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%G ./@ +“’UNCLASSIFIED

/

$3.44$ @ >9.(L .

&$+’ &

#~.‘9 *J’ LAMs-2726

# ~0 ,eJ$

&@’ti cf. .%A Q

C-91,NUCLEAR REACTORS

H

FOR ROCKET PROPULSION

‘“ @%

(M-3679,=~thEd.)

.9‘:””y # Thisdocumentconsistsof 64 pages

‘“+ @o’

No

m

of 148 copies,SeriesA

LOS ALAMOS SCIENTIFIC LABORATORY

OF THE UNIVERSITYOF CALIFORNIA LOS ALAMOS NEW MEXICO

REPORT WRITTEN: July18,1962

REPORT DISTRIBUTED: November 5,1962

EXAMINATION OF GROSS PARTICLES FROM KIWI-A3NUCLEAR

ROCKET PROPULSION REACTOR AT NEVADA TEST SITE

(TitleUnclassified)

1

Work doneby: ,

HaroldM. Ide~

JeanMcClelland

WilliamD. Mcjss

Evan E. Cam+ell

?:

,!

\

Reportwrittenby:

Evan E. Campbell

J

co ~05-ENG.36 withtheU. S.Atoml

All

ratory rather than for

genexal distribution en edited, reviewed, or verffied

for accnr

s of the authors as of tbe

tim n and do not nece

c Laboratory or the final opinio

“ ~

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!:*

.

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UNC*

● ● ✘ ✘

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L. ::80”

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MKYIRACT

Tld.sreport presents the data obtained from the anslysis of large

particles found in the effluent from Kiwi-A3 test reactor. The methods

used> and their application to future test operations> are discussed.

Procedures are described for the Lsolatd.onof particles from static

sampling systems and for paper chromatography of the fission products.

A Polaroid film fallout tray for static sampling of particulate slso

is described.

AcKNOWLEDGMENTS

The author acknowledges the work of (1) Group H-5, of the Laboratory’s Health Division, who obtained the data presented here, and (2)

the members of Group H-8, in collaboration with whom this work was done,

and who collected the particles and obtained the data at the Nevada Test

Site.

!!p!fCLASSIFIED

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IED

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comm

Page

ABSTRACT ● ..000..000. . ..000.... ● . . . . . ...00 ● 0....0.0.. . 000 ..0.... . . 3

ACKNOWLEDGMENTS ..● .● ● . ● ● . . . c . ● .0 . . ● ● . . ● . ● 0. ● . ● *.. ● ● ● . ● . ● ● . . . . ● ● ● O 3

INTRODUCTION ..0...........● ... ...* ● . ● . ● ● . ● *. . . . . ● . ..* . ● . .0 . . . . . . . 7

Objectives .................................................... T

Discussion ....................................................

li3cationof Particles ......................................... i

MICROSCOPY .....................*....*..00.0.00. ..0..... . . . . . . . . . 9

Technique ..................................................... g

Results ....................................................... 9

Conclusion .................................................... 10

RADIOMETRIC ANALYSIS ............................................. 10

Beta and Gamma Counting ....................................... 10

Gamma Spectra ................................................. 11

Beta Absorption Curves ........................................ 12

Radioautography ............................................... 13

X-ray Film ................................................. 13

Polaroid Film ................... . ...00.0 . ...0.... . . . . . . . . . ● 14

CHEMISTRY .0. .00.... .0..0.00. . ..0...00 . . . . . . . . . ..0.0...0 ..00.0000 ● 15

Introduction .................................................. 15

Dissolution ................................................... 16

Alpha Activity ● ...0.......0.6............● ..0....0............ 17

Chromatography ● ...0.0.. . ..0...0. . . . . . . . . . ..00.00.0 .0...00.. ● OO 17

SHZCIA.LANALYSES ...● .● .0. ..0.0. ● ● O ● . ● .0 ● . . . . . . ● 0 ● ● ● *. . . ● . ● ● . . ● . . ● 18

Spectrographic AnslYsis ....................................... 18

X-ray Diffraction ............................................. 18

High Volume Air Sample ........................................ 19

suMMARY ...0...... . . . . . . . . . ..000.00. . ..00.00. . . ...00.0 ● 0....... . . . 21

CONCLUSIONS ........**...S**● **....● .● ● ● ● ● ● ...● ..● ● ● ● ● ● ● .● ..● ● ● ● ● . 23

. UJIICLASSIFIED

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APPENDIX

APPENDIX

APPENDIX

APPENDIX

A

B

c

D

● ☛

☛

‘ ::: $●1 ‘: s

“:*:: ..:●

● *

●s: ●:@ S*

● *

9**** d 8’

● 0 ●

● O :

● 0 ●0:● 00 1A!-,QcL~~slFi~~

ISOLATION OF PARTICLES FRCM SOIL AND FROM

FALLOUT TRAYS ........................0.00........00.0

Equipment ........................................

Technique ........................................

Soil Samples ...................O....O.........

Fallout Trays or Other Surfaces................

Resin or Resin-Coated Trays ...................

X-RAY FIIM RADIOAUTOGRAPHY ..● ..● .● ..● .● .............

Introduction .....................................

Equipment ........................................

Exposure .........................................

Interpretation ...................................

POLAROID FIIM RADIOAUTOGRAPHY ● .● ● .........● ● ● ● ..0.● .

Introduction .....................................

Equipment ........................................

Preparation of Tray for Use in Field ...● ....● ...●

Exposure .........................................

Development and Study ..● ● .● ......0....● ● .....● ...

CHROMATOGRAPHY OF FISSION PRODUCTS ...,.......,......

Introduction .....................................

Reagents .........................................

Reduction of Samples for Paper Chromatography.....

Chromatography ....0...00.....0.......0000........

● ..● ● ● ● 0..● ● ...● ....● ......● ..● ......● ● .........● .● .● .

TABLES .● ...● ● ..● .● ......● .....● ....● ● .......● ...● ● ● ● ● .........0 .

PHOTOGRAPHS ...● ● ● ● ..● .● .....● .......● ● .....● .● ..● ● .......● ..● ● ..

. ● ✎ ✎ ✎ ● ● 00 ● . . . . . . . . ● . . . . . . . . . . . . . . . . . . . . . . ● ● . . . . . . . . . . . . . .

UNCLASSIFIED.

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57

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u

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INTRODUCTION

Objectives

This study was to gain an

with the chemical and physical

insight into the problems associated

anslysi.sof discrete particles, to

evaluate techniques for application to future nuclear rocket engine

effluents, and to accumulate sufficient data to identify the particles

by simple methods. Recommendations for methods and techniques to be

used in the future are based on the experiences gained in this study.

