrate, 4 ml of 

citrate alone, and 4 ml of citrate mixed at 37°C — all 

added to 4 ml of packed red cells Trials on humans, 

however, did not indicate such drastic differences and, 

therefore, the standard procedure of altering the cells 

with excess citrate (1 ml of citrate per ml of packed red 

cells) IS now used 

Chnical evaluation involving double isotope studies 

has indicated that >5% of the cells accumulate in the 

spleen and that good spleen visualization is achieved at 

these levels The alteration procedure contains only one 

additional step during the labehng procedure, making it 

easier to carry out than the more commonly used heat 

treatment method Better uniformity of the citrate 

altered cells may also make dynamic studies more 

reproducible The higher photon yield and imaging 

characteristics of Tc 99m make this procedure superior 

to the Cr-51 labehng and heat treatment method 

Plan for Next Period 

Clinical evaluation of the red-cell labeling procedure 

will be completed 

Reports Published 

W Eckelman, P Richards, W Hauser, and H Atkins, 

Technetium Labeled Red Blood Cells, / Nucl 

Med , 12 22(1971) 

W Eckelman,? Richards, H L Atkins, W Hauser, and 

J F Klopper, Visualization of the Human Spleen 

with Tc-99m Labeled Red Blood Cells, / Nucl 

Med , 12 310(1971) 

W C Eckelman, P Richards, W Hauser, and H L 

Atkins, Reply to a Letter to the Editor, / Nucl 

Med Concerning Comparison of Tc-labeled Red 

Blood Cells Prepared by Two Methods, / Nucl 

Med,12 577(1971) 

Estimated Date of Final Report 

June 1972 
38 

NEW CESIUM-137 SOURCE COMPOUNDS 

DEVELOPMENT AND EVALUATION* 

Objective of Work 

The objectives of this project are (1) the study and 

development of new Cs-137 source compounds (other 

than CsCl) having a high degree of stability in contact 

with aqueous solutions and in a high temperature 

environment, including preparation methods and product characterization, and (2) an economic assessment of 

the conceptual process designs resulting from the study 

Progress and Results 

The hterature study and the preliminary experimental 

investigation continued in order to evaluate technical 

feasibihty and economic potential of Cs-137 source 

compounds other than Cs(137)Cl High temperature 

stabihty, low solubihty in aqueous solvents, and good 

mechanical properties are among the criteria estabhshed 

for such compounds The initial phase of the study was 

the development of preparation methods for cesium 

mobates and cesium tantalates The three methods 

investigated were the molten CsOH-MjOs reaction (M 

IS either Nb or Ta), the CSOH-M2O5 (or 

CS2CO3—M2O5) slurry reaction, and the simultaneous 

solvent extraction—chemical reaction Of these 

methods, the one based on slurry reaction appears most 

attractive. 

Characterization of the cesium mobates and tantalates 

included determination of the chemical composition 

(M/Cs ratio, M is either Nb or Ta), solubilities in 

seawater and distilled water, and stability at elevated 

temperatures The volumetric specific activities 

(Ci/cm^) of the products were computed from the 

chemical composition and estimated values of densities, 

assuming an isotopic purity of 36 5% Cs-137 Various 

properties of the cesium mobates and tantalates thus 

determined were correlated with the methods of preparation as well as the reaction conditions 

The volumetric specific activit> of cesium tantalate 

products ranged from 60 to 82 Ci/cm^, and was 

primarily governed by the stoichiometry (1 e , Ta/Cs 

ratio) of the product which, m turn, is strongly 

influenced by the calcining temperature For products 

from the molten CsOH—Ta2 0s reaction and the 

CS2CO3—Ta2 05 slurry reaction, the amount of seawater msolubles (68 to 100%) is favored by a high 

Ta/Cs ratio which results m a low specific activity The 

*K H Lin, Oak Ridge National Laboratory, P O Box X, Oak 

Ridge, TN 37830, Contract W-7405 eng-26 

melting points (temperatuie at complete melting) of 

most cesium tantalates were m excess of 1350°C Runs 

with short slurry reaction times resulted m products 

with low melting points Compounds with low Ta/Cs 

ratios had a tendency to display some degree of thermal 

instability, 1 e . low melting point, mcongruent melting, 

and thermal decomposition 

For cesium mobates, the trend in the variation of the 

specific activity (60 to 90 Ci/cm^) with the product 

stoichiometry (Nb/Cs ratio) was the same as that for 

the tantalates However, no simple relation was apparent between the stoichiometry, the amount of 

seawater msolubles, and the thermal stability In general, cesium mobates were thermally less stable than 

cesium tantalates Especially notable was the presence 

of several mcongruent melting temperatures for most 

cesium mobate products The melting point (790 to 

1340°C) increased with increasing calcining temperature 

Both cesium tantalates and mobates have good 

potentials as Cs-137 gamma sources The volumetric 

specific activity of these compounds compares favor 

ably with that of Cs(137)Cl gamma sources (~100 

Ci/cm^) They exhibit considerably lower solubility in 

an aqueous solution and higher stability in a high 

temperature environment than cesium chloride Cesium 

tantalates appear to be especially attractive since it is 

feasible to obtain a product having a specific activity 

greater than 70 Ci/cm^, with extremely low solubihty 

and with a melting point in excess of 1350°C A 

summary of the characteristics ot cesium tantalates and 

mobates obtained to date is given m the table 

According to the prehminary economic evaluation 

(based on the conceptual flow diagram and estimated 

processing factors), the fixed capital costs and the 

manufacturing costs for the processes producing cesium 

tantalates (or mobates) would probably be of the same 

order of magnitude as those for the CsCl process based 

on the (NH4)2C03-NH4 0H eluant 

Cesium vanadates were also prepared using methods 

similar to those for cesium mobates and tantalates The 

volumetric specific activity of cesium vanadates was 

estimated to be about the same (74 to 83 Ci/cm^) as 

those of mobates and tantalates of equivalent stoichiometrics Cesium vanadates have an advantage over 

cesium tantalates and mobates in that the mass absorption coefficient for the gamma radiation would be 

appreciably smaller However, the low thermal stabihty 

(melting points are probably 700°C or lower) and the 

relatively high solubihty (~70% solubles) of cesium 

vanadates m an aqueous solution make them less 

desirable than either mobates or tantalates as a gamma 

source 
39 

Characteristics of Selected Cesium Tantalate and Niobate Products 

(Tentative) 

Composition 

(atomic ratio) 

Estimated 

density 

g/cm^ 

Sea water 

insoluble" 

wt % 

Melting Temperature, C* 

Complete Incongruent 

Estimated 

volumetric 

spec act 

Ci/cm 

3c 

Cesium Tantalates 

Ta/Cs 

1 28 

1 10 

1 55 

Nb/Cs 

145 

1 49 

67 

66 

69 

5 1 

5 1 

93 7 

90 0 

100 0 

>1350 

>1350 

>1350 

67 8 

73 8 

60 5 

Cesium Niobates 

-90 

-90 875,1005 

885 

1325 

64 9 

64 3 

"Powder sample 

^Based on observation under high temperature microscope (maximum 1350 C) 

i^Volumetnc specific activity of a ^^^CsCl gamma source is approximately 100 Ci/cm 

Studies are in progress on ceramic compounds of 

cesium , such as Cs2 0-AI2 O3 • nSi0 2 and 

Cs2 0-MgO-nSi02 These compounds were prepared by 

first forming the water-glass4ike compound 

Cs2 0-nSi02, followed by reaction with AI2O3 or 

A1(0H)3 and MgO, respectively, and finally calcining 

the products at elevated temperatures The volumetric 

specific activity of the products is estimated to be in 

the range of 43 to 66 Ci/cm^ depending upon the value 

of n (' to 4) 

Plans for Next Period 

The study and development of new Cs-137 source 

compounds will continue More detailed and precise 

characterization will be carried out for selected products The production process conditions will be defined 

more specifically and economic assessment made for 

most promising source compounds 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

STRONTIUM SILICATE 

BETA SOURCE DEVELOPMENT* 

Objective of Work 

The objectives of this project are to develop methods 

for fabrication of high performance Sr-90 beta sources 

that have thm windows to yield high radiation output, 

to characterize the physical properties of the sources, 

and to determine radiation output characteristics 

Progress and Results 

Studies were carried out to determine high temperature compatibility of strontium sihcate minibeads m 

aluminum matrix and encapsulated in 347 stainless 

steel Fabricated sources were heated in air for a period 

of 1080 hr at temperatures ranging from 350 to 900°C 

In all test source samples heated m the temperature 

range of 600 to 900°C, mtermetallic diffusion between 

the matrix material and stainless steel capsule occurred 

The reaction progressed to a depth of 0 006 in into the 

capsule wall Samples tested at 250°C showed no 

evidence of reaction between the capsule wall and the 

aluminum/strontium sihcate, indicating sources prepared by this method can be subjected to a continuous 

use m temperatures up to 250°C Evaluation of the test 

sources indicates that severe reaction between the 

source capsule and the aluminum/strontium sihcate will 

occur above 500°C 

Graphite was substituted for aluminum as a matrix 

for strontium sihcate beads Beads were coated with 

pyrolytic carbon using a mixture of propane and helium 

at a temperature of 1050°C A second method using a 

mixture ot graphite flour and a phenohc binder was 

mvestigated A mixture of strontium silicate beads and 

*T S Mackey and F N Case, Oak Ridge National Laboratory, P O Box X, Oak Ridge, TN 37830, Contract 

W 7405-eng-26 
40 

the graphite mixture was extruded, and after baking 

had adequate mechanical strength for handhng for 

encapsulation The method was demonstrated to be 

feasible 

Measured surface dose rate from a source loaded to 

the maximum with strontium silicate beads in aluminum matrix of 38 7 Ci/hnear inch in a capsule 0 085 m 

thick by 0 395 in wide and with 0 010 m stainless 

steel walls was determined to be 5 X 10* R/hr 

The output from a disc source 0 750 in in dia and 

0 030 m thick containing 3 mCi of Sr-90 sihcate beads 

distributed m an aluminum matrix and covered with 

0 005 in stainless steel was measured in an extrapolation chamber to be 1 5 X lO"* Rads/hr-cm^ as a surface 

dose rate 

Plan for Next Period 

The original objectives have been completed 

Reports Published 

F N Case and T S Mackey, Preparation of Stron 

tmm-90 Sihcate Beta Sources, USAEC Report 

ORNL-4340, February 1969 

Estimated Date of Final Report 

1972 

LOW-ENERGY PHOTON 

RADIATION SOURCES* 

Objective of Work 

The objectives of this project are to develop lowenergy radiation sources that have high radiation 

intensity and useful energy spectra and to define safety 

characteristics of the source capsules The development 

of prototype sources is essential to the development of 

devices to measure compositions or density by secondary x-ray emission, backscatter, and photo attenuation 

Progress and Results 

The principal radiochemical impurities m gadohnium-153 produced by irradiating norma! europium are 

high energy components of europium-152-154 Sources 

of gadohnium-153 used m x-ray fluorescence analysis 

must be essentially free of europium A relatively 

*R S Pressly, T S Mackey, and E H Acree, Oak Ridge 

National Laboratory, P O Box X, Oak Ridge, TN 37830, 

Contract W-7405-eng-26 

low-cost supply of high purity gadohnium-152 was 

developed as by-product to the operation of the HFIR 

(High Flux Isotope Reactor) by recovery of gadohnium-152 produced m the europium control plates 

Sources were prepared m which the concentration of 

radionuchdes of europium in the gadohnium-153 was 

less than 10 ppM. The sources were fabricated as point 

sources using stainless steel encapsulation and the 

radiation output was characterized A method was 

developed m which the gadohnium-153 as nitrate was 

extracted into tri-butyl phosphate and this solution 

dispersed m polyurethane When the polyurethane 

solution was apphed to an aluminum substrate and 

allowed to polymerize, a uniform, large surface, flat 

plate source was achieved 

Cadmium-109 purification methods and source fabrication methods were studied to obtain very high 

radiochemical purity, high output sources for use in 

fluorescence x-ray analysis To maximize the spectra 

purity and output, thm graphite substrates were used to 

stabihze the cadmium-109 activity into a fixed geometry Carrier-free cadmium-109 prepared by proton 

bombardment of a silver target was used m preparing 

sources up to 55 mCi The graphite, containing cadmium-109, was covered with a 4-mil aluminum window 

Particular emphasis was directed toward extracting the 

22 keV photon 

Methods to prepare high integrity americium-241 

sources were studied Photon sources were prepared by 

using amencium metal alloys with aluminum and 

copper Alummum cladding of amencium metal is 

under study as a method for obtaining thm window 

alpha sources Output measurements and spectral characteristics are being correlated with alloy composition 

Literature reviews concerning low-energy and alpha 

sources were carried out to determine the state-of-theart Work was carried out to characterize source output 

parameters through the use of an extrapolation chamber and silicon detector system 

Plan for Next Period 

Work will continue on state-of-the-art reviews to 

assemble existing information concerning low-energy 

sources Study of sources and source collimators to 

improve the quantity and quality of radiation reaching 

a sample being analyzed will be continued 

Reports Published 

F N Case, E H Acree, and N H Cutsh^ll, Production 

Study of Gadohnium-153, USAEC Report ORNLTM-2632, August 1969 
41 

R. S. Pressly, The Development and Use of Low-Energy 

Gamma, Secondary X Ray, and Beta Sources, 

Trans. Amer. Nucl. Soc, 14(2): 497-8 (October 

1971). 

Estimated Date of Final Report 

Continuing project. 

ADVANCED SOURCE DEVELOPMENT* 

Objective of Work 

The objective of this program is to evaluate present 

and future heat- and radiation-source application requirements and to relate them to present and future 

encapsulation technology. The goal of the current work 

is concerned primarily with the development of thinfilm encapsulation and evaluation techniques for 

alpha—photon sources. Emphasis is on the technique of 

rf sputtering as a means to obtain thin films of 

radioisotope and containment materials. 

Progress and Results 

Alpha—photon radiation sources, having an Am-241 — 

containing active layer, were fabricated by rf sputtering 

in several different source preparation runs. Both the 

*J. H Jarrett, Battelle, Pacific Northwest Laboratory, Richland, WA 99352, Contract AT(45-1)-1830. 

active layer and the containment layer were deposited 

by rf sputtering. 

The rf-sputtering system located in a radioisotope 

glove box was modified by adding or replacing a 

number of components. The updated system is easier to 

operate and maintain, and with it two different 

materials may be deposited consecutively. Preliminary 

results indicate that the use of sequential rf sputtering 

available in these glove-box systems gives sources that 

have better radioisotope containment than the sources 

prepared in the original system. 

The rf-sputtering system outside the glove box was 

used for nonradioisotopic sputtering work such as 

source preparation hardware development. Hardware 

for preparing ten radiation sources simultaneously (see 

figure) was developed and used to prepare Am-241 

radiation sources. The hardware allows accurate positioning of a Vj-in.-dia Am-241-containing active layer 

on Vg-m.-dia substrates. The positioning mask is removed for deposition of the active layer. 

An Am(241)02-copper sputtering target (the source 

of sputtered material) was used in preparing the active 

layer for radiation sources. The target was prepared by 

cold-pressing pellets of Am(241)02 and copper powders, and bonding the pellets to a copper backing plate. 

The radioactive layer sputtered from this target contained less than 5% Am-241. A target yielding a 

sputtered film containing a much greater portion (over 

50%) of Am-241 was also prepared similarly. Techniques were developed for minimizing radioisotope 

Sputtering hardware for preparing 10 radiation sources in a single run. 
42 

inventory in the target while still providing a target face 

that contained a high proportion of Am(241)02 

Experiments to demonstrate the production of high 

activity, high integrity alpha photon sources from this 

target were started 

Assistance in evaluating PNL prepared alpha photon 

sources was provided by Oak Ridge National Labora 

tory The test results on a group of alpha—photon 

sources were encouraging since the demonstrated source 

integrity was greater in most tests than the source 

integrity determined on previous PNLpiepared alphaphoton sources However a pioblem m radioisotope 

containment at elevated temperature was indicated 

Contamination was released m this test when the 

sources were heated to over 900°C in one hour m 

flowing air The results of all tests were factored into 

the design and preparation of the next generation 

alpha photon sources The ORNL evaluation involved 

boiling water leach testing temperature—humidity test 

ing and the ORNL source capsule classification testing 

(Class I A) 

The primary advantages of sputtering for preparing 

tiun film radiation sources are 

Most metals, ceramics and cermets may be de 

posited by sputtering 

Sputtered tilms generally have high density good 

integrity, and good uniformity 

A number of similar sources may be prepared in a 

single run, and different geometry sources may be 

conveniently prepared 

Source layer thicknesses and source activity may be 

accurately controlled 

Source preparation by sputtering is well suited to 

the automated production of a number of similar 

sources per run on a continuing basis 

Techniques for minimizing radioisotopic cross 

contamination when preparing sources containing 

different radioisotopes, and techniques for re 

moving sources from the sputtering system without 

adding significant surface contamination to them 

have been demonstrated 

The disadvantages of sputtering are 

Because of the radioisotope inventory required m 

the target, sputtering is not a convenient method 

for preparing a one of a kind source The exceptions 

would be cases where a sputtering target containing 

the desired radioisotope is available from past 

source preparation work or where the radioisotope 

layer is deposited by a technique other than 

sputtering, and sputtering is used to provide the 

encapsulation or containment layer 

Conventional sputtering systems are not fast How 

ever, extended runs and unattended equipment 

operation have been successfully demonstrated 

Metals may be deposited at about one to two 

microns per hour and ceramic materials have 

deposition rates of about an order of magnitude 

slower As rates are increased, substrate coohng 

becomes a problem unless there is good path of 

thermal conduction between the substrates and the 

water cooled substrate plate 

Plan for Next Penod 

Another generation of alpha photon sources will be 

fabricated using rf sputtering They will be given 

preliminary evaluation at PNL and then sent to ORNL 

for extensive evaluation The preparation of high 

specific activity sources will be investigated and the 

preparation of various geometry sources for select 

apphcations will be considered The rf sputtering 

systems will be further automated Attempts will be 

made to correlate residual gas analysis (RGA) m the 

vacuum chamber, before, during and after a deposition 

run, with the properties of sputtered films If success 

ful, RGA could provide a useful quahty control 

technique Projected system economics will be briefly 

evaluated to give an indication of source costs on a 

production scale basis 

Reports Published 

None 

Estimated Date of Fmal Report 

Continuing project 

NONDESTRUCTIVE TESTING 

TECHNOLOGY IN SUPPORT OF 

DID CAPSULE DEVELOPMENT 

ACTIVITIES AND RADIATION 

SOURCE PROGRAMS* 

Objective of Work 

The objective of this program is to develop nonde 

structive test methods, devices and instruments that 

will assist the designer or fabricator of isotope encapsu 

*D R Newman Battelle Pacific Northwest Laboratory 

Richland WA 99352 Contract AT(45 1) 1830 
43 

BACK SURFACE 

FRONT SURFACE SIGNAL 

FLAW SURFACE 

BACK ELECTRODES 

PIEZOELECTRIC 

FRONT ELECTRODE 

ULTRA SONICWAWS 

INVERTED SIGNAL 

RESULTANT SIGNAL 

FRONT AND BACK SIGNALS CANCEL 

ONLY FLAW SIGNAL REMAINS 

- 4 -

SUMMING 

CIRCUIT 

BACK SURFACE REFLECTION 

FRONT SURFACE REFECTION 

TYPICAL 

TRANSDUCER 

CONNECTORS 

CASE 

BACKING 

MATCRIAL 

ACTIVE ELEMENT 

Differential transducer technique. 

lations by (I) evaluating the as-fabricated encapuslation 

for comparison with designed parameters, (2) helping to 

select and evaluate encapsulation materials and materials compatibihty, and (3) developing faster, more 

economical, and more easily interpreted test methods. 

Cooperation of the nondestructive test (NOT) development and fabrication efforts assures the isotope user 

and the^public of optimum encapsulation integrity. 

Progress and Results 

Construction and evaluation of a differential transducer system was completed (see figure). This technique was developed to permit the inspection of thin 

materials, or to locate anomahes lying close to the 

surface of thicker materials. It is based upon placing 

two electrodes on the back of a piezoelectric ultrasonic 

transducer, inverting the signal from one of the electrodes, and summing the inverted and noninverted 

signals. Common signals (such as those from the front 

and back surfaces of the object under test) will cancel, 

leaving only the signals due to any small anomahes 

present under only one of the electrodes. Evaluation 

estabhshed that the differential transducer worked 

quite well. Front and back surface reflections were 

reduced by a factor of 20 or more, allowing flaws close 

to the surface to be resolved. 

Plan for Next Period 

Due to budgetary limitations, further work on this 

program is presently curtailed. 

Reports Published 

D. R. Newman and R. W. Steffens, Multielectrode 

Ultrasonic Transducer Test Techniques for Radioisotope Encapsulation Inspection, USAEC Report 

BNWL-1491, February 1971; also printed in the 

Proceedings of the 8th Symposium on Nondestructive Evaluation in the Aerospace, Weapons and 

Nuclear Industries, San Antonio, TX, April 1971 

(Available from Western Periodicals, 13000 

Raymon St., N. Hollywood, CA 91605). 

D. R. Newman, Radioisotope Bond Test Applications 

of a Pulsed Laser Schlieren System, in Proceedings 

of the 8th Symposium on Nondestructive Evaluation in the Aerospace, Weapons, and Nuclear 

Industries, San Antonio, TX, April 1971 (Available 

from Western Periodicals, 13000 Raymon St., N. 

Hollywood, CA 91605). 

D. R. Newman and J. C. Crowe, Recent Developments 

in Nondestructive Evaluation Applicable to Encapsulated Isotopes, in Proceedings of the 3rd 

International Symposium on Paclcaging and Transportation of Radioactive Materials, Richland, WA, 

August 16-20, 1971, pp. 138-65, USAEC Report 

CONF-710801, 1971. 

Estimated Date of Final Report 

Topical reports will be issued. 
44 

SHIPPING CASK DESIGN AND EVALUATION* 

Objective of Work 

The objective of this project is to determine whether 

packages for shipping large quantities of radioactive 

materials meet the performance standards developed by 

*R D. Seagren, Oak Ridge National Laboratory, P O. Box X, 

Oak Ridge, TN 37830, W-7405-eng-26. 

the Atomic Energy Commission, the Department of 

Transportation, and the International Atomic Energy 

Agency. These standards cover normal conditions during transport, as well as hypothetical accidents. 

Progress and Results 

Packages having several different designs were evaluated and approved as meeting the required performance 

34-in DIAM 

44-in DIAM 

Neutron shielded fire and impact shield assembly. 
45 

standards The packages were required to withstand a 

30 ft drop, a 40-in puncture test (dropped onto a 

6-in -dia pm from a distance of 40 m ), and a 30-min 

open fire The designs included the Puerto Rico Ram 

Forest Irradiator, a Canadian fissile package, and a 

British package utihzmg a wooden overpack 

The overpack for Specification 55 packages developed 

last year, utihzing hthium hydroxide monohydrate as a 

thermal-conducting medium, was successfully subjected 

to the consecufive hypothetical accident tests (see 

figure) 

Plan for Next Penod 

New shipping-package concepts and designs wdl continue to be evaluated under this program 

Reports Published 

R D Seagren, Safety Analysis of ORNL BulJc Radioisotope Shipping Cask, USAEC Report ORNL 

TM-3506, August 1971 

R D Seagren, Safety Analysis of the ORNL Type B 

Gas Cylinder Protective Packaging, USAEC Report 

ORNL-TM 3544, October 197] 

R D Seagren and L B Shappett, Indexed Bibliography 

on Transportation and Handling of Radioactive 

Materials 2, USAEC Report ORNL-NSIC 84, Janu 

ary 1971 

D Seagren, Shipping Cask Evaluations, Isotop 

Radiat Technol ,8(3) 350-59(1970) 

R 

Estimated Date of Final Report 

Continuing project 

RADIOISOTOPE SAFETY TESTING* 

Objective of Work 

The objective of this program is to determine the 

reliabihty of radioactive sources m containing the 

radioactive material under the conditions of normal use 

as well as m the event of an accident The investigations 

produce data that will enable source manufacturers and 

regulatory agencies to evaluate existing and future 

source designs from the standpoint of safety to the 

users and general pubhc Test procedures are also 

developed that can be used by manufacturers for 

quality assurance purposes 

Progress and Results 

A study of tritium losses fiom commercial tritium 

foils used in gas chromatograph detectors was com 

pleted These foils had nominal tritium concentrations 

of 250, 500, and 1000 mCi/in ^ as titanium tritide on a 

stainless steel backing The corresponding measured 

total activities m each foil weie 62 5, 125, and 250 

mCi Tritium losses were determined as a function of 

foil temperature, foil-heating rate, carrier-gas composi 

tion, carrier-gas flow rate, time that foil is exposed to 

temperature, and foil-cleaning procedure The tritium 

losses as a function of temperature increased slowly 

with increasing temperatuie to a break point, above 

which the losses increased at a much higher rate The 

tritium losses when new foils were heated at 150°C for 

1 hr m an argon flow were 4 9, 51 1, and 14 9;uCi/in ^ 

respectively, for the 250, 500, and lOOOmCi/m^ 

foils The temperatures at which the break points occur 

are approximately 238, 198, and 200°C, respectively, 

for the 250 , 500-, and 1000-mCi/in ^ foils (see figure) 

Tritium losses as a function of operating time at 

225°C (maximum temperature allowed by USAEC 

regulations) were obtained m an argon flow for each 

type of foil The losses were relatively high during the 

first few hours of operation but quickly decreased with 

time and remained nearly constant for the remainder of 

the test Since new foils were used for each of the tests 

1600 

1400 

1200 

1000 

O 250-mCr/in2 FOIL 

_A 500-mCi/m2 FOIL 

® 1000-mCi/in2 FOIL 

O » 0 

600 

4 0 0 

2 0 0 

*R G Niemeycr, Oak Ridge National Laboratory, P O Box 

X, Oak Ridge, TN 37830, Contract W 7405-eng 26 

175 200 225 250 275 300 

FOIL TEMPERATURE (»C) 

Tritium loss as a function of temperatuie in argon. 
46 

in the study, the test results represent the maximum 

losses that would be expected under the test conditions 

A proposed procedure for accurately measuring the 

radiation dose rates from small commercial light sources 

containing Pm-147 and Kr-85 was developed as an aid 

to source manufacturers, standards groups, and individuals involved m their use These dose-rate measurements are complicated by many vaiiables including 

geometry, type and quality of the radiations involved, 

and energy dependence of the common survey instruments used m making the measurements Over 2000 

dose-rate measurements were made using eight different 

survey meters and thermoluminescent dosimeters to 

identity the problems involved m obtaining accurate 

dose-rate measurements of 16 commercial sources 

Additional data were obtained on the 10-year aging 

and drying effects study on the release of tritium from 

luminous phosphor pamt and on the aging effect of 

alpha calibration sources The paint samples have shown 

a steady physical deterioration over the years and they 

are extensively cracked and pieces have flaked off the 

surface Over the past six years, the water leach tests of 

the samples have shown an increase of about a factor of 

three m the amount of leachable tiitium, however, the 

total quantity is still below that permitted by present 

regulations The plated uranium and plutonium alpha 

cahbration sources have not shown any significant 

change since the start of the test 

Plan for Next Period 

Tests will be performed on watches having luminous 

tritium-painted dials and hands to deteimme if any 

tritium IS released during normal use 

The 10-year study of tritium paints will be terminated 

and fresh supplies of currently manufactured tritiated 

paints will be obtained for a new study m which more 

emphasis will be placed on determining losses of tritium 

m normal use and to observe any improvement m 

stability of the newer paints 

Studies will be initiated to determine the optimum 

leak test sensitivity for encapsulated sources by obtaining data on the amounts of activity released under 

various conditions from source capsules having known 

leak si/es 

Specific tests will be carried out when requested by 

the AFC 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

RADIOISOTOPE CHARACTERIZATION, 

QUALITY CONTROL, AND STANDARDS* 

Objective of Work 

The objectives of this progiam aie to select or 

determine radionuclide characteristics such as half-lives 

and modes and energies of decay, to review and 

recommend quahty-control procedures and analyses, 

and to study radioisotope measurement methods and 

standards Critically evaluated constants are essential m 

all aspects of analysis, handling, and use of radio 

isotopes, and m supplying information about them 

Methods are reviewed and selected, and special analyses 

are performed when required Both local and national 

needs are involved m the study of standard materials 

and measurement methods 

Progress and Results 

Half-lives have been determined for 60 nuclides since 

out last publication ot such data, these included the 

controversial nuchdes Mo 99, Eu-155, W-181, and 

Hg-203 The reactor-neutron cross section of Ni-59 was 

estimated as 85 barns, and the cross section and 

resonance integral foi production of Ag-llOm were 

determined Information, some of types not previously 

included, was collected for revisions to the Isotope 

User's Guide The majority of recipients of the Guide 

who responded to a questionnaire found the sections on 

characteristics and standards "very useful " 

Some needs m quality-control analysis were satisfied 

by recommendations of neutron activation to determine chlorine m elemental C-14, and gamma spectrometry for traces of Kr-85 m inactive fission-product 

xenon With respect to raw material for Sr-90 sources, 

study of methods and results yielded the conclusion 

that present techniques are satisfactory, provided that 

characteristic elemental and isotopic compositions are 

taken into account 

The National Academy of Sciences published the 

report of the ad hoc panel on standard radioactive 

materials, based m large part on our survey of national 

needs Over 700 copies of the panel report have been 

distributed to selected individuals and institutions Its 

recommendations, supported by other groups, have 

influenced pohcies at the National Bureau of Standards 

(NBS) and actions by organizations concerned with 

radioactivity With the conclusion of the survey, and in 

line with panel recommendations, emphasis is being 

placed upon making local calibrations traceable to NBS 

*S A Reynolds, Oak Ridge NaUonai Laboratory, P O Box 

X, Oak Ridge, TN 37830, Contract W-7405-eng-26 
47 

whenever practicable A report was prepared on ORNL 

calibrations, especially as related to NBS, containing a 

brief history of the work during the past quarter 

century 

Plan for Next Period 

Studies of radioisotope characteristics, quahty-control 

procedures and standards, and nonroutine analytical 

problems will continue as required Emphasis will be on 

nuchdes of biomedical and environmental usefulness, 

and HFIR products It is expected that the revised 

Isotope User's Guide will be issued Collaborative 

efforts will include beginning preparation of a general 

manual on cahbrations, acceptable to organizations 

requiring radioactivity measurements, and gathering and 

disseminating information on standards 

Reports Published 

S A Reynolds, A Survey of Needs for Radioactivity 

Standards, USAEC Report ORNL-TM-3239, September 1970 

S A Reynolds, Radioactive Materials Problems Under 

Scrutiny, 5«e«ce, 171 955(1971) 

S A Reynolds, Cooperafive Isotopes Program, Radioisotope Characteristics and Measurements, m Analytical Chemistry Division Annual Progress Report 

for Period Ending Sept 30, 1970, USAEC Report 

ORNL-4636, pp 22-24, January 1971 

National Academy of Sciences, National Uses and 

Needs for Standard Radioactive Materials, Washington, DC, 1970 

Estimated Date of Final Report 

Continuing program 

THERMAL APPLICATIONS 

v'."T.|.;ii..i :;r:-i;; 

'.)i;iVL .I'iiiii i 

Si'lCi.-. I fti •,. lf;ii-\,-| . AiU/v 

s p ' ciini i\. iN.)[-cr"r. ' HAv 

i,s Vi! ••.ivf V 'Ji-\;',-

•-•', .-•r.'" i ;.;,• • -r , ,c: .•H,.-. 

: i;'i,..~L '•; ...LRotating arm impact test facility. 

Thermal Applications 

The objective of the Thermal Apphcafions Program is 

to develop uses of the thermal energy generated by 

radioisotope decay. (This does not include the development of radioisotope thermoelectric generators for use 

in space, which is supported by the Division of Space 

Nuclear Systems.) In a hke manner, the development of 

thermoelectric generators for other than space use, e.g , 

the nuclear pacemaker and terrestrial thermoelectric 

generator units, is supported by the Division of Reactor 

Development and Technology. 

The heat sources range from simple ones, requiring 

httle or no temperature control, to more complex units 

distributing the thermal energy and controlhng temperature within narrow limits. All require a high degree of 

reliabihty and inherent safety Current emphasis m this 

program is on (1) research related to the development 

of fuels for an implantable radioisotopic power source 

for heart assist devices, (2) evaluation of the practicabihty of developing a radioisotope thermal converter 

for an artificial heart having a minimum weight and 

volume and a minimum life of 10 years, (3) development and ground test of a waste-management/waterreclamation system for aerospace apphcations; (4) 

development and test of a large Co-60 heat source using 

an electric converter for test purposes; and (5) studies 

and development of small radioisotopic heat sources for 

thermal control. 

