EPA-600/3-77-067
June 1977
Ecological Research Series
129
I IN ANIMAL THYROIDS FROM NEVADA
AND OTHER WESTERN STATES
Environmental Monitoring and Support Laboratory
Office of Research and Development
U.S. Environmental Protection Agency
Las Vegas, Nevada 89114
-------
RESEARCH REPORTING SERIES
Research reports of the Office of Research and Development, U.S. Environmental
Protection Agency, have been grouped into nine series. These nine broad cate-
gories were established to facilitate further development and application of en-
vironmental technology. Elimination of traditional grouping was consciously
planned to foster technology transfer and a maximum interface in related fields.
The nine series are:
1. Environmental Health Effects Research
2. Environmental Protection Technology
3. Ecological Research
4. Environmental Monitoring
5. Socioeconomic Environmental Studies
6. Scientific and Technical Assessment Reports (STAR)
7. Interagency Energy-Environment Research and Development
8. "Special" Reports
9. Miscellaneous Reports
This report has been assigned to the ECOLOGICAL RESEARCH series. This series
describes research on the effects of pollution on humans, plant and animal spe-
cies, and materials. Problems are assessed for their long- and short-term influ-
ences. Investigations include formation, transport, and pathway studies to deter-
mine the fate of pollutants and their effects. This work provides the technical basis
for setting standards to minimize undesirable changes in living organisms in the
aquatic, terrestrial, and atmospheric environments.
This document is available to the public through the National Technical Informa-
ttonS^Vice, Springfield, Virginia 22161. ,
-------
EPA-600/3-77-067
June 1977
129I IN ANIMAL THYROIDS FROM NEVADA AND OTHER WESTERN STATES
by
D. D. Smith
Monitoring Systems Research and Development Division
Environmental Monitoring and Support Laboratory
Las Vegas*. Nevada 89114
ENVIRONMENTAL MONITORING AND SUPPORT LABORATORY
OFFICE OF RESEARCH AND DEVELOPMENT
U.S. ENVIRONMENTAL PROTECTION AGENCY
LAS VEGAS, NEVADA 89114
-------
DISCLAIMER
This report has been reviewed by the Environmental Monitoring and Sup-
port Laboratory-Las Vegas, U.S. Environmental Protection Agency, and approved
for publication. Mention of trade names or commercial products does not
constitute endorsement or recommendation for use.
ii
-------
FOREWORD
Protection of the environment requires effective regulatory actions
which are based on sound technical and scientific information. This infor-
mation must include the quantitative description and linking of pollutant
sources, transport mechanisms, interactions, and resulting effects on man and
his environment. Because of the complexities involved, assessment of specif-"
ic pollutants in the environment requires a total systems approach which
transcends the media of air, water, and land. The Environmental Monitoring
and Support Laboratory-Las Vegas contributes to the formation and enhancement
of a sound integrated monitoring data base through multidisclplinary, multi-
media program designed to:
•develop and optimize systems and strategies for moni-
toring pollutants and their impact on the environment
•demonstrate new monitoring systems and technologies by
applying them to fulfill special monitoring needs of
the Agency's operating programs.
This report discusses the levels of iodine-129 found in the thyroids
collected from domestic and wild animals from the Nevada Test Site and other
western states. The results of this biological monitoring may be used to
estimate the significance of iodine-129 contamination resulting from the
nuclear testing program. This report should be of value to other researchers
and to such agencies as the Office of Radiation Programs and the Nuclear
Regulatory Commission. Further information on this subject may be obtained
by contacting the Farm and Animal Investigation Branch of the Monitoring
Systems Research and Development Division, Environmental Monitoring and
Support Laboratory, Las Vegas, Nevada.
Director
Environmental Monitoring and Support Laboratory
Las Vegas
iii
-------
CONTENTS
Foreword ill
Tables v
Introduction 1
Conclusions 1
Recommendations 1
Materials and Procedures 2
Results and Discussion 3
References 5
Appendices
A. Technical Approach: Neutron Activation of Thyroid
Samples and Iodine-129 Analysis by General Electric
Company, Vallecitos Nuclear Center, Pleasanton,
California 15
B. Technical Approach: Neutron Activation of Thyroid
Samples and Iodine-129 Analysis by Applied Physical
Technology (APT), Smyrna, Georgia 16
iv
-------
TABLES
Number
1 Summary of 129I Thyroid Samples from Cattle - Area 18, NTS 6
2 Summary of 129I Thyroid Samples from Area 18 Cattle -
Area 15 Feedlot for 4.5 Months 8
3 Summary of 129I Thyroid Samples from Cattle and a Coyote -
Area 15, NTS 9
4 Summary of 129I Thyroid Samples from Cattle, Goats, and
Foxes - Area 13, NTS 10
5 Summary of 129I Thyroid Samples from Mule Deer - NTS 12
6 Summary of 129l Thyroid Samples from Cattle - Northern
Nevada 13
7 Summary of 129I Thyroid Samples from Cattle - Rocky Flats,
Colorado 14
8 Summary of 129I Thyroid Samples from Elk - Wyoming 14
-------
INTRODUCTION
For years, the nuclear tests conducted at the Nevada Test Site resulted
in the formation of iodine-129. It was presumed that the iodine-129 would
result in some degree of dosage to the thyroid of the local animals. How-
ever, prior to this study, the thyroid iodine-129 burdens had not been deter-
mined for either wild or domestic animals that live on and near the Nevada
Test Site.
This study was conducted to measure the concentrations of iodine-129 in
the thyroids of animals that reside on and around the Nevada Test Site, and
to correlate these data with those from similar studies made around other
nuclear facilities. The animals sampled included various species of wild
animals and cattle from herds maintained on the Nevada Test Site since 1957
as biological monitors as well as cattle and goats used for special research
projects.
CONCLUSIONS
Although levels in thyroids from Nevada Test Site cattle are statisti-
cally higher than levels in a northern Nevada background population, they
are similar to those considered to be background by other investigators. The
iodine-129/iodine-127 atom ratios reported are several orders of magnitude
lower than those reported for animal thyroids collected near nuclear separa-
tion facilities. These findings indicate that the Nevada Test Site is not a
significant source of iodine-129.
