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  1. Joint Meeting of the Hanford Advisory Board’s (HAB) River & Plateau Committee (RAP) and Health, Safety & Environmental Protection Committee (HSEP) Richland, WA, January 8th, 2009 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 99354-4959 tjames@tricity.wsu.edu www.ustur.wsu.edu “Learning from Plutonium and Uranium Workers”

  2. This Presentation • 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. RAP/HSEP Joint Committee Meeting, Jan 8th, 2009 - James

  3. Why Handling Plutonium Was Expected to be Hazardous! 1920’s tragic experience of bone necrosis and osteogenic sarcoma in young women painting radium-luminized instrument/watch dials. 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). USTUR: Learning from Plutonium and Uranium Workers

  4. Radium Workers at Deadly Task! From: Toohey, R. E. Available at http://www.ustur.wsu.edu/Radium/files/SagaOfRaDPs.pdf USTUR: Learning from Plutonium and Uranium Workers

  5. 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). USTUR: Learning from Plutonium and Uranium Workers

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

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

  8. Bone Tumor Incidence Ra intake, µCi Cases Bone tumors More than 2500 16 4 1000 -- 2499 22 15 500 -- 999 18 8 250 -- 499 32 9 100 -- 249 27 2 Less than 100 644 0 100 µCi = 3.7 MBq (3.7 Million Bq)! “Radium in Humans: A Review of Human Studies”, R.E. Rowland ANL/ER-3

  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 http://www.ustur.wsu.edu/Radium/files/SagaOfRaDPs.pdf

  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 http://www.ustur.wsu.edu/Radium/files/SagaOfRaDPs.pdf

  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 5 • 100 nCi x 2/5 = 40 nCi Toohey, R. E. Available at http://www.ustur.wsu.edu/Radium/files/SagaOfRaDPs.pdf

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

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

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

  15. USTUR Registrant Status USTUR: Learning from Plutonium and Uranium Workers

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

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

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

  19. 2008 Whole-Body Donations • January: 87-y-old 239Pu-contaminated puncture wound(s) (Hanford – 1960s). • March: 95-y-old 239PuO2 acute inhalation (Rocky Flats – 1965 Pu fire – high intake). • March: 72-y-old 241AmO2 chronic inhalation (U.S. Radium Corporation – 1960s – very high intake – heavily chelated). • September: 83-y-old U3O8-fume acute inhalation (Hanford – 1948 – up to 300 μg-U/d in urine). USTUR: Learning from Plutonium and Uranium Workers

  20. Current Active Registrants: Potential Whole-Body Donors Total Registrants (WB) = 14: Average age 78 y (± 14 y) [Excluding #0263 - Average age 81 y (± 8 y)] (As of September 30th, 2008) USTUR: Learning from Plutonium and Uranium Workers

  21. Exposure Characteristics of USTUR Registrants • Self-selected for relatively “high” (recorded) intakes of transuranium elements – primarily 239Pu/238Pu/241Am. • 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). RAP/HSEP Joint Committee Meeting, Jan 8th, 2009 - James

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

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

  24. 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 USTUR: Learning from Plutonium and Uranium Workers

  25. 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 USTUR: Learning from Plutonium and Uranium Workers

  26. 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 USTUR: Learning from Plutonium and Uranium Workers

  27. 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 USTUR: Learning from Plutonium and Uranium Workers

  28. Malignant Neoplasms as Primary Cause of Death in USTUR Registrants (with Exposure Co-Factors): 1. ICD-10 Codes C02.9 – C20 • SEER: Surveillance, Epidemiology & End Results - http://seer.cancer.gov/ USTUR: Learning from Plutonium and Uranium Workers

  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

  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

  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

  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

  33. 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 115.16) • - 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 USTUR: Learning from Plutonium and Uranium Workers

  34. How Do We Determine Tissue Doses for Plutonium? – Example of USTUR Case 0262 • Worked as engineer at Hanford (1951-82). • 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 238Pu, 239+240Pu, 241Am measured for all tissues/organs. USTUR: Learning from Plutonium and Uranium Workers

  35. 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., < 0.025 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. USTUR: Learning from Plutonium and Uranium Workers

  36. “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: 114-119 (2007) USTUR: Learning from Plutonium and Uranium Workers

  37. Measured and “Modeled” Excretion of 239Pu 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: 114-119 (2007) USTUR: Learning from Plutonium and Uranium Workers

  38. Measured and “Modeled” 239Pu Content of Tissues (At Autopsy)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: 114-119 (2007) USTUR: Learning from Plutonium and Uranium Workers

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

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

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

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

  43. Percent Contribution of Various Sources of Exposure to the Average AnnualEffective 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 http://www.ncrponline.org/PDFs/Elec_prepub_160.pdf. USTUR: Learning from Plutonium and Uranium Workers

  44. Average Annual Equivalent Doses to U.S. Adults From Natural Radionuclides of the Uranium and Thorium Series Incorporated in the Body aExcluding 222Rn, 220Rn and their short-lived decay products. Source: NCRP Report No. 160, "Ionizing Radiation Exposure of the Population of the United States" can be found at http://www.ncrponline.org/PDFs/Elec_prepub_160.pdf. USTUR: Learning from Plutonium and Uranium Workers

  45. 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 http://www.ncrponline.org/PDFs/Elec_prepub_160.pdf. USTUR: Learning from Plutonium and Uranium Workers

  46. 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) USTUR: Learning from Plutonium and Uranium Workers

  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, 279-284 (2001)

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

  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, ifplutonium 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 http://www.ustur.wsu.edu/Radium/files/SagaOfRaDPs.pdf