51 

53 

EVALUATION OF PRACTICABILITY 

OF A RADIOISOTOPE THERMAL CONVERTER 

FOR AN ARTIFICIAL HEART DEVICE* 

Objective of Work 

The objective of this program is to determine the 

practicabihty of developing a compact radioisotope 

thermal converter having a minimum weight and vol 

ume and a minimum life of 10 years In this context, 

the converter is the mechanism by which thermal 

energy from a radioisotope heat source is converted to 

another energy form suitable for pumping blood The 

program is divided into two phases, with the objective 

ot Phase I bemg to evolve and evaluate innovative 

concepts for a variable powered thermal converter 

incorporating a vented radioisotope heat source Pre 

estabhshed selection criteria will be used to recommend 

the most promising concept tor Phase II verification of 

theoretical and experimental practicabihty 

Progress and Results 

The Phase I technical effort was completed mid 

October 1971 with recommendations that a Stirhng 

cycle power source providing pulsed input to a blood 

pump diaphragm by means of a mechanical drive tram 

was the most promising approach This selection was 

made with the aid of a decision modeling analysis of 

eight final candidate systems that had been screened 

from the approximately 25 concept variations mvesti 

gated Concepts included static conversion devices as 

well as dynamic systems representing several different 

thermodynamic approaches Included in the eight contending concepts were systems using triple cascaded 

thermoelectrics, Stirhng cycle gas dynamic systems, and 

vapor-cycle dynamic systems including both heat rate 

devices and high speed Rankme cycle devices The three 

basic methods that were used for transforming and 

transferring the power source output to pulsed opera 

tion of the blood pump diaphragm were (1) mechani 

cal drive, (2) direct hydrauhc drive, and (3) accumu 

lator hydrauhc drive 

The recommended Stirling mechanical thermal con 

verier concept shown m the figure has two major 

assembhes a Stirhng mechanical power source and a 

blood pump, interconnected by a flexible mechanical 

*R E Lochbaum, Westmghouse Electric Corp , Astronuclear 

Laboratory, P O Box 10864, Pittsburgh, PA 15236, Contract 

AT(11 1) 3043 [tormerly AT(30 l)-4277] 

shaft to transmit diive power and by coolant lines to 

cairy waste heat rejected from the pov/er souice to a 

blood heat exchanger located in the blood pump 

assembly System characteristics are 

Power to blood pump 4 45 W(t) 

initial isotope inventory 28 8 \\(t) 

Temperature peak 1520 F 

Temperature sink 110 1 

Systtin vvti{,ht 1546^ 

System volume 706 cm 

The power source is a Stirling cycle heat engine with 

rhombic drive connected through step up gearing to a 

magnetic coupling that provides a hermetic interface 

between the powei source and the flexible drive shaft 

The hot portions of the power source — the isotope 

capsule the engine hot finger and the combined 

displacer and regenerator are enclosed in vacuum foil 

insulation The heat sink is located above the power 

piston and below the displacer where waste heat is 

lemoved by a circulating isotonic cooling water mix 

ture Hehum vented from the isotope capsule which is 

enclosed m the engine volume diffuses into the engine 

working space, into the crankcase, and out through a 

selective vent into the body cavity 

The blood pump and drive tram are powered by a 

flexible shaft which enters the pump assembly from the 

left It drives the flywheel through right angle bevel 

gears that transmit the power through a double reduc 

tion planetary gear system to two sets of right angle 

bevel gears that drive a set of Scotch yokes The Scotch 

yokes, in turn, drive the actuating rod which pushes the 

blood pump diaphragm assembly to expel the blood on 

systole The pushing motion of the two Scotch yokes is 

coordinated by connection to the actuation rod 

through a yoke pivot to insure balanced operation 

Plan for Next Penod 

During Phase II, parametric and trade studies will be 

conducted to optimize the prehminary design of an 

implantable version of the recommended concept A 

realistically sized bench model will be designed, built, 

and tested in support of practicabihty assessment 

Reports Published 

None 

Estimated Date of Final Report 

January 1972 
Stirling mechanical thermal converter schematic. 
55 

PREPARATION AND EVALUATION OF 

PLUTONIUM-238 RADIOISOTOPIC 

HEAT SOURCES* 

Objective of Work 

The objectives of this work are (1) prepare and 

evaluate medical grade Pu-238 compositions for hfe 

support apphcations, (2) fabricate and characterize heat 

source capsules (up to 50 W) for dosimetry, systems 

studies, and implantation studies, (3) provide heat 

source capsule on a interim basis which will also 

estabhsh process rehabihty and product quahty control 

for guidance m developing a commercial capabihty,(4) 

estabhsh the compatibihty of biomedical fuel forms 

with container materials, and (5) measure the rate of 

helium and radon release from biomedical 

Pu(238)02(16) fuel forms 

Progress and Results 

The preparation of potential Pu-238 fuel forms during 

1968 and 1969 led to the development of four fuel 

forms having mmimal radiation properties These forms 

*L J Mulhns and G R Waterbury, Los Alamos Scientific 

Laboratory, P O Box 1663, Los Alamos, NM 87544, Contract 

W-7405-eng-36 

are the metal, Pu-238~-3 at % Ga, Pu(238)N(15), and 

Pu(238)02(16) All four fuels were prepared from 

electrorefined metal of high chemical purity Theoretical and experimental evaluations of these forms led to 

the conclusion that Pu(238)02(16) was the preferred 

form for high temperature application m the artificial 

heart program During 1970 and 1971, emphasis was 

placed on the development of procedures for the 

ceramic fabrication of 20- and 50-W cyhnders of 

Pu(238)02(16) Three 30-W and six 50-W cyhnders 

were fabricated for delivery to the USAEC Properties 

of two 30-W sources and three typical 50-W sources (80 

at % Pu-238) are given in the table The 30-W sources 

were prepared before the 50-W sources A comparison 

of the neutron emission rates shows a small but steady 

decrease in the neutron emission rate as the procedures 

were improved The neutron emission rates of sources 

30-3, 30-6, 50-3, and 50-6 were 3608, 3519, 3488, and 

3466 n/(secXg)Pu-238, respectively 

A study of the exchange of 0-18 and 0-17 with 

sintered pellets of Pu(238)02(16) m atmospheres of 

argon-p!us-02, dry air, and air saturated with water 

vapor has shown that 50-W cylinders may be handled m 

air-fiiled glove boxes without any measureable oxygen 

exchange This behavior is m marked contrast to that of 

Pu(238)02(16) powders, which must be handled in 

inert atmosphere glove boxes to avoid oxygen-isotope 

Properties of Five Pu(238)02(16) Cylinders 

Wt of Fuel Pellet, g 

Wt ofPu, g 

Oxygen/Pu Atom Ratio 

Pu isotopic Composition 

Wt % Pu-238'' 

ppm Pu-236'' 

Dimensions 

Diam , m 

Height, m 

Density, gPu02/cc 

Power, watts 

Power Density, watts/cc 

Neutron Emission Rate 

n/(sec)(g) Pu 

n/(sec)(g) Pu-238 

Dose Rates at 10 cm 

Neutron, mrem/(hr) (g) Pu-238 

Gamma, mr/(hr) (g) Pu-238 

30-W Pu(238)0: 

LAS 30-3 

74 76 

65 9 

2 01 

79 82 

0 70 

0 846 

0 803 

10 11 

29 8 

4 03 

2880 

3608 

0 36 

0 14 

>(16) cylinders 

PNL 30-6 

74 69 

65 4 

2 01 

86 96 

0 25 

0 858 

0 808 

9 77 

32 2 

4 20 

3060 

3519 

0 35 

0 14 

NHl 50-2 

125 08 

110 

1 99 

79 72 

0 76 

1 006 

0 996 

9 65 

49 7 

3 83 

0 35 

0 17 

50 W Pu(238)02(16) cylinders 

(80 at % Pu-238) 

NHl 50-3 

125 27 

110 

199 

79 98 

0 75 

0 997 

1003 

9 75 

49 8 

3 88 

2790 

3488 

0 35 

0 14 

NHl 50-4 

124 68 

110 

199 

79 62 

0 58 

1 004 

1 013 

9 49 

49 6 

3 78 

2760 

3466 

0 35 

0 16 

''gPu 238/100 gPu 

*gPu-236/10*gPu 
56 

exchange Two processes are still under study for the 

preparation of Pu(238)02(16) powder In one, the 

oxide IS prepared by converting electrorefined metal to 

Pu(238)02(16) In the other, Pu(238)02(nat) is con 

verted to Pu(238)02(16) by isotopic exchange At 

present, the electrorefined metal route is preferred and 

has been used for the preparation of all 30- and 50-W 

sources 

Work was started during 1971 on measurements of 

the rate of release of helium and radon from 

Pu(238)02( 16) cyhnders 

The characterization of Pu 238 fuel materials con 

tinues A nondestructive analytical method was de 

veloped for determining 0 17 and 0-18 in 

Pu(238)02(16) by measuring the intensities of the 

(a,n) reaction gamma rays of O !7 and 0-18 The 

reliability of the mass spectrometric measurement of 

0-18 in Pu(238)02(16) was shown to be satisfactory by 

the new nondestructive technique Continuing study of 

the basic radiation properties of Pu 238 has revealed 

two previously unreported gamma rays having energies 

of 1428 and 1435 keV, the absolute intensities of these 

rays were measured 

The experimental facility for the synthesis and 

fabrication of heat sources is operational One line of 

shielded glove boxes is used for the conversion of 

Savannah River Pu(238)02(nat) to bomb-reduced 

metal, two large inert atmosphere glove boxes are used 

for the preparation of metal and ceramic fuel forms, 

and another hnc of glove boxes is used for the 

encapsulation of sources 

Plan for Next Period 

The radiation properties of isotopically pure Pu-238 

will be measured Fifty-watt Pu(238)02(16) heat 

source capsules for implantations in miniature swine 

will be supplied The measurement of hehum and radon 

release rates from Pu(238)02(16) fuels will be continued, as will compatibility studies on vented and 

unvented capsules 

Reports Published 

L J Mulhns and J A Leary, Purification, Encapsulation, and Characterization of Pu-238 for Implantation Purposes, Trans Amer Nucl Soc , 13 496-97 

(1970) 

L J Mulhns and J A Leary, Plutonium-238 Radioisotopic Heat Sources for the Artificial Heart 

Application, Amer Inst of Chem Engineers, 

Symposium on Applications of Radioisotopes, 

December 1970 

Estimated Date of Final Report 

Continuing project 

EVALUATION OF PRACTICABILITY 

OF A RADIOISOTOPE THERMAL CONVERTER 

FOR AN ARTIFICIAL HEART DEVICE* 

Objective of Work 

The objective of the program is to determine the 

practicability of developing a radioisotope thermal 

converter for an artificial heart device The thermal 

converter, including the radioisotope heat source, and 

all associated power conditioning and control systems 

are to be fully implantable and capable of functioning 

for 10 years with high reliability The device must 

supply the necessary mechanical, hydraulic, or pneu 

matic power for a blood pump which provides 100% of 

the left ventricular pumping function 

Progress and Results 

The program is divided into two phases The first 

phase is a 7-month evaluation of candidate concepts 

and the selection of a prefened design for further 

detailed evaluation The second phase, which is not 

currently a part of the contractual effort, will be a 

17-month effort that will include detailed analyses of 

the preferred concept and culminate in the design, 

fabrication, and test of a lealistically si/ed thermal 

converter using a radioisotope fueled heat source 

During Phase 1, a list of evaluation criteria was 

compiled for use in selecting a preferred thermal 

converter system for Phase il development The principal design criteria included a daily average power level 

of 2 8 W(e) delivered to the blood pump and the 

following maxima 60 W(t) heat source, 1 5-liter vol 

ume, specific gravity of 2 0, and peak power level of 

4 44 W(e) 

The concepts evaluated included various mechaniza 

tions of reciprocating, rotary, and thermoelectric 

cycles, with both gas and vapor operating fluids, as well 

as various combinations of these devices Eight different 

thermal converter systems were found to be capable of 

meeting all the design criteria 

These eight systems were compared, using the previously defined evaluation criteria and scoring meth 

odology The preferred concept shown in the figure is 

*! R Jones, M G Ridgway, and D R Snoke, TRW Systems 

Group, One Space Park, Redondo Beach, C A 90278, Contract 

AT(04 3) 857 
57 

Hybrid engine (le! 

an ah electric output hybrid engine that powers a motor 

that m turn, mechanically actuates a Kwan—Gett type 

blood pump The total weight and volume of the 

engine, motor, and actuator are 1 83 kg and I 33 liters 

The hybrid engine includes cascaded Si Ge(Te) ther 

moelectric modules mounted on each end of a 49 W(t) 

vented, cylindrical heat source with hot and cold 

junction temperatures of 1740°F and 460°F 

The cold side of the thermoelectrics and surrounding 

msulation system serves as the source of heat for the 

boiler of a rotary vapor turbogenerator which uses 

CP 34 as the working fluid operates between 430°F 

and 116°F and puts out 7 24 W(e) at 15 volts The 

thermoelectric system, after dc to dc conversion pro 

vides 2 61 W(e) at 15 volts The motor uses the total of 

9 85 W(e) to power a 15 volt 9000 rpm brushless dc 

motor that is geared down to drive a rotary cam at 120 

rpm The rotary motion is converted to reciprocating 

motion by a cam-follower operating in a continuous 

elhptical groove on the inner diameter of the rotary 

cam The reciprocator is mechanically coupled to an 

automatic actuator that provides passive autoregulation 

for a modified Kwan-Gett blood pump This feature 

permits the actuator to operate at a constant 120 cycles 

per minute and accommodate blood flow rates ranging 

from 6 to 12 hters/mm Because the overall efficiency 

and motor (right) 

of the motor and automatic actuator is 45%, the power 

delivered to the blood pump is 4 44 W(e) which 

corresponds to the peak activity requirement 

The hybrid thermal converter employs only fibrous 

thermal msulahon with an inert gas fill Some volume 

and weight can be saved by use of vacuum foil 

insulation but at the expense of reduced system 

rehabihty Heat is rejected directly into the abdominal 

body tissues and fluids although about half the heat 

can be rejected through the blood pump if required 

When high energy, high density sohd electrolyte bat 

teries are developed, the hybrid concept offers consider 

able growth capability since the device could then be 

sized to provide the average power level (2 81 W) rather 

than the maximum power level (4 44 W) Options 

include a pure rotary vapor system (most compact), a 

pure thermoelectric system (most rehable), or a hy 

brid/battery system (smallest heat source) 

Plan for Next Penod 

The Phase I Final Report will be completed and 

submitted to the AEC 

Reports Published 

None 
58 

Estimated Date of Final Report 

The Phase I Final Report will be issued in November 

1971 

RECIPIENT RADIATION EXPOSURE 

AND RADIOLOGICAL ENGINEERING STUDIES 

RELATING TO CIRCULATORY 

SUPPORT SYSTEMS* 

Objective of Work 

The major objective of this study is to determine the 

dose from radioisotopic heat sources suitable for 

circulatory support systems This is accomplished by 

measuring and calculating, with suitable codes, the dose 

rates withm and surrounding various tissue-equivalent 

phantoms Another portion of the program concerns 

the development of radioisotopic blood heaters for use 

m an animal study aimed at assessing the combined 

effects ot heat and radiation in miniature swine 

implanted with 50-W plutonium heat sources 

Progress and Results 

Completed studies on shielding, dose prediction, and 

dose measurement with a 30-W Pu-238 medical-grade 

metal source demonstrated that the computer code. 

*h T Cross, J C Sheppard, and B D Bingham, Battelle, 

Pacific Northwest Laboratory, Richland, WA 99352, Contract 

AT(45-1) 1830 

QAD-P5A, when suitably modified, can be used to 

calculate the dose rates to various organs for a wide 

variety of source configurations 

For many organs, the center point dose rate is a 

satisfactory estimate of the average organ dose rate The 

calculated dose rates to various organs from a 30-W 

Pu-238 metal source placed on the inside surface of the 

left ilium are shown in the table The coordinate system 

IS centered in the bottom plane of an elliptical cylinder 

that represents the body, with a Z-axis positive in the 

vertical direction, the X-axis positive to the left side of 

the body, and the Y-axis positive to the back of the 

body The relevance of these dose rates is highly 

dependent on the source and organ coordinates simulating an actual implant Any other source location would 

significantly change the dose rates to those organs 

proximal to the source 

Dose rates from Pu-238 and the daughters of Pu-236 

contained in the Hittman—Rankine dosimetry subsystem, a prototypic power source, and various prototypic circulatory support systems have also been computed Whereas calculation of the neutron contribution 

to the dose appears straight-forward and verifiable by 

measurements, calculation of the photon dose rates 

remains subject to the uncertainties of assigning buildup 

factors for multilayer systems The measurements on 

the more complex power source systems provide 

guidance on the choice of buildup factors 

Measurements of the neutron dose rates from a 32-W 

Pu(238)02(16) source contained m the Rankine device 

Total (n -I- 7) Dose Rates to "Mathematical" Organs" 

Organ 

Spleen 

Left kidney 

Stomach 

Small intestine 

Left ovary 

Left testis 

Uterus 

Bladder 

Left adrenal 

Heart'' 

Center 

coordinates 

(X,Y,&Z) 

11, 3, 37 

6,3,32 5 

8, 4, 35 

6,0, 15 

12,- 2 2, 2 3 

0, 2, 14 

0, - 4 5,8 

4 5,6 5,38 

1,-^3,51 

Center to center 

distance cm 

195 

15 8 

175 

10 

(equivalent) 

3 61 

21 5 

9 17 

136 

21 3 

34 3 

Average 

dose rate, 

mrad/hr* 

1 4 

27 

2 0 

7 0 

44 

0 99 

8 3 

3 5 

1 1 

0 24 

Average 

dose rate, 

mrem/hr"-

2 1 

4 4 

3 1 

13 

100 

1 4 

16 

5 8 

1 6 

0 27 

''From a 30-W Pu 238 metal source shielded with 30 mil Ta and 63-mil Al 

centered at 8, 0, 18, and placed with its axis parallel to the body axis 

^Estimated accuracy +25% (dose rates exclude Pu 236 contribution) 

'^Neutron Quahty Factor = 10 

In an artificial heart implant, these values would represent the dose rates to 

the blood pump occupying the same location 
59 

and placed in a large homogeneous phantom and 

Remab phantom filled with tissue equivalent fluid were 

completed Californium-252 was used as a stand-m for 

the Pu-238 so that long measurement times would not 

be necessary Small tissue-equivalent proportional 

counters were used for these measurements In addition, measurement was completed of the photon dose 

rates from the oxide source placed m the Remab 

phantom The combined (n + 7) dose rates on the 

phantom surface shown in Figs 1 to 4 can be compared 

with the dose rates reported in the 1970 Project 

Summary for the metal source, but, because the oxide 

source was contained in the Rankine device, it was 

physicaUy too large to place m the same exact location 

The source is still placed on the left ilium in hne with 

the 5th lumbar vertebra, but its center is closer to the 

front surface of the body, and the effect of shielding by 

the device materials and the source relocation is 

reflected in the measurements In addition, the photon 

dose rates from the daughters of Pu-236 in the metal 

source were repeatedly measured The measurements 

confirmed predictions of the growth of the dose rates 

from the daughters of Pu-236 

Engineering studies to develop radioisotopic blood 

heaters in support of a project for the Division of 

Biology and Medicine (Biological Effect of Intracorporeal Radioisotope Heat Source) were initiated this 

year Heater geometry, materials, and temperature 

changes in the bulk stream and boundary layer of swine 

blood were investigated Heat exchangers incorporating 

telemetry units for 50-W Pu(238)02(16) sources and 

various biological shams were developed for interposing 

the thoracic aorta. The temperature analysis indicated 

that, upon the death of the animal and loss of blood as 

coolant, the plutonium heat source centerline temperature would reach about 972°F if the ambient temperature was 75°F 

Also initiated was the design of heat conduit systems 

for abdominal heat sources, with exchangers similar to 

the devices designed for thoracic implant but with an 

SIGHT SHWIKR 

om 

GONADS 

1 2 

A 

MIDPOINT 

OF THIGHS 

0.24 

n 

LEFTSIK 

2.7 

32W ^Pu4 ' RANKI»€ PROTOTYPIC 

POUm SOURCE ON LEFT ILIUM 

RIGHT SHOaSER 

MIDPOINT 

OF KNEES 

O W 

32W ^uol*RANKINE PROrOTYPIC 

pam.n soiRCE m UFT ILIU M 

BOTTOM Of FEET 

0.016 

Fig 1. 

Total (n + 7) dose-rates m mrads/hr on surface of remab 

phantom. (Excluding Pu-236 contribution) 

BOTTOM OF reEI 

0.(06 

Fig. 2 

Total (n -^ 7) dose-rates m mrems/te on surface of remab 

phantom. (Excluding Pu-236 contribution QF =10) 
60 

interconnecting heat conductor to allow dumping of 

waste heat into the larger blood vessels in the thoracic 

region 

mem SURFACE 1.2 

1 FT FROM SURFACE ai l 

J FT FROM SURFACE affl? 

BACK SURFACE %i 

FT FROM SURFACE a % 

3 FT FR(HI SURFACE aiS2 

UFT SURFACE J 8 

I n FROM SURFACE a % 

3 FT FROM SURFACE ae s 

32W ^uOj ' RANKINE PROTOTVPIC 

POtilER SOURCE ON UEFT IIIUM 

FRONT SURFACE S 

1 n FROM SURFACE at< 

3 FT FROM SURFACE aiSf 

Fig. 3. 

Total (n + 7) dose-rates m mrads/hr m bisecting radial plane 

of source. (Excluding Pu-236 contribution) 

Plan for Next Period 

Measurements of the dose rates from the oxide source 

contained in the Rankine device will be completed and 

compared with the QAD-code predictions A User's 

Manual for dose rate calculations from Pu-238 heat 

source' will be written The dose rates from future 

prototypic power sources will be determined, and 

guidance will be provided on the dose rates received by 

animals with implanted heat sources The design and 

fabrication of the animal blood heaters and shams will 

be completed 

Reports Published 

None 

Estimated Date of Final Report 

A topical report is scheduled for July 1, 1972 

POPULATION RADIATION EXPOSURE 

FROM HEART DEVICE* 

Objective of Work 

The objective of this project is to identify the 

radiation dose to the population that would result from 

introduction of artificial heart devices fueled with 

Pu-238 

RIGHT SURFAa 2 1 

1 FT FROM SURFACE 0 33 

3 FT FROM SURFACE O M 

FRONT SURFACE Tl 

1 FT FROM SURFAa 2 1 

3 FT FROM SURFACE 0 30 

BACK SURFACE S.< 

1 R FROM SURFAa 0 75 

3 FT FROB SURFACE 0 13 

lOT SURFACE 10 

1 FT FROM SURFACE O S 

3FTFR(»ISURFAa 0 15 

32W ^u4 ' RANKINE PROIOIYPIC 

POMER SOURCE ON LEFT ILIUM 

Progress and Results 

The procedure in this study develops an estimate of 

the potential radiation dose from artificial heart devices 

through construction of time—distance relationships 

between persons typifying potential heart recipients 

and other members of the population A profile of 

potential artificial heart recipients is being constructed 

based on previous National Heart Institute studies and 

U S Public Health Service survey results, and an 

epidemiological study is being conducted to determine 

appropriate life-expectancy factors for recipients of 

artificial hearts 

A computer program is being written to combine the 

data on heart recipient profile, life expectancy, and 

device failure probabilities and to calculate the number 

of devices in use and the age and sex distribution of the 

users, under various implantation rate assumptions The 

methodology for measuring the time—distance relationships of heart recipients to the rest of the population is 

Fig. 4. 

Total (n + y) dose-rates in mrems/hr in bisecting radial plane 

of source. (Excluding Pu-236 contribution QF = 10) 

*R W McKee, Battelle, Pacific Northwest Laboratory, 

Richland WA 99352, Contract AT(45 1) 1830 
61 

being developed, taking into consideration studies in 

the field ot environmental psychology relating to 

interpersonal distance requirements ot individuals 

Plan for Next Period 

Substantial survey measurements of time—distance 

relationships of people in the principal activities ot 

present day society (including occupation, leisure, 

travel, etc ) are anticipated The time—distance relation 

ships determined from the survey will be converted to 

radiation dose using a computer program Results will 

be summed up for all contacts of heart recipients with 

the rest of the population to provide an estimate of 

total radiation dose to the population 

Reports Published 

None 

Estimated Date of Final Report 

December 1972 

ARTIFICIAL HEART PROGRAM* 

Objective of Work 

Monsanto Research Corporation's (MRC) participation in the Artificial Heart Program consists of developing, in conjunction with TRW Systems, the design for 

the 50-W heat source and a process for fabricating the 

heat source and of producing both test and fueled 

sources for TRWs use 

Progress and Results 

Progress has been limited so far to conceptual 

discussions with the system's contractor 

Plan for Next Period 

During the next year, MRC will have completed the 

objectives listed above The hardware delivery quantities are twelve test capsules and three fueled heat 

sources 

Reports Published 

None 

*E W Johnson, Monsanto Research Corp Mound Laboratory, Miamisburg, OH 45342, Contract AT(33 1)-GEN53 and 

NASA, Ames Research Center, Moffett Field, CA 

Estimated Date of Final Report 

December 1972 

INTEGRATED WASTE MANAGEMENT -

WATER SYSTEM USING RADIOISOTOPES 

FOR THERMAL ENERGY* 

Objective of Work 

In the piesent Apollo spacecrafts water is not 

recovered from biological wastes because drinking water 

IS produced as a by-product ot the fuel cell electncal 

power system The waste management system does not 

provide earth-type convenience because of the short 

mission and the spacecraft restrictions on weight and 

electrical power, but longer space missions and more 

personnel will require a more acceptable approach to 

waste management Water must be recovered so that 

launch weight will be minimized For example, four 

men on a 180-day space mission will need nearly 

10,000 lb of water — which could cost as much as 

510,000,000 to supply 

The objectives of this program are to design, develop, 

fabricate, and test an engineering model of a completely 

integrated Waste Management Water System 

(WM—WS) using Radioisotopes for Thermal Energy 

(F^ITE) The complete system must be capable of 

collecting and processing wastes from four men for a 

180-day simulated space mission Subsystems include 

feces, trash, and urine collection, water reclamation, 

storing, heating, and dispensing the water, storage and 

disposal of the feces and urine residue and all other 

nonmetalhc waste material by incineration 

Progress and Results 

The system has been designed and fabrication has 

begun A new solids pump-filtei has been developed 

and IS being tested m the breadboard system for an 

additional 30 days The water recovery portion of the 

system is being operated at approximately 130% of 

capacity to ensure that excess water can be provided if 

necessary The water recovery efficiency is in excess of 

98% The incineration process typically reduces solids 

weight and volume bv 99% A new packaging arrangement has been derived (see photo) which permits 

separation of the waste collection from the processing 

section This arrangement also permits the use of several 

collection units with one central processing unit 

*R W Murray, General Electric Company, Space Division, P 

O Box8555,Philadelphia, PA 19101 Contract AT(11-1) 3036 
62 

,i €f 

• , .- " 

•. i 

Hi 

^ .. 

R--

,*w ^ 

Intergrates waste management water system. 

Plan for Next Period 

The total system will be assembled and tested. The 

radioisotope heater will be concurrently fabricated for 

use in a 4-man, 180-day test of the total system in a 

simulated space cabin. The selected fuel for the heater 

is Pu-238, with a thermal output of 400 W. 

Reports Published 

None. 

Estimated Date of Final Report 

February 1972. 

INTEGRATED WASTE MANAGEMENT PROGRAM 

[RADIOISOTOPES FOR THERMAL 

ENERGY (RITE) HEAT SOURCE] * 

Objective of Work 

The objectives of the work are to develop and 

fabricate the RITE heat source for use in the integrated 

waste management—water system. Present plans are to 

use the heat source in a system which will be used in a 

simulated space mission designed to accommodate four 

men for 180 days. Again, sources fueled with 

Pu(238)02 were selected because of their reliabiUty and 

weight savings. 

Progress and Results 

None. 

Plan for Next Period 

A modified Pioneer heat source fueled with 400 W(t) 

of Pu(238)02 shards will be fabricated at Mound 

Laboratory for delivery in February 1972. The heat 

source will be placed in a HasteUoy-C container and will 

be used initially for ground-test studies. 

Reports Published 

None. 

*C. E. Burgan, D. L. Coffey, and C. O. Brewer, Monsanto 

Research Corp., Mound Laboratory, Miamisburg, OH 45342, 

Contract AT(33-l)-GEN-53. 
63 

Estimated Date of Final Report 

Continuing project 

BIOMEDICAL ENGINEERING SUPPORT* 

Objective of Work 

The objectives of this project are (1) to determine the 

power required to drive an artificial heart under various 

conditions, (2) to determine the efficiency of a Kwan— 

Gett hemispherical artificial heart and the source of 

energy losses, and (3) to provide the USAEC with 

artificial ventricles and any information and expertise 

required m the development of an implantable power 

supply. 

Progress and Results 

The power requirements for an artificial heart with 

60% pump efficiency in a 25-yr-old 68-kg male 173 cm 

tall — with a daily energy requirement of 3295 kcal, an 

arterial pressure of 100 mm Hg, and pulmonary artery 

pressure of 15 mm Hg — have been determined from 

the literature. The average power for the total artificial 

heart is 3 23 W with a peak power requirement of 4 9 W 

during moderate exercise The average power requirement increases from 2 95 W at a body weight of 45 kg 

to 3.25 W at a body weight of 80 kg for the 25-yr-old 

male The average power requirement decreases from 

3.23 W at 25 years of age to 2.85 W at 70 years of age 

for the 68-kg male 

For measurement of the efficiencies of a Kwan—Gett 

artificial heart, the necessary equipment has been 

assembled to determine the energy input to the system 

at five locations (see figure) These measurements will 

be made under simulated circulation and verified in 

animal experiments The rates of energy transfer at two 

points are calculated from the flow rate of air determined by a venturi meter and the air pressure 

Pressure—volume diagrams are used to determine the 

energy transfers to the diaphragm in the air chamber 

and from the diaphragm to the blood chamber The 

volume of blood m the heart at any instant is 

determined by volume transducers The energy dissipated during simulated circulation is calculated from 

the fluid flow rate measured by an electromagnetic flow 

transducer and the arterial pressure No energy measurements have been made at this time. 

^00 0 FROf^ 

VEIN 

^JOOO TO 

ARTERY 

OlAPWASy 

® 

CHmfBER 

® \ARTIRCIAL 

VENTRICLE 

AIR DRIVE 

Lll ^ 

© 

PUL^S OF AIR 

FROM DRIVE 

SYSTEM 

Schematic of blood pump system. 

Plan for Next Period 

The efficiencies and energy losses for the artificial 

heart will be determined during simulated circulation 

These measurements will be verified by implanting 

artificial hearts m calves and measuring the energy 

transfer into the distal end of the air drive line under 

various cardiac outputs and arterial pressures in the 

animal 

Reports Published 

None 

Estimated Date of Final Report 

July 15,1972 

RADIOISOTOPE HEATER DEVELOPMENT 

PROGRAM - PHASE II* 

Objective of Work 

Phase I of this program was performed under spon 

sorship of the National Aeronautics and Space Administration, Manned Spacecraft Center (Contract 

*F M Donovan, Jr and W J Kolff, Department of Surgery, 

Division of Artificial Organs, Building 512, University of Utah, 

Salt Lake City, UT 84112, Contract AT(11-1)-2155 

*R B Goranson, McDonnell Douglas Astronautics Company, 

Donald W Douglas Laboratories, Richland, WA 99352, Contract AT(45-1)-2166 
64 

NAS-9-8846), and was completed during the second 

quarter of 1969. Phase I effort concentrated on 

preparation of 10- and 50-W plutonia and promethia 

reference design heaters for manned spacecraft using 

current technology. Designs included the largest number of potential applications with a minimum number 

of heater configurations. 

The Phase 11 program - completed August 30, 1971 

- included both manned and unmanned spacecraft 

applications and was directed toward development of 

radioisotope heater technology using improved containment and ablation materials. A major objective was to 

establish practical design configurations so that identifiable apphcations could be studied rapidly and efficiently. 

Progress and Results 

Data from questionnaires sent to NASA aerospace 

centers, the Department of Defense, and commercial 

satellite prime contractors about potential applications 

of 1- to 50-W heaters in manned and unmanned 

spacecraft were used to update the Phase I design 

criteria and identify a wide range of potential applications. 

Initial experimental effort was directed toward obtaining physical and thermophysical properties of candidate insulator and ablator materials. After a preliminary 

screening, efforts were concentrated on pyrolytic graphite (PG) and expanded pyrolytic graphite (EPG) insulators and on the DWDL-developed HfBj composite 

reentry ablator material. Thermal conductivity measurements gave values for hemispherical PG specimens lower 

than previously reported and confirmed the ideal 

conditions of thermal conductivity at normal temperatures. The very low thermal conductivity at reentry was 

confirmed by a series of arc-tunnel tests. 

By application of the experimentally determined 

thermal and physical properties of candidate materials, 

optimized heater designs were developed. Computer 

techniques have been developed that permit rapid 

design of minimum-weight heaters with an array of 

optional materials and geometries. For a given heater 

size and geometry (spherical or cylindrical capsule, 

spherical or cylindrical insulator, and cubic, cylindrical, 

or prismatic ablator), the program determines pressurevessel wall thickness and the required thickness of 

insulator and ablator layers for given lifetime and 

mission conditions. 

Post-test view of HfB2 composite cube and cylinder (left) and comparable ATJ-S models (right). 
65 

After initial design studies, 24 ablation test specimens 

were fabricated tor testing in the arc-tunnel facility of 

Aerotherm Corporation, Mountain View, CA The 

specimens included solid cubes and cylinders of ATJ-S 

and HfBj composite ablator material as well as a 

thermocouple-instrumented set of specimens containing 

Zr02 fuel simulant and PG insulator internal to the 

ATJ-S ablatoi Tests were run using full scale models at 

calculated reentry conditions The figure shows the 

HfBj composite ablators (left) and ATJ-S ablators 

following tests at identical reentry conditions The 

material loss evident on the ATJ-S specimens was not 

observable on the HfB2 composite 

Impact survival after reentry is another area of 

concern m heater safety Impact-test specimens were 

prepared (fuel simulant, container shell, and insulator) 

and tested at various velocities using the unique 

rotating-bloc impact-test facility at DWDL, which permits precise control of impact temperature, velocity, 

and orientation, minimum turnaround time (15 min for 

a cold specimen), and greatly reduced test costs A 

photograph of this apparatus is shown m the section 

frontispiece Data eliminated any existing preference 

for EPG over PG as a bumper material and yielded the 

basis lor semiempirical impact-survival prediction techniques for materials examined 

A brief series of simulated launch-abort debris tests 

was conducted at the MDC Aerophysics Laboratory, El 

Segundo, CA Heater models were subjected to 2000 

fps impact by 22 and 30/06 caliber bullets Results 

showed less capsule deformation when the ATJ-S 

ablator is replaced by the DWDL HfB2 composite 

Design, fabrication, and test capabihties — using 

advanced materials and techniques — have been devel 

oped to permit efficient response to specific heater 

questions 

Plan For Next Period 

The final report will be pubhshed 

Reports Published 

The Phase I Summary Report — pubhshed as McDonnell Douglas Report MDC-G2029 - was submitted to 

the USAEC in November 1970 

Estimated Date of Final Report 

A draft of the Phase II Final Report was submitted to 

USAEC on Sept 30, 1971 

DEVELOPMENT OF COBALT-60 HEAT SOURCES* 

Objective of Work 

The purpose of this project is to provide basic data 

that will be required to design, fabricate, and operate 

Co-60 heat sources Primary emphasis is on selecting 

materials to encapsulate cobalt fuel forms and estabhshmg temperature limits for long-term operation of 

capsules Development of specific heat source concepts 

IS not included, but assistance is provided when 

required for developing and testing demonstration 

units 

Progress and Results 

Heating tests ot four selected superalloys containing 

iiradiated and uniriadiated cobalt were continued The 

four alloys are 

Haynes 25 (Trademark of Cabot Corporation) 

Inconel 600 (Trademark of International Nickel 

Company) 

Hastelloy X (Trademark of Cabot Corporation) 

Hastelloy C (Trademark of Cabot Corporation) 

Measurements on 13 capsules, initially containing 

~13 thousand Ci of Co-60 each, after exposures up to 

20 thousand hr at 900° or 1000°C, showed maximum 

diameter changes of 

1 A decrease of 0 007 in on an Inconel-600 capsule 

heated 20 thousand hr at 900°C, the decrease 

piobably reflects spaOing of the oxide scale 

2 An increase of 0 008 in on a Haynes-25 capsule 

heated 18 thousand hr at 1000°C, this change 

probably reflects a density decrease in this ahoy due 

to precipitation of C02W 

Metallographic examination of two Hastelloy-X capsules (10 thousand and 20 thousand hr at 1000°C) and 

two Haynes-25 capsules (5 thousand and 20 thousand 

hr at 1000°C) showed that the widths of the reaction 

zones and the oxidation-affected zones were m good 

agreement with those measured on "inactive" capsules 

*S Mirshak E I du Pont de Nemours and Co Savannah 

River Laboratory, Aiken SC 29801, Contract AT(07 2)-l 
66 

heated under similar conditions For example, Hastelloy-X capsules heated 20 thousand hr at 1000°C had 

reaction zones between the alloy and the cobalt 0 0185 

m wide for the active capsule and 0 017 m wide for 

the inactive capsule. The depth affected by oxidation 

was 0 014 in. on the active capsule and 0.010 in on the 

inactive capsule Examination of the remaining capsules 

IS continuing 

These tests demonstrate that Haynes-25, Hastelloy-C, 

Hastelloy-X (20 thousand hr at 1000°C), and 

Inconel-600 (20 thousand hr at 900°C and 10 thousand 

hr at 1000°C) will perform satisfactorily as capsules at 

least at the indicated condition However, an inactive 

Haynes-25 capsule oxidized severely after 29 thousand 

hr at 1000°C, resulting in loss of weld integrity 

Nondestructive examination of this same capsule after 

11,500 hr had shown that the capsule was intact The 

oxidation reduced the wall thickness from 0 095 in to 

<0 050 in This amount of oxidation is essentially 

equivalent to the initial weld penetration and, therefore, caused the loss of weld integrity Tests of these 

alloys to 50 thousand hr are continuing 

Satisfactory performance through 1000 hr at 1200°C 

was demonstrated with a tungsten capsule containing 

unirradiated cobalt metal wafers Although the cobalt 

wafers bonded to each other, they did not bond tightly 

to the capsule and fell out during sectioning for 

metallographic examination 

Cobalt diffused into the wall of a W—Re capsule 

heated 1000 hr at 1200°C to a depth of 0 0065 in In 

another capsule, heated 1000 hr at 1400°C, the total 

depth was 0 012 in Extrapolation of these results to 50 

thousand hr predicts penetrations of 0 045 in at 1200°C 

and 0 085 in at 1400°C No more work on the 

compatibihty of cobalt metal with refractory metal 

alloys IS planned 

Construction of the new shielded cell to be used for 

long-term Co-60 capsule testing is complete Cold runs 

are in progress prior to installation of the Co 60 

Technical assistance is being provided in the project 

of Westinghouse Astronuclear Laboratory to design, 

fabricate, and test an experimental heat source containing ~2 MCi (30 kW) of Co-60 Tests were completed to 

measure the oxidation resistance of Nickel-200, Hastelloy-X, and Haynes-188 at 1000° and 1125°C 

Nickel-200 is similar to the stronger and slightly more 

oxidation-resistant Nickel-201 that will be used for the 

heat source core Hastelloy-X and Haynes-188 were 

candidate materials for the fuel capsules and pins, 

Hastelloy-X was selected because of its better oxidation 

resistance 

Because of the potential application of high-activitycobalt metal m heat sources, the USAEC has established 

a loan program for this material About 10 MCi (150 

kW) of Co-60 at over 350 Ci per gram of cobalt will be 

available for this program Most of this material is in the 

form of 0 745-in -dia wafers, plated with nickel Individual companies or groups of companies are invited to 

participate by contacting the Savannah River Operations Office of the USAEC Moderate activities and 

amounts of Co-60 can be obtained commercially 

Plan for Next Period 

During the next year, destructive examination of 

capsules removed from tests will be continued and 

technical support of the 30-kW heat source project will 

continue Heating tests of Co-60 capsules in the new 

cell will begin Compatibility of oxidized cobalt fuel 

forms with indium will be investigated 

Reports Published 

C L Angerman and C P Ross (Compilers), Savannah 

River Laboratory hotopic Power and Heat Sources 

Quarterly Progress Reports, USAEC Reports 

DP-1254, July September 1970, DP-1267, October-December 1970, DP-1272, January-March 

1971, DP-1279, April-June 1971 

Estimated Date of Final Report 

Continuing project 

COBALT-60 HEAT SOURCE 

DEMONSTRATION PROGRAM* 

Objective of Work 

The objectives of this project are to design, develop, 

fabricate, and test a terrestrial radioisotope heat source 

fueled with Co-60 for the purposes of estabhshmg 

heat-source integrity and safety, obtaining engineering 

information to guide the design of future devices to 

power a variety of energy conversion systems, demonstrating rehability and freedom from maintenance, and 

showing that a heat source of this type can be 

economically attractive 

*J W Sadler, Westinghouse Electric Corp , Astronuclear 

Laboratory, P O Box 10864, Pittsburgh, PA 15236, Contract 

AT{38-1)543 
67 

• # '>,<; 

Heat pipe for Co-60 emergency cooling subsystem. 

