research seminar - washington state university€¦ · 1845 terminal drive, suite 201, richland, wa...
TRANSCRIPT
Radiochemical Analysis of Plutonium in Tissues from Former Nuclear Workers
Sergei Y. Tolmachev and George Tabatadze
United States Transuranium and Uranium Registries
College of Pharmacy, Washington State University
1845 Terminal Drive, Suite 201, Richland, WA 99354
www.ustur.wsu.edu
Research SeminarOregon State University, School of Nuclear Science and Engineering
November 27, 2017
“Learning from Plutonium and
Uranium Workers”
Outline
Research Seminar at Oregon State University, November 27, 2017
• U.S. Transuranium and Uranium Registries
• Radiochemistry at the USTUR
• Plutonium in human
U.S. Atomic Energy Commission Vision
• 1966 meeting “Plutonium Contamination in Man”
“to protect the interests of workers, employees, and the public
by …. the acquisition and provision of the latest and most
precise information about the effects of the transuranic
elements on man.”
Research Seminar at Oregon State University, November 27, 2017
National Plutonium Registry: Blue Ribbon Committee
Standing left to right: Carlos E. Newton, Jr., W. Daggett Norwood, H.D. Bruner, Philip A. Fuqua
Seated left to right: Thomas F. Mancuso, J.H. Sterner, Robley D. Evans, Herbert M. ParkerNot photographed: Clarence C. Lushbaugh, Lloyd M. Joshel
Research Seminar at Oregon State University, November 27, 2017
REGISTRIES MANAGEMENT ANALYTICAL SUPPORT
1968 National Plutonium Registry Rocky Flats Pacific Northwest
at Hanford Environmental Health Foundation Facility Laboratory
1970 United States Transuranium Registryat Hanford Environmental Health Foundation
1971 Los Alamos
National Laboratory
1978 United States Uranium Registryat Hanford Environmental Health Foundation
1987-90
1992 United States Transuranium and Uranium Registriesat College of Pharmacy, Washington State University
Genealogy of the USTUR
Research Seminar at Oregon State University, November 27, 2017
USTUR Mission
• Follow up occupationally exposed individuals
(nuclear workers) by studying the biokinetics
(uptake, translocation, retention, and excretion),
and dosimetry of actinides (uranium, plutonium,
americium)
• Refine internal radiation dose assessment
methods as the bases for reliable epidemiological
studies, risk projection, and credible standards for
radiological protection
• Assess adequacy of historical and current U.S.
regulatory controls and practices
Research Seminar at Oregon State University, November 27, 2017
USTUR Today
• Unique resource worldwide for the
comprehensive study of the biokinetics and
internal dosimetry of actinide elements in the
human body
• National Human Radiobiology Tissue Repository
• The USTUR has provided important scientific
information to ensure the adequacy of the safety
standards for these radioactive elements
Research Seminar at Oregon State University, November 27, 2017
• Inhalation
i. Americium Oxide (AmO2)
ii. Plutonium Oxide (PuO2)
iii. Plutonium Nitrate [Pu(NO3)4]
iv. Uranium Hexafluoride (UF6)
• Wound
i. Americium Nitrate [Am(NO3)3]
ii. Plutonium Nitrate [Pu(NO3)4]
iii. Plutonium Oxide (PuO2)
• Ca-EDTA/DTPA Chelation
i. Americium Oxide (AmO2)
ii. Plutonium Nitrate [Pu(NO3)4]
Primary Research: Biokinetic Modeling and Dosimetry of Actinides
Courtesy of W.J. Bair
Model development, validation, and parameterization
Research Seminar at Oregon State University, November 27, 2017
USTUR Registrants (I)
• Voluntary tissue donors (posthumous):
whole-(44) and partial-body (307) donations
• Former nuclear workers from DOE sites
Research Seminar at Oregon State University, November 27, 2017
USTUR Registrants (II)
• Documented radiation exposure and work history
• Acceptance criteria:
i. actinide internal deposition of ≥74 Bq (2 nCi)
ii. external dose to whole body ≥0.1 Sv (10 rem)
Research Seminar at Oregon State University, November 27, 2017
Primary Exposure
Research Seminar at Oregon State University, November 27, 2017
USTUR Donations
Research Seminar at Oregon State University, November 27, 2017
