BRH/DER 70-1
RADIOLOGICAL
SURVEILLANCE
STUDIES AT A
BOILING WATER
NUCLEAR POWER REACTOR
ENVIRONMENTAL PROTECTION AGENCY
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NOTE:
This report was originally prepared by the Division of Environmental Radiation,
Bureau of Radiological Health, Department of Health, Education, and Welfare
with the first printing in March 1970. With the formation of the Environmental
Protection Agency and the transfer of the Division of Environmental Radiation's
Staff and functions to this new Agency, the cover and title page have been
changed accordingly for the second printing. ,
V
TECHNICAL, REPORTS OF THE DIVISION OF ENVIRONMENTAL RADIATION. BUREAU OF RADIO-
LOGICAL HEALTH, are available from the CLEARINGHOUSE FOR FEDERAL SCIENTIFIC
AND TECHNICAL INFORMATION, Springfield, Va., 22151. Price is $3.00 for paper
copy and $0.65 for microfiche.
DER 69-1 - EVALUATION OF RATON 222 NEAR URANIUM TAILINGS PILES PB 188 691
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RADIOLOGICAL
SURVEILLANCE
STUDIES AT A
BOILING WATER
NUCLEAR POWER REACTOR
Bernd Kahn
Richard L. Blanchard
Herman L. Kri eger
Harry E. Kolde
David B. Smith
Alex Martin
Seymour Gold
William J. Averett
William L. Brinck
Gerald J. Karches
Radiological Engineering Laboratory
Division of Surveillance and Inspection
5555 Ridge Avenue
Cincinnati, Ohio 45213
Second Printing February 1971
ENVIRONMENTAL PROTECTION AGENCY
Radiation Office
Rockville, Maryland 20852
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FOREWORD
The Bureau of Radiological Health carries out a national program designed
to reduce the exposure of man to hazardous ionizing and non-ionizing radiation.
Within the Bureau, the Division of Environmental Radiation conducts
programs relating to 1) public health evaluation of planned and operating
nuclear facilities, 2) field studies at operating nuclear facilities to
develop environmental surveillance technology, and 3) systems of national
radiation surveillance programs to evaluate population exposure from all
sources of environmental radioactivity.
The Bureau publishes its findings in Radiological Health Data and Reports
(a monthly publication), Public Health Service numbered reports, appropriate
scientific journals, and Division technical reports.
The technical reports of the Division of Environmental Radiation allow
comprehensive and rapid publishing of the results of intramural and con-
tractor projects. The reports are distributed to State and local radiological
health program personnel, Bureau technical staff, Bureau advisory committee
members, university personnel, libraries and information services, industry,
hospitals, laboratories, schools, the press, and other interested individuals.
These reports are also included in the collections of the Library of Congress
and the Clearinghouse for Federal Scientific and Technical Information.
I encourage the readers of these reports to inform the Bureau of any
omissions or errors. Your additional comments or requests for further in-
formation are also solicited.
John C. Villforth
' Bureau Director
III
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PREFACE
The projected increase in the utilization of nuclear power for electrical
generating plants has resulted in both State and Federal public health
agencies placing increased program emphasis on the surveillance of nuclear
power plants. Hie Bureau of Radiological Health provides recommended nuclear
facility surveillance program information for the guidance of health agencies.
In order to provide a better technical basis for our surveillance recom-
mendations, a series of field studies were conducted at operating nuclear
facilities to obtain better data on radionuclides in plant effluents and
their subsequent distribution in the environment.
TTiis technical report summarizes the first such study which was conducted
at the Dresden Nuclear Power Station. The study was planned and performed by
the staff of the Division of Environmental Radiation, Bureau of Radiological
Health, Environmental Control Administration, with close cooperation of the
111 inois Department of Public Health, the Commonwealth Edison Company, the
Division of Compliance, AEC, and the Division of Radiation Protection Stand-
ards , AEC.
We wish to thank all of the reviewers of this report for their extensive
cormients on the preliminary draft.
Charles L. Weaver
Director, Division of Environmental
Radiation
V
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CONTENTS
Page
1. introduction 1
1.1 Need for Study 1
1.2 Study Design 1
1.3 References 2
2. RADIONUCLIDES IN LIQUIDS ON SITE 5
2.1 Samples 5
2.1.1 Collection 5
2.1 2 Primary coolant 5
2.1.3 Fuel storage pool 6
2.1.4 Contaminated deminerali zed water 6
2. 2 Analysis 7
2.2.1 Gamma-ray spectrometry 7
2.2.2 Alpha-particle spectrometry 7
2.2. 3 Radiochemistry 7
2.3 Results and Discussion 7
2.3.1 Radionuclides in primary coolant 7
2.3. 2 Radionuclide losses in sanples 7
2.3.3 Generation rates of fission products in fuel and transfer rates
to primary coolant .. 9
2.3.4 Generation rates of progeny of gaseous radionuclides in coolant. 11
2.3.5 Turnover rates of gaseous radioiodine ... 12
2.3.6 Formation and turnover rates of tritium 13
2.3.7 Turnover rate of activation products in primary coolant 14
2.3.8 Radionuclides in fuel pool and contaminated demineralized water. 14
2. 4 References 14
3. RADIONUCLIDES IN LIQUID WASTE EFFLUENTS ..... 17
3.1 Samples. 17
3.1.1 Collection. ... 17
3.1.2 Liquid wastes 17
3.1.3 Effluent radioactivity , ....... 18
3.1.4 Effluent sampler 18
, 3.2 Analysis, ......................... 19
3. 2.1 Liquid wastes.,,. .r..,.... 19
3.2.2 Coolant-canal samples ..,. ...,... 19
3.3 Results and Discussion................................... ...........». 21
3.3.1 Radionuclide content of liquid wastes 21
3.3.2 Solubility of radionuclides in high-conductivity waste,... ,v.,r,. 22
3.3.3 Turnover rate in primary coolant vi* release rate in
liquid waste, 22
3.3.4 Concentration of ionic raclionuclides at point of discharge!...^,. 23
VII
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25
25
26
27
29
29
29
31
32
32
33
34
34
38
38
40
40
41
43
43
43
43
43
43
44
46
46
47
51
51
51
51
51
54
54
54
55
56
59
59
59
60
61
61
62
62
62
63
65
3.3.5 Retention efficiency of effluent sampler
3.3.6 Insoluble radionuclides suspended in cooling-canal water
3.3.7 Tritium concentrations in water
3.4 References
4. RADIONUCLIDES RELEASED FBCM STACK
4.1 Samples
4.1.1 Description of system „
4.1.2 Sample collection
4.2 Analysis
4.2.1 Gamma-ray spectrometry
4.2.2 Radiochemical analysis
4.3 Results and Discussion
4.3.1 Radioactive noble gases and 3H
4.3.2 Airborne particles in the stack
4.3.3 Gaseous 13*1 in the stack
4.3.4 Airborne particles in ventilating air...
4.3.5 Sources of airborne particles
4. 4 References
5. RADIONUCLIDES IN ENVIRONMENTAL AIR
5.1 Introduction
5.1.1 Purpose.
5.1.2 Environment and meteorology
5.2 Short-term Radionuclide Concentrations and Radiation Exposure Rates...
5.2.1 Measurements
5.2.2 Radioxenon collector..
5. 2. 3 Meteorology
5.2.4 Estimation of radionuclide concentrations and exposure rates....
5.2.5 Results and discussion
5.3 Long-term Radiation Exposure Rates
5.3.1 Measurement
5.3.2 Analysis
5.3.3 Estimation of exposure rates
5.3.4 Results and discussion
5.4 Portable Survey Meters
5.4.1 Measurement
5.4.2 Calibration
5.4.3 Results and discussion
5.5 References
6. RADIONUCLIDES IN SURFACE WATER
6.1 Water Use in the Illinois River
6.1.1 Public water supply and fishing
6.1.2 Radiation exposure calculations
6.2 Water at Peoria, Illinois
6.2.1 Sampling and analysis
6.2.2 Results and discussion
6.3 Fish at Dresden
6.3.1 Sampling and analysis..,..
6.3.2 Results and discussion
6.4 References
VIII
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7. RADIONUCLIDES IN THE TERRESTRIAL ENVIRONMENT 67
7.1 Dresden Environment 67
7.1.1 Site 67
7.1.2 Environmental surveillance 69
7.2 Estimation of Radioactivity Concentrations 70
7.2.1 Precipitation 70
7. 2.2 Deposition 71
7.2.3 Uptake in cattle thyroids and transfer to cows' milk 72
7.3 Rain and Snow , 72
7.3.1 Samples and analyses,... 72
7.3.2 Results and discussion 73
7.4 Soil 73
7.4.1 Samples and analyses 73
7.4.2 Results and discussion 73
7.5 Food and Feed 74
7.5.1 Sanples and analyses 74
7.5.2 Results and discussion 74
7.6 Milk 76
7.6.1 Samples 76
7.6.2 Analysis 77
7.6.3 Results and discussion,,,,,.,,,.....,.,.,,. 78
7.7 Cattle Thyroids 79
7.7.1 Samples 79
7.7.2 Analysis ...... 79
7.7.3 Results and discussion 79
7.8 Radionuclides in Wildlife 80
7.8.1 Samples and analyses 80
7.8.2 Results and discussion 81
7.9 References 83
8. SUMMARY AND CONCLUSIONS 85
8.1 Radionuclides in Dresden Effluents 85
8.2 Radionuclides and Radiation from Dresden in the Environment...,.,,.... 86
8. 3 Monitoring Procedures. 87
8.4 Considerations in Developing Recommendations for Environment-al
Surveillance
8.5 Suggested Future Studies 89
APPENDICES:
Appendix A Acknowledgments 91
Appendix B Estimation of Radionuclide Formation and Turnover Rates 92
Appendix C Estimation of Radionuclide Concentrations in Air and
Radiation Exposures in Environment 97
Appendix D Estimation of Radionuclide Concentrations in Environmental
Samples -
IX
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Tables
Page
2.1 Radionuclide Concentration in Primary Coolant 8
2.2 Radionuclide Concentrations in Fuel Pool Water and Contaminated
Demineralized Water . 14
3.1 Radionuclide Concentrations in High-Conductivity Liquid Waste, 22
3.2 Radionuclide Concentrations in Liquid Laundry Waste . 23
3.3 Concentration of Ionic Radionuclides in Coolant-canal Water... 24
3.4 Radionuclide Content of Suspended Silt Collected from Coolant-canal
Water 26
3.5 Tritium Concentrations in Water 26
4.1 Stack Releases of Fission Product Noble Gases.. 36
4.2 Observed vs. Estimated Stack Release Rates of Noble Gases 36
4.3 Comparison of Off-gas Release Rates Measured in Delay Line and in Stack. 38
4.4 Release Rate of Tritium from Condenser Air Ejectors . 38
4.5 Stack Releases of Particulate Radionuclides and Gaseous Iodine-131 39
4.6 Summary of Stack Releases of Particulate Radionuclides and Gaseous
Iodine-131 40
4.7 Iodine-131 Concentration in Stack Monitor.,..., 40
4.8 Airborne Particles in Sphere and Turbine Building 41
5.1 Test Conditions for Sampling ENPS Stack Effluent in Environment 48
5.2 Radiation Exposure Rate and Radionuclide Concentration Measured in .
Air Near Ground Level Beneath Plumes from DNPS Stack....... 49
5.3 External Radiation Exposure Rates Near Dresden Measured with Powdered
Calcium Fluoride TLD's. 52
5.4 External Radiation Exposure Rates from Natural Background Measured
with Calibrated Nal(Tl) Monitors.. ,. 54
6.1 Radionuclide Concentration at Peoria, 111., Water Treatment Plant, 62
6.2 Radionuclide and Stable Ion Concentration in Fish Tissue..... 63
7.1 ®^Sr, ^Sr, and ^Cs £n Rain Water 72
7.2 Radionuclide Content of Snow.. 73
7.3 Concentration of Radionuclides and Stable Ions in Dresden Soil 74
7.4 Radiostrontium Concentration in Vegetables and Grass 75
7.5 Concentrations of Radionuclides and Stable Ions in Corn Kernels and
Husks 76
X
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7.6 131i Concentration in Raw Milk 78
7.7 Content of Cattle Thyroids., 80
7.8 Radionuclide Concentration and Stable Ion Concentration in Deer
Samples 82
7.9 Radionuclide and Stable Ion Concentrations in Tissue of Rabbits 82
XI
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Figures
Page
2.1 Primary Coolant Flow Schematic 5
2.2 Gamma-ray Spectra of Primary Coolant Water, 40-804 keV 9
2.3 Gamma-ray Spectra of Primary Coolant Water, 805-1,608 keV 10
2.4 Dresden Electrical Loading, May 1967 to August 1968 10
3.1 Gamma-ray Spectrum of High-conductivity Waste Solution 19
3.2 Gamma-ray Spectra of Cation-exchange Resins in Intake and Discharge
Coolant-water Canals 20
3.3 Gamma-ray Spectra of Anion-exchange Resins in Intake and Discharge
Coolant-water Canals 20
3.4 Ganma-ray Spectra of Suspended Silt in Intake and Discharge Coolant-
water Canals 21
3.5 Gamma-ray Coincidence Spectra of Suspended Silt in Intake and
Discharge Canals 21
4.1 Sources of Airborne Effluent 30
4.2 Gamma-ray Spectra of Off-gas from Delay Line 32
4.3 Gamma-ray Spectrum of Off-gas from Delay Line 33
4.4 Gamma-ray Spectrum of Off-gas from Delay Line 34
4.5 Ganma-ray Spectra of Off-gas from Delay Line after Various Periods
of Decay 35
4.6 Ganma-ray Spectra of Off-gas from Delay Line after Various Periods
of Decay 37
5.1 Location of Field Tests and Dosimeter Stations Near Dresden 44
5.2 Gamma-ray Spectra of Charcoal Xenon Collector 45
5.3 Gamma-ray Spectra of Air Filters 46
5.4 Gamma-ray Spectrum of Charcoal Xenon Collector, 24 Hours after
Collection 47
5.5 Exposure Rates under Neutral Conditions, Measured with Muscle-
equivalent Ionization Chamber 48
5.6 Exposure Rates under Stable Conditions, Measured with Muscle-
equivalent Ionization Chamber 49
5.7 Plume Rose and Estimated Exposure Rates at Dosimeter Stations 52
5.8 Comparison of Measured and Estimated Exposure Rates at HD Stations
Near Dresden on August 15—29. 1968 53
5.9 Typical Exposure Rates Measured with Portable Nal(Tl) Survey Meters,.,, 55
XII
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5.10 Net Gamma-ray Spectra Measured on Ground Near Centerline of Plume
with 10 X 10 cm Nal(Tl) Detector 56
6.1 Illinois River Below Dresden 59
7.1 Sampling Locations in Immediate Vicinity of Dresden Nuclear Power
Station 67
7.2 Sampling Locations in General Vicinity of Dresden Nuclear Power
Station 68
7.3 Gamma-ray Spectra of Corn Kernels 77
7.4 Gamma-ray Spectra of Cattle Thyroids 81
XIII
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1. INTRODUCTION
1.1 Need for Study
Radiological surveillance at central-
station electric power reactors under normal
operating conditions provides assurance of
adequate control over radionuclide effluents
and a means for estimating the resulting
radiation exposure of the population. The
purpose of this study was to identify and
quantify the radionuclides in effluents and
in the pathways from the point of discharge
in the environment to man in order to pro-
vide the technical basis for improving
surveillance programs. Improvements are
needed because of the projected increase of
commercial nuclear power stations in the
United States. The current interest of
the public in reducing environmental pollu-
tion and of the industry in conducting more
informative monitoring programs lends
support to the aims of this study.
Monitoring fallout from the nuclear
weapon tests and discharges at atomic energy
research laboratories has provided extensive
knowledge and experience. These are re-
flected in the many publications on environ-
mental monitoring,(2-23) radioactive waste
management,(24-30) anJ radionuclide trans-
fer in the biosphere. (31-45) Some informa-
tion on waste management is also available
in the periodic reports by commercial
operators of nuclear power plants to the
Atomic Energy Commission (ABC).
The Bureau of Radiological Health has
begun a series of studies at central-station
electric power reactors with the following
specific objectives: (1) to gain informa-
tion on individual radionuclides in the
effluent as a basis for developing recom-
mended radiological surveillance programs,
(2) to evaluate programs associated with
measuring discharged radionuclides and
interpreting results in terms of radiation
exposure, (3) to observe the movement of
critical radionuclides from a plant through
the environment under routine conditions of
station operation, (4) to develop compe-
tence within the Bureau of Radiological
Health for assisting public agencies in
monitoring sites of nuclear power plants.
It should be noted that the studies are not
intended to investigate waste management or
radiological surveillance practices at
specific nuclear power stations.
1.2 Study Design
The first radiological surveillance
study in this program, described here, was
undertaken at the Dresden Nuclear Power
Station of the Commonwealth Edison Company.
Dresden I is a boiling water reactor (BWR)
that has generated more than 9 X 10^ kilo-
watt-hours since it began operation in
1959, and lias been operating at a rated
power of 700 thermal megawatts (MWt) and
210 megawatts of electricity (MWe) since
1962• The power plant is a dual-cycle,
forced circulation system, built by the
General Electric Company. Fuel elements
consist of slightly enriched UOg clad in
Zircaloy-2. The station is located in
Illinois, 80 km SW of Chicago. Liquid
wastes are discharged into the cooling-
water discharge canal which empties into
the Illinois River; gases and airborne
particles are released from a 91-m stack;
and solid wastes are transported off-site
for burial.
The study was planned and performed by
the staff of the Division of Environmental
Radiation, Bureau of Radiological Health,
Environmental Health Service, PHS, with
I
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the close cooperation of the Illinois
Department of Public Health, Commonwealth
Edison Company, Division of Compliance of
the AEC, and Division of Radiation Protec-
tion Standards of the AEC. The data were
collected in five field trips on November
14-16, 1967, January 16-18, 1968, January
31-February 1, 1968. June 25-28, 1968, and
August 20-22, 1968« Participants in the
field trips are listed in Appendix A. Re-
sults were reported to all participants soon
after the field trips and have been reviewed
by them.
Emphasis was placed on relating dis-
charges to environmental levels of radio-
nuclides and radiation, and on evaluating
critical pathways and radionuclides. The
greatest efforts were devoted to measuring
the concentration of individual radionu-
clides in liquids and gases on site and in
effluent liquids, gases and airborne
particles; determining the radiation ex-
posure rate and radionuclide concentration
in air at ground level beneath the plume
from the stack; and testing devices that
concentrate radionuclides in air and water
for subsequent analysis. Other environ-
mental samples were analyzed, but further
work is needed in this area to provide more
specific information and to attain greater
analytical sensitivity. The study was
planned to avoid duplicating the following
active monitoring programs: (1) gross
activity in the effluents measured by
Dresden staff, (2) environmental radio-
nuclides measured by Dresden's surveillance
contractor, (3) environmental gross activity
measured by the Illinois Department of
Public Health, and (4) the Aerial Radio-
logical Measuring Survey conducted by an
AEC contractor.
Similar studies are in progress at a
pressurized water reactor and limited
studies are planned for some of the larger
stations that are now being placed into
operation. These studies will be directed
toward evaluating differences in the radio-
nuclide content of the liquid and gaseous
effluents and the transfer through the
biosphere to man.
1.3 References
1. Office of the Assistant General Manager
for Reactors, USAEC, "Nuclear Reactors
Built, Being Built or Planned in the
United States as of June 30, 1969*',
AEC Rept. TID-8200 (20th Rev.), (1969).
2. Committee 4, International Commission on
Radiological Protection, ''Principles of
Environmental Monitoring Related to the
Handling of Radioactive Materials'',
ICRP Publication #7, (Pergamon Press,
Oxford, 1965)•
3. ''Manual on Environmental Monitoring in
Normal Operation'', Safety Series #16
(International Atomic Energy Agency,
Vienna, 1966)*
4. ''Techniques for Controlling Air Pollu-
tion from the Operation of Nuclear
Facilities'', Safety Series #17 (Inter-
national Atomic Energy Agency, Vienna,
1966).
5. Setter, L. R., et al., ''Routine Surveil-
lance of Radioactivity around Nuclear
Facilities'', Public Health Service
Publication I999-RH-23 (1966).
6. Terrill, J. G., Jr., C. L. Weaver, E. D.
Harward, and D. R. Smith, ''Environmental
Surveillance of Nuclear Facilities'',
Nuclear Safety 9, 143 (19*68).
7. Ishihara, T., ''Environmental Radio-
logical Monitoring System at Nuclear
Installations'', Health Phys. I3t 549
(1967).
8. Joint Committee on Atomic Energy,
Congress of the U.S., ''Selected Materi-
als on Environmental Effects of Pro-
ducing Electric Power1', U.S. Gov't
Printing Office, Washington, D.C. (1969).
9. Roberts, I. C., ''Effluent Monitoring and
Evaluation, A Power Reactor Design
Guide'', AEC Rept. BNWL-251 (1967).
10. Terrill, J. G., Jr., E, D. Harward and
I. P. Leggett, Jr., ''Environmental
Aspects of Nuclear and Conventional
Power Plants'', Ind* Med. and Surgery
36, 412 ( 1967).
11. Weaver, C. L. and G. E, Stigall, ''Public
Health Evaluation of Nuclear Power
Plants", Health Phys. 13, 189 (1967).
12. Weaver, C. L. and E. D. Harward, Jr.,
''Surveillance of Nuclear Power Plants",
Public Health Fepts, 82, 899 (1967).
2
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13. Reinig, W, C., Ed.., Environmental Sur-
veillance in the Vicinity of Nuclear
Facilities (C. C. Thomas, Springfield,
111., 1970), in press,
14. Pelletier, C, A., ''Environmental Surveys
for Nuclear Facilities'', Nucleonics
17, #1, 58 ( 1959).
15. Grummitt, W. E., ''Environmental Surveys
for Nuclear Power Stations'', AEC Rept.
AECL-1656 (1962).
16. Godebold, B. C, and J, K. Jones, Eds.,
Radiological Monitoring of the Environ-
ment, (Pergamon Press, New York, 1965).
17. World Health Organization, ''Routine
Surveillance for Radionuclides in Air
and Water1', (WHO Geneva, 1968).
18. Soldat, J. K., ''Environmental Monitoring
Lecture Notes*', AEC Rept. BNWL-SA-125
(1965).
19. ''Safety Standards and Health Aspects
of Large-Scale Use of Atomic Energy'' in
Proceedings of the International Con-
ference on the Peaceful Uses of Atomic
Energy, Vol. 13 (United Nations, New
York, 1956) pp. 263-393.
2U. ''Environmental Aspects of the Large-
Scale Use of Atomic Energy'' in Proceed-
ings of the Second United Nations Inter-
national Conference on the Peaceful Uses
of Atomic Energy, Vol. IS (United
Nations, Geneva, 1958) pp. ^45-624.
21. 1'Safety Aspects of Large-Scale Use of
Atomic Energy'' in Proceedings of the
Third International Conference on the
Peaceful Uses of Atomic Energy, Vol. 14
(United Nations, New York, 1965) pp. 5-
216.
22. Preston, A.. ''Site Evaluation and the
Discharge of Aqueous Radioactive Wastes
from Civil Nuclear Power Stations in
England and Wales" in Disposal of Radio-
active Wastes into Seas, Oceans, and
Surface Waters (International Atomic
Energy Agency, Vienna, 1966) p. 725.
23. Dunster, H. J., A. W, Kenny, W. T. L.
Neal and A, Preston, ''The British
Approach to Environmental Monitoring''.
Nuclear Safety 10, 504 (1969).
24. ''The Treatment of Radioactive Wastes'',
in Proceedings of the Second United
Nations International Conference on the
Peaceful Uses of Atomic Energy, Vol. 18
(United Nations, Geneva, 1958) pp. 3-240.
25- ''Radioactive Waste Management'' in
Proceedings of the Third International
Conference on the Peaceful Uses of Atomic
Energy, Vol. 14 (United Nations, New
York, 1965) pp. 219-280.
26. Straub, C. P., Low-level Radioactive
Wastes (U.S. Gov't Printing Office,
Washington, D.C., 1964).
27. Mawson, C. A., Management of Radioactive
Wastes, (Van Nostrand Co., Inc., Prince-
ton, 1965).
28. ''Management of Radioactive Wastes at
Nuclear Powe,r Plants'', Safety Series
#28 (International Atomic Energy Agency,
Vienna, 1968).
29. Blomeke, J. 0. and F. E. Harrington,
''Management of Radioactive Wastes at
Nuclear Power Stations'', AEC Rept.
ORNL-4070 (1968).
30. Stolzenbach, C. F,, ''Current Practices
in the Disposal of Waste Radioactive
Gases from Nuclear Reactors'', Nuclear
Safety 6, 436 (1965).
31. Klement, A. W,, Jr. and V. Schultz,
''Terrestrial and Freshwater Radio-
ecology: A Selected Bibliography", AEC
Rept. TID-2910 (1962) and supplements 1 -
5 (1963-1968).
32. Agricultural and Public Health Aspects of
Radioactive Contamination in Normal and
Emergency Situations (FAD, WHO, and IAEA,
Rome, 1962).
33. Slade, D. H., Ed., ''Meteorology and
Atomic Energy, 1968", AEC Rept. TID-
24190 (1968).
34. Aberg, B. and F, P. Hungate, Eds.,
Radioecological Concentration Processes
(Pergamon Press, New York, 1967).
35. Russell, R. S., Ed,, Radioactivity and
Human Diet (Pergamon Press, New York,
1969).
36. Hungate, F. P., Ed., ''Radiation and
Terrestrial Ecosystems", Health Phys.
11, 1255 (1965).
37. Eisenbud, M., Environmental Radioactivity
(McGraw-Hill, New York, 1963).
3
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38. Tamplin, A. R. , et al,, ''Prediction of
the Maximum Dosage to Man from the Fall-
out of Nuclear Devices'AEC Rept.
UCRL-5U163, Parts 1-IV (1967-8).
39. Mawson, C, A., Ed., 1'USAEC Meteoro-
logical Information Meeting, Sept. 11-14,
1967", AEC Rept. aECL-2787 ( 1967).
40. Schultz, V. and A. W. Klement, Jr., Eds.,
Radioecology (R^inhold, New York, 1965).
41. .Joint Committee on Atomic Energy, Con-
gress of the United States, ''Federal
Radiation Council Protective Action
Guides'', U.S. Gov't Printing Office,
Washington, D.C. (1965).
42. Joint Committee on Atomic Energy, Con-
gress of the United States, ''Fallout,
Radiation Standards and Countermeas-
ures'', U.S. Gov't Printing Office,
Washington, D.C. ( 1963).
43. Polikarpov, G. G., Radioecology of
Aquatic Organisms (Reinhold, New York,
1966).
44. Honstead, J. F., ''A Survey of Environ-
mental Dbse Evaluations", Nuclear Safety
9, 383 (1968).
45. Barton, C. J., ''Environmental Con-
tamination Around Nuclear Facilities'',
Nuclear Safety 4, 92 (1962)*
4
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2. RADIONUCLIDES IN LIQUIDS ON SITE
2.1 Samples
2.1.1 Collection. Radionuclides were
measured in primary coolant, fuel pooL, and
contaminated demineralized water to identify
them in a relatively concentrated state, and
to compare concentrations on site and in
effluents. The first sample of primary
coolant water was obtained at the water
sampling port of the primary steam drum on
February 1, 1968. On August 22, 1968, two
more samples of primary coolant water (one
acidified to 0.6 N in HC1 to reduce radio-
colloidal losses), one sample of fuel pool
7.3 x |
'
PRIMARY STEAM
1.4 x 1 O4 kg/hr
water, and one of contaminated demineralized
water were obtained. Dresden staff provided
1-liter volumes of all samples in poly-
ethylene bottles.
2.1.2 Primary coolant. This sample is
representative of 1.9 X 105 liters (50,000
gal) of low conductivity demineralized water
that circulates as shown in the simplified
schematic drawing of Figure 2.1* In brief,
steam is generated in the reactor and the
secondary steam generators, produces me-
chanical energy for generating electricity
in passing through the turbines, and is
then condensed for recirculation. Material
kg/hr
OFF GAS
TURBINE
SECONDARY
STEAM
GENERATOR
CONDENSER
DEM IN ERA LIZER
WATER VOLUME
PRIMARY SYSTEM: 190,000 kg
SECONDARY SYSTEM: 4 x 7,700 kg
Figure
2.1. Primary coolant flow schematic.
5
-------
may leave the system during shut-down when
it is opened for refueling or repair, and
during routine operation by the following
paths:
1. Gas flows from condenser air ejectors
through a delay line and two filters in
series to the stack for release; minor
fractions of gas reach the stack from
gland-seal condenser air ejectors through
a delay line, and from leaks to the
ventilating air.
2. Water is removed in the course of blow-
downs, escapes at leaks as steam or
water, and is carried with released gas;
it is recovered and reused except for
high-conductivity liquid waste and water
vapor in the stack effluent.
3. Ionic and solid impurities are removed
in the course of periodic replacement of
the reactor water demineralizers (the
used resins are shipped for burial as
solid waste); weekly regeneration of
condenser-water demineralizers(the
regenerating solution is discharged as
high-conductivity liquid waste); periodic
replacement of filters and low-con-
ductivity-water demineralizers; and blow-
down of each of four secondary steam
generators (the blowdown water is fil-
tered, deminera1ized, and reused).
Fission products enter the primary cool-
ant water from fuel elements through holes
or cracks in the cladding, or from uranium
that was released from failed fuel elements.
Tramp uranium and diffusion through intact
cladding are believed to be minor sources
of fission products.^ At Dresden, much of
the fission product activity in primary
coolant water is attributed to uranium that
had entered the primary coolant several
years previously from failed fuel ele-
ments, ^ Activation products are formed in
the reactor by irradiation—mostly with
neutrons—of air, coolant water, and cor-
rosion products, erosion products, and
water impurities in the coolant.
Radionuclides are removed from the water
in the reactor vessel by radioactive decay,
deposition on surfaces and accumulation as
"crud" in recesses, ion exchange and
filtration on the reactor-water demineral-
izer, and carryover with steam to the
turbines and condensers. At the condenser,
most non-gaseous radionuclides, including
the particulate decay products of the
radioactive gases that are formed as the
gases are carried from reactor to con-
dense rs, remain in the condensate. ^ ^'
Accumulation occurs in the condenser-water
demineralizer and secondary-steam-generator
water. Most particulate radionuclides that
are carried with or formed from the gases
decay within the delay line, and others are
flushed from the delay line with condensed
moisture; those that pass through the
delay line are removed on the filters to
the extent of filter efficiencies before
entering the stack. Radioactive gases are
discharged in gaseous effluent at the top
of the stack, together with particulate
radionuclides that (a) are descendants of
these gases and have been formed after
filtration, (b) penetrated the filters, and
(c) are carried in unfiltered gas streams
(i.e., ventilating air and gland-seal
condenser off-gas).
2.1.3 Fuel storage pool. j^e pool
contains 3.8 * 105 1iters' (100,000 gal) of
demineralized water, and is an independent
system during reactor operation. The water
is circulated through a filter to remove
suspended material and insoluble radio-
nuclides. Longer-lived fission products
leached from the stored fuel elements either
circulate in the water, are filtered, or
deposit in the fuel pool system.
When the reactor is being refueled, the
refueling canal is flooded with demineral-
ized water to combine the reactor vessel,
the refueling canal, and'the fuel pool into
a single body of water. Water from the
bottom of the reactor vessel is continuously
blown down to the radioactive liquid waste
treatment system during this operation.
This water is filtered, demineralized, and
returned to the refueling canal. The gross
radioactivity concentration in fuel pool
water is maintained below 1 X 10pC/ml by
Dresden.
2.1.4 Contaminated demineralized water
Approximately 7. 6 * 105 liters (200,000
gal) of water that has been reprocessed is
stored for reuse. This water enters the
storage tank by being rejected from the
6
-------
demineralized condensate water when the
water level rises in the condenser hot well,
or by transfer of filtered and demineralized
liquid radioactive waste.
2.2 Analysis
2.2.1 Gamma-ray spectrometry. Radio-
nuclides that emit gamma rays were identi-
fied and quantified in sample aliquots by
multichannel spectrometry with a Ge(Li)
detector, as shown in Figures 2.2 and 2.3.
Decay measurements with eight spectra
obtained from 0.5 to 150 days after sample
collection were used to measure long-lived
radionuclides without interference by short-
lived ones and to confirm identification by
gamma-ray energies. The minimum half life
of radionuclides detected by this procedure
was 6 hours, and the maximum, 30 years.
Mi nimum detectable concentrations at these
half 1 ives were approximately 5 * 10 * and
1 X 10~^ microcurie per milliliter (^Ci/ml),
respectively.
2.2.2 Alpha-particle spectrometry. Radio-
nuclides that emit alpha particles were
analyzed in evaporated aliquots by spec-
trometry with a Si-diode detector, and
quantified with a proportional counter.
Only a single alpha-particle group at
6.11 ± 0.02 MeV could be definitely identi-
fied in the primary coolant; this was
attributed to 242Cm.
2.2.3 Radiochemistry. All of the expected
radioelements except rhodium and curium were
separated chemically and then measured with
appropriate radiation detectors. Radio-
chemical analysis confirmed spectral identi-
fication by gamma-ray energy and half life,
was more sensitive than instrumental analy-
sis by itself, and provided values for
radionuclides that emit no gamma rays, or
whose gamma rays were obscured in the
spectra. Thus, ®^Sr and ^®Sr were measured
with a low-background G-M counter, tritium,
with a liquid scintillation counter after
distillation, and ^Fe, with a xenon-filled
proportional counter plus spectrometer.
Radionuclides that emit gamma rays were
measured after chemical separation with a
Nal(H) detector plus spectrometer. Aliquots
°f 10-20 ml were usually analyzed. Because
of improved techniques, results for the
primary coolant sample of August 22 are
more precise than for the earlier sample.