RECOMMENDATIONS
Because of the possible higher levels of iodine-129 in the thyroids of
Nevada Test Site animals, it is recommended that periodic surveillance of
iodine-129 levels be continued by collecting thyroids from free-ranging deer
and cattle, and analyzing them by neutron activation analysis.
-------
MATERIALS AND PROCEDURES
To attain the objectives stated in the introduction, thyroids were col-
lected from animals sampled during the routine Animal Investigation Program
surveillance activities with Nevada Test Site wildlife and the beef herd as
described by Smith et al. (1976a). In addition, thyroids were collected from
animals dying of natural causes at the Area 15 farm, from those sacrificed
for other studies (e.g., salt feedlot studies, Shuyler et al., 1975), for the
Area 13 grazing studies (Smith et al., 1976), and special investigations
(Smith and Black 1975). During the annual hunting season, thyroids were col-
lected from deer and elk in northern Nevada, Utah, and Wyoming. In addition,
thyroids were collected from cattle slaughtered in certain abattoirs of
northern Nevada to provide baseline values.
After collection, each thyroid was trimmed, weighed, and frozen. Thy-
roids of foxes and rabbits from the same area were pooled in order to have at
least 1 gram of tissue. Each thyroid sample was placed in a plastic envelope
with powdered paraformaldehyde prior to shipment to the analytical laboratory
in lots of 20.
Preliminary investigations were made to determine the method of choice
for the analysis for iodine-129 in the thyroids. Methods considered were the
Phoswich detector, liquid scintillation, and neutron activation. Although
iodine-129 is a radioactive nuclide, its extremely long half-life (1.7 x 107
years) results in a specific radioactivity of only 163 microcuries per gram.
Furthermore, the low energy of its radiations (150 kiloelectronvolt beta
and 38 kiloelectronvolt gamma) also makes detection by ordinary counting tech-
niques very difficult. A reasonably large cross section (27 barns) for ther-
mal neutron capture, leading to the formation of the activation product
iodine-130 with a 12.6-hour half-life, makes the detection of iodine-129 by
neutron-activation analysis highly practical. This method of analysis was
chosen and a request for a proposal was prepared in November 1973. On May 10,
1974, a suitable contractor was selected and thyroids samples were submitted
for analysis during May, August, and December 1974, and May 1975. Unfortu-
nately, several of these samples (among them composite rabbit thyroid samples
and thyroids collected from deer in northern Nevada and Utah) were lost during
the analytical procedures. A total of 40 samples was successfully analyzed
by the contractor.
While the original contract negotiations were in process, five bovine
thyroids were analyzed by the successful bidder and another five were analyzed
by a second applicant. In April 1975, a contract was awarded to a third
applicant to provide neutron activation and iodine-129 analysis of 60 thyroid
samples. These samples were sent to the second contractor in May and Septem-
ber 1975, and February 1976.
The neutron-activation and analytical procedures utilized by the two
contractors are described in appendices A and B. Basically, both companies
used the neutron-activation technique outlined by Magno et al. (1972).
-------
RESULTS AND DISCUSSION
After the data were received from the analytical laboratories, they were
tabulated according to the geographic location and date of collection.
Tables 1 through 4 present analytical data about the thyroids collected from
cattle maintained in Areas 18, 15, and 13 of the Nevada Test Site. In addi-
tion, analytical data on the thyroids collected from several goats, foxes,
and coyotes from these same areas are given in these tables. Table 5 pre-
sents data on the thyroids of mule deer collected in the mountainous areas of
the Nevada Test Site. Tables 6 and 7 present thyroid data from cattle that
grazed areas that were 650 kilometers (northern Nevada) and 1,600 kilometers
(Rocky Flats, Colorado) from the Nevada Test Site. Table 8 presents data
from two elk collected in Wyoming. These tables also include information
about the animals sampled, collection dates, micrograms of iodine per gram of
tissue, picocuries of iodine-129 per gram of tissue, and picocuries of
iodine-129 per gram of iodine. In order to assess whether the iodine-129
levels were elevated and to facilitate the comparison of these data with the
data of other investigators in other parts of the country, the iodine-129 to
iodine-127 atom ratios were also calculated.
Brauer et al. (1974) list typical values of the iodine-129 to iodine-127
atom ratios for cattle thyroids near nuclear separation facilities as
4 x 10~6. They found a typical ratio of 8 x 10~9 in States such as Wisconsin,
Kansas, and Texas, which are considered as background values in this report.
Magno et al. (1972) reported atom ratios from bovine thyroids collected in
the vicinity of the Nuclear Fuel Services Plant in New York ranging from
1.6 x 10 about 1.6 kilometers from the stack to 2.2 x 10~5 about 16 kilo-
meters from the stack. In the same report, atom ratios are given for bovine
thyroids from the Boston area (background) varying from 1 x 10~7 to 4 x 10~7.
In a personal communication, R. C. McFarland of Applied Physical Technology,
Smyrna, Georgia, (July 9, 1975) stated that small animal thyroids from the
South Carolina areas have atom ratios on the order of 2 x lO"4. Examination
of the data contained in tables 1 through 8 show that the iodine-129 to
iodine-127 ratios reported fall between the two background ranges cited by
Brauer and Magno.
The atom ratios in thyroids collected from beef cattle of northern
Nevada (table 6) approach the background levels cited by Brauer and are gen-
erally one or two orders of magnitude lower than those observed for the
Nevada Test Site and Rocky Flats, Colorado, beef cattle. The median
iodine-129 to iodine-127 atom ratios in thyroids from the Nevada Test Site
Area 18 beef cattle were 1.5 x io~7 in 1973, 1.6 x io~7 in 1974, and
1.4 x 10~8 in 1975. The apparent decrease in iodine-129 in 1975 may not be
real, but rather may result from differences in analytical reporting by the
two laboratories involved, as most of the thyroids in 1973 and 1974 were
processed by the second contractor.