Progress and Results 

The Co-60 heat-source demonstration program has 

been divided into five phases: (1) preliminary design; 

(2) detail design; (3) fabrication; (4) demonstration test 

program; and (5) disassembly. 

The Phase II design, completed in October 1970, was 

modified early in Phase III based on results obtained 

from the supporting SRL Co-60 Material Technology 

Program, which indicated that the previously selected 

Co-60 encapsulating materials, Haynes-188 and 

Haynes-25, were subject to breakaway oxidation at the 

elevated temperatures corresponding to the emergency 

cooling mode. The heat source design was therefore 

modified to allow the use of Hastelloy-X as the 

encapsulating material and to provide a means of 

controlling the fuel pin cavity environment. The modified design provides for an argon coolant outlet 

temperature of 1350°F. 

Extensive testing of the heat pipes (see figure), which 

function as the passive emergency cooling subsystem, 

has confirmed the operating characteristics of the 

inert-gas-controlled heat pipe, specifically a switching 

temperature difference of 55°F from the 1040°F "off 

condition to the point at which 1 kW is transferred. The 

upper limit on heat pipe capability is approximately 1.5 

kW. Over 4000 hours of heat pipe testing, including 

weekly operating cycles, has been compiled. Procurement of the heat source and demonstration loop is 

continuing, and encapsulation of the 2 X 10* Ci of 

Co-60 has been initiated. 

Plan for Next Period 

Heat source assembly and test-loop checkout will be 

completed. The demonstiation program, including thermal characteristics and subsequent endurance testing, 

will be initiated. 

Reports Published 

J. W. Sadler and G. H. Parker, Large Cobalt-60 Heat 

Source Program, in Intersociety Energy Conversion 

Engineering Conference, Boston, MA, August 1971, 

pp. 741-50, Society of Automotive Engineers, Inc., 

New York, 1971. 

Estimated Date of Final Report 

The Phase III Summary Report will be issued April 

1972. 

PIONEER RADIOISOTOPE HEATER 

UNIT (PRHU) PROGRAM* 

Objective of Work 

The objective of this program is to design and 

fabricate small heat sources of Pu(238)02/Molybdenum 

Cermet (PMC) fuel for use on the Pioneer spacecraft as 

heaters for the tanks and nozzles handling the hydrazine propellant which freezes at 1°C. The use of the 

sources obviates the need for the spacecraft's electrical 

system to provide the necessary heating. 

Progress and Results 

Thirteen heat sources (see figure) were fabricated at 

Mound Laboratory and delivered for use on Pioneer 

Flight F. 

Plan for Next Period 

Fifteen heat sources are scheduled for fabrication in 

1972 for Pioneer Flight G. 

*E. W. Johnson, Monsanto Research Corp., Mound Laboratory, Miamisburg, OH 45342, Contract AT(33-l)-GEN-53 and 

NASA, Ames Research Center, Moffett Field, CA. 
68 

la Feam Spaemn 

Pioneer Radioisotopic Heater Unit (PRHU). 

Strength M»mb«r (T-11!) 

Clod (Pt-20 ih) 

Reports Published 

None. 

Estimated Date of Final Report 

Continuing project. 

A RE'VTEW AND EVALUATION OF 

TRW SAFETY ANALYSIS REPORT, 

VOLUMES I AND II, FOR THE 

PIONEER RADIOISOTOPE HEATER UNIT* 

Objective of Work 

The objective of this review was to verify the 

technical adequacy of the TRW Safety Analysis Report 

(SAR) on the 1-W Pu(238)02 Radioisotope Heater Unit 

(RHU). Twelve heaters were considered for use on each 

Pioneer F and G spacecraft. 

Progress and Results 

As stated in Volume I of the SAR, under certain 

unlikely conditions, PUO2 may be released from the 

RHU's as a result of (1) a launch pad abort which 

involves burning of the third-stage propellant; (2) an 

*R. L Werner and D. W. Pyatt, Weiner Associates, Inc., 107 

Industry Lane, CockeysviUe, MD 21030, Contract 

AT(30-1)-4145. 

ascent abort which leads to a grazing reentry 25 months 

or more after fuel encapsulation; or (3) a random 

orbital decay 20 years or more after fuel encapsulation. 

Weiner Associates, Inc., feels that a many-skip reentry 

could cause excessive ablation of the graphite heat 

shield, especially with the uncertainty of high velocity 

ablation data. However, all materia! released during 

reentry would not produce a hazard greater than 

1/10,000 of the maximum permissible burden (MPB) in 

human lungs, and whether additional releases can occur 

from other origins should not detract from the overall 

safety evaluation of the RHU's. While pointing out a 

few specific areas where further investigation might be 

in order, WAI generally finds the TRW Safety Analysis 

Report to be adequate. 

Plan for Next Period 

None. 

Reports Published 

A Review and Evaluation of TRW Safety Analysis 

Report, Volume I and II, for the Pioneer Radioisotope Heater Unit, USAEC Report WAI-TR-70.6-

AEC, Weiner Associates, Inc., December 1970. 

Estimated Date of Final Report 

The project has been completed. 
ENVIRONMENTAL 

AND OCEAN SCIENCES 

"AUTOTAPE" NAVIGATION 

RESPONDER NO 2 

RANGE MARKER 

PANELS 

AUTOTAPE NAVIGATION 

RESPONDER NO 

PROFILE 

SURVEY RANGE 

AUTOTAPE RANGE 2 

LARC-E FOR STANDBY, 

BOTTOM SAMPLING, AND 

BOTTOM PROFILING 

Z 

RADIATION DETECTION RECORDER 

AND AUTOTAPE INTERROGATOR 

INSIDE INSTRUMENT SHELTER 

UTILITY AND 

INSTRUMENT SHELTER 

. ^ DETECTOR 

CURRENT DIRECTION AND 

VELOCITY METERS TOWING AND 

INSTRUMENT CABLE 

IN SITU STATIONARY 

DETECTOR ARRAY 

APPROXIMATELY 40 SAMPLES 

OF TAGGED SAND 

( 5 METERS APART) 

Layout on beach for radioisotope sand tracking. 

Environmental and Ocean Sciences 

The objectives of the Environmental and Ocean 

Sciences programs are to develop isotope techniques to 

aid m environmental pollution control and to assist in 

the exploration and economic development of the 

oceans 

Technological achievements and the concurrent ad 

vances in standards and patterns of living have biought 

with them a myriad of enviionmental problems, some 

of the more notable being air and watei pollution, i e , 

the unwanted presence of chemical substances m low 

but often noxious concentiations To deteimine the 

damage pollutants may do to plants and animals the 

presence of such pollutants must be detected mea 

sured, and followed The measurement problems mvitea 

consideration of isotopic tracers and related analytical 

techniques, which, because of their extreme sensitivity 

and specificity, are potentially ver> valuable In addition, low-energy x and gamma rays from isotopic 

sources can be used for x-ray-fluorescence, Moessbauer, 

and absorptiometnc deteimmations of very low concentrations of substances 

Ocean science offers hope to the growing populations 

of the world Population inciease and rising living 

standaids are exerting increasing pressute on land 

resources, and man can no longer ignore the cultivation 

and mining potentials of the oceans Techniques foi 

extracting resources fiom the seas have not been 

developed because they have been uneconomic compared with land farming and mining and because 

knowledge of location of the sea's resouices has been 

restricted However, imminent shortages of food and 

minerals are rapidly making development of the seas 

essential Isotopic and radiation techniques hold many 

possibi'ities for obtaining oceanographic data that are 

difficult 01 impossible to obtain by othei methods 

The environmental and ocean-science projects are 

being conducted in collaboration with other government agencies that have primary responsibilities m these 

aieas, and many are being cofunded by these agencies 

In particular, ocean-science projects are being selected 

and technically monitoied with the assistance of the 

Navy's Oceanogiaphic Office 

The environmental-science projects aie presented first 

and aie followed by the oceanographic projects 

71 

73 

ATMOSPHERIC DIAGNOSTICS PROGRAM* 

Objective of Work 

The atmospheric diagnostics program has the objective of developing tracing methods and instrumentation 

and applying them to the study of pollution and 

meteorology The chief emphasis has been placed on 

the isotope-ratio and sulfur hexafluonde tracer methods The sulfur-isotope-ratio method, based on variations in the ratio of the stable sulfur isotopes -

S-32/S-34 — m sulfur from different sources, uses an 

isotope-ratio mass spectrometer It provides both a 

sensitive means of physically tracking SO2 from a 

discrete source and a way of measuring the degree of 

conversion that sulfur has undergone in a chemical 

reaction (since the ratio change resulting from isotopic 

exchange after the reaction is quantitatively related to 

the degree of conversion) The chemically stable SFg is 

a gaseous tracer for stack emissions whose concentra 

tion m an can be determined with extreme sensitivity 

and precision by gas chromatography These two tracer 

methods can be used either individually or as a dual 

system in which SFg defines the shape of a stack 

plume, against which measurements of chemical 

changes determined by the sultur-isotope-ratio method 

may be normalized 

Progress and Results 

The sulfur-isotope-ratio and SFg methods aie being 

applied to the study of sulfur pollutants in power-plant 

stack plumes at two tall-stack stations in lowbackground rural areas — the 370-MW oil-fueled Northport Station of the Long Island Lighting Company and 

the 900-MW coal-fueled Keystone Station of the Pennsylvania Electric Company Primary interest is in the 

oxidation of SO2 to sulfuric acid and sulfates as a 

function of distance of plume travel from the stack and 

ot meteorological conditions Sulfui hexafluonde is 

injected into the base of the stack, and samples are 

taken, aloft, of the plume and of the background At 

the same time, samples of the flue gas are taken 

isokinetically as it enters the stack The SO2, sulfate, 

and SFg concentrations and the S-32/S-34 ratios are 

then determined The laboratory instrument used for 

•ffi Manowitz, M Smith, L Newman, and W Tucker 

Brookhaven National Laboratory, Upton, NY 11973, Contract 

A1(30-2)GLN 16 The project is jointly supported with the 

Division of Biology and Medicine and the Environmental 

Protection Agency's Division of Chemistry and Physics and 

Division of Meteorology 

determining SF^ concentrations is based on a direct 

gas-chromatographic method and can detect 1 part of 

SF6 m 10'^ parts of air with no preconcentration The 

precision of the S-32/S-34 ratio determination is ±0 2 

per mil 

Ten to 20% conversion of SO2 to sulfate at distances 

of up to to miles under the conditions prevaihng has 

been observed A second-order mechanism is postulated 

for the oxidation, with a rate constant of approximately 1 hr ' ppM ' , possibly indicating an interaction between SO2 and particles m the plume or 

moisture absorbed on such particles 

Development of a real-time portable gas chromato 

graph for airborne detection of SFg has been completed, and it IS now in routine use in plume-definition 

studies (see figure) It is stable in operation and can 

detect 1 part of SFg in 10'^ parts of air It is being 

used in conjunction with an optical densitometer on a 

single plane in studies of the correspondence of the 

particulate and gaseous plumes from a stack 

The small-city SO2-distribution analyzer developed 

for New Haven, CT, indicated that the general background level of SO2, eithei emitted from low-lying 

sources or carried in from outside the city, was 

sufficiently high to obscure the contributions from 

individual high-stack sources m the city 

Plan for Next Period 

Work will continue along the lines alieady started 

establishing ot definitive patterns for SO2 conversion in 

plumes, mode of removal of sulfur oxides from plumes, 

the structure of plumes at long distances fiom a stack, 

and the nature of particulate sulfates formed in a 

plume Development of the techniques, equipment, and 

instrumentation required for the study of pollutant 

problems in the atmosphere will be continued Applica 

tion of the SF5 tracer method to tall stack plumedispersion studies m an urban area is being initiated in 

New York City 

Reports Published 

B Manowitz, L Newman, and W D Tuckei, The 

Atmospheric Diagnostics Program at BNL Third 

Status Report, USAEC Report BNL-50280, Decembei 1970 

B Manowitz, M t Smith, M Stembeig, L Newman, 

and W D Tucker, The Isotope Ratio Tracer 

Method Applications in Atmospheric Sulfur Pollut 

ant Studies, Second International Clear Air Congress, Washington, DC, December 1970, USAIC 

Report BNL-15095 
74 

Instrumentation for plume definition studies in place on aircraft, showing optical densitometer m rear, real-time SFg analyzer 

m front, together with inverters and storage batteries m case. 

M E Smith and D A Singer, Application of a 

Multisonic Model to an Urban Study, Ibid , USAEC 

Report BNL-15455 

G S Raynor, An Isokinetic Sampler for Use on Light 

Aircraft Atmospheric Environment, USAEC Re 

port BNL-15374, November 1970 

L Newman, M Smith, J Forrest, W Tucker, and B 

Manowitz, A Tracer Method Using Stable Isotopes 

of Sulfur, American Nuclear Society Topical Meeting on Nuclear Methods in Environmental Research, 

University of Missouri, August 1971, USAEC Re 

portBNL-16100 

B Manowitz and W E Viott, Nuclear Techniques for 

Studying Environmental Pollutants, Fourth UN 

International Conference on Peaceful Uses of 

Atomic Energy, Geneva, September 1971, USAEC 

Report BNL-15843 

Estimated Date of Final Report 

Continuing project 

MEASUREMENT OF SULFUR DIOXIDE 

IN STACK GASES* 

Objective of Work 

The objective of the SO2 stack-gas monitoring program IS to develop and test an instrument for determining SO2 in stack gases, based on a mercury 

substitution nucleonic detection principle The current 

phase IS directed toward the integration of an improved 

reaction cell (developed by Battelle Memorial Institute 

in Columbus, OH) into the gage and the testing of the 

instrument m the laboratory and in the field 

Progress and Results 

In the system developed, SO2 reacts stoichiometrically with insoluble mercuric oxide in a buffered 

*R J Pfeifer, Industrial Nucleonics Corporation, Federal 

Systems Division, 650 Ackerman Road, Columbus, OH 43202, 

Contract AT(30 1) 3882 
75 

aqueous medium to produce a soluble sulfite mercury 

complex The complex flows into a measuiement cell 

wheie the mercury concentration is indicated bv the 

absorption of low-energ\ x rays from Co-60 An 

improved cell was developed following initial field 

testing of a working model, which indicated several 

performance problems with the reaction cell The new 

cell has been integrated into the previously developed 

working model, and prehminary laboratory testing 

indicates that both the response time and system 

lehability are improved 

Plan for Next Period 

The working model will be extensively field tested, 

and efforts involving the cooperation of private industry as much as possible are envisioned for the near 

tuture Instrument commercialization, in which instrument size, rehabihty, performance, and cost factors will 

be optimized, will be accomphshed concurrently with 

the extended testing programs 

Reports Published 

B Y Cho, H J Evans, and L B Anderson, Radioisotope Methods of Sulfur Dioxide Measurement, 

Trans Amer Nucl Soc ,\\ 55 (1968) 

B Y Cho, Measurement of Sulfur Dioxide in Stack 

Gases, Studies of the Measurement of Sulfur Di 

oxide in Stack Gases, USAEC Report TID-25137 

(1968) 

R J Pfeifer and B Y Cho, Mercury SubstitutionNuclaonic Detection Instrument for Sulfur Dioxide 

Measurement, Analysis Instrumentation, 1 177 

(1969) 

R J Pfeifer, B Y. Cho, and O L Utt, Mercury 

Substitution—Nucleonic Detection Instrument for 

Sulfur Dioxide Measurement, ISA Transactions, 

9(1) 9(1970) 

R J Pfeifer, Measurement of Sulfur Dioxide in Stack 

Gases Demonstration Instrument Design, Fabrication, and Test, USAEC Report NYO-3882-2 (1970) 

Estimated Date of Final Report 

June 1972 

SNOW-MANAGEMENT RESEARCH* 

Objective of Work 

The purpose of the snow-management project is to 

assist industrial contractors m designing and testing a 

remotely operated telemetered version of the profihng 

isotopic snow gage developed in this project (described 

on page 105 of the 1968 edition of Research and 

Development Projects, TID 24823) 

Progress and Results 

Performance specifications tor a remotely operated, 

telemetered gage were developed and furnished to the 

scientists designing the gage at the Materials Testing 

Reactor site at Arco, ID 

A new gage was built and delivered to the Central 

Sierra Snow Laboratory at Donner Pass m the Sierra 

Nevadas ot California The gage, described in detail in 

the next section of this pubhcation, was intensively 

tested in round-the-clock operation during a part of the 

1971 snow season No major problems were encountered in operation of the equipment, and several 

opportunities were found to decrease operation time 

and thus data-gathering costs A snow gage used in 

near by snow-hydrology studies was used for comparisons 

In January 1971, a small burst of rain - 0 2 in — fell 

onto a deep snowpack and froze into an ice layer at 

about 40 in depth Two inches more rain fell, 

beginning about 8 hr later, and ponded above the 

impenetrable ice layer, melting the top 20 in of snow 

and flowing over the snow surface to create rivulets 

Ponded water was released from the snow in a very 

short time span The entire sequence of events was 

easily followed with the gage Other types of sensors in 

the mountains indicated the increase and sudden 

decrease in water at measurement sites The cause of 

this and the effect on the snow and stream flow could 

not be found with any other type of equipment 

Plan for Next Period 

During the snow year 1971-72, four telemetered snow 

gages will be installed — and operated automatically 

from one location — by Aerojet Nuclear Co We will 

train the data-analysis crews for each gage-user group 

and will select sites for the snow gages 

Reports Published 

None 

Estimated Date of Final Report 

June 1972 

*J L Smith, Water Yield Improvement, Conifer Zone, Pacific 

Southwest Forest and Range Experiment Station, US Forest 

Service, P O Box 245, Berkeley, CA 94701, Contract 

AT(49-11)-2773 This project is jointly supported with the U S 

Forest Service and the U S Department of Agriculture 
76 

••'•^"a^te . 

rf 7 

' / 

^^''i: 

^f^;g,. 

Artist's sketch of the profiling isotopic snow gage. 
77 

TELEMETERED PROFILING ISOTOPIC 

SNOW GAGE* 

Objective of Work 

The major objectives of the telemetered snow gage 

pioject are to demonstrate the feasibility of a tele 

metered gage, to fabricate and install three additional 

gages at user selected sites, to operate all four gages as a 

telemetered network, and to effectively transfer the 

technology to users 

Progress and Results 

The gage consists of two parallel vertical tubes that 

extend from below ground level up through the snow 

surface (see figure) One tube contains a Cs 137 source 

and the other a scintillation gamma detector As the 

tubes are lifted simultaneously in fixed steps, the 

gamma attenuation by the snow, and hence the snow 

density, is determined at various levels, yielding a 

density profile of the snow pack 

An engineered telemetered version of the gage was 

designed and fabricated and then installed m Cahfornia 

m March 1971 at the Cential Sierra Snow Laboratoiy 

on Donner Pass The base station was at Berkeley, 140 

miles away The telemetry data link vi'as by leased 

telephone hne Data were sent to the base station at the 

end of each lift step The field control unit that 

operates the gage under base-station control is designed 

to operate from —30 to ^-70°F It uses 15 W when 

operating and less than 2 W when on standby The first 

gage was installed without difficulty and operated quite 

successfully 

With completion of tests at Donner Pass, three more 

gages were fabricated and were installed in Colorado, 

in Idaho, and in Oregon — in November foi use during 

the 1971-72 snow season They are being operated, 

together with the Donner Pass gage, as a network from 

a central base station at the National Reactor Testing 

Station m Idaho After each run, snow density vs snow 

height data are sent by telephone to teleprinters m each 

user agency's office In normal operation, snow profiles 

for each site are taken automatically at night and the 

data stored for transmittal to the user agency upon 

request However, the user can request a run at any 

time and there is the additional option of the user 

running his own gage from his office via the cential base 

station 

Plan for Next Period 

Opeiation of the 4-gage network will be continued for 

the duration of the 1971-72 snow season Detailed 

specifications and drawings of the snow gage will be 

prepared for use by commercial vendors, and user 

agencies will be assisted m operation and maintenance 

of gages for the 1972-73 snow season 

Reports Published 

None 

Estimated Date of Fma! Report 

July 1972 

ROLE OF PAPER MILL ADDITIVES AS 

POTENTIAL STREAM POLLUTANTS 

DEVELOPMENT OF NUCLEAR 

ANALYTICAL TECHNIQUES* 

work IS to determine how 

IS actually required by the 

function and how much of 

a potential pollutant The 

hopefully, decrease both 

and the paper industry's 

additives leave the produc 

Objective of Work 

The principal aim of this 

much of a specific additive 

fibers to fulfill a prescribed 

It leaves the paper mill as 

information obtained will, 

pollution from paper mills 

economic loss when unused 

tion lines in the waste 

Progress and Results 

The major effort has been applied to the determination of in-plant process and effluent waters containing 

glucose and starch, which have very high potentiahties 

as stream pollutants 

For the determination of glucose, alkalized water 

samples were treated with a mixture of a mercury salt 

and diatomaceous earth The salt was reduced by the 

sugar to mercury, which was sorbed by the diatomaceous earth and determined by neutron activation As 

an alternative method, a mercury salt containing 

*P D Randolph and R L Heath \erojet Nuclear Co 

National Reactor Testing Station, Idaho Falls, ID 83401, 

Contract AT(lO-l) 1375 This project is jointly supported with 

the Soil Conservation Service, the National Weather Service, and 

the Bureau of Reclamation 

*R M Chatters, Radioisotopes and Radiations Laboratory 

College of Engineering Research Division, Washington State 

University, PuUman, WA 99163, Contract AT(45 1) 2221, Task 

3 This project is jointly sponsored with Washington State 

University and Northwest Pulp and Paper Association 
78 

Hg-203 was used, thus obviating the reactor-activation 

step and shortening the analytical time to less than 1 hr 

for an individual sample Each test involves less than 

10 ' /uCi of Hg-203 

Starch was determined by treating the effluent with 

enzymes to convert starch to glucose, which was 

determined as above 

A suitable tag for the common paper-making clay, 

kaolin, was found to be indium as ammonium chloroiridate, which was reduced, by hot sodium formate 

solution, to free indium or indium oxide, which then 

bonded to the clay Indium was determined by neutron 

activation analysis 

At the request of a western paper mill, a lanthanum 

salt tracer method was developed for tracing an 

adhesive through the plant process hues A lanthanum 

salt was added to the heated adhesive, which was then 

mixed with other stock, and samples from several places 

in the mill were analyzed by neutron activation 

analysis 

Samples for study have been collected in cooperating 

paper mills under normal conditions, and test materials 

used in the laboratory have been obtained from mill 

stocks or from the suppliers of paper mill additives 

Plan for Next Period 

A detailed investigation will be made of sizings (other 

than starch), pigments, dyes, bleaching compounds, and 

coatings, and analytical techniques wiU be studied 

Reports Published 

R M Chatters, G S Clifton, S D Slater, and J E 

Kimbrell, The Role of Paper Mill Additives as 

Potential Stream Pollutants Development of Nuclear Analytical Techniques, June 1, 1970—June 1, 

1971, USAEC Report RLO-2221-T3-1, December 

1971 

Estimated Date of Final Report 

Continuing project 

Objective of Work 

The mam objective of the oil-shck identification work 

was to define the methodology and utility of neutron 

activation analysis (NAA) for the identification of oil 

slicks 

Progress and Results 

Marine oil slicks and potential sources of shcks were 

examined with respect to replicate (matched) and 

different (unmatched) samples, and the NAA data on 

them were used to define a statistical basis for 

interpreting a pair of samples as matched or unmatched 

The effect of exposure and the preparation of slick and 

suspect source samples for analysis have been defined 

A difference-score (DS) technique was developed for 

quantitative sample comparisons, the observed concentration values for each element being codified so that 

the code scores have equal weight In a pair comparison, 

the differences in code scores for each element in the 

two oils are summed, and a constant is added for each 

case in which a given element is found in only one 

sample of the pair The DS scores of matched pairs 

follow a binomial distribution in which there is a 0 28% 

chance of exceeding D = 8 and a <0 0001% chance of 

exceeding DS = 15 Unmatched pairs have an average 

DS = 54, 0 5% chance of being <15, and essentially 

zero chance of being <8 Therefore, in the vast majority 

of cases, the trace element patterns of two oils indicate 

immediately whether the oils are matched or unmatched In a very few cases where DS = 9 to 15, the 

exact odds for each interpretation (which depend on 

the number of elements observed) may be computed to 

arrive at the most probable designation 

Plan for Next Period 

Phase II of project completed 

Reports Published 

H R Lukens, D Bryan, M A Hiatt, and H L 

Schlesinger, Development of Nuclear Analytical 

Techniques for Oil-Slick Identification (Phase IIA), 

USAEC Report Gulf-RT-A-10684, June 1971 

Estimated Date of Final Report 

*H R Lukens, D Bryan, M A Hiatt, and H L Schlesinger, 

Gulf Radiation Technology, Division of Gulf Energy and 

Environmental Systems, Inc , San Diego, CA 92112, Contract 

AT(04 3)-167 

DEVELOPMENT OF NUCLEAR ^^''""^^ ''''''^ ^''' *°"^> 

ANALYTICAL TECHNIQUES FOR 

OIL-SLICK IDENTIFICATION* 
79 

RADIOISOTOPIC SEDIMENT TRACING 

(RIST) STUDY SYNOPTIC STUDY OF 

SEDIMENT TRANSPORT* 

Objective of Work 

The basic objective of the radioisotopic sand tracer 

(RIST) study is to develop data on littoral tiansport, 

with the major effort concentrated on a synoptic study 

of the mechanics and rate of sediment tiansport m the 

offshore, inshore, and beach zones and to develop a 

simphfied survey system directly applicable to such 

studies as determining the rate of httoral drift and 

patterns of sediment movement in the vicinity of 

harbor- and shore-protection structures 

Progress and Results 

Efforts during the past year have been concentrated 

on the development of improved methods of environmental data collection to provide better correlation 

between tracer results and oceanographic conditions, 

and of theoretical models to determine the volume rate 

of littoral drift from tracer results 

An instrumented sled for measuring currents in 

various water depths at various distances below the 

surface in several planes was constructed and tested 

Other devices such as pressure transducers for wave 

measurement will be added at a future date ORNL 

designed a bottom-elevation monitor using a 100-mCi 

Cs-137 source at a fixed distance below the detector 

The monitor was recently tested at Point Mugu, CA, 

and elevation changes of 1 to 2 in were defected over a 

period of a few hours at a 15-ft water depth 

A method is being investigated for using tracers m 

quantitative measurement of the littoral volume drift 

rate Tracer is continuously injected in the surf zone 

When an equilibrium concentration is attained at an 

appropriate distance downdnft from the injection site, 

the drift rate, Q, is estimated from Q = 1/c, where 1 is 

the injection rate and c is the steady-state tracer 

concentration Further details of this project are reported in the ORNL project which follows 

Plan for Next Period 

A method of quantifying littoral drift will be finalized, and efforts will then be directed toward correlat-

*D B Duane, C W Judge W R James, and P G Teleki 

U S Army Corps of Engineers, Coastal Engineering Research 

Center (CFRC) 5201 Little falls Road, NW, Washington, DC 

20016, Contract AT (49 11) 2988 This project is jointly spon 

sored with CERC and Oak Ridge National Laboratory (ORNL) 

ing the determined drift rates with various oceanographic conditions for particular areas and estimating 

long-term drift rates from an analysis of a time 

sequence of oceanographic conditions Construction of 

the simplified data-collection system will be completed, 

and personnel will be trained by ORNL m its operation 

Tests involving the unit as a total operating package will 

begin at paiticular sites wheie data aie lequiied foi 

engineering purposes Work will also begin on designing 

modifications to the RIST system for tracing water 

masses and ocean disposal of dredge spoils 

Reports Published 

None 

Estimated Date of Final Report 

Continuing program 

RADIOISOTOPIC SEDIMENT TRACING 

(RIST) STUDY FUNDAMENTAL STUDIES 

OF SAND TRANSPORT AND 

EQUIPMENT DESIGN* 

Objective of Work 

The objective of the radioisotopic sediment tracing 

work IS to develop an underwater radiation survey 

system capable of operating m the surf zone, m deep 

water, and on the dry beach and to apply the system to 

coastal engineering problems involving sand transport 

and the determination of volume rates of sand trans 

port 

Progress and Results 

A PDF 8 computer was integrated with the radiation 

detection system and the range-positioning equipment 

Data introduced to the computer were processed in the 

field to yield a display of the survey vessel track and the 

radiation intensity along the track Formerly, data 

processing to determine the completeness of the survey 

required several weeks The on-board plotting was 

demonstrated at Masonboro Inlet, NC, where a survey 

was made to determine the operation of a weir jetty 

that had been installed to produce a ship channel A 

second demonstration was made at Point Mugu, CA 

Real-time plots of the survey were displayed on an 

*F N Case, E H Acree, and H R Brashear, Oak Ridge 

National Laboratory, P O Box X, Oak Ridge, TN 37830, 

Contract W-7405-eng 26 This project is jointly supported with 

the Army Navy, Air Force, and State of Cahfornia 
80 

oscillograph, and contour maps were prepared from the 

plots 

A compact survey system was designed and fabricated 

for use by the U S Army Corps of Engineers in routine 

sediment tracing The new system was designed with all 

the required functions of the preliminary system, but it 

IS smaller and has less power demand The new unit can 

be integrated with a PDP-8 computer to provide 

real-time data processing for display and can accept 

data from three different range finders, eliminating the 

need for a specific navigation system 

Measurement of the volume rate of sand transport is 

progressing through field tests and mathematical modeling However, normal sand-injection techniques cannot 

be used for labehng the system because of the slow 

equilibrium distribution of the labeled particles, and, 

once equilibrium is reached, the starting point for a 

measurement has not been determinable Further, the 

depth of the moving layer cannot be accurately 

measured To overcome these problems, a plug-mjector 

model was constructed, and experiments were designed 

to test the model A device was fabricated for inserting 

a 12-in -dia by lO-m -deep plug of labeled sand into the 

ocean floor The plug is sampled by coring, and data 

from radioisotope detection in the plug are used to test 

the mathematical model 

Plan for Next Period 

Project to be terminated 

Reports Published 

F N Case, E H Acree, and H R Brashear, A Survey 

System for Use m Tracing Radionuclide-tagged 

Sediment m the Marine Environment, m Nuclear 

Techmaues in Environmental Pollutions, Proc 

Symp Salzburg, Austria, Oct 26-30, 1970, pp 

603-28, IAEA, Vienna, 1971 (STI/PUB/268) 

Estimated Date of Final Report 

FY 1973 

EVALUATION OF TREATMENT PLANTS 

BY TRACER METHODS* 

Objective of Work 

The objective of this project is to study the application of tracer techniques to control of process conditions in multistage treatment plants for municipal and 

industrial wastes 

Progress and Results 

In close cooperation with sewage-treatment plants m 

the Metropolitan Atlanta area, tracer tests have been 

run to study the performance of sedimentation basins, 

trickling filters, and sludge-treatment systems Postsampling activation analysis, using nonradioactive 

indium salts as tracers and neutron activation in the 

Georgia Tech Research Reactor as the method of 

analysis, has been shown to be a simple, effective, and 

environmentally acceptable procedure 

Improper operating conditions, such as shortcircuiting and excessive recirculation, were shown to 

exist at some of the plants Labeling of sludge by 

mdium salts was found to be relatively simple, and the 

labeled compounds were chemically stable Much of the 

information obtained was clearly unobtainable by other 

means, and the cost per test seemed reasonable 

Laboratory tests were conducted to explore alternative tracer elements and different methods of labehng 

solids and to establish background concentrations in 

the water and in suspended matter for several potentially usable trace elements, including cobalt, scandium, 

and manganese Manganese was found to occur in fairly 

high concentrations in most local waters 

Methods were worked out for adequate samphng 

procedures and for semiautomatic activation analysis 

using a Ge(Li) gamma-ray spectrometer 

Plan for Next Period 

An important part of the project constitutes the 

transfer of the technology to plant opeiators and to 

industry at large This will involve demonstration tests 

over a larger geographical aiea as well as further work 

to minimize the cost of the test runs Additional work 

will also be done on sludge driers and other aspects of 

sludge treatment to monitor the attainment of optimum operating conditions 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

*G G Eichholz and T F Craft, Engineering Experiment 

Station and School of Nuclear Engineering, Georgia Institute ot 

Technology, Atlanta, GA 30332, C ontract AT(40 1)4156 
81 

NUCLEAR TECHNIQUES FOR SEABED 

MINERAL EXPLORATION* 

Objective of Work 

The objective of this program is to design, develop, 

test, calibrate, and apply a nuclear probe to seabed 

mineral exploration 

Progress and Results 

During the past year, the feasibility of using a 2-mg 

Cf-252 neutron source and a Ge(L!) gamma-ray spectrometer for the study of elemental concentrations in 

terrestrial and seabed materials was shown An mvesti 

gallon of the detection sensitivity of a remote probe 

system for some 40 elements in matrixes of varying 

density, water content, neutron absorption crosssection, and overburden was completed using a developed seabed-simulation facihty capable of handhng 

samples of up to 90 kg In addition, a subcntical 

assembly for Cf-252 neutrons which provides a 40-fold 

neutron multiphcation was developed and evaluated for 

use as a neutron radiation source for seabed mineral 

analysis This subcntical multiplier mockup was composed of a homogeneous mixture of PUO2 in polystyrene reflected with Plexiglas Simulated ocean floor 

*N A Wogman and R W Perkins, Battelle Pacific Northwest 

Laboratory, Richland, WA 99352, Contract AT(45 1)-1830 

mineral samples were irradiated with a 30- to 40-fold 

flux increase over that available without multiplication 

The investigation demonstrated that a subcntical assembly could be used to enhance the thermal flux from 

a Cf-252 neutron source m the seabed probe design 

These calibrations, standardizations, and model developments provided the necessary cnterions to complete 

the prototype design of an m-situ ocean floor mineral 

analyzer The system, which is being constructed, uses a 

2-mg or a 50-jUg Cf-252 source in the subcntical 

assembly with a multiplication factor of at least 40 (see 

figure) The gamma-ray detector consists of a solid 

cryogen-cooled Ge(Li) diode of about 15% efficiency 

with a resolution of less than 2 5 keV The entire 

underwater diode package contains the diode, preamphfier, bias supply, and cryogenics, with a cooling time 

of about 48 hr The probe assembly provides sample 

stabihzation, marker buoy storage, and vertical and 

horizontal positioning and has underwater lights, Ge(Li) 

control systems, and an underwater TV camera to 

permit viewing of the sample area and placement of 

both neutron irradiator and Ge(Li) probes 

Plan for Next Period 

Following final assembly of the Cf-252 seabed probe, 

It will be tested and calibrated m shallow ocean water — 

5D-ft depth — at the Battelle-Northwest oceanography 

site at Sequim, WA The system will then be used to 

=^^ ^ 

VE»TSCM l>OSITIONER 

SSSEMIV 

MDADUTION DETECTION 

raSITWNEi IDOUSLE 

kcnm mwrnim snmtim 

»E«TI£«L POSITIONER 

IHVOSAUUC HOTOPI 

\mmmM PUMP 

V«L»ES SM P S ELECTRWU 

SWITCHIM nWUITSI 

KTECTm posirm 

In-situ ocean floor mineral analyzer system. 
82 

determine the element concentrations m minerals at 

ocean depths approaching 300 ft. 

