Calculation of Doses due to Accidental Release of Pu from a LMFBR

138 Pages·1974·2.47 MB·English

;ORNL-NSIC-74
CALCULATION OF DOSES DUE TO ACCIDENTALLY
1
B
RELEASED PLUTONIUM FROM AN LMF8.R
B. R. Fish, G. W. Keilholtz,
W. S. Snyder, S. D. Swisher
NSlC
NUCLEAR SAFETY INFORMATION CENTER

ORNL-NSIC-74
Contract No. W-7405-eng-26
Nuclear Safety Information Center
CALCULATION OF DOSES DUE TO ACCIDENTALLY
RELEASED PLUTONIUM FROM AN LMFBR
B. R. Fish, Health Physics Division
G. W. Keilholtz, Reactor Chemistry Division
W. S.. Snyder, Health Physics Division
S; D. Swisher, Atmospheric Turbulence and
Diffusion Laboratory, NOAA
NOVEMBER 1972
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iii
CONTENTS
c Page
PREFACE ............................................................. V
‘4
ACKNOWLEDGMENT.. .................................................... vii
ABSTRACT ............................................. .. .............. ix
1. INTRODUCTION .................................................... 1
2. BEHAVIOR OF RELEASED SODIUM OXIDE AND PLUTONIUM-
BEARING PARTICLES ..;............................................ 4
2.1 Aerosol Behavior Considerations . . . . . . . . . . . . . . . . . . . . . . . . . . . .
,2.1.1 Brownian motion _....................................
2.1.2 Gravity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
2.1.3 Turbulence . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
2.2 Experimental Evidence for Decay of Mass Concentration
and Changes in Particle Size of Airborne Aerosols with
Time ....................................................... 10
2.3 Empirical Models and Equations for the Decay of Mass Con-
centration and Changes in Particle Size with Time .......... 12
2.3.1 Schikarski model .................................... 13
2.3.2 Davis model ..... ..................................... 14
2.3.3 Koontz model ........................................ 15
2.4 Detailed Discussion of an Aerosol Model and Its Appli-
cation ..................................................... 16
2.5 A Postulated Release of Radionuclides from an LMFBR-
Type Reactor under Accident Conditions ..................... 24
t
References ...................................................... 27
3. TRANSPORT, SETTLING, AND REDISTRIBUTION OF AEROSOLS IN THE
ouTsIDE Am (TROPOSPHERE) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31
3.1 Meteorological Considerations .............................. 31
3.2 Properties of NazO Aerosols in the Atmosphere .............. 32
References ...................................................... 35
4. CHEMISTRY OF PLUTONIUM .......................................... 36
4.1 Compounds of Plutonium ..................................... 36
4.1.1 Plutonium dioxide and mixed oxides .................. 37
4.1.2 Plutonium carbides, nitrides, and silicides ......... 44
4.1.3 Sodium-uranium-plutonium oxides ..................... 45
4.1.4 Other inorganic compounds ........................... 45
4.2 Solution Chemistry of Plutonium ............................ 46
4.2.1 Complex formation by plutonium in aqueous
solutions ........................................... 47
4.2.2 Solubility of plutonium compounds ................... 49
4.2.3 Complex formation by plutonium in various oxida-
tion states .......................................... 50
4.3 Methods for Separation of Plutonium from Uranium and
Fission Products ........................................... 52
4.3.1 Solvent extraction .................................. 52
4.3.2 Ion exchange methods ................................ 53
iv
4.4 Analytical Methods for Determining Plutonium ............... 55
4.4.1 Conventional methods ................................ 55
4.4.2 Radiochemical methods ............................... 56
References ...................................................... 57
5. INTAKE AtiD METABOLISM OF PLUTONIUM DIOXIDE ...................... 60
5.1 Intake Pathways ............................................ 61
5.1.1 Inhalation .......................................... 61
5.1.2 Ingestion ........................................... 77
5.1.3 Deposition on body surfaces ......................... 84
5.2 Systemic Distribution and Retention ........................ 86
5.2.1 Transport in the bloodstream ........................ 86
5.2.2 Deposition and retention in bone .................... 87
5.2.3 Deposition and retention in liver ................... 88
5.2.4 Deposition and retention in gonads .................. 89
5.2.5 Elimination of plutonium from the body .............. 90
References ...................................................... 93
6. COMPUTATION OF INTERNAL DOSE .................................... 104
6.1 Physical Dosimetry and Dose Equivalent ..................... 104
6.2 Dose Calculations for Inhaled Plutonium .................... 106
6.3 Consideration of Other Plutonium Isotopes .................. 110
6.4 Consideration of Other Transuranics ........................ 113
6.5 Gastrointestinal Tract Intake During Release ............... 116
6.6 Ingestion of Plutonium in Food.and Water ................... 117
6.7 Summary Calculations ....................................... 117
6.7.1 Source term evaluations ............................. 117
6.7.2 Leakage and dispersion .............................. 119
6.7.3 Calculation of dose ................................. 119
References ....................................................... 121
7. SUMMARY ......................................................... 122
.
V
PREFACE
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vii
ACKNOWLEDGMENT
2
In the preparation of this report the authors benefitted from the
review and comment of many people who are active in various aspects of
the many fields of expertise involved in accident analysis and plutonium
dose calculation. While this does not mean that all reviewers necessa-
rily agree with the report in every detail, we do wish to acknowledge
their contribution by listing the participants. .Trusting that no one
has been overlooked, they are as follows:
Internal Reviewers (ORNL)
C. J. Barton Wm. B. Cottrell F. L. Miller
S. R. Bernard R. J. Davis P. Nettesheim
R. H. Bryan P. B. Dunaway G. W..Parker
T. J. Burnett M. H. Fontana L. F. Parsly
J. R. Buchanan A. P. Malinauskas H. B. Piper
P
External Reviewers
i
A. W. Castleman, Brookhaven National Laboratory
Patricia W. Durbin, Lawrence Berkeley Laboratory
Headquarters Staff, U.S. Atomic Energy Commission
M. M. Hendrickson, Battelle-Northwest Laboratories
H. H. Hopkins, Atlantic Richfield, Hanford Company
R. L. Junkins, Battelle-Northwest Laboratories
W. H. Langham (deceased), Los Alamos Scientific Laboratory
J. N. P. Lawrence, Los Alamos Scientific Laboratory
H. E. Meyer, Mound Laboratory
H. A. Morewitz, Atomics International
I. Nelson, Battelle-Northwest Laboratories
W. D. Norwood, Hanford Environmental Health Foundation
L. C. Schwendiman, Battelle-Northwest Laboratories
R. C. Thompson, Battelle-Northwest Laboratories