As shown in table 2, the median iodine-129 to iodine-127 atom ratios of
5.3 x 10~ 9 found in the thyroids of nine Hereford heifers maintained on a fat-
tening ration in a feedlot at Area 15 was the lowest reported for adult
Nevada Test Site cattle. Also, it was noted that the ratio of stable iodine
-------
to tissue was higher in those animals than for all other cattle sampled from
desert environments. Probably the fattening ration fed to these heifers con-
tained more stable iodine than the ration of the other range cattle sampled.
The free-ranging cattle from the Nevada Test Site and Rocky Flats beef
cattle subsisted on the native vegetation of their respective ranges with
little or no supplemental feeding. Therefore, the source of iodine-129 for
these populations was assumed to be local in nature. The Area 15 cattle were
corralled and fed hay and concentrates that originated from commercial
sources away from the Nevada Test Site. The stable iodine content of these
feeds probably had a diluting effect on the iodine-129 intake of these
animals.
The median iodine-129 to iodine-127 atom ratios found in Nevada Test
Site deer thyroids was 8.8 x 10~8 in 1973 and 1974 (six deer) and 2.2 x 10~8
in 1975 (seven deer). It was noted by Ballad et al. (1976) that deer gener-
ally acquire higher levels of iodine-129 than cattle. This relationship is
noted on the Nevada Test Site when the heifers maintained in the Area 15
feedlot are compared to Nevada Test Site deer. It is though that the near
saturation levels of mineral iodine in commercial feeds and salt licks may
account for differences in the iodine-129 levels of cows and deer.
A report by Brauer et al. (1974) listed an average atom ratio of
1.8 x 10~' for four elk thyroids collected in Wyoming during 1963. This
value is very similar to the values listed in tables 8 (2.8 x 10~7 and
1.82 * 1(T7).
Nonparametric statistical tests (the Mann-Whitney U-test, and the
Kruskal-Wallis Analysis of Variance) indicate that the iodine-129 to
iodine-127 ratios in the cattle thyroid data fall into three groups. There
are no significant differences (probability = 0.5727) between the animals
from Area 18 of the Nevada Test Site, Area 13 of the Nevada Test Site, and
Rocky Flats; thus animals from these three geographical areas may be con-
sidered as one group. The cattle from northern Nevada constitute a second
group. The cattle from Area 15 of the Nevada Test Site are a third group
with ratios of intermediate magnitude, but significantly different from the
Nevada Test Site, Rocky Flats group and the group of northern Nevada cattle.
On the basis of these tests, the probability that the paired groups of cattle
have the same average isotope ratios are summarized as follows:
a. The probability that the Area 15 thyroids would be the same as
those from northern Nevada is 0.0097.
b. The probability that the Nevada Test Site and Rocky Flats thyroids
would be the same as those from northern Nevada is 0.00001.
c. The probability that the Nevada Test Site and Rocky Flats thyroids
would be the same as those from Area 15 is 0.004.
The Bonferonni principle states that in order for all these probabili-
ties to be simultaneously true at the 5 percent level (95 percent confidence)
each one must have a probability of 0.01 or less; this was found to be the
case for this data set.
-------
REFERENCES
Ballad, R. V., et al. "Iodine-129 in thyroids of grazing animals." Health
Phy_s. 30:245-350. 1976
Brauer, F. P., et al. "Natural Iodine and Iodine-129 in Mammalian Thyroids
and Environmental Samples Taken from Location in the United States."
IAEA-SM-ISO/34. Symposium on Environmental Surveillance Around Nuclear
Installations. Warsaw, November 5-9, 1973. 1974
Magno, P. J., et al. Iodine-129 in the Environment Around a Nuclear Fuel
Reprocessing Plant. ORP/FOD 72-5. USEPA. Office of Radiation Programs.
23 pp. 1972
Shuyler, L. R., et al. "Excretion of Salts by Feedlot Cattle in Response to
Variations in Concentrations of Sodium Chloride Added to Their Ration."
pp. 336-343. PROC-275. Managing Livestock Wastes—1975. American
Society of Agricultural Engineers. 1975. Presented at the 3rd Inter-
national Symposium on Livestock Wastes—1975 at the University of
Illinois, Urbana-Champaign, Illinois, April 21-24, 1975.
Smith, D. D., et al. Animal Investigation Program 1972 Annual Report.
NERC-LV-539-35. U.S. Environmental Protection Agency, National Environ-
mental Research Center, Las Vegas, Nevada. 82 pp. 1976a
Smith, D. D., et al. "Grazing Studies on a Plutonium-Contaminated Range of
the Nevada Test Site." pp. 325-336. IAEA-SM-199/73. Proceedings of
International Atomic Energy Agency Symposium on Transuranium Nuclides
in the Environment. San Francisco, California, November 17-21, 1975.
1976b
Smith D. D. and S. C. Black. Actinide Concentrations in Tissues from Cattle
Grazing Near the Rocky Flats Plant. NERC-LV-539-36. U.S. Environmental
Protection Agency, National Environmental Research Center, Las Vegas,
Nevada. 47 pp. 1975
-------
TABLE 1. SUMMARY OF 129I THYROID SAMPLES FROM CATTLE - AREA 18, NTS
Sample
Identification
BOV-l-NTS-73*
BOV-3-NTS-73*
BOV-4F-NTS-73*
BOV-6-NTS-73*
BOV-7-NTS-73*
BOV-8-NTS-73*
BOV-10-NTS-73*
BOV-ll-NTS-73*
BOV-12-NTS-73f
BOV-l-NTS-74*
BOV-2-NTS-74*
BOV-3-NTS-74*
BOV-4-NTS-74*
BOV-5-NTS-74*
BOV-6-NTS-74*
BOV-8-NTS-74*
BOV-9-NTS-74*
BOV-l-NTS-75f
BOV-2-NTS-75f
BOV-3-NTS-75f
BOV-4-NTS-75f
BOV-5-NTS-75f
Collection
Date
05/16/73
05/16/73
05/16/73
05/16/73
10/18/73
10/18/73
11/16/73
10/18/73
10/18/73
05/15/74
05/15/74
05/15/74
05/15/74 "
05/15/74
05/15/74
10/24/74
10/24/74
05/22/75
05/22/75
05/22/75
05/22/75
05/22/75
yg Iodine
g Tissue
137
45
354
77
698
221
1,230
1,210
150
415
510
200
173
321
760
770
555
762
789
669
487
pCi
izyl
g Tissue
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0090
0023
0126
0029
0096
0060
0075
0109
00096
0052
0088
0050
0080
0178
0156
009
008
0012
0019
0016
0017
00089
pCi 12yl
g Iodine
66
51
36
37
14
27
6.1
9
4.7
34
21
9.9
40
103
49
12
10
2.21
2.52
1.99
2.58
1.84
Atom Ratio
3
2
2
2
7
1
3
5
2
1
1
5
2
5
2
6
5
1
1
1
1
1
• / ^
.9 x
.0 x
.1 x
.9 x
.5 x
• J ^
.1 x
.7 x
.9 x
.2 x
.6 x
o x
Q y
.8 x
.8 x
.7 x
.26
.44
.13
.47
.05
io-7
io-7
io-7
io-7
IO-8
io-7
lO-8
lO-8
IO-8
io-7
10- 7
lO-8
10- 7
io-7
10 7
lO-8
Hereford
Hereford
Fetus of
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Remarks
cow, 2
cow, 5
yrs.
