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Slide 1 Plutonium Exposure in Perspective: A Dose of Reality Anthony C. James, PhD, CRadP Director, U.S. Transuranium & Uranium Registries Research Professor,

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Presentation on theme: "Slide 1 Plutonium Exposure in Perspective: A Dose of Reality Anthony C. James, PhD, CRadP Director, U.S. Transuranium & Uranium Registries Research Professor,"— Presentation transcript:

1 Slide 1 Plutonium Exposure in Perspective: A Dose of Reality Anthony C. James, PhD, CRadP Director, U.S. Transuranium & Uranium Registries Research Professor, College of Pharmacy 1845 Terminal Drive, Suite 201 Richland, WA Joint Meeting of the Hanford Advisory Board’s (HAB) River & Plateau Committee (RAP) and Health, Safety & Environmental Protection Committee (HSEP) Richland, WA, January 8 th, 2009 “Learning from Plutonium and Uranium Workers”

2 Slide 2 Why were extraordinary measures taken to protect workers on Manhattan Project (and in subsequent U.S. weapons production facilities) from intakes of plutonium? Why did the U.S. Atomic Energy Commission set up the “U.S. Plutonium Registry” (in 1968)? - Current status and functions of the U.S. Transuranium and Uranium Registries (USTUR). What are USTUR’s pathological (autopsy) findings in U.S. plutonium workers? How do we determine tissue doses from internally incorporated transuranic radionuclides? - “Causation” calculations (EEOICPA). How do “plutonium” doses compare with normal “background” exposure of the U.S. population to external radiation and internally incorporated radionuclides? Conclusions about plutonium “toxicity” (hazard) in the environment. This Presentation RAP/HSEP Joint Committee Meeting, Jan 8 th, James

3 Slide 3 USTUR: Learning from Plutonium and Uranium Workers Why Handling Plutonium Was Expected to be Hazardous! Radium dial painters (Peru, Illinois) – completed dials are visible beside each painter, and painting materials are ready on the desks. From: Rowland, R. E. “Radium in Humans: A Review of U.S. Studies,” ANL/ER-3 (1994). 1920’s tragic experience of bone necrosis and osteogenic sarcoma in young women painting radium-luminized instrument/watch dials.

4 Slide 4 USTUR: Learning from Plutonium and Uranium Workers Radium Workers at Deadly Task! From: Toohey, R. E. Available at

5 Slide 5 USTUR: Learning from Plutonium and Uranium Workers Easy (Direct) Measurement of Radium “Body Burden” Inside the whole-body counter in Argonne’s Center for Human Radiobiology, a patient is ready for a measurement of gamma rays emitted from her body. From: Rowland, R. E. “Radium in Humans: A Review of U.S. Studies,” ANL/ER-3 (1994).

6 Slide 6 USTUR: Learning from Plutonium and Uranium Workers Decay Scheme of (Natural) 238 U That Includes 226 Ra and the 222 Rn (Radon Gas) Decay Chain

7 Slide 7 “Radium in Humans: A Review of Human Studies”, R.E. Rowland ANL/ER-3 Bone Sarcoma Death-Rate in Radium Dial Painters vs. 226 Ra Intake

8 Slide 8 Bone Tumor Incidence Ra intake, µ CiCasesBone tumors More than Less than µCi = 3.7 MBq (3.7 Million Bq)! “Radium in Humans: A Review of Human Studies”, R.E. Rowland ANL/ER-3

9 Slide 9 A Simple Safety Standard! Don’t eat the paint Brush-tipping was forbidden as an unsafe labor practice by the U. S. Department of Labor in 1929 No dial workers from the 1930’s on had significant intakes of radium, but were followed up because of external gamma exposure Toohey, R. E. Available at

10 Slide 10 Radium Standard No health effects noted in radium DPs with retained Ra-226 < 1.0 µCi Throw in a safety factor of 10 MPBB for Ra-226 = 0.1 µCi Toohey, R. E. Available at

