either estimate the maximum radiation dose that could have been
incurred under plausible circumstance by any member of the class, or to
estimate the radiation dose to members of the class more precisely than the
maximum dose estimate. However, at least some DuPont operational
records, as distinguished from individual records which were all destroyed,
have survived. Reference is made to the Weekly H.I. Reports on the 200
Area for 1-5- -13-, -1115-DEL. These reports indicate
there is a reasonable likelihood that such radiation doses as revealed in
these reports would have created a Health Endangerment for the
Hanford DuPont workers, but does not show levels of exposure similarly
high to those occurring during nuclear criticality accidents.

Consequently, there is no basis upon which to calculate generic or
individual external or internal exposures to DuPont workers at Hanford,
and since all the records of Hanford DuPont workers have been destroyed,
their inclusion as a Special Exposure Cohort is mandated by this lack of any
reliable data. The destruction by DuPont of Hanford worker records was a
shameful act for which the workers should not be penalized. To give the
worker the legally mandatory benefit of doubt, unencumbered by specious
assumptions, would be to establish the class of all former DuPont workers
at Hanford as a Special Exposure Cohort. .

Respectfully submitted by undersigned Petitioner on behalf of all
the former DuPont workers at Hanford, as authorized in the
attached Petitioner Authorization Forms signed by the following named
former DuPont workers or their Survivors:

1 . .. ,, Survivor of DuPont employee - _.__.

2. 1 _ Attorney-in-fact for } Survivor
of DuPont employee’ = _

3. tvivor of DuPont employee : 7

4. _ Survivor of DuPont employee i .-.-..--- _.

5. , Survivor of DuPont employee '

6 Le, * on, Survivor of DuPont employee ______.

, ~--, Survivor of DuPont employee!
"former DuPont employee.
_ Survivor of DuPont employee! ~

7 tae

9s

Page 20 of 21



the former using grasses and brush on a routine basis over a network of such locations, creating a
large body of historical biomonitoring data.

To a lesser extent, measurements of selected nuclides including radioiodine were attempted
in the 200 plants’ exhaust stacks although few reliable results are available as part of the historical
record of iodine releases, Monitoring of I-131 presented a number of setious problems: stack
measurements were complicated by little-known differences in chemical state of iodine as it was
released from fuel dissoivers and subsequent Pu extraction processes; air flows in the stacks were
‘very great and difficult to sample representatively and bulk chemicals and other long-lived nuclides
were also present. The I-131 released fiom fuel and dissolver solutions was mainly divided among
the species: volatile iodine, inorganic iodide, iodate, Cl-I and organic-I, and the filters and liquid

+ scrubbing devices deployed both for entrapment and stack monitoring had varying efficiencies to
retain the airbome 1-131 and associated aerosol droplets and particulate forms (Ma88]. Organic
iodides in particular were not appreciably sorbed by water scrubbers or fibre filters, Records indicate
that relatively little attention was paid ta this problem of the chemical states of radioiodine other than
to recognize that some fraction was particulate and aerosol spray that needed filtration; a few stack
tests were made with hydrazine scrubbers which were thought to be capable of distinguishing organic-
I, although this was not standard practice, then or since.

Direct counting of stack-monitor filters and of pellets of vegetation using beta counters was
the principal means of detecting I-13 1 during the first five years [Ma89] but this procedure led to very
large underestimates of iodine emissions mainly because of detector calibration uncertainties and 60-
70% beta self-absorption of low energy I-13 1, complicated also by some interference from long-lived
nuclides such as Ru. Correction factors of 3.3 and higher were required for radioiodine
measurements before 1948 wher a chemical extraction method was introduced but even then, iodine
extractability and radiochemical yields were variable and uncertain and it was not until a non-
destructive gamma-spectrometric method based on the 364 keV y-line was adopted in 1958 that it
was found that the prior methods, even after earlier correction factors were applied, had been
yielding low results by a further factor of 1.6 {Ke94}. Documents show that many filters and monitor
samples were measured by direct B-counting from 1948-58 because the chemical-extraction

_ procedure was time-intensive, ‘In addition to errors from counting, later tests showed that stack
monitoring through long narrow sampling lines caused low 1-131 levels to be found in the monitor
filters and bubblers by as much as 50-70% (in addition to the 60-70% losses due to beta self-
absorption from direct B-counting of filters.)

These observations about the difficulties encountered in monitoring I-131 emissions up until
1958 are highly relevant to HEDR estimates of 1-131 releases from the B, T and REDOX plants after_
1948 because attempts to measure the iodine removal efficiencies of the gas scrubbers, sand and fibre
filters and silver reactors also depended on the accuracy of radiochemical assay procedures. During
the first 3+4 years of Pu extraction at B and T plants when about half of the total fuel extracted there
had been processed, most (~90%) of radioiodine escaped from the dissolvers and subsequent
processing cells without any removal or containment devices installed. Subsequently, dissolver gas
scrubbers(‘48), sand beds(‘48) and glass fibre filters(*50) progressively reduced I-131 emissions to
about 25% until the end of 1951 when columns containing layers of silver nitrate backed up by filters

132i



dissolvings in a month. For instance, with T,y = 48 and T,,,, = 32, the formmla give T = 44.5 d
whereas the calculation above for 17 dissolvings and the sane 48 and 32 days is 44.9 days. Thus the
T release calculated using this Ty is lower (by a few percent) than that calculated by the long method
above.. As either method is assuming, for instance, a regular dissolving (e.g. once every 2 days),
small uncertainties are inevitable and acceptable.

From T, and T,, can be calculated factors to modify or correct the HEDR release; the
correction is exp {-0.0862 (Ty, - T,y)}. But for correction of Tay to Ta, Trin '8 required. In the
period 1950 - 52 these values are not available. If everything was so organised, it might be that in
amonth AT=T,y-T,,.= 14 or 15 days; or considering new pushes every week, it is perhaps 3 days;

* of course it might be that in some months very old or very green fuel might make AT longer - and
“ off-days” could result in a smaller AT than usual or indeed in a longer AT than necessary. Taking
as examples AT = 15 and AT = 10 and AT =3, T, - Tq, equals 12, 8 and 1.9. The effects of these
effective 3, 2 or 1 days less cooling are that 1.29, 1.19 or 1.10, i.e. 29%, 19% or 10% more I is
released than predicted by T,y.

Are these values of AT reasonable? From the above it seems so. Also in 1953 for the T plant
the average monthly AT for the 12 months is 14.3 d, in the Redox plant 11 days, giving effects
(correction factors of exp[-0.0862 (Tg - Tay)]) of 1.39 and 1.29 respectively.

Realising that the total dose is the important parameter, and that taking a reasonable average
will smooth out month to month variations, it ig reasonable to use a correction factor of 1.25 for the
years 1950 ~ 52: prior to 1950, batch-by-batch calculationsghouldzhave avoided the use of average

“ cootmg times and therefore its complications, and 14: vakies for 1953 - 1956 obtained from the T
“plant and Redox data of HW 89085 (Gydesen 1992) can be used.. Correction factors for this
exponential cooling time effect (ECT factor) are given in the Table 2 (column +).

D.3 First In First Out Protocol ; ‘

A variation on the average cooling time problem is violation of the First In First Out (FIFO)
protocol assumed by HED Reconstruction when batch-by-batch data is not available and so
assumptions, such as of orderly queueing, had to be made to reconstruct the sequence of events such
as cooling, dissolving, and extracting. To illustrate this, consider a series of batches of shigs which
have all had different cooling times to this minute, and bave activities in the ratios 1:2:4:8. If these
are dissolved at 8 day intervals in the above order, the I release will be 1+ 1+1+1=4 in some
appropriate units. If however order is, by mistake, changed, so that the fourth one is dissolved first, -
the release will be 8 + 0.5+0.5+0.5=9.5. Even if simply the second and third are interchanged,
the release is 1+2+0.541=4.5.

It is clear that a mistake, such as the one made in September 1963 [Soldat 65], will not only

produce a very sharp spike of activity at and after the day of dissolving, but will also increase the total
activity emitted,

In HW 83869, Aug. 31, 1964, it is stated that “From time to time a quantity of incompletely



G. Thyroid Dose Estimations
G.1 Doses within § years

Previously the source term for emission of 1-131 from Hanford in the years 1944 to 1956 has
been estimated based on modifications of the HEDR estimate. To obtain doses to individuals from
this information requires knowledge of distribution of radioactivity, probability of uptake in animals
and man, and distribution and metabolism in the body, as well as biological and nuclear parameters.

, These (intermediate) steps have been taken by HEDR and others building on HEDR.
Accepting the general correctness of these steps, (after ourselves doing scoping calculations) and
assuming that general wird patterns and weather conditions and feeding patterns do not change
markedly from five year period to neighbouring five year period, we can calculate the estimated dose
as a function of site resulting from our corrected source term by a linear modification of the HEDR -
based doses calculated by Shipler et al. (1996) and Farris et al. (1996), substituting the present
emission estimates for those of HEDR.

To explain the steps taken here, we have to note that the radiosensitivity of thyroid tissue
depends on age of the individual - young children are more susceptible than adults. We also note the
concept of “doubling dose’, the radiation dose level (at which, and) abave which it is more likely than
not that an existing thyroid cancer would have been caused by radiation rather than by any other
normal source. While we do not necessarily subscribe to the particular dose criteria or Doubling
Dose concept previously adopted by the Court, even under such standards and concept, thyorid
cancer causation could be expected throughout much of the study domain. Judge Macdonald has
taken that the relevant doubling dose is, for children of up to 0 ~ 4 years old at the time of exposure,
five rads to the thyroid. For children 5 years to 9 years, the doubling dose is 10 rads, for those 10 -
19 33 rads, and for adults 100 rads.

Concentrating initially on the youngest children, we have calculated moving (or rolling)
summations of source term emitted in 5 year periods starting 1940 to 1944, finishing 1952 - 1956.
(See Tables 3 and 4) We have also tabulated (Table 5) these 5 year rolling totals divided by the 728
746 Ci estimated by HEDR to have been emitted in the 7 years + 1 month between Dec. 44 and Dec.
51 to aid (see below) in depicting dose distributions to persons.

We have also noted that for children born 26 December 1944 Farris depicts distributions of -
doses given from Dec 44 to Dec 51 (7 year plus t month, or more exactly 7 years plus 6 days). The
HEDR emission in that period is 728 746 Ci. So we bave here from Farris a relation between
emission and dose to a child at a particular site. Use of the corrected emission over the 5 years after
birth gives a corrected dose for that site to a 0 - 4 year old at that place.

As noted, Farris bas given a drawing of dose distribution, with iso-dose contours. For this
drawing to illustrate the corrected doses, the contours may be re-designated; thus a Farris 100 rad

iS



Till, 2002, created a spreadsheet based on Heeb’s figures to show
total monthly releases from routine operational releases of each nuclide.
He also described what he termed “Unusual Release Conditions” in which
particles containing various radionuclides were released from B & T plants
in early operations, but concluded that “the process could not be

reliably modeled.” Till 2001 Draft, Pg. ¢ 2-22 . (bold emphasis added)
The following citations were taken from RAC Report No.2-0e

Final Rey -M th for ting g Radiati ion from Shi
Ga: Radionuclides and Radi the -
Atmosphi rin: Hanford erat ns , Till 2002:

“Heeb (1904) made estimates of radionuclide input to the fuel
dissolution process and those are tabulated in his report.” Till 2002, Pg.

#2-24.

“Monthly listings of the inputs of *°Sr, "Ru, Ru, “Ce, and *°Pu for
the T Plant, B Plant, and REDOX Plant were compiled for the period
December 1944- February 1961 from tables given in the report by Heeb

(1994).” Till. 2002, Pg. #2-24.

“Releases from T Plant. Monthly releases were estimated
throughout the period of operation of T Plant, from late 1944 to early 1956.”

Till, 2002, Pg. #2-27.

“Deposition density is the number of particles detected per unit area
of ground surface. Section 4.1. 6 contains a review of available data.” Till,

2002, Pg. #3-39.

“Beta activity. Document HW-9871 presents summary tables of
beta activity collected on ambient (i.e., in the outside environment) air
filters between January 1946 and April 1948 inclusive. Air was sampled
continuously through a filter of about 1-1/2 inches diameter at a flow rate of
about 2 ft? minTM. The filters were counted directly on thin mica-window
Geiger counters. The sampling frequency was weekly (HW-12677, HW-
13743), and the reporting frequency was monthly. The samplers were
located under a protective cupola type roof (HW-13743). At that time,
corrections to the measured count rates were made for geometry, collection
efficiency, and radioactive decay, with the assumption that all beta activity

Page 14 of 21



Contents

Page No.
Summary 3.
Academic and Professional Experience 4, 5.
A. Introduction 6.
B. First-in-First-Out (FIFO) Violations 7.
C. Exponential Cooling Times (ECT) Corrections 7.
D.Lag Time (LAG) Corrections 8.
E. Radioiodine Release Factor (RF) Estimates 8.
° E.1 Fiber Filters 9.
° E2 Water Scrubbers and Sand Beds 9.
¢ E3 Silver Reactors 10.
¢ E4 Organic Iodides 10.
1. ¢ E.5 Computation of Release Factors 12.
- F. Radiation Doses to Population Groups 14.
« F.1 General 14,
F.2 Consequential Thyroid Doses... 14.
r . F.3 Dose to An Adult at Ringold (1950-56) 15.
D. Conclusions 17.
E. References 17.
J. Consultants’ Statement 20.
K. Appendix 21.
L. List of Tables 24.

Lists of Documents Received



Academic and Professional Experience: K.G. McNeill

A brief resume of my academic background is givea here; a full CV is attached®.

I gained a First Class Honours degree in Physics from Oxford UK in 1947. My D.Phil
(1950) was on the D-D (deuteron-deuteron fusion) reaction. Fellowships at Yale and Glasgow UK
preceded a lectureship at Glasgow, then Associate and then Full Professorships in Physics at Toronto.
Honours included visiting scientist status at Melboume, Livermore, Ottawa (in all cases more than
once) Harwell and Saskatoon, and status as Professor of Medicine at Toronto and Special Staff
Member at the Toronto General Hospital. During the Toronto years research has been equally divided
between pure nuclear physics (photodisintegration) and nuclear physics applied to medicine (mainly
in bone disease, particularly osteoporosis).

‘The research work bas resulted in just less than 200 papers published in refereed journals.
There have also been a couple of books, several published lecture notes, and several major reports on
puclear emergency planning. I have been a consultant for safety in uranium mining and for the
Departments of Health and of Labour of the Government of Ontario, for the federal (Canadian)
Auditor General's office, and for the Atomic Energy Control Board.