yrs.
dam cow no. 4, 8.5 mos
steer,
female
steer,
cow, 4
cow, 2
steer,
steer,
cow, 6
steer,
1 yr.
, 6 mos .
1.5 yrs.
.5 yrs.
.5 yrs.
1.5 yrs.
1 yr.
yrs.
3 yrs.
cow, 15 yrs.
cow, 3
female
steer,
ID"8 Hereford cow, 9
cell carcinoma
x 1 U
x 1Q-8
x 10~8
x ID"8
x IO-8
Hereford
Hereford
Hereford
Hereford
Hereford
cow, 4
yrs.
calf, 2 wks.
1.5 yrs.
yrs , squamous
of eye
yrs.
cow, 13 yrs.
steer,
steer,
steer,
1 yr.
2 yrs.
1 yr.
-------
TABLE 1. SUMMARY OF 129I THYROID SAMPLES FROM CATTLE - AREA 18, NTS (continued)
Sample
Identification
BOV-7-NTS-75t
BOV-8-NTS-75t
BOV-9-NTS-75t
BOV-10-NTS-75t
BOV-ll-NTS-75t
BOV-12-NTS-75+
BOV-13-NTS-75t
1973 Ran»e
Median
. Range
19/4
Median
1975 Range
Median
Collection
Date
07/29/75
10/16/75
10/16/75
10/16/75
10/16/75
10/16/75
10/16/75
Ug Iodine
g Tissue
500
620
310
990
570
980
650
45-
1,230
179
150-
770
368
310-
990
635
pCi 129J
g Tissue
0.0010
0.0010
0.0012
0.0099
0.0018
0.0036
0.
0.
0.
0.
0.
0.
0017
00096-
0126
0075
005-
0178
0.0084
0.
0.
0.
00089-
0099
00165
pCi 1291
g Iodine
1
1
3
.99
.62
.86
0.995
3
3
2
4
66
27
9
103
27
0
3
2
.12
.69
.56
.7-
.9-
.5
.995-
.86
.4
1291/127! ^ _,_
Atom
1
9
2
5
1
2
1
2
3
1
5
5
1
.14
.25
.20
.68
.78
.11
.46
.7 >
.7 >
.5 >
.6 >
.8 x
.6 >
_ . JxeiuaiR.a
Ratio
x 10
i~B Hereford female calf, 1 yr.,
accident victim.
x 10~9 Hereford bull, 4 mos.
x 10
x 10
x 10
x 10
x 10
' W~
< 10"
' 10
8 Hereford bull, 4 mos.
9
Hereford cow, 4 mos.
Hereford cow, 7 yrs.
Hereford cow, 9.5 yrs.
Hereford cow, 5 yrs.
B-
7
7
: 10-8-
= io-7
: 10"
5.68 x io~
2
1
.2 >
.4 x
: 10~
: 10~
7
9_
8
8
Analytical Laboratory was General Electric Company, Vallecitos Nuclear Center, Pleasanton, California.
Analytical Laboratory was Applied Physical Technology, Smyrna, Georgia.
-------
TABLE 2. SUMMARY OF 129I THYROID SAMPLES FROM AREA 18 CATTLE - AREA 15 FEEDLOT FOR 4.5 MONTHS
oo
Sample Collection
Identification Date
820-NTS-74*
821-NTS-74*
841-NTS-74*
838-NTS-741"
856-NTS-741"
824-NTS-74*
825-NTS-741"
829-NTS-74*
842-NTS-74*
Range
Median
.Analytical
Analytical
11/13/74
11/13/74
11/13/74
11/13/74
11/13/74
11/13/74
11/13/74
11/13/74
11/13/74
yg Iodine pCi 129I
g Tissue g Tissue
920
1,180
1,150
960
500
1,440
1,100
1,260
696
0.0088
0.0093
0.0038
0.0050
0.0050
0.0010
0.0030
0.0051
0.0064
500- 0.001-
1,440 0.0093
1,100 0.0050
Laboratory was
Laboratory was
Applied
General
pCi
129j
g Iodine
0
0
0
5
11
0
3
.960
.785
.328
.717
0.406
0
0
11
0
.926
.328-
.926
Atom
5.48
4.48
1.87
2.8
6.3
4.8
1.7
2.32
5.27
1.87
6.3
5.27
11211
Ratio
x 10- 9
x 10~9
x ID' 9
x 10~8
x 10~8
x 10- 9
x 10-8
x 10~9
x 10- 9
x 10-9-
x 10" 8
x ID"9
Remarks
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
Hereford
heifer ,
heifer,
heifer,
heifer,
heifer,
heifer,
heifer,
heifer,
heifer,
Physical Technology, Smyrna, Georgia.
Electric Company, Vallecitos Nuclear Center, Pleasanton,
1
1
1
1
1
1
1
1
1
.5 yrs.
.5 yrs.
.5 yrs.
.5 yrs.
.5 yrs.
.5 yrs.
.5 yrs.
.5 yrs.
.5 yrs.
California.