2.3 Results and Discussion
2.3.1 Radionuclides in primary coolant.
Most high-yield fission products with half
lives of 6 hours or longer were identified
and measured, as well as activation products
with high (n,y), and (n,p) cross-sections
in water, steel, Zircaloy, copper, and
silver (see Table 2.1). The short-lived
radionuclides at highest concentration were
135I and 99mTc; the longer-lived (ty >1
week) radionuclides at highest concentration
were 13*1 and ^8Co. The radionuclides ^Fe,
82Br> 115mca, and 127Sb were not detected at
levels of 1 X 10-^ /-/Ci/ml, and 32P was less
than 1 X 10"^ /£i/ml,
The sum of measured radionuclide con-
centrations was 0.4 /^Ci/ml on February 1 as
compared to 0. 13 /jCi/ml on August 22, and
most individual radionuclides in the later
sample were at lower concentrations. The
lower concentrations could have resulted
from the shorter operating period since
the preceding partial refueling (see Figure
2.4), from better-clad fuel elements added
at the fifth partial refueling, or from
cleanup of the primary coolant system in the
interval. The activation product analyses
confirm earlier reports for Dresden, •4»^ )
and for a similar reactor at Garigliano,^^
except that measured concentrations are
somewhat higher. The earlier reports also
gave values for the short-lived radio-
nuclides 1.8-hr 18F, 2.6-hr ^5Ni, 2.6-hr
^Mn, and 0.9-hr 134I; these were not found
in this study because of the relatively long
time interval between sampling and analysis.
Tritium was not reported in the earlier
studies. Tritium concentrations of 7 X 10"^
and 3 X 10~3 /iCi/ml in 1965(5•8) were some-
what higher than given here. The presence
of 242Gt> had not been reported, but it was
predicted as the alpha-emitting trans-
uranium radionuclide with the highest decay
rate in fuel after reactor operation for 1
to 2 years. ^
2.3.2 Radionuclide losses in samples.
The walls of the polyethylene bottles re-
tained detectable amounts of the radio-
nuclides from unacidified primary coolant
7
-------
Table 2.1
Radionuclide Concentration in Primary Coolant*
Concentration, ^Ci/inl
Radionuclide
Feb. 1, 1968 Aug. 22, 1968
from fuel
51 -d
89Sr
1.2
X
q-4
4.4
X
0-5
28 -yr
90Sr
1.2
X
0-5
t.3
X
0-B
9.7 -hr
91Sr
2.4
X
0"2
1.2
X
0"2
10.3 -hr
9 3 y
-7
X
O-3
-2
X
0-3
65 -d
952 r**
9
X
0-4
2.4
X
0-5
17 -hr
97£ r**
1.0
X
0"2
1.3
X
0-4
35 -d
95Nb**
5
X
0"4
1.8
X
0-5
66.3 -hr
"Mo**
1.4
X
q-3
1.4
X
O-3
6.0 -hr
99mjq**
9.0
X
0-2
4.4
X
o-2
39.7 -d
03Ru
5
X
0-4
5.6
X
0-5
1.0 -yr
06Ru
NM
1.3
X
0-6
36 -hr
05Rh
X
0"3
X
q-4
78 -hr
32Te
8
X
q-4
1.9
X
0-5
8.06—d
3' 1
7.8
X
q-3
2.2
X
0-3
20.9 -hr
331
6.6
X
0-2
2.3
X
o-2
6.7 -hr
351
1.3
X
0"1
3.6
X
O-2
2.07-yr
34Cst
1.3
X
0-5
2.3
X
0-5
13 -d
36CS+
3
X
0-5
2.4
X
0-5
30 -y r
37Cs
3
X
0-5
4.4
X
0-5
12.8 -d
40Ba
1.4
X
0"3
1.0
X
0-3
32.5 -d
41Ce
9
X
0-4
4.4
X
I]"5
33 -hr
43Ce
3.2
X
0"3
1.0
X
0'4
284 -d
44Ce
3
X
0-4
8.0
X
0-6
11 -d
47Nd
3
X
0"4
-3
X
0-5
2.34-d 239NpT
2.1
X
o*2
4.1
X
0-3
163 -d 242CmT
2.2
X
0-7
1.2
X
Q*7
from water, cladding,
and construction materia
s
12.3 -yr
3hT
1.7
X
0-3
1.3
X
0-3
15.0 -hr 24Na
3.0
X
0-3
1.6
X
A'3
27.8 -d
51Cr
NM
X
0"4
313 -d
54Mn
NM
1.6
X
0-6
2.7 -yr
55pe
9.5
X
0-5
4.0
X
0"5
270 -d
57C0
~1
X
0-5
1.6
X
0-6
71 -d
5eCo
1.4
X
O-2
1.7
X
0-3
5.26—y r 80Co
2.2
X
q-3
2.6
X
0"4
12.7 -hr
84Cu
X
0-2
2.2
X
0-3
244 -d
85Zn
NM
4.0
X
0-6
253 -d n0fflAg
NM
1.9
X
0-6
115 . -d
iB2Ta
2
x 10"5
~7
X
0-7
'"Concentrations at time of sampling.
**Also activation products.
^Formed by (n,y) reactions with uranium or fission products.
fAlso from ternary fission.
NM: not measured
8
-------
1(T
10 -
I02 -
10' -
S3
o
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10°
1 _ 11—69 ( 1,000 mi/1.)
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U3
X
X
1
X
X
X
X
X
800 850 900 950 1000 1050 1100 1150 1200 1250 1300 1350 1400 1450 1500 1550
CHANNEL (1.005 keV/channel)
Figure 2.3. Gamma-ray spectra of primary coolant water, 805-1,608 keV. Same sample
and detector as in Figure 2.2.
FOURTH PARTIAL
REFUELING
PIPING
INSPECTION
FIFTH PARTIAL
REFUELING
MAXIMUM
220
200
2 180
160
140
120
100
80
60
40
20
0
1.4-1 11..
V.'/.'.'I'Ja!.
MAY JUNE JULY AUG SEPT OCT NOV DEC JAN FEB MAR
1967 1968
APR MAY JUNE JULY AUG
1968
Figure 2.4. Dresden electrical loading. May 1967 to August 1968 (from annual reports
of station operation for the years 1967 and 1968 by Dresden Nuclear Power
Stat ion).
10
-------
and A are summarized in Appendix B.1. This
is a simplification in that the calculation
ignores (n,y) reactions that link some
fission-product chains, and production of
some of these nuclides by activation of
material in the coolant water (see Table
2.1). Moreover, the actual power varied
considerably, and some values of Y are
doubtful. Note that the concentration of a
fission product in the fuel is proportional
to A only if the half life is long compared
to the irradiation time; for other fission
products, relative concentrations are less
because their radioactive decay rates ap-
proach or equal their generation rates.
The rate of turnover of fission products
in the primary coolant, R, in /iCi/sec, is
related to the measured concentration, C,
in }£.i/ml, by:
R ~ C ^7- X V ml X (A., + kt ) sec"
ml decay turnover'
(2.2)
where V is the volume of coolant (1.9 X
10® ml) and ^turnover is the turnover
constant for ions in the reactor-water de-
minerali zer
^14 h r
1
= 2.0 X 10"5 sec"1
X 3600 sec/hr
Values of R for the August 22 sample are
given in Appendix B. 2.
The turnover rate,.R, can be taken to be
equal to the rate of transfer from the fuel,
except for the following limitations:
1» It is an instantaneous value and does not
account for changes in concentration;
2. Other sources, such as release of radio-
nuclides from ''crud'', are not con-
sidered;
3. The turnover rate, based on the flow rate
through the reactor demineralizgr shown
in Figure 2.1, is appropriate to the
time of sampling, but may vary from
10,000 to 50,000 kg/hr;^moreover,
fission products that are not completely
retained by the demineralizer have
effective turnover times that exceed the
turnover time of the water.
)
4. Turnover of insoluble and volatile
fractions is not taken into account.
The ratios of turnover rates in the primary
coolant to generation rates in fuel, R/A,
(see Appendix B,2) range from the maximum
7.7 X 10~6 for 137qs the minimum 1,5 X
1Q"9 for i32Te. The radionuclides that are
expected to be least soluble in the coolant
water—Ce, Y, Nd, Zr, Nb, and Te-—have the
lowest ratios, below 4 X 10~®, These radio-
nuclides probably are mostly—i.e., 90 to
99.9 percent—in ''crud''. That longer-lived
isotopes generally show higher R/A ratios is
attributable to their greater accumulation
in the fuel, which would result in higher
transfer rates to the coolant.
2.3.4 Generation rates of progeny of
gaseous radionuclides in coolant. The
fission products ®^Sr, ^®Sr, ^Sr, 13^Cs,
and 140Ba enter the primary coolant at
least partially by decay of.gaseous pre-
cursors in the coolant within the reactor.
All are granddaughters of short-lived
gaseous radionuclides with short-lived
daughters except 13^Cs, which is the
daughter of a short-lived gaseous radio-
nuclide. The precursor gases enter the
coolant from the fuel, decay partially in
the reactor vessel, and then are carried in
steam to the turbine.
Rates of formation of the descendants
of these gaseous radionuclides within the
reactor vessel could be computed if the
transfer rate of the gases into the coolant
and the fractional decay of the gases in
the reactor vessel were known. The transfer
rates of radioactive krypton and xenon
have been observed to lie between two
extremes. An ''equilibrium mixture'' (time
of production and transfer at least one
month so that all noble gas fission products
except 10.7-yr have reached equilib-
rium) results from cladding with micro-
scopic defects;^1) a ''recoil mixture''
(immediate transfer after formation) is
associated with fuel that is in direct con-
tact with coolant. The intermediate
state is termed ''diffusion mixture'' and
has been taken(4,10) to be proportional to
A.0,5. Ac cording to current opinion, the
intermediate state represents the combined
effect of equilibrium and recoil situations,
11
-------
rather than a distinct transfer mechanism,
although calculations based on bulk transfer
mechanism predict the dependence on d)
At Dresden, the rate of transfer of each
gaseous radionuclide from fuel, Rj^j, in
/iCi/sec, has been related empirically to a
nominal gaseous fission product release
rate, N, in fJZi/sec, by: ^
R
di f
4.0 x io2 X Y X >l0*5 x N
(2.3)
N is the sum of release rates computed for a
diffusion mixture of the six radionuclides
85mKr, 87Kr, 88Kr, 133Xe, 135Xe, and 138Xe,
as shown in Appendix B.3. Dresden reports a
value of N daily on the basis of a gamma-
ray measurement of an off-gas sample.
The generation rate of the non-gaseous,
relatively long-lived, progeny of the gases
in the reactor vessel, R^, in /uCi/sec, is:
R = R.- ,, , X f X K/k
P dif(g) p' g
(2.4)
where the subscripts p and g refer to
progeny and gases, respectively, and f is
the fraction of gaseous precursor decaying
in the reactor vessel in approximately 10
seconds, as given for Dresden.Values of
Rd>f, f, and A. are tabulated in Appendix
a 3.
The generation rates (Rp), predicted
coolant concentrations, and ratios of the
generation rate from gas to the total trans-
fer rate to the coolant based on concentra-
tion measurements for the August 22 sample
(Rvalues in Appendix B.2, N = 11,600
/jCi/sec) are:
Predicted
Radio-
concen-
VR
nuclide
R,
P
trations
89Sr
0.027
/jCi/sec 7
X 10*6 /£i/wl 0.16
9°Sr
0.00024
6
X 10*8
0.049
91Sr
6.0
8
X 10"4
0.066
*37Cs
0.00018
5
X 10*8
0.0011
14%a
0.14
4
X 10"5
0.035
TTie small ratios of predicted to measured
values suggest that, at Dresden, the recoil
mechanism yields higher transfer rates to
the coolant for these very short-lived
gaseous precursors than is indicated by the
diffusion mixture, or that decay of gaseous
precursors in the coolant accounts for only
a small fraction of these radionuclides in
the coolant.
2.3.5 Turnover rates of gaseous radio-
iodine. Transfer rates of gaseous radio-
iodine into the primary coolant in a dif-
fusion mixture also can be estimated with
equation 2.3 and the values of Y and A. for
131i, 1 33j^ ancj 135j
given in Appendix B. 1.
The estimated transfer rates and ratios of
the estimated rates to turnover rates based
on concentration measurements on August 22
(R value in Appendix B.2) are:
Radionuc 1 i d e
R
di f
R
di f
/R
131I 130 /xCi/sec 15
133I 920 7.3
135I 1,500 4.5
That estimated rates were appreciably higher
than measured rates suggests that the radio-
iodine does not pass from the fuel as
rapidly as the noble gases. Hie possibility
that most of the radioiodine does not remain
in the aqueous phase was eliminated by the
observation that only a small fraction of
131I is in stack and liquid effluents (see
Sections 3.3.3 and 4.3.3).
Ratios of turnover rates (computed ac-
cording to equation 2.2) for the three
radioiodine isotopes relative to 13*1 com-
pare as follows with theoretical ratios for
the three types of mixtures:
Measured Ratio Predicted Ratio*
x?
.^5
o*
,*v
. o
&
/
.V
/
*
13 lj
133j
135j
1.0
1.0
1.0
1.0
1.0
12
39
14
38
2.2
2.1
6.8
11
21
60
~equilibrium rate = kY, where k is a constant
diffusion rate = kY\®*^
recoil rate = kY\
The two sets of ratios of transfer rates
computed from measured concentration agree
12
-------
with each other within the errors of meas-
urement. They fall between ratios for dif-
fusion and recoil mixtures, supporting the
observation that the recoil mechanism may
predominate.
To place this value in perspective, the;
average observed release rate was one-
fourth of the rate computed for R^ ^ of ®^Kr
(see Table 4.2), whose half life is similar
to that of tritium.
2.3.6 Formation and turnover rates of
tritium. The rate of turnover of tritium in
the primary coolant, computed by equation
2.2 but using the turnover constant for
demineralized water at Dresden instead of
the turnover constant for ions in the
reactor-water demineralizer, is
R = 1 X 1(T3 X 2 X 109 ml
* (1.78 x 10"9 + 2.8 X 10"8) sec*1
= 6 X 10" 2 yuCi/sec
The calculation is based on the presence of
approximately 2 X 106 liters of contaminated
demineralized water and a release rate of
1.45 X 10^ liters per month at Dresden,^)
and an average tritium concentration of
1 X 10'3 /xCi/ml, based on the values in
Tables 2.1 and 2.2. The release rate is de-
rived from the assumption that most demin-
eralized water is released as high-conduc-
tivity liquid waste (i.e., release in stack
effluent is relatively small), and that this
waste is comprised mostly of contaminated
demineralized water. The ratio of con-
taminated demineralized water on site to
the release rate of high-conductivity
liquid yields a turnover period of 420 days,
hence, a turnover constant of 2.8 X 10 8
sec " 1,
Equation 2.3 was used to indicate Rj-f
for comparison with the turnover rate,
although the rate of transfer from fuel thus
calculated may be appreciably in error:
tritium may leave the fuel more rapidly than
other gases because of its smaller molecular
size, but is too long-lived to have reached
a constant transfer rate. The calculation
yields, for 3H from ternary fission:
Rdif = 4.0 X 102 X 9.5 X 10"5
X (1.78 X 10"9)0'5 X 11,600
= 0.02 /JCi/sec
The D(n,'y)T reaction in coolant water
within the reactor is probably the main
source of tritium in the primary coolant. ^
Hie formation rate by this activation pro-
cess is computed according to:
R.et "t>2VK
(2.5)
based on the following values:
4>, average neutron
flux^D 3.x X 1013 n/cm2 sec
2, macroscopic ther-
mal neutron cross-
section
normal deuterium
content of hydro-
gen 1.5 X 10-4 atom/atom
hydrogen content
of water 0.11 g/g
water density at
290°C and 1,000
0.74 g/cm3
i-9
psi(12)
water (non-void)
fraction in
cored3^ 0.88
microscopic cross-
sectiond4) ¦ 0.57 X 10~27 cm2/atom
(2 = 6.02 X io23 x 1.5 X 10"4 x o.ll x 0.74
X 0.88 X 0.57 X 10"27
= 3.7 X 10*y cm'
V, water volume in
reactor core^D ^05 X 10 7 cm3
<{, tritium decay con-
stant 1.78 X 10_9 sec"1
Thus,
Ract- 3.1 x io13 x 3.7 x io-9 x 1.05 x io7
x 1.78 x io-9 x (3.7 x io4)-1
= 0.06 /JCi/sec
Most of the Values used to compute the
above rates are approximate; thie deuterium
content-of the water would be expected to
13
-------
be higher than indicated because of the
H(n,y)D reaction, for example.
Although the sum of the two predicted
rates, 0.02 + 0.06 = 0.08 ffCi/sec, is not
far from 0.06 /-Ci/sec based on water turn-
over, one or both of the predicted rates
may be too high, since boron in the control
rods may also be a source of tritium in
primary coolant water. ^ The total rate,
however, is confirmed by the measured re-
lease rate of tritium in liquid waste
(0.05 yuCi/sec, see Section 3.3.3).
2.3.7 Turnover rate of activation prod-
ucts in primary coolant. The turnover rates
of activation product radionuclides with
half lives longer than 1 week were computed
with equation 2.2 and are listed in Appendix
B. 4. These rates were computed for com-
parison with release rates (see Sections
3.3.3 and 4.3.2). The rates apply only to
the August 22, 1968 sample, and are subject
to the same limitations discussed for
fission products (see Section 2.3.3).
2.3.8 Radionuclides in fuel pool and
contaminated demineralized water. Only long-
lived radionuclides were found in these two
samples (see Table 2.2). Tritium was the
Table 2.2
Radionuclide Concentrations in
Fuel Pool Water and Contaminated
Demineralized Water, August 22, 1968*
Radionuclide Concentration,
pCi/ml^
Radionuclid
e Fuel Pool Water
Demi ne ra t i zed
Water
3H
880
930
54Mn
6
< 0.1
50Co
IB
1.2
boqo
74
2.0
B9Sr
2
< 0.2
90Sr
18
0.2
,3
2.4 References
1. Gilbert, R. S., Gensral El ectric Co.,
personal communication,
2. Kiedaisch, W, and R, Pnvlick, Dresden
Nuclear Power Station, personal com-
munication,
3. Brutschy, F. J,, R. S, Gilbert, and
R, N» Osborne, ''The Behavior of Cor-
rosion Products in Boiling-Water Reac-
tors'', in Proc, Conf. on Corrosion of
Reactor Materials, Salzburg, 1962, Vol.
1 (IAEA, Vienna, 1962), p. 133.
4. Gilbert, R. S.. ''Sources and Disposi-
tion of Radioactive Liquid and Gaseous
Effluents from the Dresden Plant",
General Electric Co, Rept. APED—4461
(1964).
5. Blomeke, J. 0. ^nd F, E, Harrington,
''Management of Radioactive Wastes at
Nuclear Power Stations'', AEC Rept.
ORNL-4070 (1968).
6. Blomeke, J. 0, and F, E, Harrington,
''Waste Management at Nuclear Power
Stations", Nuclear Safety 9, 238 (1968)•
7. della Rocca, C,, "System Chemistry of a
Large BWR", Nucleonics 24, #2, 39 (1966).
8. Smith, J. M,, Jr., ''The Significance of
Tritium in Water Reactors'', General
Electric Co., San Jose, Calif, (1967).
9. Arnold, E, D., Oak Ridge National Labora-
tory, Oak Ridge, Tenn., unpublished
tables.
14
-------
10. Smith, J, M,, *'Release of Radioactive
Waste to Atmosphere from Boiling Water
Reactors'', General Electric Co., San
Jose, Calif. *.1960).
11. Reactor File #8, ''Description of
Dresden'', Nucleonics 17, #12( 69 (1959).
12. El-Wakil, M. M., Nuclear Power Engineer-
ing (McGraw-Hill, New York, 1962) p« 534.
13. Wade, 1. L., Commonwealth Edison Co.,
Letter to Division of Reactor Licensing,
AEC, Sept, 6, 1961• Docket 50-10-36«
14. Kaplati, L, et a I., ''Thermal Neutron
Absorption Cross Section of Deuterium'',
Phys. Rev. 87, 785 (1952).
-------
3. RADIONUCLIDES IN LIQUID WASTE EFFLUENTS
3.1 Samples
3.1.1 Col lection. Samples of high-con-
ductivity (high salt content) liquid wastes
were collected by Dresden staff in 1-liter
polyethylene containers from the 5000-gal
waste tank^D on November 12, 1967, January
13, 1968, March 16, 1968, June 25, 1968 and
August 20, 1968. The liquid waste was
circulated by pumping during sampling in
accord with routine sample collection
procedure at Dresden. Samples of laundry
waste were collected by Dresden staff from
the 1000-gal Laundry Waste Tank^^ on
January 15 and March 12, 1968.
Radioactive ions were collected for
analysis from the cooling-water intake and
discharge canals by passing the water
samples through ion-exchange columns as
follows:
Collec-
Date,
1968
Sample
Volume,
liters
tion
period,
hours
Hardness
as CaCOj
mg/liter
Jan.
discharge
40
18
360
17-18
intake
48
21.5
June
discharge
65
16
160
25-26
intake
65
16
Aug.
discharge
153
1.5
200
20
intake
131
1.5
Intake water was pumped from the point of
entrance into the plant; discharge water
was pumped from the sampling station,
approximately 100 m beyond the point of
release of liquid wastes into the cooling-
water discharge canal. For the first two
sets of samples, water was passed contin-
uously through the column during sampling;
for the third set, water was first collected
in 55-gal drums and then passed through
the columns. The initial flow rate of
100 ml/min decreased gradually until the
flow stopped in the first two sets of
columns, but was maintained for the third
set. The second and third samples were
collected well within the 2-day periods
during which high-conductivity waste was
being discharged from its tank. The first
sample was collected near the beginning of
this period, and near the end of the period
of release of another batch of liquid
waste. ( ^)
One-liter aliquots of water were col-
lected at the time of sampling to measure
tritium, and hardness as CaOOj. On November
15, 1967, additional samples were collected
for tritium analysis in the Illinois River
at Dresden Dam, 1.5 km downstream from the
cooling-water canal discharge, and in the
Kankakee River, 0.8 km upstream from the
cooling-water canal intake.
3,1.2 Liquid wastesAlmost all of the
radioactivity released to the Illinois
River by Dresden is in the high-conductivity
liquid waste. The waste is a mixture from
several sources including cleaning opera-
tions and laboratory discharges; the main
constituent is spent solution (NaOH, H2904,
and demineralized wash water) from regen-
erating the mixed-bed ion-exchange resin in
the condensate demineralizer. The waste
solution is at pH'11-12, and is filtered
prior to collection in the liquid waste
tank, so that insoluble radionuclides are
transferred to solid radioactive waste. The
waste sampled on August 20, however, was
not filtered because the filter was broken.
17
-------
Liquid waste is discharged at rates up
to 10 Liters/min (2.7 gal/min), into the
coolant-water discharge canal which has a
flow rate of 630,000 liter/min ( 166,000
gal/min). The waste is usually discharged
as the tank becomes full, but additional
tanks are available if needed. The release
rate is adjusted on the basis of gross beta
activity to maintain gross radionuclide
concentrations in the coolant canal below
selected levels. At the usual release rates
between 5 and 10 liters/min, this waste is
discharged during less than one-half the
operating time, and is diluted approximately
100,000-fold.
The average monthly volume of high-con-
ductivity waste during 1968 was 145,000
liters (38,000 gal). Of the 5 analyzed
samples, 4 were collected during reactor
operation at power levels between 160 and
200 MWe (see Figure 2.4); the March 15
sample was collected during refueling.
The average monthly volume of laundry
waste was 68,000 liters (18,000 gal) in
1968* It is released into the coolant-water
discharge canal when it is necessary to
empty the tank, at a flow rate of 10
1iter/min.
3.1,3 Effluent radioactivity. Concentra-
tions of radionuclides in effluents to
unrestricted areas are limited by the AEC
according to paragraph 20.106 of 10 CFR
20, Concentrations above background in
water, as listed in Appendix B, Table II,
column 2 of 10 CFR 20, are applied at the
boundary of the restricted area. The limit
is 1 X 10*7 i/ml for an unidentified
mixture containing no 12H, 226Ra> or228
and 3 X 10"7 /LiCi/ml for soluble 90Sr or
1 3 1Jf which are usually the radionuclides
in reactor effluent with the lowest limits.
Higher limits are permissible under condi-
tions of subsection (b), or more stringent
limits may be applied by the AEC under
subsection (e) of paragraph 20.106.
At Dresden, concentrations of released
radionuclides are determined by measuring
gross beta concentrations in liquid waste
tanks and applying the dilution factor (the
ratio of canal flow rate to tank discharge
rate) appropriate to the point of release.
In 1968. ''the average contribution to the
unidentified activity in the water utilized
for radioactive waste dilution during the
year was calculated to be 0.189 X 10~7
jjCi/mi" at Dresden.'3^ Concentrations dur-
ing the preceding five years were within a
factor of two of this value, according to
Dresden's annual reports for these years.
3.1.4 Effluent sampler. An apparatus
was designed, tested and used at Dresden
on the three occasions listed in Section
3.1,1 to collect radionuclides in ionic
form continuously from water at the point
of release. A minimum sample volume of 10
liters was considered necessary to obtain a
sensitivity of 1 X 10"^ /iCi/ml (1 pCi/liter)
for each radionuclide that was known to
be discharged. The tested device processed
as much as 150 liters of water.
The apparatus consists of five sections
of ion-exchange resin in a 7,5-cm i.d.
column. Each of the first three sections
contains 350 cc Dowex* 50-x8 (H+, 50-100
mesh) cation-exchange resin; each of the
fourth and fifth sections, 450 cc Dowex l-x8
(CI , 50- 100 mesh) an ion-exchange resin.
The sections are separated by porous plastic
sheets so that they can be taken separately
from the column. A glass wool filter pre-
cedes the first section. The apparatus was
tested in the laboratory with tracer-level
radio-cesium, -strontium, and -cobalt in
150 liters of water with a hardness of 200
mg/liter at a flow rate of 100 ml/min.
More than 90 percent of each radionuclide
was retained by the first cation-exchange
resin section, and more than 99 percent by
the first and second in combination. More
than 90 percent of radioiodine tracer was
retained by the upper anion-exchange resin
section from water that did not contain
oxidizing agents such as chlorine. To
analyze chlorinated water (i.e., drinking
water), sufficient NaHSOj was added to keep
131j reduced as iodide. Thus, under appro-
priate conditions, these tested radionu-
clides can be collected almost completely in
the upper sections, and the appearance of
large fractions in lower sections is a warn-
ing of breakthrough.
•Mention of commercial products does not con-
stitute endorsement by the Public Health Service.
18
-------
3.2 Analysis
3.2.1 Liquid wastes. Samples were usually
divided into two portions—one unfiltered
and one filtered (the second and third
samples through Whatman #42 paper, the
fourth and fifth, through a membrane filter)
—for analysis. The high-conductivity waste
of November 12 and both laundry wastes,
however, were not filtered. Ten-ml aliquots
were evaporated to dryness on planchets to
determine gross-beta concentrations with
low-background (1 count/min) beta-particle
counters, and gross-alpha content with
proportional counters. Radionuclide analyses
were performed by gamma-ray spectrometry
with Ge(Li) and Nal(Tl) detectors, and by
chemical separation and subsequent counting
as described in Section 2.2. All radio-
nuclides observed by gamma-ray spectrometry
(see Figure 3.1) had half lives longer
than 1 week, hence chemical analysis was
restricted to the longer-lived radionuclides
that are expected to be in these samples.
Concentrations were measured within ± 1
pCi/ml for high-conductivity waste, and
± 0.1 pCi/ml for laundry waste.
3.2.2 Coolant-canal samples. The five
sections of ion-exchange resin in each
column were separated for analysis, and
each section was washed with distilled water
to remove silt. Each section was analyzed
spectrometrically with a 10 X 10 cm cyl-
indrical Nal(Tl) gamma-ray detector, as
shown in Figures 3.2 (top cation-exchange
resin) and 3,3 (upper anion-exchange resin).
Anion-exchange resin sections that appeared
to contain were measured again after
1-week intervals so that gamma spectral
identification could be confirmed by the
decay rate of the gamma-ray peak. Each
cation-exchange resin section was placed
separately into a small column and the
cations were eluted from the resin with
1.2 liter 6 N HC1. Aliquots of the elutriant
were analyzed for radio-cesium, -strontium,
103
102 -
131^ 1400a
364 438
!37cs
"'"CM u0,
605 i ,4ULa
752
1M|Sl
1498 11
U0U 140La M0La
815 868 919
M,. 925
^<58q0
B10
10° J
10-1 u
1596
0 100 200 300 400 500 600 700 800
600 900 1000 1100 1200 1300 1400 1500 1800
CHANNEL (1.01 keV/channel)
Figure 3,1. Gamma-ray spectrum of high-conductivity waste solution. Detector: Ge(Li),
6 cm2 x 7 mm. Sample: iOO ml collected Jan. 13, 1968. Count: Jan. 19
(50 min.).
19
-------
50
10 ¦
DISCHARGE
cr
=)
o
CJ
INTAKE
0.1
-------
100
in
CJ
oo
in
> /•
iW \
10
DISCHARGE
1.0
INTAKE
BACKGROUND
0.
6 2.0 2.4 2.8
C 0.4 0.0 1.2 1.
ENERGY, MeV
Figure 3.4. Gamma-ray spectra of suspended
silt in intake and discharge
coolant-water canals. De-
tector: 10 x 10 cm Nal(Tl).
Samples: 3.2 g dried silt from
intake and 4.4 g dried silt
from discharge collected Aug.
20, 1968 at 1630-1800 dfT.
Counts: Sept. 9 (100 min.).
total calcium eluted
. , from resin
Liters of water = calcium/liter of
water sample
(3. 1)
In the third set of samples, the computed
volume was confirmed by direct measurement.
The tritium content of the water samples
was determined by distilling the water and
analyzing 5-ml samples of the distilled
water with a liquid scintillation counter
that had been adapted to measure concentra-
tions as low as 0.2 pCi/ml*.
3.3 Results and Discussion
3.3.1 Radionuclide content of liquid
wastes. The average concentration of all
*We thank Dr. A. A. Moghissi, Southeastern
Radiological Health Laboratory (SERHL), BRH,
EHS, PHS, DHEW, for analyzing these samples.
' Il_L '
o J-
00 ~
. co
a "
a
u
o O
J?
« s
DISCHARGE
u o
eo *«r
o
u
10
CO,
CO
e:
o
o
UJ
INTAKE
O
1 'V
BACKGROUND-
ENERGY, MeV
Figure 3.5> Gamma-ray coincidence spectra
of suspended silt in intake
and discharge canals. De-
tectors: Two 10 x 10 cm
Nal(Tl) in coincidence, within
5-cm thick annulus in anti-
coincidence. Samples: Same as
in Figure 3,4. Counts: Nov.
19, 1968 (1,000 min.).
detected radionuclides in the five samples
of high-conductivity waste was approxi-
mately 2 X 1U"3 /iCi/ml, as shown in Table
3.1. The radioactive constituents at highest
concentrations were ^H, ^®Co, ^Co, 89Sr,
131j( 134Qgt 137CS) an(j 140gSj jn addition
to the listed radionuclides, traces of
35S, 57c0, 65znt 95zr 9SNb> 106ru> amj
141Q. were observed in one or more samples.
Similar concentrations of the major radio-
active constituents were observed in samples
collected in 1963« ^
The total activity and the concentrations
of individual radionuclides varied con-
siderably among samples. Average values
were used to compute release rates of
individual radionuclides only because better
data (i.e., values measured throughout the
year) are not available. To evaluate the
causes of variability, it would be neces-
sary to segregate waste liquids according
21
-------
Table 3.1
Radionuclide Concentrations in High-conductivity Liquid Waste, pCi/ml*
Radio-
nucli de
Nov.
12, 1967
Jan.
13, I960
March
16, 1968
June 25, 1968
Aug. 20, 1968
Average
3H
900** (NM)
950
(NM)
520
(MM)
770 (NM)
1,100
(NM)
850
54Mn
NM
(< 1)**
NM
(< D
NM
(< 0
NM (< 1)
< 1
(22)
(4)
55pe
NM
(NM)
NM
(NM)
NM
(NM)
NM (45)
NM
(50)
(48)
58Co
NM
(65)
4
(34)
880 (1,800)
3 (85)
18
(260)
230
(450)
60Co
NM
(33)
1
(46)
500
(1,350)
4 (180
11(1,400)
130
(600)
B9Sr
NM
(140)
220
(320)
140
(170)
85 (89)
24
(34)
120
(150)
CO
o
CO
H
NM
(14)
12
(17)
30
(30)
B (9)
9
(11)
15
(16)
9 1Y
NM
(66)
1
(26)
NM
(< D
NM (1)
NM
(< D
(19)
13 11
NM
(5)
6
(6)
NM
(45)
48 (49)
15
(15)
22
(24)
134Cs
NM
(8)
7
(10)
80
(90)
47 (50)
27
(34)
40
(39)
13?Cs
l-
NM
(29)
35
(35)
150
(170)
140(160)
99
(103)
106
(99)
140Ba+
NM
(45)
40
(160)
65
(95)
22 (54)
35
(105)
41
(92)
,4«Ce
x
NM
(5)
NM
(< D
NM
(< O
NM (< 1)
8
(16)
(4)
betaf
NM
(540)
440(1,040)
1,600
(NM)
NM (550)
140
(NM)
alphaf
NM
(< 0.1)
NM
:< 0.1)
NM
(NM)
NM (NM)
NM
(NM)
"¦concentration of radionuclides at indicated date of sampling; 1 pCi/ml - 1 x l(T6 /xCi/ml.
**values without parentheses are for filtered solution, values in parentheses for unfiltered
solution.
"^solutions also contained 90K at concentrations equal to its 90Sr parent; and u0La at concen-
trations 1.15 times those of its ,40Ba parent.
fgross radioactivity measured approximately 1 week after sample collection and not corrected
for decay.
NM: not measured; < values are 3 o- counting error.
to origin. It may be noted that radionuclide
concentrations were relatively high during
refueling (March 16 sample), and that the
tritium concentration in this sample was
only two-fold lower than during reactor
operation. The sample of June 25 may also
have contained waste from refueling.