For the decade or so up to 1997 | was the Technical Advisor to the Solicitor-General of
Ontario with reference to off-site effects of accidents at nuclear power plants - this involved, amongst
other things, chairing the Technical Advisory Committee and half its Working Groups, and some of its
sub committees, dealing with source term estimations, meteorological modelling of distribution of ©
tadioactive emissions, dose prediction and protective actions. I chaired, for more than 10 years, the
University's Radiation Protection Authority (the University has 230 professorial staff licenced to use
radioisotopes).

Iam a member of the Canadian Association of Physicists, of the Canadian Radiation Protection
Association, and (until retirement) a Fellow of the (UK) Institution of Nuclear Engineers.

Tam now an Emeritus Professor of Physics in the University of Toronto.

* (gee attached C.V. for details)



which needed to be applied to the HEDR estimates, deserved re-examination. In particular,
evidence of additional FIFO violations, increasing attention to other chemical forms of

27



the time this decision was made, DuPont had had experience with caustic scrubbers at Oak
Ridge where they had been used from 1944 at the RaLa (X-10) plant according to Hoffinan
[1999; see also, the attached schematics of the RaLa2 plant, 1945; Appendix].

Efficiences of 80-90% for I-131 removal by water scrubbers were not realized in
prolonged operation. Wichuer [2004] reported that, from studies at Oak Ridge, their
efficiencies were found to be unstable and were strongly affected by acidity when operated
in the recycle mode. The kinetics of the I, hydrolysis reactions complicated removal
processes in the scrubbers because, although the first step: I, — 2 I was rapid (reaction
half-time ~ 5 min.) the second reaction: HOI — IT + 10, was very slow.

Hercmann and Herrmann [1996] judged the scrubber and sand bed efficiencies to be
40% and 30% respectively based on much research and operating experiences at German
and French plants. Therefore, and with evidence of much lower operating performance at
Hanford, these (Herrmann) values (40 and 30%, respectively) have been used here for
revised RF estimates for the period May 8 up to Oct 0, when silver reactors were introduced.

£.3 Silver Beds:

Among the choices of media to trap iodine, it appears that silver was not initially
selected although knowledge of classical iodine chemistry at the time would have indicated
that silver ions and silver surfaces would tightly bind iodine from solution or from fumes.
There was much experience from before the 20 century that thin layers of silver iodide on
inert substrates such as were used in the photographic film industry, did not wash off even
with strong acids.

At Hanford, it was discovered through a random observation in some laboratory tests
around 1948, that silver and copper metal pieces in equipment exposed to radioiodine
became highly radioactive. Following some small-scale development work, beds to treat
the off-gases were made up of ceramic pieces ( addles coated with silver nitrate. Initially
in 1950 it was-asserted that 99% of I-131 was removed by these ilver reactors (Wolff, 1951].

However, early in 1951, shortly after their installation, it was found that they were
not performing as expected and that there had been a substantial increase (more than ten-
fold) in 1-131 releases [Pas and Soldat,1951]. These failing reactors were allowed to remain
in operation from Feb 1 to Aug 1 before they were replaced. It was concluded that the
operating temperatures had exceeded 370° F and the silver nitrate had melted and slid off the
coatings [Blasewitz, HW-21959, Aug 1]. The bed failure was detected mainly by off-site
vegetation nionitoring. Also, the beds were subject fo ouling and saturation by AgCl and
Agl. Excess chlorine in the off-gases competed with and replaced iodine atoms for sites on
the silver coating [duPlessis and Sutter.1969]. It was concluded that the Ag reactors needed
to be regenerated regularly after about 140-200 tons of U fuel had been processed [Burger,
1991}. However, there were times during the mid-50 when the beds were not regenerated
until after 600-800 tons had been dissolved [Warren,1961]. Burger also stated that the main
function of the Ag reactors was to hold 1-131 long enough to decay, not for the long term as
long-term buildup was marginal and used beds contained mostly AgCl, (less than 2% was



~ Exhibit C



/

Okt ASIN

ea Ds i HW-Yph10

J ) In the research leboratory, Redox studies heve eliminated previous concern ebout

fo + possible plutonium precipitation im product streams, and edditionsl acrvenging and
ozonizetion date heva been obtained, TEP process studiea have included dispersion”
atndies in liguid-liquid extractors, ecid buty) phosphates formtion ond properties
fluoride complexing, end decontemination behavior of various TBP diluents, Process
scouting for Blig. 234-5 operations has involved studies of nitric acid recovery =
leaching of sleg and crucible wastes, “slectroless" plating of nickel on plutonium,
and coupling of Redox solutions to Bldg. 234 operetions. Varidus potentiel methods
of separating aluminum end 0235 are being investigated as 2 necessary requisite to
the development of a more desirable proceaa for tha recovery of "25," .

pomrphebnicel Dirisions

In the 234-5 procese development leboretory, the study of substitution of peroxide
for oxelote purificetion hes been continued. A design basis for plutonium "ekull"
recovery hae been iasued. Considerable improvement hes been made in producing
Plutonium cores that will pess through the "Go" gage in ali directions. Impreve- “- >
ments in rediograthic methods end techniques have been obtained. - ,

Inveatigetion of sub-norml T Plent send filter efficiencies has reveeled the fil-
ter to be saturated with weter from steem leaks into the ventiletion duct and
previous cell flushes. Unnsuclly lergs quentities of iodine have been trepped in.
the filter end eppecr to ba the ceuse of low “apperent” filter efficiency. The
steam leaks have all been corrected and the filter bed is being dried out slowly.
Pilot runs on the silver reactor for iodine removel and Fibergies particle filters
are being eccelercted,

. >) Tochnical Services Division.

Role laborstory design work continued in the Analytical Section on © 6-dey week
vasia, and fabrication was initieted on several phaees of the necessery mock-up in
Bidg. 101, Semple sizes end anelytical methods continued under study, and tech-*
miques were proposed for the edequete evaluation of total iodine and 1131 in gnees
to be evolved during the disaolution of Rala slugs.

Jhe spontensous fission counter wes received from KAFL end is being installed in the
© Plant control leboratory for Anclyticel Section use with the alpha pulso cnelyzer

a in the déteriination of individual plutonium isotopes in Hanford procese materials,

The Anelytical Section has initiated 2 survey of cll sanslyticel procedures present-
ly employed in the control of the scperaticns process,. vith a view to introducing
improved mothods wherever possible, Particuler ettention ie being given initially
to the AT assay.

foueat te @ Du Pont Compeny of 2.
accumulctea by the Operetion's Centrel Files during Du Pont‘a tenure ct Heaford was
wade on Merch 29, Thie matericl, comprising 263 packing ceses, covers the period

from the fcll of 1943 through August 31, 1945. Only about 4 pecking ceses, consiat-
ing of records presenting special documentation ‘obleus remain to be Processed,

designations used et Eenford. Mcotings wore held with representatives frou
Mennfecturing, H.I., Technical, end Design end Construction, and « draft of en
Instructions Letter on the subject ia being prepored.

2B Greningersig . 165616

2 . ae



The factors above have to be further, though only slightly, modified because although most
of the emissable iodine comes out on dissolving, a fraction is emitted at extraction, He92 says that
86% of all I comes out at dissolving and after the lag (He92 used 3 days) 7.5% more is emitted - or
86 + 9.7% = 95.7% is available for emission, of which 86% comes out first, followed by the decayed
9.7%, that is, 7.5%, giving a total of 93.5%. The difference between 95.7% and 93.5% is equivalent
to an effective cooling of all the I by 0,27 days. If the lag time were only 2 days, the
effective cooling time would be increased by 0.19 days,

whereas for 4 days, by 0.36 days
and for 8 days, by 0.61 days

“In the worst case, the last, we are saying that if the extraction time is, say, 96 days, and the lag time
8 days, most of the lis only cooled 88 days, not 96 days, giving an apparent correction factor of 2.0;
however, taking into account hold-up of some of the I, a better cooling time is 88.61 days, giving a
correction factor of 1.9 rather than 2.

For conservatism, we use these slightly corrected factors in the Results, as given in the
following Table 1 and reproduced in Table 2 column 5.

Table 1 - Summary

1945 to Aug. 46 1.0

1946(Sept. to Dec.) | 1.17

1947 1.37

1948-1956 1)

E. Radiodine Releases During Fuel Processing:

From the start of U fuel processing at Hanford, very large, uncontrolled, radionuclide
emissions occurred through the 200-site stacks, notably inert gas fission products (Ep’s) and volatile
forms of radioiodine. Lesser quantities of other f.p’s (Ru,Cs), and of uranium and plutonium were
also released.

Recognizing the potential health and environmental impacts of massive releases of
radioactivity in the Hanford region, attempts were made to monitor such stack losses and to
undertake environmental monitoring to assess whether significant levels of radionuclides were
depositing over downwind areas both on-site and off-site, that is, outside the boundaries of the
Hanford reservation. Vegetation, soil and water monitoring for I-131 and alpha nuclides was done,

10



The longer-lived nuclides created in the reactor available for possible
release are not greatly affected by changes in the cooling times because rate
of decay is not a significant factor. However, for short-lived nuclides, most
particularly iodine-131 (eight-day half-life), the cooling period from time of

. discharge from the reactor to time of dissolving in the separation plants is a
maajor factor in determining the amount of activity available for
entrainment and possible release. ~

One problem with Heeb’s iodine calculations is the difference in
cooling times to be utilized to calculate amounts available to the dissolver.
Heeb changed his cooling times from his 1993 report in which he
recognized a three-day lag time error overestimation, which was omitted
from his 1994 report. He also used linear averaging of monthly amounts
when cooling time is actually a exponential factor, also causing cooling time
overestimation. Further, he failed to account for the out-of-sequence
dissolving order of fuel rods first in the cooling basis to be first sent out to
the dissolver, (FIFO). (See Exhibits B and C for a full discussion by widely
recognized and published researchers in nuclear science and iodine-131.)

The following citations were taken from Radionucli
Atmosphere from Hanford Operations. “1972, C. M. Heeb, May 1994.
Heeb was the principal author of the HEDR project source term.

“Monthly releases of ruthenium-103, ruthenium-106, cerium-144,
strontium-90, and plutonium-239, plus iodine-131 releases after 1949, were

estimated as follows:” (Heeb, 1904 Pg. # 4.3)

“The release factor is defined as the ratio of the radionuclide activity
released to the radionuclide activity processed. Release factors are
calculated from known values over a short period of time. They provide an
estimate of the fraction of radionuclide released from processing
operations. This estimate is then applied to time periods during
which processing data, but no release data, are available.” (Heeb.

1994, Pg. # 4.7)

“A monthly release factor was calculated for each of the six
radionuclides under study in this report (iodine-131, ruthenium-103,
ruthenium-106, cerium-144, strontium-90, and plutonium-239) for each
separations plant in operation. Release factors based on measurements

Page 5 of 21



|

D. Incorrect Cooling Times
D1. Introduction

Very early in our review of the Hanford problems, our attention was drawn to the incorrect,
linear, averaging of cooling times from B and T plants to give a “average” cooling time which could
be used to make calculations easier.

Linear averaging always and inevitably results in an appearance of a longer cooling time than

* is proper and therefore an underestimation of the actual I-131 in the effluent. That this is so is readily

seen if, for instance, one takes equal masses of initial equal unit activity and lets one coo! for 60 days

and the other for 100 days. The two activities at the end of the cooling periods will be 0.0055 and

.00018, total 0.0057 = 2 exp(-0.086 x T), and so T= 68 days where T is the effective cooling time

for the two masses. For comparison, linear everaging, as used in Equation 1 of the HEDR report

" He92, would give (60 + 100/2 = 80 days. The last part of the longer cooling period is effectively

wasted, as there is very little left to decay. The 12 day difference represents for 1-131 a factor of 2.8
in calculated activity.

Although the initial problem was the averaging of cooling times reported for different plants,
it was quickly realized that cooling times given for each plant were themselves averages of the actual
cooling times for individual dissolving, and that these individual dissolvings were made up of slugs
which may well have had different cooling times themselves. Again it is inevitable that linear
averaging of these times will lead to a misleading estimate of an “average” cooling time which is
always longer than the effective cooling time calculated properly, that is taking into account the
exponential nature of the decay. This problem presents itselfin three different ways, discussed below.

D.2. Exponential Cooling Times

For the very early days, when there were few dissolvings, it is possible to examine details and
indeed for the early years HEDR. dees treat batches individually. [He94] (p 4.4) states that "Records
were kept of the amount of uranium fuel dissolved, the burmup of the fuel, and the average cooling
time (General Electric 1948a). Enough of these records survived to permit a daily reconstruction of
iodine-131 from T and B Plant operations through the end of 1949. Thereafter, monthly summary
records only permit a monthly reconstruction of the amount of fuel dissolved, the average bumnup of
the dissolved fuel, and the average cooling time of the fuel throughout the operating life of each.
separations plant.”

For the years 1950-56 there are given the average cooling time for each month (a linear
average) and, for 1953 to 1956, the minimum cooling time for any dissolving in that month.
Considering first slugs from one reactor, going to one dissolving plant, as the rate of dissolving must
be approximately equal to the rate of discharge of slugs from the reactors (otherwise is there would
be a build up of slugs or, alternatively, "days-off"), the most likely distribution of cooling times is
uniform between the minimum cooling time T,,, for the month and a maxinmam Of Tyezage + (Taverge ~
Trin) Le. Tay ~ Trig = 15 days. This is obvious if there were 30 charge-worths of U pushed once

4



__- Presented By:

Attachments:

Exhibit A: Letters Confirming destruction of DuPont Records
Exhibit B: Jervis/McNeill 1999 report
Exhibit C: Jervis/McNeill 2004 report
Exhibit D: A.G. Blasewitz to the EPRP (External Peer Review Panel)
Exhibit E: Drawing attached to Blasewitz letter
Exhibit F: Stack Contamination, Martel, 1948, HDC-611.
Exhibit G: Lindeken, 1961, pg. 44
Exhibit H: Saueressig on 8/15/96
Exhibit I: The History of the Technical Steering Panel 1988-1995, 11/1996.
Exhibit J: J.V. Ramsdell Jr. et al., Health Phys.
Exhibit K: Dr. Till’s deposition admission
Exhibit L: Rood’s Deposition: Excuse for the RATCHET coding error in
Exh. M
Exhibit M: Atmospheric Tracking Code (RATCHET)
Exhibit N: Petitioner Authorization Forms

Page 21 of 21



Depariment of Energy
Richland Operations Office
P.O. Box 550
_Richland, Washington 99352 —

MAR 2 2 HD

FREEDOM OF INFORMATION ACT REQUEST (RL FOIA 2002-0114)

Your letter dated March 5, 2002, was received by this office on March 11, 2002. In that letter
you requested the radiation exposure and employment records for on behalf
of his son. These records are protected under the Freedom of Information Act therefore we have
interpreted your request under that statute.