-------
TABLE 3. SUMMARY OF J2al THYROID SAMPLES FROM CATTLE AND A COYOTE - AREA 15, NTS
Sample Collection
Identification
COW-16-NTS-73*
BULL-216-NTS-74*
COW-139-NTS-74*
BIG SAM*
BULL-516-NTS-74f
CALF-1-321+
CALF-5-26931"
CALF-4-3231"
CALF-2-3191"
CALF- 3-317 f
CALF-6-320f
CALF-7-326f
t
HEREFORD BULL
Range
Median
COYOTE-l-NTS-75
Date
05/23/73
03/13/74
03/13/74
05/09/74
05/09/74
05/22/75
05/22/75
05/22/75
05/22/75
05/22/75
05/22/75
09/03/75
09/30/75
07/23/75
yg Iodine
g Tissue
748
160
99
113
951
1,010
1,060
826
373
722
558
620
200
99-
1,060
589
220
pCi 129I
g Tissue
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
<0.
0.
0.
0.
0.
0041
0018
0018
0049
001
0004
0001
0004
00008
0002
0002
0002
0002
00008-
0049
0004
002
pCi 129I
g
5
11
18
44
1
0
0
0
0
0
0
0
<1
Iodine
.5
.33
.424
.106
.535
.205
.291
.302
.307
.21
129IX1
•27I
Atom Ratio
3.1 x
6.2 x
1.0 x
2.5 x
7.61 x
2.42 x
6.05 x
3.05 x
1.17 x
1.66 x
1.73 x
1.75 x
6.91 x
10 s
10 8
10 7
10 7
10 9
10 9
10 10
10 9
10 9
10 9
10 9
10 9
10 9
T) 1
Remarks
Holstein cow,
since 1963.
Holstein bull,
Holstein cow,
Hereford steer
lated.
Hereford bull,
Holstein-Cross
Holstein male,
Holstein male,
Holstein male,
Holstein-Cross
Holstein-Cross
Holstein male,
15 yrs. ,
4.5 yrs
5.5 yrs.
, 9 yrs.
3 yrs.
female,
1 mo.
2 mos.
3 mos.
female,
female ,
1 day.
Area 15
f istu-
2 mos.
3 mos.
3 mos.
Polled Hereford bull, Area 15
for 3 mos., originated
0
44
<0
8
.106-
.873
.29
6.65 x
2.5 x
1.75 x
4.73 x
CA.
10-10-
10-7
10~9
10~8
Female, 3 mos.
TV-
Analytical Laboratory was
Analytical Laboratory was
General Electric Company, Vallecitos Nuclear Center, Pleasanton, California.
Applied Physical Technology, Smyrna, Georgia.
-------
TABLE 4. SUMMARY OF 129I THYROID SAMPLES FROM CATTLE, GOATS, AND FOXES - AREA 13, NTS
Sample
Identification
COW-2-A13-73*
COW-3-A13-731"
Collection
Date
10/25/73
10/25/73
ug Iodine
g Tissue
112
pCi
1291
g Tissue
0.
0.
00139
00021
pCi 129i
g Iodine
12
2.7
129I/127J
Atom Ratio
6.
1.
8
5
x 10~8
x 10~8
Remarks
Hereford cow, 10 yrs., Area
since May 1973. Originally
Kingman, Arizona.
Hereford-Cross cow, 11 yrs.
13
»
Area 13 since May 1973. Origi-
CALF-12-A13-73*
COW-1-A13-74*
COW-4-A13-74*
COW-6-A13-74*
COW-5-A13-75'*'
10/25/73
07/09/74
07/09/74
07/09/74
07/29/75
496
560
610
860
1,020
0.
0.
0.
0.
0.
0074
0081
0071
0066
004
15
14
1-.6
7.7
3.90
8.
7.
9
4.
2.
5
9
X
4
21
x iQ-8
x 10~8
io--9
x 10~8
xlO"8
nally Kingman, Arizona.
Born Area 13 in May 1973. Dam
cow no. 8.
Angus cow, 12 yrs., Area 13
since May 1973. Originally
Kingman , Arizona .
Hereford cow, 11 yrs., Area
since May 1973. Originally
Kingman , Ar i z ona .
Angus cow, 12 yrs., Area 13
since May 1973. Originally
Kingman , Ar i z ona .
Hereford-Angus cow, 9 yrs.,
13
Area 13 since May 1973. Origi-
CALF-15-A13-75*
CALF-18-A13-NTS"'"
CALF-13-A13-75
COW-30-A13-76
BOV-14-A13-76
BOV-19-A13-76
01/29/75
01/29/75
01/29/75
01/16/76
01/28/76
01/28/76
1,290
629
1,090
690
380
720
0.
0.
0.
0.
0.
0.
005
002
004
004
001
003
3.55
3.93
3.85
5.36
3.62
3.78
2.
2.
2.
3.
2.
2.
02
24
20
06
07
16
xlQ 8
x 10~8
x 10~8
xlO~8
x 10~8
xlO'8
nally Kingman, Arizona.
Angus-Cross bull, 1 yr.
Newborn female calf. Dam cow
no. 5 .
Angus-Cross bull, 1 yr.
Hereford-Cross female, 1 yr
Angus cow, 2.25 yrs.
Angus bull, 0.5 yr.
•
-------
TABLE 4. SUMMARY OF 129I THYROID SAMPLES FROM CATTLE, GOATS, AND FOXES - AREA 13, NTS (continued)
Sample Collection
Identification Date
Range
Median
GOAT-1-A13-73* 08/07/73
GOAT-2-A13-73* 10/25/73
FOXES-A13-74* 05/20/74
Mg Iodine
g Tissue
112-
1,290
660
1,500
126
1,000
pCi 129I
g Tissue
0.00021-
0.0081
0.004
0.0074
<0.0026
0.0260
pCi 129I
g Iodine
2.7-
15
3.93
4.8
<21
<26
129 if 127j
Atom Ratio
1.5 x
8.5 x
2.24 x
2.7 x
<1.2 x
1.5 x
io-8-
io-8
io-8
10-8
10~7
ID"7
Remarks
Female goat, 1 yr., Area 13
since May 1973. Originally
Tuba City, Arizona.
