calculation of doses due to accidentally 1 b released plutonium from an lmf8.r nuclear safety

138 Pages·2001·9.32 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
OAK RIDGE NATIONAL LABORATORY
Oak Ridge, Tennessee 37830
operated by
UNION CARBIDE CORPORATION
for the
U.S. ATOMIC ENERGY COMMISSION
Printed in the United States of America. Available from
National Technical Information Service
U.S. Department of Commerce
5285 Port Royal Road, Springfield, Virginia 22151
Price: Printed Copy $15.00; Microfiche $15.00
This report was prepared as an account of work sponsored by the United
States Government. Neither the United States nor the United States Atomic
Energy Commission, nor any ‘of their employees, nor any of their contractors,
subcontractors, or their employees, makes any warranty, express 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.
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
The Nuclear Safety Information Center, established in March 1963 at
the Oak Ridge National Laboratory under the sponsorship of the U.S. Atomic
Energy Commission, is a focal point for the collection, storage, evalu-
ation, and dissemination of nuclear safety information. A system of key
words is used to index the information cataloged by the Center. The title,
author, installation, abstract, and key words for each document reviewed
are recorded at the central computer facility in Oak Ridge. The references
are cataloged according to the following categories:
1. General Safety Criteria
2. Siting of Nuclear Facilities
3. Transportation and Handling of Radioactive Materials
4. Aerospace Safety
5. Heat Transfer and Thermal Transients
6. Reactor Transients, Kinetics, and Stability
7. Fission Product Release, Transport, and Removal
8. Sources of Energy Release under Accident Conditions
9. Nuclear Instrumentation, Control, and Safety Systems
1-O. Electrical Power Systems
11. Containment of Nuclear Facilities
12. Plant Safety Features - Reactor
13. Plant Safety Features - Nonreactor
14. Radionuclide Release and Movement in the Environment
15. Environmental Surveys, Monitoring, and Radiation Exposure
of Man
16. Meteorological Considerations
17. Operational Safety and Experience
18. Safety Analysis and Design Reports
19. Radiation Dose to Man from Radioactivity Release to the
Environment
20. Effects of Thermal Modifications on Ecological Systems
21. Effects of Radionuclides and Ionizing Radiation on
Ecological Systems
vi
Computer programs have been developed which enable NSIC to (1) oper-
ate a routine program of Selective Dissemination of Information (SDI) to .
individuals according to their particular profile of interest, (2) make
retrospective searches of the stored references, and (3) distribute scope
and progress information on R&D contracts from the Program and Project In-
formation File (PPIF).
Services of the NSIC are available to government agencies, research
and educational institutions, and the nuclear industry on a partial cost
recovery basis designed to regain a portion of the expense associated with
disseminating the information to the user. A minimal inquiry response is
available free. NSIC reports (i.e., those with the ORNL-NSIC numbers) may
be purchased from the National Technical Information Service (see inside
front cover) while documents indexed by NSIC may be examined at the Center
by qualified personnel. Inquiries concerning the capabilities and oper-
. ation of the Center may be addressed to:
J. R. Buchanan, Assistant Director
(Phone [phone], Ext. 3-7253)
Nuclear Safety Information Center
Oak Ridge National Laboratory
Post Office Box Y
Oak Ridge, Tennessee 37830
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