From Single Bone Analysis to Total Skeleton Content

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Slide 1 European Radiation Dosimetry Group (EURADOS) WG7 Plenary Meeting Gent, Belgium, 14-16 September, 2011 From Single Bone Analysis to Total Skeleton Content S.Y. Tolmachev & A.C. James U.S. Transuranium and Uranium Registries, 1845 Terminal Drive Suite 201, Richland, WA 99354 stolmachev@tricity.wsu.edu Learning from Plutonium and Uranium Workers

Goal Slide 2 Precise estimation of total actinide activity in skeleton

Approaches Slide 3 Analysis of the entire skeleton Analysis of selected/available bones

Pros and Cons Slide 4 Entire Skeleton Analysis: most precise estimation very limited opportunities (USTUR) large number of analyses Analysis of Selected/Available Bones: typical scenario how precise is the estimation?

USTUR Mission Slide 5 to follow up occupationally exposed workers, from exposure through full lifespan, by studying the biokinetics (uptake, translocation and retention), and tissue dosimetry of the actinides (Pu, Am and U). http://www.ustur.wsu.edu/mission/index.html

USTUR Registrants Slide 6 to date, 330 former workers from various U.S. weapons or other sites with known history of exposure to actinides voluntarily donated their tissues or entire bodies for scientific research.

Registrant Statistics Slide 7 Total Active (Living) and Deceased Registrants : 416 Living Registrants: 81 Potential Partial-body Donors: 62 Potential Whole-body Donors: 12 Special Studies: 7 Deceased Registrants: 335 Partial-body Donations: 291 Whole-body Donations: 39 Special Studies: 5 Inactive Registrants: 458 Total Number of Registrants: 874 - as of August 15, 2011

Human Tissue Analysis Slide 8 Autopsy/Dissection/Vacuum Packing/Inventory Tissue sample dry/wet ashing / Dissolution Actinide radiochemical separation Counting source preparation: electrodeposition Detection: α-spectrometry/icp-ms

LANL Dissection Protocol Slide 9 McInroy et al (1985, HPJ): The U.S. Transuranium Registry Report of the 241 Am Content of a Whole Body. Part IV: Preparation and Analysis of the Tissues and Bones.

LANL Dissection Protocol (2) Slide 10 McInroy et al (1985, HPJ): The U.S. Transuranium Registry Report of the 241 Am Content of a Whole Body. Part IV: Preparation and Analysis of the Tissues and Bones.

USTUR Dissection Protocol Slide 11 Reduction in number of dissected samples: whole ribs vs VE, MS, SE hand and wrist vs carpal bones + phalanges foot and ankle vs tarsal bones + phalanges fewer numbers of skin/fat/muscle samples Reduction in the number of analyzed samples

Whole Body: Number of Analyses Slide 12 Case Lab Analysis Total Bones Ratio 0193 LANL 1982 423 307 73 % 0208 LANL 1984 307 170 55 % 0425 WSU 1994 120 87 73 % 0269 WSU 1994 106 84 79 % 0720 WSU 2005 127 84 66 % - Right side of the skeleton; odd ribs and vertebrae - Number of bones from the left side of the skeleton were analyzed

Whole- vs Partial- Body Analysis Slide 13 Type Skeleton Number of Samples Collected Analyzed Whole Body Axial 110 62 Limbs 70 50 Partial Body Total 5-7 5-7 - ribs, clavicle, patella, sternum, vertebrae, femur (MS)

Total Skeletal Activity Calculation Slide 14 Whole Body: Analysis: right side of the skeleton Calculation: interpolation for even ribs and vertebrae Total Activity: activity in right side x 2 Partial Body: Analysis: rib(s), clavicle, patella, sternum, vertebra(e), femur (middle shaft) Calculation: weighted average skeletal concentration ICRP89 skeletal weight: -10.7 + 0.119H (cm) Total Activity: skeletal concentration ICRP89 kg

Slide 15 Can we do more from less?

Tasks Slide 16 Best bone (group of bones) for the estimation of total actinide content in skeleton Precise estimation of skeleton content based on a limited number of bone analyses (partial-body donor, biopsy) Optimization of number of bone samples in wholebody analysis

Actinide Distribution in Skeleton Slide 17 McInroy et al (1985, HPJ) The U.S. Transuranium Registry Report of the 241 Am Content of a Whole Body. Part IV: Preparation and Analysis of the Tissues and Bones. Lynch et al (1988, J. Radiol. Prot.) Macrodistribution of plutonium and americium in four human skeletons. Filipy et al (2003,HPJ) Estimation of Actinide Skeletal Content in Humans Based on Bone Samples Collected At Autopsy.

Methodology Slide 18 McInroy et al (1985, HPJ): analysis of half of the skeleton. Single case analysis (first whole-body donation to the USTUR). Lynch et al (1988, J. Radiol. Prot.) defined a group of bones which best represents the total skeletal content. Analysis based on 4 whole-body cases. Filipy et al (2003,HPJ): least square regression analysis based on data from 8 whole-body cases.