Discussion

The exac’tprocedures used in isolating or examining particles

from previous nuclear events are not fully documented. Particles

associated with nuclear weapon testing are necessarily grossly contaminated with extraneous material, either from the test site or from

the weapon carrier; whereas particles from nuclear test reactors of

the Kiwi-A3 design are relatively pure fission products because they

emanate by erosion snd corrosion from inside the reactor itself.

Should the reactor be tested so as to cause excessive turbulence on

the ground surface, the particles then would become adsorbed on the ,

dust surrounding the reactor, and would not necessarily be handled

as described here.

UN~lAS#FIED %>’~e.

“W;f! #: &:f*g”m;m” ;&;: :;:-.

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● ☛

●

●

●☛☛

● S* ::OJ’

●0: 9:8 8s

The relatively large particles from the reactor test should cause

little concern from a heslth standpoint; they represent only a means

for studying radioactive decay, the distribution of masses of particles

within a given area, and a genersl prediction of isotopic composition

of the smsller fsllout particles.

The techniques used in this study are essentially standard methods

unless otherwise described. All.the radioactive data taken at the

Nevada Test Site were determined as described in --2588;A the area

under study and the devices used in ssmpling ground and air contamination are described in the ssme document.

Location of Particles

The midpoint of the run was on October 18, 1960, at 16:43 hours.

The particles were located by a ground survey tesm using a portable

beta-gsmma survey instrument. The dose rate background at 500 and

1000 feet from the reactor test celJ.male it impossible to find smalJparticles or particles of low specific activity.

The particles were clustered in the three general areas indicated

on Figure 1. Particles 1 to 17 were found 18 hours after the midpoint

of the run; particles 20 to 25 were found one week later and numbered

to indicate a second field search. Many of the particles were poorly

handled and became abraded. They were isolated from the soil by means

of cellophane tape, then, for optical and radiometric study, were mounted

on microscope slides, which proved a poor technique. The recommended

technique developed during this study, given in Appendix A, was wed

for the isolation of particles 20 to 25.

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MICROSCOPY

Technique

Each particle was photographed with a 35 mm Cents.xcamera

on a Unitron adapter and prism, through an Ortholux microscope

mounted

having

a 10X eyepiece,

Because all the

copy was useful

a 6X objective, with both substage and incident light.

particles were opaque, polarizing or dispersion microsonly for adsorbed particulate dust. Each particle was

placed on a microscope slide; as mentioned above, the early technique

for isolating the particles was poor, and some particles were crushed

by the coverslips used in mounting the particles. Photographs 1, 2,

and 3

found

are representative of the three general classes of particulate

(scsle: lcm= lw). Photograph 1 illustrates the friability of

the particles; photograph 2 shows an adsorbed gray-white substance on

black, granular materisl; photograph 3 illustrates the metallic character of the s~ace of several of

described in Table I. The size of

sn ocular micrometer and confi?xned

micrometer.

Results

the particles. Each particle is

the particles was determined with

from photographs with a stage

Table I shows the number of particles on each slide (some particles were crushed by the coverslipj, the approximate combined size,

location of the particles by distance from the reactor, a description

of the particle, and the extrapolated beta activity at 1000 minutes.

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Conclusion

The particles from within 1000 feet

nantly black, metaU.ic granules; at 6000

of the reactor are predomifeet the particles appear

mairilybrassy on a black, metdd.ic granule. The area described as

“white, ye~ow, or grsy sdded residue” wilJ.be shown later to be potassium chloride and other JATO fuel products. There is no relationship between particle size and distance, but there is some correlation

between appearance of the particle and distsnce. Particles 12, 13,

and 15 show definite fractures, iU.ustrating the friability observed

in ail.of the particles

Beta and Gamma Counting

The beta and gsmma

(Photo 1) ●

RADIOMETRIC ANALYSIS

activity was determined at the Nevada test site

with the equipment described in IAMS-2m. LLthcmgh each particle -S

followed for

the counters

the original

its decay, variations in the particle preparations and in

gave curves which were of little value in reconstructing

activity.

Figure 2 illustrates the composite beta

titles and seversl trays which were known to

title. The solid line indicates a composite

curves of W the parhave only a single parof sXl particles and the

dotted line represents only three fsllout trays and one particle. The

gamma activity is not presented because the great variations within

each particle preclude any interpretation.

10

3

●

●

●

●

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.

Gsmma Spectra

The gamma spectrum of each particle was determined at various

intervals and interpreted for gamma energies and hslf life; the spectra

indicated a similarity of the particles. Those fission products

were identified positively are given in the following summary:

Particle

No.

1

2

2

2

?

10

11

12

13

14

Special Soil

Fallout Trw

6-24

NUCL

Te-I-132

*

*

*

*

*

*

*

*

*

*

*

*

*

*

*

1-131

*

*

*

*

*

*

*

*

*

*

*

*

*

*

*

*

*

*

IE

1-133

*

*

*

*

*

*

Ba-La-140

*

*

*

*

*

*

*

*

*

*

which

7zmi---

%-

*

*

*

*

*

The gamma spectra of particles 7, 9, 10, and 14 indicated primarily

Ta182

, in such

impractical.

After the

excess that interpretation of other gannnaenergies was

particles had been returned to

radiometric procedures were carried out. The

peated on a Los Alsmos Model 200, 100 channel

8 x 4 inch thslllium activated sodium iodide

Los Alamos, many different

gamma spectra were regamma analyzer with an

crystal, shielded to

reduce the background to a minimum. The gamma spectrum was determined

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on the 34th day sfter the Kiwi-A3 reactor test.

lected and processed to remove background counts

resolving time. The areas selected were reduced

The raw data were colsnd to correct for

to relative activity

by dividing by the totsl counts in the energy range O to 2 mev. Table II

gives the relative activity of the primary gsmma energies corresponding

140

to 0.75mev for Zr-~95, 1.6 mev for w , and 1.1 and 1.2 for the

~a182 doublet.

182 Particles 9 and 10 are relatively pure Ta while the remaining

particles are grossly contaminated with fission products. Figure 3

illustrates

calibration

study ●

the curve of activity vs. channel (energy) and the energy

of the crystal for the two types of spectra found in this

Beta Absorption Curves

The beta absorption study was to determine the applicability

the technique to the identification of differences within several

titles, and not to establish precise energy levels. A direct method

of

par2

of plotting data waa used, rather than Feather’s more precise method

for determining beta energies.