Female goat, 3 yrs., Area 13
since May 1973. Originally
Tuba City, Arizona.
Composite of three foxes.
.Analytical Laboratory was
+Analytical Laboratory was
Analytical Laboratory was
General Electric Company, Vallecitos Nuclear
Georgia Tech Research, Atlanta, Georgia.
Applied Physical Technology, Smyrna, Georgia.
Center, Pleasanton, California.
-------
TABLE 5. SUMMARY OF 129I THYROID SAMPLES FROM MULE DEER - NTS
Sample
Identification
MD-4-NTS-73*
MD-l-XTS-74*
MD-2-NTS-74*
MD-3-NTS-74*
MD-4-NTS-74*
MD-5-NTS-74*
MD-l-NTS-75f
MD-2-NTS-757
MD-3-NTS-751
MD-4-NTS-75+
MD-5-NTS-757
MD-6-NTS-75 '
MD-7-NTS-75
Range
Median
Collection
Date
11/10/73
01/30/74
05/02/74
07/18/74
10/18/74
11/25/74
01/21/75
05/22/75
06/16/75
08/03/75
08/21/75
09/10/75
09/11/75
jjg Iodine
g Tissue
1,500
3,600
1,300
760
1,060
2,600
1,350
517
947
710
680
420
1,350
420-
3,600
1,060
pCi 1291
g Tissue
0.0240
0.2079
0.0270
<0.0100
0.0038
0.037
0.0165
0.0016
0.0169
0.0038
0.00026
-0.00031
0.0043
0.00026-
0.2079
<0.01
pCi 1291
g Iodine
16
58
23
<14
3.54
15
12.2
3.15
17.9
5.27
3.83
<0.744
3.14
<0.744-
58
12.2
1291/1271
Atom Ratio
9.09 x 10~8
3.3 x 10~7
1.3 x 10~7
<7.9 • 10~8
2.02 x 10"8
8.5 x io~8
6.97 x io~8
1.80 x io~fl
1.02 x io~y
3.01 x io~8
2.19 x io~8
<4.25 x io~9
1.79 x io~8
<4.25 x 10~9
3.3 * io~7
6.97 x io~8
Remarks
Mule deer male, 2.5 yrs.,
accident vicitm, Area 19.
Mule deer pregnant doe, adult,
Area 30.
Mule deer male, adult, hunter
kill, Area 12.
Mule deer, adult, road kill,
Area 12.
Mule deer male, 2.5 yrs.,
hunter kill, Area 19.
Mule deer male, 8 to 9 yrs.,
road kill, Pahute Mesa Road,
Area 19.
Mule deer female, 3.5 yrs.,
accident victim, Area 12.
Mule deer male, 3.5 yrs.,
accident vicitim, Area 17.
Mule deer male, 5.5 yrs., road
kill, Area 17.
Mule deer male, 5.5 yrs., road
kill, Area 12.
Mule deer male, mature, road
kill, Area 12.
Mule deer female, 3 yrs., road
kill, Area 20.
Mule deer female, 4 yrs.,
hunter kill, Area 20.
*Analytical Laboratory was General Electric
Center, Pleasanton, California.
tAnalytical Laboratory was Applied Physical
Company, Vallecitos Nuclear
Technology, Smyrna, Georgia.
12
-------
TABLE 6. SUMMARY OF 129I THYROID SAMPLES FROM CATTLE - NORTHERN NEVADA
Sample
Identification
COW-1*
STEER-2*
STEER-A*
STEER- B*
STEER-C
STEER-D*
STEER-E*
STEER-F*
STEER-G*
STEER-H*
STEER-I*
COW-J*
STEER-K*
STEER-L*
UNK-M*
COW-N*
Range
Median
Collection
Date
03/05/75
03/05/75
07/22/75
08/05/75
07/22/75
08/13/75
07/22/75
08/13/75
09/03/75
08/05/75
08/13/75
08/08/75
08/05/75
09/03/75
08/13/75
08/08/75
ug Iodine
g Tissue
644
1,720
492
526
330
1,510
491
876
1,150
1,000
2,170
239
717
1,180
1,520
252
239-
2,170
797
pCi 1291
g Tissue
0
.0008
0.0001
<0
0
0
0
0
0
0
0
0
0
0
0
<0
0
<0
0
0
.0001
.0005
.0002
.00002
.0004
.00005
. 00006
.001
.0006
.0003
.0009
.0001
.00001
.0003
.00001-
.001
.00025
pCi 1291
g Iodine
1
0
<0
1
0
0
0
0
0
1
0
1
1
0
<0
.27
.0742
.262
.04
.687
.0120
.849
.0566
.543
.08
.278
.07
.27
.0960
.0102
1.10
<0.0102-
1.27
0.483
129I/127J
Atom Ratio
7.
4.
<1.
5.
3.
6.
4.
3.
3.
6.
1.
6.
7.
5.
<5.
6.
25
23
50
93
92
85
84
23
10
16
59
11
25
48
82
28
<5.82
7.25
2.76
x 10"9
x 10" 1G
x 10"9
x 10"9
x 10"9
x 10~U
x 10"9
x 10" 10
x 10" 10
x 10"9
x 10"9
x 10"9
x 10"9
Remarks
Cow from Reno.
Steer from Elko.
Hereford-Cross steer,
Hereford-Cross steer,
Polled Hereford-Cross
18 mos. , Fallon.
Hereford steer, Smith
Polled Hereford-Cross
Fallon.
Reno.
Fallon.
steer,
Valley.
steer ,
Angus-Cross steer, Smith Valley.
Hereford-Angus steer,
Humbolt County.
Hereford-Cross steer,
Hereford-Cross steer,
Valley.
Holstein cow, 8 yrs.,
of Nevada, Reno.
15 mos. ,
Fallon.
Smith
University
Angus-Cross steer, Fallon.
x 10" 10 Shorthorn-Cross steer
County.
x IQ"11
x 10"9
Hereford steer, Smith
Holstein cow, 6 yrs.,
of Nevada, Reno.
, Humbolt
Valley.