Distribution of Pu in Skeleton Slide 19 Lynch et al (1988, J. Radiol. Prot.) Macrodistribution of plutonium and americium in four human skeletons Skull: 12.4 ± 1.1% Cervical Spine: 2.3 ± 0.2% Thoracic Spine: 8.1 ± 2.2% Lumbar Spine: 6.4 ± 2.0% Sacrum & Coccyx: 3.0 ± 0.7% Pelvis: 12.5 ± 1.2% Clavicles: 0.99 ± 0.14% Scapulae: 3.3 ± 0.3% Ribs: 6.8 ± 0.3% Sternum: 1.2 ± 0.2% Humeri: 5.1 ± 0.8% Femora: 16.0 ± 2.2% Tibiae: 7.6 ± 1.1% Patellae: 0.66 ± 0.09%

Proposed Methodology Slide 20 Ratio = Individual Bone Concentration Total Skeletal Concentration Best bone = C bone, Bq kg -1 C skeleton, Bq kg -1 1 ± (UNC min)

To Do List Slide 21 Conduct radiochemical analysis of available whole-body cases Calculate skeletal concentrations Populate set of C bone /C skeleton for analyzed cases

Radiochemistry Status: Whole- Body Cases Slide 22

Radiochemistry Results: Where to Find? Slide 23

Radiochemistry Results: What is Inside? Slide 24 http://www.ustur.wsu.edu/case_studies/radiochemistry/html/0425_radchem.php

Work in Progress Slide 25 Case Age, y Osteoporotic Primary Nuclide Skeletal Conc., Bq wt.kg -1 Cbone /Cskeleton Ribs Stern. Vert. Patella Clavic. 0193 62 Pu 5.83 0.77 1.24 1.10 1.21 1.04 0208 69 Pu 10.9 0.74 1.29 0.62 1.24 1.00 0212 56 no Pu 10.9 0.74 1.03 0.75 2.06 1.18 0213 68 no Pu 20.2 0.86 1.18 1.06 1.42 0.87 0242 77 Pu 42.2 0.68 0.95 0.78 1.28 1.05 0259 55 no 238 Pu 10.53 0.64 0.65 0.63 1.66 0.81 0425 83 no Pu 2.82 1.61 1.10 1.46 0.51 0.99 0679 72 yes Pu 10.52 1.29 0.62 1.13 ----- 1.04 0720 84 yes Pu 8.49 0.70 0.71 1.16 0.91 1.22 0744 67 no Pu 8.62 1.2 ----- 0.98 1.27 1.00 0269 79 yes Pu 119.1 0.91 1.01 1.01 1.16 1.05 0682 71 no 238 Pu 27.3 1.09 0.80 1.23 1.41 0.67

Work Summary Slide 26 Case Age, y Osteoporotic Primary Nuclide Cbone /Cskeleton Ribs Stern. Vert. Patella Clavic. Variability by Case 0193 62 Pu 0.77 1.24 1.10 1.21 1.04 1.07±0.19 0208 69 Pu 0.74 1.29 0.62 1.24 1.00 0.98±0.30 0212 56 no Pu 0.74 1.03 0.75 2.06 1.18 1.15±0.54 0213 68 no Pu 0.86 1.18 1.06 1.42 0.87 1.08±0.23 0242 77 Pu 0.68 0.95 0.78 1.28 1.05 0.95±0.23 0259 55 no 238 Pu 0.64 0.65 0.63 1.66 0.81 0.88±0.44 0425 83 no Pu 1.61 1.10 1.46 0.51 0.99 1.13±0.43 0679 72 yes Pu 1.29 0.62 1.13 ----- 1.04 1.02±0.29 0720 84 yes Pu 0.70 0.71 1.16 0.91 1.22 0.94±0.24 0744 67 no Pu 1.2 ----- 0.98 1.27 1.00 1.11±0.14 0269 79 yes Pu 0.91 1.01 1.01 1.16 1.05 1.03±0.09 0682 71 no 238 Pu 1.09 0.80 1.23 1.41 0.67 1.04±0.30 12 70 ±10 all Pu 0.94 ±0.30 0.96 ±0.24 0.99 ±0.25 1.28 ±0.39 0.99 ±0.15 Variability by Bone

Conclusion Slide 27 Best bone = C bone, Bq kg -1 C skeleton, Bq kg -1 1 ± (UNC min) Clavicle is the one: 0.99 ± 0.15

Future Work Slide 28 Calculate C bone /C skeleton using bone ash weights. Calculate C bone /C skeleton for other bones typically collected at autopsy from partial-body donors: femur (whole, or middle shaft), scapula, calvarium. Populate C bone /C skeleton for all individual bones. Apply advanced mathematical algorisms to define best group of 3-5-7 bones.

Slide 29 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.

Thank you! Slide 30