Reports Published 

R. W. Perkins, W. A. Haller, H. G. Rieck, L. A. 

Rancitelh, and N. A. Wogman, Cf-252 Neutron 

Activation for Remote Surface Analysis, m Neutron 

Sources and Applications, Proc. Amer. Nucl. Soc. 

National Topical Meeting, Augusta, GA, Apr. 19-21, 

1971, Vol. 3, pp. in-20-29 [summarized m Isotop. 

Radiat. Technol., 9(3)]. 

Estimated Date of Final Report 

Continuing project. 

RADIOISOTOPE DENSITY 

GAGE FOR THE DEEP-OCEAN 

SEDIMENT PROBE* 

Objective of Work 

A gage incorporating both transmission and scatter 

modes was designed and built for attachment to the 

Deep-Ocean Sediment Probe (DOSP) Collimation and 

discrimination are used to provide a narrow beam for 

accurate profihng. 

Progress and Results 

In laboratory tests, the scattei-section results indicated density changes The probe is now being tested m 

the bay, having been attached to sections of free 

flooding pipe to permit operation from a boat in waters 

up to 25 ft depth Undei a coordinated program, cores 

and in-situ electrical resistivity and foimation factor 

readings are being taken m the same locations as the 

density readings 

Plan for Next Period 

The gage will be attached to the DOSP for further 

testing m the bay. 

Reports Published 

None. 

Estimated Date of Final Report 

January 1972 

*V C Rose, 218 Crawford Hall, Department of Ocean 

Engineering, University of Rhode Island, Kingston, RI 02881, 

Contract AT(30-1)-4193 This project is jointly supported with 

the U S Navy Underwater Sound Laboratory 
RADIATION ANALYSIS AND CONTROL 

,^-^^.„%.^y/vc^, ^P^*"^^^ 

-12 00 -g 50 - 7 20 -14.80 - 2 40 0 00 2.HO 

VELOCITY MM/SEC 

4 80 7 20 9 60 12 00 

Moessbauei spectroscopy of an 18th-centuiy painting. 

The Moessbauer spectrum shown was obtained by 

backscattenng, as may be seen in the photograph 

The area analyzed is a yellow-brown color, and 

the spectrum is typical of natural iron ochre 

Radiation Analysis and Control 

The research and development objectives of the 

Radiation Analysis and Control program are (1) to 

provide improved technology for the detection and 

analysis of radioisotopes and nuclear radiation, and (2) 

to encourage and demonstrate the beneficial application 

of radioisotopes and nuclear technology to problems of 

national importance in such areas as consumer protec 

tion, quality control, public health and safety, natural 

lesouice management and law enforcement and na 

tional security 

Projects to develop instrumentation technology are 

directed toward estabhshing and upgrading basic capa 

bihties or broadening the technological base for the use 

of radioisotopes oi nuclear radiations from radioisotope 

sources The efforts are usually related to multipleusage goals and are not necessarily associated with 

specific haidware oi system requirements Projects to 

estabhsh the applications are closely related to specific 

requiiements or problems m national security, industry, 

or aerospace 

Emphasis has continued on the application ot nuclear 

technology to the problems of criminal justice and 

foiensic analysis Close liaison is maintained with 

government agencies that have the responsibility and 

opeiational requirements in these areas Special attention has been given to critical problems ot industrial 

development such as improved methods for minerals 

exploration and the application of nuclear technology 

to the field of construction materials and to civil 

engineering In general, the projects are earned through 

to an in-plant or field evaluation to clearly demonstrate 

their capabihties At this point, those industries or 

organizations who are interested in producing equipment or applying the technology are given full access, 

on an impartial basis, to the data and the reports that 

result from the development ettort 

Additionally, radioisotopes and nuclear technology 

may offer unique solutions to aerospace problems Most 

contracts in this area are jointly supported with other 

government agencies that have the specitit operational 

requirements 

85 

87 

RESEARCH ON SINGLE-CRYSTAL 

SEMI-INSULATING CADMIUM TELLURIDE 

AS A GAMMA-RAY SPECTROMETER* 

Objective of Work 

The objective of this work is to develop a roomtemperature gamma-ray spectrometer from single crystals of semi-insulating cadmium telluride (CdTe). 

Progress and Results 

The performance attained with CdTe was improved. 

Precipitates and an excess density of hole traps - the 

factors that limit resolution of devices — were analyzed. 

To overcome these obstacles, the Bridgman- and vaporgrowth techniques were refined, and crystals are being 

grown from solution. 

Semi-insulating CdTe gives good gamma response 

around room temperature. The first figure shows the 

room-temperature response of a 5-mm^ device to 

Cs-137 (662 keV) for a bias of 1000 V. The photopeak, 

Compton edge, and backscatter peak are at 95% 

charge-collection efficiency. The resolution is 30 keV 

(FWHM) and is limited by incomplete charge collection 

of holes. The second figure shows the response of the 

same device to a Co-57 source at 0°C for the same bias. 

The 136-keV line can be resolved clearly from the 

122-keV line; the resolution is ~6 keV (FWHM). For 

the linear plot (top), generators were inserted at 150 

*K. Zanio, N. Kyle, and W. Akutagawa, Hughes Research 

Laboratories, 3011 Malibu Canyon Rd., Malibu, CA 90265, 

Contract AT(04-3)-S49. 

keV with the bias off and at 175 keV with the bias on. 

The similarity of line broadenings indicates that leakage 

current does not degrade the resolution. Here, the 

resolution is limited primarily by the preamphfier noise 

and secondarily by incomplete charge collection. The 

log plot resolves the backscatter and escape peaks and 

the Pb X rays. Although spectrums from vapor- and 

Bridgman-growth modes are comparable, the best results achieved to date were obtained with Bridgmangrown material. However, much more Bridgman-grown 

material was sampled, and Bridgman growth received 

considerably greater emphasis. As the size of the device 

increases, the quahty of the photopeak degrades; with a 

1-cm^ device at 40% charge-collection efficiency, a 

photopeak could barely be resolved. The loss of 

2 V:^^^v^!V-i^'i•^:v!^'"^•;^^^^'"-•^y!"• '^^ V •' 

:^SM^-^ 

~ jfr;*-.,—-**.; V •.',-•? 

o 

Room-temperature spectra! response of a 5-mm" 

detector (linear plot) to Cs-137. 

CdTe 

Spectra! response of a 5-mm CdTe detector at 0°C to Co-57. 

Generator markers are inserted in the linear plot (top) at 150 

keV, with the bias on, and at 175 keV, with the bias off. In the 

log plot (bottom), the Compton peak, Pb \ rays from the 

coUimator, backscatter peak, escape peak, and 136-keV photons 

are apparent. 
88 

resolution is due pumanly to the presence of traps and 

piecipitates with inciease in device volume their 

effectiveness in degrading the resolution increases 

By analysis of the tiansient lesponsef of devices to 

ionizing ladiation the density and depth of tiapping 

levels have been determined A shallow electron trap 

with 0 06-eV activation energy and ~10' ^ centers/cm^ 

density was found and may be due to indium A deepei 

trap with 0 6 eV activation energy has again been 

measuied Only the deep tiaps limit the charge trans 

port, because lapid thermal emission occurs tor elec 

irons that are trapped at shallow levels In some cases, 

material has been analyzed that shows no deep electron 

trapping Because the mobility of holes (70 cm^/V sec) 

IS less than that ot electrons (1000 cm^/V sec), the 

charge tiansport of holes is generally pooier than that 

of electrons An analysis of hole transport showed a 

level at 0 13 eV with a density ot ~5 X 10'*" 

centers/cm^ At room tempeiature and at moderate 

electric fields, the charge transport is inhibited pri 

manly by the deeper-hole traps To learn moie about 

these deeper levels, improved mobility—trappmg-time 

products (iJ-T*) must be attained 

Precipitates also inhibit both election and hole 

transport Inflated microscopy of material after it was 

subjected to thermal-annealmg cycles indicates that the 

size ot precipitates can be reduced to less than the 

resolving power of the microscope (1 jum) and that, 

most likely, the piecipitates are due to deviations from 

stoichiometry and not to foieign atoms Pulse-height 

spectrums of alpha particles and of gamma rays are 

being used to analyze submicron precipitates and gross 

fluctuations in trap densities 

The resolution and the size of the detectors will be 

improved further when the concentrations of hole traps 

and precipitates are reduced The hole traps are either 

acceptor native defects or foreign atoms introduced 

into the lattice dunng crystal growth Several methods 

are in process to reduce the foreign-atom content In a 

separate research program, multiple distillation of 

synthesized CdTe is being undertaken Crystals are also 

being grown from the vapor and from solution to 

reduce not only the foreign-atom content but also the 

density of native acceptors Also to minimize precipitation, material is being vapor grown withm the phase 

field of CdTe Solution growth is being undertaken at 

the tellurium rich hquidus below 500°C under conditions that avoid precipitation 

tCoUaboration with A Albengi Quaranta, M Martini, G 

Ottaviani, and C Canah, University of Modena, Italy gave the 

results on transient response presented here 

Plan for Next Period 

The evaluation of the spectral response of semiinsulating CdTe to ionizing radiation will be continued, 

and those material imperfections that degrade resolution will be analyzed further More importantly, effort 

will be made to lower the foreign atom and nativedefect concentrations and to reduce precipitation by 

refining further the crystal growth processes 

Reports Published 

N R Kyle, Growth of Semi-Insulating Cadmium Tellunde, / Electrochem Soc 118(11) 1790 7 

(1971) 

C Canali, M Martini G Ottaviani, and K Zanio, Time 

of Flight Measurement of the Differential Negative 

Mobihty in CdTe, Phys Lett, 33A(4) 241-2 

(1970) 

A Albengi Quaranta, C Canah, G Ottaviani, and K R 

Zanio, Electron-Hole Pair Ionization Energy in 

CdTe Between 85°K and 350°K, Nuovo Cimento 

I ett ,4(19) 908-10(1970) 

C Canah, M Martini, G Ottaviani, and K R Zanio, 

Transpoit Properties of CdTe, Phys Rev B, 4(2) 

422-31 (1971) 

C Canah M Martini, G Ottaviani, and K R Zanio, 

Dependence of Electron Trapping Time on the 

Electric Field in Semi-Insulatmg CdTe, Solid State 

Commun ,9(2) 163-6(1971) 

W M Akutagawa and K Zanio, Vapor Growth of 

CdTe,/ Cryst Growth, !1 1 (1971) 

C Canali, M Martini, G Ottaviani, A Albengi 

Quaranta, and K Zanio, Characterization of High 

Resistivity CdTe for Gamma-Ray Detectors, Nucl 

Instrum Methods,96(4) 561-71 (1971) 

C Canah, G Ottaviani, M Martini, and K Zanio, Hole 

Drift Velocity m Semi-Insulatmg CdTe,^pp/ Phys 

Lett, 19(3) 51-3(1971) 

Estimated Date of Final Report 

Continuing project 

CADMIUM TELLURIDE DETECTORS* 

Objective of Work 

The objective of this project is to grow single crystals 

of cadmium telluride (CdTe), by the travehng-heater 

*F Wald and R O Bell Tyco Corporate Technology Center 

16 Hickory Dr Waltham MA 02154 Contract AT(30 1)4202 
89 

method (THM) of solution growth, for use in gammaray semiconductor detectors that can be operated at 

room temperature or above 

Progress and Results 

By the THM, primarily with Te as the solvent, CdTe is 

being grown which has the excellent homogeneity, low 

trap density, and low carrier concentration necessaiy 

for nuclear-radiation detectors The primary effort has 

been m three areas 

1 Temperature control. To successfully grow large 

single crystals of CdTe, the temperature distribution 

must be controlled carefully The heat flow must be 

adjusted, along with the length of the solvent zone, 

to produce a flat oi slightly convex solvent—solute 

interface Detailed calculations of the thermal distribution show that at least one reasonably flat 

isotherm exists in the cyhndncal geometry used m 

the THM furnace (first figure) Experimental modifications of the growth apparatus, such as the use of a 

watei-cooled section below the heater and rotation 

(~2 rpm) of the charged ampule to ensure uniform 

radial temperature distribution, have shown promise 

m achieving the goal of single-crystal growth 

2 Control of native defects After proper purification 

to remove electrically active impurities, a primary 

necessity of any semiconductor-growth technique is 

the control of native defects to minimize thermally 

generated earners and traps In the CdTe system, the 

electrical properties can be controlled by adding 

Group III elements (e g , In) and Group VII elements (e g , CI) For example, large amounts of 

indium (up to 10^° atoms/cm^) can be added to 

CdTe without drastic reduction of the mobility 

trapping-time product (JUT) while maintaining a low 

carrier concentration (<5 X 10^ atoms/cm^) A 

tentative explanation of this behavior has been 

developed by considering the doping in terms of the 

CdTe—In2Te3 solid-solution system 

3 Hall-effect measurements It has been determined 

that dc Hall-effect measurements can be performed 

successfully on high resistivity (10'' to 10^ 12 cm) 

CdTe, although great care must be taken to isolate 

and shield the leads and sample A completely 

guarded and Teflon-insulated measurement circuit is 

used The refinement of techniques for making 

ohmic low-resistivity contacts to both p- and n-type 

samples also contributes to the successful measurement Results to date are m good agreement with 

parameters derived from nuclear-detector measure0.2 0 3 

R (em) 

Positions of selected ssothermai Imes as a function of ingot 

radius and position along the ingot. 

ments The second figuie shows a pulse height 

spectrum of a CdTe detector 

Plan for Next Period 

Effort will be made to improve the fabrication of 

CdTe detectors, to study doping, including the verification of present models, to increase crystalhnity by 

seeding and by better temperature distributions, and to 

make detailed electrical, optical, and nuclear measurements on CdTe 
90 

100 

CHANNEL NUMBER 

Semilogarithmic plot of the pulse-height spectrum of a CdTe detector with a Cs-1 37 and with a Co-60 source. 

2 0 0 

Reports Published 

R. 0. Bell, Calculation of Gamma-Ray Pulse Height 

Spectrum in a Semiconductor Detector m the 

Presence of Charge Carrier Trapping, A^MC/. Instrum. 

Methods, 93(2): 341-8(1971). 

Estimated Date of Final Report 

Continuing project. 

EVALUATION OF CADMIUM TELLURIDE 

FOR RADIATION DETECTORS* 

Objective of Work 

The objective of this project is to evaluate presently 

grown cadmium telluride (CdTe) for use as radiation 

detectors. This is part of a continuing study to find a 

high-Z semiconductor material that will operate satisfactorily at room temperature and above as a counter 

and/or high-resolution spectiometei 

Progress and Results 

Cadmium telluride grown according to current stateof-the-art procedures has been evaluated by nuclear 

techniques for use as radiation detectors. The material 

was supplied by General Electnc Co., Hughes Research Laboratories, and Tyco Laboratories, Inc. The 

material had mobdity—trapping-time products (AT"^) of 

(2 to 8) X lO""* cmVV for electrons and (2 to 5) X 

*J M. Palms, Department of Physics, tmory University, 

Atlanta, GA 30322, Contract AT(40-l)-4146 
91 

< 

X 

o 

(s: 

UJ 

0 . 

z 

o 

•• 

~ 

-

-

*^Co 

14 keV 

• 

•_ 22 keV 

• • % 

'v 

Au 

1 .. 

K 

67 

K X-RAY 

ESCAPE 

97 

X RAYS 

KaV / 

1 

keV .• 

*^. 

'.*•* 

1 

• 12 2 kaV 

FWHM-10 7 kaV 

'. 136 keV 

1 ''--wJ 1 

ENERGY (keV) 

!LX)w-energy gamma-ray spectrum of Co-57. 

Detector CdTe, n-type 

Al surface-barrier 

Did, 2 mm 

Thickness, 7 mm 

Bias -40 0 V 

Preamphfier OrtecllSA 

Amplifier Tennelec TC-200 

Temperature 50°C 

10^^ cm'/V for holes. Detectors usable as alpha, 

gamma, and x-ray spectrometers were fabricated from 

high-resistivity (semi-insulating) and low-resistivity 

n-type CdTe (vapor-grown and grown from the melt) 

These devices were aluminum and gold surface-bariier 

detectors having 0.8- to 1.5-mm thicknesses and 2- to 

25-mm^ areas. Their pulse-height responses to lowenergy gamma and x rays were studied as a function of 

detector bias (0 to 1000 V), temperature (-75° to 

+52°C), and amplifier time constants (0.25, 1, and 4 

Msec). The pulse-height spectrums of all devices were 

affected by the presence of trapping sites and material 

inhomogeneities. All devices showed evidence of the 

mechanisms of trapping and detrapping of charge 

carriers; however, the total counting efficiency for most 

devices was high (>85%). The figures show some typical 

x-ray spectrums taken with a low-resistivity CdTe 

detector. The first figuie gives the gamma-ray and x-ray 

spectrums from Co-57. The energy resolution (FWHM) 

of the 122-keV line is 10.7 keV, and the pulse-peak 

resolution at the same energy is 8.6 keV. The K x-ray 

escape peaks of Cd and Te, which he ~25 keV below 

the 122-keV line, are clearly evident. The peak at 67 

keV IS due to fluorescence K x rays from a piece of gold 

used as a pressure contact to the aluminum electiode. 

The peak at ~22 to 24 keV is due to fluorescence K x 

rays from indium, which is used as a backing pad for 

the detector. The second figure shows the low-energy 

gamma and x-ray spectrums from Am-241 Even though 

the electronic resolution was not optimized for the 

spectrums shown, these spectrums demonstrate cleaily 

that material suitable for x-ray spectrometeis is now 

being grown However, considerable improvement in 

detector perfoimance is expected if mateual can be 

grown that has reduced trapping-site concentration as 

well as more-homogeneous structure. The last property 

is particulaily impoitant if larger detectors suitable foi 

higher-energy gamma-ray spectiometry are to be fabricated. 

Plan for Next Period 

State-of-the-ait material will be evaluated continuously by nuclear techniques. This woik should lead to 

an understanding of the correlations between material 
92 

< 

I 

o 

o o 

-

-

~ 

-

14 keV 

• •. 

1 

\ 33 

1 

keV 

1 

- - • 

* 

1 

59 keV 

FWHM-9 8 keV 

PULSER 

84 keV 

FWHM 

6 5 keV_ 

ENERGY (keV ) 

X-ray spectrum of Am-241. (Conditions same as for first figure ) 

characteristics and crystal-growing techniques In addition, to obtain a moie complete material characterization, with emphasis on undeistanding the trapping sites, 

electron paramagnetic resonance and fai-intiared 

Fourier spectroscopy will be used to determine the 

location, structure, and population density of the 

trapping sites, as well as the free-carrier concentration 

in the material Along with these measurements, radiation detectors will be continuously fabricated and 

evaluated 

Reports Published 

J M Palms, Newer Developments in Detector Design 

and Materials, m Semiconductor Detectors in the 

Future of Nuclear Medicine, P B Hoffei, R N 

Beck, and A Gottschalk, Eds , Society ot Nuclear 

Medicine, 1971 

Estimated Date of Final Report 

Continuing pioject, annual report will be submitted 

in early 1972 

LOW-NOISE FIELD-EFFECT TRANSISTORS'* 

Objective of Work 

The objective of this work is to develop low-noise 

field-effect transistois (FET's) particularly suited for 

the amplification of signals from radiation detectors 

Progress and Results 

The specific problem of interest is the noise generated 

by "lossy' dielectiics The source ot this noise is 

indicated by the shaded area in the equivalent diagram 

ot radiation detector charge amplifiei combination in 

the figure The noise due to dielectuc losses is generated 

m the insulating materials used for FET encapsulation 

This noise source was obscure until observed and 

analyzed quantitatively It is not inherent to the 

amplification mechanism, it represents a hmit m noise 

and therefore in energy resolution - that could be 

achieved with an otherwise ideal noiseless FET The 

properties ot this noise are summarized here, and some 

relations in terms ot easily measurable parameters are 

given 

A lossy dielectric is shown as source 4 in the figure If 

a dielectric with low dielectric losses is used, its 

dissipation factor is a constant 

D 

G(co) 

wC^j (1) 

where G(co) and Cj are the loss conductance and the 

capacitance of the dielectric as measured on an imped 

ance bridge at an angular frequency co According to 

the dissipation—fluctuation theoiem, the conductance 

•^V Radeka, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-1)-16 
93 

I SERIES WHITE NOISE 

SIGNAL 

Q 8(f) 

2 PARALLEL WHITE NOISE 

(RESISTOR, LEAKAGE CURRENT) 

(ENC)^ PC Tj INDEPENDENT OF C,n 

FET SERIES NOISE • = NOISELESS 

AMPLIFIER 

3 SERIES J NOISE 

(ENC)^ OC cf„. INDEPENDENT OF T 

^^^o—° 

4 PARALLEL "f" NOISE 

(DIELECTRIC LOSSES. 

FREQUENCY DEPENDENT RESISTOR) 

(ENC)^ INDEPENDENT OF TAN D C,n 

Noise sources m the charge amplifier and their equivalent noise charge (ENC) as a function of filter time constant, T, and input 

capacitance, Cm [Source 1 (FET channel noise) is of principal interest, source 2 (dielectric noise) sometimes exceeds and masks 

other sources ] 

G(GJ) generates Johnson noise (current) at the frequency CO, 

? (OJ) = 4 kT G(w)df = 4 kt (DCd)codf (2) 

Where k = 1 38 X 10 " joules/°K, co = 27Tf, and T is 

the temperature of the dielectric This noise current is 

converted into a noise voltage on the input capacitance. 

Two numerical relations useful for evaluating various 

dielectrics and FET packages follow from Eq 4 In the 

first, the equivalent noise charge is expressed m 

root-mean-square electron charges as a function of 

dielectric loss factor D and sample capacitance C^j, 

ENCf«^6X 10** 

295 

1/2 

(DC.)>/^ [rms e| (5) 

1^(0)) G(w) DC. df 

v2(co) =—^—- = 4 kT——r^ df = 4 kT — - — -

co"'Cf„ co^C^„ CO Cl 

(3) 

Thus, the lossy dielectric generates an |f| noise-current 

spectrum in parallel with the input, which integrated on 

the input capacitance becomes l/|f| noise The equivalent noise charge due to this noise can be calculated 

conventionally by integrating the noise voltage at the 

output of the filter with respect to frequency and 

comparing it with the signal output One obtains for the 

equivalent noise charge, 

(ENCf)^ kT (DCj) , (4) 

where e = 2 718 

The most interesting characteristic of this noise 

source is that its contribution is independent of both 

the input capacitance and the filter time constant Also, 

It depends httle on the type of the filter 

In cases where the dielectric and/or its capacitance are 

not known, it is more convenient to use the loss 

conductance as measured on an impedance bridge at an 

arbitrary frequency f,., in the range of interest By 

substituting Eq 1 and co = 27rf in Eq 5, one obtains 

ENCf = 2 44 

X 10" 

-ry/2 

295 

G(fo) 

f„ 

1/2 

[rms e] (6) 

The dielectric noise is an unnecessary component of 

the amplifier noise and can exceed the channel noise of 

the FET The channel noise is inherent in the amphfication mechanism, and its reduction is the mam target in 

this project Thus, any proposed FET package should 

first be examined tor dielectric noise The effect of 

dielectric noise on energy resolution for several differ 

ent types of FET packages is given in the table It is 

essential to use materials with low dielectric losses, such 

as beryllium oxide and high-purity alumina Aluminas 
94 

Noise of Field Effect Transistors Arismg in Dielectric Supports 

(T= 295°K) 

Type of package 

and materials 

T0 5,epoxy 

TO 5, glass metal 

BEO 

Alumina, 995 AI2O3 

Loss conductance 

G(fo)at 

= 1C* H? 

nmhos 

3 19 

0 28 

0 025 

0 02 

Equivalent noise 

ENCf 

rms e 

138 

41 

12 

11 

charge 

Lower limit for 

noise line width 

FWHM, 

eV (Si-equivalent) 

1 2X 10^ 

3 6 X 10^ 

1 04 X 10^ 

0 96 X 10^ 

are easier to work with m production The test samples 

of new FET's are being mounted in an alumina package 

Once the material is found to be satisfactory, the 

package geometry should be optimized so that the gate 

capacitance is minimized 

Plan for Next Period 

New devices with a smaller gate-channel geometry will 

be evaluated, they were developed with Texas Instruments, Inc , as a part of this program 

Reports Published 

V Radeka, State of the Art of Low Noise Amplifiers 

for Semiconductor Radiation Detectors, m International Symposium on Nuclear Electronics, Vol I, 

pp 46-1 46-28, Versailles, 1968 

V Radeka, l/lf| Noise in Physical Measurements,/iL/* 

Trans Nucl 5 a ,NS-16(5) 17-35 (1969) 

Estimated Date of Final Report 

Continuing project 

NEW RESEARCH APPLICATIONS 

OF CERENKOV RADIATION* 

Objective of Work 

The objective of this project is to develop and 

evaluate new apphcations of Cerenkov radiation Potential areas for study include fission-product analysis, 

environmental radioactivity, biomedical assay, and 

special counting systems 

*H H Ross, Oak Ridge National Laboratory, P O Box X, 

Oak Ridge, TN 37830, Contract W 7405-eng-26 

Progress and Results 

Dual-isotope experiments make up an important 

segment of biomedical tracer applications A study was 

completed which shows that the Cerenkov counting 

technique can be used to assay two radionuclides 

simultaneously The technique is rapid, precise, and 

inexpensive Also, a simple computer program was 

developed that models the Cerenkov system and that 

can be used both to establish the optimum operating 

conditions of the counting system and to estimate the 

error in the assay measurement A description of this 

work IS being prepared for publication 

The first part of a program to develop Cerenkov 

techniques for monitoring radionuclides in the environment was completed The study illustrates the very high 

sensitivity attainable for aqueous environments, typical 

results show that many radionuclides in concentiations 

<2 pCi/hter can be detected This sensitivity compares 

favorably with the sensitivities of other slower and 

more expensive low-level techniques 

Plan for Next Period 

Project terminated 

Reports Published 

H H Ross, Performance Parameters of Selected Waveshifting Compounds for Cerenkov Counting, in 

Organic Scintillators and Liquid Scintillation Counting, pp 757-69, D L Horrocks and C-T Peng, 

Eds , Academic Press, New York, NY, 1971 

Estimated Date of Final Report 

All reports are or will be published m the open 

literature 
95 

EVALUATION OF THE 200-mCi IRON-55 

X-RAY DIFFRACTION SOURCE IN 

FOCUSING AND DEBYE-SCHERRER 

ANALYTICAL APPLICATIONS* 

Objective of Work 

The objective of this work is to evaluate the feasibihty of using a 200-mCi Fe-55 source for x-ray 

analytical powder diffraction Both Debye-Scherrer 

and focusing back-reflection camera geometries are to 

be studied In each case, the exposure times required to 

obtain weU-resolved x-ray diffraction patterns will be 

evaluated critically The major advantages of an isotopic 

x-ray source for diffraction are that no power and no 

coohng are required and the source is very small, 

lightweight, and stable The major disadvantage is the 

relatively low intensity of the x rays available 

Progress and Results 

Work continued with the 2-in -dia Debye—Scherrer 

diffraction camera and the Fe-55 x-ray source Because 

of self-absorption and natural decay, the effective 

output of the source was only ~110 mCi A new 

coUimator and beam stop were designed and constructed m an attempt to reduce the amount of 

scattering inside the camera chamber The collimator 

has a 0 5- by 10 0-mm entrance sht A second sht of the 

same dimensions defines the x-ray beam A final scatter 

sht, which does not intersect the mam beam, captures a 

*L E Preuss, Edsel B Ford Institute for Medical Research, 

2799 West Grand Boulevard, Detroit, MI 48202, Contract 

Al(ll-l)-2063 

large portion of the radiation scattered by the first two 

slits With the new collimator and beam stop, the 

background scattering m the diffraction patterns has 

been reduced to an acceptable level Usually, LiFpowder-diffraction patterns are obtained in 20 to 30 hr, 

and the hne width of the reflection from the (200) 

plane is ~0 7 deg 0 (first figure) Since the active area 

of the source is 2 by 10 mm, only 25% (28 mCi) of the 

radioactivity is actually used with this collimator Use 

of a wider entrance slit would adversely affect the 

resolution 

To improve the useful intensity, the 2-mm-wide 

souice was mounted obhquely behind the 0 5-mm 

entrance slit The mounting angle of 14 5 deg allowed 

radiation from the entire source to pass through the 

entrance sht In this way, exposure times were reduced 

by ~'/3 without loss of resolution 

A 2-in -dia focusing back-reflection camera was designed and constructed The source is mounted on the 

circumference of the camera, a set of apertures m front 

of It defines the beam The powder-diffraction sample is 

placed directly opposite the source on a 30-deg arc of 

the camera, which can record reflections in the 0 range 

55 to 73 deg With this camera, a series of exposures 

was made using several apertures and powderdiffraction samples To avoid loss of resolution, only 

part of the active area of the source could be used 

With a 0 25- by 3 7-mm entrance sht, diffraction 

patterns of LiF powder could be obtained in 8 hr 

(second figure) With this sht, only 5 7% ot the active 

area of the source (~6 mCi) was being used The hne 

width was usually ~0 5 deg 6 The camera was 

equipped with a motor to continuously oscillate the 

Densitometer trace of the x-ray diffraction pattern obtained from LiF powder m the Debye—Scherrer camera m 20 hr [I rom 

the extreme edge to the center of the trace, the five prominent peaks correspond to reflections from the (222), (311), (220), (200) 

and (111) planes ] 
96 

^ 

U 

Densitometer trace of the x-ray diffraction pattern obtained from LiF powder m the back-reflection camera m 8 hr. [The peak 

near the edge of the film is from the KQ, reflection on the (311) plane, the other peak is from that on the (222) plane The 

asymmetry of the pattern is due to anomalous scattering from the aperture j 

sample through a few degrees With the motoi in 

operation, exposure times could be reduced by about 

one-half 

Plan for Next Period 

This project has been completed 

Reports Published 

W S Toothacker and L E Preuss, Developments m 

Analytical Diffraction Using Isotopic X-Ray 

Sources, in Advances in X-Ray Analysis Vol 14, 

pp 139-45, C S Barrett, J B Newkirk, and C R 

Rudd, Eds , Plenum Press, New York, NY, 1971 

L E Preuss and W S Toothacker, X-ray Diffraction 

Using Fe-55 Sources, Nature Phys Sci, 231(18) 

19-20(1971) 

Estimated Date of Final Report 

December 1971 

produced by particle accelerators, the development of 

instrumentation and techniques for a variety of applications of x-ray and gamma-iay spectrometry, and the 

study ot techniques that use x-ray, gamma-ray, and 

isotopic-neutron sources The basic data consist of 

gamma-ray spectrums, precision eneigies. intensities, 

and branching ratios for the gamma rays emitted in the 

decay of radionuclides Such data are essential to 

nuclide identification, use of the nuclides as standards, 

and both industrial and biomedical applications of 

tracers ** 

In view of the broad applications developing for 

high-resolution x-ray and gamma-ray spectroscopy, considerable emphasis is being placed on the establishment 

of usable cnterions for testing and calibrating equipment used in these techniques and on the continued 

development of on-line computer systems and software 

for automated analysis of pulse-amplitude spectrums 

Current emphasis also includes the evaluation of geometries tor containment of Cf-252 isotopic neution 

GAMMA-RAY SPECTROMETRY OF 

NEUTRON-DEFICIENT NUCLIDES* 

Objective of Work 

The major objectives ot this program continue to be 

the generation of data about neutron-deficient nuclides 

*R L Heath, J E Cline and R J Gehrke, National Reactor 

Testing Station, Aerojet Nuclear Co Idaho falls, ID 83401, 

Contract AT(10-1)-1375 

•^^These data are published m the Gamma Ray Spectrum 

Catalogue and appear tabulated in the Handbook of ChemKtn 

and Physics 
97 

sources for both prompt and conventional activation 

analysis 

Progress and Results 

Gamma-ray spectrums, energies, and intensities were 

obtained for >30 radionuclides produced by reactions 

such as (7,xn,yp), (p,xn,yp), or (n,xn,yp) on the 

100-MeV electron hnear accelerator at the Lawrence 

Livermore Laboratory and the 600-MeV synchrocyclotron at the SREL f These data wiM be included in the 

Ge(Li) Gamma-Ray Spectrum Catalogue The precise 

measurement of energies of gamma rays for use as 

energy-calibration standards has been extended up to 3 

MeV, thus providing a variety of well-estabhshed 

reference hnes for laboratory use To obtain precise 

relative and absolute intensity measurements, techniques have been developed and documented for the 

analysis of pulse-amphtude spectrums obtained with 

Ge(Li) and Si(Li) detectors This work has included 

evaluation of commercial amphfiers, analog-to-digital 

converters, and associated electronics used in highresolution x-ray and gamma-ray spectrometers The 

results will be pubhshed, and the cnterions for estabhshing meaningful performance specifications for such 

equipment will be made available to vendors and 

experimenters 

Development of techniques for automated data analysis of x-ray and gamma ray spectrums has continued 

Automated techniques for peak location, energy determination, and nuclide identification have been developed for small on-hne computer data systems for 

laboratory use The first figure is a block diagram of a 

computer data system for the measurement and analysis 

of data for apphcation in x-ray fluorescence This 

system, now in routine use, permits the complete 

automatic analysis and elemental identification of 

materials present in unknown samples The use of 

interactive techniques, including real-time data display 

on an oscilloscope screen, affords the laboratory analyst 

much flexibihty in analyzing experimental data The 

second figure illustrates the real-time analysis of data, a 

segment of a radioisotopic x-ray Puorescence spectrum 

is shown The screen display gives the elemental 

identification of the x-ray hne (by the arrow), the 

energy of the line, and the channel number 

Significant progress was made m applying x-ray 

fluorescence to the measurement of manganese in 

carbon steels With this technique, hot ingots of steel in 

rolhng-mill operations can be characterized 

fSpace Radiation Effects Laboratory, Virginia Polytechnic 

Institute, 11970 Jefferson Ave , Newport News, VA 23600 

1 Dtttctor 1 

Y , 

Source 

J Cryogenic 

1 Prsamp | 

1 

Cahbrsted 

Pulse Gen 

- — Amplifier 

DigitsI 

Csmputer 

ADC 

Ught PI 

Oscilloscope 

O O 0 o 

n 

:> 

Fwctisn 

Keyboard 

Block diagram of automated x-ray fluorescence analyzer. 