Enclosed is a copy of” radiation exposure record. We have deleted the names and
other personal identifiers of other individuals to protect their privacy. -

According to the radiation exposure record, was employed by DuPont. It is our
understanding that employment, medical and radiation exposure records of individuals whose
employment terminated during the Hanford-DuPont contracting periad (1943-1946) or who left
Hanford and continued their employment with DuPont at the end of the contracting period were
archived with DuPont and have subsequently been destroyed. You may wislr to contact the -
organization that maintains DuPont's historical records to obtain more detailed information. The
address is as follows: Hagley Museum and Library, Business Archives, Attention Michael Nash,
P.O. Box 3690, Wilmington, Delaware 19807-0630.

We have conducted a thorough search by name and Sacial Security Number (SSN) for
employment recards related to and we were unable to locate any. Therefore, this
portion of your request must be denied.

The undersigned individual is responsible for this determination. You have the right to appeal
to the Office of Hearings and Appeals, as provided in 10 CER 1004.8, for any information
denied to you in this letter or regarding the adequacy of our search. Any such appeal shall be
made in writing to the Director, Office of Hearings and Appeals, U.S. Department of Energy,
1000 Independence Avenue SW, Washington, D.C. 20585, and shall be filed within 30 days
after receipt of this letter. Should you choose to appeal, please provide this office with a copy
of your letter!



rn m-aTho
DECLASSIFIED

March 1950 . 4/10/50
SCMMARY
Pile Technology Division
The major effort of the Physics Section involved plamning for the toeding of the
central 400 tubes of the H Pile for increased P-10 production. Experimental work
in the DR Pile is being plamed to determine the optimm loading errangement.

A large development program for extraction phases of the P-10 program hes been
initieted. .

Improvements heve been effected in ‘the method of cenning P-10 fuelisluge,

An improved Pile stert-up procedure, which has significant adventages over tho
conventional “reduced power” start-up procedure wes demonstrated.

Precise meesurements of the curvature near the imer end of the gun berrel in top ;
central tubes of the piles show that the worst condition prevaiis at the F Pile,
with a radius of curvature of 660 inches. :

Develozment of equipment for insuring complete trensformation of production slugs
is continuing. .

Separations Technology Division

The first of ca. 450 ¥WiD/ton metal ia now being processed in the Separationa Plants

““undet close obsérvation, Tho causea of bigher-than-normal product hold-up obteined

in recent B Plant Acid Wash Runs are being investigated. Metathesis time cycle
shortening by production testing has been setivfactorily obtained and veriations in
the Isolation Building final product solution volume ere being studied via
production tests in an effort to improve product accountcbility and tranefers be-
tween Bldgs. 231 end 234. ‘Iniprovements in Bldg, 234 Dry Chemistry conversion
yields are being attempted. Accumlated "scow sweepings" from Dry Chemistry .
operations have been seperctely redvcod to plutonium metal buttcns,which are being
stored for future recovery operctiors. .

In Redox and Metal Waste Recovery process development, sixty-one additional

solvent extrection colum runs were made during the peat month, el] on TBP procesa
studies, Packed colum performnce with Shell Deodorized Spray Bese ag tha TBP
diluent wes pourer than that with Stodderd Solvent previously reported. Additioneal
pulse colum runs under optimm conditions heve produced weste loeses of 0.1 - 0.2%
for both the RA end RC Colume for effective “packed" heighta of only 5.4 ft.
Redox pump testing has edvenced satiafactorily to the point where pump specifica-
tions for Production Flent deaign cre now being established.

165615

1 _ |

t" $a



every month (i.e. 30 x 3.3 tons), as when each successive charge is dissolved the cooling time will
have been determined to be one day longer than that of the previous one, and so for all 30. With
fewer than 30 charges, some gaps may occur, days without dissolving, but this will still lead to a
flattish, though irregular, distribution; it is not possible to have two charges at the same time, and
therefore two identical cooling times. Jt means that the (linear) average cooling time is longer than
it could otherwise be, the maximum cooling time is also increased and so is Tay ~ Trig With two
reactors supplying U to the same dissolving plant, there is the possibility of two charges with the same
cooling time, but still an inevitably flattish distribution of cooling times. (As will be discussed later,
there may be by accident (or design) gross errors in the orderly dissolving routine - see First In First
“Out Protocol).

To illustrate the effect of distribution of cooling times, take a very simple distribution of 3
- charges of initial activity equal to unity dissolved after cooling times of 40, 48 and 56 days
respectively. The linear average cooling time is 48 days, suggesting a released activity of 3 x (1/2*)
= 3/64 = 0,047, However the actual release will be (1/25 + 1/25+ 1/27) = 0.031 + 0.016 + 0.008 =
0.055, 17% more than suggested by the linear average and with an effective cooling time of 46.2 d.
The situation would be much worse if the difference between the minimum and maximum cooling
times were about a month, 32 days. Then the cooling times for the three charges could be 32, 48 and
64 days, giving a real emission of 1/16 + 1/64 + 1/256 = 0.063 + 0.016 + 0.004 = 0.083, 75% greater
than predicted by the "average" cooling time of 48 days and giving an effective cooling time of 41.6
days.

This 75% increase is also much greater than the 17% calculated above: that is, the minimum
value of cooling times is important as well as the linear average in the determination of the correct
effective cooling time, Ty, (Le. taking into account exponential decay). Furthermore, note that if
there were 5 dissolvings of equal initial activity and individual cooling times of 32, 40, 48, 56 and 64
days the linear average cooling time is still 48 days, and the minimum still 32, but the real emission
Of 1/16 + 1/32 + 1/64 + 1/128 + 1/256 = 0,0625 +.0.03125 + 0.0156 + 0.00781 + 0.003906 = 0.121.
On the linet averaging basis, the expected dose would be 5 x 1/64 = 0.078. 0.121 is 55% greater
than 0.078 (Le. ratio is 1.55). Thus the number of dissolvings is alse relevant. Thus with cooling
times of 32, 36, 40, 44, 48, 52, 56, 60 and 64 days the linear average is still 48 and minimum 32, as
before. But the real emission is now 1/16+ 1/26.6 + 1/32 + 1/45.25 + 1/64 + 1/905 + 1/128 + 1/181
+ 1/256 = 0.0625 + 0.0442 + 0.031 + 0.0221 + 0.0156 + 0.0110-+ 0.00781 + 0.0055 + 0.003906 =

0.2036. Ona linear average basis, one would expect 0.141. The correction ratio is 0.2036/0.141 =
1.45.

Fora large number (N >> 1) of dissolvings the exponential average T, may be calculated from

the equation
i 2A (Tay ~ Tria) |
Te = Th, +> fa | ——_ +
® a eee lav ~ Tra)

T, derived from this formula is slightly higher than that calculated using a finite (< 30) number of



“The TSP identified seven priority tasks to be completed before the
panel could say that dose reconstruction models and data could be
used with confidence in Hanford health-related work. The CDC plans
these tasks to be performed by outside contractors. The seven key
issues are, in order of priority:

Air model concerns. Many people remain concerned about,
‘disappearance factors’ - the inconsistencies between measured and
predicted deposition of iodine in the 1940's - and the role weather
and topography may have played i in the amounts and locations of
radioactive iodine deposited.” See Exhibit I, Reconstructing

Hanford’s Past Releases of Radioactive Materials: The History of the
Technical Steering Panel 1988-1995, November 1996.

It will be noted that the adequacy of RATCHET was the number one
concern needing correction. Even its author, Van Ramsdell, acknowledges
under-estimates generally within a factor of four, but up to a magnitude at
the more distant domain locations. See Exhibit J, Atmospheric Dispersion
and Deposition of 131-I Released from the Hanford Site, J.V. Ramsdell Jr.
et al., Health Phys. 71(4):568-577; 1996. However, although number one of
the concerns of the TSP and the CDC, RATCHET was never changed! See
Dr. Till’s deposition admission, Exhibit K.

2) The code for RATCHET contains a mathematical error in the plume
depletion equation which doubled the rate of plume depletion. According
to Arthur Rood, a member of Dr. Till’s scientific team, Ramsdell admitted
this error in his code and that it was never corrected in his report, but he
claimed, however, that the way he ran the code the error was compensated
by another factor that exists in the code. See deposition Exhibit L for full
elaboration.

3) The problem with ORAUT’s approach is that using a one micron size for
particles ignores the fact that many plutonium particles were less than one
micron, and the average sizes of the ruthenium particles has not been
characterized by any studies. Also, there is no data to support deposition
tates for ruthenium or plutonium which were apparently just speculated as
being equivalent to the combined deposition rates of the three species of
iodine-131 (elemental, aerosol particles, and organic).

Clearly, ORAUT’s atmospheric dispersion factors were developed on

Page 18 of 21



D. Lag Time Correction Factors:

Similarly, the ag time correction factors which ranged from 1.0, 1.17, 1.37 to 1.9 have
not required further revisions here and are shown in Column 5, Table 3.

E. Radioiodine Release Factor Estimates:

The estimations of Heeb, [1993] and [1994], of emissions of I-131 from the Hanford Site
200 plants formed the basis of the calculation of doses for the HEDR94 and the Hanford
Thyroid Disease Study [HTDS, 1999] and also, of Napier re-evaluation [Napier, 2002].
Questions have arisen since as to the accuracy and variability of these estimates, In a
previous report [Jervis,1995], errors in 1-131 stack and vegetation measurements were
addressed in detail.

Napier [2002] reviewed the basic HEDR approach of using eneric release factors for the
various removal devices, presumably based on historical records, and proposed instead an
alternative approach using stack measurements. Heeb[1994] had calculated the total —_I-
13] inventory in processed U fuel from reactor power, irradiation and cooling time histories
and then estimated the fraction of total iodine released to the atmosphere using RF, release
factor values which he claimed were supported in part by historical stack data. . Napier 2002
claims an independent approach to the calculation of the amount of radioiodine emitted to
the atmosphere, based on historical stack measurements and verification of estimated
emissions based on atmospheric monitoring at sites some kilometers from the Hanford site.

Initially, from the 1944 startup until water scrubbers and sand: beds were used in 1948,
HEDR estimated that most (~90%) of 1-131 contained in the fuel had been released from the
dissolvers and subsequent processing. After the scrubbers and filters were introduced,
HEDR release estimates were reduced to about 30% and after silver reactors started to be
used (1950-51), to about 1% of I-131 released from fuel.

This approach of HEDR had a number of substantial errors, including:

@ est performance estimates of water scrubber and sand bed removal efficiencies
were used that were quite optimistic,

Gi) silver reactor efficiencies for 1959-60 were applied back to the early 1950 during
periods when records show that their performance had deteriorated drastically and
regeneration was often required (Burger, 1961], and,

(iii) there had been a complete neglect by Hanford scientists and HEDR of the
existence of an appreciable proportion of organic iodides in the off-gases, forms
of iodine that were not filtered or absorbed by removal devices and not measured
in slack gas sampling.

Almost all of the 1-131 of dissolved uranium fuel rods was released at two points: the
dissolver off-gases (50% initially, 86% after ir-sparging (Warren, 1961] and most of the
rest evolved during subsequent handling of dissolver solution. A small fraction (1-5%) was

27

i



DuPont operations. Data marked by an asterisk [*] indicates it was
collected after DuPont terminated operations at Hanford.

“The release factors calculated for the REDOX and PUREX plants
with the monthly estimates of the release factor determined from

the Roberts (1958) data for those periods of stable operation when no non-
current-production particulates were being released. These periods were
characterized by release factors ranging around 1.0 x 107. A generic
ruthenium release factor of 1.0 x 10” was used for all four separations
plants after installation of emission-control equipment in May 1948.” Heeb
1994, Pg. #4.18. [*]

“A higher generic ruthenium release factor was applied to T and B
plant operations for the period before installation of water scrubbers in
May 1948. During this period, no emission control equipment was in
operation. The water scrubbers were assumed to be at least 99-percent
efficient in removing ruthenium (Uebelacker 1960). Therefore, a generic
ruthenium release factor of 1x 10° was used for T and B plant operations
before May 1948. (The release factor for pre-scrubber operation was
increased two orders of magnitude to account for increased release due to
the absence of off-gas scrubbers.)” Heeb, 1994, Pg. # 4.18.

“Cerium-144 Release Factors - The only data available on cerium
releases were found in Anderson (1958b), which Provides data on cerium
releases from the REDOX Plant during September 1958.” Heeb 1994, 7“ #

4.23. [*]

“Strontium-9o Release Factors - Anderson (1958a) provides
average curies per day for strontium-go releases from vent stack effluent in
the “separations areas” (specific separations plants not listed) during 1957.
Using this data along with information on the number of curies of
strontium-90 processed, which were determined from the material tons
processed and the curie inventory per ton from ORIGEN2, a generic release

factor was calculated: .005 curies/day....” Heeb, 1994 Pg. # 4.25. [*]

“Plutonium-239 Release Factors - Records of plutonium release
measurements from all four separations plant vent stacks were made
available by J. K. Soldat.” Generic release factors were calculated by
dividing the curies of plutonium-239 released during a given time period by

Page 10 of 21



|
!
i

‘B. Academic and Professional Experience: R. E. JERVIS

I am presently Prof Emeritus, Nuclear Sci. & Eng, Univ. of Toronto, and a nuclear
consultant”.

I gained a First Class Honours degree in Physics from Oxford UK in 1947. My DPhil (1950)
was on the D-D (fusion) reaction. Fellowships at Yale and Glasgow UK preceded a lectureship at
Glasgow, then Associate and then Full Professorships in Physics at Toronto. Honours included
visiting scientist status at Melbourne, Livermore, Ottawa (in all cases more than once) Harwell and
Saskatoon, and states as Professor of Medicine at Toronto and Special Staff Member at the Toronto
Generel Hospital. During the Toronto years research has been equally divided between pure nuclear
physics (photodisintegration) and muclear physics applied to medicine (mainly in bone disease,
patticularly osteoporosis).

