Slide 1 Plutonium Exposure in Perspective: A Dose of Reality Anthony C. James, PhD, CRadP Director,...

Plutonium Exposure in Perspective: A Dose of Reality

Anthony C. James, PhD, CRadPDirector, 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

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

“Learning from Plutonium and Uranium Workers”

• 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 8th, 2009 - James

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.

Radium Workers at Deadly Task!

From: Toohey, R. E. Available at http://www.ustur.wsu.edu/Radium/files/SagaOfRaDPs.pdf

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).

Decay Scheme of (Natural) 238U That Includes 226Ra and the 222Rn (Radon Gas) Decay Chain

234mPa

214Po 218Po

214Pb210Pb

emission

4.47E9 y

24.1 d

1.17 m

2.46E5 y

1599 y

163.7 µs

5.01 d

stable

138.38 d

22.6 y

19.9 m

3.10 m

3.8235 d

7.54E4 y

Radon Decay Chain

Short-lived Progeny that contribute to

Potential Alpha Energy

“Radium in Humans: A Review of Human Studies”, R.E. Rowland ANL/ER-3

Bone Sarcoma Death-Rate in Radium Dial Painters vs. 226Ra Intake

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

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

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

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

U.S. Plutonium Registry: The USAEC Vision

The US Transuranium Registry (USTR)

The U.S. Transuranium & Uranium Registries – 2009

USTUR Registrant Status

As of September 30th, 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

The Registries: Historical Profile of Partial Body Donations(Routine Autopsy Cases)

(As of September 30th, 2008)

USTUR: Historical Profile of Whole Body Donations

Year of Intake for Whole Body Donors

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).

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)]

Case No Birth Date Age, y Site

0249 1918 90 LOS

0740 1918 90 HAN

0456 1921 87 ROC

0272 1922 86 HAN

0757 1922 86 CHI

0409 1924 84 ROC

0634 1924 84 LOS

0631 1925 82 LOS

0816 1926 81 ROC

0433 1928 80 ROC

0674 1934 73 HAN

0842 1936 71 MND

0266 1943 65 ROC

0263 1972 36 HAN

• 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).

Exposure Characteristics of USTUR Registrants

Pathology Database – Case Report

USTUR Internal Database – Pathology

Cigar2%

Pipe3%

Cigarette & cigar2%

Cigarette & pipe5%

Cigarette81%

All three types7%

Smoking Habits of Deceased USTUR Registrants

Non-smoking 24%

Smoking 76%

Source: Fallahian,N. A. “Study of the Association Between Exposure to Transuranic Radionuclides and Cancer Death,” PhD Dissertation, Idaho State University, 2008

Distribution of Age at Death for USTUR Registrants

20-30 30-40 40-50 50-60 60-70 70-80 80-90 90-100

Age at death (year)

Estimated Distribution of Total Effective Dose Equivalent for Deceased USTUR Registrants

0 1 14

4 2 00

0.1 1 10 100 1000 10000 100000

T ota l effec tive dose equiva lent (mS v)

Recorded External Deep Dose Equivalent for Deceased USTUR Registrants

2 2 28

0.1 1 10 100 1000 10000

E x terna l deep dose equiva lent (mS v)

Malignant Neoplasms as Primary Cause of Death in USTUR Registrants(with Exposure Co-Factors): 1. ICD-10 Codes C02.9 – C20

Case No. Source ICD-10 Site Fraction (85%)

Smoker Be Asbestos Toxic_Chem Solvents Benzene/Toluene

SEER 1975-2005

All Neoplasms Count = 111/317 35.0%0047 D C02.9 Tongue - - - - - - 0094 A C12 Hypopharynx 2.7% Y N Y Y Y - 1.9%0640 A C14.0 Pharynx Y N N N N - 0055 D C15.9 Esophagus - - - - - -0096 D C15.9 Esophagus 3.6% - - - - - - 2.5%0206 A C15.9 Esophagus - - - - - -0817 A C15.9 Esophagus Y Y Y Y Y Y0015 D C16.9 Stomach Y - - Y - Y 0030 D C16.9 Stomach 3.6% - N N N N N 3.0%0142 D C16.9 Stomach - - - - - - 0650 A C16.9 Stomach Y Y - Y Y - 0644 A C18.5 Colon Y N Y Y Y N 0183 D C18.9 Colon - N N N N N 0458 A C18.9 Colon 4.5% Y Y Y Y Y Y 0503 D C18.9 Colon N - - - - - 11.5%0325 A C18.9 Colon Y Y Y - Y -0095 D C19 Rectum - - - - - - 0260 D C19 Rectum 2.7% - - - - - - 0101 D C20 Rectum Y N N N N N

•SEER: Surveillance, Epidemiology & End Results - http://seer.cancer.gov/

Malignant Neoplasms as Primary Cause of Death in USTUR Registrants(with Exposure Co-Factors): 2. ICD-10 Codes C22 – C25.9