A Tracerlab E-3A beta absorber set was used, aud the beta activity

of the maximum absorber

was divided by the free

the normalized values.

vslues in mg/cm2 of the

was subtracted from sJJ.counts; each count then

count (no correction for air absorption) to give

These vslues were plotted against the absorber

sluminum absorber and the normalized count

12

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plotted

and 19,

~a182

.

on semi-logarithm paper as

for comparison, illustrate

Table III lists the E+ and

shown in Figures 4 to 17. Figures 18

the ssme type of data for Cs

137 and

the Emm determined from the graphs.

The energies are based on the Glendeni.nbeta absorption curves

The graphs themselves are perhaps more interesting because the

shape of the curves is an indication of the isotopic purity of the

particles, and the graphs vividly illustrate that absorbers cannot be

used to reduce gross counts for beta counting when the samples contain

unknown mixtures of nuclides, unless more than one absorber count is

made and the reduction does not exceed 30 per cent of the original

activity.

Radioautography

The particles were submitted to two types of radioautography by

placing the particles directly against (a) Kodak x-ray film and (b)

Polaroid

a simple

(a)

film (experimentally,because the Polaroid film tight prove

method for locating particles in similar field operations).

X-ray Film

The particles were placed face down on Kodak type K x-ray

film with only a coverslip separating the particles frcxnthe film.

The particles remained in cent’actfor one hour, the film was developed

and dried in the usual manner, and the size of the darkened area

measured. The beta activity was determined immediately before exposure. A comparison of the particle size, exposed spot, and activity

13

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in totsl disintegrations is given in Table IV. The film is sensitive

also to gamma rays, but gainmaactivities are not included.

Skillern4 showed that the log of the total disintegration plotted

against the log of the

shows the relationship

here. Particles 4 and

spot diameter is a straight line. Figure 20

observed in the case of the particles examined

14 are not on

diameter would give better agreement

ened, and a more accurate beta count

the line. Particle 14’s spot

had the exposure time been shortbeen possible; the method of preparation and the coverslip used to mount particle 13 caused a loss of

activity. Neither spot diameter nor beta disintegrations correlate

with the actusl size of the particle.

If the exposures could be made immediately titer isolation, the

exposure time of the particles may be brief. Standard field counting

can be done during the development of the films. See Appendix B for

recommendations for future application of x-ray film radiography.

(b) Polaroid Film

we 37 (ASA 270) and Type 57 (ASA 3000) Polaroid films were

investigated for their possible application to particle detection and

sizing in the field. Laborato~ experience indicated a similar relationship, for activity and spot dismeter, to that described above

for x-rsy film.

Particles placed on the face or paper side of the single sheet

film package

shadow-edged

gave a clearly defined spot on

clear spot on the paper, while

the film and a somewhat

particles placed on the

14

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film or back side of the package gave a clearly defined white area with

sharp edges in the precise shape of the particle. It is interesting

that the negative in the latter case gave better results because a

reversal of the film formed a halo around the e~osed area and clearly

marked the particle. The central portion of the cleared area was

identical to the size and shape of the particle (Photo 4).

During a specisl test operation, some 150 films of each of the

film types were used, prepared by covering each with a mylar film and

spraying with silicone grease for better

exposing to the atmosphere for two days,

ranged from 65° to 85°F. and 0.2 inch of

not damaged by the water and those films

particle retention, then

during which the temperature

rain fell. The films were

protected from direct midday

sun were satisfactory; however, because of a pinhole coding system being

employed, the films were fogged. A new series of experimental trays has

been prepared and tested for possible application to future fallout

studies; see Appendix C.

CHEMISTRY

Introduction

The choice of chemical analytical techniques for particles emitted

from nuclear reactor systems depends largely on the information desired.

Stmndazd methods of dissolution and anslysis are applicable when a single

given element or specific isotope is to be determined. However} the

particles or fallout debris eroded during a Kiwi-t~e reactor test

15

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operation contain the fissionable material and its fractioned fission

products, elso neutron activated nuclides from added materials. Consequently, the chemistry becomes ultrsmicro in order to determine the

inert elements of interest, end individual.isotopic composition analysis

is impractical immediately following a reactor test. When radioactive

material (gas, vapor, or particulate) has become adsorbed on to normel

atmospheric dust, the adsorbed must be distinguished chemically from

the inert materisl. Techniques have been developed for handling these

particles under high magnification> and for identifying eluted materisl

in serial elutions. Most of the analyses were qualitative in nature

because the study was to evsluate techniques.

Dissolution

The particles were returned to km Alsmos for chemical and physical

examination, and for further study of the techniques. A particle from

slide 2 and particles 1, 3, 6, 11, and 12 were transferred to platinum

crucibles and ashed with nitric and perchloric acids without carriers.

The residues finally were whitened with nitric acid, then evaporated

several times with hydrochloric and hydrofluoric acids. One hundred

microliters of a solution which was 4N in sulfuric acid and 4N in hydrofluoric acid was added to each crucible and the wsJ& of the crucibles

scrubbed down with a platinum rod. Five microliters (0.005 ml) of each

solution was analyzed according to the procedure outlined in Appendix D.

The results of the ansll.ysesare shown under Chromatography (below).

16

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Alpha Activity

Five microliters of ssmple were placed on a 3/4 inch dismeter

tsntslum plsnchet, evaporated under infra-red heat, and finally flamed.

First the planchet was alpha counted in a low background proportional

counter, then the planchet was packaged in a nylon ring and disc assembly

and counted for its beta activity in a low background beta counter. The

results of these counts are given in Table V. The elpha activity was

from uranium, which was confirmed by the stsndard ion exchange procedure

described in IJ1-18~.5 No slpha activity was found on any of the stages

from cascade impactor sample 1-10 or ssmple 2-1.1.

The slpha activity should show some relationship to the location

of the particles within the reactor. Particles 2A, 3, I.1,snd 12 are

approximately the same size and have proportionately the same amount of

uxanium activity, indicating that they were from the undersurface of the

rods, while particle 6, low in alpha activity and relatively high in tantalum activity, must have come from the surface of the rod.

Chromatography

These particles were treated according to the procedure outlined

in Appendix D. The chromatogrsms were not read on the drum counter but

were exposed to x-ray film to locate the activity associated with each

particle. The fission products had decayed to such an extent that a

24 hour exposure was necessary to demonstrate the presence of nuclides

other than tantalum.

17

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Particles 1, 3, 6, and 11 had decayed so much that identification

of R values other thsn that of tantalum was tipracticsl. f

Particle 2A

contained a smsll amount of activity at Rf 0, and particle 12 had some

activity between Rf 4 and ~; sJ3.had activity at Rf 1. The activity

at Rf O was luth~uj at 4-5} zircofi~j ~d 1 PredOmin=tW

with traces of niobium, which was confirmedly gsmma spectrum

The chromatographic techniques are satisfactory for particles

pure samples. Particles found after a nuclear detonation may

tantalum

anslysis●

and for

be eluted

serially with vaxious solvents, using microchemical-techniques, and

then placed on chromatographic paper strips

Spectrographic Anslysis

A review of SD the

SPECIAL ANAIYSES

particles by Group

for absolute identification.