‘The research work has resulted in just less than 200 papers published in refereed journals.
There have also been a couple of books, several published lecture notes, and several major reports
on nuclear emergency planning. I have been a consultant for safety in uranium mining and for the
Departments of Health and of Labour of the Government of Ontario, for the federal (Canadian)
Auditor General's office, and for the Atomic Energy Control Board.

For the decade of so up to 1997 [have been the Techaical Advisor to the Solicitor-General
of Ontario with reference to off-site effects of accidents at nuclear power plants - this involved,
amongst other things, chairing the Technical Advisory Committee and half its Working Groups, and
some of its sub committees, dealing with source term estimations, meteorological modelling of
distribution of radioactive emissions, dose prediction and protective actions. | chaired, for more than
10 years, the University’s Radiation Protection Authority (the University has 230 professorial staff
licenced to use radioisotopes).

Iam a member of the Canadian Association of Physicists, of the Canadian Radiation _
Protection Association, and (until retirement) a Fellow of the (UK) Institution of Nuclear Engineers.

ee

(see attached C.V. for details)



Report for the In Re Berg Litigation

Reference-Hanford Releases

March 1, 1999

by

K. G. McNeill and R.E. Jervis
University of Toronto



Stack Discharge Active Particle Contamination Problem” HW-9259,
3/22/1948.

Re: Dispersion. Assigned to Church, Meteorology. Unable to answer
fundamental particle dispersion problems without extensive Hanford
experimentation. Parker submits: “Small particles could ascend 10,000 to
15,000 feet in summer by thermal convection, and rarely to 3,000 feet in
winter by mechanical turbulence.” HW-9529, 3/22/1948.

“,... there is a backlog of tens to hundreds of millions of particles
unaccounted for in the Plant vicinity. The responsibilities of the Company
and of the Commission require the most energetic attempts to prove that
no significant radiation hazard can arise from this source, or to correct an
untoward condition regardless of cost.” HW-95259, 3/22/1948.

“The deposition of active particles during the month followed an
erratic pattern, with no apparent correlation with wind direction.” HW-
10166-K, 5/31/1948, H.1. May Monthly Report.

Active particles picked up in Benton City and Richland. Monitoring
implemented to determine whether deposition rate was related te
processing operations. “The only correlation found was that deposition
rate was affected by wind direction.” HW-10166-K, 5/31/1948.

“Radioactive Particle Investigation” R.C. Thorburn: “The health
hazard from such a source is apparent... . Our investigations indicate that
the particles actually were coming from the corroded fans and fan
breechings.”

“The appearance and shape of individual particles varied widely.
However, all particles appeared rough and granular under a microscope
and at least a spot of rust-brown color was common.”

“Similarity of structure between the specks found on air sample filters
and fan and duct work particles noted.”

“Radioactivity of particles varied in a range of 2.5 x 10 TM*** to 3.2 pc
per particle of beta and from <5 d/m to 3,800 d/m per particle alpha was ,
found. The possibility of even hotter specks exists.” HW-10261, 6/11/1948.

“There appears to be a general belief that the number of detectable
active particles deposited per month on the ground in the 200 West and

Page 7 of 21



from a given time period were assumed to apply to all time periods when
the same release control equipment was in service. (Heeb. 1904, Pg. # 4.7)

“¥ and B Plants. Release factors calculated for the REDOX and
PUREX plants were applied to T and B plants because the emission control
devices at T and B plants were similar to those in place at the REDOX and
PUREX plants.” (Heeb, 1994, Pg. # 4.17) (this is factually incorrect)

Heeb’s release factor for the iodine before installation of water
scrubbers in May 1948 was 0.905. Water scrubbers were calculated to
lower the release factor to 0.285, as per estimates made in the GE monthly
teport for May 1949, and when sand filters were installed in December of

1948, the release factor became 0.25. (Heeb 1994, Pg. # 2.2)
Iv.

PARTICLE PROBLEM

One factor ignored by Heeb was the particle problem that was
recognized as existing but unreported until 1947. Although this is after
DuPont terminated, there is no reason to think it was not existing in the 2
years previously, since the emission control equipment was just beginning
to be installed in mid-1948.

Health Instrument Section surveyors detected contamination in the
form of discrete active particles on the ground in the region of the Hanford
separations plants in late September 1947, HW-9259.

“Particle problem remains despite fan replacement: The active
particle contamination in the Separations Plant Areas continued to
command much attention. Since the replacement of one fan in each area,
the rate of particle deposition has diminished by a factor of less than two,
whereas the average activity of each particle has diminished bya factor of 5.

Recenth d_ phot! hic meth: ion indicate al ten times

as many particles as were found by as otd surveys... Biological monitoring
to date has been inconclusive.” HW-9191, 2/29/1948.

“There is some evidence that apparent increase of concentration with
increasing distance from the stack is real.” H.M. Parker, “Review of the

Page 6 of 21



insufficient and inappropriate data. It is also noted that ORAUT reported
no effort to validate its model. Nor was any mass balance analysis made to
determine if the modified RATCHET being used had been properly coded.

The generic data relied upon for DuPont exposures is based upon a
series of assumptions from one step to another. First, Heeb’s estimated
DuPont release factors, for which no contemporaneous data existed, which
he created by retrospectively applying release factors developed at later
times from other facilities using efficiencies assumed for the facility from
where release factors had been taken, and then back-correcting to account
for the lack of the filters at DuPont. Secondly, these Heeb estimates were
utilized by Till as the basis of his estimates of DuPont exposures which in
turn were converted by ORAUT into individual exposures. DuPont generic
exposures are necessarily dependent on extrapolated assumptions and
cannot provide estimates of individual exposure with any semblance of
reliability.

VI.

THE EFFORTS TO CREATE A DR FOR DUPONT WORKERS AT
HANFORD, HOWEVER WELL INTENDED, ARE SIMPLY NOT |
SCIENTIFICALLY DEFENSIBLE.

Even if one were to assume, arguendo, some plausibility for such
generic data, it cannot be applicable without some knowledge of the
individual dosimetry, the workers activities, the locations of his work,
protective gear, if any, and any episodes of higher t than normal air :
coticentrations, and incidents of accidents or special individual exposures,
for which data no longer exists. NIOSH cannot reasonably estimate a
dose in a factual vacuum. The worker could have been at any location in
the 100, 200, or 300 areas at Hanford and received an excessive exposure
for which the records no longer exist. Recall also, this was start-up time,
the period of the largest releases and the most prone to accidents, and also
failures to adequately protect workers as the hazards were being learned.

x.
NECESSARY CONCLUSION

The facts establish that there is not enough information available to

Page 19 of 21



redistributed after initial deposition.” HW-11499, 10/31/1948.

“A total of 88 frames exposed on the reservation and at Benton City
and Pasco showed a deposition rate of 4.4 x 10” particles per month.
Frame studies completed in the 200 Areas indicated deposition rates of 1.4
xX 10° particles per month in 200-East, and 2.2 x 10° particles per month in
200-West.” HW-11499, 10/31/1948.

H.I. November ‘48 monthly report indicates “insignificant” reduction
in the rate of deposition. Off-site air samples show high readings for
particle inhalation. HW-11835, 11/30/1948.

Paas to Singlevich, “Particle Deposition Summary” - Subtitled
“Deposition in 200 Areas”: indicates one billion particles deposited in 200
East Area between 10/7 to 10/20/1948. Bates #2004209, 6/15/1949.

Note it was acknowledged that none of these particles below 2-3 um
were being measured in the atmosphere, see HW-10378, 6/30/1948 above,
and they were not included in the stack release estimates. There is no
evidence that the additional exposures created by these particle
were factored into Heeb’s release fractions, although they most
certainly created an increase in the inhalation hazard. Dr. Till
acknowledged that particles were released from B & T plants in early
operations, but concluded that “the process could not be reliably

modeled.” Till 2001 Draft, Pg. # 2-22 .
Ve

GENERIC RELEASE FACTORS

The following contains the nub of Heeb’s methodology for the early
pre-1958 releases of certum-144, strontium-90, ruthenium-106 and
plutonium-239, with the plutonium and ruthenium particles presenting the
major inhalation and ingestion exposures for DuPont workers.

There was no release data available contemporaneous with the
DuPont operations. To create such data, Heeb used release data from later
periods to calculate a release fraction and then back extrapolated this
release fraction, as adjusted for lack of any emission controls, to the

Page 9 of 21



April 2, 1990

Mr. Shirley Gydesen

Battelle

Pacific Northwest Laboratories
P.O. Box 999

Richland, Washington USA 99352

Dear Mr. Gydesen:
RD -DUP DOCUMENTS

As we discussed today, I contacted Du Pont’s “Hall of Records”
concerning the existence of certain documents relating to the operation of the
Hanford, Washington Site as referenced in your letter of February 5, 1990.
The Hall of Records has informed me that the only surviving records are
payroll records of employees working at the site. All other records were
either destroyed or turned over to the Atomic Energy Commission in the
mid-1970's.

- My apologies for the delay in responding. Please let me know if
you have additional questions.

Very truly yours,
ae AGI

John W. Keiter
JWE:cjs

RECEIVED
APR 1.01990
SE. GYDESEN

Better Things for Better Living



01-12-06 A11:05 IN

oe

January 6, 2005

PETITION FOR SPECIAL EXPOSURE COHORT STATUS FOR
HANFORD DUPONT WORKERS

This Petition is submitted on behalf of a class of workers consisting of
all former employees of Du Pont Company working at the Hanford Nuclear
Reservation during Dupont’s operations from 1943 to September
15, 1946, when Dupont Operations at Hanford terminated.

This petition is based upon three basic facts:

First, there are no individual Hanford Dupont worker records in
existence because they have all been destroyed. This is an
indisputable fact, as demonstrated by the attached enclosures in Exhibit A.

Secondly, there is not enough information available to either estimate
the maximum radiation dose that could have been incurred under plausible
circumstance by any member of the class, or to estimate the radiation dose
to members of the class more precisely than the maximum dose estimate.

Thirdly, if one had hard data, then generic exposures might suffice in
limited circumstance. But generic exposures developed from extrapolated
data of doubtful reliability are not scientifically defensible. Such generic
exposures are really just assumptions which cannot provide estimates of
individual exposure with any semblance of reliability. It is not possible to
make a dose reconstruction for an individual Hanford Du Pont worker
based upon gemeric exposures that are necessarily dependent on
assumptions. This is demonstrated by the following references.

Page iof 21



G.3 The Distribution of Dose

As noted above, Shipler et al (1996) and Farris et al (1996) have used computer codes
{Ratchet and Descartes) to move from source term to dose as a function of position vis-4-vis Hanford
works. In particular, they have estimated and depicted in a seties of drawings the dose received by
a target group (infants) a9 a result of 728 746 Ci of 1-131 released. (Note these doses are median
doses with large errors on them, as indicated in Table 1 of Farris's paper).

In the drawings given here which are adapted from Faris, we depict the doses generated by
_J emission proper for different 5 year periods; this has been done by modifying the isodose contours
* of Farris by multiplying the dose represented by a contour by the factor M, where M is the factor
given in Table 5, the emission in Ci in a particular 5 years according to our estimates (Table 4)
divided by 728 746 Ci.

Letus consider our Figure 1, for the first 5 years of life of infants born 1/1/41 and consuming,
"back-yard” produce, This is based on Fig. 6 of Farris which is for infants eating “back-yard* food.
Our Table 4 shows that in the period 1/1/41 to Dec 1945 the I emitted is
585 090 Ci, which is 0.803 of the HEDR 728 746 Ci. So the isodose contour values must be changed
by a factor of 0.803. For the 4 highest dose regions shown in Farris Fig. 6, the boundaries are given
as 230 rad to 100 rads, 100 to 32, 32 to 10 and 10 to 3 rads. Our modifications to make the
depiction applicable to the 5 years 41-45, are to change the region boundaries to 184 rads to 80r,
80 r to 261, 26 r to Sr, and 81 to 2.6 rads. Further, we have sketched in the probable position of
the (median) 5 rad isodose contour, because of the Doubling Dose being 5 rad for infants. It is seen
that Richland, Spokane, Walla Walla and Pendleton are all within this contour, ie. a child born in
1941 in any of these places, and living there for 5 years or more would likely receive more than 5 rads
(and on the doubling dose picture would, if they later developed thyroid cancer, be more likely than
not to have had the cancer caused by radiation from the I emissions).

Fig. 2 is for infants.bomn.on or about Dec. 26 1944. For the 5 years (plus a few days) to
December 1949 a resident infant would receive (Table 5) a dose 103% of the 728 746 Ci on which
the Farris drawing is based. So here we muitiply the Faris contouss by 1.03 to give boundaries of
238 r to 103 r, 103 r to 33 1, 33 to 101 and 10 rt03 rads. Again the 5 rad contour is sketched in.

Furthermore, as the 5 year rolling summations areroughly the same from 1942-1946 to 1945-
1949, this figure 2 shows, within 10%, the 5-year doses in this extended period.

Wealso show Figure 3 (1946-1950) [and also useful for 1947-1951] and Figure 4 (1951-
1955) which also roughly (within 20%) portrays 1948-1952, 1949-1953, and 1950-1954. Beyond
1955 the doses fait off and are not illustrated.

For other circumstances, e.g. for adults, Farris Figure 7 could be correspondingly modified.
For infants consuming “commercial” food and milk Farris Figure 8 applies; our Figure 5 indicate
doses for infants bom in 1942 to 1945. The general picture is the same as for our Figure 2.

7



supported by any hard comparison data from actual conditions existing at
the T and B plants during the Dupont years at Hanford. The filtering
equipment was subject to continuous changes for improvement and
releases factors developed at one point in time were not applicable to other
time periods with different equipment. For example, when caustic
scrubbers replaced the water scrubbers the capture of iodine was greatly
improved.

To back extrapolate a RF from a later date back to the early period
before emission control devices were being developed, it is necessary to
know the effectiveness of the devices as compared with the situation of no
devices. (The release factor for pre-emission control devices (1944-1948)
was increased two orders of magnitude to account for increased releases
because of the absence of off-gas devices.) This effectiveness difference was
set by Heeb at 100 times. It is interesting to note that Till used an increase
factor of 150, which he called the “effluent treatment modifier” instead of
Heeb’s 100 (see Till 2002, pg.2-26), which emphasizes the basic
uncertainty and raw assumptions in these so-called release factors. It is not
known if ORAUT adopted Heeb’s 100 multiplier or Till’s 150 multiplier.