Gross beta and tritium values in laundry
wastes (Table 3.2) were two orders of magni-
tude lower than in the high-conductivity
wastes. Concentrations of ^H, *>®Co, 60Co,
®^Sr, ^4Cs, and ^7(^s
were all approximate-
ly 1 " 10"fa /£i/ml,
3.3,2 Solubi lity of radionuclides in
high-conductivity waste. As indicated in
Table 3.1, the radionuclides in the sample
were partially removed by filtering. The
unfiltered waste of August 20 had the
highest fraction of insoluble radionuclides,
but even wastes that had been filtered prior
to sampling contained some insoluble radio-
nuclides, Radio-cesium, -strontium, -iodine,
and -barium are in the filtered waste be-
cause they are relatively soluble in alka-
line solutions. Radio-yttrium and -lanthanum
probably were formed after filtration by
decay of their radioactive precursors. Most
other relatively insoluble radionuclides
may represent traces of solids not retained
by the filter. Radiocobalt appears to be
dissolved in complex form initially, but
becomes progressively less soluble on
standing. In tests with ion-exchange resins,
90 percent of the soluble radiocobalt was
retained on cation-exchange resins and
5 percent was retained on an ion-exchange
resin s,
3.3.3 Turnover rate in primary coolant
iis, release rate in liquid waste. Average
release rates of radionuclides in the liquid
waste, E, were computed from the average
concentrations in Table 3. 1 for comparison
22
-------
Table 3.2
Radionuclide Concentrations in
Liquid Laundry Waste,* pCi/ml
Radionuclide January 15, 1968
March
12, 1968
3H
1.3
1.5
5BCo
2.2
1.2
O
C_3
O
CO
2.3
0.6
89Sr
< u.1**
0.9
90Sr
0.1
<
0.1
1 3 11
< 0.1
<
0.1
,34Cs
0.6
<
0.1
,37Cs
3.4
0.8
'40Ba
< 0.1
<
0.1
u,Ce
< 0.1
<
0.1
gross beta
10
5
gross alpha
< 0.1
<
0.1
gross values approximately 1 week later.
**< values are 3 ancj 13?cs
at average concen-
trations of 0.4 and 0.2 X 10*9 /iCi/ml,
respectively, according to Table 3.3; these
were undoubtedly deposited by fallout from
atmospheric nuclear weapon tests. The dif-
ference in radionuclide concentrations
between water in the coolant-water dis-
charge and intake canals is attributed to
radionuclide releases at Dresden. These
values are considerably different from
estimates based on liquid waste releases at
the time of sample collection. The sums of
measured radionuclide concentrations near
the point of discharge (in Table 3.3) com-
pare as follows to estimates based on gross
beta values (or summed radionuclide concen-
trations, excluding 3H, for the August 20
sample) in high-conductivity liquid waste:
Date
Dilution
factor
in canal
Measured
total beta
from
Table 3.3
Estimated
gross beta
from
Table 3.1
January 17-18 62,000 39 pCi/liter 17 pCi/liter
June 25-26 90,000 2 6
August 20 100,000 1 21
Similarly large differences exist for
individual radionuclides.
The higher concentrations measured in the
coolant-water discharge canal on January
23
-------
Table 3.3
Concentration of Ionic Radionuclides in
Coolant-canal Water, pCi/liter*
Radio-
Jan. 17-18,
June 25-26,
Aug. 20,
nuclide
Sample
1968T
1968
1968
O
u
CO
in
di scharge
2.7
< 0.3
0.2
intake
< 0.1
< 0.3
< U.I
60Co
di scharge
1.0
< 0.3
0.2
intake
< 0.1
< 0.3
< 0.1
89Sr
di scharge
7.5 ± 0.5
< 0.1
< 0.2
intake
< 0.1
< 0.1
< 0.2
90Sr
discharge
0.8
0.5
0.5
intake
0.5
0.4
0.3
1311
discharge
17. ± 2
0.8 ± 0.3
< 0.2
intake
< 0.2
< 0.2
< 0.2
134Cs
discharge
1.6
< 0.2
< 0.1
intake
< 0.1
< 0.2
< 0.1
'3?CS
discharge
4.3
0.2
0.2
intake
0.3
0.1
0.1
uoBa
discharge
3.8
0.6 ± 0.3
0.2
intake
0.1
< 0.3
< 0.1
"•concentration at date of sampling; 1 pCi/liter -1x10"9 /zCi/ml.
"^silt not separated from ion-exchange resin in this sample.
Note: l a counting errors are ± o.i pCi/liter or as shown;
< values are 3 a counting errors.
17-18 were traced to an unusual liquid
waste—blowdown water from the secondary
steam generators to which high-conductivity
water had inadvertently been added—that
was released just before the one described
in Table 3.1.^ The lower measured con-
centrations in the two other samples can
be ascribed to radionuclides that were in-
soluble or retained by silt, since these
are not collected on the ion-exchange
resins. Approximately one-half of the
radioactivity other than tritium was in-
soluble in the June 24-25 sample, and 90
percent in the August 20 sample (see Table
3.1). Concentrations of most soluble radio-
nuclides in the liquid waste sampled on
August 20, divided by the applicable dilu-
tion factor, compare reasonably well with
the measured differences in concentration
between coolant canal discharge and intake
water:
/
3?
-------
Measured radiocesium values, however, were
appreciably lower at the point of discharge
than estimated from analysis of the liquid
waste in the tank.
For comparison, gross beta measurements
of composite canal-water samples by the
contractor for environmental surveillance
at Dresden during the first and second
sampling periods are as follows:
Gross beta
Date Location concentration
Jan. 15—21, Discharge canal 6.8 ± 0.8 pCi/liter
1968 Intake canal 3.9 ±0.4
June 23-29, Discharge canal 16.4 ± 1.6
1968 Intake canal 14,0 ±1.2
These values were probably obtained for
samples that had been evaporated and thus
did not retain and other volatile radio-
nuclides, The weekly sampling period may
include several discharges as well as
intervals during which no discharge oc-
curred. The highest difference in weekly
gross beta concentrations between discharge
and intake canals in the first 6 months of
1968 was 13 pCi/liter. ^
3.3.5 Retention efficiency of effluent
sampler. The sample of January 17—18 had
the highest radionuclide concentration of
the three, and therefore provided the best
comparison of retention on the successive
ion-exchange resin sections. Values for the
column in the discharge canal» through
which 40 liters of water had been passed,
were as follows in terms of pCi/liter
influent water:
¦-f /
'•f
>
/
2.7
< 0.4
<0.3
2.7
60Co
1.0
< 0.3
<0.2
1.0
89Sr
7.5
< 0.1
< 0.1
7.5
90Sr
0.8
< 0.1
< 0.1
0.8
13 lj
17.
< 0.2
m m-m
17.
134Cs
1.6
< 0.2
< 0.2
1.6
WCs
4.0
0.3
< 0.1
4.3
U0Ba
3.8
< 0.4
< 0.4
3.8
Ca (mg/liter)120
0.7
0.4
121
The section number refers to anion-exchange
< 1 Q I
resin for I, and cation-exchange resin
for all others. The values indicate that
90 percent or more of each radionuclide
and 99 percent of calcium was retained in
the top column. Such confirmation is im-
portant because either interfering sub-
stances or a difference in the chemical
form of the ion could reduce the retention
efficiency demonstrated in tracer studies.
3.3.6 Insoluble radionuclides suspended
in cooling-canal water. The amounts of
radionuclides washed with distilled water
from the glass wool filter and ion-exchange
resins are given in Table 3.4. Concentra-
tions in water were computed by multiplying
the radionuclide content in the silt by
the grams of silt collected per liter of
water passing through the columns. As in the
case of ionic radionuclides, the 9(^Sr and
in the intake canal are assumed to be
from fallout, and differences between
discharge- and intake-canal values, from
Dresden. Traces of ®^Sr and ^Co in the
intake water may indicate minor contamina-
tion in the intake canal at a time prior to
sampling, or the 8^Sr may have been from
fallout. In addition, the gamma spectra
(Figures 3.4 and 3.5) show the naturally
occurring radionuclides 40K, 226Ra plus
progeny, and 232^ p^us pr0geny in silt from
the intake and discharge canals.
Hie suspended radioactivity was mostly
radiocobalt and radiocesium, and included
some radiostrontium and 140Ba. A consider-
able fraction of the radiocobalt and radio-
cesium in the coolant-water discharge canal
was associated with suspended material, as
indicated by comparing Table 3,4 with Table
3.3. Radiocobalt probably was collected
with suspended material because much of it
was insoluble in the discharged waste (see
Table 3.1). Radiocesium, although entirely
soluble in the waste tank, was probably
retained partially in silt suspended in
coolant-canal water. Two-thirds of the
soluble radiocesium and 95 percent of the
insoluble radiocobalt from the liquid waste
of August 20 remain unaccounted for. These
fractions may have been deposited in the
canal upstream from the point of sampling,
or suspended i"n material that was not
collected by the sampler. An analysis of
mud samples from the discharge canal in
25
-------
Table 3.4
Radionuclide Content of Suspended Silt Collected from Coolant-canal Water
Radio-
nucl i de
June 25-26, 1968*
August 20, 196B*
Samp Ie
pCi/g dried silt pCi/liter water pCi/g dried silt pCi/liter water
58Co
60Co
89Sr
90Sr
131 j
,34Cs
13?Cs
140ga
di scharge
intake
di scharge
intake
discharge
intake
discharge
intake
discharge
intake
di scharge
intake
discharge
intake
discharge
intake
0.9
< 0.1
0.6
< 0.1
0.1
0.1
0.1
0.1
< 0.1
< 0.3
< 0.2
< 0.2
1.1
0.8
< 0.5
< 1.0
0.4
0.2
0.04
0.02
0.04
0.02
± 1
27
1
0.5
0.1
< 3
< 3
1.3
0.2
< 0.3
< 0.3
3.5 ± 0.3
< 0.3
11 ± 1
3
5 ± 2
< 5
0.1
0.7
0.02
0.04
0.005
0.1
0.3
0.07
0.1
~Amounts of dried silt: June 25-26 discharge - 27.6 g/65 liter; intake - 11.1 g/65 liter.
Aug. 20 discharge- 4.4 g/153 liter; intake - 3.2 g/131 liter.
Note: 2 o- counting errors are ± 0.2 pCi/g or as shown; < values are 3 o- counting errors.
1963 showed 0.3 pCi 60Co and 0.6 pCi 13~Cs
per gram, as well as some radionuclides
attributable to fallout, ^ 4)
3.3.7 Tritium concentrations in water.
Concentrations of tritium measured on three
occasions were not significantly higher in
the cooling-water discharge canal than in
the intake or in other nearby samples of
river water, as shown in Table 3.5. It is
improbable that the difference of 0.4
pCi/ml in the two earlier samples is
significant and attributable to Dresden,
The concentration at the point of release
estimated from the average tritium con-
centration of 850 pCi/ml on liquid waste
(Table 3.1) at a dilution factor of 1 X
10 5 is 0.008 pCi/ml during releases of
high-conductivity liquid wastes.
Table 3.5
Tritium Concentrations in Water, pCi/ml*
Nov. 15, Jan. 17, June 25, Aug. 20,
Location 1 967 [968 1_968 1968
Cooling-water discharge canal 1.2 ± 0.3** 0.6 ± 0.3 < 1.5 0.2 ± 0.2
Cooling-water intake canal 0.8 ± 0.3 0.2 ± 0.2 < 1.5 0.2 ± 0.2
Illinois R. at Dresden Dam 0.8 ± 0.3
Kankakee R.t 0.8 km upstream
from cooling-water intake 1.0 ± 0.3
*Analysis by SERHL except for June 25 sample.
**± values are 2 a counting error; < values are 3 a counting error.
26
-------
3.4 References
!• Kiedaisch, W. and R. Pavlick, Dresden
Nuclear Power Station, 1968, personal
communication.
2. U.S. Atomic Energy Commission, ''Stand-
ards for Protection Against Radiation1',
Title 10, Code of Federal Regulations,
Part 20 (U.S. Gov't. Printing Office,
Washington, D. C. . 1965)•
3. Dresden Nuclear Power Station, ''Annual
Report of Station Operation for the Year
1968*' (Commonwealth Edison Co.. Chicago,
1969), p. 21.
4. Gilbert, R. S., ''Sources and Disposition
of Radioactive Liquid and Gaseous
Effluents from the Dresden Plant'',
General Electric Co. Rept. APED-4461
( 1964).
5. Fried, R, E. and J. M. Matuszek, Jr.,
''Environs Monitoring Program, Dresden
Nuclear Power Station'', First and
Second Qiarterly Reports, 1968 (Isotopes,
A Teledyne Company, 1968).
-------
4. RADIONUCLIDES RELEASED FROM STACK
4.1 Samples
4.1.1 Description of system. Boiling
water reactors such as Dresden I contin-
uously produce radioactive gases and aero-
sols and release them to the atmosphere
during reactor operation. The discharged
radionuclides at highest concentration are
the fission-produced noble gases and ^N.
Their transfer within the plant and from
source to stack is depicted schematically in
Figure 4.1, which is based on descriptions
from several sources.(1-4)
The main flow of gaseous radionuclides
is from degassing of condensed steam by the
air ejectors. The off-gas passes at a
nominal flow rate of 9.4 1/sec through the
delay line that provides a nominal 20-
minute* period for removal by decay of
most of the initial activity (see Appendix
B. 3). The decay period is especially im-
portant in reducing the release rates of
3.2-min ®9Kr, and 33- sec 90Kr, the pre-
cursors of ®9Sr and ^Sr, respectively.
Before the gas is released to the base of
the exhaust stack, it passes through high
efficiency particulate air (HEPA) filters
(nominal removal efficiency 99.97 percent
at 0.3 fj. size) to remove accompanying
aerosols, especially the recently formed
radioactive progeny of the noble gas fission
products. An approximately 2250:1 dilution
of the off-gas is provided at the stack base
•DNPS staff reported recently that the actual
flow rate is 10,4 1/sec (22 cfm), resulting in
a holdup time of approximately 23 minutes and
dilution factor of 2050:1. On this basis, pre-
dicted concentrations of noble gases and 13N in
the stack would be 9% higher due to less dilu-
tion. On the other hand, the holdup time would
be 3 minutes longer, decreasing levels of the
short half-life nuclides, 17-min. ,38Xe and
10-min. I3N, by 11% and 19%, respectively.
by ventilation air that is exhausted without
filtration from the reactor containment
structure and the turbine building.
Several secondary sources contribute
radionuclides to the stack effluent. Ap-
proximately 0. 1 percent of the process gas
escapes through the turbine gland seals.
This gas is separated from steam by a con-
denser and exhausted without filtration
through a 2-minute delay line to the
stack,Ventilating air carries traces of
radioactivity. Airborne radioactivity may
also arise from minor leaks in the reactor
pipeways and secondary steam generators. ^
The 91-m-high exhaust stack diminishes
from a base diameter of 3 m to 1.4 m at the
top. The exhaust air requires 2U seconds for
transit through the stack at the nominal
exit flow rate of 21 mVsec. At the 30-m
elevation (~ 10 sec. above the base), an
8-nozzle probe withdraws samples of the
effluent for the stack monitoring system. ^
This air is pumped at a rate of 1.1 to
1.4 m^/hr and passes sequentially through a
5-cm-dia. membrane filter for particulate
collection, a 5-cm-dia. organic vapor
respirator cartridge (27 g charcoal bed,
Cesco type B) for collecting gaseous iodine,
and a radiation detector for continuous
on-line monitoring of noble gas activity.
The filter and cartridge are routinely
replaced at 24-hr intervals.
The stack discharge limit is prescribed
by the AEC license at an annual average
release rate for noble fission gases of
700,000 /Ci/sec. This release rate is set
in accord with 10 CFR 20 paragraph 20.105(
to prevent exceeding a dose to the whole
29
-------
CO
o
CONTAINMENT STRUCTURE
STACK
REACTOR
VENTILATION EXHAUST (2.8 m3/sec)
sec delay
Steam
VENTILATION EXHAUST (18 m3/sec)
BUILDING
TURBINE
OFF-GAS DELAY LINE
(40 m of 76-cm-dia. pipe) PARTICULATE
off-gas pwi
Steam
50 sec
delay
TURBINE
FILTERS
min. delay
9.4 Iiters/sec
Process gas and ai r
GAS DELAY LINE (40 m of 61-cm-dia. pipe)
min. delay
Ii ters/sec
CONDENSER
AND
AIR EJECTORS
Figure Sources of airborne effluent.
-------
body of any individual in an unrestricted
area of 0.5 rem in a calendar year, 0.1 rem
in seven consecutive days, or 0.002 rem in
any one hour. Release limits of individual
radionuclides are defined in paragraph
20.10 6» and concentrations in air are
tabulated in Appendix B, Table II, Column
1 of 10 CFR 20 (see Section 3.1.3).
Hie average activity release rate at the
stack to the atmosphere for 1968 while the
plant was operating was approximately 12,500
jJZi/sec* ^ ^ The reactor was in operation
during 64 percent of the year. The
gaseous fission product release rate is
determined daily at Dresden by collecting
a sample of air-ejector off-gas at the
delay-line port at 6 A.M., counting it with
a single-channel Nal(Tl) gamma-ray detector,
and converting count rate to release rate
(in fjC.i/sec) by means of a chart prepared
by General Electric Company personnel.^
The noble gas composition typical of the
Dresden stack discharge is listed in Ap-
pendix B. 3. TrtC.se data are derived from
measurements of radioactive gases at Dresden
by General Electric Company personnel,
and calculations for a ''diffusion mix-
ture" (6) (see Section 2.3.4),
4.1.2 Sample collection. Samples of the
off-gas and stack releases were obtained
to demonstrate sampling and analytical
methods and to determine the composition
of effl uent from the stack. Emission data
were used to estimate radionuclide con-
centrations in environmental ground-level
air and deposition on vegetation. Hie data
also provide comparison with the nominal
stack releases reported by Dresden, informa-
tion on release rates of 3H and 85Kr, and
values of collection efficiency for the
radioiodine sample.
The off-gas was sampled at the port,
located in the delay line 4 minutes down-
stream from the air ejectors, that is used
for daily gaseous release measurements by
Dresden staff. Measured concentrations
were converted to release rates at the stack
for a 16-min transit time from port to stack
for radioactive decay, and a flow rate of
9.4 liter/sec.
Off-gas samples were obtained from
Dresden staff 9 times in 9~cc glass serum
bottles for gamma-ray spectrometry, and
twice in 209*cc volumetric flasks for 3H
and 85Kr analyses. The bottles and flasks
were sealed with rubber stoppers held by
crimped aluminum seals. The rubber stoppers
permitted insertion of the hypodermic needle
outlet of the sampling port. The needle is
connected also by means, of a two-way valve
to a pump for evacuating the container
before sampling. The internal pressure of
the sample was approximately atmospheric.
In tests of container integrity for gas
retention with 85Kr or 133Xe for periods as
long as 4 weeks, losses were less than
5 percent.
On January 17, 1968, a 209~cc sample of
gas was obtained from the stack monitoring
system at the same time that a 9-cc gas
sample was taken at the off-gas sampling
port. The two sets of measured radionuclide
concentrations were used to compare release
rates.
Release rates of airborne particles
in the stack were determined on 17 occasions
with the membrane filters that are routinely
inserted in the stack monitoring system for
24-hour periods beginning at 2200 or 2300
hours. These samples were dissolved on
5-cm-dia. stainless steel planchets,
analyzed as usual by the Dresden staff, and
then made available seven days after
colle c tion .
Releases of gaseous I were measured
on the same 17 occasions with charcoal
cartridges exposed behind the membrane
filters for the same duration. On two
occasions, the 131I collection efficiency
of the charcoal cartridges was tested by
inserting a second cartridge identical to
the first in the stack sampling system,
followed by two 69-g beds (5.7 cm depth) of
MSA Type 85851 charcoal. The latter was
impregnated with KI and had been recom-
mended for sampling CH-jI find other organic
iodine vapors. Under conditions that are
far more rigorous than in the Dresden stack,
a 5-cm bed had been found to retain 99% of
CH3I at 140°C and 87% relative humidity.(7)
Because the laboratory was so distant
from Dresden that analyses could not be
begun until 6 hours after sampling, the set
31
-------
of samples collected on January 17, 1968
was taken to Argonne National Laboratory,*
Gamma spect romet ric analysis of these
samples began 2 hours after sampling. On
June 26 and 27, 1968, the off-gas was
analyzed within 4 minutes of sampling with
a gamma spectrometer in a panel truck
parked near Dresden.
Air filters from monitors of ambient air
in the containment and turbine buildings
were obtained from Dresden staff to assess
the contribution of the ventilation air to
stack radioactivity. At Dresden, radio-
activity of airborne particles is rou-
tinely monitored within the containment
sphere by means of a device consisting of a
detector, a continuously moving strip
filter, and an 85-1/min pump. The device is
located in front of the inlet of the ex-
haust duct. In the turbine building, a
Schmidt constant flow pump that draws air
through a 5-cm-dia, filter at 42 1/min is
located at the high pressure end of the
turbine. These samples do not accurately
represent concentrations of airborne
particles in exhaust ducts, but may in-
dicate their magnitude.
4.2 Analysis
100,000
CO
250 Xe 135
x
CO
24 HRS. DECAY (5-MINUTE COUNT)
10,000'
X
,000
o
o
28-HRS. DECAY
(50-MINUTE COUNT)
OO
as
CO
CD
X
to £
CO CO
in
in
5.2 DAYS DECAY 1-VUw1
mo-min. nnnwn
0 400 BOO 1200 1600 2000 2400 2800
ENERGY, keV
Figure 4.2. Gamma-ray spectra of off-gas
from delay line. Detector:
Nal(Tl), 10 x 10 cm. Sample:
9-cc bottle of gas collected
0900 hour EST, Nov. 16, 1967.
4.2.1 Gamma-ray spectrometry. Radio-
nuclides that emit gamma rays were analyzed
in the laboratory with a 10 X 10 cm cyl-
indrical Nal(Tl) detector coupled to a
400-channel spectrometer (see Figure 4.2)«
Gamma-ray spectra obtained with a high-
resolution 6 cm^ X 7 mm or 10.4 cm2 * 11
mm Ge(Li) detector and a 1600-channel
spectrometer assisted in identifying radio-
nuclides (Figure 4.3). Samples taken to
Argonne National Laboratory were analyzed
by single and dual 10 * 10 cm Nal(Tl)
crystals and a small Ge(Li) detector (see
Figure 4.4). The counting system carried
by truck to Dresden consisted of a 10 * 10
cm Nal(Tl) detector mounted in a lead-brick
shield, a 400-channel spectrometer (see
Figures 4.5 and 4.6 for typical spectra),
a gasoline-fueled alternator to provide
power, and a Sola transformer.
•We thank Dr. Jacob Sedlet and his associates at
Argonne National Laboratory for analyzing these
samp]es.
Samples were analyzed in their original
containers by gamma-ray spectrometry. When
possible, detection efficiencies for the
containers and radionuclides of interest
were determined with standardized radio-
activity solutions. Accurate analysis of
gases was hindered by the unavailability
of standardized radioactive gases; for some
radionuclides, even pure unstandardized
isotopes that would provide individual
spectra for calibration were not available.
Hence, calibration curves of counting ef-
ficiencies vs. photon energy were estab-
lished by normalizing the shape of ef-
ficiency curves for other samples to the
efficiency value of the ^Kr 514-keV gamma
ray. The uncertainty of this curve is
estimated to be 10 percent or less.
The radioactivity in the Cesco cartridge
was concentrated on the upstream portion,
hence measurements were made on both sides
and this distribution was simulated in the
calibration standard. Analysis was delayed
32
-------
10'
10'
10'
o
o
10
to'
1 0
-1
)ve 135Xe
01 '»«. 250
160/
t j 1 1 1 | 1 1 1 r
- 33Xe
31,35
Kr 88
Xe
MO*8 T3 |
Channels 800
i
i
0
800
JL
j L
Jl
I I I I L.
100
900
200
1000
300 400 500
CHANNEL (1.0 keV/channel)
600
700
800
Figure 4.3. Gamma-ray spectrum of off-gas from delay line. Detector: Ge(Li), 6 cm2 x
7 mm. Sample: 9-cc bottle of off-gas collected 1030 hour EST, Jan. 18,
1968. Count: Jan. 18, 2130 - 2140 hour.
several days to await reduction by radio-
active decay of radio-xenon (particularly
1 ^^Xe) and progeny that initially obscured
the peak. Bee ause of the dslsyi no
short-lived radioiodine was detected, and
°nly gamma rays from ^4, ^^Xe, and the
30-yr 137Cs daughter of were observed.
Counting intervals and techniques were
selected to provide a counting error of i
5% or less at the 95 percent (2-sigma)
confidence level for most radionuclides.
Counting of low-level radioactivity was
usually for 1000 min. Samples were re-
analyzed periodically to check the half
lives of identified radionuclides and to
measure longer-lived radionuclides that
bad previously been obscured by radiations
from shorter-1ived radionuclides, as
indicated in Figures 4.5 and 4.6,
Complex sample spectra were analyzed by
comparison with the spectral shapes of the
individual components. Because separated
short-lived radioactive gases were un-
obtainable for spectral calibrations,
analytical uncertainties for these radio-
nuclides may be as large as a factor of
two,
4.2.2 Radiochemical analysis. After
gamma spectral analysis was completed,
strontium on the membrane filters and
ventilating-air samples was chemically
separated and measured for 89Sr and 90Sr
content with low-background G-M beta count-
ers at IQQ-min. counting periods.
Tritium and ®^Kr concentrations in the
209-cc gas samples were determined by
liquid scintillation counting after the
decay of shorter-lived radionuclides. To
collect Hi in water from either gas (HT) or
water vapor (HTO), 20 ml of water were
injected into the 209-cc sample containers
and occasionally swirled for 3 to 8 days.
The water was then transferred and distilled,
and aliquots were mixed with liquid scintil-
33
-------
5
tz
'50 138
(I
5r 138
1170 to
Vv«i
CHANNEL [keV = 80 + (2.86 * channel no.)]
Figure 4.4. Gamma-ray spectrum of off-gas from delay line. Detector: Ge(Li). Sample:
9-cc bottle of off-gas collected 1100 hour EST, Jan. 17, 1968. Count:
Jan. 17, U07 - 1417 at ANL.
lator for analysis.* The difference between
the count rates in the water samples and in
water blanks was attributed to tritium from
the gas samples. Hie resulting net tritium
concentration was multiplied by 189/20 to
calculate the tritium concentration in off-
gas. Gas for ^Kr analysis* was withdrawn
from the sample bottles when the water was
introduced, mixed directly with degassed
liquid scintillator, and analyzed.
4.3 Results and Discussion
4.3.1 Radioactive noble gases and 3H.
The prominent radionuclides in stack ef-
fluent, as measured by gamma spectral
analysis of delay-line samples, were 85mKr,
*We thank Dr. A. Moghissi and staff at the
Southeastern Radiological Health Laboratory
for analyzing these samples.
87Rr, 88Kr, *33Xe, 135Xe, an(j 138^e (see
Table 4.1). Xenon-135m is the only radio-
active noble gas among the major predicted
constituents of the stack effluent (Appendix
B. 3) that could not be quantified. One day
after release, only 88Kr, 133mXe, 133Xe and
1-^Xe were detected by gamma-ray spectrom-
etry (see Figure 4.2); after one month,
only l33Xe, 8^Kr anj remained. The rapid
initial decrease in radioactivity is in-
dicated in Figures 4.5 and 4.6.
The release rates of the individual
radioactive noble gases and their amounts
relative to nominal gaseous fission product
values in Table 4.1 vary appreciably among
samples. As indicated by the data summary
in Table 4.2, releases of individual radio-
nuclides, normalized to 1 mCi of nominal
gaseous fission product release, ranged
34
-------
Table 4.1
Stack Releases of Fission Product Noble Gases*, (uCi/sec
Sample Oate and Time (Central Time)
11/15/67
11/16/67
1/17/68
1/18/68
1/31/68
6/26/68
6/27/68
8/20/68
8/21/68
Radionuclide
(0600)
(0600)
(1000)
(0930)
(0900)
(1030)
(1630)
(1928)
(0547)
4.4 -hr
—
580
340
280
—
—
—-
—
—
10,7 -yr 85Kr
—
—
—
0.024
—
—
0.25
r-
CO
f
CD
1—
—
—
—540
—540
---
~1,300
—
—
—
2.8 -hr 88Kr
~1,300
-780
~640
—
-260
—
—
—
2.3 -d 133mXe
14
11
11
—
8
5
31
20
5.3 -d 133Xe
450
420
400
410
970
160
110
910
730
9.1 -hr 135Xe
930
1,010
1,660
1,250
2,600
620
520
—
1,420
17 -m 138Xe
—
—
-850
—
—
—2,800
-2,400
—
—
Gaseous fission
product release
rate
11,000
10,000
14,800
12,600
18,400
7,500
5,700
11,600
11,600
Based on sampling off-gas delay line; computed for release at top of stack after radioactive decay and
dilution of 9.4 1/sec off-gas by exhaust air from containment and turbine buildings at flow rate of 21
m3/sec.
Blank space indicates that radionuclide was not measured.
Table 4.2
Observed vs. Estimated Stack Release Rates of Noble Gases
Radionuclide
Number of
measurements
Observed
rate*
Est imated
Observed mean
Range
Mean
rate*
Estimated
a 5m K r
3
22-58
34
32
1.06
85Kr
2
0.003-0.022
0.01 2
0.052
0.23
B7Kr
3
37-180
-85
102
-0.83
8BKr
4
35-130
-67
109
-0.62
133Xe
S
19-79
42
33
1.26
issxe
8
83-140
104
114
0.91
138Xe
3
57-420
-284
243
-1.17
~Normalized as /iCi of radionuclide per mCi of nominal gaseous fission product
release.
35
-------
100,000
e 10,000
M IN.
LO
c
u
oo oo
CD
00
,000 -
CJJ
00
00
CO
CD
CO
O
CJ
00
PJ
CO
w
OS
00
CD
00
O) r- o>
CO 00 00
CD
n
100
ENERGY, keV
Figure 4.5. Gamma-ray spectra of off-gas from delay line after various periods of
decay. Detector: 10 x 10 cm Nal(Tl). Sample: 9-cc bottle of gas col-
lected 1613 hrs. CDT, June 27, 1968. Count: Sample was centered 24.3 cm
above detector. Times shown are from sampling to midpoint of counting
interval.
within approximately a factor of two of
their mean values. The ratio of the mean
measured value to that estimated in Appendix
B.3 for a 21-minute delay period ranged
from 0.6 to 1.1 for all gases except ®^Kr,
The measured release rate of ®^Kr would be
expected to be lower than in a mixture that
contained both equilibrium and recoil
components (see Section 2.3.4) because the
period of reactor operation was too short
for ®^Kr transfer to reach equilibrium. The
agreement of most measured and predicted
release rates within a factor of two con-
firms the applicability of the constant
determined by Gilbert^ for equation 2,3.
In the single comparison of radioactive
noble gases in the stack and in the delay
line (Table 4.3), values in the stack were
consistently higher. The differences may be
due to incomplete mixing of off-gas with
ventilating air below the stack monitor,
calculation of release rates with incorrect
flow rates in delay line, stack or stack
sampler, error in standardizing the gamma-
ray spectrometer for the gas containers, or
sources of radioactive noble gases in ad-
dition to delay-line off-gas. More measure-
ments are needed to resolve the differences.
The gamma-ray spectra of off-gas measured
within a few minutes after collection (see
Figures 4.5 and 4.6) indicated the presence
of 10-min ^N, which is formed by the
1 £ 1 0 1
reaction lo0(p,a) 1JN and is reported to be
a major constituent of the radioactive
stack effluent.jts release rate could
not be quantified, however, because of
spectral interference by other short-lived
radionuclides, especially *"^mXe,
Tritium concentrations in the off-gas
and tritium release rates computed from
36
-------
100,000
10,000
c
c=
Z3
o
o
31 MIN.
45 MIN.
70 MIN.
o
CJ
X
90 MfN.
00
CO
00
o g
oo in
CO CO
C9
in
co
185 MIN.
u
00
o
as
05
OS
oo
00
00
CO
CO
CQ
ao
oo
CO
200
400
600
ENERGY, keV
Figure Gamma-ray spectra of off-gas from delay line after various periods of
decay. Detector: 10 x 10 cm Nal(Tl). Sample: 9-cc bottle of gas col-
lected 1030 hrs, CXfT, June 26, 1968. Count: Sample centered 9.8 cm above
detector. (Spectrum of 185-min. count was adjusted to simulate counting at
this distance). Times show interval from sampling to midpoint of counting.
these concentrations are given in Table
4.4. Also shown are release rates estimated
from the tritium concentration in primary
coolant on the assumptions that the off-gas
is 40 percent hydrogen from the dissociation
of water in the reactor,(V) at a temperature
of 32 C (at which the volume of 1 mole of
H2 is 25 liters), and at 100 percent
humidity. Hius, the amount of water from
which the hydrogen in the off-gas was de-
rived is
9.4 liter/sec X 0.40 X 18 ml h^O/mole
25 liter HjO/mole
= 2.7 ml I^O/sec
Water vapor contributes another 34 X 10"^ ml
HjO/liter of gas )L 9.4 liter of gas/sec ¦
0.32 ml/sec, for a total release of primary-
coolant water of 3.0 ml/sec. in off-gas.
Release rates measured on June 26 agreed
37
-------
Table 4.3
Comparison of Off-gas Release Rates
Measured in Delay Line and in Stack,
//Ci/sec
Sampling Point stank/DeI ay
Radionuclide Delay Line*Stack Line
85mKr
340
520
1.5
07Kr
~540
-1240
2.3
88Kr
~780
~910
1.2
133Xe
400
650
1.6
135Xe
1660
1970
1.2
*Computed for release at top of stack after
radioactive decay and dilution of 9.4-1/sec
off-gas by exhaust air from containment and
turbine buildings at flow rate of 21 m3/sec.
with the predicted values but the value for
January 18 was 3-fold higher. Measured
and estimated tritium concentrations may
differ because the primary coolant water
and the off-gas were not sampled at the
same times, or because of erroneous as-
sumptions concerning the content of hydrogen
and water vapor in off-gas, The analytical
procedure depends on complete exchange of
tritium in HT with the water added to the
sample, an assumption that should be tested
in view of reported slow exchange rates.
In future studies, the total tritium release
rate in stack gas should also be measured.
4.3.2 Airborne particles in the stack.
The longer-lived particulate radionuclides
observed in the stack were the activation
Tal
Release Rate of Tritium
products 5®Co and 6^Co, and the gaseous-
fission-product progeny 8^Sr, ^^Sr, 13?Cs
and 14UBa. Emi ssion rates measured for 17
samples are shown in Table 4.5, and mean
values and ranges, in Table 4,6. Activity
levels and relative composition fluctuated
considerably, and no relation was found
between release rates of particles and
nominal gaseous fission products. Partic-
ulate 13 11 was never found above the min-
imum detectabLe emission rate of 30 pCi/sec,
compared to release rates of gaseous 131[
between 200 and. 3230 pCi/sec.