CMB-l indicated that particle 14 couldbe snslyzedby spectrographic techniques and x-rsy diffraction. The results of these snslyses are given in Table VI.

The predominance of tants3um snd niobium was expected because these

elements were added to the fuel system to change the surf?acecharacteristics of its graphite. Titanium and silica are normsl in the graphite,

and the silica content may have been increased due to the absorption of

dust from the ground. The presence of platinum is unexpltinedo

X-ray Diffraction

Particles

anslysis. The

reactor system

9 and 10 were submitted to CMB-l for x-ray diffraction

results are consistent with the method of preparing the

snd confirm the spectrographic data.

18

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Particle 9 was primarily tantelum carbide, with traces of tantslum

oxide and tsntslum metal, and other patterns which were not identified.

Particle 10 consisted primarily of tantalum carbide with traces of

tsntslum oxide, in both the alpha and beta fore, and some tsntelum metal.

Particle 14 was primarily

traces of tantalum metal. The

in the beta form.

High Volume Air Sample

A high volume air sampler

heavily laden with particulate

tantalum

tantalum

carbide and tantslum oxide, with

oxide was identified as Ta O

25

suspended directly over the reactor was

matter and the activity was so high that

gamma spectrum analysis was impractical. Two weeks after the sample was

collected the activity was essentiaddy zero. The small amount of activity that did remain was not contained in a single particle but was evenly

dispersed over the entire glass filter.

the filter was from the JATO smoke used

from the reactor.

The large amount of residue on

to identify the cloud emitted

JATO fuel, 14AS1OOO Type, contained a 79 pound solid propelJ.ant

grain with potassium perchlorate as the oxidizer and an asphslt-oil

mixture as the binder-fuel.

and 115 pounds was expended.

combustion of the propellant

Combustion products obtained

The 14AS1OOO JA’10weighed 194 pounds losiied,

The potassium chloride resulting from the

is the prime source of smoke from the unit.

when using potassium perchlorate as the

oxidizer are: potassium chloride (solid), water, carbon dioxide, carbon

monoxide, unreacted carbon (solid), end hydrocarbons. The per cent of

19

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unreacted hydrocarbons and carbon is controlled by the percentage of

oxidizer and by combustion catelysts.

Much of the residue fell off the filter during trans~rtation.

Microscopic examination of some of the dust from the filter, snd microchemicsl reactions, confirmed the presence of potassium chlorate, much

potassium chloride, snd some carbonate. A few black grsnules were identified as graphite. The white residue adsorbed on some of the particles

came from the JATO smoke. The residue was eluted with distilled water,

and a microdrop of this wash tested by precipitation and microcrystsllography techniques. The presence of chloride, potassium, carbonate,

and chlorate ions was confirmed; the water washing from the particle

contained ody traces of beta activity.

The filter was washed tith distill.edwater Until reasonably clean

and the washings were centrifuged. The supernatant was decanted from

the residue and the residue again washed with water snd centrifuged,

and the supernatants combined. The residue was ashed with nitric end

perchloric acids until it was white, transferred to a platinum crucible,

and evaporated

microliters of

fluoric acid.

to dryness. The

a solution which

Five microliters

dried residue then was dissolved in 100

was 4N in sulfuric acid and 4N in hydrowere transferred to

evaporated to dryness, and flamed to red heat. The

for alpha and beta activity. The alpha activity in

proximately 30 d/m/semple and the beta activity was

a tsntdum planchet$

plsnchet was counted “

the residue was ap1670 d/m/semple.

A ~ microliter portion was placed on a chromatographic strip and treated

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as described previously. X-rey film

areas normzd.lyoccupied by zirconium

longer exposure did not indicate eny

residue was transferred to a plsstic

was exposed to the strip end the

and niobium were identified. A

other Rf areas. The remaining

weighing bottle for gamma spectrum

msis~ but the activity~ too low for photo-peak identification.

The supernatant from the filter contained sll of the water soluble

compounds

mentioned

and essentially no activity. The presence of the ions

above was confimed by chemical tests.

SUMMARY

tiing the test operation of the ~w-A3 reactor at the Nevada Test

Site

with

on October 18, 1960, the reactor emitted many large particles along

the expected fission gases and the more vola’tilenuclides. The particles ranged from 35 to 2500 microns in diameter, ~d were extremely

friable. The inert portion of the particles contained graphite, tsntelum,

niobium, and trace elements; the radioactivity was contributed primarily

182 by the activation of the tantelum to form Ta . The remaining activity

ceme from the normal distribution of fission products of uranium impregnated in the graphite.

The location of the particles in the test area was a function of

reactor gas effluent velocity and time of corrosion and erosion rather

than of particle size. There was no correlation between particle size

and distribution slong the fallout pattern. Two four-stage cascade

impactor slides from the area did not contain my uranium or tsntalum.

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Some of the

the effluent gas

of the cloud. A

particles were coated with the JATO smoke used to track

cloud, indicating that the particles actually were part

plume ssmple showed only decay dau@ters of gaseous

fission products, with no uranium or tantslum.

Radimetric procedures, such as gsmna spectrum anslysis, beta

absorption studies, x-ray film and Polaroid film radioautography$ and

gross beta and gsmma counting, were applied. Radioautography proved

extremely useful in determining the relative activity of particles found

on surfaces of static sempling units as well as those isolated from the

ground; although the size of the exposed spots formed during the study

did not correlate with particle size, the specific activity of a given

size particle could be calculated. Beta abso~tion studies proved of

little vslue except when absorbers must be used to reduce the beta

activity for gross counting. The gsmma spectrum analysis 34 days after

the day of the run was more significant than the spectrum determined

irmnediatelyafter the run because of the excessive tantalum activity and

the finding that the psrticles contained uranium

petted long-lived fission products.

The chemicsl and physical methods used were

and thus most of the exspectrography, x-ray

diffraction, microchemicsl qualitative techniques, paper chromatography)

and standard quantitative procedures. They showed that chemicsl procedures

applied immediately after a nuclea reactor test, to particles or to

static sampling systems,

unless specific isotopes

must be rapid and can be only qualitative,

are chosen for a specific decay series.

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Included in this report are those techniques which seem applicable

in a future operation producing a similar type of fsilloutdebris. A

procedure is given for the isolation of particles without undue contamination or loss. X-ray film radioautography and

trays sre described. The paper chromatographic

these particles is outlined.