Case No. Source ICD-10 Site Fraction Smoker Be Asbestos Toxic_Chem Solvents Benzene/

TolueneSEER

1975-2005

0262 D C22.0 Liver N Y - - - -

0306 A C22.1 Liver Y N N N Y N

0147 D C22.9 Liver 5.4% Y N N N N N 1.9%

0371 A C22.9 Liver Y N - Y Y -

0446 A C22.9 Liver Y Y Y N Y Y

1054 D C22.9 Liver - - - - - -

0054 D C24.1 Gallbladder 0.9% - - - - - - 0.3%

0099 D C25.0 Pancreas - - - - -

0104 A C25.0 Pancreas Y N N N N N

0461 A C25.2 Pancreas 4.5% Y N N N N N 4.9%

0341 A C25.9 Pancreas N Y N N N N

0846 D C25.9 Pancreas N Y - - N Y

Malignant Neoplasms as Primary Cause of Death in USTUR Registrants(with Exposure Co-Factors): 3. ICD-10 Codes C34.1 – C41.4

Case No. Source ICD-10 Site Fraction Smoker Be Asbestos Toxic_Chem Solvents Benzene/Toluene SEER 1975-20050240 A C34.1 Lung Y N N Y Y N 0255 A C34.1 Lung Y N Y Y Y N 0005 A C34.9 Lung Y - - - - - 0008 A C34.9 Lung Y N N N N N 0011 D C34.9 Lung Y - - - - - 0038 D C34.9 Lung Y - - - - - 0063 A C34.9 Lung N N N N N N 0064 A C34.9 Lung Y N N Y N N 0081 D C34.9 Lung Y - - - - - 0083 D C34.9 Lung - - - - - - 0091 D C34.9 Lung - - - - - - 0100 A C34.9 Lung Y N N N N N 0103 D C34.9 Lung - - - - - - 0149 A C34.9 Lung Y N N N - - 0161 D C34.9 Lung Y - - - - - 0185 D C34.9 Lung - - - - - - 0187 D C34.9 Lung Y - - - - - 0188 D C34.9 Lung - - - - - - 0197 D C34.9 Lung Y N - Y Y - 0203 D C34.9 Lung 31.5% - - - - - - 32.1%0205 A C34.9 Lung - - - - - - 0213 N C34.9 Lung Y N N N N N 0226 D C34.9 Lung Y N Y Y N - 0232 A C34.9 Lung - - - - - - 0247 A C34.9 Lung N N Y Y N - 0252 D C34.9 Lung Y N - Y Y - 0334 A C34.9 Lung Y Y Y Y Y N 0375 A C34.9 Lung Y - - - - - 0669 A C34.9 Lung Y N N N N N 0720 A C34.9 Lung Y Y N N N N 0727 A C34.9 Lung Y Y - Y Y - 0779 D C34.9 Lung Y - - - N - 0841 A C34.9 Lung Y N Y - Y - 1036 A C34.9 Lung Y - - Y - - 1065 A C34.9 Lung Y - Y - Y Y 1059 A C40.2 Bone 1.8% - - - - - - 0.2%0769 A C41.4 Bone - - - - - -

Malignant Neoplasms as Primary Cause of Death in USTUR Registrants(with Exposure Co-Factors): 4. ICD-10 Codes C43.6 – C63.9

Case No. Source ICD-10 Site Fraction Smoker Be Asbestos Toxic_Chem Solvents Benzene/Toluene SEER 1975-2005

0158 A C43.6 Skin (Melanoma) - - - - - -

0041 D C43.9 Skin (Melanoma) 3.6% - - - - - - 1.3%

0102 D C43.9 Skin (Melanoma) Y N Y Y N -

0245 A C43.9 Skin (Melanoma) Y N Y Y N -

0084 D C45.0 Mesothelioma N - - - - -

0256 D C45.0 Mesothelioma Y Y Y Y Y -

0648 A C45.0 Mesothelioma 5.4% N Y Y Y Y - -

1040 D C45.0 Mesothelioma - N - Y Y -

0677 A C45.7 Mesothelioma N - - Y - -

0013 D C45.9 Mesothelioma N N N Y N N

0020 D C50.9 Breast 0.9% Y - - - - - -

0079 D C55 Uterus 0.9% Y N N N N N -

0022 D C61 Prostate Y N - Y N -

0058 D C61 Prostate - - - - - -

0189 D C61 Prostate Y - - - - -

0253 D C61 Prostate 6.3% - - - - - - 12.8%

0269 A C61 Prostate Y N N N N N

0425 A C61 Prostate N Y - - - -

0778 A C61 Prostate Y Y Y Y Y Y

1030 A C63.9 Penis 0.9% Y N N - N N 0.0%

Malignant Neoplasms as Primary Cause of Death in USTUR Registrants(with Exposure Co-Factors): 5. ICD-10 Codes C64 – D46.9