11 Slide 11 U.S. Plutonium Standard Total alpha energy per decay of parent:  Ra-226 = 12 MeV  Pu-239 = 5 MeV about a factor of 2 All Pu alpha energy deposited on bone surface, most Ra energy deposited in bone volume, about a factor of nCi x 2/5 = 40 nCi Toohey, R. E. Available at

12 Slide 12 USTUR: Learning from Plutonium and Uranium Workers U.S. Plutonium Registry: The USAEC Vision

13 Slide 13 USTUR: Learning from Plutonium and Uranium Workers The US Transuranium Registry (USTR)

14 Slide 14 USTUR: Learning from Plutonium and Uranium Workers The U.S. Transuranium & Uranium Registries – 2009

15 Slide 15 USTUR Registrant Status USTUR: Learning from Plutonium and Uranium Workers As of September 30 th, 2008 Total Active (Living) and Deceased Registrants: 423 Living Registrants: 95 Potential Partial-body Donors: 74 Potential Whole-body Donors: 14 Special Studies: 7 Deceased Registrants: 328 Partial-body Donations: 288 Whole-body Donations: 35 Special Studies: 5 Inactive Registrants: 447 Total Number of Registrants: 870

16 Slide 16 USTUR: Learning from Plutonium and Uranium Workers The Registries: Historical Profile of Partial Body Donations (Routine Autopsy Cases) (As of September 30 th, 2008)

17 Slide 17 USTUR: Learning from Plutonium and Uranium Workers USTUR: Historical Profile of Whole Body Donations (As of September 30 th, 2008)

18 Slide 18 USTUR: Learning from Plutonium and Uranium Workers Year of Intake for Whole Body Donors (As of September 30 th, 2008)

19 Slide 19 USTUR: Learning from Plutonium and Uranium Workers 2008 Whole-Body Donations January: 87-y-old 239 Pu-contaminated puncture wound(s) (Hanford – 1960s). March: 95-y-old 239 PuO 2 acute inhalation (Rocky Flats – 1965 Pu fire – high intake). March: 72-y-old 241 AmO 2 chronic inhalation (U.S. Radium Corporation – 1960s – very high intake – heavily chelated). September: 83-y-old U 3 O 8 -fume acute inhalation (Hanford – 1948 – up to 300 μg-U/d in urine).

20 Slide 20 USTUR: Learning from Plutonium and Uranium Workers Current Active Registrants: Potential Whole-Body Donors Total Registrants (WB) = 14: Average age 78 y (± 14 y) [Excluding # Average age 81 y (± 8 y)] Case NoBirth DateAge, ySite LOS HAN ROC HAN CHI ROC LOS LOS ROC ROC HAN MND ROC HAN (As of September 30 th, 2008)

21 Slide 21 Self-selected for relatively “high” (recorded) intakes of transuranium elements – primarily 239 Pu/ 238 Pu/ 241 Am. Additional exposure to external radiation (  /n). In majority of cases, also additional exposure to industrial toxic materials - Beryllium (Be), asbestos, toxic chemicals, organic solvents, benzene/toluene. Any pathological findings are SUMMED effects of “natural” disease incidence (including “normal” incidence of malignant cancer in matched, non-exposed population) and ALL occupational exposure factors. Some self-selection for existing cancer (Rocky Flats Plant). Exposure Characteristics of USTUR Registrants RAP/HSEP Joint Committee Meeting, Jan 8 th, James

22 Slide 22 USTUR: Learning from Plutonium and Uranium Workers Pathology Database – Case Report

23 Slide 23 USTUR: Learning from Plutonium and Uranium Workers USTUR Internal Database – Pathology

24 Slide 24 USTUR: Learning from Plutonium and Uranium Workers Smoking Habits of Deceased USTUR Registrants Source: Fallahian,N. A. “Study of the Association Between Exposure to Transuranic Radionuclides and Cancer Death,” PhD Dissertation, Idaho State University, 2008