4.3.3 Gaseous ^^1 in the stack, The
] 3 1
gaseous I release rates observed in the
stack with the routinely used single char-
coal cartridge are given in Tables 4.5 and
4.6. The test of cartridge collection ef-
ficiency indicated that 88 percent of the
collected is retained on the usual
sampling cartridge and the remaining 12
percent is on a second cartridge (Table
4.7). These values agree with a similar test
conducted with filtered gas from the CP-5
reactor, wherein 95 percent was retained by
a single Cesco cartridge and 98.7 percent
by two in series.Dresden staff reports
that the conservative factor for calculating
release rates from count rates more
than compensates for incomplete radioiodine
retention in the cartridge.^3^
No (< 1,2 percent) was found on the
KI-impregnated charcoal beds located behind
the Cesco cartridges. This type of charcoal
is reported to be an effective collector
4.4
m Condenser Air Ejectors
Concentration
Concentration
Release rate, nCi/sec
Date,
in primary coolant,
in delay 1ine,
1968
pC i/m1
pCi/cc
Measured Estimated*
Jan. 18
1.5
14
Feb. 1
1,660
0.52 ± 0.03t
5.0
June 26
4.8 ± 0.3
Aug. 22
1,300
3.9
*based on equivalent water for hydrogen gas of 2.7 ml/sec and for
water vapor of 0.32 ml/sec.
^standard deviation of duplicate analyses; only one sample was
analyzed on Jan. 18.
Note: 1 nCi/sec ¦ 1 x 10'3 /uCi/sec.
38
-------
Table 4.5
Stack Releases of Particulate Radionuclides and Gaseous lodine-131, pCi/sec
Sampling Period (~24 hours)
Nov.
1967
Jan. 1968
June 1968
Aug.
1968
Radionuclide
7
8
9
10
1 7
19
20
21
22
23
24
25
26
27
28
20
21
Particles
on membrane fi1ter
71 -d
58q0
< 8
NA
NA
17
140
< 8
29
1 3
< 8
< B
< 8
9
< 8
< 8
< 8
70
120
5.26-J r
60Co
27
21
20
NA
20
25
23
2.5
8
10
19
18
11
23
12
60
95
51 -d
89Sr
NX
420
2300
1170
NA
1280
860
1180
1310
800
920
580
900
850
11.80
610
220
28 -yr
80Sr
HA
5
6
25
NA
3
2
3
3
2
3
3
3
2
3
2
3
30 -yr
137CS
25
NA
48
50
13
55
38
41
36
29
31
31
34
38
38
30
25
12.8 -d
uoBa
360
250
480
390
70
480
500
510
710
580
700
400
500
440
400
440
85
Gaseous 1311 on
charcoal
cartridge
e.OB-d
1311
360
330
3230
2560
2780
250
930
670
200
240
220
620
1060
600
670
840
210
Gaseous fission
product release
rate, (iCi/sec)
8.7
17.0
18
53
15
7.4
6.6 7.1
5.
9 5.
8 5.7
6.4
7.5
5.7
6.7
11.8
11.6
111 - No analysis made.
< values indicate nininuR detectable activity at the -3 a confidence level.
1 pCi/sec - 1 x ID"6 /iCi/sec.
1 uCi/sec = 1,000 /zCi/sec.
CO
vO
-------
Table 4.6
Table 4.7
Summary of Stack Releases of Particulate
Radionuclides and Gaseous lodine-131, pCi/sec
Number of
Radionuclide
Measurements
Mean
Range
58Co
15
26*
< 8
- 140
60Co
16
25
2.
,5 - 95
89Sr
15
970
220
- 2300
90Sr
15
5
2
- 25
13?Cs
16
35
13
- 55
1406a
17
430
70
- 710
13 1 I
17
920
200
- 3230
Gaseous fission
product release
rate, mCi /sec
17
11.7 5.7 - 53
*values below minimum detectable activity values
were taken to be zero for averaging.
1 pCi/sec = 1 x 10~6 /xCi/sec
of CHI under conditions that lead to
penetration of Cesco-type charcoal by
m.jl.(') Thus, essentially all of the
j)>).
' I reLeased at the stack appears to be
in a form that can be collected on the
Cesco cartridges.
4.3.4 Airborne particles in ventilat-
ing air. Radionuclide concentrations in
air, measured on filters that were col-
lected in the turbine and containment
buildings on one occasion are listed in
Jable 4.8. Radionuclide release rates in
ventilating air were computed from ventila-
tion rates on the assumption that the
sampled concentrations were representative
of values in the exhaust duct. Compared to
stack-monitor values on January 16-17 (Table
4.5;, release rates in ventilating air were
of the same magnitudes for ^Sr and ^'Cs,
but much smalLer for 58Co, 60Co, ®^Sr, ^*1,
and i,4,°Ba. Note that was collected on
filters (i.e., as particles) in the
ventilating air and on charcoal (as gas) in
the stack effluent.
4.3.5 Sources of airborne particles.
The airborne particulate radionuclides
detected in the stack sampler may reach the
stack (1) through ingrowth from gaseous
precursors between the high efficiency
particulate air filter in the air-ejector
off-gas line and the stack monitor, (2) by
40
lodine-131 Concentration in Stack Monitor
Exposed 2120 CDT August 20 to 2125 CDT
August 21, 1968
Sampler
1311, pCi/m3
Fi rst Cesco cartridge io ± 0.5
Second Cesco cartridge 1.3 ± 0,2
Kl-impregnated charcoal <0.15
< value indicates minimum detectable activity
at the -3 cr confidence level.
penetrating the filter, (3) in off-gas from
the turbine gland seal condenser and (4) in
ventilation air from turbine building arid
containment shell.
Contribution by sources (1), (2) and
(3) can be estimated from Gilbert's val-
ues^' for radioactive gases at the air
ejector per mCi/sec of nominal gaseous
fission product discharge. These contribu-
tions were estimated for 4 radionuclides
from the stack measurements from June 18
to 28, 1968, when the noble gas discharge
averaged 6.5 mCi/sec. The values given
below are based on decay and ingrowth
calculations for a 20-minute delay from the
air-ejectors to the filter, 0.1 percent
filter penetration, and a 10-second delay
from the filter to the stack monitors, Also
assumed were a 2-minute delay for gland
seal condenser off-gas, and a 0. 1 percent
leakage of process gas through the gland
seals.^ ^ ^
Computed release rate at stack
sampler*, pCi/sec
<
-------
Table 4.0
Airborne Particles in Sphere and Turbine Building
Concentration, pCi/m3
Estimated
release rate, pCi/sec
Release rate
Radionuclide
Sphere
Turbine
Sphere Turbine
Total
pCi/sec
O
CO
in
2.1
1.0
5.9
18
24
140
60Co
1.2
< 0.1
3.4
< 1.8
-3.4
20
GO
CO
CO
3.2
3.0
9.0
54
63
2,300
90Sr
0.11
0.35
0.3
6.3
6.6
6
13 11
16
< 0.5
45
< 9.0
-45
2,780
'3*Cs
0.4
< 0.1
1.1
< 1.8
-1.1
—
,3?Cs
1.2
0.9
3.4
16.2
20
13
uoBa
0.4
0.9
1.1
16.2
17
70
Notes: 1. Ventilation exhaust rates to the stack are 2.8 m3/sec from the
containment sphere and 18 m3/sec from the turbine building.
2. < values indicate minimum detectable activity at the 3 a con-
fidence level.
3. Sampling intervals: containment sphere - 1445 hrs.t Jan. 17,
1968 to OgOO, Jan. 18.
turbine - 0000 to 2400 hrs.,
Jan. 17.
stack - 2250, Jan. 16 to 0910,
Jan. 17, then 1100 to
2300, Jan. 17, except
that 89Sr and 90Sr
rates are for Jan. 9,
1068.
Estimated releases of ®-'Sr and ^®Ba are
lower than measured rates by factors of 2
and 3, respectively. Higher values would
result from larger-than-assumed amounts of
precursor gases, higher filter or gland
seal leakage, or appreciable contributions
from ventilating air, The much lower esti-
mates of 90Sr and 137Cs contributions com-
pared to measured rates support the finding
that ventilating air exhaust is the prin-
cipal source of ^Sr and ^7qs
in the stack
moni tor.
4.4 References
1. Blomeke, J. O, and F. E, Harrington,
''Management of Radioactive Wastes at
Nuclear Power Stations'*, AEC Rept.
ORNL-4070 (1968) pp. 33-40.
2. Gilbert, R. S. , "Sources and Disposition
of Radioactive Liquid and Gaseous Ef-
fluents from the Dresden Plant'', General
Electric Co. Rept. APED-4461 (1964).
3. Kiedaisch, W. and R. Pavlick, DNPS,
personal communication, (1968).
4. Joslin, M., Response to AEC question-
naire, Docket 50-10 (June 6, 1961).
5. Dresden Nuclear Power Station, ''Annual
Report of Station Operation for the Year
1968'', (Commonwealth Edison Co.,
Chicago, 1969), p. 21.
6. Smith, J, M., ''Release of Radioactive
Wastes to Atmosphere from Boiling Water
Reactor'', (General Electric Co., San
Jose Calif,, I960).
7. Ackley, R. D,, R, E, Adams and W. E,
Browning, Jr., ''Removal of Radioactive
41
-------
Methyl Iodide from Steam-air Systems'',
in ''Proceedings of the Ninth Air Clean-
ing Conf., Sept, 13-16, 1966'', AKC Rept.
ORNL-4040 (1967).
8. Shuping, H. K. , C, R, Phillips, and A. A.
Moghissi, ''Low-Lev el Counting of' En-
vironmental ®5Kr by Liquid Scintilla-
tion'', Anal. Chem. 41, 208 2 (1969)
9. Yang, ,J, Y. and L. II. Gevantrnan, ''Trit-
i um-/3-Had i at ion-I nduced Isotopic Ex-
change in the Tg-f^O System*', Naval
Radiological Defense Laboratory Rept,
liSNRDL-TR-471 (I960).
10. Dillow, W. D., ''Radio iodine Measurements
of the Stack Effluent from the CP-5
5.0-MW Heavy-Water Reactor'', AEC Rept.
ANL-7427 ( 1968).
42
-------
5. RADIONUCLIDES IN ENVIRONMENTAL AIR
5.1 Introduction
5.1.1 Purpose. These studios wore under-
taken to demonstrate sensitive and con-
venient techniques for detecting the plume
released at BWR stacks, measuring radio-
nuclide concentrations in the plume, and
determining the radiation exposure rate
associated with the plume. At BWH stations,
the critical pathway appears to be from the
stack through air, leading to whole-body
irradiation of persons in or beneath the
plume at ground level near the station. By
comparing, under appropriate conditions and
with sufficient frequency, radionuclide
concentrations in the environment with re-
lease rates at the stack, the degree of
atmospheric diffusion for computing release
limits is determined; by comparing exposure
rates in the environment with release rates
at the stack, release limits are determined
directly.
Survey meters were used to detect the
plume. For brief periods, (1/2 to 1 hour)
the radiation exposure rate was measured
witli sensitive muscle-equivalent ionization
chambers, radioxenon was collected wi tli a
cryogenic apparatus developed for this
purpose, and a radioactive particulate
daughter of radioxenon was collected with
high-volume air samplers. For longer periods
(2 weeks), radiation exposure was measured
with, thermoluminescent dosimeters (TLD's).
Both methods of measuring radiation exposure
were used because there is considerable
uncertainty in computing long-term exposure
from brief observations and also in measur-
ing long-term exposure near background
v a lues.
5.1.2 Environment and meteorology. Hie
environment of Dresden is sparsely wooded
and flat, except for a bluff 30 m high on
the far bank of the IL1 inois Biver, 1 km
north and east of the stack. (For further
description of the environment, see Section
7.1.1). Winds blow predominantly from the
southwest during most of the year, ' J ¦* but
westerly winds are frequent during the
winter. Rainfall is heaviest in summer.
Summer rains are from cohvective showers
and thunderstorms, winter rains from passing
cyclones.
Meteorological data for planning and
interpreting the experiments were obtained
from an instrumented 123-m tower located
0.8 km SSW of the plant,. Wind speed and
direction instruments and temperature
sensors are in the tower at levels 11,
38, 92, and 123 m above ground. Data are
recorded continuously on strip charts and
were provided on request by Dresden staff.
The data are also summarized by computer
for wind speed, direction, and direction
variance for one 15-minute average per
hour.*
5.2 Short term Radionuclide
Concentrations and Radiation
Exposure Rates
5.2.1 Measurements. Three field experi-
ments were conducted on the bluff north to
east of Dresden while the plume from the
stack was over the measurement locations.
The sites, shown in Figure 5.1, are between
1.6 and 1.8 km distant from the stack. They
were selected by observing current wind
directions at the Dresden meteorological
*We thank Dr. M. I. Goldman and Mr. P. Altomare,
NHS Inc., for providing this information.
43
-------
QNPS*
SCALE IN KM
^STRIP //'
mtw
Figure 5.4. Location of field tests (A)
and dosimeter stations (o)
near Dresden.
tower, and then traversing roads in the
predicted direction with portable Nal(Tl)
survey meters (see Section 5.4) to find the
center-line of the plume. In several other
experiments, wind directions were too
variable to permit data averaging over
1/2 to 1 hour periods. Possible sites were
limited to existing roads, although the
Dresden area is favorable because of the
checkerboard pattern of roads at 1-mile
intervals. Measurement periods were selected
so that the first and third experiments
were at neutral conditions during which the
instruments were probably within the plume;
the second experiment was under stable
conditions, with the instruments presumably
beneath the plume.
In all three tests, radioxenon was col-
lected 1.5 m above ground by pumping air
through charcoal at ~80°C (see Section
5.2.2 for details of the apparatus). Volumes
of 0.65, 0.68, and 0.40 m3 were passed
through the charcoal in tests 1, 2, and 3,
respectively. In the second and third tests,
radioactive airborne particles were col-
lected at the same locations by pumping air
at the rate of 1.4 m^/min through a glass
fiber filter (MSA CT-7 5428, 20 X 26 cm)
with conventional high-volume air samplers.
The charcoal and the filters were analyzed
by gamma-ray spectrometry with 10 X 10 cm
Nal(Tl) detectors and multichannel analyz-
ers. Two air fiIters from duplicate systems
were counted together each time. The filters
represented 157 rn3 of air in test 2 and
96 m3 in test 3, Spectra obtained immedi-
ately after collection during the second
and third experiments with detector and
analyzer mounted in a light truck that was
parked away from the plume are shown in Fig-
ures 5.2 and 5.3. All samples were analyzed
again in the laboratory, yielding gamma-ray
spectra such as the one shown in Figure
5.4, Field spectra were less precise because
of shorter counting times and less shielding.
Concurrently with the collection of
radionuclide samples, the radiation expo-
sure rate was measured with a muscle-
equivalent ionization chamber and Shonka
electrometer.^*^ The ionization chamber is
a 16.5-liter sphere with 6-mm-thick plastic
walls that contains a neon-ethylene-ethane-
nitrogen gas mixture (760 torr at 15°C).
The vibrating-reed electrometer has a
design sensitivity of 0.32 mV sec" VfR
hr"], compared to the value measured with
a radium standard of 0.33 mV sec'V/^R
hr"1 (0.34 mV sec"1//^1"3^ hr"1). At the
electrometer operating voltage of 1000 mV,
reading periods ranged from 5.5 min for
background to 1 min at the highest exposure
rates. As many readings as possible were
obtained during each experiment. The back-
ground exposure rate, measured when the
plume passed in another direction, was
subtracted from each gross exposure rate.
The average exposure rate was computed from
these readings, weighted for reading inter-
val.
5.2.2 Radioxenon collector. The apparatus
was developed to collect quantitatively
sufficient radioxenon in a 1-hour period
for measurement by gamma-ray spectrometry.
It consists of the following components:
(1) flow meter;
(2) 90 g molecular sieve (Linde MS 13 X)
in a 4-cm-dia. glass column to re-
move GOj and water vapor;
44
-------
100
6
TEST NO. 3-NEUTRAL CONDITION
INSTRUMENT
BACKGROUND
O
CJ
LkJ
>—
oc
TEST NO. 2- STABLE CONDITION
to
CJ
X o o
QD CO OD
cr> <+7
0 200 400 600 800 1,000 1,200 1,400 1,600 1,800 2,000
ENERGY, keV
Figure 5.2. Gamma-ray spectra of charcoal xenon collector. Detector: 10 x 10 cm.
Nal(Tl). Sample: 210 g charcoal in 450-cc gas~tight container, collected
Aug. 21, 1968• Counts: Test 2: Aug. 21, 0311-0321; Test 3: Aug. 21,
1905-1925.
(3) copper coil, 1-cm-dia. X {JO cm, for
cooling air by immersion in dry-ice-
acetone bath;
(4) 210 g charcoal (Columbia 6GC 10/20
mesh) in a 3.2-cm-dia. X 66 cm copper
U-tube, to collect radioxenon when
immersed in dry-ice-acetone bath;
(5) 30-liter/min vacuum pump;
(6) dry-ice-acetone bath for immersing
copper coil and U-tube.
The first five components are connected in
the specified order with plastic tubing;
the glass column, copper coil and copper
U-tube are sealed with 1-hole rubber stop-
pers and tape. To collect xenon, air is
punped at 15 liter/min for as much as 1
hour. Immediately after pumping, the U-tube
is opened, the charcoal is transferred to a
plastic 450-cc container, and the container
is sealed with a rubber-gasketed, bolted-
down lid. The container must withstand
pressures of several atmospheres as the
charcoal warms up to ambient temperatures.
The charcoal in the container is analyzed
by ganma-ray spectrometry, either immedi-
ately to measure 138Xe, or later, to measure
133Xe and 135Xe.
The apparatus was tested with ^33Xe and
85Kr tracers. At the indicated amount of
charcoal and flow rate of air, no radio-
xenon was lost from 1 m3 of air. Radio-
krypton, however, began to break through
the column after passage of 0.12 m3 of air,
and can therefore not be collected quanti-
tatively from larger volumes under the de-
fined conditions. These results agree with
earlier studies of radiokrypton and radio-
xenon adsorption on charcoal. ^
45
-------
10,000
TEST NO. 3-NEUTRAL CONDITION
O
LkJ
I
«C
az
TEST NO. 2-STABLE CONDITION
I—
PHOTONS FROM,
DAUGHTER OF '38X
100
<=>
uoo
m m m
PHOTONS FROM DAUGHTERS
nc uATIIDA I 222dm
ENERGY, keV
Figure 5.3. Gamma-ray spectra of air filters. Detector: 10 x 10 cm NaI(Tl). Samples;
Two 20 x 25 cm glass fiber filters folded into quarters for counting,
collected Aug. 21, 1968. Counts: Test 2: Aug. 21, 0325~0327; Test 3: Aug.
21, 1900-1902.
5.2.3 Meteorology. The tests were per-
formed under the conditions described in
Table 5.1. January 17, 1968, was clear and
cold with moderate southwesterly winds in
advance of a cyclone to the west. The ground
was covered with snow up to 15 cm deep from
a previous storm. Duiing August 20-21, 1968,
the dominant weather influence was a large
anticyclone over the southeastern states.
The day was hot, and the night was warm and
humid. Skies were clear except for scattered
afternoon cumulus.
Tests 1 and 3 were conducted between the
time of afternoon maximum temperature and
sunset. This is a period of neutral stabil-
ity marking the transition from afternoon
unstable to evening stable atmospheric
conditions. At this time, considerable mix-
ing of effluent from the 91-meter stack to
the ground is expected after it travels
over the bluff. Hie sampling sites for tests
1 and 3 were at the plume centerline,
according to the wind direction trace at the
92-m level in the tower.
Test 2 was conducted after midnight,
during stable conditions that were in-
dicated by the rate of temperature and wind
speed increase with height. Effluent from
the Dresden stack would be expected to
spread moderately in the horizontal plane
but very slowly in 'the vertical plane, re-
maining mostly at the effective emission
height. Wind direction data at the 92-m
level showed 5- to 10-degree oscillations
of variable periodicity. The mean wind
direction, i.e., plume centerline, was about
4° (100 m) from the sampling point.
5.2.4 Es timation of radionuclide con-
centrations and exposure rates. Concen-
I q * i -1 r
trations of Xe and Xe at the measure-
ment locations were estimated from the
46
-------
10'
10J -
c.
zn
o
u
10'
£
BACKGROUND
-(INSTRUMENT PLUS
CHARCOAL)
101
200
SOU
400 600
ENERGY, keV
Figure 5.U. Gamma-ray spectrum of charcoal
xenon collector, 24 hours
ajter collection. Detector:
10 x 10 cm Nal(Tl). Sample:
210 g charcoal in 450-cc gas-
tight container, collected
Jan. 17, 1968. Count: Jan. 18,
1800-1850.
generalised Gaussian diffusion equation ' ^
given in Appendix C.1. Normalized concen-
trations (Xu/Q, see Appendix C. 1) as a
function of distance from the stack from
extensive studies at Brookhaven^^ ) were
used, except for vertical dispersion under
stable conditions, for which Hanford studies
provide the most realistic estimates.^'''
The effective stack height was calculated
by the Holland formula as modified by
Moses(9); however, the effective height was
reduced by one-half of the elevation of the
bluff above the base of the stack, i.e.,
15 m. Release rates for 133Xe and ^^Xe on
January 17 and August 21 are given in Table
4. 1.
JOQ
To estimate the concentration of Cs
at the measurement site, the release rate
at the stack of its parent ^3®Xe was assumed
to be 2.1 times the 1 3 5Xe release rate
(see Appendix B.3), The fractional ingrowth
o f 131ts five minutes after release was
computed to be 9.4 percent of the i38Xe
release value, and the same normalized
concentrations were used as for 133Xe and
135Xe.
The model for estimating radiation
exposure rates is similar in approach to
that described in the FSAR for Dresden 2
and and that by Stuart and May,
witli tlie following modifications: (1) dose
calculations were made for photon energies
of 0.4 and 2.0 MeV to represent by 2 average
values all photons of energies less than
and greater than 1 MeV, respectively;
(2) dispersion of the stack plume was cal-
culated as described above, based on a
1-hour sampling for all meteorological and
plume-related measurements; and (3) no
cross-wind averaging was done; exposures
were computed for specific plumes. The
estimated exposure rates are based on a
45-minute period for test 1, 10-minute
averaging times for test 2, and a 30-minute
period for test 3.
Calculation of these exposure estimates
is shown in Appendix C.2. The gamma-ray
energies and intensities that were averaged
in terms of U.4- and 2.0-MeV gamma rays are
listed in Appendices C. 3 and C. 4. The
Holland methodwas used to check the
estimation technique, as shown in Appendix
C.5.
5.2.5 Results and discussion. Under the
10 0
neutral conditions of tests 1 and 3, Xe
and 135Xe were readily detected in the
charcoal trap, as shown in Table 5.2 and
Figure 5.4, For the described collection and
detection conditions, these radionuclides
47
-------
Table 5.1
Test Conditions for Sampling DNPS Stack Effluent in Environment
Test No.
Date
Time
Atmospher ic stabiIi ty
classification
Distance from stack, km
Samp Iing point azimuth,
degrees
Wind di rection, degrees
92-m level
38-m level
Wind speed, m/sec
92-m level
38-m level
Temperature di fference
between 120 m and 10 m,
Plume travel time,
stack to sampler, min
1
Jan. 17, 1968
1620-1705 CST
neutral
1.8
012
195
190
8.5
5.8
-0.5 to -0.2
3.5
2
Aug. 21, 1968
0208-0258 CDT
stable
1.6
045
229*
210-230
6.7
3.1
+1.3
3
Aug. 21, 196B
18 16-1846 CDT
neutral
1.8
039
220
230-212
6.2
4.5
-1.1 to -0.7
5
'Average of 10-min values which ranged from 225 to 233 degrees.
are detectable at nominal gaseous fission
product release rates as low as 1000 /-£i/sec.
Gamma-rays from short-lived ^®Xe and its
10 0
Cs daughter appear in the spectrum taken
immediately after collection (Figure 5.2),
but not clearly enough for analysis.
Under the neutral conditions in test 3,
1 Q O
the air filters collected shoFt-lived Cs
that could be measured with high precision
15 minutes after collection (see Figure
5.3). Interference by naturally occurring
progeny of ^2^Rn limits the sensitivity of
this analysis, but was not serious at the
indicated levels of *^Cs. No radionuclides
were found on the filter after 24 hours.
Collection of the particulate daughter of
138Xe thus is an alternative to collecting
133Xe and *35Xe, but filters must be anal-
yzed for ^3®Cs within several minutes, com-
pared to hours for *3^Xe and days for *33Xe.
The average exposure rates in tests 1
and 3 were 40 and 24 //R/hr, respectively
(see Table 5.2); the variability of the
individual measurements is indicated by the
respective ranges from 22 to 46 and from
12 to 36 /jR/hr shown in Figure 5.5. The
TIME, HOUR (CST, JAN. 17, 1968)
1625 1645 1705
50
CO
o
a-
x
1820 1840 1900
TIME, HOUR (CDT, AUG. 21, 1968)
Figure 5.5. Exposure rates under neutral
conditions, measured with
muscle-equivalent ionization
chamber.
48
-------
Table 5.2
Radiation Exposure Rate and Radionuclide Concentration Measured in Air
Near Ground Level Beneath Plumes from DNPS Stack
Test No.
1
2
3
Atmospheric stabi 1 i ty
neutral
stable
neutral
Stack release rate, /uCi/sec
gaseous fission product release rate
15,000
11,600
11,600
133Xe
400
730
730
135Xe
1,660
1,420
1,420
Radiation exposure, ^tR/lir
measured
40
13
24
calculated
This study (App. C.2)
20
9
19
Hoi land (App. C.5)
28
9
29
Concentrations, nCi/m3
measured
133Xe
3.8 ± 0.1**
< 0.10
3.8 ± 0.
CO
cn
X
CD
8.5 ± 0.4
< 0.17
7.0 ± 0.
138CS
NS*
< 0.04
1.76± 0.1
calculated
,33Xe (App. C.1)
1.0
0.003
2.2
,35Xe (App. C.I)
4.1
0.005
4.3
' 3®Cs
NS
0
0.9
~Not sampled
~~Values are standard deviations in counting; < values are 3
-------
beneath the plume, approximately 4° distant
from the measurement location, wouLd be
expected to be twice as high—i.e., 2b
/uR/hr. Exposure rate at the center! ine of
tlie plume therefore would be approximately
the same under stable and neutral conditions,
t I
111e average measured ratio of tlie Xe
or ^ ^Xe concentrations at ground level 1,8
km from the stack under neutral conditions
relative to their release rates at the
stack (in terms of X/Q, as defined in
Appendix C,1) was 6.2 * 10~6 sec/m3; normal-
ized for wind speed (Xu/Q), the average
r 9
ratio was 4. 7 " 10"J m . According to these
ratios, atmospheric diffusion was lower—
i.e., concentrations in environmental air
were higher—than estimated from the Brook-
haven data by approximately a factor of two.
In view of tlie uncertainties associated with
diffusion calculations, the two-fold dif-
ference should not be considered signif-
icant. Possible causes for the differences
include: (1) slightly different wind di-
rections at measurement locations than at
the meteorological tower; (2) differences in
wind speed with height; (3) a more complex
effect of bluff height than was accounted
for by the 15-m decrease in effective stack
height in tlie estimates; (4) different ^^Xe
or *^Xe release rates during environmental
measurements than during gas sampling at the
station; (5) insufficient environmental
concentration measurements for computing
averages.
The average of the three measured ex-
ternal exposure rates was somewhat higher
than the average of either of the two sets
of calculated values; as indicated above,
however, the differences are too small to
be considered significant. Note that the
results of the two sets of calculations
themselves differ in two of the tests be-
cause of different approaches in computed
exposure from a complex mixture of photon
energies.
To indicate the utilization of such brief
exposure measurements, an annual radiation
exposure per unit release rate at the stack,
D, in /vR/yr per mCi/sec,was estimated in 10°
sectors from average short-term (1/2 to
1 hour) exposure rates, D', in /xR/hr, and
nominal gaseous fission product release
rates, N, in mCi/sec, as follows:
- D' hr
D — — X 8760 — X 0,75 X wind freq. to sector
N yr
wind speed (during test)
ind speed (avg. in sector)
w 1
(5.1)
The factor 0.75 converts centerline ex-
posure values to sector averages, according
to the calculations by computer referred
to in Section 5.2.4. The value of D' in
test 2 must be multiplied by 2 to compensate
for the off-centerline measurement. Values
of D, based on sector averages at a 46-m
height of wind speed and frequency at
Argonne National Laboratory,^ are:
rr'P
.S? j?
X
Av
1
190° 5,6 m/sec 0.041 1.1
mR/y r
mCi/se<
2 210°-230° 6.1 0.044 0.7
3 220° 6.2 0.040 0.5
From the average wind frequency and wind
speed data,^ the highest annual exposure
is estimated for wind from the 210° sector
(i.e., at a direction 30° east of north
from Dresden); this estimated exposure is
approximately one-fifth higher than for
test 1, and one-third higher than for tests
2 and 3.
The average annual radiation exposure
estimated from these three brief measure-
ments in the three tests is 0.8 mR/yr per
mCi/sec. At the 1968 annual release rate
of 12,500 /iCi/sec during 64 percent of the
year, the exposure rate would be 6 mR/yr.
Tliis value can not be considered an accurate
measure of the annual exposure rate at
Dresden because the average short-term
exposure rate is based on too few measure-
ments and meteorological data were obtained
at a distant location and at a height below
that of the stack. The procedure suggests,
however, that long-term external radiation
exposures can be obtained from a sufficient
50
-------
number of short-term measurements of ex-
posure rate, combined with the meteorolog-
ical data that, are now being collected at
Dresden.
5.3 Long term Radiation
Exposure Rates
5.3.1 Measurement. TLD's were exposed
for two periods at the 11 locations near
Dresden shown in Figure 5.1, and at one
background location 32 km NE of Dresden.
The first exposure was between May 6 and 24,
for 17 or 18 days, during refueling. The
reactor was not in operation at this time
and release rates of radioactive gases at
the stack were undetectably low(l^), The
second period was for 14 days between
August 15 and 29, during which the reactor
was in operation for 12.2 days. The ex-
posure rate at each station was measured
with Nal(Tl) survey meters when the TLD's
were placed in position and collected. Six
dosimeters were exposed at station 110 to
evaluate data reproducibility; duplicate
dosimeters were placed at all other sta-
tions, Several stations were located in the
prevailing direction of the plume toward
northeast, and none was placed toward south-
west, a relatively improbable plume di-
rection.
5.3.2 Analysis. The TLD's (E.C&G model
TL-12) were a powdered calcium fluoride-
manganese mixture bonded to an electrical
coil in an evacuated glass tube,* The
dosimeters were annealed at 350°C at the
Cincinnati laboratory on the day before
exposure, and taken to the stations by car.
After collectipn, the dosimeters were re-
turned by car to the laboratory and sent
by air mail to Las Vegas, Nevada, for
reading. Five TLD's were annealed at the
laboratory on the day before collection and
sent to Las Vegas with the other dosimeters
to measure the background during transporta-
tion to Las Vegas and storage at Las Vegas
prior to reading.
The net radiation exposure of each TLD
was computed from the gross reading by
*We thank Mr. C. L. Fitzsimmons, Southwestem
Radiological Health Laboratory, BR1I, EHS, PUS,
DUEW, for providing and reading these dosimeters.
subtracting the above mentioned background
value for shipment and storage, and also a
constant internal background of 29 /iR/hr.
Gross readings were approximately 21 mi 11i-
roentgen (mR), of which 17 mB was internal
background, 1 mR, background from transpor-
tation and storage, and 3 mR, the net read-
ing. The exposure rate, in /iR/hr, was cal-
culated by dividing the net exposure by the
number of hours that each TLD had been ex-
posed at the stations. To obtain the net
exposure rate attributable to radiation from
the Dresden plume, the average exposure rate
at each station during refueling was sub-
tracted from the average exposure rate at
the same station during operation.
5.3.3 Estimation of exposure rates.
Exposure rates from radiation in the plume
at the eleven TLD stations between August
15 and 29 were estimated for comparison with
measured values by the same computer tech-
niques as for short-terin exposures. The
source term was taken to be an average
gaseous fission product release rate of
11.6 mCi/'sec during the 12.2-day period of
reactor operation. Exposures were summed for
the time intervals at which the plume passed
near the TIT) stations. Meteorological data
were provided by the computer summary of
Dresden tower readings, described in Section
5.1.2. The calculations are described in
Appendix C.6, and an example is given in
Appendix C.7. Estimated exposure rates and
the plume rose (i.e., the wind rose rotated
through 180°) for August 15 to 29 are shown
in Figure 5.7, On the basis of wind di-
rection frequency and wind speed, the high-
est exposure rate for the period was cal-
culated to be 3.2 /uR/hr in a direction 20°
east of station 110*
5.3.4 Results and discuss ion. The TLD
exposure rates for the two periods of
measurement range from 5.3 to 12.7 /-fR/hr at
the various stations (see Table 5.3), with
an overall average of 9 yuR/hr. This can be
taken as an average background radiation
exposure rate. Reproducibility of these
dosimeter measurements, according to the
standard deviation of six TLD's at station
HO and the mean standard deviations of
duplicates at all stations, was approximate-
ly 1 /jR/hr. The average exposure rate
51
-------
2 7 0'
30 hrs
Figure 5.7. Plume rose and estimated
exposure rates at dosimeter
stations. Exposure rates in
fdR/hr. Numbers on c ircular
grid indicate distance from
Dresden in km. Occurrence of
plume in indicated direct ion
is shown in hours.
Table
measured with pocket-type dosimeters by
Dresden's contractor for environmental
surveillance was 130 mR/yr (15 /LtR/hr). ( 1 4 )
The differences in values between the
two sets of exposure rates, attributed—at a
first approximation—to radiation from the
Dresden plume, are inconclusive. Improve-
ments in techniques are necessary if long-
term exposures are to be measured with
ILD's at Dresden's current gaseous fission
product release rates. Of the difference
values in Table 5.3, three (#104, 106, and
110) are at exposure rates of 2 to 3 /iR/hr
and are larger than their standard devia-
tion; all other exposure rates are less,
and are smaller than their standard de-
viations. Note that three difference values
are negative.
Although the values of individual
measured exposure rates from radiation in
the plume are uncertain, the sets of meas-
ured and estimated values are highly cor-
related, as shown in Figure 5.8. Lines of
best fit have been drawn for all 11 values
and for the 8 positive values; both lines
5.3
External Radiation Exposure Rates Near Dresden
Measured with Powdered Calcium Fluoride TLD's*
Station^
#
Measured
Exposure Rate.