Case No. Source ICD-10 Site Fraction Smoker Be Asbestos Toxic_Chem Solvents Benzene/

TolueneSEER

1975-20050092 D C64 Kidney - - - - - -0199 D C64 Kidney 2.7% - - - - - - 2.3%1007 A C64 Kidney Y - - Y - -0028 D C67.9 Bladder Y - - - - - 0106 A C67.9 Bladder 2.7% - - - - - - 3.5%0992 A C67.9 Bladder Y Y Y Y - - 0027 D C71.9 Brain - N N N N N0049 D C71.9 Brain - - - - - -0085 D C71.9 Brain - - - - - -0146 D C71.9 Brain 6.3% Y - - - - - 1.8%0216 D C71.9 Brain - - - - - -0228 D C71.9 Brain - - - - - -0107 A C72.4 Nervous System - - - - - -0156 D C78.5 Lung/Colon (Met) Y N - Y Y - -0044 D C79.0 Kidney (Met) - - - - - -0445 D C79.0 Kidney (Met) Y Y N N Y N0032 A C85.0 Lymphosarcoma 0.9% - N N N N N -1044 D C85.9 NH Lymphoma 0.9% Y Y - Y N - 3.4%0794 A C90.0 Multiple Myeloma 0.9% Y N N N Y - 1.7%0035 D C91.0 AL Leukemia 0.9% - - - - - - 0.1%0194 D C92.1 CM Leukemia 0.9% - - - - - - 0.4%

1001 D C95.0 AU Leukemia Thorotrast Injection (Female)

0274 A D45 Polycythaemia vera 0.9% Y - - Y - - -

0397 A D46.9 Myelodysplastic syndrome 0.9% Y N N N - - -

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).

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.

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.

“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)

Measured and “Modeled” Excretion of 239Pu in Urine for Case 0262

Measured and “Modeled” 239Pu Content of Tissues (At Autopsy)for Case 0262

Use “Modeled” Biokinetics (Intake and Absorption Behavior) to Calculate Equivalent Dose Received by Liver in Each Year (After Intakes)

NIOSH-IREP “Probability of Causation” Software - on the Web

Run Calculated Annual Equivalent Doses Through “Interactive RadioEpidemiological Program” (NIOSH-IREP) – as Done for EEOICPA

NIOSH-IREP “Probability of Causation” Results – Case 0262

Legal Standard

EEOICPA Standard

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 http://www.ncrponline.org/PDFs/Elec_prepub_160.pdf.

Average Annual Equivalent Doses to U.S. Adults From Natural Radionuclides of the Uranium and Thorium Series Incorporated in the Body

HT (µSv)

(µSv)Tissue , T 238/234U 230Th 226Ra 210Pb/210Po 232Th 228/224Ra Sum

surfaces 8.48 3.23 107 250 0.59 53.2 423 0.01 4.2

Lunga 17.2 6.40 4.85 88.5 7.07 62.9 187 0.12 22.4

Kidney 7.73 4.08 4.85 242 1.40 9.44 269 0.0092 2.5

Liver 2.76 4.32 4.85 504 1.20 9.60 527 0.04 21.1

Other 1.45 0.84 4.87 59.1 0.75 1.98 69.0 0.70 48.3

marrow2.68 66.5 13.9 101 41.1 8.68 234 0.12 28.0

E 126.6aExcluding 222Rn, 220Rn and their short-lived decay products.

Frequency Distribution of “Natural Background” Annual Effective Dose (mSv) for Members of the U.S. Population

Ubiquitous Background Doses to the US Population (303,631,185 as of 2008 March 14)

5,000,000

10,000,000

15,000,000

20,000,000

25,000,000

30,000,000

35,000,000

0 2 4 6 8 10 12 14 16 18 20

E (mSv y-1

2.3 million > 20 mSv y–1

Average = 3.06 mSv y–1

Median = 1.99 mSv y–1

Frequency Distribution of “Natural Background” Annual Effective Dose (mSv) for Members of the U.S. Population – c.f. USTUR Registrants

Ubiquitous Background Doses to the US Population (303,631,185 as of 2008 March 14)

5,000,000

10,000,000

15,000,000

20,000,000

25,000,000

30,000,000

35,000,000

0 2 4 6 8 10 12 14 16 18 20

E (mSv y-1

2.3 million > 20 mSv y–1

Average = 3.06 mSv y–1

Median = 1.99 mSv y–1

Approximate range of “occupational” dose

Average 10 mSv/y (< 0.1 to 200 mSv/y)

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)

Isotopic Signature in Environmental Plutonium

1950 1955 1960 1965 1970 1975 1980 1985

Deposition Date

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)

Isotopic Signature in USTUR Tissue Samples

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.

• 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”

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.”

Slide 1 Plutonium Exposure in Perspective: A Dose of Reality Anthony C. James, PhD, CRadP Director,...

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