25 Slide 25 USTUR: Learning from Plutonium and Uranium Workers Distribution of Age at Death for USTUR Registrants Source: Fallahian,N. A. “Study of the Association Between Exposure to Transuranic Radionuclides and Cancer Death,” PhD Dissertation, Idaho State University, 2008

26 Slide 26 USTUR: Learning from Plutonium and Uranium Workers Estimated Distribution of Total Effective Dose Equivalent for Deceased USTUR Registrants Source: Fallahian,N. A. “Study of the Association Between Exposure to Transuranic Radionuclides and Cancer Death,” PhD Dissertation, Idaho State University, 2008

27 Slide 27 USTUR: Learning from Plutonium and Uranium Workers Recorded External Deep Dose Equivalent for Deceased USTUR Registrants Source: Fallahian,N. A. “Study of the Association Between Exposure to Transuranic Radionuclides and Cancer Death,” PhD Dissertation, Idaho State University, 2008

28 Slide 28 Malignant Neoplasms as Primary Cause of Death in USTUR Registrants (with Exposure Co-Factors): 1. ICD-10 Codes C02.9 – C20 USTUR: Learning from Plutonium and Uranium Workers Case No. SourceICD-10SiteFraction (85%) Smoker BeAsbestosToxic_ChemSolvents Benzene/ Toluene SEER All NeoplasmsCount =111/ % 0047DC02.9Tongue AC12Hypopharynx2.7%YNYYY-1.9% 0640AC14.0Pharynx YNNNN- 0055DC15.9Esophagus DC15.9Esophagus3.6% % 0206AC15.9Esophagus AC15.9Esophagus YYYYYY 0015DC16.9Stomach Y--Y-Y 0030DC16.9Stomach3.6%-NNNNN3.0% 0142DC16.9Stomach AC16.9Stomach YY-YY- 0644AC18.5ColonYNYYYN 0183DC18.9Colon-NNNNN 0458AC18.9Colon4.5%YYYYYY 0503DC18.9ColonN % 0325AC18.9ColonYYY-Y- 0095DC19Rectum DC19Rectum2.7% DC20Rectum YNNNNN SEER: Surveillance, Epidemiology & End Results - /http://seer.cancer.gov /

29 Slide 29 Malignant Neoplasms as Primary Cause of Death in USTUR Registrants (with Exposure Co-Factors): 2. ICD-10 Codes C22 – C25.9 USTUR: Learning from Plutonium and Uranium Workers Case No. SourceICD-10SiteFractionSmokerBeAsbestosToxic_ChemSolvents Benzene/ Toluene SEER DC22.0LiverNY AC22.1LiverYNNNYN 0147DC22.9Liver5.4%YNNNNN1.9% 0371AC22.9LiverYN-YY- 0446AC22.9LiverYYYNYY 1054DC22.9Liver DC24.1Gallbladder0.9% % 0099DC25.0Pancreas AC25.0PancreasYNNNNN 0461AC25.2Pancreas4.5%YNNNNN4.9% 0341AC25.9PancreasNYNNNN 0846DC25.9PancreasNY--NY