Polaroid film fallout

procedure developed for

CONCLUSIONS

The discrete particles found in the fallout area were from the

reactor fuel elements where tantalum oxide hsd been applied. The particles were eliminated from the reactor at different times during the

run. The large particle size precluded any heslth hazard from inhalation, but did contribute to the integrated dose rate. The amount of

uranium in the particle after hydrolysis of the carbide becomes a

measurable ground contaminant. All of the tantalum carried out of the

182 reactor in the form of Ta was contained in large particles; essentially

no uranium was found in the fdd.out srea samples, as determined fmxn

analysis of the plume and cascade impactor samples. me fission products

found in the fallout area were short-lived, while those associated with

the psrticles were primarily normal fission products because of the

fission of the uranium contained

the particles from the reactor.

Those procedures which seem

in the particles before elimination of

applicable to future reactor environmental health

Polaroid film

studies are the techniques of particle isolation and

fallout trays. X-ray film radioauto~aphy should be an

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integral part of the standard fe.111.out tray examination, to detezmrinethe

distribution of particles based on their activity and size, as well as

their specific activity where possible. The chromatographic technique

has limited application for presumptive group identification because

large amounts of radioactivity must be confined in a small volume.

Aluminum absorbers canbe used to reduce gross beta activity for counting

purposes} provided that more than one absorber density count is taken.

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*

APPENDIX A

ISOLATION OF PARTICIES FROM SOIL AND FROM FAILOUT TRAYS

Equipment

Beta-Gamma Portable Survey Instrument

Low Power Magnifier

(A shop microscope or similar optical system having 60 to 200X

magnification is preferred.)

Beta Particle Probe

(The probe used in the study, prepared by the

consisted of a 1/4 inch diameter by 1/8 inch thick

Electronics Group,

beta phosphor coupled

to a 1-1/2 inch photomultiplier tube by a light pipe. The unit was operated at maximum voltage for lowest background. The response of the

tube was measured through a proportional counter to a count rate meter

and recorder.)

Particle Holder

(The particle holder is essentially that described by Mackin,

6

et al. Insert a dissecting needle through a #000 cork and wipe with a

thin coat of silicone grease> then store in a 2 ml.glass visl. Sharpen

the needle or pu31 a glass rod to a fine tip for finer manipulations.)

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Technique

Soil ssmples

When the soil sample is received in the laboratory spread it on

a glass plate and divide

beta-gamma activity with

containing no activity.

it into two portions. Check each portion for

a portable instrument, and discard the hslf

Divide the remaining hslf again, check for

activity, and discard the helf containing no activity. Repeat the

hslving process until only a few grains of dust remain on the plate.

Accomplish the finsl separations with a small brush and a lead shield.

Finally} observe the particles under low power> and> with the aid of

the beta probe, pick up smsll particles with the dissecting needle.

Often the particle can be selected by its color or surface character.

Usually there is only one particle in the soil} with a small.smount of

activity abraded from it; however, if care is taken when the soil is

selected in the field, abrasion wi~ be

the selected particle in the glass vial

Fallout trays or other surfaces

minimsl. Store the needle and

until ready for analysis.

Scan fsllout trays, which are to be examined for single particle

activity, with a portable beta-gamma instrument. After isolating a

given area of activity scan the sector with the beta probe to narrow

the area to less than 1 sq.cm. Mark the area clearly with a pen or

other marking tool. Observe the area under low power to identify the

particle.

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Resin or resin-coated trays

Place a small circle of filter paper over the particle and, with

a fine-tipped suction tube and a micro dropper} add acetone to one side

of the filter circle and aspirate the acetone from the opposite side.

The acetone removes the resin or oil and the particle usually is picked

up by the fibers of the filter disc. Then pick up the particle with the

needle for

Use

further study, for storage, or for shipment elsewhere.

the needle in the field to isolate particles from surfaces

which normally are free from dirt, such as stationary fallout trays, or

building surfaces on which spot activity haa been found.

Note:

The particles may be gamma counted directly without removal from

the vial and may be studied under low magnification directly. The

particle may be transferred eaaily to laboratory ware or to microscope

slides for further examination.

transferred directly to a cavity

cover slip.

For microscopy, the particles may be

microscope slide and covered with a

27

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APPENIIIXB

X-RAY FIIM RADIOAUTOGRAPHY

Introduction

Many authors have discussed at length the use of x-ray film

radioautography, but its application to field operations has been limited to weapons tests in which discrete particles were involved. This

technique was not applied to the Kiwi-type reactor because the results

of the study did not seem to warrant the expenditure of time and effort.

Several factors which occurred with the past series of Kiwi tests, as well

as the operational design of future reactors, changed this opinion.

Fallout trays, poor as they are for collecting fsllout data, still may

be the best technique for stationary sapling of ground deposition.

As in Kiwi-A3, the reactor corroded and eroded. The eroded particles

fell within the test area and were counted on fsll.outtrsys as if they

were representative of the genersl ground deposition. Soon after a run

the specific activity of the individual particles is relatively high

and is suitable for x-ray radioautography.

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Mylar films on fallout trays in field operations are not advisable because the mylar is difficult to handle and may become contaminated. The trays normally are sandwiched together face to face at

pickup, which destroys the normal distribution of perticles but gives

the same total activity deposition; although larger particles are crushed,

they are plainly visible and the total

unchanged.

After the trays have been returned

activity of the two trays remains

to the laboratory, sesled in

polyethylene, and counted at least once, they can be exposed to x-ray

film for a known length of time.

Equipment

Kodak Ty_peK X-ray Film

(Number each film and package

envelopes, Ill.x 14 inches. Store

from possible radiation.)

Exposure

Place the trays in pairs face

A and B trays in the ssme order.

each in individual, light-tight

sXl_of the film in an area removed

down on the film, always keeping the

Allow the trays to remain in position

for a given length of time as shown below:

Surface Reading Exposure Time

(mr/hr) (minutes)

5.0 15

1.0

0.5 :

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Record the following information:

Time of Exposure ....... minutes after midpoint

Length of Exposure ....... minutes

Film Number

Trsy Number

Expose the trays to the x-ray film, snd store the films at some

point removed from the general area.of radiation to prevent fogging of

the film. Expose only a few trays at a time, depending on the operational surface area available for the study. Develop the x-ray film

in the USUS3 manner snd dry it as rapidly as possible for study.

Interpretation

1. General fogging of the film: indicates even dispersion of

fsllout in the area represented by the tray.

2. Many small black spots on the film: represent particulate

that

dust

could be either discrete particles or

particles.

3* Large black spots on the film:

discrete particles which may be removed by

nique described above, if desired.

adsorbed activity onto inert

represent relatively large}

the particle handling tech4. Combinations of these: represent the type of distribution

of the particles throughout the fallout test area.