This basic uncertainty has been confirmed by a letter report by A.G.
Blasewitz to the EPRP (External Peer Review Panel, see attached as Exhibit
D) that was organized to provide a non-public review of HEDR, in addition
to the public sessions and critiques by the Technical Steering Panel (TSP).
This attached review make precisely the same points made by Petitioner in
the foregoing paragraph, and concludes that the RF for Ce, Ru, Srand PU
should be 4 x 10“ instead of 4 x 10% concluded by Heeb. See Exhibit E, page
3. With the estimated activity being released under no emission controls
(DuPont era) ranging from the 100 times to 1000 times
the release factors developed later under emission controls, the Dupont
generic release factors are mere assumptions, at best, and cannot support
an individual Dose Reconstruction.

Tn further support of the Till & Blasewitz disagreement with scrubber
efficiency of 99% is the August 6, 1948 scrubber testing, finding a collection
efficiency under 96% and predominately under 90%. See attached Exhibit
F, Stack Contamination, Martel, 1948, HDC-611.

Heeb’s methodology (and that of Tilland ORAUT) to calculate release

Page 12 of 21



the curies of plutonium-239 processed during that period. Release data
and release factor data are provided in Table 4.8. A sample release factor

calculation follows the table.” Heeb, 1994, Pg. # 4.27.

Note that superscript (a) references HEDR Project Document No.

10930320), “Plutonium and Uranium Releases from Hanford

Separations Facilities/Raw Data,” from J. K, Soldat (Battelle NW) to
HEDR Project Office, October 26,1903. However this Soldat document

gives data developed in 1952 and 1957 from the T & B plants and REDOX
and Purex, and would not be applicable to the T and B plants before
September 1*, 1946. [*]

“T and B Plants - The T and B plant plutonium-239 release factor
was based on the combined plant average monthly releases of 3.9 x 107
(rounded to 4.0 x 10”) for operations after installation of emission-control
equipment in May 1948. [*] Emission-control equipment was assumed.
to have been about 99-percent efficient, so the early period plutonium-239
release factor for the T and B plants was 4.0 x 10°. (The release factor for
pre-scrubber operations (1944-1948) was increased two orders of
magnitude to account for increased releases because of the absence of off-

gas scrubbers.)” Heeb, 1994, Pg. # 4.27.

Plutonium-239 Release Estimates - Figure 4.8 shows that
plutonium-239 releases were largest in the early period of separations plant
operations, reaching a maximum of 0.0755 curies during the month of
October 1945. Releases were reduced after water-scrubber installation in
May 1948. The late~period maximum was reached in January 1966, witha
plutonium-239 release value of 0.006456 curies for the month.” Heeb,

1994, Pg. # 4.27.

It is clear that Heeb did not have any contemporaneous data to
support a release factor (RF) for any of four radionuclides being considered
in the particle inhalation exposures to DuPont workers. In each case Heeb
used release factors developed in other facilities and in other time periods,
different from the early conditions during DuPont tenure at the T and B
plants when no emission control devices were being utilized. For
plutonium and ruthenium, Heeb retrospectively adjusted these release
factors to reflect an assumed 99% removal efficiency from the later
developed emission control devices. The 99% efficiency assumption is not

Page 11 of 21



radioiodine, especially organic-iodides, which HEDR ignored, and the increased radiation
doses to exposed populations that would result from our less conservative, revised
corrections factors, were the impetus for this joint supplemental report.

B. FIFO:

In McNJ99 there were documented 10 cases, between the years 1954 to 1964, in
which the emission of 1-131 was greater than expected. These out-of-ordinary emissions
were attributable to the processing of "greener" fuel than expected, and in its tum this was
attributed to accidental violation of the First-In-First-Out protocol ~ under this FIFO
protocol the fuel first removed from the reactor was the first to be processed. (The Dec.,
1949 "Green Run" was not included as one of these cases since, in the Green Run, the
violation was deliberate [Harlan et al, 1950). In the 10 cases above, six had emissions of
less that 10 Ci, while in the other four, the emissions were 75 Ci, 28 Ci, 40 Ci and 60 Ci.
This total of about 200 Ci occurred when the grand total (normal emissions plus these 200
Ci) was about 6000 Ci; the extra was thus about 3%.

Since McNJ99, three more extra-ordinary cases of greater than expected emissions
that could be attributed to accidental violations of the FIFO protocol have been
documented. These occurred in September 1959 {HW-62179), when the I emission was of
20 Ci, in April 1962 [HW-73514], 40 Ci, and Dec.,1963, 8 Ci [Keane,1963]. All three of
these cases occurred in the same period: 1954-64 as with the cases discussed above[HW-

. 89067}. Adding in these 3 new cases gives a new total of about 200 Ci + 68 Ci. This totals to
an extra of 268/6000 (Ci), or 4%. Just as McNJ99 rounded up the estimated (extra) emission
from 3 to 5%, so it would be reasonable to round up the 4% to 6% as a result of these new
findings. This value of 6% bas been estimated on the basis of data for the period 1954 to
1964; however. McNJ99 justified its use over the whole range of reactor years of interest
{except for the time period: Sept.,1946 to Dec.,1949 during which period the push dates
were known for each particular batch, so no generalized FIFO correction should need to be
thade for that period), ~~"

A summary of revised FIFO factors is shown in Column 3, Table 2, as follows:

FIFO Correction Factors:
Dec 1944 to Aug 1946 = 1.06

Sept 1946 to Dec 1949 1.00
Jan 1950 to Dec 1956 1.06

C. ECT Corrections:

The exponential cooling time correction factors, ranging from 1.0 to 1.7, as shown in
Column 4, Table 3 do not require any revisions here.



RF. = 0.86 (1-0.75)=0.21, plus canyon air content (0.075) = 0.28,

Efficiency tests on sand filter beds installed on B and T plant ‘canyon’ ventilation air, Now/Dec.’48,
also yielded widely different removal efficiencies ranging from 27-68% (depending on whether they
were wet or dry). Considering that separate tests had shown that dry sand beds removed only small
fractions of inorganic iodine, no organic-I and mainly particulates, it is our opinion that the lower
figure is more realistic (whereas Heeb used a broad average value). Therefore, the appropriate,
effective RF. when both sand beds and scrubbers were operating (1948-51), was:

RE. = 0.2) + (0.73 x 0.075) = 0.26.

After their installation in 1951/52, the silver reactors considerably reduced emissions below

. the 26% levels but their performance was found highly variable. During early months, Paas and
Soldat [Pa51} estimated ‘ideal’ RF. = 0.01, but measured values (which may also have been
appreciably underestimated because of the inaccuracy ofrelease monitoring before 1958, cited above)
increased more than tenfold within 6 months when 13% releases were reported. Rather than using
these limited and inaccurate release data after initial commissioning, HEDR [He94] chose to base B
and T plant silver reactor plus fibre filter efficiencies from 1952, on a documented set of 158
measurements from the newer REDOX plant. Heeb[He94] derived a median RF. value of 0.012,
from a range of 0.002 to 0.09 results. We contend that, based on a linear dose/response model for
estimating biological effects, the appropriate estimate to use is the average or mean releases, namely
RF. = 0.022, a result yielding 75% higher radioiodine releases for the rest of the plants’ operations
until the 1956 last stiutdown of T plant, compared to the HEDR calculated release estimates (He94].

Even these increased release figures are undoubtably conservative underestimates, not only
because of the inaccuracy of J-131 release monitoring before 1958, but also because the efficiencies
of these control devices decreased particularly at breakthroughs when the Ag reactors became
exhausted, were fouled with excess chlorine that acted to replace already adsorbed iodide, and when
release episodes occurred such as the “Green Run’ and the accidental 72 Curie release from PUREX

~- in 1963 [He94]. Also, there were frequent incidents reported when breaks, tears and cortosion of
filters permitted excess fission products and actinides te by-pass stack filters and be released.

Considering (a) the different chemical forms of radiviodine, (b) differential removal of them
by the several control devices and (c) deposition and condensation occurring in the ventilation and
release stack ducting, the released 1-131 would have been depleted in reactive I, and particulates that
had a greater tendency to deposit locally, and result in enrichment of the volatile, less reactive, .
organic iodides which were not appreciably adsorbed on vegetation and remained airbome for periods
of >200 h [Bu91}, dispersing in a downwind plume to much greater distances off-site. Recently
published research on the behaviour of fission product 1-131 in releases from irradiated U and the
Telative absorbability of elemental I,, iodides, iodates, JOH and organic-I on equipment surfaces
including small diameter leagthy stack sampling lines, filters, charcoal, HEPA and various liquid
chemical scrubbers [Ev94] provided quantitative information on the fate of ‘carrier-free’ radioiodine
nuclides in these various chemical states. Based on information such ss this, it can be estimated that
the bulk of I-131 released from the first stage dissolvers had an approximate composition of 70%

GB



A. Academic and Professional Experience: .G. McNeill
A brief resume of my academic background is given here; a full CV is attached”,

gained a First Class Honours degree in Physics from Oxford UK in 1947. My D Phif (1950)
‘was on the D-D (fusion) reaction. Fellowships at Yale and Glasgow UK preceded a Jectureship at
Glasgow, then Associate and then Full Professorships in Physics at Toronto. Honours included
visiting scientist status at Melbourne, Livermore, Ottawa (in all cases more than once) Harwell and
Saskatoon, and status as Professor of Medicine at Toronto and Special Staff Member at the Toronto
General Hospital. During the Toronto years research has been equally divided between pure nuclear
physics (photodisintegration) and nuclear physics applied to medicine (mainly in bone disease,
particularly osteoporosis).

‘The research work has resulted in just less than 200 papers published in refereed journals.
‘There have also been a couple of books, several published fecture notes, and several major reports
on nuclear emergency planning, I have been a consultant for safety in uranium mining and for the
Departments of Health and of Labour of the Government of Ontario, for the federal (Canadian)
Auditor General's office, and for the Atomic Energy Control Board.

For the decade or so up to 1997 I have been the Technical Advisor to the Solicitor-General
of Ontario with reference to off-site effects of accidents at ouctear power plants - this involved,
amongst other things, chairing the Technical Advisory Committee and halfits Working Groups, and
some of its sub committees, dealing with source term estimations, meteorological modelling of
distribution of radioactive emissions, dose prediction and protective actions. I chaired, for more than
10 years, the University's Radiation Protection Authority (the University has 230 professorial staff
licenced to use radioisotopes).

I am a member of the Canadian Association of Physicists, of the Canadian Radiation
Protection Association, and (until retirement) a Fellow of the (UK) Institution of Nuclear Engineers.

*
(see attached C.V. for details)



Opinions and Conclusions

Although the HED Reconstruction has been carried out with diligence and overall care,
there are a number of incorrect assumptions made or points neglected which make
necessary correction of the 1-131 emissions from Hanford. None vary greatly the massive
ouput in 1945, but they do strongly alter calculations of later emission estimates.

Tn particular we note

(2) _ incorrect averaging of cooling times, with correction factors ranging from

unity to 1.67
+ () violation of First In First Out Protocol, with correction factors of from 1 to
1.05
(c) __ lag time (time between dissolving and extraction) correction factors
ranging from 1 to 1.9

(@) _ stack monitoring of 1-131 being vented to the atmosphere was inaccurate
and unreliable because of poor design of the long, narrow stack air
sampling lines, poor calibration and variable collection efficiencies of the
bubblers and filters connected to the lines, and improper radioassay
procedures, The ‘generic release factors’ that HEDR applied to calculate
fractions of iodine released were not well known from 1948 to 1956 and
the few measured values were subject to the same errors of stack
monitoring. The use of an RF. estimated from 1959 REDOX plant
performance as a basis for calculating 1951-56 losses from the older B and
T plants is highly questionable, and in addition mean, not median, values
are appropriate. The release correction factors range for 1.0 to 1.76

The overall effect is such that in one month (Jan 1953) the correction factor is 6.28, that
is HEDR underestimated the emission by a factor of more than six.

Using the corrected emissions and the relationship between Iémission and distribution of
dose in thé proximity of Hanford developed by Shipler et al (1996) and Farris et al (1996),
depictions of dose received by e.g. infants drinkiag “back-yard" and commercial milk are
presented, showing in particular areas within which doses of more than 5 rads to the thyroid may
have been received.

Signed: : Leslelt R. = Swroria

K.G. McNeill RE. Jervis
Ment 1 [44 March, 1.1999
I

Date:

18



yon PP

ACADEMIC AND PROFESSIONAL EXPERIENCE: K.G. MCNEILL ....0---0eccceseceeeees T
ACADEMIC AND PROFESSIONAL EXPERIENCE: B. E. JERVIS ....--0cccsonsceverssscens 2
HANFORD INTRODUCTION .....ccecessccccccnensenassuvstsesseceterarsetarssensece D

INCORRECT COOLING TIMES ......

D2 EXPONENTIAL CoouING TES -
D3 PirstIN First Out PROTOCOL .
DA LaGTME ......
DA1 1944-1947
D42 1948-56 ..
DAZ
Table I - Stmmary ,
BADIODINE RELEASES DURING FUEL PROCESSING:
SUMMARY OF CORRECTED I-13] RELEASE FACTORS - REPRODUCED IN TABLE 2 COLUMN ...-.-.040- “4

SUMMARY OF CORRECTED EMISSIONS ....0.seeeeecsseseesecctevevecsereeseees seen 1G

THYROID DOSE ESTIMATIONS ,,...00ssessencccscccevererserseacessrsassees rer 5

Gl Doses WITHIN 5 YEARS
G2 YEARS OUTSIDE THE INITIAL 5 YEARS OF LIFE.
G3 THEDISTRIBUTION OF Dose ..,.........-

OPINIONS AND CONCLUSIONS .....:cssecccccveerersenscsresunsrssecasatocsceseees 1B

(MAIN REFERENCES .....0e0eceveeee eee rr erer ees wtneeeeneecreseecerceereerere LF



200 East Areas is increasing. In round figures, 100 million such particles
fell in each area during June. Preliminary measurements of particle size
within the exhaust system showed that much of the total emitted
activity was concentrated in particles below 2 to 3 1 diameter.
These are the potentially dangerous ones with respect to inhalation, and
none of this size-range is being currently measured in the
atmosphere. Possibly 10” particles above 3 1 diameter, and 10% (trillion)
below this size were emitted during this month.” HW-10378, 6/30/1948.

May “48 - 270 million particles deposited in East Area and 190
million in 200 West. The highest deposition rate noted was 2 to 4 p.s.f. per
week in both areas. HW-10378, 6/30/1948.