30 Slide 30 Malignant Neoplasms as Primary Cause of Death in USTUR Registrants (with Exposure Co-Factors): 3. ICD-10 Codes C34.1 – C41.4 USTUR: Learning from Plutonium and Uranium Workers Case No.SourceICD-10SiteFractionSmokerBeAsbestosToxic_ChemSolventsBenzene/TolueneSEER AC34.1Lung YNNYYN 0255AC34.1Lung YNYYYN 0005AC34.9Lung Y AC34.9Lung YNNNNN 0011DC34.9Lung Y DC34.9Lung Y AC34.9Lung NNNNNN 0064AC34.9Lung YNNYNN 0081DC34.9Lung Y DC34.9Lung DC34.9Lung AC34.9Lung YNNNNN 0103DC34.9Lung AC34.9Lung YNNN DC34.9Lung Y DC34.9Lung DC34.9Lung Y DC34.9Lung DC34.9Lung YN-YY- 0203DC34.9Lung31.5% % 0205AC34.9Lung NC34.9Lung YNNNNN 0226DC34.9Lung YNYYN- 0232AC34.9Lung AC34.9Lung NNYYN- 0252DC34.9Lung YN-YY- 0334AC34.9Lung YYYYYN 0375AC34.9Lung Y AC34.9Lung YNNNNN 0720AC34.9Lung YYNNNN 0727AC34.9Lung YY-YY- 0779DC34.9Lung Y---N- 0841AC34.9Lung YNY-Y- 1036AC34.9Lung Y--Y AC34.9Lung Y-Y-YY 1059AC40.2Bone1.8% % 0769AC41.4Bone------

31 Slide 31 Malignant Neoplasms as Primary Cause of Death in USTUR Registrants (with Exposure Co-Factors): 4. ICD-10 Codes C43.6 – C63.9 USTUR: Learning from Plutonium and Uranium Workers Case No.SourceICD-10SiteFractionSmokerBeAsbestosToxic_ChemSolventsBenzene/TolueneSEER AC43.6Skin (Melanoma) DC43.9Skin (Melanoma)3.6% % 0102DC43.9Skin (Melanoma) YNYYN- 0245AC43.9Skin (Melanoma) YNYYN- 0084DC45.0MesotheliomaN DC45.0MesotheliomaYYYYY- 0648AC45.0Mesothelioma5.4%NYYYY DC45.0Mesothelioma-N-YY- 0677AC45.7MesotheliomaN--Y DC45.9MesotheliomaNNNYNN 0020DC50.9Breast0.9%Y DC55Uterus0.9%YNNNNN- 0022DC61ProstateYN-YN- 0058DC61Prostate DC61ProstateY DC61Prostate6.3% % 0269AC61ProstateYNNNNN 0425AC61ProstateNY AC61ProstateYYYYYY 1030AC63.9Penis0.9%YNN-NN0.0%

32 Slide 32 Malignant Neoplasms as Primary Cause of Death in USTUR Registrants (with Exposure Co-Factors): 5. ICD-10 Codes C64 – D46.9 USTUR: Learning from Plutonium and Uranium Workers Case No. SourceICD-10SiteFractionSmokerBeAsbestosToxic_ChemSolvents Benzene/ Toluene SEER DC64Kidney DC64Kidney2.7% % 1007AC64KidneyY--Y DC67.9Bladder Y AC67.9Bladder2.7% % 0992AC67.9Bladder YYYY DC71.9Brain-NNNNN 0049DC71.9Brain DC71.9Brain DC71.9Brain6.3%Y % 0216DC71.9Brain DC71.9Brain AC72.4Nervous System DC78.5Lung/Colon (Met) YN-YY DC79.0Kidney (Met) DC79.0Kidney (Met)YYNNYN 0032AC85.0Lymphosarcoma0.9%-NNNNN- 1044DC85.9NH Lymphoma0.9%YY-YN-3.4% 0794AC90.0Multiple Myeloma0.9%YNNNY-1.7% 0035DC91.0AL Leukemia0.9% % 0194DC92.1CM Leukemia0.9% % 1001DC95.0AU Leukemia Thorotrast Injection (Female) 0274AD45Polycythaemia vera0.9%Y--Y AD46.9 Myelodysplastic syndrome 0.9%YNNN---