It would be possible, then, from the above data, to establish

the distribution of particles throughout the test area, based on the

relative size of the particles. Single particles can be removed from

the general debris of the tray and followed separately, if desired.

:

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lummtix c

POLAROID FIIM RADIOAUTOGRAPHY

Introduction

Polaroid film is used to isolate given particles, size them as

rapidly as possible,

field work comected

however, some of the

come. Polaroid film

and identify their origin. Polaroid film for

with nuclear devices has not been satisfactory;

problems associated with its use have been overdoes offer a rapid method for observing nuclear

events occurring on the surface of the film} providing background

rsdiation is minimal. Particles falling onto the film surCace expose

both the paper and

the film surface.

is rapid.

Equipment

Trays

the film and thus record the particles’ location on

Iocating the particles by low power magnification

(1OXI.2 x3/16 inch Masonite sheets with al/2 x 3/16 x12

inch strip of Masonite glued along opposite edges and a 3/16 inch hole

drilled in the center of each strip. The holes are used to stack the

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trays for placement and collection and also are used to nail the tray

to the ground to prevent the tray from blowing away or turning over.)

Film

[me 37 (AsA

4 x 5 inch film.]

Holder

270) and Type 57 (ASA 3000) Polaroid single sheet

(Sheet film adaptor #500 for 4 x 5 inch camera, to be used for

development of the film.)

Preparation of Trsy for Use in Field

Place a sheet of each of the film types on the Masonite tray with

the film face toward the tray, and tape elong the center between the

two films to prevent excessive meting of the film. Cover the fil.mwith

a 10 x 12 inch sheet of black glazed paper (weighing paper) and tape

the paper to the tray with masking tape slong the three flat edges,

then fold the overhanging edge under the tray and tape to the back of

the tray. Be careful not to break the developer pod in the film pocket.

The tray maybe left unrefrigerated for as long as a week without demonstrable change in the films’ response. Just before placing in the

field, sprsy the glazed paper suz%ace with a thin coat of Dow Corning

Antifosm A.

Exposure

Place the trays on the ground in the field and hold in position

with two large nails through the holes in the tray. Place each tray

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so that direct radiation from the reactor is minimized. Smaller particles can be detected by this technique because their specific activity is extreme~ high within a few minutes after a nuclear event,

so they begin to expose the film immediately upon deposition; the particles decay so rapidly that they would be missed at later times.

Development and Study

After the exposure has been completed and the trays colJ.ected,

cut the paper along the folded edge and remove the films carefully to

prevent separation of the film pack itself. Place the films in the

holder and develop them in the usual manner. Immediately titer developing examine each film for the presence of particles, then replace

film and paper in the tray for future reference; discard those trays

void of activity. Disregard the pinhole white areas observed at

regular intervals throughout a series of films. If desired} individual

particles mey be isolated by microscopy and the technique described

above for particle location.

Note:

When films can be attached directly to a surface, the films mey

be packaged in the glazed paper by folding the paper over three times,

taping the double fold together on the face side of the film, and

sealing each end. Then spray the back of the paper with the Antifosm

and expose by clipping or taping the package to the surface.

.

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APPENDIX D

CHIKMATOGRAPHY OF FISSION PRODUCTS

Introduction

For chromatography, ssmples from many sources are reduced to a

pure residue and dissolved in a mixed acid. An sliquot is placed on

a multiple strip CRL/1 chromatography paper and chromatographed with

an acetone-HF-HCl-HOH solvent. The new technique was necessary for

field use because the rapid decay of the early fission products would

give a diffuse separation in the butanol solution used in other studies.

The migration time on an unequilibrated paper is 12 minutes as compared

tith 45 minutes using butanol. Given below, in the order of their

relative activity, are the nuclides in fsllout at 1 hour} 1 dsy~ and

10 days (99 per cent of the tot~ activitY is included in ‘he ‘sOtopes listed).

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1 HOUR 1 DAY 10 DAYS

Te (some) I* I*

U* Xe* Sr

Rb Y Te (some)

Ce Te (some) La

I* Sb (some) Ba

Ba Ce Y

*

Xe Kr* Ce

Br* Sr Pr

La Nb Sb

Y La Nb

Sb (some) Ba

Se (some) Zr

Pr

*

Those elements which are lost are marked with an asterisk.

In addition to these elements, activated elements also must be

considered, i.e., Ta, MO} W, and Ti. The chemical procedure used to

reduce the samples to a chromatographic form causes a loss of many of

the more volatile isotopes. The experimental work using this technique

has been reported by several authorsT}8~9 and has been modified for

application to this particular situation. Below are the elements

listed above, with the reported Rf value for each. For a more complete

list of elements snd their Rf Veluej see Table 1, Appendix D} page 52.

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ELEMENT

‘f

1.0 Ta, W, Se

0.83 Mo

60.86 Sb

0.82 Nb

0.64 Ti

0.48 Zr

0.24 La

0.15 TeO ‘-

3

0.05 Rb

0.00 Y, Ba, Ce

Te04-, Sr

Reagents .

Prepare the following reagents from snslyticsl reagent grade

chemicals; store each concentrated reagent in its originsl container:

Sulfuric Acid 96$

Nitric Acid n$

~drochloric Acid 36?

Digestion Mixture

To 60 ml of cone. nitric acid, sdd

and allow to cool to room temperature.

Hydrofluoric Acid ~%

Ammonium Hydroxide 31$

Perchloric Acid 70$

20 ml of cone. sull?uricacid

Add 20 ml.of cone. perchloric

acid and store the mixed acids in a glass storage bottle fitted with a

syringe dropper.

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Dissolving Solution

To 25 ml of distill.edwater in a graduated cylinder, add 10 ml of

cone. sulfuric acid and cool. Trsnsfer to a polyethylene storage bottle

and aid 10 ml of cone. hydrofluoric acid.

Chromatography Solvent

To ~ ml of acetone in a polyethylene storage bottle, add 5 ml of

cone. hydrochloric acid, 4 ml of distilled water, and 1 ml of hydrofluoric acid. Prepare the solution fresh daily, always stopper it

tightly, and refrigerate it when not in use. The reagent need not come

to room temperature before use.

CRL/1 Chromatography pa erlo

(Paper shape cut J+-1/2x 8 inches, slotted to permit

running of ten ascending chromatogrems.) H. Reeve Angel

Inc., ‘j2Duane Street$ New York 7, New York.