USTUR Operation
AutopsyTissue
CollectionRadiochemical
AnalysisBiokinetic Modeling
Drying and Ashing
Digestion and Dissolution
Radionuclide Separation
α-source Preparation
Actinide Measurements
Research Seminar at Oregon State University, November 27, 2017
Radiochemistry at USTUR
Research Seminar at Oregon State University, November 27, 2017
• Laboratory Facilities
• NHRTR
• Radiochemical Tissue Analysis
• Plutonium in Human
USTUR Laboratory Building
• Office
• Autopsy Lab
• Chemistry Lab
• Counting Room
• Drying/ashing room
• Sample storage area
6,500 sq. ft. facility
Research Seminar at Oregon State University, November 27, 2017
Autopsy Laboratory
MORTECH® Mortuary Refrigerator
MORTECH® Autopsy Station and Elevating Table
Research Seminar at Oregon State University, November 27, 2017
Tissue Ashing Room
Research Seminar at Oregon State University, November 27, 2017
VWR® 1685 HAFO Series Forced-Air Oven, Fisher Scientific® Isotempâ Muffle Furnace 550 Series, LINDBERG® Muffle Furnace Model 52641
Radiochemistry Laboratory
Research Seminar at Oregon State University, November 27, 2017
Counting Room
Research Seminar at Oregon State University, November 27, 2017
Sample Storage Area
Research Seminar at Oregon State University, November 27, 2017
National Human Radiobiology Tissue Repository
• Established in 1992
• Resources for radiation dosimetry and biological
effects studies
USTUR frozen-tissue collection:
Research Seminar at Oregon State University, November 27, 2017
Tissue Sample Analysis Protocol
Drying/Ashing
Digestion/Dissolution
Radionuclide Separation
α-source Preparation
Actinide Measurements(Alpha-Spec)
Research Seminar at Oregon State University, November 27, 2017
USTUR 106: Sample Drying and Ashing
• Drying: @ 100 ˚C for 4 days, max. 48 samples
• Ashing: @ 450 ˚C for 4 days (×2), max. 32 samples
Research Seminar at Oregon State University, November 27, 2017
USTUR 110: Sample Digestion
• Microwave Digestion
Soft tissue: HNO3 – HCl – HF, 9:3:4 (mL)
Bone: HNO3 – HCl, 10:3 (reverse aqua regia)
Controlled temperature: 220 ˚C
Monitored pressure: 40 bar
• Radiochemical tracers (NIST): 242Pu, 243Am, 232U
MARS-5 Microwave EasyPrep® Vessel
Research Seminar at Oregon State University, November 27, 2017
USTUR 350: Actinide Separation
• Vacuum-Assisted Extraction Chromatography
TEVA
DGA
TRU
Research Seminar at Oregon State University, November 27, 2017
USTUR 350: Actinide Separation (Pu)
9) Pu Elution: 20 mL0.1M HCl - 0.05M HF – 0.04M
Rongalite
5) Beaker rinse: 2 × 5 mL 3M HNO3
6) Separate cartridges 7) TEVA rinse: 30 mL 3M HNO3 8) Rinse: 20 mL 9M HCl (Th)
1) Sample in 40 mL 3M HN03 – 1M Al(NO3)3
2) Add 0.75 mL 1.5M Sulfamic Acid + 6 mL 0.75M Ascorbic Acid
3) Add 2.5 mL 3.5 M Sodium Nitrite
4) Sample loading (1 drop sec-1)
1 mL TEVA Resin
(50-100 µm)
1 mL TRU-Resin
(50-100 µm)
Alpha spectrometry
Electrodeposition
1 mL DGA-Resin
(50-100 µm)
Discard (4 – 8)
(6)
Research Seminar at Oregon State University, November 27, 2017
USTUR 350: Actinide Separation (Am)
10) Am to DGA: 15 mL 4M HCl11) Separate cartridges
Discard (10)
1 mL TRU-Resin
(50-100 µm)
1 mL DGA-Resin
(50-100 µm)
(11)
14) Am Elution: 10 mL 0.25M HCl
Alpha spectrometry
Electrodeposition
12) Rinse: 3 mL 1M HNO3
13) Rinse: 10 mL 0.1M HNO3 (U)
Discard (12,13)
1 mL DGA-Resin
(50-100 µm)
(14)
TRU – DGA cartridges from Step 6
Research Seminar at Oregon State University, November 27, 2017
USTUR 350: Actinide Separation (U)
TRU cartridge from Step 11
15) Rinse: 12 mL 2.0 M HCl – 0.2M HF (Th)16) U Elution: 15 mL 0.1M Ammonium Bioxalate
Alpha spectrometry
Electrodeposition Discard (15)
(16)
Research Seminar at Oregon State University, November 27, 2017
USTUR 520: Electrodeposition
• Phoenix® EP-12 Series electrodeposition unit
• Custom Electrolytic Cell
• Na2SO4 electrolyte solution
• 1 hr electrodeposition @ 0.75 A
• α-source: 5/8˝ stainless steel disk (planchet)
Research Seminar at Oregon State University, November 27, 2017
USTUR 600: Alpha-Spectrometry
• ORTEC: Ensemble (3) and Octête PC (3) systems
• Detector: ENS-U450 (48)