33 Slide 33 USTUR: Learning from Plutonium and Uranium Workers Summary of Preliminary Findings on USTUR Registrants (Through 2008) No association found between exposure to transuranic radionuclides and malignant cancer as a primary (or secondary) cause of death (α = 0.05). Statistically significant associations found between cause of death due to any type of cancer and exposure to: - benzene or toluene (odds ratio = 5.71; 95% CI: 1.04 to 31.34) - smoking habit (odds ratio = 5.41; 95% CI: 1.42 to 20.67) - rate of cigarette smoking (odds ratio = 2.70; 95% CI: 1.37 to 5.30). Lung cancer deaths found to be related to exposure to: - chlorinated solvents (odds ratio = 10.85; 95% CI: 1.02 to ) - duration of exposure to these materials (odds ratio = 1.12; 95% CI: 1.01 to 1.24). Source: Fallahian,N. A. “Study of the Association Between Exposure to Transuranic Radionuclides and Cancer Death,” PhD Dissertation, Idaho State University, 2008

34 Slide 34 USTUR: Learning from Plutonium and Uranium Workers How Do We Determine Tissue Doses for Plutonium? – Example of USTUR Case 0262 Worked as engineer at Hanford ( ). Died 1990 – at age 71 y. Cause of death: - hepatocellular carcinoma with metastasis to diaphragm, lungs and liver (ICD-10 Code C22.0). At autopsy: - all major soft tissue organs harvested, including axillary lymph node (for radiochemistry and NHRTR sample storage); - Skin of both hands saved for histology/autoradiography; - Bones from half skeleton dissected out – for radiochemistry; - Contents of 238 Pu, Pu, 241 Am measured for all tissues/organs.

35 Slide 35 USTUR: Learning from Plutonium and Uranium Workers Health Physics/Incident Data for USTUR Case 0262 Two suspected Pu inhalation intakes (1956) – of nominally ‘fresh’ weapons grade material: - 1,834 days after starting Pu work, exposed to substantial airborne Pu concentration (no respirator); - 2 weeks later, both hands contaminated (  10,000 dpm Pu); - Inhalation intakes from both incidents indicated by measurable Pu α- activity in prompt urine sample – subsequent samples negative (i.e., < dpm per 24-h sample). Third Pu intake occurred about 500 d later – by puncture wound of left thumb (broken drill bit through glove) while working in glove box: - No general airborne release; - Initial count rate (α-probe) from contaminated wound surface  500 cpm.

36 Slide 36 USTUR: Learning from Plutonium and Uranium Workers “Biokinetic” Model for Wound/Inhalation Plutonium Uptake and Tissue Retention Source: James, A.C., et al. “USTUR Whole Body Case 0262: 33-y Follow-up of PuO2 in a Skin Wound and Associated Axillary Node.” Radiat. Prot. Dosim. 127: (2007)

37 Slide 37 USTUR: Learning from Plutonium and Uranium Workers Measured and “Modeled” Excretion of 239 Pu in Urine for Case 0262 Source: James, A.C., et al. “USTUR Whole Body Case 0262: 33-y Follow-up of PuO2 in a Skin Wound and Associated Axillary Node.” Radiat. Prot. Dosim. 127: (2007)

38 Slide 38 USTUR: Learning from Plutonium and Uranium Workers Measured and “Modeled” 239 Pu Content of Tissues (At Autopsy) for Case 0262 Source: James, A.C., et al. “USTUR Whole Body Case 0262: 33-y Follow-up of PuO 2 in a Skin Wound and Associated Axillary Node.” Radiat. Prot. Dosim. 127: (2007)

39 Slide 39 USTUR: Learning from Plutonium and Uranium Workers Use “Modeled” Biokinetics (Intake and Absorption Behavior) to Calculate Equivalent Dose Received by Liver in Each Year (After Intakes)

40 Slide 40 USTUR: Learning from Plutonium and Uranium Workers NIOSH-IREP “Probability of Causation” Software - on the Web

41 Slide 41 USTUR: Learning from Plutonium and Uranium Workers Run Calculated Annual Equivalent Doses Through “Interactive RadioEpidemiological Program” (NIOSH-IREP) – as Done for EEOICPA

42 Slide 42 USTUR: Learning from Plutonium and Uranium Workers NIOSH-IREP “Probability of Causation” Results – Case 0262 Legal Standard EEOICPA Standard