Reduction of Samples for Paper Chromatography

Single Particles

simultaneous

and Company,

Place the particle in a platinum crucible and treat with 1 ml of

digestion mixture; evaporate to copious fumes of sulfur trioxide in sn

sluminumblock adjusted to 350°C. After the organic matter is ashed,

treat the residue with several drops of cone. hydrochloric acid and

evaporate to dryness. Dissolve the residue in 100 microliters (0.1 ml)

of dissolving acid mixture, using a platinum stirring rod to wash down

the sides of the crucible. Transfer a 5 microliter (0.005 ml) sliquot

to a tantalum planchet and evaporate to dryness for alpha counting.

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Place a third 5 microliter

to be counted for beta and

Filter Papers

aliquot on a 7/8 inch dismeter glass filter

gamma snd followed for decay.

This technique is applicable provided no large amount of foreign

material is on the filter sample. Fold carefully paper swipes, air

samples, and filter paper or other cellulose ssmples; place in a

platinum crucible; wet with cone. nitric acid; and evaporate to dryness

at l~°C. Repeat the acid-evaporation until only a small emount of

char remains in the crucible, then tid 2 ml of digestion mixture ~d

evaporate to copious fumes of sulfur trioxide. Treat the residue with

several drops of cone. hydrochloric acid and again evaporate to dryness.

Dissolve the residue in 100 microliters of dissolving solution} careftiy washing down the sides of the crucible with a platinum stirring

rod. Transfer a 5 microliter sliquot to a chromatographic strip.

Transfer a second 5 microliter

evaporate to dryness for alpha

diquot on a 7/8 inch dismeter

al.iquotto a tantalum planchet and

counting. Place a third 5 microliter

glass filter to be counted for beta and

gamma and followed for decay and growth.

Glass Fiber Filters

Fold the glass filter carefully, place in a platinum crucible,

and hold in the crucible with a stirring rod. Slowly add cone. hydrofluoric acid until the filter is completely disintegrated. The HE’must

be added to the filter cautiously, because the exothermic reaction

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between the HP and the filter fibers causes evolution of a large amount

of free hydrogen fluoride.

After the filter is completely wet with the Ill’,place the crucible

on a heating block at l~°C. and evaporate to dryness. Add several

drops of digestion mixture and evaporate again to dryness. When dry,

or when fumes of stiur trioxide no longer are visible, add 2 to 3 ml.

of cone. nitric acid and several crystals of boric acid, waxm, dilute

to about 10 ml with water, and warm again. Transfer the solution to

a Lusteroid centrifuge tube and centrifuge. Transfer the supernatant

solution to a clean platinum crucible. Wash the residue out of the

Lusteroid tube with several drops of cone. HE’and seversl ml of water,

and transfer it to the

1 ml of cone. sulfuric

to the same centrifuge

natant solution to the

original platinum crucible, treat with about

acid, heat to boiling, then transfer with water

tube and centrifuge again. Transfer the supersecond crucible and evaporate the combined washings to dryness. Treat the residue with sulfuric acid and hydrofluoric

acid until sJ.1of the silicates and silica have been volatilized. After

sll the silica has been removed, evaporate the sulfuric acid, dissolve

the residue in 100 miczmliters of the dissolving acid, and place a

s microliter sliquot on a chromatographystrip. Transfer a second

5 microliter aliquot to a tantalum planchet and evaporate to dryness

for alpha counting. Place a third 5

diameter glass filter to be counted

for decay and growth.

microliter aliquot

for ‘alphaand beta

on a 7/8 inch

end followed

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Chromatography

Place 5 microliters of the sliquot to be tested on CRL/1 chromatography paper. Prepare the paper by drawing a line with absllpoint

pen across sJJ.12 strips, about 3 mm above the cut. place the ~iquot

over the line; add a second 5 microliter sliquot to the strip if the

activity is considered too low for the counting technique to be used.

The sulfuric acid that is present will.char the paper if allowed to

stand more than several hours in the open. Make the chromatogrsm as

soon as possible after adding the aliquot.

Label the strips with a pencil and chromatographyby curving the

paper snd placing it in a polyethylene chamber (one quart Teflon storage bottle cut flat on the top proved the best chamber for this purpose).

The solvent system should be about 1/4 inch deep in the chamber. Cover

the chamber with a glass plate or watch glass ad allow the solvent to

migrate to within 0.5 cm of the top of the cut. The front of the solvent is visible only by the migration of the blue from the ballpoint

ink marking (the point of addition is marked by a black line). Air dry

the paper for seversl seconds to remove the excess acetone and then

expose to ammonia vapors in a similar chamber in which cone. smmonium

hydroxide is contd.ned in a small beaker. Fan the ammonium salt fog

out of the chamber occasionally to observe when the paper is completely

neutralized. Remove the paper and cut into strips; measure in mm and

record the distance from the point of addition to the front. Tape the

strip on a drum counter calibrated so that the front of the chromatogrsm

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can be marked on the accompanying count-rate recorder. After making

the activity record, cut the paper according to the distribution of the

activity. The predetermined cutting points are:

‘f Possible Element

0.00 to 0.10 Y, Ba, Ce, Sr, R, Te

0.10 to o.~ La, Zr

o.~ to O.go Ti, Sb, Mo

O.$X)to 1.00 Ta, W, Se

Package each of these areas in a nylon ring snd disc assembly, and

count for beta activity in a plastic scintillation counter. Compare the

total activity to that in the direct-plated sliquot to determine the

ratio of

to gslmna

present.

the activities, then submit the sections and the direct plate

spectrometry for more precise identification of the isotopes

Because of the fractionation that occurs in the originel sample

during the ashing and dissolving of the filtersJ take aiklitiomil.aliquots

at 3, 6, 12, 24, and ~ hours tier plating the first ssmple. Follow

the chromatograms for decay in order to establish the relative growth

and decay of the activity with respect to the direct plate. The additional eliquots are for establishing with certainty the original constitution of the activity present. Soon after fission the migration

of daughters of the elements having an Rf of O will cause a diffuse

pattern of activity. For exsmple, the daughters of tellurium would be

distributed from Rf O to Rf 1 because cesium has an Rf of 1, snd tellurium an Rf of O. 41

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REFERENCES

10 Jordan, H. S., et al., “Radiation Measurement of the Effluent from

the Kiwi-A Series of Reactors,” Ios Alsmos Scientific Laboratory

Report, LAMS-2588, June 29, 1961.

2. Feather, N., Nuclear Stability Rules (Cambridge University Press,

New York, 1952).

3* Glendenin, Lawrence E., “Determination of the Energy of Beta

Particles and Photons by Absorption,” Nucleonics ?, lZ?-32(1948).

4. Skillern, Clarence, “How to Measure Beta Activity of Fission

Particles Using Film,” Nucleonics IQ, ~-~ (1955).

