Plutonium Exposure in Perspective: A Dose of Reality

1
Plutonium Exposure in Perspective A Dose of
Reality
Joint Meeting of the Hanford Advisory Boards
(HAB) River Plateau Committee (RAP) and Health,
Safety Environmental Protection Committee
(HSEP) Richland, WA, January 8th, 2009

• 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_at_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 USTURs 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.

3
Why Handling Plutonium Was Expected to be
Hazardous!
1920s 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).
4
Radium Workers at Deadly Task!
From Toohey, R. E. Available at
http//www.ustur.wsu.edu/Radium/files/SagaOfRaDPs.
pdf
5
Easy (Direct) Measurement of Radium Body Burden
Inside the whole-body counter in Argonnes 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
Decay Scheme of (Natural) 238U That Includes
226Ra and the 222Rn (Radon Gas) Decay Chain
7
Bone Sarcoma Death-Rate in Radium Dial Painters
vs. 226Ra Intake
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
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A Simple Safety Standard!

• Dont 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 1930s on had
  significant intakes of radium, but were followed
  up because of external gamma exposure

Toohey, R. E. Available at http//www.ustur.wsu.ed
u/Radium/files/SagaOfRaDPs.pdf
10
Radium Standard

• No health effects noted in radium DPs with
  retained Ra-226 lt 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.ed
u/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.ed
u/Radium/files/SagaOfRaDPs.pdf
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U.S. Plutonium Registry The USAEC Vision
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The US Transuranium Registry (USTR)
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The U.S. Transuranium Uranium Registries 2009
15
USTUR Registrant Status
16
The Registries Historical Profile of Partial
Body Donations(Routine Autopsy Cases)
(As of September 30th, 2008)
17
USTUR Historical Profile of Whole Body Donations
(As of September 30th, 2008)
18
Year of Intake for Whole Body Donors
(As of September 30th, 2008)
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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).

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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)
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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).

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Pathology Database Case Report
USTUR Learning from Plutonium and Uranium Workers
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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/

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Malignant Neoplasms as Primary Cause of Death in
USTUR Registrants (with Exposure Co-Factors) 2.
ICD-10 Codes C22 C25.9
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Malignant Neoplasms as Primary Cause of Death in
USTUR Registrants (with Exposure Co-Factors) 3.
ICD-10 Codes C34.1 C41.4
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Malignant Neoplasms as Primary Cause of Death in
USTUR Registrants (with Exposure Co-Factors) 4.
ICD-10 Codes C43.6 C63.9
32
Malignant Neoplasms as Primary Cause of Death in
USTUR Registrants (with Exposure Co-Factors) 5.
ICD-10 Codes C64 D46.9
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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 (a
  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
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, 239240Pu, 241Am measured
  for all tissues/organs.

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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 a-activity in prompt
  urine sample subsequent samples negative (i.e.,
  lt 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 (a-probe) from contaminated
  wound surface ?500 cpm.

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)
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)
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)
39
Use Modeled Biokinetics (Intake and Absorption
Behavior) to Calculate Equivalent Dose Received
by Liver in Each Year (After Intakes)
40
NIOSH-IREP Probability of Causation Software -
on the Web
41
Run Calculated Annual Equivalent Doses Through
Interactive RadioEpidemiological Program
(NIOSH-IREP) as Done for EEOICPA
42
NIOSH-IREP Probability of Causation Results
Case 0262
Legal Standard
EEOICPA Standard
43
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/Ele
c_prepub_160.pdf.
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/Ele
c_prepub_160.pdf.
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/Ele
c_prepub_160.pdf.
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 (lt 0.1 to ? 200 mSv/y)
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 Todays
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, 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 http//www.ustur.wsu.ed
u/Radium/files/SagaOfRaDPs.pdf
51
Conclusions Plutonium Toxicity

• 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!
• DONT IGNORE INDUSTRIAL HYGIENE CHEMICAL
  TOXINS! They are likely to pose a bigger real
  risk.

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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
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The views and opinions of authors expressed
herein do not necessarily state or reflect those
of the United States Government or any agency
thereof.
Thank you for your attention!
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