Second Meeting of Stack Gas Problem Working Group - Admits that
very small particles may exist that can’t be detected using present
equipment or methods. The number of particles discharged per month to
the atmosphere from the 200 area stacks is 10°° in the 10 micron size and
10” to 10° in 2 micron size. The highest density of particle distribution on
the ground is 3 to 6 per square feet. Studies indicate that a resident of
Richland would have a possibility of inhaling an average of .3 particles per
month and that a worker in the 200 Area 10 to 12 particles per month.
Recently, however, this probability of inhalation has increased as much as
100 to 200%. “The general pattern of distribution is a function of

prevailing wind direction.” Bates #122393 to 122408, 8/20/1948.

H.I. September ‘48 report: Fall of active particles in the reservation
was “incorrectly reported to total 10%. This should have been 10”.” Active
particles were readily detectible in the atmosphere in Spokane, 130 miles
distant, and even at Mullan Pass, 200 miles away and at an elevation of
6,000 feet. Report states it is difficult to see why operations should be
permitted without respirators. Further, in fact, it is difficult to justify
further operations, pending completion of the sand filters. HW-11226,
9/30/1948.

HLL October ‘48 Monthly Report: “Initial Results on active particle
deposition, following completion of sand filter in the 200-W Area (T Plant)
showed a reduction of a factor of 4 only. Conclusions from this would be
premature, but it is tempting to surmise that trouble may still be
anticipated either from particles emitted from the stack itself, or

Page 8 of 21



Exhibit A



A. INTRODUCTION

This report is supplemental to a previous document, McNJ99, in which we considered
the validity and accuracy of HEDR estimates of I-131 releases from the Hanford Site 200 B,
T and REDOX chemical separation plants over their operating lifetime (1944-1956).
While some of the HEDR calculations were based on historical records of fuel radioiodine
inventories and various release estimates, a uumber of significant assumptions and
approximations were also made and several of these we consider to have been erroneous and
to have led appreciable underestimates of iodine releases. In the period, 1944-1956,
considered here, greater than 90% of iotal 1-131 releases to atmosphere at Hanford occurred.

Tn McNJ99, correction factors were computed to be applied to HEDR [Heeb,1994]
release estimates to allow for errors such as:

(i) — Exponential Cooling Times (ECT): correction was required for errors resulting
from their incorrect inear averaging of fuel cooling (decay) times as a
simplification for calculations. The McNJ99 ECT factors were based on true
exponential I-131 decay over the time period from fuel discharge to processing.

Gi) __ First-In-First Out Protocol (FIFO): corrections were required to correct for events
in which average cooling times assumed by HEDR were not applicable because
orderly queuing of fuel batches for cooling, dissolving and extraction was not
always followed.

Gii) Lag Time: another source of incorrect cooling times was the time difference
between dissolution and extraction of fuel (so-called ag time. Cooling times
assumed by HEDR were the period between reactor shutdown and extraction, not
time of dissolving when the major evolution of iodine occurred.

{iv)  Radioiodine Release Factors (RF): corrections were applied in McNJ99 to HEDR
iodine release factors to account for inefficiencies of the removal devices in the
1948-56 period. HEDR used est case scenarios based, in part, on unreliable
stack release measurements to estimate a set of eneric release factors which were
quite low, at times by an order of magnitude.

Mathematical details of how the ECT, FIFO, LAG and RF correction factors were
computed were given in McNJ99 and are not repeated here.

In this report, as a consequence of reviewing relevant Hanford and HEDR documents,
and, critical reviews made by NRC, CDC [Anspaugh,2001] and other reputable experts, we
have found compelling evidence that some of our earlier estimates of the correction factors

27



1.05 (5%) is applied to this period as well as to the "no log book period” May to August 1946. After
August 1946 the push date was known for a particular batch until the end of 1949, so no general
FIFO correction should need to be made.

\

Summary for FIFO Factors ( repeated in Table 2, column 3)

FIFO correction Dec. 44 - Aug. 46 of 1.05
No FIFO correction Sept. 46 - Dec. 49
FIFO correction Jan. 50 - Dec. 56 of 1.05

‘D4 Lag Time

Another source of incorrect cooling time is the fact that although the major evolution of
iodine is at the dissolving of the U slugs, and so the time that primarily matters is that between reactor
shut down and dissolution, the time which is given (in the Metal Histories, for instance) is the time
of extraction, not of dissolving. On the basis of early (1945) data, HEDR concluded (and used in
He92) that the lag between dissolving and extraction was (around) 3 days. This is for instance
indicated by the Figure 2.1 of {He92], where cuts are in storage for several days. Then the cooling
time is taken by [He92] as time to extraction less 3 days (or some variation around 3, see [He92]
page 4.23, where the mode is taken as 3 and variability 0-7 days). This would be reasonable if the

Jag time were always 3 days. Even within the bounds of [He92}, however, this lag time is shown to
be incorrect.

For Nov. 47 the Metal History [FTS 71] for the T plant gives push dates and extraction dates
which (linear) average to give 96 days "cooling time”. This is the value which Gy92 gives but He(94)
gives 94 days in Table A.1. This looks as if something like the 3 days has been removed (and so it
looks as if He94 buys into He92 in this respect), For October 47 there is the same story. We find
the average time push to extraction is 87 days, [Gy92} gives 87 days and He(94) gives 85 days:
However this is perhaps just fortuitous. Looking over the wholé of the comparison between Gy(92)
and He(94}for the period 1944-47, for the T plant, there is almost a random difference between the
two, with differences ranging from 7 days (March 46) to - 4 (June 43) and (neglecting the egregious
Jan. 46 (32 day difference) an average of 1 day longer for Gy92 than for He94. Thus the evidence
that He(94) has adopted the 3 day lag seems weak to non-existent.

For Dec. 47, however, in FTS 71 two lots of numbers (of different physical size - the bigger
ones are here called the "main" numbers, the smaller the "subsidiary". - are both in the "cooling time” -
column, a column which is under the general heading of “extraction”. Again push dates and
extraction dates are given. Doing the arithmetic of averaging the time of push to time of extraction
averages for Dec. 47 to 96 d. for the subsidiary numbers. Gy92 also gives 96 d. (He94 gives,
inexplicably, 99 days - did he add 3 days?) The main numbers however average 89 days. This must
be interpreted as a noting down of both the time to extraction and the real cooling time, that is the
days to dissolving, and it follows that the fag is 7 days, not 3 days. Taking a few other worked
examples, for Jan. 48 plant B the subsidiary numbers give 100 days (Gy92 gives 99) and the main
nusmbers 91.6, a lag of 8.5 d. For August 498 the numbers are 102 (Gy 92 - 102) and 93 days, lag



9 days, March 53 has 88 days (Gy-88}, and 81, so lag of 7d. The average lag time on the data is
8 days, Wider inspection of the data indicates that 8 is not far from the truth at all post 1947 times
(to 1953). We might note here that, post-1947, Gy92 and He94 agree.

DAA 1944 - 1947

If there be evidence of a lag time of 3 days in 1945, the only other datam in this period, the
Metal History for Dec. 47, gives 7 days in 1947 (a figure bolstered by later data). Reasonably one
would assume 2 value of 5 for 1946. The use by HEDR of 3 d as a lag time, instead of 5 or 7, results
“in the use of longer than correct cooling times, and so an underestimation of activity of exp(-0.0862
x 2) or exp (-0.0862 * 4) ie, 1.19 or 1.41. That is, the real I release has an increase of 19% or41%
respectively over HEDR for 1946 and 1947, (modified slightly as shown below).

In [He921 it is asserted that lag time need only be used from Aug. 46 to Dec. 47 (“as the
Metal History Reports .... regrettably do not give the time of dissolving but do give the time of
extraction".) For the blank period May 22 1946 to August 46 the reconstruction was so total that
dissolving dates were as readily estimated as extraction dates.

Taking all this into account, no lag correction factor is used until the end of Angust 1946.
For the remainder of that year 1.19 is used, and for 1947 a factor of }.41 (modified slightly as
discussed below).

0.4.2 1948 - 56

We use a lag time of 8 days for this period based on Metal Histories. This lag time of
(fortuitously) one half-life produces a factor of 2.0 correction to the estimated I release in this period.
We considered whether 3 of these 8 days had already been incorporated by He94, but came to the
conclusion that it had not, based on

(a) the production in He94 of a new Tabie (A.1) with a specific column for Cooling Tire
which in this period agrees very well indeed with the Cooling Time of Gy92 which itself
gives push date to extraction date.

(®) the lack of any clear indication that in this Table He94 bad attempted to incorporate the
fag time dealt with extensively in He92 and

(c) the lack of any reference to lag time in He94.

We therefore use a factor of 2 (modified slightly); if it can be shown that a 3 day lag has
already been incorporated, the extra factor is 1.54 rather than 2.0.

D.4.3 Modifications



Errors in HEDR I-131 Release Estimates and Corrections

to Dose Estimates to Account For These Errors

by

RE. Jervis and K.G. McNeill

Report to the Hanford Radiation Litigation

Tom H. Foulds and Richard Eymann, Attorneys

Supplemental Report

March, 2004

University of Toronto



-2- MAR 2 1 2002

If you have any questions regarding your request, please contact Sarah Prein, of my staff, at our
address on the previous page or on (509) 376-2516.

Sincerely,

Wi fd—

Marvin, Director

/V~ Office of Intergovernmental, Public
~- IPESLP and Institutional Affairs

Enclosure



were appreciably overestimated and, the role of the organic-I was not properly taken into
account.

27



references at the end of each DR to these technical basis documents.)

3) The ORAUT Technical Basis Document for Occupational Environmental
Dose is ORAUT-TKBS-0006-4, and the ORAUT Technical Basis Document
for Occupational Internal Dose is ORAUT-TKBS-0006-5. These
documents primarily concern inhalation exposures and are in turn based.

upon work done by Dr. Till in RAC Report No. 2-CDC, Final Report -

Methods for Estimating Radiation m Short-Live
Radionuclides and Radioactii icles R ed to the
during Early Hanfor tions , Till 2002.

4) Dr. Till’s work for these exposures was based upon the work done by Mr.

Heeb for the Hanford Environmental Dose Reconstruction (HEDR) project,

Radionuclide Releases to the A here from Hanford Operations, 1944-
. Hee

5) In other words, Heeb’s release estimates were adopted and modified by
Till, and Till’s estimates were adopted and modified by ORAUT site
characterizations, which in turn were utilized as the basis of each individual
DR.

6) Consequently, it is necessary to examine the validity of each stage of
development upon which the following stage was based.

i.

WHY HEEB’S GENERIC RELEASE FACTORS CANNOT BE USED

Heeb’s methodology was to first calculate the amount of each
radionuclide created in the reactor fuel rods which he determined from the
known basic physics of nuclear fission as a function of reactor power levels
and the time fuel rods were in the reactor. Then he determined the amount
of activity in the fuel rods being dissolved in the separation plant
processing and the estimated amounts of the nuclides being released to the
environment during dissolving and subsequent processing in the
| separation plant. This enabled him to establish a release factor or fraction
i for the nuclide in question as the ratio of the radionuclide activity released
i to the radionuclide activity processed.

Page 4 of 21



contour may be now designated the 27.3 rad contour, if the emission in a particular 5 year period is

27.3% of the 7 year plus 1 month base HEDR emission of 728 746 Ci. This is discussed further in
G3.

G.2 Years outside the initial 5 years of life

IfE be the normally expected incidence of a disease, and O the observed incidence (the
increase being due to radiation) the Relative Risk RR is O/E. The dose which makes O = 2E is the

Doubling Dose DD. In general, if the dose be (9-4), the dose received in the first 5 years of life
. 20-4)
1+—_—-

the O/E will be given by DD) where DD(4) is the doubling dose fos this age group. If
E(0-4).

z is>1
* DD(4) it is more likely than not that radiation has caused the observed disease.

But now consider that dose after the age of 4 may add to the probability of causing the

disease, though this, rad for rad, is less likely. If 26-9) were the dose for the next 5 years, and if
at this age the DD is DD(9), the disease would more likely then not be caused by radiation if
HS-9) , WO-9 5

PDS)  PD(4) Similarly for older ages, with DD(4) = 5 rads, DD(9) = 10 rads, DD(19)
= 33 rads and DD(>19) = 100 rads.

Then a child born in Jan. 1945, living at such a distance from Hanford that he/she does not
receive 5 rad in 1945-1949, may move in 1950 or 1951 much closer to the site of emission and pick
up additional rads in the next 5 years. Or a child born in 1941 may well have a sub-criticat dose up
to and including 1945 but still have an above critical dose for the first 10 years of life.

For instance, if a person born in 1947 received 4.5 ads in the first 5 years of life (to Dec. 31
1945) he/she could well, if living in the same place, receive (0.25/0.80) x 4.5 = 1.4 rads in the next

2H. 0940.14 =1.04

5 years. The relevant probability figures are 5 10 » Le. the total excess
relative risk is greater than unity, so if the person has thyroid cancer, it is more likely than not thet
the radiation dose caused the cancer.

These cases will have to be looked at case-by-case.



inorganic, 20% onganic and 10% zerosol and particulate iodide. After penetrating the control devices
and ventilation, material released from the stack was probably altered in composition to 50-60%
inorganic, 30-45% organic and 0-5% particulate. Owing to the reactivity and short lifetime of fodine
in the atmosphere, dry and wet deposition processes occurring both on-site and off-site, the
composition distribution among these iodine species would have been changing continuously with
distance in a downwind plume, enriching the volatile onganic-iodides.

Summary of Corrected £131 Release Factors - reproduced in Table 2 column 7

Startup to April, 1948

May, 1948 to Oct, 1948 028, 7
Nov, 1948 to Oct, 1950 0.25

Nov, 1950 to Fuly, 1951 6.01-0.13
after Aug, 1951 0,012,

F, Summary of Corrected Emissions

We believe that the estimates of HEDR may be taken as a basis of I-13 source term, but that
significant corrections need be made. Jn this paper conservative estimates of the corrections have
been discussed. In Table 2 are given the appropriate correction factors due to cooling times and
release factors, and overall correction factor (the product of the individual factors) and both the
HEDR emissions and the corrected (HEDR ~ overall corvection factors) emissions on a monthly
(1944 - 1953) or yeady (1954 - 1956) basis.



came from “I. Data that showed residual long-lived activity after
the decay of I-1g1were not included in this document.” Till, 2002.
Pg. #4~10. (i.e. no data for the rest of the nuclides of interest)

“Operations began at T Plant in December 1944 and at B Plant in
April 1945. We have found no routine air monitoring data for 1945.” Till,

2002, Pg. #4-11.