/Jl/hr
Estimated Exposure
August 15-29
May 6-24
Di fference
Rate, /iR/hr
101
8.3 ± 1.3**
7.9 ± 0.6**
0.4 ± 1.4
0.8
102
9.3 ± 1.3
8.0 ± 2.2
1.3 ± 2.6
0.1
103
9.4 ± 1.8
8.3 ± 1.4
1.1 ± 2.3
0.7
104
10.6 ± 1.1
8.6 ± 0.6
2.0 ± 1.2
1.3
105
9.9 ± 1.5
9.3 ± 1.4
0.6 ± 2.3
0.4
106
8.1 ± 1.3
5.3 ± 1.5
2.8 ± 2.0
1.2
107
7.7 ± 1.1
6.6 ± 0.0
1.1 ± 1.1
1.0
108
10.3 ± 2.8
12.7 ± 0.4
-2.4 ± 2.8
0.4
109
9.4 ± 1.1
10.5 ± 1.4
-1.1 ± 2.0
0.0
110
12.1 ± 0.9
8.9 ± 0.8
3.2 ± 1.2
1.9
11)
9.2 ± 2.4
Lost
—
1.7
112
7.8 ± 1.5
9.9 ± 0.9
-2.1 ± 1.7
0.0
*EG&G Model TL-12
1"See Fig. 5.1 for location
**± values are 0.86 of range for duplicate dosimeters and standard deviation of sex tup I i ca t e
readings at station #110.
Note: The reactor was in operation for 12.2 days between August 15 and 29, 1968; it was being
refueled and was not in operation between May 6 and 24, 1968.
52
-------
ALL POINTS
CIRCLES
ESTIMATED
EXPOSURE
RATE,
/ifi/h r.
^ 1
3
-3-1-
Figure 5.8• Comparison of measured and
estimated exposure rates at
TLD stat ions near Dresden on
Aug. 15-29, 1968.
have a correlation coefficient of 0.77, and
a slope that indicates that measured ex-
posure rates near 2 /iR/hr were approximately
1.5 times as high as estimated values.
In view of the significant correlation,
further testing of the dosimeters for this
purpose appears warranted. Annual external
radiation exposures could thus be determined
by summing biweekly or monthly measurements.
To indicate the magnitude of the maximum
annual exposure above background, the high-
est measured exposure rate, at station #110,
was adjusted for annual w i nd-di r ec t ion
frequency and wind speed in the appropriate
sector, and the annual average gaseous
fission product release rate during 1968,
as follows:
frequency
n = D
y 00 1* mc&s
year
speed
frequency
speed
year
release
year
release.
= (3.2 t 1.2) , , 8.0 m/sec
0.078 5.9 m/sec
0.64 X 12,500 /i.Ci/sec
11,600 AiCi/sec
= 1.6 ± 0.5 /LtiVhr
= 14 ± 5 mR/year (5. 2)
The extrapolation to annual exposure is
based on meteorological data collected at
Argonne National Laboratory, at a height of
46-m,^D and is therefore not directly ap-
plicable to Dresden. It suggests, however,
that the highest value will be measurable,
but with considerable degree of uncertainty.
Note that the uncertainty arises from the
low exposure rate, and that exposure at
higher rates would be accompanied by in-
creased precision of measurement.
Whether differences in exposure rates
between operating and non-operating periods
may be attributed to radiation from the
plume depends on the constancy of the
natural radiation background. Although the
negative difference values near stations
108 and 109 may be due to random error,
they could alternatively result from a
decrease in the background during the second
exposure period. One indication of relative
stability in background is the set of four
exposure rate measurements with Nal(Tl)
survey meters summarized in Table 5.4. With
the single exception of station 101, dif-
ferences among these measurements were less
than the standard deviations for measure-
ments with replicate TLD's. Only year-round
tests will demonstrate whether one or even
the average of several measurements of
exposure rates from the natural radiation
background can be subtracted from measure-
ments during exposure from radiation in the
plume to yield net exposures due to the
plume at these low values.
In future studies, techniques can be
improved by using TLD's with appreciably
lower internal background, and by reading
dosimeters near the stations to eliminate
background exposure during transportation.
53
-------
Table 5.4
External Radiation Exposure Rates from Natural Background
Measured with Calibrated Nal(TI) Monitors, /xR/hr
Station #
Location, km
May 6 and 24
August 15 and 29
101
3.7 NNE
9.5 ± 0.8*
8.0 + 0.2*
102
2.4 ESE
9.9 ± 0.1
9.9 ± 0.0
103
1.4 E
10.0 ± 0.2
10.1 ± 0.2
104
•
CO
m
11.1 ± 0.2
10.6 + 0.0
105
1.3 N
10.5 ± 0.0
10.1**
106
1.4 WNW
8.3 ± 0.1
7.91"
107
1.6 WSW
7.7 ± 0.4
7.7 + 0.2
108
1.6 S
10.2 ± 0.6
10.1 ± 0.5
109
2.7 SE
9.4 ± 0.2
9.1 ± 0.1
110
1.3 NNE
10.7 ± 0.0
10.1 ± 0.1
111
I.I NNE
6.9 ± 0.1
7.3 + 0.4
112
32 NE
8.9 ± 0.4
8.9 ± 0.2
""values are 1/2 range of duplicate measurements obtained when dosimeters were exposed
and when they were collected.
**value for August 29 only; centerline of plume from Dresden stack near station con-
tributed to exposure rate on August 15.
"'"value for August 15 only; centerline of plume from Dresden stack near station con-
tributed to exposure rate on August 29.
5.4 Portable Survey Meters
5.4.1 Measurement. Cylindrical 5 X 5 cm
Nal(Tl) detectors with count-rate meters*
were tested near Dresden for use as rela-
tively sensitive and portable detectors of
gamma radiation from the plume in the en-
vironment. To obtain readings, plumes were
traversed by automobile, where roads per-
mitted, in the directions indicated by
instruments at the Dresden meteorological
tower. The survey meters were also used to
locate test sites at the centerline of the
plume for detailed exposure-rate measure-
ments, as described in Section 5.2.1. The
Nal(Tl) survey meters are far more rugged
and easier to read than the ionization
chamber and Shonka electrometer, but provide
only approximate exposure-rate values.
To attain even greater sensitivity, the
plume was traversed with a cylindrical 10
X 10 cm Nal(Tl) detector on the roof of a
light truck, 2.5 m above ground. The de-
~We thank Mr. Richard Stoms, BRH, Cincinnati,
for making these survey instruments and their
background calibration, as well as the Shonka
electrometers, available to us.
tec tor was covered with a 4-cm-thick
urethane cover for thermal insulation.
Gamma-ray spectra were analyzed with a
400-channel spectrometer within the truck.
A gasoline-fueled alternator with Sola
transformer provided power. Both types of
instruments were frequently checked with
radionuclide performance standards and by
comparing background readings at fixed
locations distant from the plume.
5.4.2 Calibration. The portable survey
meters were calibrated for exposure-rate
response by reading the Shonka eleetrometei-
at the same time. Calibration for radiation
from the plume was obtained for a plume
that had been released at the stack ap-
proximately 5 minutes earlier. The curve
of count rate by survey meter versus
exposure rate by ionization chamber ranged
from 4 to 47 /i.R/hr above background as
the plume shifted above the instruments.
Calibration could be expressed in terms
of the linear equation, Exposure Rate
= rn (Count Rate) + b, where the constants
m and b depended on the voltage discrim-
inator settings and varied among survey
meters. Count rates of 20,000 counts/min
54
-------
above background corresponded to exposure
rates from the plume of' approximately 20
yLiR/hr. Similar calibrations for the expo-
sure rate from the natural radiation back-
ground had been obtained earlier by com-
parisons witli the Shonka electrometer at a
variety of locations. At the typical back-
ground exposure rate of 9 /liR/hr, the count
rate of the portable survey meters was
6,000 to 7,000 counL/iniii.
Calibration of the large Nal(TL) de-
tector in terms of the concentration in air
of gamma-ray-emitting radionuclides was
attempted. The speetra obtained from plumes
cou 1 d not be analyzed, however, because
comparison spectra were not available for
short-lived radionuclides that contributed
significantly to the total spectra (see
Sect ion 4.2.1).
5.4.3 Results and discussion. The plume
from the Dresden stack was readily de-
tectable by Nal(Tl) survey meters within a
5—km radius of Dresden. Examples ol the
response of the instrument for 2-minute
measurements in Figure 5.9 demonstrate the
sensitivity as welL as the variation in
exposure rate in traversing the plume. On
the basis of readings at the centerline of
the plume, the average environmental ex-
posure rate of 9 /-<-H/hr is approximately
doubled at distances of J,6 km by a stack
release of 2 tnCi/sec. 'Hie values in Figure
5.9 do not show a true profiLe of exposure
rates in the plume, because the plume moves
during the traverse of the plume with the
survey meter. Exposure values based on the
calibration are approximate, since the
relative intensity of gamma-ray energies
changes with the time of travel of the
plume. The calibrations appear to be suf-
ficiently accurate, however, to permit use
of the instruments to indicate significant
changes in radionuclide releases at the
stack and potential health hazards.
The spectra obtained with the larger
detector mounted on the truck roof, shown
by the lO-minute measurements in Figure
5 20. indicate that the plume can be
identified 15 km distant from the stack at
DRESDEN STACK*
,35
,28
,32
44'
30'
COUNTY LINE
V ^ BRIDGE
24 8
28'
K I LOMETERS
LOffENZO RD.
Figure 5.9. Typical exposure rates
measured with portable Nal(Tl)
survey meters. Values are in
jjR/hr above background; values
south-east of stack were
measured on Nov. lb, 1967,
values to south on Nov. 15,
1967. All values were measured
in plume from Dresden stack.
release rates of 15,000 /iCi/sec. This
sensitivity should also be attainable with-
out spectrometer, by counting in energy re-
gions that have high count rates in the
plume, compared to the natural radiation
background. The count rate between 40 and
200 keV, for example, is 3,600 counts/min
above background at the most distant point
(spectrum 5 in Figure 5.10), compared to
16,000 counts/min background; a more favor-
able energy region according to Figure
5.10 would be 200-300 keV. The 10-minute
average exposure rate measured with the
portable survey meter at that location, 18
km NE of Dresden, was 2.5 /i.R/hr above
backgrou n d.
55
-------
CDrnTDiiu vunnv
DISTANCE
(sec)
o
o
BACKGROUND
0 200 400 600 800 1,000 1,200 1,400 1,600 1,800 2,000 2,200 2,400 2,600 2,800 3,000
ENERGY. keV
Figure 5.10. Net gamma-ray spectra measured on ground near center-line of plume with
10 x 10 cmNal(Tl) detector.
5.5 References
1. Moses, H, and M. Bogner, ''Argonne
National Laboratory Fifteen-Year Clima-
tological Summary'', AEC Rept, ANL-7084
( 1967).
2. Kastner, J., J. Rose and F. Shonka,
''Muscle-Equivalent Environmental Radia-
tion Meter of Extreme Sensitivity.''
Science UO, 1100 (1963).
3. Gustafson, P. F. , J. Kastner and J.
Luetzelschwab, ''Environmental Radiation:
Measurements of Dose Rates.'' Science
m, 44 (1964).
4. Ackley, R. D. , R. E. Adams and W, E,
Browning, Jr., 4'The Disposal of Radio-
active Fission Gases by Adsorption.'' in
Proceedings of the Sixth AEC Air Cleaning
Conference, AEC Rept. TID-7593, pp. 199~
216 (1959).
5. Slade, D. H., ed., ''Meteorology and
Atomic Energy 1968*', AEC Rept. TID-
24190 (1968)i equation 2.116.
6. Singer, I. A, and M. E. Smith, ''At-
mospheric Dispersion at Brookhaven
National Laboratory'', Intern. J, Air
and Water Pollution 10, 125 (1966).
7. Slade, op, citp. 141.
8. ibid, p. 191.
9. ibid, p. 193.
10. Commonwealth Edison Company, ''Dresden
Nuclear Power Station, Units 2 and 3,
Final Safety Analysis Report'', AEC
Docket No. 237-249 (Nov. 17, 1967),
Appendix A, Section 2.21.
11. May, M. J. and I, F. Stuart, ''Com-
parison of Calculated and Measured Long-
term Gamma Doses from a Stack Effluent
of Radioactive Gases", in Symposium on
Environmental Surpeillance in the
56
-------
Vicinity of Nuclear Facilities, W. C.
Reinig, ed. , (Charles C, Thomas, Spring-
field, 1970)> in press.
12. Holland, J. Z. , in ''Meteorology and
Atomic EnergyAEC Rept. AECU-3066
(1955), p. 109.
13. Kiedaisch, W,, and R. Pavlick, DNPS,
personal communication (1968).
14. Fried, R. E. and J. M, Matuszek, Jr.,
''1967 Annual Report, Environs Monitoring
Program, Dresden Nuclear Power Station'',
Isotopes, A Teledyne Company, Westwood,
N.J. (1968).
-------
6. RADIONUCLIDES IN SURFACE WATER
6.1 Water Use in the Illinois River
6.1.1 Public water supply and fishing.
Liquid wastes at Dresden are discharged into
the coolant-water discharge canal. The canal
empties into the IlLinois River at the con-
fluence of the Des Plaines and Kankakee
Rivers at Illinois River Mile* (IRM) 272.4,
just upstream from Dresden Dam at IRM 271.6
(see Figure 6.1). Flow rates at the Mar-
seilles gaging station (IRM 246.6), which
are only a few percent higher than at
Dresden Dam,^^ for the period 1920 to
1963 were: ^
Maximum daily - 94,000 cubic feet per
second* (cfs) on July
14, 1957
Minimum daily - 1,500 cfs on October
16, 1943
Average - 10,900 cfs
Because its water has been polluted with
domestic sewage and industrial waste from
Chicago since the opening of the Sanitary
PEORIA
FOX RIVER
FISH
DRESDEN LOCK
& DAM, ^
STARVED
ROCK
DAM
US66
HENNEPIN
MORR.IS
MARSEILLES ,
x ON PS
FISH saws /
MAZON QS3
RIVER
^DES PLAINES RIVER
^KANKAKEE RIVER
Figure S.l> Illinois River below Dresden.
1 mile * 1.61 km; 1 cfs = 28,3 liters/sec.
59
-------
and Ship Canal into the Des Plaines River in
19001 the Illinois River is not used for
public water supply, fishing, or irrigation
near Dresden.
The fish in the river near Dresden con-
sist primarily of carp, goldfish, shiner,
and catfish.'3^ Catfish that were ''fun-
gused'' and otherwise in unwholesome condi-
tion were found in 1912, and malformed
(knothead) carp, in 1928; both conditions
were attributed to pollution.'3^ According
to inhabitants of Morris (IRM 262), the fish
have a reputation for bad taste and odor,
and only someone unfamiliar with the river
would fish at this location. The only com-
mercial fishing in the Illinois River above
Hennepin (IRM 209) is by a single fisherman
in the mouth of the Fox River (IRM 241).^
Sport fishing begins below Starved Rock
Dam (IRM 232).( 1 >
The first use of the Illinois River below
Dresden as public water supply is at
Peoria*1) (IRM 166), The Peoria water supply
has three sources: ground-water wells, an
infiltration gallery with induced recharge
from the Illinois River, and direct intake
from the Illinois River via a well for
settling prior to treatment. Treatment is
by pH control and chlorination. Ground-water
wells are the major source of water; the
infiltration pit is used only when the
river is extremely turbid. The average
dilution factor for radionuclides in the
Illinois River at Peoria relative to the
coolant-water discharge canal at Dresden is
approximately 50, based on a flow rate at
Peoria that was 1.6 times as great at
Peoria as at Marseilles in 1961—1962^^
(i.e., 1.6 X 10,900 cfs = 17,000 cfs),
and a flow rate in the canal of 370 cfs
(166,000 gal/min). At maximum and minimum
flow rates, the dilution factors are 400
and 6, respectively.
6.1.2 Radiation exposure calculations.
Although Section 6.1.1 indicates that
neither drinking water nor food fish are
obtained at the mouth of the coolant-water
discharge canal, it is of interest to
estimate the potential radiation exposure
from radionuclide discharged by Dresden at
that point. For drinking water, the average
radionuclide concentrations measured on
three occasions for ionic substances and on
two occasions for insoluble substances com-
pare as follows to AEC limits:
N*
o°V^>X
CP V
3h
-------
fold), radionuclide concentrations in
drinking water at Peoria would be approxi-
mately 200-fold lower than at the point of
discharge by Dresden. A further decrease in
the concentration of some radionuclides in
water would be expected through mechanisms
such as radioactive decay, uptake by aquatic
organisms, or retention on benthal deposits
in the 106-mile passage to Peoria.
To evaluate potential radiation ex-
posure from eating fish that had lived at
the point of discharge of liquid effluent
at Dresden, the amount of fish was estimated
that would correspond to the consumption of
2,200 ml of water at AEC limits:
a *
^ fj*
s o « >
w a .« \
"Vy A -V
£) . •
^ ^
o O
¦C P
cT Sk, *C" O '"¦» \ ^
'
O tT
£
*
** t *
o J* A
c o A)
s
f o
CJ "»v 4
I
3h
0.9
7
X
10 "6
1
™Co
500
6
X
10"4
400
60Co
500
4
X
10"4
300
89Sr
40
1
X
io-4
70
9°Sr
40
9
X
10 "6
70
13 lj
1
6
X
10 "6
100
134cs
1,000
6
X
10-4
30
13?Cs
1,000
2
X
10"3
20
UOga
10
1
X
10 "5
7,000
•Assuming density of 1 kg/1 in fish flesh,
~•At water intake of 2.2 liter/day; i.e.,
weight of fish in kg/day = 2,200 ml/day X
limit in /JZi/ml + concentration in fish in
^iCi/kg; limit from 10 CFR 20, Appendix B,
Table II, Column 2, for soluble substances.
To compute the hypothetical radionuclide
concentrations in fish flesh, the soluble
and insoluble concentrations measured in
coolant-canal water were added for each
isotope, and the sum was multiplied by the
concentration factor for each element in
fresh-water fish.^4*
The critical radionuclides by this path-
137 1 ^ -iy—
way are Cs and X!s, at daily individ-
ual consumption of 20 and 30 kg of fish,
respectively. For all of the listed radio-
nuclides, the limit for continuous daily
consumption is 9 kg of fish, which is con-
siderably more than the reported daily
average intake by fishermen of 0.05^) or
0.1 kg. Radionuclide concentrations in
fish that are caught farther downstream
would be expected to be lower because radio-
nuclide concentrations in downstream water
are undoubtedly lower. On the other hand,
the above estimate does not consider the
possible concentration of radionuclides
in the food chain between water and the food
fish, i.e., in aqueous biota or fish that
are consumed by the food fish. Moreover,
intake of radionuclides with other foods
reduces the amount of radioactivity that
may be consumed with fish,
6.2 Water at Peoria, Illinois
6.2.1 Sampling and analysis. Radio-
nuclides in ionic form were collected with
the effluent sampler described in Section
3.1.4 from two sources on May 6-7, 1968:
Sample
Collection Hardness
Volume, period, as CaCOg,
liters hours mg/liter
settled, untreated 52
river water
drinking water 100
18
18
320
340
In addition, 1-liter aliquots of water were
collected to measure hardness and tritium.
The effluent samplers were operated in the
Peoria Water Treatment Plant with the aid
of plant staff,* During the sampling period,
22 percent of the water supply was from the
river and 78 percent from ground-water
wells, The infiltration pit was not used.
Procedures described in Section 3.2.2
were followed, except that the ion-exchange
resins were not washed with distilled water
*We thank Messrs. J. Behee and A. Cherry, Peoria
Water Treatment Plant, for helping to collect
these samples and describing tne plant opera-
tion.
61
-------
to remove silt. Tritium was measured with a
less sensitive liquid scintillation system
and was not found at a minimum detectable
level of 2 pCi/ml. Radiocobalt and radio-
cesium concentrations were too low to dis-
tinguish between and ^Co, and between
134Cs and 137Cs, respectively.
6.2.2 Results and discussion. Ri ver
water at Peoria contained radiocobalt
and 90Sr at concentrations of approximately
1 X 10"9 ^/Ci/ml each, and no detectable
89Sr or
131i(
as shown in Table 6.1. Stron-
tium-90 concentrations of 1.5, 1.1, and
1.1 pCi/liter, measured at Peoria by the
Federal Water Pollution Control Administra-
tion^- in September 1967, March 1968, and
September 1968, respectively, agree with
the listed ^Sr value. The Dresden environ-
mental monitoring contractor reported a 90Sr
concentration of 0.8 ± 0.3 * 10"^ /"Ci/ml,
and an 89Sr concentration of 2.7 i 0.8 *
10"5 /Xi/ml, for the May 1—15 composite
sample of Illinois River (Dresden Dam)
water.^' All radionuclide concentrations
were well below the AEC limits listed in the
last column of Table 6.1.
The radiocobalt and possibly part of the
radiocesium and ^Sr are attributed to
sources other than fallout. Concentrations
of 9°Sr an£J from fallout in Kankakee
River water (Dresden coolant-water intake
canal) averaged respectively 0.4 X 10"9 and
0.2 X 10"9 /U.Ci /'ml in January, June and
August, 1968 (see Table 3.3). Dresden,
Argonne National Laboratory,^^ and sewage
and industrial waste from Chicago may have
contributed the radioactivity that did not
originate in fallout.
As shown in Table 6.1, radionuclide con-
centrations in drinking water were lower
than in river water for all measured radio-
nuclides. This can be accounted for by the
almost five-fold dilution of river water
wi tli ground water. The latter would be
expected to contain no radiocobalt, and
less 9(JSr and 13'Cs than 111 ino i s River
water.
6.3 Fish at Dresden
6.3.1 Sampling and analysis. Fish were
caught with electro-shocking equipment* at
the 2 locations shown in Figure 6.1 on
June 27, 1968. The following fish were
collected:
Wet
Location
Type
Number
weight
Illinois River
c arp
11
11.8 kg
(IRM 262)
shad
10
1.0
Des Plai nes Ri ver
carp
7
5.0
(1 mi. W of high-
goldfi sh
30
5.4
way US 66 bridge)
*We thank Messrs. W. Starrett, D. Dooley, and J,
Stalter, Natural History Survey Division, State
of Illinois, for collecting these samples.
Table 6.1
Radionuclide Concentration at Peoria, III., Water Treatment Plant
May 6-7, 1968, pCi/liter*
Permissible
Radionuclide River water Drinking water concentrationt
5 8Co +
6°C0
1.0 ± 0.3
0.3
± 0.1
5 x 104 (SOCo)
89Sr
< 0.1
< 0.1
3 x 103
90Sr
1.1 ± 0.2
0.7
± 0.1
3 x 102
1 3 11
< 0.1
< 0.1
3 x 102
134Cs -
h '37Cs
1.5 ± 0.2
0.3
± 0.5
9 x 103 (134Cs)
~Concentration at samp Iing; pCi/liter = 1 x 10"9 >uC i/mI.
Tfor soluble substances in effluents to unrestricted area, 10CFR20, Appendix B, Table II,
Column 2 (1965).
Note: ± values are 1 a counting error; < values are 3 o- counting errors.
62
-------
Fish from the Des Plaines Biver, 4,5 miles
upstream from Dresden, were obtained to
determine background vaLues attributable to
fallout from nuclear weapon tests, sewage
and waste from Chicago, or discharge by the
Argonne National Laboratory. The downstream
sample was co 11 ected below Dresden Dam,
approximately 10 miles from the coolant
canal discharge point.
Fish were collected just below Dresden
despite the absence of fishing in this
region on the assumption that these fish
would accumulate at higher concentrations
the same radionuclides retained by fish
farther downstream. To minimize confusion
due to the movement of individual fish
upstream, downstream, or into tributaries,
all samples were composited for analysis.
Samples were frozen immediately after
collection. For analysis, the fish, were
weighed, thawed, and dissected to separate
tissues that were expected to concentrate
the radionuclides of interest:
heart area
(for thyroid) - 131j analysis
muscle - *34Cs and 137Cs analysis
kidney - 58Co and 60Co analysis
liver — and analysis
bone — ®^Sr and ^®Sr analysis
The tissues were combined by type of fish.
Heart area, liver, and kidney were analyzed
directly by gamma-ray spectrometry with a
10 * 10 cm Nal(Tl) detector. Muscle was
ashed at 400°C and then analyzed by gamma-
ray spectrometry. Muscle, kidney and liver
samples were also analyzed with the gamma-
ray coincidence/anticoincidence system (see
Section 3.2.2). Bone samples were ashed at
600°C, strontium was separated chemically,
and radiostrontium and ^Oy were measured
with low-background beta counters. Stable
strontium and calcium in bone were de-
termined chemically, and potassium in muscle
was determined by gamma-ray spectrometric
measurement of
6.3.2 Results and discussion. Concen-
trations of 9^Sr and in fish are sum-
marized together with stable potassium,
strontium and calcium levels in Table 6.2.
Only the radionuclides ^3^Cs and ^Sr were
in the fish in detectable amounts. No
significant concentration differences were
observed between fish collected above and
below the nuclear power station. The average
137Cs concentration in the muscle, weighted
according to the number of fish in each
group, was 14.5 pCi/kg wet weight, and the
average 137Cs/K ratio was 6.9 pCi/g K,
The average 90gr concentration measured in
the bone, weighted according to number of
fish in each group, was 500 pCi/kg fresh
weight, 4.1 pCi/mg Sr and 6.3 pCi/g Ca.
The average strontium concentration was
0.12 g/kg.
Reported concentrations of and ^°Sr
in fresh-water fish vary greatly; both
range from about 20 to 20,000 pCi/kg fresh
weight,(10,14, 16,17) The variations are due
to a number of factors, including:
1. the concentration of the radionuclide in
the aquatic environment;
Table 6.2
Radionuclide (pCi/kg)* and Stable Ion (g/kg)* Concentration in Fish Tissue
June 27, 1968
Tissue Substance Des Plaines Carp Pes Plaines Goldfish Illinois Carp Illinois Shad
Muscle ,37Cs 14.3 ± 0.5T 11.1 ±1.1 9.6 ± 0.4 31 ±3
Potassium 1.9 2.3 1.8 2.3
Bone** 90Sr 590 ± 60 420 ± 50 590 ± 60 550 ± 30
Strontium 0.14 0.14 0.11 0.08
*AII kg values are wet weight.
~"Calcium content = 78 g/kg.
T± values are 2
-------
2. exposure frequency; ^'
AI,137Cs- 10
AFsr = 690
3. the presence of other elements; for ex-
ample, the uptakes of stable strontium
and 90Sr are affected by the calcium
content of the water; 17)
4. the effect of temperature, because
metabolic processes of cold-blooded
aquatic organisms generally become
slower as the water temperature de-
creases; ' and
5. the trophic level. Predatory fish nearly
always contain greater concentrations of
^^Cs and ^Sr than non-predatory fish.
For example, Kolehmainen, et al.'1"
observed an average predatory/non-preda-
tory ratio of 3.8 for ^^Cs; Gustafson,
et al. reported a ratio of 3.5 for pike
vs. perch (the perch being largely con-
sumed by pike),(16)
Although 9^Sr
was not measured in the
scales of the Dresden fish, it is inter-
esting that Ruf has reported nearly identi-
cal concentrations in fish bone and scales,
and simi lar !37Cs concentration in meat and
bone.^5^ Similarly, Ophel and Judd found
concentrations of Sr and Ca to be similar
in bone, scales and gills,^^
Another approach to evaluating concentra-
tions is in terms of the accumulation
factor (AF)—the ratio of wet-weight con-
centration in fish to concentration in
water. Water analyses by the U.S. Public
Health Service and the Federal Water Pol-
lution Control Administration in the
Illinois River at Peoria^?) confirm the
hardness value in Section 6.2. 1» which
indicates a calcium concentration of 130
mg/liter. They also show average strontium
concentrations (1962 to 1968) of 180
/jg/liter. Relative to these stable-ion
concentrations and the 90gr and radiocesium
concentrations (assuming that all radio-
cesium is ^Cs) in Table 6.1, the average
concentrations in fish yield the following
accumulation factors:
AF90Sr = 450 AFCa = 600
A?" values are in meat for 137Cs and in bone
for strontium and calcium.
Accumulation factors for strontium in
bone have been reported to be 100-4030 for
perch,(1' ) 50-8810 for pike, (17 ) 70-9170 for
roach, ^^ 145—10,000 for brown trout, (19)
and an average of 3940 for c rapp i e. ( 1 4-)
TTie AFg for skin and scales of fish appear
to be about the same as for bone.^ ^ For
9tlSr, Ruf found values between 200-600 for
bone of carp, trout, and pike.'1^) -^he
average AF90 an(^ AFsr ^or ^ie Dresden fish
fall within their respective ranges, and
there is no significant difference between
these two values, or between them and the
AFCa. The accumulation factor reported
for 1 ^Cs varies greatly, being 232-15,000
for perch, 195-11,000 for pike, 122-4,850
for roach, 122-895 for bream and 990-1,920
for whi tefish. (-12, 16 ) AFigy observed
Cs
in the Dresden fish is small compared to
these observed ranges. In the presence of
Chicago sewage, however, the Illinois River
does not provide a typical aqueous environ-
ment for fish at the sampling points,
A third basis for comparison is the
observed ratio for 90gr—in case of fish,
the OR, , „ for strontium relative to
bone/water.
calcium, computed by dividing the AFg~ by
S r
the AFr . In Dresden fish, the OR. ,
Ca bone/water
is 450/600 =0.8 for 90Sr and 690/600 =1.2
for stable strontium. A range of values
would be expected because of fluctuations
in the concentrations of ^Sr, strontium
and calcium during the lifetime of the fish.
Reported observed ratios are 0.2 to 0.7 for
s tro n t ium ( 10 , 1 5, 18 ) an(j Q.l 0.4 for
90Sr. U5) The calculated ORbone/water for
strontium and 90gr in Dresden fish are thus
higher than the ranges listed in the
literature.
No other radionuclides were found in
fish. Minimum detectable concentrations set
64
-------
by sample size and sensitivity of radiation
detector were:
Ti ssue
Radio-
nuclide
Carp and
goldfish
Shad
muscle
134CS
1 pCi/kg
3 pCi/kg
bone
89Sr
1,000
1,000
kidney
58Co
100
500
6 0Co
80
300
liver
5®Co
9
40
60Co
7
25
heart
area
131 j
300
800
Shad was analyzed with poorer sensitivity
because the sample was small. Increased
sensitivity is desirable in future analyses
for ®^Sr and
6.4 References
J, U.S. Public Health Service, ''Report on
the Illinois River System'', DWSPC Great
Lakes - Illinois River Basin Project
(1963).
2. Commonwealth Edison Co., ''Preliminary
Design Safety Analysis Report for Dresden
II", Exhibit III-5-2 (1965).
3. Mills, H. B. W. C, Starrett, and F. C.
Bellrose, "'Man's Effect on the Fish
and Wildlife of the Illinois River'',
Illinois Natural History Survey Bio-
logical Notes #57, State of Illinois,
Urbana (1966).
4. Chapman, W. H., H. L. Fisher, and M. W,
Pratt, 1'Concentration Factors of Chem-
ical Elements in Edible Aquatic Organ-
isms'', AEC Rept. UCRL-50564 (1968).
5. Cowser, K. E. , et al., "'Evaluation of
Radiation Dose to Man from Radionuclides
Released to the Clinch River'' in
Disposal of Radioactive Wastes into Seas,
Oceans, and Surface Waters (International
Atomic Energy Agency, Vienna, 1966) p.
639-
6. Essig, T. H., ed,, ''Evaluation of
Radiological Conditions in the Vicinity
of Hanford for 1966", AEC Rept. BNWL-
439 (1967).
7. Kopp, J. F« » FWPCA, Cincinnati, Ohio,
personal communication (1969).
8. Fried, R. E. and J. M. Matuszek, "Second
Quarterly Report, April, May, June, 1968,
Environs Monitoring Program, Dresden
Nuclear Power Station'', Isotopes, A
Teledyne Company, Westwood, N.J. (1968)•
9. Sedlet, J, and F, S. Iwami, ''Environ-
mental Radioactivity at Argonne National
Laboratory, Report for 1964", AEC Rept,
ANL-7104 (1965),
10. Templeton, W. L. and V. M. Brown, "Ac-
cumulation of Strontium and Calcium by
Brown Trout from Waters in the United
Kingdom'', Nature 198* 198-200 (April
13, 1963).
11. Kolehmainen, S., E. Hasanen, and J. K.
Miettineri, ' ' l^Cs Levels in Fish of
Different Limnological Types of Lakes
in Finland During 1963", Health Phys.
42, 917-922 (1966).
12. Brungs, W, A., ''Experimental Uptake of
Strontium-85 by Fresh Water Organisms'',
Health Phys. 11, 41-46 (1965).
13. Krumholz, L. A., E. D. Goldberg and H.
Boroughs, ''Ecological Factors Involved
in the Uptake, Accumulation, and Loss of
Radionuclides by Aquatic Organisms",
in The Effects of Atomic Badiation on
Oceanography and Fisheries, JVAS-NRC
Publication #551, (National Academy of
Science-National Research Council,
Washington, D.C., 1957), pp. 69-79.
14. Nelson, D. J., et al., "Clinch River and
Related Aquatic Studies" AEC Rept,
ORNL-3697, 95-104 (1965).
15. Ruf, M., "RadioaktivitSt in Sflsswasser-
fischen'', Zeit. Veterinarmed. 12, 605—
612 (1965).
16. Gustafson, P. F., A. Jarvis, S. S, Brar,
D. N. Nelson and S. M. Muniak, ''In-
vestigation of l^Cs Freshwater
Ecosystems", AEC Rept. ANL-7136, 315—
327 (1965).
17. Agnedal, P. 0., "Calcium and Strontium
in Swedish Waters and Fish and Accumula-
tion of Strontium-90'*, AEC Rept. AE-224
(1966).
18. Ophel, I. L. and J, M. Judd, ''Skeletal
Distribution of Strontium and Calcium
and Strontium/Calcium Ratios in Several
Species of Fish", in Strontium Metabo-
65
-------
Lism, J. Lenilian, J. Loutit and J. Martin,
eds, (Academic Press, New York, 1967),
pp. 103-109.
19. TempLeton, W. L. and V, M. Brown, ''The
Relationship Between the Concentrations
of Calcium, Strontium and Strontium-90
in Wild Brown Trout, Salmo Trutta L. and
the Concentrations of the Stable Elements
in Some Waters of the United Kingdom, and
the Implications in Radiological Health
Studies'', Int. J. Air Water Poll. 8,
49-75 (1964).