Graphic display of automated analysis of x-ray spectrums. 

The availabihty of Cf-252 isotopic neutron sources at 

reasonable cost has greatly expanded interest m the 

possible industrial-laboratory and field use of neutron 

techniques Extensive experiments have been made to 

estabhsh recommendations for optimizing design geometries for both internal-sample and external-beam 

arrangements of these neutron sources The availability 

of this information and the experimental verification of 

elemental sensitivities for both prompt and conventional activation techniques that use these neutron 

sources should be of value m assessing the potential of 

the activation technique in this mode 
98 

Plan for Next Period 

The first edition of Ge(Li) Gamma-Ray Spectrum 

Catalogue will be pubhshed in February 1972 

Reports Published 

R J Gehrke, J E Cline, and R L Heath, Determination of Relative Photopeak Efficiency and System 

Linearity for Ge(Li) Gamma-Ray Spectiometers, 

Nucl Instrum Methods,9\ 349-56(1971) 

R J Gehrke and R A Lokken, Efficiency Calibration 

of a Low-Energy Si(Li) Photon Spectrometer, 

Trans Amer Nucl Soc , 14(1) 126-7 (1971) 

R L Heath, Table ot the Isotopes, Handbook of 

Chemistry and Physics, 52nd Ed , Chemical Rubber 

Co , Cleveland, OH, 1971 

J E Chne, Gamma Rays Emitted by the Fissionable 

Nuclides and Associated Isotopes, USAEC Report 

IN-1448, December 1970 

J E Chne, P D Randolph, E L Mum, M J Laird, 

and R L Heath, Elemental Determinations in 

Idaho Wildlife Samples, / Idaho Acad Sci , Special 

Issue No 2 28 (Aug 1, 1971) 

R C Greenwood, Prompt-Neutron Activation Analysis 

with a Cf-252 Source, Trans Amer Nucl Soc , 

14(2) 932(1971) 

Estimated Date of Final Report 

Continuing project 

APPLICATION OF NUCLEAR 

TECHNOLOGY TO ART-IDENTIFICATION 

PROBLEMS* 

Objective of Work 

A number of nuclear techniques offer promise in 

solving problems of art identification, including the 

objective detection of forgeries and the objective 

characterization of genuine works of art The purpose 

of this project is to develop such techniques tor use by 

museum authorities, appropriate government agencies 

such as the Internal Revenue Service, or interested 

private individuals 

*B Keisch, Carnegie-Mellon University, 4400 Fifth Ave , 

Pittsburgh, PA 15213, Contract AT(30-l)-3953 This project is 

jointly supported with the National Gallery of Art, Washington, 

DC 20565 

Progress and Results 

By methods developed eailier m the history of the 

project, neutron activation analysis (NAA) was shown 

to be usable for distinguishing among artists on the 

basis of the measuied trace-element content ot the lead 

white used in their woiks The procedure necessarily 

involves the separation of the pigment and its impurities 

from extianeous material also present in the usual work 

of art Data analysis based on the estabhsliment ot 

probable ranges of trace-element content is used to 

calculate the overall probabihty that a questioned work 

belongs to a particular source 

Neutron activation analysis was also used to help 

determine the commonality of sources of various 

terra-cotta statuaiy, as well as various bronze and brass 

objects, at the National Gallery of Art 

The technique of identifying man-made C-14 in 

hnseed oil as a means to detect forgeries of oil paintings 

produced since the 1950's was extended to other 

artists' materials such as wood and paper Methods for 

the simple but efficient conversion of such materials 

into a form suitable for hquid scintillation counting 

were explored A new method, that of dissolving 

sample-derived acetylene in a toluene-base liquid scintillation solution, was developed This method shows 

great promise in its ability to handle samples of 

intermediate size (e g , 1 to 2 g of paper) 

The use of the Moessbauer effect to analyze works of 

art was explored A variety of frequently used artists' 

pigments contain iron compounds There is, at present, 

no satisfactory way to distinguish among ochres, 

siennas, and various red, black, and yellow synthetic 

compounds and mixtures thereof In a series of measurements (by transmission) performed on samples of 

pigment from a variety of sources, it was demonstrated 

that (1) meaningful classification can be made, (2) the 

composition oi mixtures of various oxides can be 

determined semiquantitatively, (3) particle sizes can 

sometimes be determined on the basis of observation of 

superparamagnetism, and (4) natural materials can 

often be distinguished from synthetic It was shown 

that, with a backscattenng configuration, such measurements can be made m situ on actual paintings (see 

figure at start of this section), from which the same 

information as described above can be derived without 

sampling or harming the work in any way 

It was also shown that the temperature at which 

terra-cotta, or alleged terra-cotta, statuary had been 

fired can be estimated This information may help with 

the authentication of a number of questionable works 

The apphcation ot Moessbauer-effect spectrometry to 

other iron-bearing pigments, such as green earth and 
99 

Prussian blue, was also explored as a means to determine the composition (for the former) or the mechanism involved in the process of fading (for the latter) 

Plan for Next Period 

Since the exploratory and demonstration phases of 

this research project are essentially completed, the U S 

Atomic Eneigy Commission's support of this work will 

be terminated at the conclusion of the current contract 

year However, because of the successful nature of the 

work accomplished, much of the work wiU be continued by personnel of the National Gallery of Art 

Research Project This work will include the gathering 

of large quantities of data to make the apphcation of 

these various techniques into a practical and useful 

methodology 

Reports Published 

B Keisch, Application of Nuclear Technology to Art 

Identification Problems, Third Annual Report, February I, 1970-February 28, 1971, USAEC Report 

NYO-3953-3, September 1971 

B Keisch, X-Ray Diffraction and the Composition of 

Lead White, Studies in the History of Art, National 

Gallery of Art, Washington, DC, 1970 

Estimated Date of Final Report 

March 1972 

STUDY OF TOOTH-ENAMEL DENSITY* 

Objective of Work 

The objective of this project is to apply the avalanchetype beta-particle detector, developed under a previous 

USAEC contract with the General Electric Co , to the 

problem of accurately determining the density of tooth 

enamels m vivo Accurate density measurements are 

needed to study tooth-density differences as related to 

the onset of dental caries and to provide a means of 

measuring the rate of etching and solubihty of tooth 

enamels in various solutions under m-vitro conditions 

It was proposed to study tooth-enamel density in 

porous regions created during tooth formation, in 

regions demmerahzed due to dental decay, m areas of 

*F C Besic, R Zechman, P Johnston (General Electric Co , 

Philadelphia, PA), P Hoffer, M R Wiemann, Jr , and O Keller, 

ZoUer Dental Clinic, University of Chicago, Chicago, IL 60637, 

Contract AT(Il-l)-2095 

increased mineralization due to aging, and m teeth 

susceptible to acid dissolution and teeth resistant to 

dissolution 

Progress and Results 

The detector was obtained to measure tooth density 

The instrument is unique m that both the radiation 

source and the backscatter detector are located m the 

probe head The probe was constructed initially with 

Tl-204 (20 /tCi), brass cones were placed over the probe 

head to hold the sample at a fixed distance from the 

radiation source To eliminate abnormal backscatter 

obtained with the brass cones, they were replaced with 

five Lucite cones However, count rates produced from 

crystalhne material by the radiation source were too 

low to be useful To increase count rates, the radiation 

source was changed to Pm-I47 (5 mCi) The probe 

again gave mechanical problems The main tunnel diode 

was replaced but operated for only a few minutes 

thereafter The control systems ceased to function and 

were replaced 

The on-going work consists in the following 

1 The construction of a stabilizer—holder for the 

probe prior to its assembly at a determined optimum 

source—specimen distance A graduated microscopical stage, designed for precise calibrated travel, 

IS being incorporated into the system to allow exact 

positioning and adjusting of the probe—specimen for 

obtaining desired parameters 

2 The use of the probe (minus the radiation source in 

the probe head) as a tool to monitor the uptake of 

F-18 apphed topicaUy to the surfaces of extracted 

teeth Experiments are being designed to show the 

relation between the observed F-18 and the total F, 

measured with an electron microprobe, in the 

sample teeth 

Plan for Next Period 

The contract has been terminated However, the 

contractor proposes to continue the project, at his own 

expense, in order to obtain an effective approach to 

determining differences in tooth-enamel densities, a 

measurement that may yet be possible when the new 

radiation source is properly positioned m the probe 

head Some of the recent laboratory studies, exclusive 

of the beta-probe project, indicate that the density of 

the enamel surfaces is related to their solubility If this 

is so and if such critical densities can be measured with 

the probe, teeth vulnerable to dental decay could be 

detected before cavities begin to develop 
100 

Reports Published 

None. 

study are: Mg, Al, Si, P, S, CI, Ca, V, Fe, Cu, Zn, As, Br, 

Mo, Ag, 1, Hg, and Pb. 

Estimated Date of Final Report 

September 1971. 

RADIOISOTOPIC X-RAY FLUORESCENCE 

SPECTROMETRY FOR MULTIELEMENT 

ANALYSIS OF AIR POLLUTANTS* 

Objective of Work 

The purpose of this project is to investigate the 

sensitivity of energy-dispersive radioisotopic x-ray fluorescence for the analysis of particulate air pollutants 

and to develop a technique for their routine multielement analysis that is rapid, nondestructive, and 

inexpensive. The elements provisionally selected for 

*J. R. Rhodes and A. H. Pradzynski, Columbia Scientific 

Industries, P. O. Box 6190, Austin, TX 78762, Contract 

AT(40-l)-4205. 

Progress and Results 

Standards for 20 elements were prepared by depositing standard solutions and solid compounds (mainly 

oxides as fine powders) on separate filter-paper disks of 

the same brands as those on which air particulates are 

collected [Whatman 41 and Schleicher & Schuell (S&S) 

589]. 

A laboratory system and a routine procedure for the 

measurement of 17 elements in samples of air-pollution 

particulates were set up (see first figure). In cooperation 

with the Texas State Air Pollution Control Board, two 

batches of samples collected on Whatman 41 filter 

paper in 43 different locations in Texas were analyzed 

(see second figure). 

Another batch of 14 samples collected on S&S 589 

filter paper in New York City was measured for 14 

elements, including cadmium and barium. The data 

were compared with the results of atomic absorption 

Facility for x-ray fluorescence analysis. 
101 

10.000 

1,000 

100 

10 

5C-

• 

RAY 

Ca 

FLUORESCENCE SPECTRUM OF AIR PARTICULATE 

Ke< 

1 

• 

"•• • 

'.•.• • 

F t K « 

t 

Zn Ke< 

1 

•. 

i • 

• • . 

SAMPLE 

Pb L«<+AsK« 

t! 

« '

FROM 

PbL ^ 

. 

Br K»< • 

Zn K^ • ? 

1 

, .' 

1 1 1 

EXCITATION SOURCE Pu-23 8 

COUNTING TIME lOMIN 

AIR VOLUME IS90 tr? 

FILTER PAPER WHATMAN 41 

TOTAL DEPOSIT 106 >i g/em 2 

• 

, • 

• • 

S8 K»<. 

•A .' 

• 

WEST, TEXAS 

• 

, 

; • 

..' 

*".• 

go 4 0 SO iO 100 liO 140 160 ISO 200 ZZO 

CHANNEL NO. 

X-ray spectrum of an air particulnte sample collected m an industrial site m west Texas. 

analyses The majority showed good agreement, the 

differences are being investigated 

The grain-size effect is an important potential source 

of error m x-ray fluorescence analysis of particulates 

The most accurate theory on particle-size effects'''^ 

assumes "infinitely" thick samples that contain par 

tides of a single size The theory was generalized to 

include samples of arbitrary finite thickness with 

continuous distributions of particle sizes Useful formulas have been obtained for practical correction factors 

**? } Berry, T Furuta and J R Rhodes Particle Size 

Effects in Radioisotope X ray Spectrometry m Advances in 

X Ray Analysis, Vol 12 pp 612 32, C S Barrett J B 

Newkirk, <<nd G R Mallett, td s Plenum Press, New York, NY, 

1969 

Plan for Next Period 

Different standard-preparation techniques and types 

of sample collection filters will be comj ared The 

validity of the derived formulas for particle size effects 

will be tested experimentally 

The investigation will also include reseaich into the 

possibility of using simple chemical techniques for the 

mditect determination ot Be, C, F, Mg Al, Si, P, and S 

in particulates 

Reports Published 

None 

Estimated Date of Fmal Report 

Continuing project, annual report, August 1, 1972 
102 

PORTABLE RADIOISOTOPIC X-RAY 

FLUORESCENCE DETECTOR OF 

BULLET HOLES* 

Objective of Work 

The objective of this work is to determine the field 

applicability, in law enforcement, of radioisotope x-ray 

fluorescence for detecting lead residues from a projectile. 

Progress and Results 

In a field examination where the types of firearms 

and projectiles may not be known, a control procedure 

must be established to evaluate the primary means of 

examination — in this case, the radioisotopic probe with 

*M. Brewer, Dade County Public Safety Department, 1320 

NW 14 St., Miami, FL 33125. This work is related to the work 

at Panametrics, Inc., under Contract AT(40-1)-3561. 

connecting console and counter used to identify lead 

residues around a suspect bullet hole. The sodium 

rhodizonate colorimetric method for lead was used as a 

chemical control. By this method, as little Pb as ~0.1 

/ig can be determined. The lead was extricated from the 

suspect bullet hole with a cotton swab and was 

determined colorimetrically. This chemical control was 

laboratory tested on several micro and semimicro 

quantities of lead standards prior to use as a control in 

the field. The materials examined in the field included 

wooden surfaces, cement, screen, plastered cement, 

Sheetrock, glass, and cloth. Soft-solid materials (mostly 

crystalline) frequently gave negative results by both the 

colorimetric and x-ray fluorescence methods. Pulverization of the material that receives the Pb wipe may 

partially explain the negative results; the pulverized 

material falls from the crater produced by the projectile 

and causes what is tentatively called "crater wipeout" 

(see figure). The shock wave that results from the 

Photograph showing crater "wipeout" effect on wall. 
103 

impact of the projectile and that precedes the projectile's passage through the solid material may be a 

cause of this wipeout 

Sheetrock walls often gave negative results for both 

the entry and the exit sides of the holes If complete 

entry or passage through the wall did not occur, a 

positive result was more frequently obtained 

Cloth composed of both synthetic and natural fibers 

gave positive results The cloth was not examined 

extensively, because a microscopic study of the suspect 

cloth IS frequently conducted in many gunshot cases 

Positive results obtained by the x-ray fluorescence 

method were reliable and, in all cases, correlated with 

wet-chemical test lesults 

Negative x-ray fluorescence results (which also agreed 

with wet-chemical test results) indicated an absence of 

lead residue However, in some instances, the suspect 

hole was definitely caused by a lead projectile Thus, 

the mstiumental x-ray fluorescence examination of 

suspect bullet holes is a reliable indicator if the results 

are positive but not if they are negative Research 

completed to date indicates a need to study further the 

mechanism of the transfer of lead from projectiles to 

surfaces Further research is needed on a greater variety 

of materials that may recieve the Pb residue 

Plans for Next Period 

None 

Reports Published 

None 

Estimated Date of Fmal Report 

February 1972 

X-RAY FLUORESCENCE ANALYSIS SYSTEM 

FOR LEAD IN BLOOD* 

Objective of Work 

The purpose of this woik is to develop an x-ray 

fluorescence system foi measuring lead in blood In the 

health-depaitment laboratories of most large cities, 

blood lead is now determined by atomic absorptiometry — a method that requires at least 5 cc of blood 

and certain chemical manipulations Obviously, there is 

*G R Laurer and T J Kneip, New York University Medical 

Center, 550 ! irst Ave, New York, NY 10016, Contract 

AT{30 l)-4252 

reluctance to taking serial 5-cc samples from a 2- to 

3-year-old child Nevertheless, this is necessary for 

sound diagnosis and treatment planning, especially 

where chelation is being considered To minimize delay 

and the number and size of samples, a portable analysis 

system is needed ~ one that can be used at regional 

health clinics or m a mobile van 

Progress and Results 

For children's blood, a lead concentration of ~0 3 

ppM IS considered to be normal, a concentration as high 

as 0 4 to 0 8 ppM is abnormal, 0 6 ppM being generally 

accepted as the level at which treatment should be 

given X-ray fluoiescence analysis for lead in paint 

indicated that this method, with sufficient increase m 

sensitivity, might detect lead at sub-ppM levels in blood 

Increase m sensitivity means essentially an increase in 

the signal-to-noise ratio Consequently, the emphasis 

has been to maximize both the production of characteristic X rays in the sample and the detection of these x 

rays Thus, the variables selected to be optimized were 

(1) energy and half-hfe of the excitation souice and (2) 

source—sample—detector geometry 

Since the most efficient production of characteristic x 

rays arises from absorption of photons just above the 

absorption edge, Fu-238 was chosen, it emits x rays 

(uranium—L x rays) just above the Li and L3 absorp 

tion edges of lead Although this x-ray emission is not 

as abundant as that fiom some other radioisotopes, e g , 

Cd-109, It IS essentially free from any higher-energy 

gamma rays and hence does not present shielding 

problems Also, it has a long half-life (86 yr) and is 

relatively inexpensive 

The primaiy factor in the design of the sourceholder—collimator was the size of the blood sample, 

chosen to be 0 05 ml an amount easily obtainable 

with a hematocrit tube from a fingei puck Several 

source—sample detectoi configurations were designed, 

and the efficiency of each was estimated The fust 

figuie shows the one selected, a design inspired by the 

availability of Pu(238)02 as 250-/i-dia miciospheres 

bach microspheie contains 1 0 mCi of Pu, which allows 

25 mCi of radioactivity to be arranged in a 2-mm-dia 

circle With this arrangement, the sample in the form ot 

a 1-mm-cross-section "doughnut" can be irradiated 

thioughout 360 deg of the source plane with no 

external scattering to other material Also, two detectors can be used face-to-face This contiguiation allows 

the closest possible proximity of both source to sample 

and sample to detector, the estimated geometiical 

eificiencies of which are ~11 and ~10%, respectively 
10-fti!l Be 

250-p-dIo PuO, Spheres (25 altogether) 

SECTION B-B 

Source-holder - collimator (top view). 

:A 

\ 

Cryostot Surface 

Blood "Doughnut" Target 

5 to 10-mil Be "Window" 

o 

200-tnm''Si(LO Diode 

Source-holder - collimator in place on cryostat with sample in position. 
105 

The blood doughnut is formed by dropping the 

red-blood cells, after centnfugation, onto a precut 

Milhpore backing filter placed on a Teflon form 

Heat-lamp drying shrinks the doughnut to approximately the dimensions shown 

A 200-mm^ Si(Li) detector will be placed 5 mm 

below the beryllium entiance window (see second 

figure) This detector size is a balance between resolution and detection efficiency Since only the 10 5-keV 

La peak of lead will be observed and since the closest 

large interfering peak will be the 11 9-keV Ka of 

bromine, the 270-eV resolution attainable with a 

200-mm^ detector should be adequate and stiU maintain a reasonably narrow lead peak 

Plan for Next Period 

When the source and detector system are received, the 

reproducibihty of results, obtained with the doughnut 

geometry, wiU be determined with blood samples of 

known lead content Also, the hmit of detection of the 

method will be estabhshed, it should be ~0 1 ppM for an 

~15-mm counting time Two background interferences 

are foreseen that may further limit the sensitivity (1) 

scatter-peak taihng due to edge effects in the detector, 

and (2) La x rays from the detector's gold entrance 

window Both of these could be limited by use of a 

facing metal other than gold and/or use of a guard-ring 

detector For a large-area detector, the improvement 

possible with the latter is uncertain 

The use of a Cm-244 (half4ife, 17 6 yr) source, also 

available m microspheres, is planned The radioactivity 

of a 250-iLt-dia Cm-244 sphere is about five times that of 

a Pu(238)02 sphere of the same size The source 

configuration for Cm-244 has not been decided 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

KRYPTONATES FOR THE ANALYSIS 

OF AUTOMOBILE EXHAUSTS* 

Objective of Work 

The objective of this project is to develop an 

instrument that uses Kryptonates'** in the analysis ot 

air pollutants in automobile exhausts Instruments now 

accepted for use have the disadvantages of being 

sophisticated laboratory devices that require trained 

operators In the instrument being developed, the same 

principle is used to detect carbon monoxide, hydrocarbons, and nitrogen oxides The prediction is that 

such an instrument could be operated by service 

personnel and be suitable for monitoring an pollutants 

emitted by automobiles during periodic or random 

inspections 

Progress and Results 

Kryptonates have been prepared from a number of 

substrates The Kr-85, which is introduced and stably 

incorporated into a solid substrate, is located in the 

surface layers only Upon reaction of the solid with a 

gaseous air pollutant, Kr-85 is released at a rate that 

depends on the concentration of the pollutant and on 

the Kr-85 concentration in the surface layers By use of 

small-particle-size powders and long times for the 

Kryptonate preparation, sensitivity to a particular 

gaseous species can be maintained constant during the 

detection hfetime of the Kryptonate 

Phase I of this program (a feasibility study) illustrated 

that adequate sensitivity can be achieved easily to meet 

the projected 1975 Federal standards for automobileexhaust emissions (50 ppM foi hydrocarbons, 250 ppM 

for NOj^, and 5000 ppM for CO) 

The current effort (Phase II) is devoted to constructing and testing a breadboard instrument (see 

figures) No effort was spent on package design, 

nevertheless, the potentiahty for developing a portable 

instrument is demonstrated by the fact that the 

breadboard instrument can be housed in a container 

having ~1 25-ft^ volume and ~20-lb weight The fiont 

panel contains the samphng inlet and all the necessary 

controls 

The Kryptonate sensors selected are PtOa Kryptonate for hydrocarbons, I2O5 Kryptonate for CO, and 

hydrocarbon clathrate for NO2 Since NO does not 

react with the hydroquinone sensor under the operating 

conditions, it is oxidized to NO2 by catalytic conveision The catalyst is Draeger CH294 (Draegerwerk, W 

Germany), which is effective at room temperature In 

an alternate method, a heated copper hehx is used 

Each method has advantages and drawbacks, but 

catalysis is currently used for simplicity 

*P Goodman, Panametrics Inc , 221 Crescent St Waltham, 

MA 02154, Contract AT(30-1)4069 

**Registered trademark of Panametrics, !nc 
AMBIENT 

'^"' - DRIERITE I-KX H FLOWMETER 

106 

CATALYST 

(DRAEGER CH294) A NO, SENSOR 

(HYDROQUINONE-®^Kr) -^Sh 

POLLUTANT *.0<3— FLOWMETER 

CO SENSOR 

I2O5-

-eK2> 

-mitHEATER 

•p 

DETECTOR PUMP 

READOUT 

HC SENSOR 

(Pt02-*^Kr) 

-^^x)—^ 

-wvw>-

HEATER 

Block diagram of auto-exhaust quality monitor. 

Photograph of auto-exhaust quality monitor. 
107 

The exhaust gases from a "dirty," laboratory, 4-cycle 

test engine were examined with the breadboard instrument The results were compared with measurements of 

hydrocarbons by flame-ionization detection and of CO 

by nondispersive infrared spectrometry The agreement 

was excellent Automobiles were also tested under 

various conditions and at several installations, both 

private and governmental Again, the results agreed 

excellently with those of the other two methods No 

comparison instrumentation for determining NO^ was 

available, however, m all test situations the NO^ reading 

was consistent with that expected in view of CO and 

hydrocarbon responses Signal levels remained constant 

over the duration of the test cycle and did not 

deteriorate on exposure to the exhaust gases 

Plan for Next Period 

From experience with the breadboard unit, the design 

configurations will be optimized in terms of sensitivity, 

r> ponse and recovery times, and sensor lifetime 

Sc^ I il prototype instruments will then be constructed 

and piCiented to independent groups in the field of 

pollution control for critical assessment After that, 

further changes may be needed The resulting exhaust 

monitor should be a state-of-the-art, portable, prototype instrument suitable for a wide variety of applications 

Reports Published 

None 

Estimated Date of Fmal Report 

Phase II report Early 1972 

NUCLEAR INSTRUMENT 

LANDING SYSTEM* 

Objective of Work 

The objective of this project is to develop a shortrange guidance system for landing aircraft The recent 

efforts by the U S Federal Aviation Agency and the 

aircraft industry to decrease the minimum-visibihty and 

ceiling requirements for landing of aircraft have created 

a need for a very accurate and rehable aircraft-guidance 

system Phase I, which was completed in July 1971, 

*R A Kammskas, TRW Systems, One Space Park, Redondo 

Beach, CA 90278, Contract AT(04-3)-828 

includes the design and laboratory test of a breadboard 

system The Nuclear Instrument Landing System 

(NILS) IS designed as a short-range guidance system that 

will augment the Instiument Landing System (ILS) and 

will provide highly accurate aucraft-position information during the last phases of descent and touchdown, 

where the present landing aids fail to function adequately In conjunction with the ILS, the NILS 

provides a means to guide aircraft during completely 

automated landings in zero-visibihty weather The NILS 

can also serve as an independent monitoring system to 

check the position of the aircraft before it is committed 

to a landing 

Progress and Results 

The NILS consists of ground and airborne equipment 

The ground equipment comprises four beacons, permanently installed at the airport near the runway as 

illustrated in Part A of the figure The airborne 

equipment is carried in each aircraft The operating 

principles of the NILS are similar to those of the ILS 

except that the rf beams are replaced by gamma 

radiation from Co-60 radioisotopic sources The gamma 

radiation emitting from the beacons is colhmated and is 

modulated with four characteristic frequencies by 

mechanical shutters to provide radiation beams similar 

to those used by the present ILS 

The mechanical shutters consist of a thick metal 

cyhnder having three equally spaced slots m the top 

half and two slots m the lower half The radioisotopic 

source is placed m the center of the cylinder When the 

shutter is rotated about its axis, it modulates the 

emanating radiation at one frequency m the top region 

above the center plane perpendicular to the axis of 

rotation and at another frequency below the plane 

All beacons are identical in construction, however, 

the shutters of beacons on the right of the runway are 

rotated at 1800 rpm, and those on the left at 720 rpm 

so that four frequencies are produced 

Part B of the figure gives a block diagram of the 

airborne equipment A radiation detector detects the 

radiation, and the frequency content of the detector 

output IS recognized by four frequency detectors tuned 

to receive frequencies Fi, F2, F3, and F4 The position 

of the aircraft in relation to the NILS beacons is then 

determined by comparing the frequencies to give lateral 

and vertical displacements as shown m Part C of the 

figure The aircraft-position information is displayed to 

the pilot on a standard ILS indicator m the cockpit 

By use of cone-shaped shutters in the NILS beacon, it 

is possible to provide a curved flight path and to 

incorporate a flare before touchdown 
108 

3<5 HZ 90 HZ 

24 HZ 60 HZ 

BtAm FORMATION 

(C) 

( A ) 

(. DOWN-RANGE 

BEACONS 

FENCE OR EKCLUSION 

AREA 

f 

Hli i MCnVIS IIOCK Ot«@t*M 

m £C OS 

l e ; 

L„ 

ftsetKNCv 

?3 

ES1^CTQ« 

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-

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r^ 

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'"a^sEiy 

IS NOlCATOIf 

Nuclear Instrument Landing System. 

Plan for Next Period 

Phase 11 was started in July 1971, and will result in 

construction and flight-test demonstration of a complete NILS 

Reports Published 

Phase I Final Report, October 2, 197! 

Estimated Date of Final Report 

Not estimated 

NEUTRON RADIOGRAPHY 

WITH CALIFORNIUM-252* 

Objective of Work 

The objective of this program is to develop and apply 

low flux neutron radiography with Cf 252 as a neutron 

source The portable shield and exposure facility that 

evolved from earlier work are being made more portable 

and efficient Fast neutron radiography will be explored 

further Low flux imaging techniques will receive em 

phasis A position sensitive proportional counter is 

being developed to give instantaneous readout of data 

that represent the imaged objects Various converter 

foils and films are under study as means to radio 

graphically record images 

Progress and Results 

The first neutron source holder (NC 1) was evaluated 

and a second source holder and exposure system were 

developed The second unit (NC 2, see first figure) has 

the same egg shaped Fiberglass shell used m NC 1, but 

*K L Svimth Battelle Pacific Norttiwest Laboratory Rich 

land WA99352 Contract AT(45 1) 1830 
109 

WATER FILL AND VENT TUBES 

FIBERGLASS SHELL COLLIMATOR 

Sketch of the NC-2 source holder designed for ease of 

positioning. 

PLASTI C FOR SOURCE SUPPORT 

?-^ 

Position-sensitive counter for imaging in thermal-neutron fields. 
110 

the internal moderators were replaced with water. Thus, 

the weight that must be handled when the facility is 

positioned is only that of the shell and miscellaneous 

hardware (75 lb); the NC-1 weighs 350 lb. After the 

unit is positioned, it is filled with water and the source 

is installed. To facilitate the handling of large sources, 

this procedure could be done remotely. This unit has a 

fixed collimator with a length-to-diameter ratio of 15:1; 

however, other collimators can be installed. The thermal flux at the face of the unit is 9.4 X 10^ n/cm^ -sec, 

the cadmium ratio is 1.8, and the neutron-to-gamma 

ratio is 4.2 X lO" n/cm^-mr. Radiographs produced 

with this unit are better than those produced with 

NC-1. With NC-I in a position where the geometrical 

unsharpness is cosnparable with that of NC-2, the 

thermal flux is 2 f X 10^ n/cm^ -sec and the cadmium 

ratio is 1.45. 

Direci imaging m low-flux beams can be performed 

satijf;, 'oiily with standard techniques, such as the use 

of i J lir.ium foils; however, use of the fastest techni(: ^ Tossible is desiiable. Gadolinium oxysulfide and 

f!" tics-coupled Lif6)F' /nS(Ag) have been investi-

? . means to enhance the resolution and sensi-

: .. lie gadolinium oxvMilfide screens with Kodak 

'X %i. Slue film are mucli faVic than gadolinium metal 

• ^ils, but Li(6)F--ZnS scinSiiators are still the fastest 

leans. Although the i-.solution achieved is better than 

•at v/iih Li(6)F—ZnS scintillat(.is, the gamma discrimii.ition is not as good. The piimary emission peaks of 

gadolinium oxysulfide are above 4800 A, which suggests the use of a green-sensitive film such as Kodak 

Type O. Comparison of the foil with Type O and Royal 

Blue films showed that the Royal Blue film is faster. 

Fiber-optics face plates in conjunction with 

Li(6)F—ZnS scintillators were studied as a means to 

increase the resolution obtainable wilh Lif6)F-ZnS 

scintillators. Because of light attenuation in the fibeioptics face plates, this technique increased the requited 

exposure time 50 to 400%, the increase depending on 

the fiber optics used. The resolution and contrast of 

neutron radiographs made by this technique were 

improved. 

Proportional counters that have the ability to read 

out the position of interaction of radiation are being 

investigated for imaging thermal neutrons Their use 

will result in a device that can determine neutron 

transmission with resolution in the range 0.5 to 1 mm. 

The information will be stored in digital form. The 

preliminary results with this counter are promising. The 

second figure shows the prototype counter, which is so 

designed that the gas pressure, degree of coUimation, 

converter foil, and anode-to-cathode spacing can be 

varied to determine their effects on imaging. The 

counter now has a geometrical unsharpness of ~3 mm. 

Plan for Next Period 

Information derived from the prototype imaging 

counter will be used to fabricate a large-area device for 

further evaluation. Investigations will continue on the 

counter, image intensifiers, and foil-film techniques to 

optimize imaging in low-flux neutron beams. Techniques and source holders will be developed for 

fast-neutron imaging in beams from Cf-252 sources. 

Reports Published 

J. L. Cason, Design and Fabrication of a Portable 

Device for Neutron Radiography, USAEC Report 

BNWL-1329, March 1971. 

C. B. Shaw and J. L. Cason, Portable Neutron Radiographic Camera Using Californium-252, Mater. 

fra/., 29(2): 40-4 (1971). 

K. L. Swinth, Developments in Low-Flux Neutron 

Radiography at Battelle-Northwest, Trans. Amer. 

Nucl. Soc, 14(2): 516-7(1971). 

Estimated Date of Final Report 

Continuing project. 

INDWELLING INTRACRANIAL 

PRESSURE SENSOR* 

Objective of Work 

The basic objective of the Intracranial Pressure Sensor 

(IPS) Program is to demonstrate the feasibility of a 

fully implantable, long-term, intracranial pressure sensor using a radioisotope to transmit a pressure signal 

without the use of signal leads. The IPS unit is intended 

primarily for the use in hydrocephalic children. 

Progress and Results 

The device employs three fluid chambers, of which 

two contain a radioactive fluid to give the pressure 

reading. The IPS device is presented in the figure. 

Chamber one contains an inert fluid and is implanted 

within the cranium so as to be exposed to the 

intracranial pressure. The pressure is transferred to the 

second chamber, which has rigid walls and a flexible 

*T. S. Bustard, Hittman Associates, Inc., 9190 Red Branch 

Rd., Columbia, MD 21043, Contract AT{ll-l)-3206. 
I ll 

Indwelling, intracranial pressure sensor. 

diaphragm. A radioactive fluid is contained in the upper 

portion of the second chamber. Radioactive fluid above 

the diaphragm is displaced into a third chamber, which 

also contains a flexible diaphragm. It is this displacement of radioactive fluid that serves as a measure of the 

intracranial pressure. 

Americium-241 emits a 59-keV gamma ray such that 

the quantity of radioactive fluid in the third chamber 

can be monitored from above the scalp by a scintillation detector. The quantity of fluid in the third 

chamber is directly related to the intracranial pressure. 

The initial effort on the program has included 

selection of a suitable radioisotope, selection of an inert 

fluid and radioisotope form, and materials selection 

such that they will be compatible with body tissue. 

Detail design has been completed and components 

fabricated for assembly. Initial bonding studies have 

also been completed. 

Plan for Next Period 

The components fabricated during the initial period 

will be assembled. Fabrication procedure will be developed by the assembly of a unit completely filled with 

an inert fluid to determine filling procedure and 

possible problem areas. After assembly procedures have 

been developed, a unit that contains an Am-241 salt 

solution will be assembled and tested. Both static and 

dynamic pressure testing are planned. 

Reports Published 

None. 

Estimated Date of Final Report 

February 1972. 