“Alpha activity. There was a limited amount of routine monitoring
of alpha activity in air by the Hanford contractor during this time period.
Reporting of these data began in the second quarter of 1951.” [*] Till,
2002. S

“4.1.5 Particle Counts in Air. Beginning in the fourth quarter of
1948, Hanford’s routine environmental reports included data on the
number of radioactive particles present in a certain volume of ambient
(outside) air (HW-13743).” Till, 2002, Pg. #4-33. [*]

“Chronological Review of Survey Data. Health Instrument
Section surveyors detected contamination in the form of discrete active
particles on the ground in the region of the Hanford separations plants in

late September 1947 (HW-9259).” Till, 2002, Pg. #4-38. [*]

“Tn fact, H.M. Parker (HW-9259) stated that measured deposition
was 1-10% of the estimated emission of active particles, meaning that go-
99% of particles were not detected within the surveyed area.”

Till, 2002, Pg. #4-42.

“A factor is included in the spreadsheet to account for particles not
detected by the survey instruments used. A factor of 10-100 increase is
suggested by comparison of surveys for large active particles released in the
1940's with more sensitive methods (HW-9141; HW-10941). However, if
this were done, then the dose assessment from the particles would need to
reflect the inclusion of smaller particles and their activity characteristics.
We have not made any adjustments to the measured deposition
densities for the example calculations included with this report.”
Till 2002, Pg. #3-30 (In other words, Till’s computer file, scrlist.dat, which
provided ORAUT 0006-4 with its source term did NOT INCLUDE Till’s
suggested increases 10-100 times to account for particles not detected.)

Page 15 of 21



Executive Summary

During the chemical separation of plutonium at Hanford in the state of Washington
in the years 1944 to 1972, fission products, particularly 1-131, were released to the
atmosphere. A fraction of this I-13] was distributed in the downwind ecosystem and reached
the human thyroid gland through various environmental pathways where became a potential
for the induction of thyroid disease.

In this report we estimate the quantities of 1-131 released, mainly during dissolution
of isradiated uranium, calculate how that activity was distributed in the air, how much was
ingested by cows and into milk as a source for human ingestion, and finally, how much was
deposited in the thyroid of a typical person living at a particular place and how much dose
was piven to the gland.

The complex pathways for the iodine released from the Hanford Plant make accurate
estimation of the final biological effects of the 1-131 very challenging. However, certain
facts are clear - for instance, the greater the release of I-131 the greater will be the potential
for causing thyroid disease.

The HEDR approach (Heeb[1993}and Heeb [1994]) was reviewed by the present
authors in 1999 (McNJ99). Corrections were made to the HEDR estimates of I-13 released
into the plant - at times these corrections were of the order of a factor of two — and
consideration was given to the fraction of [-131 which escaped into the atmosphere despite
attempts to filter out this and other fission products.

” The ‘present report looks particularly at the Release Factors, the proportion of the I-
131 in the plant which escaped into the atmosphere. One of the authors (REJ) has researched
and published extensively in this field. The major difference between the HEDR estimations
and the present work results from a new and better understanding of the role of organic-1 in
releases - the organic-I is much less reactive than, say, gaseous I, and I, and so was not
trapped by most off-gas filters. After April 1951 the Release Factor estimated in this report
is 11 times higher than that estimated by HEDR.

This large factor (of 11) makes a considerable difference to the estimated dose in
practical cases. Thus the dose to an adult living in Ringold from 1950 through 1956 was
twelve times greater than the dose calculated by HEDR (Napier 2002), while the isodose
contour for a child bom Jan 1 1945 and living on " back yard food “ was significantly further
distant from Hanford than for the equivalent contour based on the HEDR estimates. The
HEDR Release Factors are too low, mainly because the removal efficiencies of filter devices



entrained in condensate running down the stack walls [Smith,1946]. However for the first
45 years after startup, absolutely no engineered measures or devices were implemented to
reduce I-131 discharges, notwithstanding evidence of high levels of radioactivity downwind
aud high levels on vegetation off-site and in distant communities [Healy,1946].

Among the media used in attempts to mitigate such releases were:

E.1 Fiber Fitters:

Although there was little evidence that appreciable I-131 was evolving from the
dissolvers and processing streams in particulates, a bank of fiber filters were installed in
futile attempts to trap radioiodine from the off-gases. In current industrial use were the so-
called ambridge absolute filters asbestos and other paper composite types such as the
wartime CWS (gas mask) filters, some of which were used in sampling lines. However,
glass fiber filters were selected for the stack gases out of concem for flammability and
susceptibility to corrosive fumes. Probably, the composite filters would have filtered and
absorbed more I-131 but the glass fiber filters were very ineffective (<5% removed) because
the radioiodine was predominantly, 95-99%, in gaseous forms.

Filter tests done m the Chalk River radioactive exhaust stack by the author [Jervis,
1956] about 50 years ago using both CWS and Millipore membrane filters showed that very
little iodine could be collected on filters. On the other hand, based on information
published in 1934 [Robertson], granular charcoal filters would have been much more
effective had they been selected, removing also organic-iodides.

E,2 Water Scrubbers and Sand Beds:
Wet scrubbers had been tried in unsuccessful attempts for n-line stack snonitoring in
1945 and were also considered as a means of 1-131 recovery for commercial, medical
_ applications in mid-1946 [Heaky,1946], rather than.as a safety measure to reduce excessive
vegetation contamination. However, by mid-1948 much concem was expressed by the
AEC Reactor Safeguards Committee about Hanford I-131 stack emissions and GE was
instructed that up to 99% needed to be removed [AEC, 1948]. Sand beds were reported to
yemove as much as 98% in early tests but this was for new beds. An October,1948 HEW
report [HW-11449] indicated: widely varying efficiency reaching a maximum of 25% in
one run, also, .sand beds ranged from 27-68% ([HW-i3610]. Sand beds frequently became
ouled by liquids and other chemicals, such as the January,1950 water clogging at the T plant.
Further, in HW-67520 it was reported that bed efficiencies based on vent samples collected
were not valid due to inadequacy of the sampling system.

Water scrubbers were considered to have efficiencies as high as 85% but, in other
tests it was found that .only about one-half of the I-131 was caught in water scrubbers [HW-
74-6391). The choice of water and soda ash (carbonate) for wet scrubber media was
curious, if not negligent, because caustic scrubbers (having a much higher pH) were
considerably more efficient for iodine removal, particularly from acidic fumes. Further, at



j
1
i
i
i

the extensive research preformed by Heeb (1994). The files from
Till et al. (2002) provide monthly release estimates for the period from
Hanford Site startup in 1944 through 1961.” ORAUT-0006-4, Pg. #15.

“Intake of Airborne Radionuclides - The computer program
RATCHET and an Excel® spreadsheet were used to calculate claimant
favorable but realistic intakes from airborne radionuclides as opposed to
the computer program ‘Hcalec’ (Till et al. 2002) because ‘Heale’ calculates
“worst case” or maximum hypothetical dose as opposed to a realistic dose.”

ORAUT 0006-4, Pg. #14.

“The computer program RATCHET (Ramsdell, et al. 1994) was used
to calculate annual average atmospheric dispersion coefficients. The
RATCHET code was run for unit releases of 1 ym particles, noble gases, and
iodine speciated as a combination of elemental iodine, particle-bound
iodine, and organic iodine as described in Farris, et al. (1994).” ORAUT-
0006-4, Pg. #16.

(Note: no basis given for assuming RATCHET could run the non-
iodine particle dispersion correctly, or that 1 wm represents the
average size of the non-iodine particles. See discussion below.)

The Till spreadsheet results were adopted by ORAUT and multiplied
by air dispersion coefficients developed by RATCHET to develop the
individual exposure from inhalation of the nuclides. Interesting to note
that Till had developed an air dispersion model for particle air transport,

" Till 2603, section 3.2, but for unexplained reasons ORAUT utilized

RATCHET.

There’s no full explanation as to exactly how RATCHET was
modified. There are many difficulties with RATCHET, as follows:

1) It’s tendency to under-estimate. The Technical Steering Panel
(TSP), a group of independent academics and scientists was organized to
monitor and provide critical review of the HEDR project as it was being
developed by DOE contactor, Battelle NW (a.k.a. Pacific NW Laboratories).
The final report of the TSP upon completion of HEDR states, however, that:

“Key Issues Remain to be Resolved”

Page 17 of 21



fragmentary, as they primarily consist of contract files and in-
house histories. We do not have any documentation about
employment, medical, and radiation exposure.”

e) Letter of March 11, 2002 from Pacific NW Laboratories (which
keeps all the Hanford dosimetry records) states:

“As we have discussed in the past, when DuPont left Hanford,
they took all their records with them. We have had no success
in obtaining these records from them.”

However, at least some DuPont operational records, as distinguished
from individual records which were all destroyed, have survived.
Reference is made to the Weekly H.I. Reports on the 200 Area for 1-5-45

thru 2-13-46, Parker, 7-1115-DEL. These reports indicate there is a
reasonable likelihood that such radiation doses as revealed in these reports

would have created a Health Endangerment for the Hanford DuPont
workers but does not show levels of exposure similarly high to those
occurring during nuclear criticality accidents. See Exhibit B.

IL.

WHY THE NIOSH DOSE RECONSTRUCTIONS BASED ON
ORAUT TECHNICAL BASIS DOCUMENTS ARE INVALID FOR
DUPONT OPERATIONS WHICH TERMINATED SEPTEMBER 1”,

It is important to recognize the development history of the inhaled
exposure in any dose reconstruction (DR) attempted for DuPont workers at
Hanford. The DR work has been done by Oak Ridge Associated
Universities Team (ORAUT) under contact with NIOSH.

1) Since there are no individual dosimetry records, the ORAUT dose
reconstructions for Hanford DuPont workers have attempted to establish
generic inhalation exposures based on estimates of the various
radionuclides being released into the air from the separations plants.

2) The generic exposures used are from the ORAUT Technical Basis
Documents that characterize the Hanford site exposure conditions, (See

Page 3 of 21



aged irradiated fuel has been sent by mistake from the reactors to the processing area” where fission
products may be released. The control systems to prevent this had a “weakness” as attested by the
“occasional shipments of fresh fuel”. HW 84001, Sept. 14, 1966 says that “The potential of shipping
a bucket of metal that has aot had sufficient decay time is a common problem ...”. Thus violation
of FIFO occurred fiom time to tame. 1fJ-131 emission were calculated on the basis of stack sample
emissions the extra pulse of I from a FIFO violation would be noted in the sampling and taken into
account, However if total emission be calculated from reactor power and other characteristics,
including the assumption of FIFO, violation of the protocol would result in an underestimate of the
actual I emission.

Ten docaments [HW 32916 Aug. 56, 56029 Aug. 54, HW 33266 Sept. 54, 39260 Oct. $5,
HW 58330 Nov. 58, HW 58305 Dec. 58, 2191065 May 62, HW.89067 Sept. 63, HW 83869 Ang.
64, HW 84001 Sept. 64] found and read refer to FIFO violation or its results between 1954 and
1964. In this period, the emission was usually of the order of 1 Ci per day; the reported excess
“emissions (as indicated by the abave documents) were in each case less than 10 Ci except for HW
32916 (up to 75 Ci) HW 58305 (20 Ci), 2191065 (May9 1962, 40 Ci} and HW 89067 (Sept 63, the
“Hom Rapids” release of 60 Ci). The Dec. 1949 deliberate use of green fuel (the Green Run) which
produced 7000 Ci of emission is not inchded above as it was deliberate.

Pre - 1954 there is need for computation. FIFO was violated pre-1950 - Jaech (FTS - CLVI-
73) documents that metals from pushes in January 1946 (days 480 and 482) were dissolved in June,
after metals pushed in February and in March (days 519, $33 and 538), But would the pre - 1950
batch-by-batch calculation be more likely to note and take account of FIFO violation; would the
_ Telative inexperience of operators lead to greater probability of FIFO or would have operators
become more cavalier as time went on? It should be noted that the figures above (a total of ~200 Ci
in an overall emission of 6000 Ci) indicate an increase of 3% in emission dus to FIFO violation; and
that a corresponding probability in the 1950 to 1953 period would lead to an extra 0.03 «
40 000 Ci= 1180 Ci. And correspondingly, on the reasonable hypothesis of a linear relationship
between output and-dose (and effect) there would be a 3% increase in dose to all exposed,

We noted that in the period 1954 to 1964 there were remarked-on violations of FIFO. We
also noted that these marked violations produced 3% increase in I output over expected. But the
probability of violations resulting in individually smalt increases in output is much higher (with a train
of 10 events, there is only one way one can transpose the beginning aud the end, but 9 ways one can
transpose next-door neighbours). We feel it very conservative to round-up the factor of 1.03 (3%)
to 1.05, and this $% figure is used henceforward. .

Considering all the uncertainties, it may fairly be said that there is indeed evidence of FIFO
violation, even until 1964, and that there is little reason to believe violation was less probable pre -
1954, and that therefore the HEDR estimations of emission may reasonably be thought to be a few
percent underestimated for the period 1950 - 53. For the period 1944 to May 46, there was
apparently [He(92) p 2.4] a0 knowledge of the push data for a particular batch and so, to reconstruct
the operations, again an orderly queuing was assumed. As there may well have been violations of
FIFO (which in that high output time for lack of experience would have gone unnoticed), the factor



~ ...3. Hagley MUSEUM AND LIBRARY

Thank you for your letter of March 28, 2002. Hagley’s records relating to the
Hanford Site are quite fragmentary. as they primarily consist of contract files and in-
house histories. We do not have any documentation about employment. medical. and
radiation exposure.

aave an} further questions about our collections piease Feel tree to contac:

Sincerely,

fe | Wut fIAAS

Chief. Curator,
Library Collections

”

MN/mem



I.
DUPONT RECORD DESTRUCTION
(Exh. A Enclosures)

a) Title page and page 2 from the Hanford monthly report for March
1950 states:

“Shipment to the Du Pont Company of copies of essentially all
classified records accumulated by the Operation’s Central Files
during Du Pont’s tenure at Hanford was made on March 29.
This material, comprising 263 packing cases, covers the period
From the fall of 1943 through August 31, 1946. Only about 4
packing cases, consisting of records presenting special
documentation problems, remain to be processed.”

b) Letter of April 2, 1990 from DuPont legal department stating:

“The Hall of Records has informed me that the only surviving
records are payroll records of employees working at the ste.
All other records were either destroyed or turned over to the

Atomic Energy Commission in the mid-1970’s.”

c) Letter of March 21, 2002 from the FOIA officer for the Hanford
Department of Energy states:

‘It is our understanding that employment, medical, and
radiation exposure records of individuals whose employment
‘terminated during the Hanford-DuPont contracting period
(1943-1946) or who left Hanford and continued their
employment with DuPont at the end of the contracting period
were archived with DuPont and have subsequently been
destroyed. You may wish to contact the organization that
maintains Du Pont's historical records to obtain more detailed
information. The address is as follows: Hagley Museum and
Library, Business Archives, Attention Michael Nash, P.O. Box
3690, Wilmington, Delaware 19807-0630.”

d) Letter of April 2, 2002 from Hagley DuPont Museum:

“Hagley’s records relating to the Hanford Site are quite

Page 2 of 21



L Main References

[Bu91} PNL-7210HEDR: "Fission Product Iodine During Early Hanford Site Operations: Its
production and Behavior During Fuel Processing, Off-Gas Treatment and Release to the
Atmosphere", LL. Burger (1991).