66
-------
7. RADIONUCLIDES IN THE TERRESTRIAL ENVIRONMENT
7.1 Dresden Environment
7.1.1 Site. The Dresden Nuclear Power
Station is located on a 3.9-km2 (953-acre)
tract in Goose Lake Township, Grundy County,
Illinois, on the shore of the Illinois and
Kankakee Rivers (see maps in Figures 7.1 and
7.2). The plant is on rolling prairie that
is readily drained; bedrock is within four
feet of the surface. Plant elevation is
155-160 m. The only higher area near the
plant is Kankakee Bluffs at elevation 180-
190 m to the north and east of Dresden on
the far shore of the Illinois River,
An exclusion distance of 0.8-km radius
surrounds Dresden. Dresden II and III plants
are under construction immediately to the
west of Dresden I and will have similar
exclusion distances. The Midwest Fuel Re-
processing Plant of the General Electric
Company is being built 2 km south of the
Dresden Nuclear Power Station complex.
Surrounding Dresden are small farms growing
field corn, pasture grass for grazing beef
cattle, and, to a lesser extent, soybeans
and winter wheat. Eleven relatively small
dairy herds —some of only 2 to 4 cows —
were seen at distances between 3 and 20 km
from Dresden. Wooded areas consist of the
McKinley (Channahon) State Forest Preserve
on Kankakee Bluffs, and the Des Plaines
Wildlife Conservation Area, east of Dresden
between highway US 66 and the Kankakee
Cutoff. There are several abandoned strip
wines 10 km south of Dresden, and a small
mine operates 3 km south. In addition to the
Kankakee, Des Plaines, and Illinois Rivers,
there are sm.all streams in the neighbor-
hood, including the Illinois and Michigan
Canal, the DuPage River emptying into the
Des Plaines River 5 km NE, the Aux Sable
KEY
"-—rainwater
C—CORN
R---RABBITS
F— LEAFY VEGETABLES
HEIFERS
U.S. ROUTE 6
OC1
OC3
OR
SCALE. Km
Figure 7,1 Sampling locations' in immediate
vicinity of Dresden Nuclear
Power Station,
Creek flowing south into the Illinois River
5 km W, and the Mazon River flowing north to
the Illinois River 11 km SW of Dresden, The
entire area is accessible by highways and
dirt roads that generally lie on a 1-mile
(1.6 km) grid pattern.
67
-------
KEY
F...LEAFY VEGETABLES
W...WATER
M...MILK
C...CORN
D...DEER
S...SNOW
0 1 2 3 4 5
JOUET
L
ELhOOD
JOL ET
ARSENAL~|
KANKAKEE
RIVER
Figure 7.2. Sampling locations in general vicinity of Dresden Nuclear Power Station.
68
-------
The nearest, homes are cottages 1.2 km
SSE of Dresden along the west bank of
Kankakee River, 2 houses on the Kankakee
Bluffs approximately 1.4 km NE of Dresden,
and the operating station at the Dresden
Dam and Locks, 1.4 km NW of Dresden. Within
a 5-km radius, there are numerous cottages
on the island SE of Dresden formed by the
Des Plaines River, Kankakee River and
Kankakee Cutoff, and scattered farm houses.
The town of Channahon (pop. 1,200), 5 km
NE of Dresden, is the largest population
center near Dresden. Within 13 km of
Dresden are Morris (pop. 7,900) to the west,
and the smaller towns of Coal City and
Wilmington, S and SE, respectively. Large
cities in the vicinity of Dresden are
Joliet (pop. 67,000), 20 km NE, and Aurora
(pop. 64,000), 40 km N. Chicago is 80 km
NE of Dresden.
The largest industrial complex near
Dresden is the Joliet arsenal, 9 km E. The
north shore of the Illinois River is being
developed as an industrial area, and there
are factories along highway US 66, 6 km to
the east.
7.1.2 Environmental surveillance. It was
the purpose of this study to demonstrate
and test sensitive and informative monitor-
ing techniques rather than to parallel the
extensive surveillance program that is
carried out at Dresden. Emphasis was placed
on collecting foods (as direct sources of
radiation exposure to humans) or indicators
of radioactivity concentrations in foods,
measuring even very low concentrations of
radionuclides rather than reporting less-
than values, and comparing measured con-
centrations with estimated values. Estimates
were based on release rates at the Dresden
stack, meteorological data, diffusion cal-
culations, and environmental and biological
transfer coefficients. The study criteria
were met in several instances, but further
efforts are required to measure very small
amounts of radionuclides in a number of
medi a.
Environmental surveillance that provides
specific information about radionuclide
concentrations is difficult at many nuclear
facilities, including Dresden, because
release rates of radionuclides to the air
are low, and radionuclides in fallout from
atmospheric nuclear tests interfere with
analyses. Of the radionuclides discharged
at the Dresden stack, 3H, ^°Sr, and ^^Cs
are also continuously deposited in fallout;
the p resence and relative concentrations of
131j^ l40ga) anj 89gr jn fallout
depend on
the time interval between the tests in which
the fallout radionuclides were formed and
sample analysis. Short-lived radionuclides
in fall out during the study period were
derived from the mainland Chinese atmospher-
ic nuclear test on December 24, 1967. Other
possible, although unlikely, sources were
leakage from underground and cratering tests
in Nevada on Jan. 18, Jan. 26, and March 13,
1968, and the French atmospheric nuclear
tests in the South Pacific on July 7» July
15, and Aug. 3, 1968.
Radionuclides that could be attributed
to Dresden stack effluent if found in the
immediate neighborhood of Dresden include
the short-lived noble gases, their short-
lived progeny, and 58Co and 60Co; these are
released at the Dresden stack (see Section
4,1) and are usually not detected in fallout
from nuclear tests. The short-lived noble
gases and their short-lived progeny do not
remain long in env i ronmen t al samples,
however, and radiocobalt is released at the
stack in extremely low amounts (see Table
4. 6).
As an alternative approach, radionuclide
concentrations were compared in samples
collected near the stack and at a distance
from it, or in the downwind direction versus
upwind. Higher concentrations of indicator
radionuclides in the nearby or downwind
samples may be attributed to discharge at'1
the Dresden stack. Strontium-89 and 131j
were selected as indicator radionuclides
for deposition, because their release rates
were highest among stack effluents other
than noble gases and tritium. The release
rate of ®^Sr in stack effluent is actually
higher than measured at the stack because
it is formed in the 8^Kr-89Rb-8^Sr decay
chain to the extent of 42 X 10"6 fd 89Sr
per fj£i 8%r at maximum ingrowth (after
100 minutes). At the average gaseous fission
product release rate of 12,500 /xCi/sec
during operating periods in 1968, and a
1.2 percent 89Kr content relative to the
69
-------
nominal, gaseous fission product release at
the stack (see Table 15.3), ingrowth added
89Sr at the rate of 42 X 10~6 X 12,500 X
0.012 - 6.3 X 10"3 /xCi/sec to the 1,0 X
10"3 /iCi/sec measured at the stack. Thus,
the virtual release rate to air increases
with travel time from the value measured at
the stack (1.0 X 10"3 /iCi/sec) to the total
ingrowth value (7.3 X 10~3 ffCi/sec) at 100
minutes and longer.
The longer-lived radionuclides, ^^Co,
90Sr, and 137Cs can be used as indicators
of long-term accumulation. Measurement of
^'Cs was emphasized because, of the three,
it was released at highest average concen-
tration (see Table 4.6) from the stack, and
also is formed in air by decaying ^^Xe.
The activity of ^'Cs reaches 0,25 X 10*^
fi£.i per fjCi of ^^Xe after 25 minutes, and
2.8 percent of the nominal gaseous fission
product release rate at the stack is ^"Xe
(Appendix B. 3). Hence, ingrowth added l^Cs
at the rate of 0.25 X 10"6 x 0,028 * 12,500
= 88 X 10" /iCi/sec to the average rate at
the stack of 35 X 10"6 fJZi/sec.
The results of this study are summarized
by sample types in Sections 7.3 to 7«8« Only
in a few instances—131j in three cattle
thyroids (Section 7,7)» ®^Sr in one snow
sample (Section 7.3), ^7Cs in one sample of
field corn (Section 7,5)—may the detected
radioactivity be attributable to stack ef-
fluent at Dresden, All other measurements
are reported to describe analytical tech-
niques (Section 7,6, for ISlj in milk) and
to report the absence, at the indicated
levels of detectability, of radionuclides
attributable to Dresden.
Other information on radionuclides in the
environment of Dresden is available in the
report of Dresden's contractor for environ-
mental surveillance,^^ The contractor's
program at the time of this study included
the following:
air filter gross beta and ^lj analysis
milk 13lj^ 137qS( 89gr> anfj 90gr
analysis
well water gross beta analysis
rainwater gross beta analysis
surface water gross beta, ^H, ®^Sr, and
90Sr analysi s
vegetation gross beta, gross gamma, ®^Sr
and 90Sr analysis
soil gross beta, gamma-ray spectral, ®^Sr
and ^"Sr analysis
externaL radiation exposure rates
In addition, the Illinois Department of
PubLic Health has analyzed surface and well-
water samples for gross alpha and beta
activity;(2) the Argonne National Laboratory
has analyzed water and silt samples in the
DuPage River at Chan n a ho n and in the
Illinois River at Dresden Dam and Morris
for gross alpha and beta activity; ^ the
Federal Water Pollution Control Administra-
tion (FWPCA) analyzes Illinois River water
at Morris for 90Sr and gross alpha and beta
activity; and the Public Health Service
(PHS) analyzes milk at Chicago for ®^Sr,
^Sr, '3~Cs, and ^^Ba, and surface
air and precipitation at Springfield,
Illinois, for gross beta activity. The FWPCA
and PHS data are reported at regular in-
tervals in Radiological Health Data and
Reports.
7.2 Estimation of Radioactivity
Concentrations
7,2,1 Precipitation. Deposition by wash-
out, W (in pCi/m^), for ®^Sr in rain and
snow was estimated by the following equa-
tion, derived from equation 5.6 of Slade:
Qo L T exp (-L x/u)
where Q^: virtual release rate at stack,
pCi/sec
L : washout coefficient, sec"'
T : duration of washout, sec
9 : sector width, radians
u : wind speed at release height,
m/sec
x : distance from stack to sampling
point, m
Values of Q^, T, 9, u, x, and the resulting
W are given in Appendix D. 1. The virtual
release rate for ^Sr was the average re-
lease rate at the stack from Table 4.6,
70
-------
plus a value based on decay that in-
creased with the travel time of the plume
as indicated in Section 7.1.2. The value of
L for was estimated to be 1 X 10"^
"I ^^ Deposition values were converted
sec
to concentrations in water by dividing by
the mm of rainfall, and by the cm of snow-
fall.
7.2.2 Deposition. To estimate dry deposi-
10 1
tion of 1J1J on pasture grass for uptake by
dairy cows and beef cattle, and the con-
centration of ^Sr on Soil, leafy vege-
tables, corn husks, and grass, equation
5.44 of Slade^4) was integrated with respect
to the crosswind direction and then distrib-
uted across an appropriate sector width,
generally 10°. The equation was generalized
to:
(2/77) 1/2 VdQxT
D = * I~
exp [~ h2/2 a-2]
x cr u
z
where:
(7.2)
D = deposition, pCi/m2
v^ = deposition velocity, m/sec
Q'x = depletion-corrected release rate
at point of interest, pCi/sec
T = total duration of deposition,
sec
6 = sector width, radians
x = distance to point of interest,
meters
er - standard deviation of vertical
concentration distribution,
meters
u = release height wind speed, m/sec
h = effective release height, meters
Hie deposition velocity on pasture grass and
other vegetation was taken to be 3 X 10"3
m/sec^ for 89Sr and 1 X 10"2 m/sec (6) for
1311, To compute the radionuclide concen-
tration in grass, it was assumed that
deposited activity was completely retained,
that the average grass density was 0.33 kg
dry weight/m2,^^ and that ash constituted
7 percent of dry weight, Concentrations
in cabbage were based on a published ratio
of concentration in cabbage hearts to ground
contamination, For corn husks, 10 percent
retention of deposition and a crop yield of
1 bushel of whole ears per square meter were
assumed.
Dry deposition at a distance—for the
background samples—was simplified by com-
puting average values over the entire time
interval of interest for stable and neutral
conditions. Deposition during unstable con-
ditions and rainstorms was judged to be
relatively insignificant during the periods
of interest. Based on the derivation in
Appendix D. 2, the simplified equations at
locations 22 and 26 km NNE were:
D
0.19T
tab 1 <
7.93 X ]0
4
D
neutral
Q. Q34T
4.68 x 104
(7.3)
(7.4)
D = deposition, pCi/m2
T = interval duration, sec.
Disposition during rainfall near Dresden
was computed according to equation 7.1. Con-
centrations in vegetation were derived from
washout with the same factors that were
used for dry deposition. The value of L for
^^1 was selected from Slade's Figure
5. 12. (4)
Examples of deposition estimates for
and 8^Sr are given in Appendices D.3 to
D.9. The deposited radionuclide was summed
for the entire period that contributed
toward the radioactivity at the time of
measurement, as shown in Appendices D.7 to
D,9, correcting for the decrease of radio-
nuclide concentration through decay and
transfer to other media. For Estimating
137Cs concentrations in soil, the following
were assumed: an average virtual release
rate at the stack of 72 pCi/sec (which
includes partial ingrowth from the i37Xe
parent), the same deposition velocity and
washout coefficient as for ®^Sr, complete
retention in soil (except for radioactive
decay) and 50 percent retention in the top
1 cm, and 137Cs accumulating over the 7-year
operating period, adjusted for 20 percent
down-time.
71
-------
7.2.3 Uptake in cattle thyroids and
transfer to cows' milk. From the estimated
deposition of during 20 days before
milk collection, levels of *31j were
predicted in Appendices D. 11 and D.12 from
the graph by Garner and Russe 11 ^ 1 0 ^ fo r
which values are shown in Appendix D. 10. The
daily intake of 131j was related to levels
in milk at specified times by correcting for
decay of 131I on grass (Tj >2 = 5 days),
assuming that a cow effectively grazes
45 per day, and summing 131j doses on
the dates of deposition.
The estimate of 131j ln the thyroids
of three heifers that grazed for three
weeks prior to slaughter near the Dresden
stack was based on Garner and Russe 11 ' s
model (Appendix D. 10 ) . It was assumed
that 20% of the dai ly intake of 1 3 1 [
goes to the thyroid ^0) and that 1 3 1 J
turns over in the thyroid with a 7-day
half life^l' (Appendix D. 13).
7.3 Rain and Snow
7.3.1 Samples and analyses. Radionuclides
released from the stack are transferred
to soil and vegetation near Dresden by
precipitation and dry deposition. A pre-
liminary estimate suggested that collection
of several hundred liters of rain water
would be necessary to detect ^Sr, 131j( or
1*°Ba from the Dresden stack at ground
level. One set of 1-liter rain samples was
collected, nevertheless, and analyzed for
radiostrontium and radionuclides that emit
gamma rays. Two snow samples were collected
for the same purpose.
Rain water was taken from puddles and
ditches within 3 days after the tropical
storm of June 22-24, 1968, at the six loca-
tions near Dresden listed in Table 7. 1;
a rain collector at a dairy 22 km NNE
of Dresden provided a background sample.
Snow was collected four days after the
snowfall of January 13-14, 1968» from the
surface of areas approximately 1-m square,
at the two locations shown in Figures 7.1
and 7.2. The area near the meteorological
tower, 0.8 km SSW of the stack, was beneath
the plume from Dresden during snowfall,
but not in the period between the end of
snowfall and sampling. The area at the
intersection of highways US 6 and 66, 10
km NE of the stack, was upwind from Dresden
during the snowfall. Upon melting, the
downwind sample contained 3.5 liter, and
the upwind sample, 5.0 liter.
The samples were evaporated to 40 ml and
analyzed by gamma-ray spectrometry with
10 X 10 cm Nal(Tl) detectors. Aliquots were
analyzed radiochemically for ®^Sr and 90gr>
The rain samples were also analyzed radio-
chemically for j-37qS) ancj the snow samples,
Tab Ie 7.1
89Sr, 90Sr, and 137Cs in Rain Water, pCi/liter
#
Location
Col lection
date, 196B
Measured
Estimated
137Cs
90Sr
89Sr
89Sr
1*
3.2 km W
June 25
< 0.2
2.7
< 1
2.0 x 10*4
2
0.8 km S
25
< 0.2
2.0
< 1
0
3
0.8 km SSW
27
< 0.2
3.4
< 1
0
4
2.4 km ESE
26
< 0.2
5.6
< 1
5.2 x io"4
5
1.5 km N
26
< 0.2
1.3
< 1
7.2 x 10"4
6
1.6 km NNE
27
0.4
3.6
< 1
0
7
22 km NNE
25
< 0.2
0.8
< 1
0
~Locations of #2 to 6 are shown in Figure 7.1, #1 and 7 are shown in Figure 7.2.
Mote: < values are 3 o- counting errors.
72
-------
for 3H. Snow was analyzed for 6 ^Co by
coincidence spectrometry.
7.3.2 Results and discussion, 'lhe rain-
water samples do not appear to contain
radionuclides from Dresden, Only 90Sr was
found in all samples (see Table 7,1); in
the ab sence of 89Sr, the 90Sr is at tributed
to fallout. Concentrations of ®9Sr and i3^Cs
were below the limits of detectabi1ity
(except for one ^'Cs value), and no radio-
nuclides (< 3 pCi/1) that emit gamma rays
were found by spectrometry. Concentrations
of ®9Sr from Dresden were estimated in
Appendix D. 1 to be three orders of magnitude
below minimum detect abl e concentrations.
The est imates are quite approximate, how-
ever, because values of all the predictive
components, especially the washout coef-
ficient, are so uncertain.
The downwind sample of snow near Dresden
contained **9Sr while the upwind sample did
not (see Table 7.2), suggesting that the
89Sr was released at the Dresden stack. The
89Sr concentration of 2.3 X 10"2 pCi/liter,
estimated in Appendix D. 1, is lower by 400,
but washout coefficients for snow are even
more uncertain than for rain.^ All other
radionuclides are at similar concentrations
jn the two snow samples, and are therefore
attributed to fallout from atmospheric
nuclear weapon tests, especially the Chinese
test on December 24, 1967. Higher-than-usual
gross beta values in two samples collected
early in January by Dresden's contractor
for environmental surveillance are also
associated with this nuclear test.
Although the measured concentration of
89Sr in snow is 300 times lower than the
permissible concentration for drinking water
of 3000 pCi/liter, and the less-than values
0f 89Sr in
rain water are even lower, ad-
ditional measurements of ®^Sr in large
precipitation samples would be desirable in
view of the uncertain values of washout
coefficients. Analysis of snow to check
the detection of 89Sr would be of special
interest.
7.4 Soil
7,4.1 Samples and analyses. Soil may
accumulate radionuclides deposited in pre-
Table 7.
2
Radionucl
ide Content of
Snow, pCi/liter
Near
Radio-
Meteorological
Intersection
nucl ide
Tower
US 6 & 66
3H*
500 ± 200
600 ± 200
60Co
< 1
< 1
88Sf
10 ± 2
< 1
90Sf
2.5 ± 0.1
2.0 ± 0.1
95Zr
55
35
1 03Ru
25
30
106Ru
15 ± 10
< 10
131 ]
10
10
'3?Cs
< 10
15
,40Ba
40
25
141Ce
35
25
analysis by SERHL.
Notes:AlI analytical 2 c- values are ± 5 pCi/liter
except as shown; < values are 3 o- counting
error.
Concentrations corrected for decay to Jan.
18, 1968.
cipitation and from air, and transfer these
radionuclides to food and vegetation; long-
lived radionuclides such as ^Sr and ^^Cs
accumulate in soil over many years. Samples
were collected at five locations within 0.9
to 3.2 km of Dresden, at the same location
as the corn samples (see Figure 7.1), so
that radionuclide concentrations in corn
kernels and soil could be compared.
Soil was dried at 110°C, and samples of
400 cc—approximately 500 g—were analyzed
by gamma-ray spectrometry with a 10 X 10 cm
Nal(Tl) detector. Aliquots of 5 g were
analyzed radiochemically for 89sr and 90Sr,
and other aliquots were analyzed for stable
strontium and calcium.
7.4.2 Results and discussion. Gamma-
ray spectral analysis showed 1:^Cs (see
Tabl e 7. 3) and the naturally occurring
radionuclides 40K, ^"^Th, and 226Ra. Concen-
trations of and ^^Cs
were each ap-
proximately 0.3 pCi / g dried soil. No
73
-------
Table 7.3
Concentration of Radionuclides and Stable Ions in Dresden Soil, August 21, 1968
Stable Ions Measured Radionuclides,
Samp 10 Sample s»'' !"'/» s°'1 Estimated >«Cs,
Location wt., g K Ca Sr 89Sr 90Sr 137Cs pCi/g dry soil
#1 -
1.7
km
NE
470
13
3.3
0.015
< 2
0.3
±
0.1
0.40
±
0.10
2 x 10"5
#2 -
1.6
km
N
470
13
6.5
0.020
< 2
0.3
±
0.1
0.30
±
0.08
2X10-5
#3 -
1.7
km
E
540
11
3.3
0.011
< 2
< 0.1
0.20
±
0.05
2X10"5
#4 -
3.2
km
W
480
13
4.8
0.013
< 2
0.3
±
0.1
0.29
+
0.07
6 x 1 0"6
#5 -
0.9
km
S
300
10
3.5
0.011
< 2
0.2
±
0.1
0.40
•jr
0.10
2 x 10"5
Notes: 1. ± values are based on 1 a counting error for sample and < values are based on
3 cr estimated counting error in background, except that uncertainty in ,37Cs
measurements is estimated to be ± 25%.
2. Estimated concentrations of 90Sr are less than 1 percent of estimated ,37Cs
values at every location.
89Sr (< 2 pCi/g) was found, Dresden's con-
tractor for surveillance reported 9®Sr con-
centrations of 1.8 and 1,6 pCi/g, arid
concentrations of 1.9 and 1.8 pCi/g in
June, 1968. Estimated ^^Cs concentra-
tions, based on accumulation over 7 years
as described in Section 7.2.2, were lower
than measured values by four orders of
magnitude, suggesting that the measured
concentrations of the two radionuclides are
not attributable to routine releases from
the Dresden stack.
7.5 Food and Feed
7.5.1 Samples and analyses. Foods are a
potential vector for the transfer of radio-
nuclides to humans from both soil and air,
but only a few private vegetable gardens
grow food near Dresden. A bushel basket of
leafy cabbage plus a few heads of leaf
lettuce were obtained on June 26, 1968,
from two gardens ?.t Channahon, 3.8 and
5.4 km NE of Dresden (see Figure 7.1).* As
a background sample of leafy vegetables,
only mustard greens, purchased at a large
truck farm near Plainfield, 26 km NNE of
Dresden, were available.
A bushel basket of field corn was col-
lected on August 21, 1968, at each of the
*We thank Mr. A. McDonald and Mrs. Hulbert for
providing these samples.
five locations near Dresden shown in Figure
7.1; a bushel of sweet corn grown near
Gibson City, 111., 110 km S of Dresden, was
obtained on August 22 for background
measurements.** Grass was collected at two
dairies, on the pastures used for grazing
by the cows whose milk was analyzed (Section
7.6). Hie grass was cut on June 26, during
the period of milk collection.
The leafy vegetables, grass, corn kernels
and corn husks were each analyzed by gamma-
ray spectrometry with the 10 X 10 cm
Nal(Tl) detector. The samples were then
ashed and reanalyzed by gamma-ray spectrom-
etry. Aliquots were analyzed for ®^Sr,
90Sr, stable strontium, and calcium."^"
7.5.2 Results and discussion. The leafy
vegetables and grass contained 2 to 6 pCi
90Sr per gram ash and no detectable ®^sr
as shown in Table 7.4. The gamma-ray
spectra showed the usual longer-lived
fission-products, including I41/144ce
1 0 3/106pu^ 137qS) ancj 95£r + 95^]-^ that
were in fallout from nuclear tests at the
time of sampling. The Dresden contractor,
however, reported detectable concentrations
**We thank Messrs. Dirker, Vandborg, and Henker,
Stokely-Van Camp, Inc., and the Commonwealth
Edison Company for providing the corn.
^"We thank Mrs. T-, L. Rehnberg and Mrs. A.
Strong, SERHL, for analyzing the leafy vege-
tables and corn.
74
-------
Table 7.4
Radiostrontium Concentration in Vegetables and Grass, June 26, 196B
Cabbage & Lettuce, Mustard Greens, Grass, Grass,
3.8 and 5.4 km NE 26 km NNE 3.4 km W 22 km NNE
measured estimated measured estimated measured estimated measured estimated
Wet weight, kg 3.42 7.35
% Dry weight 11.1 6.8
* Ash weight 4.29 1.12
89Sr, pCi/g ash < 0.2 1.5 x 10'6 < 0.2 8.4 x 1 0_B < 1.0 4.1 x i(T2 <1.3 1.9 x 10~2
90Sr, pCi/g ash 2.2+0.2 — 1.8 ± 0.2 — 5.9 ±0.2 — 2.3 ± 0.2
Ca, mg/g ash 62 — 93 44 — 25
Sr. /jg/g ash 140 — 140 — 140 — 310
Notes: 1. 90Sr values are + 2 a, based on estimated counting error; less-than values for B9Sr are based on 3 a
estimated counting error.
2. Estimated 89Sr values trom Appendices 0.7, 0.8, and D.9.
—-4
cn
-------
of 89Sr (1.6 to 1.9 pCi/g ash) in three
vegetation samples collected in June; his
strontiurn-90 concentrations were 3.5 to
3.6 pCi/g ash, similar to values reported
here. ^^ Hie radionuclides are attributed
to fallout because the gamma-ray spectra
were similar in the near-by and distant
samples of grass and leafy vegetables, and
because 89Sr concentrations were lower than
concentrations. The concentration of
e^Sr estimated from stack releases at
Dresden to be in the nearby grass is ap-
proximately 20-fold lower than could be
measured. Because the estimated values for
the leafy vegetables are based on cabbage
hearts, a more appropriate value may lie
between the given estimates and those for
grass. The results of the analyses of
leafy vegetables should be checked by
measurements of washed samples because the
observed ash weight in this sample is un-
usually high. It is possible that the ash
contained some soil.
Concentrations of 90§r and ^^Cs also
were of the order of 1 pCi/g ash in corn
husks (Table 7.5). Strontium-89 was not
detected. Corn husks, like leafy vegetables
and grass, would be expected to accumulate
most radioactivity from deposition of air-
borne particles.
The corn kernels, which are relatively
sheltered from airborne radionuclides,
contained undetectably low levels of
and 9^Sr; concentrations of ^?Cs were, with
one exception, between 0.2 and 0.8 pCi/g
ash (see Table 7.5). Gamma-ray spectra
indicate only ^7Qg anc| naturally occurring
10K (see Figure 7.3). The highest concen-
tration of 13?C.s was 4.3 pCi/g ash in the
corn grown near the meteorological tower,
1). 9 km S of Dresden. The field corn is used
for .animal feed, not for human consumption.
It would be of interest to find the reason
for the elevated level of ^?Cs, especially
since the ^^Cs concentration was not
correspondingly higher in the soil sample.
7.6 Milk
7.6.1 Samples. Milk is a major potential
vector for the transfer of radionuclides to
the population. If dairies are located
near nuclear power stations, milk samples
are usually analyzed as part of the environ-
Table 7.5
Concentrations of Radionuclides and Stable Ions in
Corn Kernels and Husks, August 21, 1968
Wet wt. % Dry % Ash mg/g ash pCl/g ash
Locat ion
kg.
wt.
wt.
K
Ca
Sr
89Sr
90Sr
137Cs
Kernels
#1 - 1.7 km NE
4.21
46.9
0.87
350
1.2
0.009
< 1
< 0.1
0.2 ± 0.1
#2 - 1.6 km N
4.40
30.6
0.86
410
1.6
0.012
< 1
< 0.1
0.4 ± 0.1
#3 - 1.7 km E
3.94
35.1
1.02
380
1.5
0.014
< 1
< 0.1
0.8 + 0.2
#4 - 3.2 km W
3.48
43.5
0.86
350
1.7
0.015
< 1
< 0.1
0.8 ± 0.2
#5 - 0.9 km S
2.44
30.6
0.81
380
2.6
0.017
< 1
< 0.1
4.3 ± 0.2
n - 110 km S
3.82
37.1
0.92
390
1.7
0.014
< 1
< 0.1
0.7 ± 0.2
Husks
#1 - 1.7 km NE
2.22
27.7
CO
CO
•
240
18.7
0.036
< 1
0.7 ± 0.3
0.4 ± 0.2
#6 - 110 km S
1.72
20.5
1.00
290
19.2
0.050
< 1
0.6 ± 0.3
1.1 ± 0.2
± value based on I a estimated counting error for particular sample.
< values based on 3 a estimated counting error tor background sample.
Standard deviation of duplicate analyses was ± 0.3 mg calcium/g ash, ± 10 percent for
potassium, and ± 25 percent for stable strontium.
-------
CO
c
S>
O
o
9 km S
7 km NE
0.01
ENERGY, MeV
Figure 7.3. Gamma-ray spectra of corn
kernels. Detector: 10 x 10 cm
Nal(Tl) at SERHL. Sample:
11.3 g ash of corn collected
0.9 km S of Dresden and 21.7 g
collected 1,7 km, NE of Dresden
on 8-21-68. Counts: 50 min.
on 9-12-68 (bgd subtracted).
mental surveillance program. At Dresden, the
contractor for environmental surveillance
collects weekly composites of daily samples
at two dairies located 10 and 22 km NNE of
Dresden. He reports weekly average con-
centrations of an(j mC)nthly averages of
B^Sr, 90sr> anc| 137cs. (1) Any significantly
higher values at the nearby dairy would
suggest that radionuclides from Dresden have
entered the milk. During the second quarter
of 1968, the ranges of reported values
were as follows:
131I 0.8 - 3.8 pCi/liter
137Cs 7.0-13.1
89sr 2.7 - 4.6
90Sr 2.4 - 7.4
Concentrations at the nearer dairy were not
significantly higher than at the farther
dairy, suggesting that these radionuclides
originated in fallout from atmospheric
nuclear weapon tests.
A preliminary estimate of radionuclide
concentrations in milk at the nearer dairy,
based on radionuclide release data in Table
4.5, indicated that could be detected
with the greatest sensitivity among these
radionuclides, but that its concentration
would be below the limit of detectability
of 0.1 pCi/liter. It was considered more
probable that 131j could be detected in
milk of the dairy herd nearest Dresden,
3.4 km west (see Figure 7.2). "Hie herd con-
sists of 11 Holstein cows, and the milk is
grade B—not bottled for sale. During the
grazing season, however, the wind very
infrequently blows from Dresden toward the
pasture. After awaiting this occurrence
throughout spring and summer of 1968, it
appears that the recorded incidence of winds
at 75° to 85° consists mostly of rotation
through this angle for short periods.
Upon observing that the wind had been in
the 75° to 85° sector for1 several hours on
June 22, milk samples were collected at the
dairy west of Dresden in the evenings of
June 25 and the following two days.* Each
consisted of 45 liters of milk produced by
5 cows selected at random. For comparison,
45-liter samples were taken on the first
and third day at the farm 22 km NNE of
Dresden that supplies weekly composites to
Dresden's contractor for environmental
surveillance.* These samples represented
the combined milk of all cows (12-15
Holsteins). One sample at each location had
been collected previously to test collection
and analytical procedures.
7.6.2 To concentrate ^3^I,
22.5-liter portions of each sample were
passed through 80 ml Dowex l-x8 anion-
exchange resin (Cl~, 20-50 mesh) in a 3. 1-
cm-diameter column. The flow rate was
initially 100 ml/min and decreased slowly
with time. Hie resin was washed with water,
transferred to a Petri dish (9.0-cm dia.
•We thank Messrs. A. Dirker and H. Dhuse for the
milk samples.
77
-------
X 1.5 cm high), and counted for 300 to
1000 minutes with either a 10 * 10 cm
Nal(Tl) detector plus multichannel analyzer,
or two such detectors facing each other
within an annular anticoincidenee shield.
A 100-keV range at the 364-keV character-
istic photopeak was used to compute the
I T 1
amount of 1J1I in the sample.
Recovery of by this procedure had
been found to be 90 ± 5 percent by tracer
tests with in vivo spiked cows' milk and
by comparison with gamma spectral analysis
of milk that contained from fallout
at the Nevada test site, 113) The minimum
detectable concentration, based on the 3-
sigma statistical deviation at a background
of 30 counts per minute and a counting
efficiency for 131j 0f
either 30 percent
(sum/anticoincidence) or 16.5 percent
(single detector) was 0.07 and 0,13
pCi/liter, respectively. Examination of the
reproducibility of background measurements
and of 131I samples in the range of 1 to
10 pCi confirmed a minimum detectable value
of 0.1 pCi/liter, In late June and early
July, however, high background values in
the counters increased the minimum de-
tectable levels (3 sigma of deviation of
background values for 300 to 1000 minutes)
to 0.3 and 0.5 pCi/liter, respectively, at
the time of counting. Correction for radio-
active decay from the time of sampling
increased these minimum detectable values.
7.6.3 Results and discussion. No
was found, as shown by the *'less-than* '
values in Table 7.6, suggesting that neither
fallout from atmospheric testing of nuclear
devices nor releases from Dresden caused
"I n i ...
I concentrations in inilk to reach 0.6
pCi/liter, The values for the herd 22 km
NNK of Dresden disagree with a concentration
of 1.6 ±0.4 pCi /liter in Table 3 of the
report by Dresden's contractor,''' The
1311 detected in the contractor's weekly
composite may have originated in samples
from the 5 other days, but a more probable
cause is systematic error in analysis by a
small but constant amount.
The concentrations predicted in Ap-
pendices 1). 11 and I). 12 from stack releases
support the measured ''less-than'' values,
as shown in Table 7.6. Estimated concentra-
tions in the milk of cows grazing 3.4 km
west of Dresden for released from the
stack were approximately 10-fold less than
could be measured, and concentrations in
the milk of cows grazing 22 km NNE were
50-fold lower. The estimated values are
quite approximate, in that variations by
factors of at least two may be expected in
each of the following: release rate, dilu-
Table 7.6
,3,1 Concentration in Raw Milk, pCi/liter
3,4 km W 22 kin HNE
Date, 1968 measured estimated measured estimated
May 7 < 0,30 0* < 0.17 0*
<0.14 <0.17
June 25 < 0.60 0.047 < 0.67 0.013
<0.71 <0.60
June 26 < 0.71 0.075
< 0.71
June 27 < 0.67 0.090 < 0.62 0.013
<0.71 <0.71
Notes: 1. Directions and distances are from Dresden stack.