PROCESS RADIATION 

i^-

\ 

. % 

Glass polymer composite material 

Process 

The Process Radiation Program is concerned with the 

preparation and processing of products employing 

radiation as an energy source to effect chemical, 

physical, and biological change The primary objective 

IS the development of technology necessary to advance 

large-scale uses of radiation important to the national 

economy Food preservation by irradiation is not 

included in this program 

The process radiation effort is divided into three 

categories radiation synthesis of chemical products, 

modification of materials, and radiation technology 

area support New and promising synthesis systems are 

investigated in the first category, and composite ma 

terial development and grafting methods are investigated in the second category The third category 

includes the acquisition of a broad base of radiation 

technology useful to industiy and encompasses dosimetry studies, design and evaluation of radiation sources, 

and engineering development for radiation energy utilization 

Three BNL projects related to the food irradiation 

program are given in this section 

Portable Irradiator Support, 

adiation 

Field Dosimetry Standardization, and 

General Engineering and Technical Assistance 

To be supported, a concept of the proposed process 

should offer a unique advantage in the use of ionizing 

radiation or indicate a cost less than that ot the 

competitive process currently in use Unique advantages 

in the use of ionizing radiation include one or more of 

the following 

Low-temperature initiation of a chemical or polymerization reaction 

Solid-phase initiation of a chemical or polymeriza 

tion reaction 

Production of a product with no catalyst impurities 

Control of the reaction rate in exothermic processes 

by varying the dose rate 

Irradiation of material either in its final container or 

in Its final shape 

Initiation of a reaction that cannot be brought 

about by other means 

115 

117 

CONCRETE-POLYMER MATERIALS* 

Objective of Work 

The objective of this project is to develop concretepolymer composites for use as improved materials of 

construction. Current program priorities are: 

1. Developing systems for yielding optimal product 

quality and process technology at minimal cost. 

2. Providing information and obtaining an understanding of the major factors that control the 

physical, chemical, and mechanical properties of 

concrete—polymer materials. 

3. Obtaining an understanding of the fundamental 

nature of concrete and concrete—polymer materials 

through theoretical and experimental studies. 

4. Aiding in the transfer of laboratory techniques and 

materials development to potential full-scale applications. 

Progress and Results 

Three distinct types of materials are being investigated in the concrete polymer materials program. 

These are (1) polymer—impregnated concrete (PIC) 

precast portland-cement concrete impregnated with a 

monomer that is subsequently polymerized in situ; (2) 

polymer—cement concrete (PCC) - a mixture of water, 

Portland cement, and aggregate to which a monomer is 

added and is subsequently polymerized after pouring of 

the mix; and (3) polymer—concrete (PC) an aggregate 

mixed with a monomer that is subsequently polymerized after pouring. 

In general, all of the composites show significant 

improvements in strength and durability. Monomers 

currently being tested for normal-temperature applications are concrete with methyl methacrylate (MMA), 

styrene, methyl methacrylate-10 wt% tnmethylolpropane trimethacrylate (TMPTMA), acrylonitnle, chlorostyrene, and 90 wt% styrene- 10 wt% polyester. The 

MMA- impregnated concrete has given the best results. 

*B Manovvitz, M Steinberg, L E Kukacka, and P. Colombo, 

Brookhaven National Laboratory, Upton, NY 11973, Contract 

Al(30-2)-GEN-16 This project is jointly supported with the 

US Bureau of Reclamation, Office of Saline Water, Federal 

Highway Administration, and Bureau of Mines. Cooperative 

efforts are also in progress at the Naval Civil Engineering 

Laboratory, Port Hueneme, CA, Army Corps of Engineers 

Construction Engineering Laboratory, Champaign, IL, and with 

the American Concrete Pipe Association 

The Strength improvements appear to be a function of 

polymer loading, and radiation polymeiization gives 

slightly better strength properties than thermal-catalytic 

polymerization. Improvements in durability appear to 

be mainly a function of polymer loading and effectiveness of sealing the surfaces of the concrete. 

A number of preparation variables, including concrete 

composition, drying temperature, curing time, and age 

at test, were investigated. The age of concrete at 

impregnation or its initial strength does not appear to 

significantly affect the ultimate strength. 

The potential application of concrete—polymer composites as a material of construction for desalting plants 

IS being evaluated. Two monomer mixtures - 60 wt% 

styrene-40 wt% TMPTMA and 90 wt% diallyl phthalate (DAP) 10 wt%MMA have been studied in detail. 

Stiuctural properties such as compressive strength, 

Poisson's ratio, modulus of elasticity, tensile splitting 

stiengths, creep, and steel rod pullout strengths have 

been measured at temperatuies up to 290°F. The 

resistance to chemical attack by hot brine and distilled 

water is also being determined. Based upon these tests, 

the 90 wt% DAP-10 wt% MMA system was found to 

be unsatisfactory. Other candidate materials are currently being surveyed. 

Significant advances have been made with PC. Monomers and monomer mixtures investigated include MMA, 

styrene, acrylonitnle, MMA-TMPTMA, polyester 

styrene, and styrene- TMPTMA. With the use of silane 

coupling agents to obtain bonding between the organic 

and inorganic phases, and the use of graded aggregate to 

obtain minimum void volume, compressive strengths as 

high as 20,000 psi have been obtained for samples 

containing 6 wt% polymer. 

Only limited success has been achieved with PCC 

because of the inherent incompatibility of organic 

monomers with water and alkaline inorganic silicate 

cement materials. 

A number of potential applications tor concrete 

polymer materials are being evaluated as part of 

cooperative programs with other governmental agencies. 

The field testing of impregnated sewer pipe by the 

Water Utilities Department of the City of San Diego has 

been continued but data are not yet available. Ten 

additional lengths of 8-in.-diameter by 4-ft-long pipe 

have been impregnated and will be installed at San 

Diego during the current year. Laboratory tests are 

being performed at BNL. Compared with controls that 

failed after 17 days (25% weight loss), pipe impregnated 

with polyester—styrene has shown no attack after 

exposure to 5 wt% H2SO4 for 60 days. 
118 

The initial stage of a cooperative effort among the 

American Concrete Pipe Association, USAEC, BNL, 

and the Bureau of Reclamation to determine the value 

of concrete—polymer composites for pipe applications 

has been completed Test results showed a sutficient 

improvement m strength from both the three-edge 

bearing and the hydrostatic tests to warrant further 

investigation This work is in progress 

Experiments are being performed m conjunction with 

the Federal Highway Administration to determine the 

feasibility of using concrete—polymer materials for 

highway applications To date, these studies indicate 

potential applications in bridge decks and other structural elements 

Plan for Next Period 

Development of concrete—polymer materials will be 

continued Emphasis will be on the development of 

process technology and the transfer of laboratory 

techniques and materials development to potential 

full scale applications 

Reports Published 

M Reich and J M Hendrie, Report on Polymer 

Concrete Applications Development for the Bureau 

of Public Roads Design Studies on Highway Bridge 

Decking and Luminaire Supports, January 1969— 

June 1970, USAEC Report BNL-15139, August 

1970 

J T Dikeou,W C Cowan, G W DePuy, W G Smoak, 

G B Wallace, M Steinberg, L E Kukacka, A 

Ausiiern, P Colombo, J M Hendrie, and B 

Manowitz, Concrete-Polymer Materials, Third 

Topical Report, USER Report REC-ERC-71-6 and 

USAEC Report BNL-50275, January 1971 

L E Kukacka, P Colombo, M Steinberg, and B 

Manowitz, Concrete-Polymer Composites, Journal 

of the Structural Division, ASCE, September 1971 

Estimated Date of Final Report 

Fourth topical report scheduled for January 1972 

DEVELOPMENT OF 

CONCRETE-POLYMER MATERIALS* 

Objective of Work 

The Bureau of Reclamation and Brookhaven National 

Laboratory are engaged in a joint program to develop 

concrete—polymer composites for use as new materials 

of construction The program objectives are (1) development of process technology for economic production 

of a uniform material having exceptionally high 

strength and durability properties, (2) investigation of 

the physical, chemical, and mechanical properties, and 

the fundamental nature of the materials, (3) evaluation 

of these materials and transfer of the laboratory 

technology to potential full scale production apphca 

tions, and (4) development of reliable design and 

construction criterions 

The work sponsored by the USAEC is directed 

primarily to the production of materials for normal 

temperature applications and preferably to using radia 

tion-imtiated polymerization The work sponsored by 

the OSW IS directed to development of materials for 

saline-water desalting plants, these materials must be 

capable of withstanding exposure to concentrated 

brines and distilled water at high temperatures 

Progress and Results 

Three distinct types of materials for normal tempera 

ture apphcations are under investigation (1) polymerimpregnated concrete (PIC) — precast portland-cement 

concrete impregnated by a monomer that is subsequently polymerized in situ, (2) polymer—cement 

concrete (PCC) — a premixed combination of portland 

cement, aggregate, water, and monomer, in which the 

monomer is added during conventional concrete mixing 

and polymerized after pouring, and (3) polymerconcrete (PC) — a composite material formed by 

polymerizing a monomer with an aggregate mixture 

The monomers are polymerized by gamma radiation 

and by thermal catalytic techniques 

Investigations to date indicate that the most successful concrete—polymer material for construction is PIC, 

and It is now receiving the major emphasis m the 

program Five impregnating materials are presently 

under test - methyl methacrylate (MMA), MMA plus 

10% trimethylolpropane trimethacrylate (TMPTMA), 

styrene, acrylonitnle, and chlorostyrene In addition, 

there is a continuing survey program to select other 

promising monomers for testing 

All monomers used for impregnation have produced 

improvements in the properties of concrete — MMA and 

MMA—TMPTMA showing the greatest improvements 

Compressive strengths of over 25,000 psi and tensile 

*J T Dikeou, U S Bureau of Reclamation, Denver, CO 

80225, Contract AT(49-11) 3003 This project is jointly supported by the Bureau of Reclamation, Office of Salme Water, 

Washington, DC and Brookhaven National Laboratory 
119 

strengths of 1700 psi (increases of more than 300% over 

unimpregnated concrete) have been obtained. Durability tests still in progress show improvements of 

1000% or more in resistance to 15% HCl and to freezing 

and thawing, and essentially no sulfate attack occurs 

alter an exposure three times as great as that required 

to cause failure in unimpregnated concrete. 

Development work in process technology has included studies on the effects of both concrete-mix 

design parameters and concrete-curing conditions on 

the properties of polymer-impregnated concrete, and 

also on improvements in specimen fabrication and 

polymerization techniques The specimen-fabrication 

Technique may be improved through ehmination of a 

wrapping step. Prehmmary studies have indicated the 

feasibihty of eliminating this step by polymerizing 

under water or by using live steam for thermal—catalytic 

polymerization mside an impregnation vessel. 

Work on PC and PCC has been limited, but the results 

obtained thus far look promising. The PC studies have 

shown that mechanical packing of especially selected, 

sized aggregate has reduced monomer weight requirements from as much as 25% to 5 to 6%. The PCC 

studies are in very preliminary stages. 

Plan for Next Period 

The testing program for evaluating various monomers 

and the properties of PIC will continue. Two new PIC's 

are to be tested one will contain polyester—styrene and 

the other MMA polymerized under water The effects of 

concrete-mix design parameters on properties of PIC 

will be further explored, and new polymerization 

techniques using a promoter—catalyst system will be 

studied. Plans are being made to develop impiegnation 

and polymerization techniques for treating variously 

shaped concrete members, such as large slabs and long 

beams. 

Investigations are continuing with PCC and PC because these materials may have many potential applications if suitable properties and feasible fabrication 

methods can be developed. Mechanical packaging of 

aggregate for PC will be further explored and the 

feasibility of incorporating several acrylic monomer and 

polymer emulsions, and furfural—aniline polymers in 

the concrete mix will be investigated in the PCC studies. 

Reports Published 

J. T. Dikeou, W. C. Cowan, G. W DePuy, W. G. Smoak, 

G. B. Wallace, M. Steinberg, L. E, Kukacka, A. 

Auskern, P. Colombo, J. M. Hendrie, B. Manowitz, 

Concrete-Polymer Materials, Third Topical Report, 

USER Report REC-ERC-71-6 and USAEC Report 

BNL-50275, January 1971. 

Estimated Date of Final Report 

Fourth topical report scheduled for January 1972. 

RADIATION CHEMICAL ENGINEERING* 

Objective of Work 

The purpose of these investigations is to study the 

interaction of the kinetics of radiation-mitiated chemical reactions with phenomenons of radiation physics, 

fluid dynamics, and mass and heat transfer The results 

ot the theoretical and experimental work are useful m 

devising scale-up procedures, in designing irradiators for 

optimum source utilization or optimum product arrangement, and m interpreting radiation-chemical experiments, where chemical and physical processes 

interact. The results should apply to irradiators for the 

radiation mactivation of contaminants in liquids and 

particulate materials as well as to radiation-chemical 

reactors. 

Progress and Results 

Photoactivation is being used in the prehmmary work. 

An experimental study of mixing effects in chain 

reactions is underway. The reaction is the benzoinsensitized bulk photopolymenzation of methyl methacrylate and It IS carried out in a partially illuminated, 

stirred, quartz dilatometer The rate of reaction and the 

molecular weight distribution of the polymer are 

measured as a function of the size of the illuminated 

region and the stirrer speed. The most interesting result 

of these measuiements to date is the finding of a 

bimodal molecular weight distribution. The relative 

amounts of polymer associated with the two peaks and, 

in certain circumstances, the average molecular weight 

vary with stirrer speed and size of the illuminated 

region. 

Two supplementary studies have been started which 

may disclose the origin of the bimodal distributions. In 

the first, experiments designed to reveal the flow paths 

of propagating chains are being performed. The reaction 

vessel IS filled with a monomer containing a photochromic dye (l,3,3-tri-methyhndohno-6'-nitrobenzopyrylospiran), and the vessel is partially illuminated, as 

in the experiments without dye. Under illumination the 

*F B Hill and A C MuUer, Brookhaven National Laboratory, Upton, NY 11973, Contract AT(30-2)-GEN-16 
120 

dye assumes its colored form, which persists after 

illumination for periods of seconds to minutes depending on the temperature Thus the flow pattern of the 

dye as it leaves the illuminated region may be followed 

and is presumably the same as that of the propagating 

chains in photopolymenzation Initial results of these 

experiments include the finding of considerable flow by 

natural convection m the absence of stirring and the 

observation of highly stratified flow patterns at low and 

intermediate stirrer speeds 

The second study is theoretical and is concerned with 

the calculation of the molecular weight distribution in a 

partially illuminated vessel Steady-state kinetics is 

assumed, with free radicals being produced in the 

illuminated region and diffusing into the dark region It 

is reasoned that a bimodal distribution may be associated with the situation m which a high concentration 

of free radicals exists in the illuminated region and a 

low concentration in the dark 

Apparatus has been completed for the study of 

radiation-initiated polymerization m flow systems A 

20-Ci Sr-90—Y-90 hne source of beta particles is used 

on the axis of an annular flow reactor The first runs 

have been made using methyl methacrylate in singlepass flow and in recirculating flow 

A series of experiments has been conducted on a 

gas—hquid radiation-chemical reaction Measurements 

were made of the apparent rate of oxidation of aqueous 

ferrous salfate in the presence of interphase gas—hquid 

transfer of oxygen Oxygen was absorbed by or stripped 

from the hquid phase, and mass-transfer coefficients 

were calculated from the data This study is a forerunner for a later study of gas—hquid chain reactions 

A comparison of the relative advantages of chemical 

and radiation initiation of chemical reactions conducted 

on a large scale is being made Stability and ease of 

control are the characteiistics emphasized Initial calculations have shown a larger region of stable operation of 

continuously stirred tank reactors when using radiation 

initiation. Experimentally, the stabihty of batch radiation-chemical reactors is being studied m a series of 

experiments on the production of poly(methyl methacrylate) sheet by a radiation process 

Plan for Next Period 

Additional work as required will be done on the 

experimental and theoretical aspects of the batch 

photopolymenzation to determine the cause of the 

bimodal molecular weight distributions 

Experimental study of conversion and molecular 

weight distribution in continuous radiationpolymerization reactors will continue 

Calculations of batch-reactoi stability and of the 

effect of dose-rate variation on stability in batch 

reactors will be made Tliese calculations will be used to 

guide experimental work 

Reports Published 

R M Felder and F B Hill, Mixing Effects in Chemical 

Reactors Cham Reactions in Batch and Flow 

Systems, Ind Eng Chem Fundam , 9 360-7 

(1970) 

L H Shendalman and F B Hill, Thermal Ignition and 

Stability of Batch Reactors with Nonuniformly 

Initiated Radiation-Induced Reactions, in Chemical 

Reaction Engineering, pp 449-57, Pergamon Press, 

Oxford, 1971 

H T Chen and F B Hill, Radiation-Induced Polymerizations m Continuous Stirred-Tank Reactors, 

AIChE (Amer Inst Chem Eng j J, 17 933-9 

(1971) 

Estimated Date of Final Report 

Continuing project 

SURVEY EXPERIMENTS 

APPLICATION OF ISOTOPIC 

RADIATION FOR CHEMICAL 

PROCESSINGS^ 

Objective of Work 

The objective of this project is to investigate the 

significant effects of radiation on a variety of chemical 

reactions that have a potential for chemical processing 

application 

Progress and Results 

Effort has continued to center upon the synthesis 

and, more recently, the decomposition ot ozone under 

the influence of ionizing radiation from Co-60 Experiments involving irradiation of carbon monoxide to 

evaluate the G value for carbon black formation and 

irradiation of metal salts in aqueous solution for 

possible reduction to pure metal have also been 

performed 

A detailed study of the kinetics of O3 formation and 

decomposition was continued at temperatures from 27° 

down to — 100°C, dose rates of 0 4 to 4 Mrads/hr using 

Co-60, and pressures primarily at 2 atm The findings 

*R N Dietz and M Steinberg, Brookhaven National Laboratory, Upton NY 11973, Contract AT(30-2) GEN 16 
121 

from this study are 

1 The condition of the walls of a stainless steel vessel 

has a marked effect on the ozone steady-state 

concentration An ultrasomcally cleaned vessel in 

the presence of ultrapure O2 gave a much lower O3 

concentration than one previously exposed to air 

The wall effect was more significant at lower 

temperatures and pressures 

2 With increasing amounts of NO2 (N2O4) adsorbed 

on the wail of a 30-ml vessel, the ozone steady-state 

concentration at a pressure of 2 atm of ultrapure 

O2, a temperature of — 100°C, and a dose rate of 0 4 

Mrad/hr markedly increased 175 ppM O3 with 

- 0 001 mg N2O4, 475 ppM with 0 010 mg, and 

>1600 ppM with 0 39 mg The initial G value 

increased from 6 6 to 9 3 over the same range 

3 The addition of a small amount of sulfur hexafluoride (0 64%) caused the yield—dose curves at 

temperatures above —20°C to exhibit sharp maximums occurring near 1 to 2 Mrads of absorbed dose 

At —60°C, typical yield—dose curves were obtained, 

but the O3 steady-state concentration was fiom 12 

to 36 times that in the absence of SFg 

4 The decomposition of 3 65% O3 in ultrapure O2 was 

studied at 27°C, 2 atm, and 0 4 to 3 5 Mrads/hr The 

rate of decomposition, G (-O3), was proportional 

to the O3 concentration and inversely proportional 

to the square root of the radiation intensity The 

initial G values of O3 decomposition ranged from 

2'700 to 7000 at the conditions given, indicating a 

chain reaction 

In the nuclear industry, it is generally conceded that a 

no-loss radioactive off-gas system is technically feasible 

and most economical through cryogenic processing 

One method proposed involves distillation of the 

off-gases at — 180°C The radioactive xenon and krypton are concentrated in a reboiler containing several 

gallons of liquid O2 A preliminary calculation has 

shown that, depending on the size of the nuclear 

reactor, intensities ranging from 10 to 1000 Mrads/hr 

could be attained Experiments with liquid O2 at 

— 170°C, 15 dtm, and 5 8 Mrads/hr m a 30-ml stainless 

steel vessel have given steady-state O3 concentrations of 

>7 mole % The potential hazard of this mixture was 

demonstrated by an explosion m one vessel, which 

fused pait of the stainless steel Catalysts for destroying 

the O3 m situ are being investigated 

A study of radiation-induced reactions of CO is being 

conducted to find possible ways of utilizing the 6 to 60 

million tons per year of CO currently produced as a 

by-product of the steel industry's basic-oxygen-furnace 

process The radiation and thermal decomposition of 

CO to produce carbon black has been investigated At 

temperatures above 100°C the products are predominantly C and CO2, with the G value for carbon black 

being about 10 

Recent experiments by others have shown that metals 

can be prepared from their aqueous salt solutions by 

irradiation with 2-MeV electrons In a series of experiments using a 25% ferrous chloride solution, suppression of the rate of oxidation of ferrous to ferric iron by 

dissolved O2 was achieved with Co-60 radiation There 

was no indication of reduction to metalhc iron, 

however 

Plan for Next Period 

The study of the formation and decomposition of O3 

will continue and will include the effects of solid 

additives as well as different vessel materials More 

details of the formation of O3 in hquid O2 will be 

investigated 

Other reactions of carbon monoxide will be examined, but reactions of salt solutions in the presence of 

radiation will be terminated shortly 

The treatment of sewage and waste waters with ozone 

has been studied by others in detail, as have the effects 

of radiation on such treatment Ozone in combination 

with radiation will be examined in view of the growing 

awareness ot possible toxicity problems associated with 

chlorine disinfection 

Reports Published 

None 

Estimated Date of Fmal Report 

Continuing project 

COMPOSITE MATERIALS* 

Objective of Work 

The objective of this work is to develop composite 

materials for structural applications from inexpensive 

raw materials and waste products Various aggregates 

are mixed with hquid monomers that are subsequently 

polymerized by either radiation or thermal catalytic 

methods 

•*M Steinberg P Colombo, and A Auskern, Brookhaven 

National Laboratory, Upton, NY 11973, Contract 

AT(30 2) GEN 16 
122 

Progress and Results 

Basic studies have centered on the mixing of silica 

sand of various sizes and stone aggregates with methyl 

methacrylate monomer prior to polymerization 

Samples of Ottawa sand from 20 to 270 mesh were 

used to determine the effect of single size particles on 

packing density The main conclusion was that with 

each sand-particle size used, sand occupied ~60% ot the 

volume ot the packing This was determined by 

measunng the volume of monomei lequired to All the 

voids The compressive strengths of all specimens 

prepared with various single sizes of sand were essentially the same — ~11,500 psi 

Based on both experimentation and theoretical calcu 

lations, d sand mixture was selected that leduced the 

monomer requirements to 10% by volume (5% by 

weight of sand) This mixture consists of sand of mesh 

sizes 170-270, 40-60, 20-30, and of 0 5-in stone in 

weight proportions of 6 1, 10 2, 23 0 and 60 7%, 

respectively For practical purposes, only the four size 

ranges were used With the above sand sizes and 

sand-size distribution, the compressive strength for 

cured specimens requiring 5% by weight of monomer 

was ~11,000 psi 

A simple technique has been developed for prepanng 

composite mixes without use of vibrators, pressure or 

vacuum The aggregate monomer mix is contained m a 

shaped mold, which is placed m a radiation field, after 

curing, the composite is released from the mold 

Various additives such as colorants, flame retardants, 

plasticizers, ultraviolet absorbers, etc , can be mixed 

with the monomer before adding the aggregate 

Effect of Method of Silane Coupling Apphcation 

on Compressive Strength of Polymer Concrete 

Sample 

No 

1 

2 

3 

4 

5 

6 

7 

8 

9 

10 

11 

12 

''Union 

methoxysr 

Compressive 

strength, psi 

13,875 

13,790 

13 800 

L5,750 

15,825 

15,790 

15,900 

16,150 

16,000 

11,200 

10,950 

10,750 

Method of silanization 

l%bywt of silane" blended with 

methyl methacrylate prior to 

contact with aggregate and sand 

Aggregate and sand treated with 

1% silane hydrolyzed m water, 

dned, and contacted with MMA 

Aggregate and sand exposed 

to silane vapor before contact 

with MMA 

No silane couphng agent added 

Carbide A-174 ^aMma-methacryloxypropyltri 

lane 

Silane coupling agents as additives to enhance bonding between the inorganic substrate and organic monomer are under study In particular, 7-methacryloxypropyltrimethoxysilane has been used with methyl 

methaciyldle monomer This bifunctiondl material is 

capable of reacting with and forming covdlent chemical 

bonds between an inorganic substrate, such as sihca, 

and an organic monomer The various methods for 

applying the coupling agent and its effect on compres 

sive strength are given m the table Experiments are 

underway to optimize the method of application dnd 

the concentration of coupling agent required 

A study IS also underway to determine the potentidl 

foi use of solid wastes m structural materials such as 

pipe and building block Initial efforts have included 

visits to various Fedeial and industiial facilities to 

determine raw material availability and product desird 

bihty One potential application - sewer pipe 

employs glass residue or waste as an aggregate and 

requiies only a small percentage of a monomer 

Specimens have been prepared from crushed glass that 

has been screened and graded to provide optimum void 

density for minimum monomer requirements The 

graded glass is placed m a form, and methyl methy 

acrylate containing 1% silane as a binder is diffused up 

through the glass With benzoyl peroxide as a thermal 

catalyst, the monomer m the sample is polymerized 

with heat The resulting product, designated as "Glastic," is impervious to water, resists 5% sulfuric acid 

solution, and has compressive and tensile strengths ot 

16,000 and 1200 psi, respectively Glastic contains 93% 

glass and 7% methyl methacrylate by weight A sample 

of sewer pipe, called "Eco-pipe," has also been produced fiom this material 

Work on development of a ceramic—polymer bone 

substitute of porous AI2 O3 in which the poies are filled 

with poly(methyl methacrylate) is continuing Methyl 

methacrylate is polymerized with Co-60 gamma radiation to avoid possible problems of toxicity from the use 

of a promotor and catalysts A high-pressure mercury 

porosimeter is being used m the development of AI2O3 

ceramics with the appropriate pore size 

Plan for Next Period 

Attempts will be made to optimize the aggregate 

mixture to further lower monomer requirements It has 

been observed that the stone aggregate is the weak link 

in the system, and stronger stone aggregates will be 

tested Work with waste materials will be expanded and 

directed as review of the literature and of the information gathered from plant visits indicates A preliminary 

cost analysis of material applications will be made 
123 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

BASIC AND ENGINEERING STUDIES 

OF RADIATION-INDUCED REACTIONS 

IN THE LIQUID PHASE* 

Objective of Work 

The objective of this work is to explore m depth the 

basic and engineering features of a number of radiationinduced hquid-phase reactions of potential industrial 

significance 

Progress and Results 

The basic aspects of the work have been concentrated 

on the radiation-induced grafting of styrene to polybutadiene in latex form, the polymerization of vmyl 

chloride under precipitating conditions, and the ionic 

polymerization of vmyl ethers 

The grafting of styrene to polybutadiene latex using 

radiation initiation has been studied, together with 

parallel chemically initiated graft polymerizations The 

resulting grafted latexes are of the type used for 

high-impact polystyrene plastics, and the corresponding 

styrene—acrylonitnle grafts form the basis for acrylonitnle—butadiene—styrene (ABS) plastic materials It is 

hoped that the radiation initiation will show advantages 

over chemical catalysis m the efficiency of graft 

formation and m the structure of the graft copolymers 

The results obtained thus far show somewhat parallel 

yields of grafts with the two initiation systems However, preliminary analyses of the graft copolymers gave 

an indication that the grafted side chains are shorter 

and more numerous with the radiation process 

Studies m the radiation polymerization of vmyl 

chloride under precipitating conditions have been continued, in certain nonsolvents, poly(vinyl chlonde) 

(PVC) remains separated as a fine powder up to very 

high conversions A reasonable mechanism for the 

reaction and the detailed kinetics have been elucidated 

The radiation-induced ionic polymerization of superdry monomers has continued to center around the vmyl 

ethers Tertiary-butylvmyl ether and isopropylvinyl 

*V T Stannett and E P Stahel, Department of Chemical 

Engineering, North Carohna State University, Raleigh, NC 

27607, Contract AT(40-1) 4063 

ether have both been polymerized under apparently 

optimum conditions This was estabhshed by the 

square-root dependence of the polymerization rate on 

the dose rate High molecular weight products were 

obtained from both ethers, and it seems clear that the 

molecular weight is governed by a chain transfer to the 

monomer 

Work with isobutylvinyl ether has been concentrated 

on the use of Molecular Sieves for drying to provide 

data for the engineering research The effect of two 

solvents — methylene chloride and diethyl ether — has 

also been studied under these conditions Considerable 

increases in the G values were obtained with diethyl 

ether The polyvinyl ethers seem to be degraded by 

radiation, and some details of this concurrent process 

are now being determined 

The engineering aspects of the work have centered on 

the three separate pilot plants and their backup 

engineering studies Small-scale research pilot plants of 

approximately 8 hters reaction volume have been 

operated for the study of both ionic and emulsion 

polymerization A third system has been under design 

and construction for the bulk polymerization of vmyl 

chloride under precipitating conditions 

Successful operation of the pilot plant for dry ionic 

polymerization has continued with an in-depth study of 

isobutylvinyl ether, both m bulk and in methylene 

chloride solution Engineering analysis has yielded a 

combined chemical—kinetic and flow model that fits 

performance well 

The pilot facility is being converted for processing 

gaseous monomers under continuous medium-pressure 

conditions The initial program is the ionic polymerization of isobutylene, with future work centering about 

copolymer rubbers of this monomer 

Successful operation of the emulsion pilot plant has 

continued after modification to a continuous moderatepressure system for the study of vmyl chloride A 

complete study of parameters of the emulsion PVC 

system employing recycle has disclosed interesting 

interactions that lead to enhanced polymerization rates 

Additional equipment is being constructed for continuous copolymerization of other monomers with vmyl 

chloride 

The design of an integrated pilot plant for bulk 

polymerization of PVC under precipitating conditions 

was completed, and the construction is nearly finished 

The plant is centered about a recirculating two-phase 

reactor, with the discharge product stream being sepa 

rated into PVC and unreacted monomer The use of a 

polymer nonsolvent retards the agglomeration tendency 

and aids in the removal of residual monomer from the 
124 

PVC powder Hydrocyclones and a solvent recovery 

unit are integral parts of the separation systems, making 

the pilot plant design complete with only a vinyl 

chloride continuous feed and a pure powder PVC 

product withdrawal 

Plan for Next Period 

The studies of the radiation-induced ionic polymerization ot the vmyl ethers will be continued and extended 

to copolymerization systems 

The grafting of vmyl monomers to diene polymers in 

emulsion will be extended to acrylonitnle—styrene 

systems (ABS type polymers) 

The vinyl chloride studies in precipitating systems will 

be continued with a search tor more efficient nonsolvents 

The engineering studies will continue, centering 

around the three pilot plant systems described above 

Reports Published 

S Russo and V Stannett, The Mechanism of the 

Gamma-Ray Polymerization of Vinyl Chlonde in 

Bulk I Dependence of the Degree of Polymerization on Temperature and Conversion, Makromol 

Chem , 143 47-56(1971) 

S Russo and V Stannett, The Mechanism of the 

Gamma-Ray Polymerization of Vinyl Chloride in 

Bulk II Polymerization Rates and Kinetic Approaches, AfaA;rowo/ Chem ,\A3 57-66(1971) 

F T Osborne, S Omi, V Stannett, and E P Stahel, 

Radiation-Induced Solution Polymeiization of Styrene m an Engineering Flow System,/ Polym Sci, 

Part A 7,8 1657-74(1970) 

V Stannett, E P Stahel, J Kohler, E Oda, S Omi, A 

Goineau, H P Shah, and F T Osborne, Research 

and Development Studies into the Basic Technology 

of Radiation-Induced Ionic Polymerization Including Small-Scale Pilot Plant Systems, Final Report, 

USAEC Report ORO-3667-1, June 1971 

Estimated Date of Final Report 

Vinyl Chloride in Precipitating Media, Topical Report, June 1,1972 

Emulsion Polymerization of Vinyl Chloride Continuous Engineering Systems, iune, 1, 1972 

RADIATION-INDUCED CHAIN REACTIONS 

IN HETEROGENEOUS SYSTEMS* 

Objective of Work 

The primary aim of this program is to study chemical 

engineering problems associated with the design and 

operation of a system for conducting chemical reactions 

m radiation fields In addition, lelationships between 

the physical and mechanical chaiacteristics of the 

product and the reaction conditions are being developed 

Progress and Results 

The reaction system for grafting gaseous butadiene 

(BD) to polyvinyl chloride (PVC) powder has received 

major interest Factors studied included the effects of 

dose rate, BD concentration, and PVC particle size on 

grafting rate, postirradiation graft yields, and the effect 

of BD solubihty in the grafted polymer The results of 

major interest in the study of grafting of BD and PVC 

particles in a fixed-bed reactor were 

1 Under all conditions the grafting rate increases to a 

maximum of ~10 wt%/hr and then decreases to a 

hmiting steady-state value of ~2 5 wt%/hr The 

limiting value of the reaction rate is insensitive to 

dose rate in the region 1 X 10" to 8 X 10" rads/hr 

However, the maximum graft rate achieved depends 

strongly on dose rate 

2 In the transient region, wet BD grafts at a higher rate 

than does dry BD, but dilution of the BD gas with 

N2 monotonically decreases the graft rate 

The continuous chemical-reactor system for the study 

of heterogeneous reactions employing gamma radiation 

was completed in June 1971 The reactor section in the 

gamma-radiation field is similar to a plug-flow reactor 

This portion of the loop reactor will be analyzed by 

techniques developed for classical plug-flow chemical 

reactors The system has been so designed that residence times mside and outside the radiation field can be 

varied independently Thus, the desired degree of 

grafting can be obtained with a minimum radiation 

dose 

*T G Smith and J Sifverman, Laboratory for Radiation and 

Polymer Science, Department of Chemical Engineering, University of Maryland, College Park, MD 20742, Contract 

AT(40-1 )-4213 [ formerly AT(3 0-1 )-4122 ] 
125 

To determine the effect of process variables on the 

reaction kinetics and the products produced, the 

products must be characterized In the batch studies to 

date, a "weight-gained" measurement has been used to 

determine the degree of grafting This method cannot 

be used foi the continuous4oop reactor because a 

sensitive mass balance is not possible A hnear-densitygradient column was constructed, and polymer produced m batch runs was used to evaluate the efficacy of 

density measurements for determining the degree of 

grafting 

Plan for Next Period 

Demonstration runs will be made on the continuous 

reactor system with the goal of determining how 

reaction conditions — eg , temperature, butadiene 

concentration, dose, and postirradiation grafting time — 

affect the grafted material produced Products are 

expected to be characterized by using a chemical 

method for determining the degree of grafting and 

dynamic mechanical testing and spectroscopic analysis 

to obtain information on the polymer fine structure 

Kinetic models will be developed from these studies 

Reports Published 

I Block and J Silverman, Radiation-Induced Grafting 

of Butadiene to Chlorinated Polyethylene and 

Poly'^Vmyl Chlonde), Trans Amer Nucl Soc , 14 

503 04(1971) 

Estimated Date of Final Report 

Continuing project 

INFLUENCE OF RADIATION UPON 

HETEROGENEOUS CATALYTIC 

SELECTIVITY* 

Objective of Work 

The objective of this work is to ascertain whether or 

not irradiation of a catalyst prior to or during a 

catalytic reaction will enhance the selectivity in complex reaction networks 

Progress and Results 

Irradiation of supported silver catalysts with 7 rays 

from a I2-kCi Co-60 source followed by measurements 

of ethylene oxide yield m the silver-catalyzed oxidation 

0 f 

0 6 

0 5 

0 4 

ENGELHARD! SILVER CATALYST 

IRRADIATED 

_ TEMP=280°C 

REDUCED IN Hj AT 300»C 

REIRRADIATED AFTER 

REDUCTION 

' ^ c 

I I I 

-

~ 

1 

ENGELHARDT SILVER CATALYST 

TEMP = 280 °C 

^ _^ IRRADIATED 

gH NONIRRADATED 

\ 

\ 

0 2 0 3 

CONVERSION 

*J J Carberry and G C Kuczynski, University of Notre 

Dame, Notre Dame, IN 46556, Contract AT(ll-l)-38 

Ethylene oxide yield vs. ethylene conversion for 7-irradiated (Co-60) and nonirradiated Engelhardt supported silver 

catalyst. 