University
x 10-n-
x 10" 9
x 10"9
*Analytical Laboratory was Applied Physical Technology, Smyrna, Georgia.
13
-------
TABLE 7. SUMMARY OF 129I THYROID SAMPLES FROM CATTLE - ROCKY FLATS, COLORADO
Sample Collection
Identification Date
BOV-2-RF*
BOV-4-RF*
BOV-5-RFf
BOV-6TRF*
BOV-7-RFf
BOV-9-RF*
Median
11/16/73
11/16/73
11/16/73
11/16/73
11/16/73
11/16/73
pg Iodine
g Tissue
1,140
610
400
1,910
147
2,000
610-
2,000
1,525
pCi
129i
g Iodine
0.
0.
0.
0.
0.
0.
0.
0.
0.
0690
0076
0013
0120
0006
0200
0006-
0690
0098
pCi
129i
g Iodine
60
12
3
6
4
10
3
12
8
.4
.3
.3
.1
.1
.3-
.4
.2
Atom
3.4
7.04
1.9
3.6
2.3
5.7
1.9
3.4
4.7
Ratio
x
X
X
X
X
X
X
X
X
10~7
10~8
10~8
10~8
10~8
10~8
10~B-
10~7
10~8
Angus cow
Shorthorn
Hereford
Hereford
Shorthorn
Hereford
Remarks
, 18+ yrs.
female, 6 mos.
cow, 18 yrs.
female, 6 mos.
female, 5 mos.
female, 6 mos.
Analytical Laboratory was General Electric Company, Vallecitos Nuclear Center, Pleasanton, California.
^Analytical Laboratory was Georgia Tech Research, Atlanta, Georgia.
TABLE 8. SUMMARY OF 129I THYROID SAMPLES FROM ELK - WYOMING
Sample
Identification
ELK-1-74*
ELK-2-RAWLINGSf
Collection
Date
10/21/74
10/21/74
yg Iodine pCi I29j
g Tissue g Tissue
760 0.038
554 0.018
pCi 129I
g Iodine
50
31.9
„ . Remarks
Atom Ratio
2.8 x 1Q~7 Hunter kill, Rawlings.
1.82*10~7 Hunter kill, Rawlings.
t
Analytical Laboratory was General Electric Company, Vallecitos Nuclear Center, Pleasanton, California.
Analytical Laboratory was Applied Physical Technology, Smyrna, Georgia.
-------
APPENDIX A. TECHNICAL APPROACH: NEUTRON ACTIVATION OF THYROID SAMPLES AND
IODINE-129 ANALYSIS BY GENERAL ELECTRIC COMPANY, VALLECITOS
NUCLEAR CENTER, PLEASANTON, CALIFORNIA
It is proposed to analyze thyroids received in sets of 20 by the neutron
activation technique as outlined in the U.S. Environmental Protection Agency
report "Iodine-129 in the Environment Around a Nuclear Reprocessing Plant" by
Paul J. Magno, Thomas C. Reavey, and John C. Apidianakis (October 1972),
available from U.S. Environmental Protection Agency, Office of Radiation
Programs, Field Operations Division, Washington, DC 20460. Five to 10 grams
of thyroid are cut in small pieces together with 10,000 dpm of freshly manu-
factured iodine-131 separated from freshly fissioned uranium so as to be low
in iodine-129, and solubilized in alcohol and sodium hydroxide. The mass is
slowly heated over several hours to a final temperature of 600° C to complete
the fusion. Great care must be taken to avoid foaming or rapid reaction.
The sample is cooled, dissolved in water, oxidized with chlorine to exchange
iodine-131 with iodine-129, -127, acidified with nitric acid, and extracted
twice with carbon tetrach^oride and hydroxylamine hydrochloride. The iodine
is back extracted into a sodium sulfite solution.
A second extraction is performed into toluene from nitric acid and
sodium nitrite and back extracted into sodium sulfite solution. The toluene
extraction is repeated once again and extracted into amonium sulfite to
separate the iodine from bromine. The ammonium sulfite solution is gently
evaporated to dryness in a quartz ampoule, sealed, and irradiated in the
General Electric Test Reactor for 1 to 4 hours at 8 x 1013 neutron flux in
the shuttle tube. One hour is required for samples greater than 4 grams.
A 1-gram sample requires 4 hours of irradiation. Known samples containing
10 milligrams of iodine-127 and National Bureau of Standards iodine-129
standard will be included for calibration purposes and cobalt-aluminum flux
wires will monitor total exposures for each irradiation. Each irradiation
capsule will hold five quartz vials. A period of 12 hours is allowed for
decay after irradiation. The ampoules are opened, water and 10 milligrams
of iodine carrier are added; the solution is acidified and sodium nitrite
added to release iodine which is extracted into toluene. The organic phase
is scrubbed with 0.01M nitric acid to remove activated bromine, sodium, and
other impurities. The iodine is stripped into an ammonium sulfite solution.
The iodide is precipitated as palladium iodide and filtered onto a paper
disk for counting on a germanium (lithium) detector. The iodine-127 is
calulated from the number of microcuries of iodine-126 present and the
iodine-129 is calculated from the iodine-130 present after correction for
in-pile and out-of-pile decay. Chemical recovery is calculated from iodine-
131 recovery. Calibration is by known iodine-127 and iodine-129 samples.
Blanks on the iodine-131 are run to establish that iodine-131 is fresh and
the iodine-129 blank is low. One day is required to solubilize samples and
15
-------
APPENDIX A. (continued)
1 day is required to purify them. Irradiation and cooling is performed at
night. The third day is spent purifying the irradiated samples and counting
them. A maximum of 2 runs of five samples can be made in a 5-day week.
APPENDIX B. TECHNICAL APPROACH: NEUTRON ACTIVATION OF THYROID SAMPLES AND
IODINE-129 ANALYSIS BY APPLIED PHYSICAL TECHNOLOGY (APT),
SMYRNA, GEORGIA
The basic task will be to provide iodine-127 and iodine-129 analyses on
40 to 60 samples of thyroid tissue supplied by the U.S. Environmental
Protection Agency. Samples should be in the range of 1 to 30 grams (wet)
and shipped in paraformaldehyde. Analyses will be reported as: micrograms
iodine-127 per gram tissue, picocuries iodine-129 per gram tissue, micrograms
iodine-129 per gram iodine-127, and picocuries iodine-129 per gram iodine-127.