[Ev89} G.J. Evans, RE. Jervis, SM. Mirbod, "Iodine Speciation and Volatility in Relation to
Accidental Releases from Nuclear Reactor Facilities", Proceedings of 1988 Amer. Chem.
Society Symposium: “Nuclear Reactor Severe Accident Chemistry", ACS, Washington
publisher, p. 245 (1989).

[Ev94] G.J, Evans, C. Deir, J.M. Ball, "Retention of Iodine in Stainless Steel Sample Lines", 23"
DOE/NRC Nuclear Air Cleaning and Treatment Conference, 12 pp. (1994).

[Farris 96] W.T. Farris et al_, Radiation Doses from Hanford Site Releases to the Atmosphere and
the Columbia River, Health Physics vol 71 (1996) p 588 .

[Gy92] SP. Gydesen Selected Monthly Operating Data 1944-72 HW89085, PNWD 2028 (1992).

[He92] PNWD-2033 HEDR, "Todine-131 Releases From the Hanford Site, 1944 Through 1947",
CM. Heeb (1992).

[He94] PNWD-2222 HEDR, “Radionuclide Releases to the Atmosphere front Hanford Operations,
1944-1972", CM. Heeb (1994).

[Ke94} HEDR-2235, "Vegetation Radiomuclide Contamination Overview for Hanford and Vicinity,
1957", J. Keene (1994).

[Ma88] E.1 Mart, Batelle memo, Feb 10/88 {Bates no. 4014214}, "Hanford's Air Monitoring
~ “Program from 1945 to 1955", (1988).

[Ma89} HEDR-0342: "Preliminary Estimates of Biases in the Reported 1-131 Concentrations in
Vegetation from Sep/45 to June/S7”, E.L. Mart, (1989).

{Metal Histories} FIS 71
FTS 179
FTS 311
HW 89085

[Pa51} HW-21891, "Summary of Measurements for the Activity Density from I-131", H.J. Paas, LK.
Soldat, (1951).

[Shipler 96] D.B Shipier et al., Hanford Environment Dose Reconstruction Project - An Overview
Health Physics vet 71 (1996) p 532.

19



C. Hanford Introduction

In this report we consider the validity and accuracy of the I-131 releases estimated for HEDR.
from the Hanford Site 200 B, T and REDOX plutonium extraction plants over their operating
lifetime. While some of the HEDR calculations were based on historical records of fuel inventories
and of various release measurements, a number of significant assumptions were made also and several
of these were erroneous. The assumptions made were mostly conservative and led to (significant)
underestimation of radioiodine releases during some of the early years of operation. Later, emaission
control devices and extension of fuel cooling times before processing were introduced to mitigate

eteleases because of concerns about high emission Jevels of I-131 such as occurred during the years
ptior to 1951.

fn order to evaluate the HEDR calculations we have had to review the timing of plant start-
ups, fuel histories and processing records, the sequence of installation of the various emission cortrol
devices and their reputed efficiency and performance testing.

Jodine 131, a radioisotope of half-life 8 days, radioactive decay constant 4 = 0.0862 days”,
is a fission product released on dissolving of irradiated U fuel. The route by which biological harm
may have been caused to nearby resident and neighbouring communities by effluent iodine from the
Hanford works can be broken up into different stages.

(a) __ the production of the fission products in slugs and their ejection from the reactors

(bh). the "cooling time", in which I-131 partially decays

(c) _ the emission of 1-131 resulting from the dissolving of cooled fisel slugs

(d) the filtering of the effluent iodine

(e) distribution of effluent iodine

iC) pick-up into the human system with a radiation dose being given, poimarily to the
thyroid .

(g) _ - biological effect of that dose ©

It may first be noted that very great time and effort has been expended in the HED
Reconstruction of]-131 emissions. Scoping calculations and knowledge of similar systems have been
used by the present writers to show to their satisfaction that ab initio detailed recalculation is
unnecessary even if it were possible; but this same approach showed that in particular parts of the
whole reconstruction erroneous assumptions had been made, in all good faith. We concentrate our _
efforts in these parts of the whole in sections D and E, while consequences are discussed in G and H.
D deals with “cooling times” and E with “fractional releases”.

By the end of 1949, 90% or more of the total nominal emission of I-131 had taken place. In
much Jater years the emissions were lower and so less hazardous. Nevertheless, the uncertainties in
measurement and assumptions made in calculation of releases in the fifties led to the need for carefiul
assessment, to check on biologically significant releases in the earlier part of that decade, for instance
when Ag reactors were being "broken-in". However, releases after 1956 were so sniall that this
petiod has been ignored.



reduced losses further, about tenfold according to various estimates [He92]. Iodine emissions had
also been mitigated to some extent in the interval by increases in fuet cooling times from 30-40 days
to 90-100 as detailed above in Section D. However, by that time, computations from fuel content
indicate that more than 700,000 Ci, had been vented through the Hanford 200 site stacks.

That HEDR [He9Z, He94} neglected most of the historic data on 1-131 stack release
monitoring results and based most estimates of releases on computations of firel content and on
‘generic release factors (RF’s)’ was presumably due to the considered unreliability of stack
measurements (with implicit sources of error, detailed above). Also, because of the variability of

arly B and T plant emission measurements even after Ag reactors were commissioned, Heeb [He94}
evaluated R.F's froma set of 1959 measurements at REDOX and applied them to 1951-56 and 1951-
52 operations at the more primitive T and B plants, respectively. The continuous, on-line 1-131 stack
monitors were not independently calibrated and considered only asa qualitative indication of emission
levels but did serve to alert operators about abnormal release events which occurred not infrequently
-and were related to breakdowms of the Ag reactors and filters [Bu91}. The inaccuracies of measured
iodine removal efficiencies of the control devices, and the validity of assuming that 1959 release
estimates from REDOX could be applied for calculating 1951-56 releases from the older plants, are
further considered below,

In May, 1948, water scrubbers were installed over the fel dissolver tanks of the B and T
plants to treat the “off gases” and in Nov/Dec ‘48, dry sand beds were installed to ‘filter’ an estimated
7.5% of 1-131 escaping into the plants’ ‘canyon’ ventilation system, mainly to trap particulate iodine
with varying efficiencies, depending on the extent of condensation occurring. Deep bed fibre glass
filters were later installed in Oct.(B plant) and Dec ‘50 (T) also in an attempt to reduce particulates
and sprays. Finally, because emissions were estimated still to be over 25%, the filter beds were
deployed in series with silver nitrate-coated reactor columns in Nov, 1950 (T plant) and Jan, 1951
{B). Radioiodine releases from each plant were estimated for HEDR by Heeb [He92, He94] on the
basis of various measurements of the filtering/trapping efficiencies of the control devices used at
different times. Heeb provides a summary of the “best estimate’ release factors:

RF. = (radioiodine released from piant) (calc. fuei radioiodine content)

Release factors for the period 1944 to May, 1948 were based on a mean estimate of 86% I-
131 released, with sparging, from dissolver gases, with a further 5-10% lost during subsequent
processing steps and approximately 3% contained in stack condensate, or

RF. =0,86 +(5 + 10/2 - 0.03 = 0.90,.

Tests of the removal fraction of the 1948 water scrubbers yielded highly variable results which can
be explained on the basis of the chemical form(s) expected in the oxidizing conditions of the
dissolvers: estimates would be approx. 85% inorganic, 15% organic with a fraction of each contained
in off-gas droplets and particulates [Ev89}. Water scrubbers are efficient for tapping the latter, less
so for iodine and inefficient (< 20%) for organic iodides. Heeb [He92} reported that about 75% of
1-131 was removed by the scrubbers, or,

2



Exhibit B



fractions depends upon three factors:

First: All the emission control devices in operation at the time a RF is
calculated must identified. This was not done adequately.

Second: The efficiency of each device must be known along with the
efficiency of two or more of the devices in combination. This was not fully

applied.

Third: The sampling measurements of releases must be reasonably
accurate. This is the Achilles heel of even the best efforts to calculate RF.
Before a back-extrapolation is even made to calculate an RF, it is necessary
to have reasonably accurate sampling measurements of activity being
released. Such sampling measurements were not available. Not the least of
the problems is that the sampling filters being used, from CWS paper to the
Whatman 40 to the HV-70 to measure releases, were not adequate to “see”
or capture all of the sub-micron size particles being released, which
accounted for most of the number of particles being released.

“The first quarter 1949 report (HW-14243) states that the CWS filter
paper used in the air monitoring program had been shown to be about
3.5% efficient for gaseous radioiodine.” Till, 2002, Pg. #4-10 and Pg. #4-
1.

See also Exhibit G, Use of Natural Airborne Activity to Evaluate

Filters for Alpha Sampling, Lindeken, 1961, pg. 44, showing HV-70 filters
at Just 18% to 28% of alpha activity absorbed depending on the thickness.

Lastly, see attached Exhibit H, Notes of Interview With Bernard
Saueressig on 8/15/96, confirmed with his signature and initials. “We did
not try to catch those particles less than 2 microns.”

It is clear the sampling results upon which RF were being calculated
were results of dubious reliability, considering that much of the activity was
not being captured by the sampling.

Vi.

TILL’S MODIFICATIONS OF HEEB

Page 13 of 21



[Soldat 65] K. Soldat, Health

Physics, (1965) vol 11 P 1009 and HW89067. See also Unusual
Radiation Release to

Atmosphere Pyrex Plant - Sept 2 1963 - 4006052, NP 1965 11 p1009.

20



.

Academic and Professional Experience: R. E. JERVIS

I am presently Prof. Emeritus, Nuclear Science and Engineering., Univ. of Toronto, and
a nuclear consultant”.

After earning an undergraduate degree in Physics and Chemistry majors in 1949 at
Toronto, I undertook master’s and doctoral research in physical chemistry, programs that included
formal instruction in nuclear physics and radiochemistry. As a research nuclear chemist at the
Chaik River Nuclear Laboratories, Atomic Energy of Canada Ltd. starting in 1952, I engaged in
radiochemical extractions of plutonium and heavy actinides, radioiodines and other fission
products using Geiger counters, alpha chambers and rudimentary gamma-ray spectrometers (all
techniques and procedures contemporary with and relevant to Hanford operations at the time). I
participated in investigations into the monitoring of radionuclide releases, including iodine, from
reactor and chemical processing stacks using various filter types. Other research done in
cooperation with GE and Westinghouse involved at-power testing of the integrity of prototype
power reactor and submarine fuel using rapid radioiodine detection for early fuel failure
recognition. As developer in Canada of the applied radiochemical technique of RAA,
radioactivatiou analysis, I have measured major and trace levels of many radioisotopes in
solutions, air filters and biological materials.

In 1958 J accepted a faculty position at the Univ. of Toronto in the Applied Science and
Engineering Faculty as Professor, Nuclear Science and Eng. Among academic research projects
undertaken since (and published in 230 papers) have been: measurements of iodine and other
inorganics in urban air filters; developing size ~ selective aerosol sampling with the aid of electron
microscopy; application of different receptor models for air pollution source recognition and
apportionment based on particle-size characteristics and correlated concentrations, studies of the
chemical siates of radioiodine as released from reactor fuel under accident conditions, their
air/water/steam partitioning and the relative volatilities, solubilities and absorbabilities of I, , I
, IO; , organic-I and. I-bearing aerosols. These latter studies-were done for redctor safety in
cooperation with AECL and the Ontario Hydro, Canada largest nuclear utility.

Thave been active in developing and promoting environmental and nuclear safety standards
with the CSA (Can. Stds. Assoc.), jatterly as Chair, Advisory Comm. on Nuclear Safety of the
Atomic Energy Control Board of Canada, regulator of all Canadian nuclear activities. I have been
named Fellow: Can. Soc. Chemistry; Can. Nuclear Soc.; Royal Soc. of Canada; Amer.
Scientific Affiliation; have been honored with 3 international medals and other of awards. A
registered (licensed) Professional Engineer since 1963; consultant on research reactors and
radioisotope applications to the UN Agency: International Atomic Energy Agency, Vienna;
Associate Editor of an international radiochemical journal.

* (see attached C.V. for details)



VIL.
ORAUT’S MODIFICATIONS OF TILL

ORAUT’s calculation of dose estimates are based upon
Heeb, 1994, and Till, 2002, as modified by ORAUT. ORAUT developed an
individual dose calculator utilizing RATCHET, the HEDR air dispersion

sub-program.

“5.2.1 Plutonium. By far the most serious intakes at Hanford involved
plutonium and “Am. Routine urinalyses for plutonium started in

September 1946.” Technical Basis Document for the Hanford Site —
tional In’ : ORAUT-0006-5, Pg. #13. [*]

“Air sampling was performed in facilities from the earliest days of
operation. Workers routinely exposed to areas with detectable airborne
concentrations or performing high risk jobs that might produce airborne
contamination were on routine bioassay schedules (except prior to about

1948).” [*] ORAUT-0006-5, Pg. #48.

“For routine releases from T and B plants the estimated monthly
release is the product of the following factors:

¢ The monthly processing rates for each radionuclide compiled by
Heeb (1994), which are the rates at which the radionuclide enter the
separation plants as irradiated fuel from the reactors. The
processing rates were estimated by Heeb (1994) for Sr,
Ru, Ru, “1, “Ce, and *°Pu and by Till et. al. (2002) for
70g.
« The release fraction which is the ratio of the rate that the
radionuclide was released to the processing rate of the radionuclide.
+ The “effluent treatment modifier” which accounted for
increased release rates in the early years of operation of T and B
plants when there were no scrubbers or filters on the effluents.”

hnical Basis Do it for thi rd Site — Occupational

Environmental Dose: ORAUT 0006-4, Pg. #10.

“The computer file scrlist.dat (Till et al. 2002) provided the
initial source terms in the spreadsheet. That file was based on

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