2. "Less-than" values are 3-sigma for measured mean detector backgrounds.
3. Duplicate samples were analyzed for 4 evening mHkings at nearer farm,
and for 3 evening milkings at farther farm; values are at time of milking.
""Dresden reactor was shut down for refueling.
78
-------
tion in air, deposition velocity or washout
coefficient, transfer from grass to cow, and
metabolic transfer to milk.
It would be desirable to repeat these
measurements at the nearer pasture under
circumstances that might yield definite
13*1 values. For example, improved stability
in detector background would reduce minimum
detectable concentrations to approximately
0.1 pCi/liter; and the five-fold higher
releases of 131| that have been measured
(see Table 4.5) would lead to concen-
trations of 0.3 pd/liter under similar
meteorological conditions. On the other
hand, occasions for sampling at detectable
concentrations are infrequent because pre-
vailing winds are not to the west, and the
farm has been sold, so that dairy operations
at this location will probably cease.
7.7 Cattle Thyroids
7.7.1 Samples. Cattle thyroids are not
eaten (to the best of our knowledge) and
therefore are not a vector in the transfer
of 131I to man. They are sensitive indi-
cators of 131j on pasture, and potentially
in milk, however: 12 pCi 13iI/g of thyroid
has been taken to be equivalent to 1 pCi
13*I/liter of milk, Small herds of beef
cattle were observed to be on pasture in
several directions from Dresden within a
few kilometers.
Use of cattle thyroids as indicators for
131j can only be recommended under defined
conditions. By common practice, beef cattle
are removed from pasture and given stored
feed for several weeks before slaughter, so
that any J I from grazing would have de-
cayed appreciably at the time of slaughter.
Metabolic and dietary variations signif-
icantly affect the uptake of 131j j-,y the
thyroid, and may reduce it drastically. ^5^
Moreover, the relative concentrations of
jn milk and thyroid are not constant,
but depend on the time interval between
uptake by the cow and measurement.
At our request, three heifers were kept
on pasture 2.3 km east of Dresden (see
Figure 7.1) from June 16 until they were
shipped on July 7 for sale and slaughter.*
~We thank Mr. M. McDonald for making these
heifers available to the study.
The three heifers were 1'back-tagged'' to
identify them at slaughter, Tluir thyroids
were removed, placed in formaldehyde and
mailed at Green Bay, Wisconsin on July 10.**
Thyroids of five steer from more distant
locations were obtained on July 29 at
Morris, 111.1" Although intended as ''back-
ground'' samples, they were not, because of'
the difference in date of slaughter and the
stored feed consumed by these cattle before
slaughter.
7.7.2 Analysis. The thyroids were
measured for 131j content by placing them
in Petri dishes on the Nal(Tl) detector or
within the 2-detector/annulus system, in the
same way that in milk had been analyzed
(Section 7.6.2)» Spectra were accumulated
for 300 to 1,000 minutes, and 131j was
determined from the count rate of the
characteristic 364-keV gamma ray. The
minimum detectable 13lj activity at the
time of counting (3 sigma of counting
error) was 3 pCi; computed minimum de-
tectable levels at sampling were higher
because of *31j decay.
7.7.3 Results and discussion. As shown
in Table 7.7» thyroids from the three
heifers that had grazed 2.3 km east of
Dresden contained measurable amounts of
13*1, while the other thyroids did not.
The magnitude of the peak in the former
thyroids is indicated in Figure 7.4. The
estimated value for cattle grazing 2.3 km
east of Dresden, computed in Appendix D.13,
agrees with the average of the three
measured values. The estimation is subject
to all the uncertainties discussed in
Section 7.6.3, and the agreement therefore
is appreciably better than expected. At the
12/1 ratio, the indicated 13*1 concentra-
tion in milk, if milk cows had'grazed on
the same pasture, would be 0.04 pCi/liter.
The excellent agreement between measured
values and the estimate based on *31j re_
lease at the Dresden stack suggests that
**We thank Dr. LeVan, DVM, Meat Inspection Pro-
gram, USDA, for providing these samples.
"f"We thank Mr. Floyd Schaible, Circle S Foods,
for providing these samples and Dr. R. Conner,
DVM, for identifying the thyroids at slaughter.
79
-------
Table 7.7
,31| Content of Cattle Thyroids
Sample
Location
Date of
slaughter
Thyroi d
wt., g
13,l Content
at slaughter,
pCi
2-yr old
hei fers
2.3 km E
July 10,
73
39 ± 6
1968
78
23 ± 5
58
30 ± 6
Average
31
Estimated
28
2-yr old
steer
21 km ENE
July 29,
27
< 9
26 km W
1968
26
< 5
38 km SW
69
< 7
5.6 km NW
24
< 5
11 km N
27
< 6
Notes: 1. Directions and distances are from stack.
2. ± values are at 1-sigma level for counting error.
3. "Less-than" values are 3-sigma for measured mean.
4. Values are at time of slaughter.
Dresden was the source of the 131I. In the
absence of the ''background'' samples,
however, one can not be certain. If the
131j analyses in milk by the Dresden con-
tractor (see Section 7.6.3) are correct,
for example, the 131I in the thyroids may
have originated in fallout. Routine analyses
of cattle thyroids collected throughout the
United States in April, May, and June show
only a single value above the ''barely
detectable level'1, but these analyses
are ten times less sensitive than in this
study.
Analysis of cattle thyroids for
content appears to be a relatively sensitive
and convenient procedure for relating stack
releases to the amount deposited on the
ground and expected in milk. Simultaneous
measurement of thyroids obtained at a
greater distance is necessary, however, and
the cattle diet must be controlled. Radio-
nuclide analyses of the meat from beef
cattle that had been on pasture near nuclear
power stations would also be desirable.
7.8 Radionuclides in Wildlife
7..8,1 Samples and analyses. Animals in
the neighborhood of Dresden that are hunted
include squirrel, rabbit, deer, opossum,
raccoon, muskrat, beaver, weasel, skunk,
fox, duck, pheasant, quail, and crow.
Hunting for all except fox and crow is
restricted to short seasons. Rabbit, quail,
and deer (with arrow) may be hunted in the
Des Plaines Wildlife Conservation Area in
the triangle between the Des Plaines and
Kankakee Rivers, to the east of Dresden.
Hunting is forbidden in the McKinley
(Channahon) State Forest Preserve, north of
the Des Plaines River and east of Dres-
den. (I?)
To begin evaluating the radionuclide
content of wildlife in the area, 3 rabbits
and 2 deer were collected near Dresden,
and 2 deer for background values at dis-
tances of 27 and 40 km.* The rabbits were
shot in the McKinley State Forest Preserve,
at point R in Figure 7.1» The nearby deer
were obtained 7 km E and 10 km SE from
Dresden (see Figure 7.2), after they had
been struck and killed by automobiles. All
samples were wrapped in plastic bags and
preserved in dry ice until dissection,
*We thank Herman Heir, Jr., District Game Biolo-
gist, State of Illinois, and Ray Heintz, Game
Warden, Will County, for collecting the deer and
rabbit samples.
80
-------
*
e
e
¦v.
a
=3
Mcdonald heifer
o
o
m
UJ
I—
an
BACKGROUND
. & STEER,
I—
80
100
0
20
60
40
CHANNEL [20.3 keV per channel]
Figure 7,it- Gamma-ray spectra of cattle
thyroids. De tec tor: Two 10 x
10 cm Nal(Tl) in anticoinci-
dence shield. Sample: 73-g
heifer and 69-g steer thy-
roids. Count: Heifer - 600
min. on July 12. Steer - 1000
min. on Aug. 9-10.
Separate analyses were performed for
thyroids, liver plus kidney, muscle, and
bone. In addition, rabbit skins and car-
casses and deer rumen contents were ana-
lyzed. Muscle, liver plus kidney, and rumen
content were ashed at 450°C; bone was ashed
at 600°C; and thyroids were not ashed. All
samples were analyzed by gamma-ray spectrom-
etry with a 10 X 10 cm Nal(Tl) detector. Ra-
diostrontium was determined radiochemically
in bone (femurs) and rumen content,
7.8.2 Results and discussion. As shown
in Table 7.8t radionuclide concentrations
in deer rumen, muscle, and bone were too
variable for detecting any distinction
between the nearby samples (#3 and 4) and
the relative distant ones (#1 and 2). The
rumen contained 9^Sr, 95£r + 95^^^ anj
137Cs; bone contained 90Sr; and muscle
contained ^'Cs. All radionuclides are
attributable to fallout from atmospheric
nuclear weapon tests. Gamma-ray spectra of
the rumen contents showed also naturally
occurring and the progeny of 22tlRa and
232Th, and spectra of muscle also showed
40K. No radiocobalt was found in liver
plus kidney, no 89Sr (< 500 pCi/kg) in bone
and rumen, and no 131I in thyroids.
Concentrations of 137Cs in the muscle
of white-tailed deer range from 100 pCi/kg
to more than 100,000 pCi/kg,(18•19> hence
the average 137Cs content of 67 pCi/kg in
the analyzed deer is among the lowest
values. Highest concentrations are observed
in late winter at specific locations; ^18-20)
at these locations, soils of low-mineral
content may favor growth of grasses with
high fractional uptakes of minerals from
the soil, and these grasses may provide the
high-radiocesium diet for deer. The ac-
cumulation factor, pCi ^37Cs/kg muscle per
pCi 137Cs/kg rumen content, ranged from
0.4 to 2.6 in the four samples, compared to
reported values of 3.3^18^ and 0.68-*19*
The 90Sr/calc ium ratios of the deer
bones ranged from 11 to 38 pCi/g, with an
average value of 23 pCi/g. Similar values
were observed in Colorado mule deer,(21)
and higher values, at the Savannah River
plant site^9' and in Alaska caribou.(22,23)
The OR, ... the Sr/Ca ratio in bone
bone/diet
divided by that in the diet (taking the
rumen content to be the diet)—averaged
0.16 for ^Sr relative to calcium, and 0.077
for stable strontium relative to calcium^
Gamma-ray spectral analyses of the rabbit
tissues showed only in the skins and
137Cs and 40K in the carcasses, ITie concen-
tration o f ^37Cs (Table 7,9) was approxi-
mately 110 pCi/kg muscle (27 pCi/g po-
tassium ), and of 90Sr, 1,400 pCi/kg bone
(26 pCi/g calcium, if the calcium content
in bone is assumed to be the same in the
three rabbits). No radiocobalt was found
in liver plus kidney, no 89Sr in bone, and
no 13iI in thyroids. Thus, although samples
collected at a distance are necessary to
81
-------
Table 7.8
Radionuclide Concentration (pCi/kg)* and Stable Ion Concentration (g/kg)* in
Oeer Samples Collected June, 1969
Substance #1 - 27 km SE #2 - 40 km NE #3 - 10 km SE #4-7 km ESE
Rumen content
'37Cs 30 + 3+ 100 ± 8 140+9 34 ±2
K 2. 0 2. 8 4. 6 1. 02
90Sr 48 + 5 144 + 9 320 + 16 65 + 4
Sr 0.0033 0.0062 0.0073 0.001 8
Ca 0.73 1.08 1.56 0.34
95Zr + 95Nb 5 ±2 13 ±2 280 ± 20 16+2
Muscle
137Cs 49+5 69+5 61 ±6 90 ±7
K 4.03 4.13 2.77 3.76
Bone
90Sr 1 230 ± 90 2060 + 100 1600 + 70 3170 ±150
Sr 0.039 0.034 0.042 0.029
Ca ill 80 101 84
*kg wet weight.
"t± values are 2 counting error.
evaluate the background from fallout, no
radionuclides were found that would be
clearly attributable to Dresden.
Analysis of deer and rabbits is de-
sirable to evaluate their contribution to
the dietary intake of radionuclides by
humans, and may also be useful for monitor-
ing environmental vegetation. The latter
has been suggested with regard to 90gr
bones of jack rabbits at the National
Reactor Test Site, Idaho, where values of
approximately 15 pCi/'g calcium were ob-
served off-site between 1956 and 1960.(24)
Most of the retention of ^Sr in rabbit bone
was found to occur during the first year
of life. The observed ratio from diet to
bone, ORbone^diet, for strontium relative
to calcium is 0.12 in the rabbit, compared
to approximately 0.25 in man, and the
average stable strontium/calcium ratio in
Table 7.9
Radionuclide (pCi/kg)* and Stable Ion (g/kg)*
Concentrations in Tissue of Rabbits Shot on
August 21, 1968
Tissue Substance Rabbit #1 Rabbit #2 Rabbit #3
Muscle
137Cs
114 ± 12**
114+10
91 ± 10
K
4.5
3.5
3.8
Bone
90Sr
1270 + 70
1560 ± 90
1330 ± 70
Sr
0.022
0.025
0.023
Ca
54
*kg wet weight.
**± values are 2 a counting error.
82
-------
rabbit bone is 0,52 mg/g> ^5) por 13 7cS(
the rabbit body at equilibrium contains
approximately 8 times its daily intake; (26)
in man, the ratio of body burden to the
daily intake is approximately 100.
7.9 References
1. Fried, M. E. and J. M. Matuszek, ''Second
Quarterly Report—April, May, June
1968—Environs Monitoring Program for
Dresden Nuclear Power Station'', Iso-
topes, Westwood, N.J, (1968).
2. Courtney, R., Illinois Department of
Publ ic Health, personal communication
(1968).
3. Sedlet, J. and F. S. Iwami, ''Environ-
mental Radioactivity at Argonne National
Laboratory, Report for 1964* * > AEC Rept,
ANL-7401 (1965).
4. Slade, D. H., ed., ''Meteorology and
Atomic Energy 1968'', AEC Rept. TID-
24190 (July 1968).
5. Bryant, P. M. , ''Derivation of Working
Limits for Continuous Release Rates of
9"Sr and ^37qs Atmosphere in a Milk
Producing Area'', Health Phys. 12, 1394
(1966).
6. Van der Hoven, I., ''Deposition of
Particles and Gases'' in ''Meteorology
and Atomic Energy 1968'', D. H. Slade,
ed., AEC Rept. TID-24190 (1968).
7. Koranda, J. J., AEC Rept. UCRL-12478,
pp. 20 and 31a, (1965),.
8. Nay, U., ''The Adsorption of Fallout
90Sr at the Surface of Different Grass
Species'', in Radioecological Concentra-
tion Processes, B. Aberg and F. P.
Hungate, eds., (Pergamon Press, Oxford,
1967) pp. 489-491.
9. Russell, R. S., Radioactivity and Human
Diet, (Pergamon Press, Glasgow, 1966),
p. 205.
10. Garner, R. J. and R. S. Russell, "Iso-
topes of Iodine'', in Radioactivity and
Human Diet, R. S. Russell, ed, (Pergamon
Press, Glasgow, 1966) pp. 301-303.
11. Garner, R. J. and H. G. Jones, ''Fission
Products and the Dairy Cow, IV. The
Metabolism of 131I Following Simple and
Multiple Doses'', J. Agric. Sci. 55, 387
(1960).
12. Fried, R, E. and J. M. Matuszek, ''First
Quarterly Report—January, February,
March 1968—Environs Monitoring Program
for Dresden Nuclear Power Station'',
Isotopes, Westwood, N.J. (1968).
13. Porter, Charles R. , Southeastern Radio-
logical Health Laboratory, Montgomery,
Alabama, personal communication (1968).
14. Falter, K. H. and G. Murray, ''Measure-
ments of 131I in Bovine Thyroids'', Rad.
Health Data 6, 451 (1965).
15. Rust, J. H., University of Chicago,
personal communication (1969).
16. ''Iodine in Bovine Thyroid'', Radiol.
Health Data Repts. 9, 695 (1968).
17. Piazza, John, Area Game Biologist,
Illinois Department of Conservation,
personal communication (1969).
18. Jenkins, J. H. and Fendley, T. T., ''The
Extent of Contamination, Detection, and
Health Significance of High Accumulations
of Radioactivity in Southeastern Game
Populations'', presented at the 22nd
Annual Conference of the Southeastern
Association of Game and Fish Commissions,
Baltimore, Oct. 22, 1968,
19. Rabon, E. W., ''Some Seasonal and
Physiological Effects on 13^Cs and
89,90gr o^^ent Qf the White-tailed Deer,
Odocoileus virginianus'', Health Phys.
15, 37-42 (1968).
20. French, N.R., and H.D. Bissell, "Stron-
tium-90 in California Mule Deer'',
Health Phys. U, 489-494 (1968).
21. Whicker, F. W. , G. C. Farris, E. E.
Remmenga, and H. H. Dahl, ''Factors
Influencing the Accumulation of Fallout
13?Cs in Colorado Mule Deer'', Health
Phys. 11, 1407-1414 (1965).
22. Watson, D. G., W. C, Hanson, and J. J.
Davis, ''Strontium-90 in Plants and
Animals of Arctic Alaska, 1959-61''i
Science 444, 1005-1009 (May 22, 1964).
23. Schulert, A, R., ''Strontium-90 in
Alaska1', Science 136, 146-148 (Apr. 13,
1962).
83
-------
24. Fineman, Z, M. , R. McBride, and J.
Detmer, ''Use of the Jack Rabbit as
Bioindicator of Environmental ^°Sr
Contamination'', in Radioecology, V.
Schultz and A. W. Klement, Jr., eds.
(Reinhold, New York, 1963) p. 455.
25. Lloyd, E., t4A Comparison of the Metab-
olism of Calcium and Strontium in Rabbit
and Man'', in Strontium Metabolism, J.
Lenihan, L. Loutit, and J, Martin, eds.
(Academic Press, New York, 1967) p. 167.
26. Fugita, M., J. Iwamoto, and M. Kondo,
''Comparative Metabolism of Cesium and
Potassium in Mammals — Interspecies
Correlation between Body Weight and
Equilibrium Level''. Health Phys. 12,
1237 (1966).
84
-------
8. SUMMARY AND CONCLUSIONS
8.1 Radionuclides in Dresden
Effluents
One of the purposes of this study was
the identification and quantification of
individual radionuclides in Dresden ef-
fluents. Radionuclides in liquids on site
and in gaseous, airborne particulate, and
liquid wastes were therefore measured during
all five trips in the 9-month period of
study; the results are presented in Sections
2, 3, and 4, and are summarized below. It
should be noted, however, that only con-
tinuous measurements over extended periods
can yield definitive values.
1. Average release rates of the measured
noble gas fission products were:
2, Average release rates of the other
measured radionuclides were:
4,4-hr 85mKr
10.7-yr 85Kr
76 -min 87l(r
2.8-hr 88Kr
2.3-d 133mXe
5.3-d 133Xe
9.1-hr 135Xe
17 -min ^8\e
3 X 102 yuCi/sec
1 X 10
- 1
7 x 102
5 x 102
1 x 101
3 X 102
8 x io2
2 x 103
The release rates were measured in the de-
lay line for off-gas from the condenser air
ejectors. The average values were computed
for the 1968 average fission-product noble
gas release rate of 12,500 /iHi/sec during
64 percent of the year. These values are
generally in accord with measurements per-
formed earlier by General Electric Co. staff.
Radio-
nuc1 ides
in stack
e ffluent,
in 1i qu i d
effluent,
jiC i / sec
3h
6
X
10"3
5
X
10"2
*8Co
2
x
10"5
2
X
10"2
60Co
2
X
10"5
3
X
10"2
8?Sr
7
X
10*4
8
X
10'3
9 0Sr
3
X
10"6
9
X
10"4
1 3 1 j
6
X
IO*4
1
X
10"3
134Cs
< 1
X
10" 5
2
X
10'3
137Ca
2
X
10"5
6
X
10"3
i^OBa
3
X
10"4
5
X
10"3
l44Ce
< 3
X
10"5
2
X
10'4
The following should be noted concerning
these values: (a) stack effluent values take
into account operation during only 64 per-
cent of the time in 1968; the liquid wastes
that contained most of the radionuclides
were released during.less than one-half of
the year; (b) for stack effluent, radio-
active particles were measured on filters
in the stack, I31j was measured on charcoal
cartridges in the stack, and 3H was measured
in the delay line for off-gas from the con-
denser air ejectors; (c) release rates in
liquid effluent were computed from radio-
nuclide concentrations measured in waste
tanks before discharge; they can be con-
verted to concentrations in water at the
point of release by dividing by the flow
rate in the coolant-water canal of 1 X 10^
ml/sec; (d) the 13*I release rate in the
stack has been compensated for an 88-per-
cent collection efficiency (see Section
4.3.3); (e) effective release rates of
85
-------
8®Sr and ^'Cs are higher than measured
because of formation by decay of 8^Kr-
89Rb and ^3'Xe, respectively, in the en-
vironment (see Section 7,2.2); (f) concen-
trations of radiocobalt and radiocesium 111
water at the point of discharge from Dresden
were considerably lower than indicated by
the above release rates; it is probable
that radiocobalt was mostly insoluble and
that radiocesium was mostly retained on
silt; (g) the measurements show considerable
variations in concentrations and release
rates.
3. The measured release rates are con-
sistent with the average annual releases
reported by Dresden Nuclear Power Station
for the year 1968 of 0. 189 X 10~7 /Xi/ml
of water and 12,500 X 0.64 = 8,000 /iCi/sec
in air. The sum of measured radionuclides
in liquid effluent (see above) of 12 X
10*" fjCi/sec, divided by the flow rate of
1 X ]07 ml/sec, is 0.12 X 10"' /iCi/ml. The
sum of measured noble gas fission products
(see above) is 4, 600 /-iCi/sec; the gases
83mKr, 89Rr, 135mXe, 137Xe, and 13N would
be expected to contribute additional activ-
ity amounting to several thousand /iCi/sec.
4. The influence of plant operation on
radionuclide release rates in effluent is
indicated by comparing these release rates
to fission production rates in the reactor
core. The ratios of the fission product re-
lease rates shown above to estimated produc-
tion rates (see Appendix B.1, adjusted for
64 percent operation 1968) are:
noble gas other
f issi on
p ro due t s
fission
P
re
iducts
85"kr
1
X
10 "6
3H
1
X
10*3
85Kr
5
X
10-5
89Sr
4
X
10-9
87Kr
6
X
10"7
9°Sr
6
X
10 "8
U
CO
CO
7
X
10"7
1 31 j
2
X
10"10
133mXe
6
X
10"5
137Cs
4
X
10 _7
133Xe
1
X
10"5
U0Ba
4
X
10-10
135Xe
2
X
10"6
144Ce
4
X
10-iO
138Xe
2
X
10-7
Thus, only small fractions of these fission
products are released. The ratio for
fission-produced tritium is actually lower
than shown because most of the discharged
tritium is probably produced by neutron
activation of deuterium in reactor cooling
water.
8.2 Radionuclides and Radiation from
Dresden in the Environment
The main effort in the environmental
aspect of this study was devoted to measur-
ing radionuclides in the plume from the
Dresden stack and the exLernal radiation
exposure from these radionuclides. The plume
was detected as much as 18 km distant from
the stack with large Nal(Tl) survey in-
struments. Within 1 to 2 km from the stack,
radiation exposure rates were measured at
the centerline of the plume under stable
and neutral conditions with a tissue-
equivalent ionization chamber and sensitive
electrometer. Average exposure rates
measured during three tests 1'or 1/2- to
1-hour periods were 13, 24, and 40 /iR/hr,
Concentrations of ^33Xe, ^3jXe, and ^3®Cs
in ground-level air were measured at the
same time as the radiation exposure rates
(see Section 5.2.5). Estimated concentra-
tions and exposure rates, based on measured
release rates at the stack and diffusion
calculations, were within a factor of two
or better of the measured values.
Thermoluminescent dosimeters exposed
during two 2-week periods at ten stations
located between 1 and 4 km from Dresden
showed an average background radiation
exposure rate of 9 ftR/hr. During reactor
operation, TLD's at three locations in-
dicated radiation exposure from the plume at
average rates for a 2-week period of 2 to
3 /jR/hr above the natural radiation back-
ground. The TLD values are uncertain, how-
ever, because their standard deviation is
± 1 yuR/hr, and variation in the background
could have introduced significant error.
Samples collected in the Dresden en-
vironment for analysis of individual radio-
nuclides usually contained radionuclides
such as 90Sr and 137Cs from fallout associ-
ated with atmospheric testing of nuclear
devices, and naturally occurring radio-
nuclides such as 40R, ^3^Th plus progeny,
and 226Ra plus progeny. To search for radio-
nuclides attributable to Dresden, nearby
samples were compared with more distant
86
-------
samples, and downstream or downwind samples
with those collected upstream or upwind.
In addition, measurement of ^Co, ^°Co,
S^Sr, 131I, and was emphasized, be-
cause these were discharged at Dresden
while their concentrations in fallout were
low or undetectable.
No radioactivity attributable to Dresden
was found in the following samples:
rainwater (Section 7.3.2)
soil (Section 7.4.2)
cabbage (Section 7.5.2)
grass (Section 7.5.2)
corn husks (Section 7.5.2)
milk (Section 7.6.3)
deer (Section 7.8.2)
rabbit (Section 7.8.2)
surface water (Sections 6.2.2 and 3.3.7)
drinking water (Section 6.6.2)
fish (Section 6.3,2)
Estimated concentrations and measured less-
than values suggest that a sensitivity of
approximately 0.05 pCi/liter appears neces-
sary to measure 131f from Dresden in milk,
and 0.001 pCi/liter to measure 8^Sr from
Dresden in rainwater, for example.
Indications of radioactivity from
Dresden were found in the following samples:
1. The average 13 1j content of three
thyroids of heifers was 31 pCi (0.45
pCi/g). These heifers had been placed on
pasture 2.3 km east of Dresden for sever-
al weeks before slaughter specifically
for testing cattle thyroid as a sensitive
indicator of deposition on pasture
grass.
2. Snow collected 0.9 km south of Dresden
contained 8^Sr at a concentration of 10
pCi/liter, while snow collected 10 km
NNE of- Dresden contained no 89Sr (< 1
pCi/liter). The area to the south of
Dresden was downwind during the snowfall.
3. Kernels of field corn grown at the same
location south of Dresden contained
at a concentration of 4 pCi/g ash (at
0.8 percent ash weight), compared to
0.2 to 0.8 pCi/g ash in corn kernels
from other locations.
On the basis of these measurements,
exposure to the surrounding population
through consumption of food and water from
radionuclides released at Dresden was not
measurable. External exposure from radio-
active gases discharged from the Dresden
stack was detectable, but it was only a
small fraction of the natural radiation
background over an extended period of time,
and well within Federal Radiation Council
guidance.
8.3 Monitoring Procedures
The following techniques were demon-
strated in this study for monitoring radio-
nuclide release and environmental transport:
1. analysis by gamma-ray spectrometer with
Ge(Li) detectors of multiple radio-
nuclides in samples of water from the
station and in effluent before dilution;
2. radiochemical analysis of 35 radio-
nuclides in the primary coolant;
3. collection of radioxenon from environ-
mental air on charcoal for analysis by
gamma-ray spectrometry;
4. co 11 ection of 138Cs in environmental air
on filters with high-volume samplers, and
analysis by gamma-ray spectrometry;
5. use of portable Nal(Tl) survey meters as
sensitive detectors of the plume from
the Dr esden stack;
6. use of muscle-equivalent ionization
chamber and Shonka electrometer for
quantifying the radiation exposure rate
during brief periods within or beneath
the plume;
7. use of TLD's for a 2-week period to
quantify the average long-term radiation
exposure rate from the plume;
8. collection of ionic radionuclides in
water from 100-liter volumes ^n ion-
exchange resins, and analysis by gamma-
ray spectrometry and radiochemical
s epa rat i on;
9. collection of radioiodine from 22.5-
liter volumes of milk on anion-exchange
resin, and analysis by gamma-ray spec-
trometry;
10. measurement of 1311 in thyroids of
cattle that had grazed under defined
conditions near station;
87
-------
11. collection and analysis of food samples,
including vegetables, milk, fish, rabbit,
and deer; and of drinking water;
12. use of measured release rates at the
station, meteorological data, and trans-
fer coefficients lo estimate radionuclide
concentrations in samples for comparison
with measured or minimum detectable
v al ues.
Additional tests are required for several
of the techniques; for example, no 131j was
detected in milk, and detection of external
radiation with the TLD's was marginal.
8.4 Considerations in Developing
Recommendations for
Environmental Surveillance
The available guidance for radiological
surveillance at nuclear power stations re-
ferred to in Section 1.1 and the experience
from this study suggest a change from past
emphasis at stations in the U.S. on monitor-
ing gross radioactivity in effluent and
extensively sampling the environment. The
following approach is presented for con-
sideration:
1. thorough monitoring of significant
individual radionuclides in effluents;
2. specific studies of predicted critical
nuclides, pathways, and populations by
measuring transfer coefficients from
plant to man in the environment;
3. direct measurement of radiation and
radionuclides at the point of population
exposure; and
4. periodic checking of potential concen-
tration media for radionuclides in path-
ways from plant to man.
Many of the techniques for measuring
individual radionuclides in effluents are
available, some were demonstrated in this
study (see Section 8.3), and others remain
to be developed. Significant nuclides that
should be measured include the critical
radionuclides, the major radioactive con-
stituents, and radionuclides that serve as
indicators for more hazardous ones because
they are easily measured. The list of radio-
nuclides to be measured should be changed
as it becomes possible to predict release
rates for previously measured radionuclides
and as interest becomes focussed on others,
A wel1-designed program should make it
possible to obtain more useful dosimetric
information by monitoring individual radio-
nuclides in effluents and computing the
potential radiation exposure to man, than
by the usual determination of ''less-than'•
values in environmental samples.
If effluent monitoring is to be a major
component of radiological surveillance, then
accurate transfer coe fficients from the
point of release through the station en-
vironment to the population at risk must
be developed. These can be obtained during
the early years of station operation by
undertaking specific studies, as demon-
strated at Dresden in comparing the release
rate of gaseous fission products at the
stack with the radiation exposure rate
beneath the plume in the environment, The
studies can usually be performed within a
few years of startup with radionuclides in
effluents; alternatively, radioactive or
stable tracers may be used before or soon
after initial operation. As more nuclear
stations begin operation and undertake these
studies, the accumulation of information on
the ecological cycling of radionuclides will
decrease the need for further research,
until only unusual waste management prac-
tices or environmental conditions will re-
quire such research.
Since control of exposure to man is of
primary importance, it is necessary to
monitor exposure directly. For these
measurements, ''less-than'' values of ex-
ternal radiation exposure, radionuclide
intake, or radionuclide body burden at-
tributable to station operation are ac-
ceptable if the values are sufficiently
below limits. After effluent monitoring and
measurements of environmental transfer
coefficients have provided quantitative
data for predicting radiation exposure to
the population, the frequency and intensity
of monitoring radiation exposure should be
adjusted to respond to the level of radio-
nuclide releases.
Finally, some environmental measurements
are desirable to maintain surveillance of
potential concentrating media for radio-
nuclides. The program of these measurements
88
-------
should be flexible in responding to changes
in station operation, the environment and
the population, to new information on uptake
and transfer of radionuclides, and to un-
usual analytical results. As the knowledge
of the environment increases, fewer measure-
ments will be needed.
A more source-oriented program than is
now customary is recommended because large
nuclear power stations will be numerous,
relatively close to population centers, and
with little operating experience (except
at considerably lower power levels) during
the next few years. Over the long term, the
program should provide more information at
lower cost than many current environmental
surveillance programs which appear to be
exercises in measuring fallout radioactivity
and the natural radiation background.
6. Perform similar but less extensive
studies at other nuclear power stations
to evaluate the behavior of radioactive
effluents under different operating con-
ditions and in different environments.
8.5 Suggested Future Studies
The following studies at nuclear power
stations are suggested on the basis of the
field trips to Dresden:
1. Incorporate and test the suggestions in
Section 8.4 for a radiological surveil-
lance program;
2. Test for extended periods several of the
techniques that were demonstrated in this
study, such as long-term measurements of
external radiation exposure with dosim-
eters, calculation of long-term radiation
exposure by short-term measurements, and
use of concentration devices in analyzing
radionuclides in water, milk, and air;
3. Relate radionuclide release rates to
operating and waste-handling procedures
to permit accurate estimation of release
rates in future operations and for new
stations;
4. Examine the effect of radioactive waste
treatment on discharge practices in order
to evaluate the cost of reducing the
radionuclide content of effluents;
5. Demonstrate efficient techniques for
monitoring individual radionuclides in
gaseous, airborne particulate, and liquid
effluent; develop new techniques, if
necessary; and
89
-------
APPENDIX A
Acknowledgments
This report presents the work of the staff of the Radiological Engineering
Laboratory, consisting of the following:
Participants from other agencies are listed below, and their help is grate-
fully acknowledged:
R. W, Courtney, Illinois Department of Public Health
L. Schnltz, Illinois Department of Public Health
C. D. Hampelmann, Division of Compliance, AEC
H. D, Thornburg, Division of Compliance, AEC
A. P, Kenneke, Division of Radiation Protection Standards, AEC
D. T. Oakley, NFB, DER, BFH, EHS
J. M. Snith, NFB, MR, BRH, EHS
W. Kiedaisch, Dresden Nuclear Power Station
R. A. Pavlick, Dresden Nuclear Power Station
M. Watson, Dresden Nuclear Power Station
J. Marshall, Dresden Nuclear Power Station
Assistance by C. L, Weaver, E. D. Harward, and J, E. Martin, DER, BRH,
EHS, in planning the study is gratefully acknowledged. We wish to thank the
above for reviewing the manuscript, and also G. A, Pliner and J, Russell,
NFB, DER, BRH, EHS; R. S. Gilbert, J. M. Snith and T. Slozek, General Electric
Company; Dr. I. Van der Hoven, Air Resources Laboratory, ESSA; Prof, J,
Leonard, U, of Cincinnati; Prof, G, Hoyt Whipple, U, of Michigan; and Prof.
C, P. Straub, U. of Minnesota.
Bernd Kahn
Richard L. Blanchard
William L. Brinck
Harry E, Kolde
Herman L. Krieger
Seymour Gold
Alex Martin
Jasper W. Kearney
Glen R. Mills*
David B. Smith*
Betty J. Jacobs
Eleanor R. Martin
George W. Frishkorn
Elbert E. Matthews
Gerald J. Karches*
William M. Cox*
William Averett
James B. Moore
B. Helen Logan
Teresa B. Firestone
•Formerly with REL.