43 Slide 43 USTUR: Learning from Plutonium and Uranium Workers Percent Contribution of Various Sources of Exposure to the Average Annual Effective Dose to Each U.S. Person for 2006 (6.2 mSv) Source: NCRP Report No. 160, "Ionizing Radiation Exposure of the Population of the United States" can be found at

44 Slide 44 USTUR: Learning from Plutonium and Uranium Workers Average Annual Equivalent Doses to U.S. Adults From Natural Radionuclides of the Uranium and Thorium Series Incorporated in the Body Source: NCRP Report No. 160, "Ionizing Radiation Exposure of the Population of the United States" can be found at H T (µSv) wTwT w T H T (µSv) Tissue, T 238/234 U 230 Th 226 Ra 210 Pb/ 210 Po 232 Th 228/224 RaSum Bone surfaces Lung a Kidney Liver Other Bone marrow E126.6 a Excluding 222 Rn, 220 Rn and their short-lived decay products.

45 Slide 45 USTUR: Learning from Plutonium and Uranium Workers Frequency Distribution of “Natural Background” Annual Effective Dose (mSv) for Members of the U.S. Population Source: NCRP Report No. 160, "Ionizing Radiation Exposure of the Population of the United States" can be found at

46 Slide 46 USTUR: Learning from Plutonium and Uranium Workers Frequency Distribution of “Natural Background” Annual Effective Dose (mSv) for Members of the U.S. Population – c.f. USTUR Registrants Approximate range of “occupational” dose Average  10 mSv/y (< 0.1 to  200 mSv/y)

47 Slide 47 Plutonium Already in the Environment Source: Taylor, R. N., et al. “Plutonium Isotope Ratio Analysis at Femtogram to Nanogram Levels by Multicollector ICP-MS.” J. Anal. At. Spectrum 16, (2001)

48 Slide 48 Isotopic Signature in Environmental Plutonium Source: Ketterer, M. E. “ICP-MS Studies of Plutonium in the Environment.” In: Application of ICP & ICP- MS Techniques for Today’s Spectroscopist.” (November, 2005)

49 Slide 49 Isotopic Signature in USTUR Tissue Samples USTUR: Learning from Plutonium and Uranium Workers

50 Slide 50 What About “Deadly Plutonium” In a follow-up of several dozen Los Alamos workers with plutonium intakes (mostly via contaminated wounds), one osteosarcoma of the pelvis was observed. However, if plutonium had been used instead of radium in the dial-painting industry, no cancers would have been observed, due to extremely low absorption (0.001%) from the gastrointestinal tract. Toohey, R. E. Available at

51 Slide 51 As for all other internally-incorporated radionuclides, the health effects of plutonium depend purely on the amount of plutonium in the tissues – i.e., on the amount of radiation DOSE delivered to the tissues. Very small amounts of plutonium – as already present in everyone (worldwide) have NEGLIGIBLE TO ZERO effect on human health. It is hard to imagine any (realistic) exposure scenario that would lead to SIGNIFICANT intake of plutonium by members of the public from WELL MANAGED operations at the Hanford Site (or other clean-up sites). Any SIGNIFICANT HEALTH HAZARD from plutonium would fall on WORKERS involved in HANDLING concentrated sources of plutonium. It is imperative that CAREFUL AND COMPREHENSIVE MANAGEMENT of all plutonium clean-up work be maintained – to PROTECT WORKERS. PLUTONIUM IS NOT THE MOST TOXIC SUBSTANCE KNOWN TO MAN! DON’T IGNORE “INDUSTRIAL HYGIENE” – CHEMICAL TOXINS! They are likely to pose a bigger “real” risk. Conclusions – Plutonium “Toxicity” RAP/HSEP Joint Committee Meeting, Jan 8 th, James

52 Slide 52 RAP/HSEP Joint Committee Meeting, Jan 8 th, James Disclaimer: “This presentation was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof.”


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