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) ------- |