• Software: AlphaVision 6.0.4
• Calibration: E&Z Analytics (1); USTUR (8)
• Sample count time: 150,000 s
Research Seminar at Oregon State University, November 27, 2017
USTUR Case Analysis Timeline
2 weeks
Actinide Measurements
2 weeks
α-source Preparation
1 week
Radionuclide Separation
2 – 3 Weeks
Digestion/Dissolution
2 weeks
Ashing
1 – 2 Weeks
Drying
~ 10 weeks
Research Seminar at Oregon State University, November 27, 2017
48 Tissue Samples
Tissue Analysis Throughput
Samples Analyzed
233
337
271
432
332
2013
2014
2015
2016
2017
Research Seminar at Oregon State University, November 27, 2017
Plutonium in Tissues of Occupationally Exposed Individuals
Research Seminar at Oregon State University, November 27, 2017
Deposition and Retention in Human Body
Research Seminar at Oregon State University, November 27, 2017
Liver (45%)
Skeleton (45%)
Soft tissues (10%)
Pu intake BloodstreamSystemic
deposition
Deposition and Retention in Human Body
Research Seminar at Oregon State University, November 27, 2017
• Respiratory tract (major)
• Systemic deposition (minor)
InhalationInsoluble material
Respiratory Tract +
Systemic
Route of Intake
Research Seminar at Oregon State University, November 27, 2017
239Pu Activity Concentration: Lung
Range 0.00055 – 7,225
Bq
kg
-1
Geometric Mean 1.43
95% CI for Mean 0.98 – 2.09
Median 1.28
95% CI for Median 0.52 – 2.61
Research Seminar at Oregon State University, November 27, 2017
239Pu Activity Concentration: LNTH
Range 0.0018 – 68,400
Bq
kg
-1
Geometric Mean 20.83
95% CI for Mean 13.83 – 31.38
Median 18.80
95% CI for Median 9.98 – 37.59
Research Seminar at Oregon State University, November 27, 2017
239Pu Activity Concentration: Liver
Range 0.00045 - 924
Bq
kg
-1
Geometric Mean 1.28
95% CI for Mean 0.92 – 1.78
Median 1.23
95% CI for Median 0.74 – 1.85
Research Seminar at Oregon State University, November 27, 2017
239Pu Activity Concentration: Skeleton
Range 0.0035 – 209
Bq
kg
-1
Geometric Mean 0.40
95% CI for Mean 0.30 – 0.53
Median 0.35
95% CI for Median 0.25 – 0.49
Research Seminar at Oregon State University, November 27, 2017
Summary: 239Pu Activity Concentration
Skeleton < Liver ≈ Lung << LNTH
1 4 54
Research Seminar at Oregon State University, November 27, 2017
239Pu Activity Concentration in Organs: USTUR vs Mayak PA
Research Seminar at Oregon State University, November 27, 2017
Hanford Site vs Mayak
Hanford
• 586-square-miles of shrub-steppe
desert in southeastern Washington
State
• In 1943, site was used to produce
plutonium for the bomb
• Continued operation during the
cold war
• Last reactor ceased operation in
1987
• Site clean up operation 1989 -
present
Research Seminar at Oregon State University, November 27, 2017
http://www.hanford.gov/page.cfm/HanfordHistory
Mayak
• The Mayak Production Association
• Built between 1945–48
• Secret Soviet Union atomic bomb
project
• Five nuclear reactors
• Plutonium for weapons
• Later reprocessing spent nuclear
fuel from nuclear reactors
• Mayak is still active as of 2017
https://en.wikipedia.org/wiki/Mayak
http://www.jccem.fsu.edu/Partners/MAYAK.cfm
LNTH-to-Lung: 239Pu Concentration Ratio
LNTH : Lung > 19 ICRP Type S
Range 0.009 – 561
Geometric Mean 13.5
95% CI for Mean 10.9 – 16.5
Median 16.5
95% CI for Median 12.1 – 19.8
Research Seminar at Oregon State University, November 27, 2017
Skeleton-to-Liver: 239Pu Activity Ratio
1:1 (Systemic Model Assumption)
Range 0.03 – 125
Geometric Mean 1.63
95% CI for Mean 1.39 – 1.91
Median 1.41
95% CI for Median 1.17 – 1.63
Research Seminar at Oregon State University, November 27, 2017
USTUR: Take Home Message
• In-depth study of actinide biokinetics and
dosimetry
• Unique resource of data from former nuclear
workers
• Obtain, analyze, and preserve tissue samples for
future research
• Significant impact on national and international
radiation protection advisory bodies
• 50-y research funded by U.S. DOE
Research Seminar at Oregon State University, November 27, 2017
Questions?
www.ustur.wsu.edu
Research Seminar at Oregon State University, November 27, 2017