Neutron activation analysis of thyroid tissue for iodine-129 requires
chemical separation of the iodine prior to irradiation to reduce interference
from other reactions. The iodine-129 is determined by the neutron gamma
reaction iodine-129 (n,y) iodine-130; the iodine-130 decays by beta emission
with a 12.4-hour half-life. The iodine-127 is determined by the neutron
gamma reaction iodine-127 (n,y) iodine-128, where the iodine-128 decays by
beta emission with a 25-minute half-life. Primary interfering reactions are:
(1) 1-127 (n,y) 1-128 (n,y) 1-129 (n,y) 1-130
(2) U-235 (n,f) 1-131
(3) Cl-37 (n,y) Cl-38
(4) 1-127 (n,2n) 1-126
(5) Br-81 (n,y) Br-82
Pre-irradiation chemical separation greatly reduces the interference
from reactions (2), (3), and (5). Interferences from reaction (4) can be
eliminated by using a well moderated neutron flux for irradiation such as a
heavy water reactor where the thermal neutron flux is high and the ratio of
thermal neutrons to fast reactions is also high. The irradiation of chemical
blanks is used to assess the interference of reagent contamination and
interference from reaction (1).
The analytical method used by APT is an adaptation of a method developed
by P. Magno, T. Reavey, and J. Apidianakis of the U.S. Environmental Protec-
tion Agency. The sample of thyroid tissue is fused with sodium hydroxide and
iodine-131 tracer for chemical yield determination. A series of solvent
extractions is used to chemically separate the iodine from other interfering
elements present in the original sample. The product of the solvent extrac-
tions is an ammonium sulfite solution containing the iodine for neutron
activation analysis. Iodine solutions in ammonium sulfite can be irradiated
in polyethylene containers without significant adsorption on the container
walls. The iodine solution is irradiated in a thermal neutron flux of about
•I Q
1013 neutrons per square centimeter per second for about 14 hours. Following
16
-------
APPENDIX B. (continued)
irradiation more solvent extractions further decontaminate the iodine. Final-
ly, the iodine is precipitated as palladium iodide for counting. The samples
are first counted as soon as possible after irradiation for the 25-minute
half-life iodine-128. After several hours decay, the samples are counted
again for iodine-130 and iodine-131. Comparison with a National Bureau of
Standards iodine-129 standard and a known quantity of iodine-127 and iodine-
131 carrier irradiated simultaneously with the samples permits a determination
of the iodine-129 and iodine-127' content of the original thyroid sample.
The sensitivity of this procedure has been determined as 2 x 10~9 micro-
curies iodine-129. For samples of 1 to 30 grams, the sensitivity is 2 x 10~9
microcuries iodine-129 per gram of tissue and 7 * 10"11 microcuries iodine-129
per gram of tissue, respectively. These limits are in compliance with the
requested sensitivity of 1 x io~8 microcuries iodine-129 per gram of tissue.
Due to the lengthy pre-irradiation and post-irradiation chemical proce-
dures, the relatively short half-life of the iodine-130 (12.4 hours), and the
long counting time required, the maximum number of samples that can be effec-
tively analyzed with the required sensitivity is limited. Samples submitted
in groups of 20 will require 45 days for analysis and the report can be for-
warded in 60 days from receipt of samples. Data for any given sample can be
provided on request within approximately 2 weeks after the sample arrives at
APT.
*U. S. GOVERNMENT PRINTING OFFICE: 1977-784-817
17
-------
TECHNICAL REPORT DATA
(Please read Instructions on the reverse before completing)
1. REPORT NO.
EPA-600/3-77-Q67
2.
3. RECIPIENT'S ACCESSION"NO.
4. TITLE AND SUBTITLE
129I IN ANIMAL THYROIDS FROM NEVADA AND OTHER WESTERN
STATES
5. REPORT DATE
June 1977
6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
D. D. Smith
8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
Environmental Monitoring and Support Laboratory
Office of Research and Development
U.S. Environmental Protection Agency
Las Vegas, Nevada 89114
10. PROGRAM ELEMENT NO.
1FA083
11. CONTRACT/GRANT NO.
12. SPONSORING AGENCY NAME AND ADDRESS
U.S. Environmental Protection Agency-Las Vegas, NV
Office of Research and Development
Environmental Monitoring and Support Laboratory
Las Vegas, Nevada 89114
13. TYPE OF REPORT AND PERIOD COVERED
Final project report
14. SPONSORING AGENCY CODE
EPA/600/07
15. SUPPLEMENTARY NOTES
16. ABSTRACT
The data from over 80 thyroids collected during 1973, 1974, and 1975 from animals
residing on the Nevada Test Site indicate that iodine-129 levels in these thyroids are
near background levels. However, the median levels in the thyroids of animals living
jn the Nevada Test Site are slightly elevated from those found in northern Nevada, but
ire similar to those found near Denver, Colorado, and Rawlins, Wyoming. Statistical
malyses of the iodine-129/iodine-127 ratios in cattle thyroids suggest that three
jopulations were sampled. These populations are: (1) northern Nevada cattle which
were considered as a baseline population, (2) corralled Nevada Test Site cattle with
intermediate ratios, and (3) free-grazing cattle from Nevada Test Site and Rocky Flats,
olorado, which had the highest ratios reported.
17.
KEY WORDS AND DOCUMENT ANALYSIS
DESCRIPTORS
b.IDENTIFIERS/OPEN ENDED TERMS
COSATl Field/Group
animals
cattle
iodine isotopes
thyroid gland
Nevada Test Site
I-129/I-127 ratios
western States
02 E
06 C, P
07 B
13. DISTRIBUTION STATEMENT
RELEASE TO PUBLIC
19. SECURITY CLASS (This Report)
UNCLASSIFIED
21. NO. OF PAGES
24
20. SECURITY CLASS (Thispage)
UNCLASSIFIED
22. PRICE
EPA Form 2220-1 (9-73)
------- |