of ethylene was undertaken for two catalysts — a 

commercial AI2O3-supported silver catalyst and a similar catalyst prepared in this laboratory 

To assess the influence of 7 irradiation upon a 

supported silver catalyst, a sample of commercial 

supported silver catalyst was placed in a laboratory 

chemical reactoi, and steady-state values of ethylene 

conversion and yields (A in figure) of ethylene oxide 

and carbon dioxide were measured at a temperature of 

280°C in excess oxygen The sample was removed from 

the reactor and exposed to 7 rays (Co-60) for 10 hr at a 

dose rate of 10'^ eV/g-min The irradiated catalyst 

sample was then returned to the reactor, and measurements of conversion and yield (B) were made as before 

The irradiated catalyst was then reduced m situ in H2 

for 3 hr at 290°C, swept with N2, and then exposed to 

air The reduced and reoxidzed sample was again tested 

for ethylene conversion and yield (C) Then the catalyst 

sample was again removed from the reactor, reirradiated, and tested for conversion and yield (D) 

The data suggest that the influence of radiation on 

conversion and yield, which is eliminated by reduction 

and reoxidation, is obviously reversible since a cycle of 

reduction, oxidation, and reirradiation restores the 

enhancement of yield 

Ethylene conversion and yields of ethylene oxide and 

carbon dioxide for the normal and the irradiated 

catalyst at 280°C both indicate that irradiation of the 
126 

catalyst increases the total conversion of ethylene, does 

not change the yield of CO2, and increases the yield of 

ethylene oxide 

Laboratory-prepared alumina-supported silver catalyst 

containing calcium and Na2S04 as imposed impurities, 

was tested at 240°C for conversion of ethylene and 

yield of ethylene oxide before and after 7 irradiation 

The results were 

Yield of ethylene oxide, % 

Conversion of ethylene, % 

unirradiated irradiated 

10 43 67 5 

20 46 67 

30 44 65 

35 38 62 

As yields of ETO are 60 to 65% with irradiated 

commercial catalysts containing moderators, the significant benefits of irradiation are manifest The data at 

240°C show dramatic improvement of the laboratory 

catalyst by irradiation to give an industrially competitive yield for a "homemade" catalyst 

Samples of ZnO catalyst were prepared for studying 

the dehydration (desired reaction) and dehydrogenation 

of ethanol Catalysts were sintered for different lengths 

of time and temperatures, and under various atmospheres, 1 e , air, hydrogen, and vacuum The catalysts 

were used prior to and after 7 irradiation and over a 

range of reaction temperatures The following observations were made 

1 Irradiation of the catalysts has no effect on dehydrogenation of ethanol 

2 Irradiation of the catalysts enhances the dehydration 

reactions, with the magnitude of the effect depending strongly on previous reduction treatment of the 

catalyst 

3 Enhancement of catalyst activity is completely 

eliminated after the catalyst is heated to about 

350°C in the reaction environment The catalysts 

heated m a reducing atmosphere (irradiated or not) 

behave the same as those heated m air 

Plan for Next Period 

A number of industrially important catalytic reactions need study to determine the influence of 7 

irradiation of the catalyst upon selectivity Dehydration 

selectivity of oxides of copper will be explored, and 

studies will continue on ethylene oxidation over our 

prepared catalysts to define precisely those kinetic 

parameters that are altered by irradiation Experiments 

will be continued to identify alterations in surface 

chemistry 

Other systems of prime industrial importance needing 

study are methanol oxidation over silver, propylene 

oxidation over silver and copper oxide, and xylene and 

naphthalene oxidation over V2OS 

Reports Published 

Because patent application filing on behalf of the 

AEC required withholding of our experimental results 

from the hterature until all patents were filed, only 

recently have papers for publication been prepared 

Estimated Date of Final Report 

July 1972 

RADIATION CROSS-LINKING OF 

POLYMERS WITH SEGREGATED 

METALLIC PARTICLES* 

Objective of Work 

The objective of this project is to optimize conductive 

polymer—metal composites, design economic fabrication techniques, and demonstrate potential applications 

Progress and Results 

During the past two years, the principle of segregated 

conducting networks was estabhshed Conductive polymer—metal composites with low metal loadings are now 

possible Thus 6 vol% of nickel powder (4 to 7 n) m 

poly(vinyl chloride) reduced the resistivity from 10'"* 

to 1 ohm-cm If the networks are formed by random 

mixing, a metal loading of 20 to 30% is necessary for an 

equivalent resistivity 

In essence, the principle is the compaction of large 

polymer particles with much smaller metal particles, 

which leads to a continuous conductive network 

throughout the material (see figure) For example, 

poly(vinyl chloride)—nickel composites were made by 

compacting 150-M polymer particles with S-jd nickel 

particles (10 vol%) at about 120°C under 10,000 psi 

pressure The resulting compacts showed a resistivity of 

about 1 ohm-cm 

*R D Cornehussen, Drexe! Institute of Technology, Philadelphia, PA 19104, Contract AT(30-1)-4216 
127 

A fracture surface of a polyurethane/nickel composite. 

With the development of conductive polyurethane— 

nickel composites, the principle of segregated conductive networks has been shown feasible for all classes of 

polymers — semicrystaDine, glassy, and elastomeric. 

Experience to date has shown that the critical fabrication condition is compaction without shearing. Shearing 

prevents the continuous network formation necessary 

for conductivity. Preliminary work with extrusion, 

rolling, and compression molding with open dies led to 

nonconductive compacts. All these processes may yet 

be used, but considerable modification will be necessary. However, preUminary review of the process 

economics indicates that rapid, semiautomated compression—molding cycles are competitive, particularly 

for small parts. Hence this limitation is probably not a 

serious deterrent to future applications. 

Prototype construction and demonstration of feasibility is critically important to the rapid use of these 

conductive composites. After a series of meetings with 

private organizations to extend this technology, the 

development of a transparent conducting window is 

underway in cooperation with one company and a 

conductive electrical shield for a connector is being 

considered by another. 

This process has been extended to polyurethane 

composites. The difficulty with these rubbery materials 

is the movement of the metal particles into the soft 

polymer rather than forming a continuous network. 

This was prevented by polymerizing a glassy polymer 

within the polyurethane particle before compaction. 

The conductive polyurethanes were obtained by the 

following two-step process. 

1. Irradiation of polymer powder and monomer with a 

1-Mrad dose. Polymer powder is stabilized by 

polymerizing the allyl methacrylate within the polyurethane matrix, thus preventing metal penetration 

during compacting. 
128 

2. Irradiation of compacted polymer-metal composite 

with a 14-Mrad dose. Metal powder is mixed with 

the treated polymer particles, compacted, and then 

irradiated, increasing the gel content and hence the 

strength. 

Plan for Next Period 

The next phase of work involves definition of critical 

fabncation conditions, cost analysis, optimization of 

properties, and demonstration of applications. Further 

attempts will be made to extend this technology to 

interested parties in industry. Attempts will be made to 

convert the batch process of preparation to a continuous preparation method. 

Reports Published 

R. P. Kusy and D. T. Turner, Electrical Resistivity of a 

Polymeric Insulator Containing Segregated Metallic 

Particles,yVafwre, 229. 58-9 (Jan. 11, 1971). 

A. Mallians and D. T. Turner, Influence of Particle Size 

on the Electncal Resistivity of Compacted Mixtures 

of Polymeric and Metallic Powders, / Appl Phys , 

42 614-18(1971). 

R P Kusy and D. T Turner, Radiation Chemistry of 

Polymers Studied by Depression of Melting Temperature, 7kf«cromo/ecMte, 4' 337-41 (1971) 

R. P. Kusy and D T. Turner, Increased Energy 

Deposition m a 7 Irradiated Polymer via a Metallic 

Microphase, MacromofecM/es, 4. 266-68 (1971). 

Estimated Date of Final Report 

Report of work from June 1, 1971 to July 31, 1972 

will be submitted September 1972 

ELECTRON AND X- AND 

GAMMA-RAY RESEARCH FOR 

RADIATION PROCESSING* 

Objective of Work 

The objectives of this project are (1) to perform 

experimental research and development on methods of 

measurement of electron and x- and gamma-ray dose 

distributions m materials of interest m practical radiation processing, (2) to continue development of radiochromic dye dosimeters as accurate and precise measurement devices for radiation doses between 10^ and 

10* rads and as quahtative indicators for dose levels in 

*W L McLaughhn, National Bureau of Standards, Washington, DC 20234, Contract AT(49-2)-1165 

this range, (3) to evaluate, develop, and make available 

new radiation measurement techniques for specific 

apphcations by radiation-process users; and (4) to 

coordinate this work with associated theoretical and 

experimental projects (funded separately) of the National Bureau of Standards, Center for Radiation 

Research. 

Progress and Results 

During the past year extensive dose-distribution 

studies were made with particular emphasis on radiation-processing geometries involving electron beams of 

0.3 to 10 MeV. Target geometries included semiinfimte 

and finite slabs of one material and of more than one 

material, so that dose distributions across the interface 

of two materials could be investigated. The effect of 

various angles of incidence was also studied. The results 

show that experiments using thin radiochromic-dye 

films give results that agree well with theoretical 

calculations, even close to interfaces between materials 

of widely differing atomic numbers, e.g., plastic and 

gold. Since the response of the dosimeters does not vary 

with dose rate, energy, temperature, etc., the present 

Monte Carlo calculations may be considered to be 

500 600 700 

WAVE LENGTH, nm 

Spectrophotometer traces of the radiochromic dye solutions 

for Co-60 7-ray doses from 0 to 100 kilorads. 
129 

sufficient for indicating dose distributions with electron 

beams and x and gamma rays in complex geometries 

New radiochromic-dye dosimeters were developed for 

monitoring profiles of high-intensity beams These 

include inexpensive impregnated papers and "grainless" 

white plastic tilms, which give a permanent highresolution image of the radiation field Also, the 

development of liquid dye dosimeters (see figure) for 

use in radiation measurements for insect population 

control, food shelf-hfe extension, mutation breeding, 

blood inadiation, etc , has been completed The response range of the hquid systems is now from 1 to 

1000 krads, and, because of ease of handhng and good 

reproducibihty, they have distinct advantages over the 

ferrous sulfate dosimeter The film, paper, and liquid 

dosimeters are now commercially available 

Several types of calorimeters of various materials 

(carbon, aluminum, copper, etc ) have been fabricated 

for calibrating the response of thm-film dosimeters for 

industrial radiation-process users and radiationchemistry experimenters These calorimeters can be 

used either m air or m vacuum and in high-intensity 

pulsed or continuous radiation fields The first draft of 

an ASTM standard method of test for thm-film dosimeters has been written A simple thm-film dosimeter 

package has been devised, matching the geometry and 

response of biological test samples (radiation-resistant 

bacteria) for precise radiation-stenhzation calibrations 

A calib ation system has been developed for dose and 

dose-rate studies of thin dosimeters, specifically calorimeters and dye films, that are exposed to monoenergetic-electron and to high-intensity, pulsed electron 

beams Basically, a measurement is made of energy 

deposition by a perpendicularly incident electron beam 

m a thm layer of a homogeneous medium The primary 

dose-measuring device is a thin aluminum calorimeter 

Compansons of the response of the system with 

electron-transport calculations by Berger and Seltzer 

have shown good agreement tor incident monoenergetic 

beam energies of 0 5 to 1 0 MeV 

Several old and new dosimeter systems were evaluated 

for their response characteristics (energy dependence, 

dose-rate dependence, temperature dependence, response range, and reproducibihty) These included clear 

Perspex, dyed Perspex, blue cellophane, several commercial dye films and papers, cellulose acetate, cellulose 

acetate butyrate, polycarbonate, and thermoluminescence systems 

The holographic interferometer, previously developed 

for three-dimensional dose-distribution studies of 

pulsed broad-spectrum electron beams, has now been 

used with monoenergetie electron beams Current investigations show that this device can be used to determine 

the average spectrum of a beam during a single pulse A 

two-beam interferometer has also been built to measure 

energy imparted duiing the irradiation of a water 

absorbei This device can be used for doses as low as 10 

krads and can be used with either pulsed or continuous 

beams The latter instrument was also used as an 

accurate nontactile thickness gage, measunng to about a 

wavelength of light 

Two high-resolution scanning photometers were designed and built for use in evaluating dose-distribution 

images in radiochromic films One of these instruments 

IS a scanning microdensitometer for use with transparencies, and the other is a scanning microspectrophotometer for use with both reflecting and transparent 

mediums 

Plan for Next Period 

Project terminated 

Reports Published 

W L McLaughlin, E K Hussmann, H Eisenlohr, and 

L Chalkley, A Chemical Dosimetei for Monitoring 

Gamma-Radiation Doses of 1 — 100 krad, Int J 

Appl Radiat Isotop ,22 135-40(1971) 

M Rosenstein, Electron Depth-Dose Distribution Measurements in Polystyrene, Doctoral Dissertation, 

University of Maryland, 1971 

W L McLaughlin, M Rosenstein, E K Hussmann, and 

J J Lantz, Jr , Scanning Densitometer for Continuous Recording of Spectral Transmission Density at 

Low Spatial Contrast,/ Res Nat Bur Stand , Sect 

CIS 23-7(1971) 

M Rosenstein, W L McLaughlin, and J Silverman, 

Energy Deposition of Electron Beams m Insulating 

Materials, in Conf Proc Electron and Ion Beam 

Science and Technology, Fourth International Con 

ference, Los Angeles, CA, May 1970, pp 591-604, 

R Bakish (Ed), The Electrochemical Society, 

1970 

E K Hussmann and W L McLaughhn, Dose-Distnbution Measurement of High-Intensity Pulsed Radiation by Means of Holographic Inteiterometry, 

Radiat Res ,47 1-14(1971) 

M Rosenstein, H Eisen, and J Silverman, Electron 

Depth-Dose Distribution Measurements m Polystyrene as a Function of Angle and Thickness, 

Trans Amer Nucl Soc , 14 397-98 (1971) 

H Eisen, Electron Depth-Dose Distribution Measurements in Metals and Two-Material Slabs, Doctoral 

Dissertation, University of Maryland, 1971 
130 

M J Berger, Distribution ot Absorbed Dose Around 

Point Sources of Electrons and Beta Particles m 

Water and Other Media, / Nucl Med , 12, MIRD 

Suppl No 5 7-23 (March 1971) 

M J Berger, Energy Depositions by Low-Energy 

Electrons Delta-Ray Effects m Track Structure and 

Micro-dosimetric Event-Size S-pQctxa, Proceedings of 

3rd International Symposium in Microdosimetry 

Stresa, Italy, October 18-22, 1971 

M J Berger and S M Seltzer, Absorption of Electron 

Energy m Multilayer Targets, Trans Amer Nucl 

Soc , 14 887-88(1971) 

Estimated Date of Final Report 

Open literature pubhcations 

HIGH INTENSITY RADIATION 

DEVELOPMENT LABORATORY 

OPERATIONS* 

Objective of Work 

The objective of this pioject is to use the appropriately staffed, equipped, and maintained facilities at 

the High Intensity Radiation Development Laboratory 

(HIRDL) in preparing sources, loading and modifying 

portable irradiators, intermittently or continuously 

irradiating large and small samples, providing reference 

gamma fields for dosimetiy standardization, and devel 

opmg radiation—engineering techniques and standards 

Progress and Results 

At present the HIRDL inventory includes 1 9 X 10^ 

kCi of Co-60, 66 kCi of Cs-137, and 38 kCi of Sr-90 

Approximately 300 kCi of the Co-60 is being used in 

the Gamma Facihty Operations in the Gamma Facility 

totalled 35,667 hours of irradiat'on time given to 1,473 

samples m 632 separate irradiations Dose rates presently available in this facihty range from 3 X 10^ R/hr 

to8 5 X 10* R/hr 

In a continuing program to upgrade the capability of 

the irradiation cell, a new elevator has been installed in 

the irradiation-cell pool to decrease the time necessary 

to modify loading the source plaque for its various 

tasks A stepwise programmer has also been installed on 

the General Mills Model 300 manipulator so that a 

plane 4 5 ft high and 10 ft long can be automatically 

scanned In-ceU support irradiations ranged from pep-

*J S Milau, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-2)-GEN-16 

permint cuttings for the BNL Biology Department to 

monomer-impiegnated concrete pipe 

Preparation-cell usage included inspecting and loading 

96 sources for Pakistan, reclaiming 26 radioactive 

Co-alloy tensile specimens foi use in cdrosion studies, 

upgrading the activity of the Biology Dept s Gamma 

Field Irradiator, inspecting Natick sources destined for 

Penn State, loading and unloading of various sources foi 

the round-robm calibration, and repairing a small 

Cs-137 irradiator foi the Biology Dept 

Maintenance tasks have continued, with the Model-8 

mampulatois requiimg extensive caie A recheck of the 

absolute filters m the cell ventilation system was made 

using an aerosol smoke and dust photometric method 

The system was 99 9% effective in removal of the test 

aerosol 

Plan for Next Period 

Near-capacity operation of the preparation and irradiation cells will be required to accomphsh the research, 

development, and service tasks scheduled No major 

facility changes oi additions are contemplated 

Reports Published 

None 

Estimated Date of Fmal Report 

Continuing project 

RADIATION SOURCE DEVELOPMENT, 

TESTING, AND EVALUATION=^ 

Objective of Work 

The objectives of this project are to develop safe, 

versatile, and economic standard gamma and beta 

sources and to devise appropriate testing, inspection, 

and calculation procedures 

Progress and Results 

The automated pool-air-cychng corrosion apparatus 

was completed, and a trial run showed satisfactory 

functioning An attempt to load about 0 6 MCi of 

Co-60 demonstrated the need of modification of the 

active source holder because of thermal expansion 

effects Long-term automated cychng tests were initiated on high (~400 Ci/g) and normal (~80 Ci/g) 

*J I Wagner, Brookhaven National Laboratory, Upton NY 

11973, Contract AT(30-2)-GEN-16 
131 

intensity cobalt sources and on inactive dummy 

sources, which are adjacent to and irradiated by active 

cobalt and cesium sources. The inactive sources, which 

have experienced the same corrosion conditions as the 

active sources, can thus be examined in the laboratory 

without radiation hazard. 

Testing of potential cladding materials and corrosion 

mechanisms continued at a low level. Internally heated 

dummy sources partially immersed in a very dilute 

aqueous solution (saturated with Pyrex) showed extremely rapid build-up of solids at the source surface/Uquid/vapor interface at a solution temperature of 

90°C. 

Analytical calculations and experimental measurements have begun in a study of the relative characteristics of irradiators containing Cs-137 and Cs-134 

sources. The purpose of this work is (1) to compare 

analytical and experimental results obtained with pure 

Cs-137 and Cs-134 sources as well as with sources 

containing a known mixture of the two isotopes; and 

(2) to compare relative benefits of the two isotopes in 

thick- and thin-target irradiations in two-pass and 

multipass irradiator systems and in thin-rectangular and 

thick-cylindrical source-element geometries. 

The following progress has been made: 

1. Two sets of sources were designed (fabricated by 

ORNL): one set was of the typical BNL flat type (V4 

in. thick) and the other set was a thick (1.0 in. 

diameter) cylindrical type. Each set contained three 

sources: one with pure Cs-137, one with pure 

Cs-134, and a third with half of each. Each source 

activity was less than 2 Ci. 

2. An automatic programmed x-y-z positioner was 

designed, constructed, and installed for use in the 

HIRDL irradiation cell (see figure) and made use of 

the existing heavy-duty General Mills arm in that 

cell. 

A thorough review of the technical and economic 

aspects of, and future prospects for, separated fission 

product radioisotopes was prepared by the Division of 

Isotopes Development, using AEC staff and contractor 

input. Participation by BNL involved primarily the 

Programmed movement of GM arm automatically exposes instrumented taigets to low level cesium sources in dose distribution 

experiments. 
132 

preparation of economic and application comparisons 

of existing and projected Co-60, Cs-137, and 

Cs-134/Cs-137 sources 

Source standardization activities are discussed under 

the "General Engineering and Technical Assistance," 

reported below 

Plan for Next Period 

Experimental comparisons of low-activity Cs-137 and 

Cs 134 sources will be completed Accelerated source 

corrosion testing will continue Response techniques to 

maximum-credible-accident situations involving cesium 

sources, e g , source rupture in a pool, will be developed Strontium source studies will be accelerated 

Reports Published 

J Wagner and A Oltmann, BNL Cobalt Radiation 

Sources, Trans Amer Nucl Soc, 14 498 99 

(1971) 

Estimated Date of Final Report 

Continuing project 

DOSIMETRY AND DOSIMETER 

DEVELOPMENT* 

Objective of Work 

The objectives of this project are to devise, impiove, 

and evaluate dosimetry methods apphcable to largescale irradiators, to consult and render assistance to 

USAEC contractors, and to cooperate with AEC contractors, personnel of other government agencies, industrialists, and representatives of educational and 

private institutions in the dissemination and exchange 

of information and techniques 

Progress and Results 

The procedure for use of the ferrous sulfate—cupric 

sulfate dosimeter has undergone several revisions and 

has finally passed the ASTM balloting and been 

accepted for publication as a standard procedure The 

ceric sulfate dosimetry procedure has, after several 

revisions, passed both ASTM Dosimetry Section balloting and Subcommittee D/20 balloting The procedure is 

presently being reviewed by an ASTM editorial committee before final publication as an ASTM standard 

procedure The new procedure for the Fricke dosimeter 

''F X Rizzo, Brookhaven National Laboratory, Upton NY 

11973, Contract AT(30-2)-GEN-16 

has passed Dosimetry Section balloting and, after 

several revisions, has been submitted for balloting m 

Subcommittee D/20 

The long-term studies of solutions of radiochromic 

dye (RCD) c>anide powders have been completed It 

was found that these solutions can be used successfully 

for accurate measurement of absorbed dose in the range 

from 5 to 500 krads Solutions may be stored for six 

months or more if they are protected from ultraviolet 

light Numerous solvents for the dye powders were 

tested - ethoxy ethanol, ethoxy methanol, dimethyl 

sulfoxide, and isopropanol, among others For the work 

at this laboratory the isopropanol was found to be best 

suited with respect to dose-range reproducibility, accuracy, availabihty, and safety Work continues on 

supported and unsupported RCD films as well as on 

impregnated papers 

Tests on a new 1 0-mm-thick ultraviolet-transmitting 

Lucite dosimeter manufactured in Argentina show it to 

be similar to the Perspex-HX dosimeter The nonlinear 

usable total-dose range of this system was found to be 

slightly better than that of Perspex-HX (1 to 5 Mrads) 

The dosimeter bleaches thermally at a rate that is 

temperature as well as total-dose dependent 

Studies were made to test the effects of monomolecular coatings on Perspex-HX dosimeteis The four coatings used were applied by exposing the dosimeters to 

ammonia plasma, carbon dioxide, moist air, and hehum 

The purpose of the coatings was to inhibit oxygen 

diffusion into the dosimeters, which is related to 

postirradiation bleaching No long-term improvements 

were noted for any of the coatings 

A large volume of standard ferric ion solution was 

prepared and standardized for BNL by a commercial 

analytical laboratory Samples of this solution are being 

sent to three commercial laboiatones and three institutions (government laboratories and/or universities) for 

cross calibration Upon completion of standardization 

procedures, the solution will be made available to other 

institutions and commercial companies for spectrophotometer calibration 

Further calibration of the HIRDL Gamma Facihty 

continued m this period, and several new tubes were 

added and calibrated Previous calibrations were rechecked Calibrations were made on all portable iriadi 

ator units passing through HIRDL, including one 

Brookhaven Portable Cesium D'^velopment Irradiator 

(BPCDI) and the Portable Cesium Irradiator (PCI) 

An IAEA Panel of Consultants was assembled in 

Vienna m April, 1971, for the purpose of drafting an 

IAEA Food Irradiator Calibration Manual The first 

rough draft of BNL's contribution to this document has 
133 

been completed. This publication will replace the 

previously scheduled AEC Food Irradiator Calibration 

Manual. 

The Fifth Dosimetry Workship was held in February 

1971, in Goleta, CA, with EG&G as host. The three 

main topics discussed were Radiation Dosimetry in 

Radiation Processing, Dosimetry in Medical Irradiation, 

and Dosimetry in Industrial Machine Irradiation. The 

Workshop was attended by about 80 people from 50 

institutions, approximately one-half being from commercial companies. 

Plan for Next Period 

Arrangements are underway for the Sixth Dosimetry 

Workshop planned for June 1972. The host will be the 

Atomic Research Establishment at Risoe, Denmark. 

The theme will be Dosimetry in Radiation Research, 

and it is expected that dosimetry standards for medical 

products and food dosimetry will receive considerable 

discussion. 

Cooperation with the IAEA and with individual 

foreign laboratories on international dosimetry standards and irradiator calibration will continue, as will 

involvement with ASTM on dosimetry procedures. Beta 

dosimetry, delayed this year, will be emphasized next 

year. 

Reports Published 

F. X. Rizzo, L. Galanter, and K. Krishnamurthy, 

Tabulated Dose Uniformity Ratio and Minimum 

Dose Data for Gamma Irradiator Design, US AEC 

Report BNL-50145 (Rev.), December 1970. 

F. X. Rizzo, L. Galanter, and K. Krishnamurthy, 

Tabulated Dose Distribution Data for Gamma Irradiator Design, USAEC Report BNL-50147 (Rev.), 

December 1970. 

F. X. Rizzo, L. Galanter, and K. Krishnamurthy, 

Tabulated Dose Distribution Data for Gamma Irradiator Design. I. Cobalt-60 Square Plaque Sources, 

Int. J. Radiat. Eng., 1(1): 15-48 (July 1971). 

Estimated Date of Final Report 

Continuin-g project. 

PORTABLE IRRADIATOR SUPPORT* 

Objective of Work 

The objective of this pioject is to ensure the 

operational capability of new and reassigned pool-type 

*P. T. Fallon, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-2)-GEN-16. 

Installing the tank for a Mark IV Research Irradiator in 

Lyallpur, Pakistan. 

and portable research irradiators owned or financed by 

the USAEC. Design, construction, and operation consultation concerning irradiator operation, e.g., source 

handling, and irradiator elements — source elevators, 

conveyors, instrumentation, etc. — will be provided to 

foreign or domestic installations of AEC—DID interest. 

Progress and Results 

Photographs received from Pakistan in early 1971 

showed the tank and tower for the Mark IV pool-type 

Research Irradiator being placed in the ground prior to 

construction of the building to house the unit (see 

figure). When later photographs showed the building in 

the final stage of construction, the final consignment 

was shipped including the isotopic radiation sources 

(25,000 Ci of Co-60). BNL has only one fully approved 

isotope shipping container; since that cask is in periodic 
134 

use tor routine domestic shipments, it seemed unwise to 

release it for the several-month round trip to Pakistan 

One of the old ETR casks*-^ (previously used for 

overseas shipments but currently nonapproved) was set 

aside for the shipment An added advantage of its use is 

that the ETR cask may be left with the irradiator in 

Pakistan tor source storage in the unlikely event of tank 

leakage The Pakistani AEC concurred in this decision 

and, after the understandable delays m gaining formal 

approval from all concerned parties, a Department of 

Transportation Special Permit was issued for the shipment 

Final installation of the irradiator by a BNL engmeei 

will occur in early 1972 This will be followed by a visit 

of a dosimetry expert to assist the Pakistani researchers 

m calibrating the unit 

Shipboard Irradiatoi II, after its short-term use in 

Louisiana and subsequent shipment to Korea, was 

installed in that country by a BNL technician Repair of 

some minor damage suffered in use m Louisiana and in 

shipment was necessary before the unit could be made 

operational Of paiticular concern was the fraying 

observed in the hoist cable The cable was replaced with 

one of finer wire construction which should reduce the 

possibility of a recurrence of this problem 

After thorough testing of the unit and instruction of 

personnel by the technician, the iiradiator was turned 

over to the Korean opeiators 

When the irradiator was being packaged m Louisiana, 

the radiation-monitoring equipment seemed faulty 

Rather than risking the sending of defective instruments 

to Korea, they were returned to BNL, and replacements 

were sent by air freight to Korea 

During routine operation of Shipboard Irradiator 111 

on loan to the University of Nebraska, the hoist cable 

failed A new cable, letained at BNL for emeigencies, 

was sent by air freight to the University, where it was 

installed with the assistance of a BNL engmeei returning from a meeting in California The new c^ble was 

also of finer wne construction such as that installed m 

Korea The unit was examined carefully for additional 

damage but was found to be in excellent condition 

After cleaning, lubrication, and some minor adjustments, the iriddiatoi was returned to operation 

Plan for Next Period 

instdlldtion of the Mark IV Pool Type Research Unit 

in Pakistan will be completed 

**The ETR casks were previously used to ship cobalt sources 

irradiated in the Experimental Test Reactor (ETR) 

Transfer of the Brookhaven Portable Cesium Development Irradiator (BPCDI) No 1 from Argentina to 

Brazil IS planned The Indian AEC has suggested the 

possibility ot moving BPCDI No 2 from Trombay to a 

coastal location 

The Portable Cesium Irradiator (PCI) may be transferred from Its current California location to Louisiana 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

GENERAL ENGINEERING AND 

TECHNICAL ASSISTANCE=* 

Objective of Work 

The objective of this project is to maintain the 

technical cognizance required by the programs con 

ducted at the High Intensity Radiation Development 

Laboratory (HIRDL) or involved in HIRDL consultations Activities include the planning and designing of 

advanced iiradiators, maintenance of source standards, 

assisting of otf-site investigatois, upgrading of on-site 

facilities to meet changing service requirements, and 

continued examining of the extent, nature, and control 

of undesiiable side effects of radiation processing 

Progress and Results 

Technical assistance requests from commercial organizations univeisities, and government or governmentsponsored facilities continued at a high level, most 

involved dosimetry, calibration, and shielding problems 

Irradiator design activity was slight 

Souice calibration and standardization activities were 

transterrf^d to this group during this period Source 

calibration at BNl consists of standardization of a few 

sources by calorimetrv, then using these standard 

sources as leferences to assay the remainder of the 

inventory Both the calorimeter, used for standardization, and the source assayer have been in use at HIRDL 

for many years Recent concern over the existence of a 

truly ddiabatic system in the caloumeter has led to 

extensive modification and testing With these changes, 

*J H Cusack, Brookhaven National Laboratory, Upton NY 

11973, Contract Ar(30-2)-GEN-16 
135 

coupled vi'ith theoretical calculations, it has been 

determined that the system remains adiabatic over 

much more adverse conditions than exist during normal 

operation 

Previous data collected from the source assayer 

relating the activity of an unknown source to that of a 

standardized source were taken from a moving chart 

paper. This technique, and the use of instrumentation 

with a high rate of drift, led in some cases to gross 

errors This problem has been corrected with the design 

and fabrication of highly stable instrumentation containing a digital readout 

A major portion of the effort relating to radiationsource standardization at BNL is in conjunction with an 

interfacihty cross-calibration program, the purpose of 

which IS to set up industry-wide (and, possibly, international) standards The present participants in this 

program are General Electric Co , Neutron Products, 

Inc , Atomic Energy of Canada Ltd , Commissariat a 

I'Energie Atomique (Saclay, France), the Radiochemical Centre (Harwell, England), and Brookhaven 

National Laboratory 

An IAEA-sponsored Consultants Meeting on Source 

Standardization was held in Baden, Switzerland, m 

August 1971 This meeting, an outgrowth of the BNL 

source-standardization efforts, was attended by Enghsh, 

French, German, Swiss, Canadian, and U S (BNL) 

representatives Major emphasis in the resulting consultants report was on source-specification requirements, 

recommendations for future work stressed isodose 

plotting and spectrum-distribution determinations by 

experimental and Monte Carlo calculation techniques 

Plan for Next Period 

Technical-assistance requests are expected to continue A growing interest m the development, production, and use of cesium sources is especially apparent 

Investigation of new irradiator concepts will continue 

Source standardization activities will continue m 

cooperation with the IAEA and with commercial 

organizations 

Reports Published 

None 

FIELD DOSIMETRY STANDARDIZATION* 

Objective of Work 

The objective of this work is to ensure the accuracy 

and reproducibihty of all gamma dose-measurement 

data generated under AEC sponsorship or in support of 

AEC food and process irradiation interests 

Progress and Results 

Dosimetry and/or calibration procedures performed 

by personnel at Michigan State University, Bulk Gram 

Irradiator facility. University of Hawaii (research irradiator), Hawau Development Irradiator (HDI) facility. 

University of Washington, and Bureau of Commercial 

Fisheries at Seattle and Gloucester were reviewed in 

depth 

The dosimetry section of the strawberry petition was 

expanded to include the irradiations performed at the 

University of California in the Portable Cesium Irradiator (PCI) and the Mark II Research Irradiator 

Reviews of the dosimetry sections of the marine 

products petition and the petition for papayas are in 

progress 

Technical assistance in dosimetry, dose calculation, 

and dose standardization was given to several companif^s 

and universities Among the recipients were Gamma 

Processing Corporation, Radiation Technology, Inc , 

Tampa Bay Engineering, University of Massachusetts, 

New York State Atomic and Space Authority, Korean 

Government, Medical Department, BNL, AME, Inc , 

Radiation International, Inc , Brazilian AEC, Argentine 

AEC, Plastics Division, Allied Chemical Corp, US 

Veteians Administration, Neutron Products, Inc , 

NUMEC, and the Radiation Division of BNL 

Plan for Next Period 

Brookhaven National Laboiatory will continue to 

review reports by AEC contractors prior to their 

pubbcation Dosimetry updating or lecalibration will be 

conducted at AEC facihties upon request 

Final drafts of the strawberry and marine-products 

FDA petitions will be completed All other FDA 

petitions will undergo m-depth reviews and evaluation 

before submission 

Estimated Date of Final Report 

Continuing project 

*F X Rizzo, Brookhaven National Laboratory, Upton, NY 

11973, Contract AT(30-2)-GEN-16 
136 

Reports Published 

None 

Estimated Date of Final Report 

Continuing project 

PATENT REVIEW - PROCESS 

RADIATION DEVELOPMENT* 

Obj'ective of Work 

The objective of this search by the Isotopes Information Center (IIC) is to review, categorize, abstract, and 

compile U S , British, and Canadian patent literature 

regarding process radiation to provide backup information for the DID Process Radiation Staff In addition, 

other foreign patents are being included as spinoff from 

the Center's retrieval system 

The audience for this review will include all potential 

manufacturers of materials produced by irradiation as 

well as manufacturers of radiation-processing equipment This review should provide those manufacturers 

with information concerning processes or equipment 

that have been developed and thus reduce the possibihty of patent infringement The review should also be 

valuable to both manufacturers and research and 

development institutions to help direct the effort of 

new work in the field If kept current, this report 

should be a valuable index to the growth of the 

radiation-processing industries 

Progress and Results 

During the last year Part 1 was completed It contains 

information on more than 700 U S patents for the 

years 1950 through 1968 as weU as a partial listing of 

the 1969 and 1970 patents 

*R E Greene, P S Baker and H S Warren, Oak Ridge 

National Laboratory, P O Box X, Oak Ridge, TN 37830, 

Contract W-7405-eng-26 

The subject index, although not exhaustive, contains 

appioximately one thousand terms taken from compounds given in the title, from typical starting mateiials 

and end products, and from basic piocesses (e g , 

synthesis, polymerization) An analysis of the findings, 

from which tiends may be depicted, is included 

Patent cards were leproduced as an appendix to the 

full report and were prepared for all in-scope patents 

Each card contains patent number, country, assignment 

date, apphcation date, priority date, category (process 

or irradiator design), title, assignee, patentee, code class, 

international code class (where applicable), and an 

abstract when available and not prohibited by copyright 

laws When no abstract was available, the U S Patent 

Gazette descuption was used as a substitute When such 

sources were stiU inadequate, pertinent mtormation on 

the radiation application was reproduced from the 

patent itself 

An AEC-generated announcement of the availability 

of the document was made on August 12, 1971 

Plan for Next Period 

Indexing of Part 2, British and Canadian patents, is 

following the same procedure as that for Part 1, and 

subject and assignee indexes will be prepared Patent 

cards will be compiled and listed numerically in an 

appendix to the report The basic report will include 

findings and graphs showing growth and trends 

A 1969 and 1970 supplement to Part 1 is m 

preparation 

Reports Published 

R E Greene, H S Warren, and P S Baker, Patent 

Literature on Process Radiation and Irradiator 

Design Part I United States Patents 1950 Through 

1968, USAEC Report ORNL-IIC-24 June 1971 

Estimated Date of Final Report 

Publication of Part 2 is expected in late 1972 
RADIATION PRESERVATION OF FOODS 

Astronaut Buzz Aldrin demonstrates for the camera how to make a sandwich with 

irradiated bread. Both irradiated bread and bread from irradiated flour have been 

tested satisfactorily on several Apollo flights. (Photo courtesy of Manned 

Spacecraft Center, National Aeronautics and Space Administration, 

Houston, Texas.) 