5. McClelland, J. (Ed.), “Analytical Procedures of the Industrial

Hygiene Group,” Los Alsmos Scientific Laboratory Report, IA-1858

(2nd ed.), August 19~.

6. Mackin, J., P. Zigman, D. Love, D. MacDonald, and D. Ssm, “Radiochemical Analysis of Individual FaXlout Particles,” J. Inorg. Nucl.

Chem. ~, 20-36 (1960).

7“ Ritchie, A. S., “A Paper Chromatographic Scheme for the Identification of Metallic Ions,” J. Chem. Ed. Q, 400-405 (1961).

42

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8. Grand-Clement, A., et d.., Proceedings of the SWP osium on Microchemistry, “Paper Chromatography of Inorganic Ions -- XVIII Separations with Some Solvents Containing H??”(Pergamon Press, London,

1958), p. 231-242.

9= Oncescu, T. snd S. Zwiebel> “The Relation Between Rf Values and the

Composition of Isopropanol-HydrochloricAcid (1:1) Mixtures Used

as Eluant)” Z. And. Khim. ~, 44)9-412(1960).

10. Hunt, E. C., A. A.North, and R. A. Wells, “Application of PaperChromatography Methods of Anslysis to Geochemical Prospecting,”

Analyst 80, 172-194 (1955).

43

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w’

g

N m =t In w t- Cn n

I-1

0

44

APPROVED FOR PUBLIC RELEASE
b

‘j

$

Ha

~

ii

ij

f%i

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.

H

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N’

88

1+

N’

46

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TABLE II ● RATIO OF NUCLIDE ACTIVITY TO TOTAL GAMMA ACTIVITY

Particle No.

1

2

3

4

5

6

7

9

10

u.

12

13

15

17

Peak 0.75 mev

o ●l12

0.111

0.090

0.099

0.115

0.109

0.109

0.0

0.0

0.093

0.080

0.135

0.105

0.121

~eak1.6mev

o ●014

0.025

0.019

0.023

0.036

0.017

0.020

0 ●0

0.0

0.024

0.022

0 ●022

0.021

0.017

)oublet1.1

and 1.2

0.349

0.413

0.289

0.321

0.303

0.346

0.348

0.3574

0.354

0.316

0.284

0 .31.I.

0.279

0.281

Beta Activity

(d/m) n/7/60

32 days past O

69,977

326,457

276?395

61,980

76,302

4,97

2,331

68,612.

77,435

89,502

156,~5

61,620

310,529

522,155

47

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TABLE IIIo EQUIVALENTBETA ENERGY (from loss of activityby aluminum

absorbers)

Psrticle

No.

1

2

3

4

5

6

7

8

9

10

11

12

I-3

14

15

16

17

~#37

Ta182

Loss of

99.0$

A&ivity

E=

Absorber Energy

mg/cm2 mev

323 0.82

420(@$) 1.07

3@ 0.87

285 0.77

525 1 ●17

Activitytoo low for counting

Activitytoo low for counting

675 1.5

575 1.32

675 1.5

380 0.95

460 1.1

450 1008

740 1.5

455 1.12

Used for chemicalanalysis

490 1.16

185 0.56

350 0.9

Loss of

50.0$

Activity

Absorb r

E

Energy

mg/cm mev

22 0.12

10 0.083

26 0.147

25 0.146

45 0.21

20

30

22

40

&l

45

30

42

44

15

17

0.125

0 ●16

0.135

osg2

0.25

0.21

0.16

0.20

0.21

0.106

0.125

48

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APPROVED FOR PUBLIC RELEASE
49

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TA.mE v. ALPHA AND BETA ACTIVITY OF SELECTED PARTICIWS*

Particle

No.

2-A

xl.

6

1

12

3

d/m

-X+

sl.pha

732.

640.

18.8

96.

872

704

d/m

beta

39,140

18,300

1,310

7,640

24,500

41,200

beta-alpha

ratio

53.6

28.6

69.6

79”7

28.1

*Plated directly on 3/4” tsntslumplanchets

*Confirmed as U by ion exchange procedure

50

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TABLE VI. SPECTROGRAPHIC ANALYSIS OF PARTICLE 14

ELmm

Tantalum

Niobium

Platinum

Titanium

Silica

sodium

Aluminum “

Calcium

Iron

Rhodium

Zirconium

CONCENTRATION RANGE

Greater than 10?

1- 10$

0.1 - 1$

0.1 - 1$

0.1 - 1$

0.01 - 0.1$

0.01 - 0.1$

0.01 - 0.1$

0001 - 0.1*

0001 - 0.1$

0.001 - 0.01%

No detectable lines observed for: Li, Be, B, p,

Sc, V, Cr, Mn, Co, Ni, Cu, Zn, Sr, Y, Mo, Ru,

Pd, A& Cd, In, Sn, S%, B%La, Hf, W, Ir, Au,

I%, Bi, Th, and U.

51

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‘lXf3LE1. APPENDIX D. Rf VALUES OF IONS IN HC1-HF-ACETONE-HOHON

PAPER CHROMATOGRAMS

Rf Value Ions Rf Value Ions

1.00

1.00

0.94

0.93

0.$32

o.g2

O.go

0.86

0.85

0.82

0.82

0.82

0.77

0.68

0.65

0.64

0.64

0.64

0.62

0.59

SeO ‘2

3

Ta+5

+2

M

~+5

Pt-2

Hg+l

M004“2 Comet

Zn+2

Fe+3

pd+3

s~+3

Sn+2

~n+3

Cd+2

(la+3

AS+3

~. +2

2

Ti+4

v+5

pa+5

AS04-3

0.46-0.59

0.48

0.48

0.48

0.46

0.45

0.29

0.27

0.25

0.22

0.16

0.05

0.05

0.04

0.03

0.03

0.03

0.02

0.0

0.0

Ag+l

Pbi-2

+4

Zr Comet

S04-2

+4 Hf comet

CO+2

Ge+4

cr+3

Mn+2

+2

Be

TeO ‘2

3

~+1

Rb+1

Li+l

Ni+2

Mg+2

CS’-l

fi+3

+2 +2 +2 Ca Sr Ba

~+4h+3ce+3

~+3 SC+3

52

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Friable Black Granular Particle

*4J ,

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Photograph 2. particle 8

Balck GranularParticle with White Added Residue

54

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. . . . .

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Photograph 3. Particle 4

Black Granular Particle with Metallic Luster

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Photograph 4.

Polaroid Film Radioautograph

Enlargement of a rsdioautograph on Type 57 Polaroid negative- ‘I’hesolid

black, irregular shape is a facsimile of the particle used. (The radioautograph would be reversed on the negative.)

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