Radiation Preservation of Foods 

The objective of the Radiation Preservation of Foods 

Program is to develop the process of low-dose radiation 

treatment of food (pasteurization, disinfestation, and 

contiol of pathogens) to the point of commercialization Technical feasibihty and cost-benefit studies have 

identified East Coast finfish, papayas (and mangoes), 

strawberries, shrimp, and mushrooms as being the most 

promising products of all those studied, for these, a 

concerted research and development effort is to continue m order to bring the irradiation process to the 

point of commercialization The majority of the work 

to be performed must necessarily be a direct input 

toward the preparation and presentation of Irradiated 

Food Petitions to the Food and Drug Administration 

(FDA) Since radiation is classified as a food additive, 

all the requirements imposed by the FDA for chemicaladditive petitions are also imposed on radiation processing 

During 1969, the program was reduced because of 

budgetary hmitations, and only that work necessary to 

complete the accumulation of data for the strawberry 

and papaya petitions has been continued There is also 

some work continuing on East Coast finfish, but this 

effort has been reduced until advanced microbiological 

studies are completed and the AEC has reviewed all the 

data The AEC has completed a 2-year animal feeding 

study on irradiated strawberries and is preparing a 

petition to the FDA requesting that a regulation be 

issued allowing unlimited human consumption ot this 

product A second animal-feedmg study with rats and 

mice on irradiated papayas has been completed A 

reproduction study with dogs is scheduled for completion m early 1972, and the petition for papayas should 

be submitted to FDA approximately 6 to 8 months 

later 

The AEC is also completing a technical feasibihty 

study on the use of irradiation in conjunction with 

centralized retad cutting of fresh red meats At the 

present time, any decision to conduct 2-year animalfeeding studies will await the completion of the U S 

Army's feeding study on radiation sterilized beef, which 

IS scheduled for completion within the next 3 years 

The AEC responsibility for this program is divided 

between the Division of Isotopes Development (DID) 

and the Division of Biology and Medicine (DBM), with 

DID responsible for overall program direction, the 

technology and feasibility of the process, and the 

selection of items in the program Once the technology 

has been estabhshed, DBM initiates and conducts the 

necessary wholesomeness and safety studies designed to 

demonstrate that consumption of the irradiated food 

product constitutes no pubhc health hazard A list of 

DBM contracts in this field may be obtained by 

contacting that division directly 

Projects concerned with design and construction of 

irradiators for the food program and with dosimetry in 

all irradiators m the program are also reported in the 

Radiation Processing section of these summaries 

139 

141 

MARINE PRODUCTS DEVELOPMENT 

IRRADIATOR PROGRAM* 

Objective of Work 

The primaiy objective of this program is to conduct 

radiation research on a semicommercial scale to develop 

data that will demonstrate the feasibility of extending 

the shelt life of n radiated tresh seafoods The program 

also provides irradiation services for other Federal, 

state, and municipal agencies or private industry 

Progress and Results 

The procedure developed to attain the minimum 

effective dose is as follows (a) purchase commercially 

produced haddock fillets wrapped in conventional 

cellophane units in 10-lb shipping containers, (b) 

irradiate them to doses of 50 to 250 krads at 

increments of 50 krads, (c) store samples of the 

controls and of each of the five dose levels at 33°F, 

42°F, and 46°F, and (d) analyze the wrapped cellophane packages of fillets at appropriate storage intervals 

for total bacterial count and subject duplicate samples 

to sensory (odor) evaluation 

Haddock caught and processed in January, April, and 

June showed that the minimum effective dose level as 

determined by bacterial counts and odor rejection fell 

between 100 and 250 krads Further testing is necessary 

to establish more precisely the minimum effective dose 

In cooperation with private industry, a study of the 

effects of ionizing radiations at different rates is being 

made The MPDl radioactive source imparts energy at a 

level of about 10^ rads/sec in contrast with the 

ultrahigh rate of 10'^ rads/sec imparted by machinegenerated pulsed electrons The effects of ionizing 

radiation from different sources and at different dose 

rates have been compared before but not to the 

magnitude of dose-rate difference m the current study 

Generally, there is good agreement between the two 

systems with respect to bactericidal effect against 

Bacillus pumilus and Streptococcus faecalis There is a 

difference indicated between the two systems of ionizing radiation with respect to material damage mechanisms in complex molecular structures Adverse chemical effects seem to be more pronounced when caused 

by ionizing radiation of low dose rate (10^ rads/sec) 

than by an ultrahigh (10''' rads/sec) rate Materials 

tested so far include insulin, plasma, enzymes, fibrino 

*J D Kaylor, National Marine Fisheries Service, Atlantic 

Fishery Products Technology Center, Emerson Ave , Glouces 

ter, MA 01930, Contract AT(49-11)-3005 

gen, and detergents A report on the damage due to rate 

effects will be published 

Plan for Next Period 

The plan for the next period is (1) to perform at least 

two more simulated shipping studies to establish the 

minimum effective dose and carry out actual shipping 

studies and (2) to continue to provide irradiation 

services and maintain the MPDI at peak efficiency 

Reports Published 

L J Ronsivalli, J D Kaylor, E J Murphy, R J 

Learson, and M S Schwartz, Studies in PetitionOriented Aspects of Radiation Pasteurization of 

Fishery Products, in Preservation of Fish by Irradiation, Report of a Panel, Vienna, Dec 15-19, 1969, 

IAEA, Vienna, pp 1-11, November 1970 

(STI/PUB/196) 

J D Kaylor, E J Murphy, J H Green, and W S Hill, 

Marine Products Development Irradiator Program 

Irradiated Fresh Shrimp Shipping Studies, USAEC 

Report TID-25543, October 1970 

Estimated Date of Final Report 

Continuing project 

RADIATION PASTEURIZATION 

OF FRESH MEATS AND POULTRY* 

Objective of Work 

The overall objective of this work is to provide a 

technology by which centralized cutting and packaging 

of fresh meats and poultry may be achieved The 

technology will (1) control microbial spoilage by use of 

ionizing radiation plus conventional refrigeration, (2) 

control pigment and lipid oxidation principally through 

effective atmosphere control and packaging as well as 

possible additives such as ascorbic acid, and (3) minimize fluid exudation with drip-controlhng agents Controlhng these deteriorative processes through such an 

integrated procedure will make feasible the complete 

preparation of fresh red-meat consumer cuts and 

poultry at a central location to provide sufficient 

product life to permit distribution to retail outlets 

under refrigeration 

*W M Urbam, Department of Food Science and Human 

Nutrition, Michigan State University, East Lansing, MI 48823, 

Contract AT(11-1 )-1689 
142 

Progress and Results 

The procedure developed through laboratory-scale 

tests to attain the objective is as follows: (a) treating 

the meat with condensed phosphates (e.g., tripolyphosphate) to control liquid exudation and to maintain 

normal red color; (b) packaging each cut in oxygenpermeable film, grouping of a number of such packaged 

cuts, and placing them in a bulk container which is 

sealed under vacuum; (c) irradiating the bulk-packaged 

product at 100 to 200 krads with gamma radiation; (d) 

distributing and storing under refrigeration; and (e) 

opening the bulk container at the retail outlet, at which 

time the normal red color develops and the product has 

a normal display-case Ufe (3 days). 

An attempt to obtain a picture of the microbial 

outgrowth patterns of beef handled according to the 

proposed procedure is in progress, which involves 

examination of the beef for (a) numbers of organisms 

present (both mesophihc and psychrophilic) and (b) 

coliform, Clostridium perfringens. Staphylococcus 

(coagulase positive), and salmonella microorganisms. 

Knowledge of the outgrowth pattern is important 

for characterizing the sensory spoilage which ultimately 

occurs and also for assessing any health hazard which 

might develop. 

The primary purpose of the phosphate treatment is to 

control "drip" (weepage of Uquid) from the meat cut. 

Two methods of incorporation of the phosphate have 

been studied: dipping or spraying a water solution and 

injecting through hollow-needle pumping devices. On 

the basis of similar phosphate additions to certain 

meats, limits of 0.5% added phosphate and 3.0% total 

weight gain (including solvent water) have been set. 

In the final step of the handMng procedure, the meats 

are exposed to air to develop and maintain the normal 

red color. Chemical analyses have determined that the 

oxygen of the air oxidizes the fat present in the meat. 

This is true also of meats as they are now handled. The 

addition of ascorbic acid prevents this oxidation. The 

level of fat oxidation, however, is very low and efforts 

to correlate taste panel evaluations with chemical 

analyses have not established that a flavor change is 

caused by this oxidation. 

Oxygen must be removed from the primary package 

to secure meat color stability. Design of a packaging 

system to accomplish this is being undertaken. 

Plan for Next Period 

Future work will be aimed at completing the microbiological studies, determining the best method of 

phosphate addition, and designing an effective packaging system. Meat handling procedures prior to cutting 

also will be investigated. 

Reports Published 

W. M. Urbain, G. G. Giddings, and W. W. Ballantyne, 

Radiation Pasteurization of Fresh Meats and Poultry, Annual Report, USAEC Report COO-1689-6, 

1971. 

Estimated Date of Final Report 

Continuing project. 

A STUDY OF CONTROL OF PUBLIC HEALTH 

PROBLEMS USING IRRADIATION* 

Objective of Work 

This project was undertaken to determine the impact 

of irradiation on microorganisms of pubhc health 

significance in ground red meat, the behavior of the 

residual microflora during simulated commercial handUng of ground red meat, and the usefulness of 

commonly accepted evaluation systems for public 

health safety in meat products. 

Progress and Results 

Most of the exploration of usefulness was based on a 

low dose application (68 krads), with recognition that 

the ultimate dose level would depend on many factors. 

Various dose levels were apphed when individual factors 

such as the resistance of a specific species of microorganism were to be studied. Pathogens and indicator 

organisms were studied to determine the relative sensitivity of representative species. Ground red meat 

products were chosen because their sanitation is one of 

the major challenges of the industry and because the 

quality of these products seems to be a plateau of 

minimal tolerance by regulatory agencies for public 

health protection. 

Previous data indicated that ground red meat commercially distributed is near the threshold of microbial 

and detectable organoleptic spoilage. Shelf hfe beyond 

the point of retail sales is only 1 or 2 days. Even as 

improved by irradiation, this product does not fit into 

the ultimate goal for maximum pubhc health protection, which would consist of central processing, packaging, and irradiation. Irradiation would make central 

*R. Burt Maxcy, Department of Food Science and Technology, University of Nebraska, Lincoln, NB 68503, Contract 

AT(ll-l)-2038. 
143 

Comparative counts and LD50 values calculated from 

mortality figures of chick embryos 

Treatment MPN per ml 

Plate count per ml 

PCA BGA SSA 

LDso 

(Number 

of cells) 

Unirradiated 2 0 X 10« 1 0 X lO' 9 6 X lO** 3 2 X ID* 0 5 

Irradiated 5 7 X 10^ 6 4 X 10= 3 5 X 10^ 1 6 X 10'' 13 

processing and wide distribution possible through extension of shelf hfe Furthermore, even the low dose of 

68 krads reduces the pathogenic and toxm-producmg 

organisms by 90 to 99%, thus providing a public 

motivation for acceptance of the irradiated product 

During the last year, basic data have been obtained on 

which the generahzations m the preceding paragraph are 

based The applicability of the commonly accepted 

methods for determining salmonellas, cohforms, and 

other members of the Enterobactenaceae was determined Cell injury affects the number of microorganisms recovering on selective media, and the reduced recovery after irradiation is of the same general 

magnitude found when other methods of cell injury are 

involved 

Relative infectivity of irradiated and unirradiated 

salmonella cells was determined using the egg yolk sac 

challenge technique In addition, counts were made 

with most probable number (MPN) technique and plate 

count on plate-count agar (PCA), brilliant green agar 

(BGA), and salmonella-shigella agar (SSA) Data (Table) 

indicate that irradiated cells are less capable of initiating 

growth even in the highly favorable environment of an 

egg yolk sac The fear of increased mfectivity from 

salmonellas after irradiation is therefore unfounded and 

will remain so until some unforeseen data to the 

contrary can be presented 

Since irradiation naturally alters the microflora, the 

nature and significance of the residual microorganisms 

were studied A major share of the residual microorganisms belongs to the Moraxella group, which 

includes Moraxella, Acinetobacter, and perhaps closely 

related genuses Certain of the species were extremely 

radio-resistant Exploratory work on the source and 

significance of these bacteria indicated that they were 

widespread m the various inputs to ground beef In 

ground beef irradiated at 68 krads, the surviving 

members oi the Moraxella group grew slower than other 

types of microflora both at 5°C and at 25°C Thus, 

irradiation does not add to the significance of these 

organisms 

Work on the Enterobactenaceae indicated that there 

are a great number of these contaminants present in 

ground meat The diversity of isolates indicated that 

many of the microorganisms presently associated either 

directly or indirectly with gastro-intestinai disorder may 

have their origin in ground meat products There are 

many diseases caused by food-borne microorganisms 

that might be controlled or eliminated by a reduction in 

the number of microorganisms m products taken home 

Plan for Next Period 

Fundamental studies of radiation pasteurization of 

ground red meat will be continued, with particular 

emphasis on higher radiation doses at the pasteurization 

level 

Reports Published 

N P Tiwar and R B Maxcy, Impact of Low Doses of 

Gamma Radiation and Storage on the Microflora of 

Ground Red Meat,/ FoodSci , 36 833-34 (1971) 

R B Maxcy, N P Tiwari, andC C Anagnostis, S^Mcfy 

of Control of Public Health Problems Using Irradiation, Annual Report, May 1, 1969-Apnl30,1970, 

USAEC Report COO-2038-2, 1971 

Estimated Date of Final Report 

Continuing project 

RADIATION TECHNOLOGY IN CONJUNCTION 

WITH POST-HARVEST PROCEDURES AS A MEANS 

OF EXTENDING THE SHELF LIFE 

OF FRUITS AND VEGETABLES* 

Objective of Work 

The overall objective of this program is to demonstrate the use of radiation m controlling post-harvest 

*E C Maxie, University of Cahfornia, Davis, CA 95616 

Contract AT(11 1) 34, P 80 
144 

Percent Marketable Shasta Strawberries After Irradiation and Shipment 

Shipment 

method 

Truck 

Truck 

Truck 

Truck 

Truck 

Surface ship 

Surface ship 

Destination 

Mmneapohs 

Atlanta 

Atlanta 

Atlanta 

Atlanta 

Honolulu 

Honolulu 

Date 

shipped 

7/16/70 

7/31/70 

8/26/70 

9/17/70 

10/1/70 

8/16/70 

8/21/70 

Dose 

krads 

0 

150 

235 

0 

150 

235 

0 

150 

235 

0 

150 

235 

0 

150 

235 

0 

150 

235 

0 

150 

235 

Before 

shipment 

98 92 

98 54 

98 67 

96 27 

98 40 

97 96 

98 66 

Percent marketable fruit 

On 

arrival 

94 93 

91 97 

9152 

93 66 

95 75 

94 80 

85 26 

88 47 

90 96 

85 01 

91 17 

92 70 

94 43 

95 58 

94 78 

49 98 

92 64 

89 89 

95 51 

97 10 

94 97 

After 3 days of 

simulated storage 

90 31 

91 46 

90 92 

86 67 

93 19 

90 05 

87 59 

86 45 

86 60 

45 63 

81 83 

86 97 

84 49 

92 99 

89 80 

19 66 

80 34 

84 18 

85 26 

87 50 

85 60 

disease of selected fruits and vegetables Work performed m the terminal year of the contract was aimed 

at determining the effectiveness of irradiation in con 

trolling the post-harvest incidence of decay m Cahfornia 

strawberries after commercial shipping, storage, and 

handling 

Progress and Results 

During the 1970 Cahfornia harvest season, seven test 

shipments of irradiated strawberries were made, using 

near-commercial conditions to determine the effectiveness of irradiation m controlhng the incidence of decay 

after commercial handhng Preliminary results were 

reported last year The irradiation levels used were 150 

and 235 krads at the point of maximum absorbed dose, 

with a uniformity ratio of 1 35 

Both irradiation and the physical operation of the 

pilot plant irradiator tended to contribute (ahhough 

not significantly) to the shghtly higher amount of fruit 

that suffered from mechanical injury as a result of 

transportation, however, the market acceptability of 

the fruit was judged not to be affected 

The Portable Cesium Irradiator (PCI) used for the 

1970 studies did less mechanical injury to the fruits 

than did the Mobile Gamma Irradiator (MGI) used for 

the preliminary 1969 studies 

These tests (Table) showed irradiation to be significantly effective m controlling decay during and after 

shipments of long duration such as the marine shipment 

to Honolulu Transcontinental shipments via refrigerated trucks showed less effect, although decay control 

was consistently better with the irradiated samples 

Irradiation to a maximum dose of 150 krads (111 

krads minimum) has a slight but consistent superiority 

to controlhng decay over the maximum dose of 235 

krads (173 krads minimum) 

Plan for Next Penod 

This contract terminated on June 1, 1971 

Reports Published 

E C Mzxie, Radiation Technology in Conjunction with 

Post Harvest Procedures as a Means of Extending 

the Shelf Life of Fruits and Vegetables, Annual 

Report, USAEC Report UCD-34P80-9, 1971 
145 

Estimated Date of Final Report 

This project has been terminated. 

HAWAII FOOD IRRADIATION PROGRAM: 

STUDY OF DOSIMETRY, TOLERANCE, 

AND SHELF LIFE EXTENSION RELATED TO 

DISINFESTATION OF FRUITS AND VEGETABLES* 

Objective of Work 

The primary objective of this project is to develop 

data in support of a petition to the Food and Drug 

Administration (FDA) for approval of radiation treatment and early commercialization of fruit and vegetable 

disinfestation by ionizing radiation. Papaya is the 

primary product under study because of the concentration, organization, and growth of the industry. Hawaii 

has a vital interest in radiation disinfestation of papayas 

and other fruits and vegetables. The State's exports 

require development of effective and economic treatments for products subject to quarantine measures. 

*A M Dollar, Department of Agriculture, State of Hawau, 

Contract AT(26-l)-374 

Present treatments are batch processes that impose 

delays prior to packaging and shipment Radiation 

treatment not only effectively controls insects subject 

to quarantine but also is a continuous process apphcable to packaged products, allowing efficient handhng. 

Progress and Results 

Treatment of papaya at an absorbed dose of more 

than 21 krads provides probit 9 assurance that no fruit 

flies will emerge to create a hazaid at the destination 

Comprehensive studies have demonstrated clearly that 

papaya and other fruits and vegetables can tolerate 

absorbed doses m excess of those required to achieve 

disinfestation. Extensive data collected for papaya 

handled under commercial-scale conditions supported 

earlier University of Hawau research studies showing 

that there were no adverse changes in appearance, color, 

aroma, texture, or nutritional values during the market 

hfe of papaya treated at absorbed doses of less than 150 

krads. These data have been evaluated and are being 

prepared for FDA petition action. 

Optimum disinfestation treatment of papaya by 

ionizing radiation requires continuous flow of fruit 

from receipt at the processing plant until ready for 

0.7 

0.6 

0 5 

0.4 

0.3 

0.2 — 

0 1 

TEMPERATURE, °F 

110 120 130 140 150 160 

3.20 3 15 3.10 3 05 3 00 2 95 2.90 

Papaya decay control. (Saturated vapor/hot water treatment) 
146 

shipment. For treatment of the quantity of fruit on a 

continuous basis (now a batch system), a hot water 

treatment that can be carried out m 30 sec or less must 

be adopted. The conventional hot water dip treatment 

at 118° ± 2°F for 20 min was compared with 

high-temperature, short-time treatments with a continuous system that consisted of a pump, heater, and spray 

unit recycling only 30 gallons of water After hot water 

treatment at the desired temperature, fruits were 

irradiated at a minimum absorbed dose of 25 krads and 

then stored under normal commercial conditions. 

Fruit decay is reduced two-fold by treatment at 145° 

+ 5°F for 20 sec when compared to conventional 

treatment. Another two-fold improvement in marketing 

hfe IS obtained by combining the treatment with a 

disinfestation dose of 25 krads. Treatment at 145°F for 

25 sec increases the risk of chill injury (surface scald) 

when fruits are stored at 50° + 5°F The longer 

treatment delays color development by 1 day when 

fruits are stored at 75° ± 2°F Time—temperature 

tolerance curves were determined for the range of 100 

to 150°F (see figure). 

Plan for Next Period 

The petition will be completed and submitted to FDA 

once biological safety evaluations are finished Commercial-scale marketing evaluations will be undertaken once 

FDA approval can be obtained. The facility can treat 

commercial quantities on a cost recovery basis while 

developing a suitable commercial facdity near the 

production center of Hawaii 

Reports Published 

A. M. Dollar, M. Hanaoka, G. A. McClish, E. K. 

Akamine, J. H Moy, E. Ross, and K Ohinata, 

Hawaii Food Irradiation Program, USAEC Report 

NVO-374-17,Vols. 1 &2, 1970. 

Estimated Date of Final Report 

Continuing project. 

LOAN OF 50.000 CURIES OF Co-60 FOR USE IN 

RADIATION FACILITY FOR RESEARCH IN FOODS* 

Objective of Work 

The aim of this project is to make available, on the 

campus of the University of Massachusetts, a 50,000-Ci 

Co-60 radiation facility to be used for research on the 

preservation and pubhc health aspects of food and food 

products. Four areas will be investigated (1) effect of a 

simultaneous heating and radiation process to inactivate 

Salmonella senftenberg in egg, (2) stability of food 

hpids to radiation, (3) degradation of carbohydrate 

systems by radiation, and (4) sensitivity of psychrophilic spoilage microorganisms in seafoods to radiation In addition, arrangements are being made to make 

the facility available to the entire University and to 

Amherst, Smith, Mt Holyoke, and Hampshire Colleges. 

Progress and Results 

Installation of the radiation facihty began in January, 

1971, and the Co-60 was delivered on Aprd 1 

Preliminary dosimetry and in-service training of operating personnel by the AEC and the facility contractor 

have been completed. The facihty is on a standby basis 

until final system security and monitoring measures can 

be completed. 

Plan for Next Period 

Research wiU be initiated when final monitoring and 

security measures are instaUed. 

Reports Published 

K. S Purohit, J. E. Manson, and J. W. Zahradnik, 

Theoretical Evaluation of Combined Irradiation and 

Thermal Processes in Cylindrical Containers with 

Gamma Sources, /. Food Sci, 36 750-51 (1971) 

K. S. Purohit, J. E. Manson, and J. W. Zahradnik, 

Computer Evaluation of Irradiation Processes in 

Cyhndrical Containers with Gamma Sources, /. 

Food Sci, 36 747-49(1971). 

Estimated Date of Final Report 

None. 

*W B Esselen and J W Zahradnik, Department of Food 

Science and Technology and Department of Mechanical and 

Aerospace Engineering, University of Massachusetts, Amherst, 

MA 01002, Contract AT(30-1)-4166 
AUTHOR INDEX 

Acree,E H ,40,7 9 

Akutagawa, W , 87 

Auskern, A , 121 

Baker, P S , 1,136 

Bell,R O ,88 

Besic, F C , 99 

Bingham, B D , 58 

Brashear, H R , 79 

Braski,D N ,8 

Brewer, C O , 62 

Brewer, M , 102 

Brown, L C ,21,30,31,3 2 

Bryan, D ,78 

Burgan, C E , 62 

Bustard, T S ,110 

Butler, T A , 7, 18, 30 

Carberry, J J , 125 

Case,F N ,39,79 

Chatters, R M , 77 

Clme, J E , 96 

Coffey, D L , 62 

Colombo,? , 117, 121 

Cornehussen, R D , 126 

Craft, T F ,80 

Cross, F T , 58 

Cusack,J H,13 4 

Dietz, R N , 120 

Dikeou,J T ,118 

Dollar, A M , 145 

Donovan, F M , 63 

Duane, D B , 79 

Eckelman,W, 34, 35,37 

Eichholz, G G , 80 

Esselen, W B , 146 

Fallon, P T ,133 

Gehrke,R J ,96 

Goodman, P , 105 

Goranson, R B , 63 

Greene, R E , 136 

Heath, R L,77,9 6 

Hiatt,M A , 78 

Hin,F B , 119 

Hoffer P , 99 

James, W R , 79 

Jarrett, J H ,41 

Johnson, E W , 61, 67 

Johnston, P ,99 

Jones, I R 56 

Judge, C W,7 9 

Kaminskas, R A , 107 

Kaylor, J D,14 1 

Keisch, B , 98 

Keller, O , 99 

Kemper, R S , 14 

Kneip,T J, 103 

Kolff, W J , 63 

Kyle,N ,87 

Kuczynski,G C , 125 

Kukacka,L E , 117 

Ldrkin,D J , 13 

Ldurer,G R , 103 

Lebowitz, E , 23, 25, 26, 27, 28, 29 

Lm,K H , 8, 21 , 38 

Lochbaum, R E , 53 

Lukens, H R , 78 

Mdckey,T S ,39,4 0 

Manowitz, B ,73 , 117 

Maxcy, R B ,142 

Maxie,E C ,143 

McKee,R W, 10,60 

McLaughhn,W L , 128 

Milau,J S , 130 

Mirshak, S , 65 

Moore, J D 13 

Muller,A C , 119 

Mulhns, L J , 55 

Murray, R W ,61 

Newman, D R ,42 

Newman, L , 73 

Niemeyer, R G ,45 

Palms, J M , 90 

Perkins, R W,81 

Pfeifer, R J , 74 

Poggenburg, J K , 

Pradzynski, A H 

Pressly,R S,4 0 

Preuss, L E , 95 

Pyatt,D W,6 8 

19,20,21,22 

100 

Radeka, V , 92 

Randolph, P D , 77 

Rathkamp, W R , 7 

Reynolds, S A ,46 

Rhodes, J R,10 0 

Richards, P , 22, 23, 25, 33 

Ridgway, M G , 56 

Rizzo,F X , 132, 135 

Roberts, F P , 14 

Rohrmann,C A,1 5 

Rose, V C , 82 

Ross, H H , 94 

Sadler, J W , 66 

Schaich,R W , 17 

Schlesinger, H L , 78 

Seagren,R D ,44 

Sheppard,J C ,14,16,5 8 

Silverman, J , 124 

147 
148 

Smith, J. L., 75 Teleki, P. G., 79 Warren, H. S., 136 

Smith, M., 73 Tucker. W., 73 Waterbury, G. R., 55 

Smith, T.G., 124 Weiner. R. I., 68 

Snoke,D.R.,56 Urbain. W. M., 141 Wiemann, M. R , Ji., 99 

Stahel,E. P., 123 Wogman, N. A., 81 

Stang, L. G., Jr., 23 Van Tuyl, H. H., 12 

Stannett, V. T., 123 Zahradnik, J. W., 146 

Steinberg, M., 117,120, 121 Wald, F., 88 Zanio,K.,87 

Swinth,K. L.,108 Wagner, J. I., 130 Zechman, R., 99 
CORPORATE AUTHOR INDEX 

Aerojet Nuclear Co ,77, 96 

Atlantic Fishery Products Technology Center, 141 

Atlantic Richfield Hanford Co , 13 

Battelle, Pacific Northwest Laboratory, 10, 12, 14, 15, 

16,41,42,58,60,81, 108 

Brookhaven National Laboratory, 22, 23, 25, 26, 27, 28, 

29,33,34,35,37,73,92, 117, 119,120,121,130, 

132,133,134,135 

Carnegie-Mellon University, 98 

Columbia Scientific Industries, 100 

Dade County, Florida, Pubhc Safety Department, 102 

Department of Agriculture, State of Hawaii, 145 

Drexel Institute of Technology, 126 

du Pont de Nemours (E I ) and Co , 65 

Edsel B Ford Institute for Medical Research, Henry 

Ford Hospital, 95 

Emory University, 90 

General Electric Company, 61, 99 

Georgia Institute of Technology, 80 

Gulf Radiation Technology, Division of Gulf Energy and 

Environmental Systems, Inc , 78 

Hittman Associates, Inc , 110 

Hughes Research Laboratories, 87 

Industrial Nucleonics Corporation, 74 

Los Alamos Scientific Laboratory, 55 

McDonneh Douglas Astronautics Company, 63 

Michigan State University, 141 

Monsanto Research Corp , Mound Laboratory, 61, 62, 67 

Mound Laboratory 

see Monsanto Research Corp 

National Bureau of Standards, 128 

New York University Medical Center, 103 

North Carolina State University, 123 

Oak Ridge National Laboratory,1,7,8,17,18,19, 20, 

21, 22, 30, 31, 32, 38, 39, 40,44, 45,46, 79, 94, 

136 

Pacific Southwest Forest and Range Experiment 

Station, 75 

Panametrics, Inc , 105 

TRW Systems, 56, 107 

Tyco Corporate Technology Center, 88 

U S Army Coastal Engineering Research Center, 79 

US Bureau of Reclamation, 118 

University of California, Davis, 143 

University of Chicago, 99 

University of Maryland, 124 

University of Massachusetts, 146 

University of Nebraska, 142 

University of Notre Dame, 125 

University of Rliode Island, 82 

University of Utah, 63 

Washington State University, 77 

Weiner Associates, Inc , 68 

Westmghouse Electric Corp , 53, 66 

149 
SUBJECT INDEX 

Accelerator products, 5, 22, 23, 25, 27, 30 

Barium-133m, 31 

Bismuth-204, 29 

Bismuth-206, 32 

Dysprosium-157, 25 

Galhum-67,30 

Indium-111,31 

Lead-203, 32 

Xenon-127,28 

Activation analysis, 98 

Aircraft landing, 107 

Americium-241,40,41 

Artificial heart, 53, 55, 56, 61, 63 

Automobile exhaust analysis, 105 

Bismuth-204, 2Q 

Bismuth-206, 32 

Brookhaven Lmac Isotope Producer (BLIP), 23 

Bullet hole detector, 102 

Cadmium telluride, 87, 88,90 

Cadmium-109,40 

Cadmium-111, 31 

Calcium-43, 19 

Cahfornium-252,81, 108 

Catalytic activity, 125 

Cerenkov radiation, 94 

Cesium-137,8,10, 12,13,38 

Cesium chloride, 8 

Cesium niobates, 38 

Cesium tantalates, 38 

Chlorine-36, 20 

Cobalt-60,65,66 

Concrete—polymer materials, 117, 118 

Composite materials, 121 

Cyclotron products, 25, 26 

Dating, 98 

Density gage, 82,99 

Determination of lead m blood, 103 

Dosimetry 

Circulatory support program, 58, 60 

Development, 128, 132 

In food program, 135 

Dysprosium-157, 25 

Environmental and Ocean Sciences, 71 

Program description, 73 

Field effect transistor, 92 

Fission Products Development Laboratory (FPDL), 7, 17 

Fission products, 5, 7 

Cesium-137,7,8 

Krypton-85,7,45 

Stable, 14, 15 

Strontium-90, 10,39 

Fruit preservation, 143, 145 

Gadolinium-15 3,40 

Galhum-67,30 

Half-life values, 46 

Hanford Waste Management Program, 10, 12, 13 

Heart, artificial 

see Artificial heart 

High Flux Isotope Reactor (HFIR), 18 

High Intensity Radiation Development Laboratory 

(HIRDL), 130 

Hydrogen-3 

see Tritium 

Indium-111, 31 

Intracranial pressure sensor, 110 

Isotopes Information Center, 1 

Krypton-85,7,45 

Krypton-85 enrichment, 7 

Kryptonates, 105 

Lead-203, 32 

Lead-204, 32 

Lead-206,29,32 

Lead-207, 32 

Marine Products Development Irradiator, 141 

Meat preservation, 141, 142, 146 

Medical radioisotopes, 33 

Mineral identification, 81 

Moessbauer effect, 98 

Neutron-deficient nuclides, 96 

Neutron radiography, 108 

150 
151 

Nondestructive testing, 42 

Nuclear Instrument Landing System, 107 

Oil slick identification, 78 

Oxygen-16, 55 

Palladium, 14 

Paper mill pollution, 77 

Phosphorus-33,20 

Platinum-194,22 

Platinum-195m, 22 

Plutonium-238,55,67,68 

Ponution,73,77,78, 100 

Polymer—metal composites, 126 

Portable irradiators, 133 

Potassium43, 19 

Pressure sensor, 110 

Process Radiation, 115 

Program description, 117 

Patent review, 136 

Promethium-146, 16 

Promethium-147, 16,45 

Radiation Analysis and Control, 85 

Program description, 87 

Radiation chemical engineering, 119 

Radiation-mduced chain reactions, 124 

Radiation-induced chemical reactions, 120 

Radiation polymerization, 123 

Radiation Preservation of Foods, 137 

Program description, 139 

Radiation source development, 130 

Radiation source standardization, 134 

Radioisotope heater, 63, 67, 68 

Radioisotope Production and Materials, 3 

Program description, 5 

Radioisotope standards, 46 

Reactor products, 5, 18 

Phosphorus-33,20 

Platmum-195m, 22 

Potass]um43, 19 

Silicon-32, 21 

Thuhum-170,21 

Rhodium, 14 

Ruthenium, 14 

Safety testing 45 

Sand tracing, 79 

Sewage treatment plants, 80 

Sihcon-32, 21 

Shipping casks, 44 

Snow depth gage, 75, 77 

Spectrometry, 96 

Strontium-90, 10,39 

Strontium silicate, 39 

Sulfur-33,20 

Sulfur-34,21 

Sulfur-32—sulfur-34 ratio, 73 

Sulfur dioxide determination, 73, 74 

Technetium, 14 

Technetium-99m, 34, 35, 37 

Thallium-203, 32 

Thermal Apphcation Development, 49 

Program description, 51 

Thuhum-170,21 

Tooth-enamel density, 99 

Tntmm,45 

Technology Utilization, 1 

Waste management, 61, 62 

Water recovery, 61, 62 

X-ray diffraction, 95 

X-ray fluorescence, 100, 102, 103 

Xenon-127,28 

Xenon,15 

Van de Graaff generator, 27 

Zinc-68, 30