91
-------
APPENDIX B.l
Estimated Generation Rate of Fission Products in Fuel
Fission Fission Yield Decay Constant Generation Rate
Product
Y*
sec-1
A, /xCi /sec
3H
9.5 x 10"st
1.78 x io"9
8.5 x
01
89Sr
4.5 x 10'2
1.57 x io-7
3.6 x
06
90Sr
5.9 x 10"2
7.82 x IO"10
2.3 x
O4
9,Sr
5.8 x NT*
1.98 x 10"5
5.8 x
08
9 3y
6.4 x 10*2
1.86 x IO'5
6.0 x
08
95Zr
6.3 x io-2
1.23 x io-7
3.9 x
0®
97Zr
6.1 x io-2
1.13 x io"5
3.5 x
08
95Nb
6.3 x io-2
2.29 x io-7
8.5 x
O6"
99Mo
6.1 x io*2
2.90 x io"6
8.9 x
o7
99mIc
6.1 x io-2
3.21 x io"5
9.6 x
o7**
103Ru
3.0 x io'2
2.02 x io-7
3.1 x
oe
,06Ru
0.4 x io-2
2.19 x io*8
4.4 x
o4
,05Rh
0.8 x io*2
5.33 x io'6
2.1 x
o7
132Te
4.3 x IO"2
2.46 x 10-6
5.3 x
o7
13 11
2.9 x 10"2
0.96 x io"7
1.5 x
o7
13 31
6.5 x IO"2
9.21 x io"6
3.0 x
o8
13 51
6.0 x 1O"2
2.87 x io*5
8.6 x
0B
'37CS
5.9 x io-2
7.30 x 10"'°
2.2 x
o4
'4003
6.6 x io*2
6.26 x io*7
2.1 x
o7
141Ce
6.0 x 10"2
2.47 x io*7
7.4 x
oe
M3Ce
6.2 x io-2
5.82 x 10"8
1.8 x
o8
'^Ce
6.2 x io-2
2.83 x 10"8
8.8 x
o5
,47Nd
2.6 x 10"2
7.30 x 10"7
9.6 x
0B
*Harley, N., I. Fissnne, L. D. Y. Ong, and J. Harley, "Fission Yield and Fission
Product Decay" in AEC Rept. HASL 164 (1965) p. 251; Russell, I. J. and Griffith,
R. V., "The Production of ,09Cd and 1l3mCd in a Space Nuclear Explosion" in AEC
Rept. HASL 142 (1964) p. 306.
tAlbenesius, E. L. and R. S. Ondrejcin, "Nuclear Fission Produces Tritium", Nu-
cleonics 18 (9), 100 (1960).
**EquiIibrium with longer-lived parent is assumed.
-------
Estimated Generation Rate of Fission Products in Fuel (Cont.)
Fission Product
Generation Rate A, /^Ci/sec
85Kr
3.0 x 103
B5mKr
2.9 x 108
8?Kr
1.9 x io9
88Kr
1.2 x io9
133Xe
5.0 x i07
133mXe
2.8 x io5
135Xe
6.7 x 10s
138Xe
1.9 x 1010
Note: See Appendix B.3 for fission yields and decay constants.
-------
APPENDIX B.2
Estimated Turnover Rate of Ionic Fission Products in
Primary Coolant Water Based on Concentration Measurements,
and Ratio of Turnover Rate to Generation Rate
Fi ssi on
Product
r M13'
~mT"
^decay + ^turnover'
sec-1
R,
//C i
sec
R/A*
3H
1.3
X
0"3
CD
CO
CO
4.4
X
0~5
2.0
X
10*5
1.7
X
10"'
4.7
X
Q"8
90Sr
1.3
X
o"6
2.0
X
1 o*5
4.9
X
10"3
2.1
X
0"7
9'Sr
1.2
X
0-2
4.0
X
10"5
9.1
X
10'
1.6
X
0"7
9 3y
-2.0
X
0"3
3.9
X
10"5
1.5
X
101
2.5
X
0"8
95Zr
2.4
X
0"5
2.0
X
10~5
9.1
X
10"2
2.3
X
0"8
97 Zr
1.3
X
o"4
3.1
X
10"5
7.6
X
10"'
2.2
X
IT9
95Nb
1.8
X
O*5
2.0
X
10"5
6.8
X
10"2
8.0
X
0"9
"Mo
1.4
X
0"3
2.3
X
10"5
6.1
6.9
X
0"8
9 9m Jq
4.4
X
0"2
5.2
X
10"5
4.3
X
102
4.5
X
0"6
103ru
5.6
X
0"5
2.0
X
10"5
2.1
X
10"'
6.S
X
Q"fl
10BRu
1.3
X
0"6
2.0
X
10"5
4.9
X
10"3
1.1
X
0"7
105Rh
-4.0
X
0"4
2.5
X
10"5
-1.9
-3.0
X
0"8
,32Te
1.9
X
0"5
2.3
X
1Q"5
8.2
X
10"2
1.5
X
0"9
1 311
2.2
X
0"3
2.1
X
10"5
8.7
5.8
X
0"7
1 331
2.3
X
o"2
2.9
X
10"5
1.3
X
102
4.3
X
0"7
1 351
3.6
X
0"2
4.9
X
10*5
3.3
X
102
3.8
X
0"7
1 37CS
4.4
X
0'5
2.0
X
10"5
1.7
X
10"1
7.7
X
0"B
u0Ba
1.0
X
0"3
2.1
X
10"5
4.0
1.9
X
O"7
<41Ce
4.4
X
0"5
2.0
X
10"5
1.7
X
10"1
2.3
X
0"8
,43Ce
1.0
X
0"4
2.6
X
10"5
4.9
X
10"'
2.7
X
0'9
144Ce
6.0
X
Q'6
2.0
X
10"5
3.0
X
10"2
3.4
X
0"8
147Nd
-3.0
X
0"5
2.1
X
10"5
-1.2
X
10"'
1.3
X
0"8
~For value of A, see Appendix B. 1; R = turnover rate, A = generation rate.
Motes: f. C is concentration in primary coolant on August 22, 1968.
2. Turnover rate was computed on basis of radioactive decay and removal of
radionuclides with 14-hour mean time on reactor coolant cleanup deminer-
al i zer.
-------
APPENDIX B.3
Estimated Release Rates of Fission-produced Noble Gases
Release rate
Release rate
f **
1 »
Fission
from fuel,+
after 21 min.,
10-sec
Radioactive
Fission
product
yield*
K
sec*1
/j. Ci/sec
/j£ i /sec
period
Progeny
1.9-hr
83mKr
5.4 x 10"3
1.0
X
10"4
( 22)
19
—
—
10.7-yr
85Kr
2.9 x 10*3
2.05
X
10*9
( 0.052)
0.052
—
—
4.4-hr
85niKr
1.3 * 10"2
4.37
X
10"5
34
32
—
—
76 -min
B7Kr
2.5 x 1 0*2
1.52
X
10"4
123
102
—
—
2.0-hr
0BKr
3.6 x 10"2
6.87
X
10"5
119
109
—
8BRb
3.2-min
B9ftr
4.6 x I0~2
3.6
X
10"3
(1,100)
12
0.05
89Rb, B9Sr
33 -sec
90Kr
5.0 x 10"2
2.2
X
10"2
(3,000)
—
0.20
90R5f 90Sr? 90y
10 ~s®c
a,Rf
3.4 x 10-2
6.9
X
io-z
(3,600)
—
0.50
91Rb, 9,Sr, 9,f
12 -d
131mXe
2 x io"4
6.7
X
10"7
( 0.07)
—
—
—
5.3-d
,33Xe
6.6 x 10"2
1.52
X
10'6
33
33
---
...
2.3-d
133mXe
1.6 x 10-3
3.5
X
10"6
( 1.2)
1.2
—
...
9.1 -hr
,35Xe
6.3 x 10-2
2.11
X
10"5
117
114
—
' 3®Cs
15.6-min
,35mXe
1.9 x 10"2
7.39
X
10"4
( 210)
84
---
...
3.8-min
,37Xe
6.0 x 10*2
3.0
X
10"3
(1,300)
28
0.05
'37Cs, ,37mBa
17 -Din
,38Xe
5.5 x 10"2
6.8
X
10"4
574
243
---
,38Cs
43 -sec
,39Xe
5.4 x 10'2
1.6
X
10"2
(2,700)
—
—
139Cs, 139Ba
16 -sec
U0Xe
3.8 x 10*2
4.3
X
10"2
(3,200)
1,000+
• ••
0.30
140Cs, 140Ba, 140L
*Katcoff, S., Nucleonics 18, #11, 201 (Nov. 1960).
+per 1000 ^i/sec of radionuclides not in parentheses. Calculated for "diffusion mixture" by
equation 2.3 of Section 2.3.4.
**fraction of decay in reactor vessel.
95
-------
APPENDIX B.4
Estimated Turnover Rate of Ionic Activation Products in
Primary Coolant Water Based on Concentration Measurements
Radionuclide
C,
/xCi
"mT
^decay + ^"turnover '
sec'1
R,
/j£ i
- sec
5'Cr
~5
X
10"4
2.0 X 10"5
y2.
54Mn
1.6
X
10"6
2.0 x 10"5
6.1
x 10*3
55Fe
4.0
X
10"5
2.0 x 10"5
1.5
x 1 0"'
57Co
1.6
X
10"6
2.0 x io"5
6.1
x 10'3
58Co
1.7
X
10'3
2.0 x i(T5
6.5
O
CJ
o
CD
2.6
X
10"4
2.0 x i(T5
1.0
65Zn
4.0
X
10"6
2.0 x 10*5
6.1
x 10"2
110iling
1.9
X
10"6
2.0 x io-5
7.2
x 10"3
134Cs
2.3
X
10"5
2.0 x io*5
8.7
x 10"2
«36Cs
2.4
X
10"5
2.1 x io"5
9.6
x 10*2
182Ta
-7
X
10"7
2.0 x 10"5
~3.
x io*3
242Cm
1.2
X
10"7
2.0 x 10"5
4.6
x 10'4
Notes: 1. C is concentration in primary coolant on August 22, 1968; R is turnover rate.
2. Turnover rate was computed on basis of radioactive decay and removal of
radionuclides with 14-hour mean time on reactor coolant cleanup deminer-
alizer.
3. Only radionuclides with t^ > 7 days are listed.
96
-------
APPENDIX C.l
Estimation of Radionuclide Concentrations in the Environment
Standard diffusion equation and Brookhaven dispersion coefficients:*
X ~ (Q/7t o-y(Jz U) exp (-h2/2crz2)
where
X = ground-level centerline concentration, Ci/ni3
Q = release rate, Ci/sec
cry, az ~ lateral and vertical dispersion coefficients, m
(J = mean wind speed at height of release, m/sec
h - effective release height, m
Test 1
Test 2
Test 3
Q, ,33Xe, /JJi/sec:
400
1,660
115
75
730
1,420
65
21
730
1,420
115
,35Xe, /xCi/sec:
cry, m:
o-z, m:
u, m/sec:
h, m:
Xu/Q, m'2
X, 133Xe, pCi /tn3:
2.1 x 10'5
990
8.5
60
2.4 x 10-8
2.6
6.7
90
1.9 x 10"5
2,200
75
6.2
90
135Xe, pCi/to3:
4,100
5.0
4,300
~except ctz for test 2.
97
-------
APPENDIX C.2
Estimation of Radiation Exposure in the Environment
D' = 10(Q;/U) [0.66 D'(0. 4) + 0.34 0 '(2.0)J
where
D' = exposure rate, /zR/hr
QJ - effective release rate at point of measurement, mCi/sec
u = mean wind speed at height of release, m/sec
D'(0.4), D'(2.0) = exposure rate calculated at photon energies of
0.4 and 2.0 MeV, /xfi hr-'/mCi m'1
The exposure rates, D', were calculated by computer on the basis of a release rate of
1 mCi/sec, a photon abundance (gamma rays per disintegration) of 1.0, and a wind speed
of 10 m/sec. Independent variables in the calculations are stability, effective re-
lease height, downwind distance and off-centerIine angle. Calculation of the multiplj-
cation factors for exposure rates D'(0.4) and D'(2.0) is shown in Appendices C.3 and
C.4.
Test 2
Averaging interval
Test 1
1
2
3
4
5
Test 3
u, m/sec
8.5
6.7
6.2
6.5
6.8
7.1
6.2
6, degrees
3
7
0
2
4
7
1
0'(0.4), ^R/hr
1.4
< 0.1
0.5
0.4
0.25
< 0.1
0.56
D'(2.0), /ifi/hr
2.2
0.5
1.9
1.7
0.9
0.5
1.90
QJ, mCi/sec
15
11.6
11.6
D', ^R/hr
20
9
19
-------
APPENDIX C.3
Calculation of Fraction of Gamma Rays Between 0 and 1 MeV, for
0.4 MeV Exposure Rate, D'(0.4) Multiplication Factor
Photon
Photon
Nucl ide fraction
Energy
Abundance
of total activity,
Product
Nucli de
(E), MeV
(A)
(F)
E.A.F
,33Xe
0.081
0.37
0.04
1 x 10"3
85mKr
0.150
0.74
0.04
4
138Xe
0.160
0.16
0.27
7
08Kr
0.166
0.07
0.14
1
88Kr
0.196
0.35
0.14
10
,35Xe
0.250
0.91
0.15
34
138Xe
0.260
0.49
0.27
34
85mKr
0.305
0.13
0.04
2
88Kr
0.360
0.05
0.14
3
87Kr
0.403
0.84
0.13
44
'3SCS
0.411
0.03
0.02
0
138Xe
0.420
0.19
0.27
21
,37Xe
0.455
0.33
0.02
3
138Cs
0.463
0.23
0.02
2
138Xe
0.510
0.04
0.27
6
135mXe
0.527
0.80
0.09
38
138CS
0.550
0.08
0.02
1
135Xe
0.610
0.03
0.15
3
88Kr
0.850
0.23
0.14
27
8?Kr
0.850
0.16
0.13
18
138CS
0.870
0.04
0.02
1
88Rb
0.898
0.13
0.02
2
262 x 10"3
EAF
0.262
nx = °-66
.0)
^(0.4)
(0.4X1 .0)(1
-------
APPENDIX C.4
Calculation of Fraction of Gamma Rays Above 1 MeV, for
2.0 MeV Exposure Rate, D'(2.0) Multiplication Factor
Photon
Photon
Nuclide fraction
Energy
Abundance
of total activity,
Product
Nuclide
(E), MeV
(A)
(F)
E.A.F
'38CS
1.010
0.25
0.02
1 x 10-3
oscs
1.430
0.73
0.02
21
88Kr
1.550
0.14
0.14
30
,38Xe
1.780
0.32
0.27
154
88Rb
1.863
0.21
0.02
8
i38Xe
2.010
0.28
0.27
152
87Kr
2.050
0.05
0.13
13
88Rb
2.110
0.01
0.02
0
88Kr
2.190
0.18
0.14
55
1 38Cs
2.210
0.18
0.02
8
8BKr
2,400
0.35
0.14
118
87Kr
2.570
0.35
0.13
117
»38CS
2.630
0.09
0.02
5
88Rb
2.650
0.02
0.02
1
Others
3.0
0.01
0.02
1
684 x 10-3
EAF
0.684
EAF(2.
0) (2.0X1
.0)(1.0)
-------
APPENDIX C.5
Holland Prediction Technique for Environmental Radiation Exposure
D' = (D/Q) Q'E/0.7 u, where
D' = exposure rate, /Jt/hr
Q' = release rate, mCi/hr
E = mean energy weighted for photon abundance and release rate, MeV
u = mean wind speed at height of release, m/sec
D/Q is from Holland nomograph with parameters:
n - stabiIity parameter
c
= diffusion coefficient, (meters)n/2
h
= effective release height,
m
h'
= equivalent point source height, m
Test 1
Test 2
Test 3
n
0.3
0.5
0.25
C, (meters)n/2
0.20
0.05
0.10
h, m
80
go
90
h\ m
B0
90 to 235
90
D/Q, R/kW-sec
3.5 x 10*3
1.15 x 10"3
3.5 x 10*
(average)
Q', mCi/hr
54 x io3
42 x io3
42 x |03
E, Me V
0.88
0.8B
0.88
u, m/sec
8.5
6.7
CN
•
CO
0', /xR/hr
28
9
29
-------
APPENDIX C.6
TLD Radiation Exposure Estimations
Exposure rate estimations for TLD stations were made with the computer
model by the equation:
10 Q; t;
D' - ——I— [0.66 D'(0.4) + 0.34 D'(2.0)]it
T i u
i
whe
re
D' r mean exposure rate over period, /^R/hr
Q'x = mean release rate over period, mCi/sec
T = length of period, hr
= mean release-height wind speed, m/sec
t^ - length of period of meteorological condition, i, described by
stability type, mean wind speed, effective stack height' and mean
wind direction azimuth sufficiently close to the station to produce
a significant exposure, hr
[D'(0.4), D'(2.0)]i = calculated exposure rates, as described in Ap-
pendix C.2 for meteorological condition, i, /jR/hr
A sample set of calculations is shown in Appendix C, 7. The exposure rates
from the FSAR (Section 5.5, Ref. 10) and our model are not directly com-
parable. To permit a comparison, the latter was computed for angles from 0 to
11 degrees off-centerline and integrated to give a 22-degree-wide sector
mean. The FSAR exposure rates are for a noble gas diffusion mix after 30
minutes; these calculated values are for a mix with only a 21-minute decay.
Hence, the FSAR values are lower. For the following conditions, the values
are:
downwind distance, 1500 m
effective release height, 125 m
release rate, 1 mCi/sec
wind speed, 10 m/sec
receptor, ground-level and on sector centerline
Stability FSAR This report
Neutral 0.35 0,43 //R/hr
Stable 0.29 0.32 HR/hr
102
-------
TLD Radiation Exposure Estimations (Cont.)
Station 110, Sample Calculation
As an example, the TLD exposure rate is estimated at a wind azimuth of
204° and at a distance of 1200 m in Appendix C.7. The following symbols are
used:
6 ~ mean wind azimuth
££) - mean off-centerline angle
h r effective stack height, m
D! = [0.66 D'(0.4) + 0.34 D'(2.0)] i
Other symbols are defined above.
APPENDIX C.7
Sample Calculation for Radiation Exposure at Station 110
li-
0,
A9,
h,
Of.
Mf/Ui.
Condi tion
hr
degree
m/sec
degree
m
/ifl/hr
/jR-sec/m
Unstable
1
201
6.5
3
105
0.44
0.068
1
198
7.8
6
100
0.39
0.050
1
187
3.8
17
115
0.16
0.042
5
215
5.9
11
105
0.28
0.238
4
226
4.9
22
110
0.08
0.065
Neutral
2
205
5.3
1
95
1.09
0.412
9
203
9.8
1
85
1.22
1.122
4
198
8.3
6
85
0.63
0.304
2
185
4.2
19
100
0.07
0.033
1
185
8.8
19
85
0.07
0.008
6
215
6.3
11
90
0.27
0.257
13
225
6.5
21
90
0.04
0.080
Stabl e
11
205
7.2
1
90
0.99
1.512
2
196
8.0
8
85
0.35
0.088
2
188
7.4
16
90
0.09
0.024
6
212
7.5
8
90
0.34
0.272
11
217
7.5
13
90
0.13
0.191
1
228
1.9
24
130
0.03
0.016
20
224
6.4
20
90
0.04
0.125
2 ip [0.66 D'(Q.4) + 0.34 0'(2.0)]j = 4.900
i
_ 100!
D' =^JL (4.90)
= 10 x 11.6 x 4.9/295
D' = 1.8/xH/hr
-------
APPENDIX D.l
Estimated 89Sr Concentrations in Precipitation Samples
Location
Date,
1968
T, sec
Q0 , pCi /sec
u, m/sec
x, m
W, pCi/m2
89Sr Cone.,b pCi /I
Rain
1
June 25
3,600
2,300
7.5
3,200
0.020
2.0 x io"4
4
June 27
3,600
1,300
6.5
800
0.052
5.2 x io*4
5
June 26
7,200
1,700
6.5
1,500
0.072
7.2 x io*4
Snow
Met Tower
Jan. 18
21,600
1,400
6.5
900
0.13
2.3 x io*2
"Based on average 89Sr release at stack of 1000 pCi/sec, plus ingrowth by decay of 89Kr
constituting at top of stack 1.2% of nominal gaseous fission product mixture released at
rate of 12,500 i/sec; ingrowth time = x/u.
bConc. = W x 0.01 for rain
Cone. = W x 0.17 for snow
Hote: 8 = 0.174 radian for rain
6 = 0.392 radian for snow
104
-------
APPENDIX D.2
Simplified Calculations of Dry Deposition at a Distance
For dry deposition at the distant farm, the following basic expression was
used (Slade, Section 7.9, Ref. 4, Eq. 5.41):
D ~ Vj T X
where D, vd, and T are defined in Section 7.2 2 of this report and X is the
average concentration in air at the deposition point, in pCi/tn3. 'lhe disper-
sion factor, K, in m*2, for various Pasquill diffusion conditions, normalized
for wind speed, is given graphically in Slade's Fig. A.7, page 413- It is
defined as:
and
KQ'
X=-rr
u
From Slade, Eq. 5.49:
(.iV (%\ V*2 v
?2 1
Subscript 1 ' 1*» denotes terms used in the graphs of Slade (Ref. 4, Section
7.9), Figure 5.5, and subscript ''2'' denotes terms desired for a specific
application. The depletion-corrected release rate at a wind speed, Ug, and
deposition velocity, vd » different from those chosen for the graphs in
Slade's Figure 5.5, (Q^) 2 are desired. Thus,
(4 ¦ («).(!}
because « vd = 10m/sec and = 1-m/sec. It follows that:
kq: ko: /o:\i/n
-------
where the term (Q^/Q„) is chosen directly from Slade's Figure 5.5. Substi-
tuting for X in the first equation,
<3:^dT /q;\ i/u
For dry deposition of 131] ^he Qhuse farm, 22 km NNE of the site under
Pasquill-type D (neutral) and type F (stable) conditions, K and Q'x/Q'0 values
were determined graphically (pp. 413 and 205 of Ref. 4, Section 7.9)• Under
neutral conditions, K was 1.1 X 10"^ m"2 and Q^/Qq was 0.45. The values were
2.4 X 10~6 m"2 and 0„75, respectively, for stable conditions. Q'o was taken as
550 pCi/sec. The factor (Q^/Q^)*approached unity. Wet deposition was
considered to be insignificant.
During the period of interest prior to June 26, wind blew from the Dresden
I stack over the Dhuse farm under neutral conditions for totals of 13 hrs at
an average speed of 7.7 m/sec. and under stable conditions for 22 hrs. at an
average speed of 5.5 m/sec. Total deposition of 13il for the period was
0.037 pCi/m2 and 0.19 pCi/m2 for the respective meteorological conditions.
Hourly depositions on any day could thus be calculated as fractions of the
total depositions by equations 7.3 and 7.4 in Section 7.2.2.
APPENDIX D.3
Estimated ,31| Deposition at Dirker Farm (075°-085°)
T, sec
u,
h,
L.
0 or W,
Date
x 10*3
n/sec
Stabi 1 ity
m
m
sec"1
pCi/m2
June 8
3.6
0.7
U
400
200
—
0.084
15
4.3
3.6
U
400
115
—
0.020
15
8.0
7.1
N
120
100
—
0.049
16
1.4
4.2
U
400
110
—
0.006
22
5.4
1.1
U
400
180
—
0.082
22
9.0
6.2
N
120
110
—
0.059
25
3.6
9.0
Ri
—
—
1.2 x 10"3
0.284
26
10.8
5.7
N
120
110
—
0.077
26
1.8
6.4
r2
---
3 x 10"4
0.067
6 = 0.1 74 radian
x = 3.4 x 103 nt
vd = 1 0"2 m/sec
Q„ ~ 550 pCi/sec
L on June 25 for rainfall of 10 mm/hr
L on June 26 for rainfall of 1 mm/hr
-------
APPENDIX D.4
Estimated ,31l Depositions at Dhuse Farm (180°-190°)
Date
T, sec
x 1 (T3
Stabi1i ty
0,
pCi M2
June 5
7.2
N
0.006
5
10.0
S
0.026
6
14.4
S
0.035
7
10.8
S
0.026
B
3.6
S
0.009
10
3.6
S
0.009
11
7,2
S
0.017
13
10.8
N
0.009
15
3.6
S
0.009
17-18
10.8
S
0.026
20
3.6
N
0.003
20
3.6
S
0.009
20-21
21.6
N
0.014
24
10.8
S
0.026
25
3.6
N
0.003
26
3.6
N
0.003
6 - 0.174 radian
x = 22 x 103 m
107
-------
APPENDIX D.5
Estimated ,3,l Deposition at M. McDonald Field (2B5°-280°)
T,
sec
u,
°V
K
0.
Date
x 1 0"3
m/sec
Stab i 1 i ty
m
m
pCi M2
June 9
3.6
1.5
U
270
140
0.059
9
14.4
4.4
U
270
100
0.082
11-12
50.4
10.3
N
90
85
0.254
21
3.8
7.0
N
90
85
0.027
21
3.6
4.0
N
90
100
0.039
24
10.0
2.6
N
90
120
0.138
26
7.2
B.O
N
90
85
0.047
27
57.5
7.8
N
90
85
0.382
28
25.0
6.3
N
90
85
0.206
July 1
10.5
6.3
N
90
85
0.086
3
7.2
2.5
U
270
110
0.071
3
7.2
2.7
N
90
110
0.102
5
7.2
3.0
U
270
110
0.059
x = 2.3 x 103 m
9 = 0.261 radian
v 10"2 m/sec
n = 550 pCi/sec
0
108
-------
APPENDIX D.6
Estimated 89Sr Deposition at Two Sites at Channahon* (210°-235°)
Date
T.
sec
x 10"3
u,
m/sec
Stabi1i ty
q;.
locat ion
pCi/sec
1 location 2
°zi'
m
°~z2*
ID
h,
m
D,.
pC i /hi2
o2,
pCi/m2
June 6
28.8
4.6
U
3,700
4,600
400
550
95
0.086
0.052
7
3.B
3.8
N
4,200
5,100
100
100
50
0.051
0.044
10
7.2
2.2
U
5,500
6,300
400
550
120
0.062
0.037
13
7.2
2.5
U
5,100
6,000
400
550
110
0.051
0.031
14
7.2
12.7
N
2,100
2,500
130
180
85
0.011
0.007
14
18.0
7.6
N
2,800
3,400
130
180
90
0.058
0.040
18
14.4
10.8
N
2,300
2,800
130
180
85
0.033
0.019
21
21.6
11.6
N
2,200
2,700
130
180
85
0.044
0.025
23
3.6
6.6
M
3,000
3,700
130
180
90
0.018
0.010
23
10.8
10.5
N
2,300
2,800
130
180
85
0.026
0.015
24
3.6
9.2
U
2,500
3,100
400
550
85
0.003
0.002
24
3.6
2.5
U
5,100
6,000
400
550
110
0.026
0.016
*0, = at John McDonald vegetable garden, 3.8 Km NE of site
02 = at Mrs. Hulbert vegetable garden, 5.4 km NE of site
6 = 0.437 radian
vd = 3 x 10'3 m/sec
QJ Based on average a9Sr release at stack of 1200 pCi/sec, plus ingrowth by decay of 89Kr
constituting at top of stack 1.2% of nominal gaseous fission product mixture released
at rate of 12,500 yu€i/sec; ingrowth time = x/u.
109
-------
APPENDIX D.7
Estimated 89Sr Concentration from Deposition in Leafy Vegetables at Cfiannahon
0, on 6/26,c
02 on 6/26/
Date
Days to 6/26
A/A Q«
pCi/to2
pCi/m2
June 6
20
0.28
0.024
0.015
7
19
0.30
0.015
0.013
10
16
0.36
0.022
0.013
13
13
0.44
0.022
0.014
14
12
0.47
0.005
0.003
14
12
0.47
0.027
0.019
18
8
0.60
0.019
0.011
21
5
0.73
0.032
0.019
23
3
0.83
0.015
0.008
23
3
0.83
0.022
0.012
24
2
0.83
0.003
0.002
24
2
0.88
0.023
0.014
Total
0.229
0.143
On leafy vegetable,
b pCi/g, ash
1.5 x 10~e
Effective half life = 11 days [half life on pasture = 14 days (Russell, Section 7.9,
Ref. 9, p. 302)]; A/A0 = fractional decrease of radioactivity in sample.
bEstimation for e9Sr in cabbage and lettuce based on Russell's data (p. 205) for uptake
of 90Sr in cabbage hearts, viz. 1 mCi/hi2 on soil = 3.15 x 10"3 mCi/kg dry weight; ash
wt./dry wt. = 0.39, from Table 7.4.
cBased on values in Appendix 0.6.
110
-------
APPENDIX D.8
Estimated 89Sr Deposition at Dhuse Farm and at Plainfield Truck Farm,
and Estimated Concentration in Grass and Leafy Vegetables
Date
D,a *b
pCi/to2
Days to
6/26
*/A0c
D
cor. for decay,
pCi An2
June 5
0.131
21
0.26
0.034
6
0.143
20
0.28
0.037
7
0.106
19
0.30
0.031
8
0.037
16
0.32
0.012
10
0.037
16
0.36
0.013
11
0.070
15
0.39
0.027
13
0.037
13
0.44
0.016
15
0.037
11
0.50
0.018
17-18
0.106
8
0.60
0.064
20
0.049
6
0.68
0.033
21
0.057
5
0.73
0.042
24
0.106
2
0.88
0.093
25
0.012
1
0.94
0.011
26
0.012
0
1.00
0.012
Total
0.44
On leafy vegetables, pCi/g, ashd
8.4 x 10~6
On grass, pCi/g, ash8
1.9 x 10*2
Computed from previously calculated ,3,l deposition at this location as follows:
Qx Sr-89 Vd Sr-89
x X
bQi Sr-89 = 7'300 PC'/Sec
Effective half-life on grass and vegetation = II days.
Estimation for 89Sr in mustard greens based on Russell's data (p. 205) for uptake
of 90Sr in cabbage hearts, viz. I mCi/in2 on soil = 3.15 x 10"3 mCi/kg dry weight.
'Assuming 100« retention on grass, 0.33 kg dry grass/in2 (Koranda, Section 7.9, Ref.
7, p. 31a) and 1% ash weight from dry grass (Nay, Section 7.9, Ref. 8).
Ill
-------
APPENDIX D.9
Estimated Deposition of 09Sr at Dirker Farm (075°-085°)
Date
«;•
pC i/sec
D.a
pCi/m2
Decay to 6/25,b
Decay
to 6/27,b
A/A,
pCi M2
A/A „
pCi M2
June 8
7,200
0.330
0.34
0.112
0.30
0.099
15
4,000
0.044
0.53
0.023
0.47
0.021
15
2,600
0.070
0.53
0.037
0.47
0.033
16
3,700
0.012
0.57
0.007
0.50
0.006
22
6,800
0.306
0.83
0.254
0.73
0.224
22
2,900
0.094
0.83
0.078
0.73
0.069
25
2,300
0.356
1.00
0.356
0.88
0.314
26
3,100
0.130
^ v «•
—
0.94
0.122
26
2,900
0.106
—
—
0.94
0.119
Total, pCi/m2
0.87
1.01
On grass, pCi/g,
ashc
4.1
x 10"z
8,b,cSee footnotes a, c, and e, respectively, in Appendix 0.8.
112
-------
APPENDIX D.10
Transfer of ml from Grass to Cows' Milk
(Single Deposition, Cows Remaining on Pasture)8
Time after Deposition
Concentration,b
(Days)
%/\ i ter
0.5
0.14
1.0
0.27
1.5
0.31
2.0
0.34
2.5
0.36
3.0
0.35
4.0
0.32
5.0
0.29
6.0
0.25
7.0
0.22
10.0
0.14
Thereafter, concentration decreases with 5-day half life
"Taken from graph by Garner and Russell, Section 7.9, Ref. 10, p. 303.
bPercent of total intake on day of deposition appearing per liter of milk at day
stated in first column.
113
-------
APPENDIX D.ll
Estimated 131l in Milk from Dirker Cows
on June
25
on June
26
on June
27
Deposi tion
Dai 1ya
Cone.,
Cone.,
Cone.,
on date,
Uptake,
Transfer,11
pCi/l
Transfer,11
PCi/l
Transfer,11
pCi/l
Date
pCi /to2
pCi
%/\ iter
CM
CD
X
%/\ i ter
x 102
VI i ter
x 102
June B
0.084
3.78
0.053
0.20
0.046
0.17
0.040
0.15
15
0.069
3.11
0.14
0.44
0.12
0.37
0.11
0.33
16
0.006
0.27
0.16
0.04
0.14
0.04
0.12
0.03
22
0.141
6.35
0.35
2.22
0.32
2.04
0.29
1.85
25
0.204
12.0
0.14c
1.00
0.31d
3.97
0.366
4.61
26
0.144
6.48
—
—
0.14°
0.91
0.31d
2.01
Total, pCi/l 0.047 0.075 0.090
"Assuming cow effectively grazes 45 m2/day (Koranda, Section 7.9, Ref. 7).
b6ased on Appendix D.10.
c0.5-day interval from deposition to milking.
d1.5-day interval from deposition to milking.
®2.5-day interval from deposition to milking.
114
-------
APPENDIX D.12
Estimated ,3'l in Milk from Dhuse Cows
on June
25
on June
27
Dai ly
Cone.,
Cone.,
Deposition
Deposi tion,
Uptake,
Transfer,
pCi/l
T ransfer,
pCi./l
Date
pCi/m2
pCi
%/\ i ter
x 102
%/\ i ter
x 102
June 5
0.032
1.44
0.035
0.05
0.027
0.04
6
0.035
1.57
0.040
0.06
0.030
0.05
7
0.026
1.17
0.046
0.05
0.035
0.04
8
0.009
0.41
0.053
0.02
0.040
0.02
10
0.009
0.41
0.070
0.03
0.053
0.02
11
0.017
0.77
0.080
0.06
0.060
0.05
13
0.009
0.41
0.11
0.05
0.080
0.03
15
0.009
0.41
0.14
0.06
0.11
0.05
17-18
0.026
1.17
0.22
0.26
0.16
0.19
20
0.012
0.54
0.29
0.16
0.22
0.12
20-21
0.014
0.63
0.32
0.20
0.25
0.16
24
0.026
1.17
0.27
0.32
0.35
0.41
25
0.003
0.14
0.14°
0.02
0.36®
0.05
26
0.003
0.14
—
—
0.31d
0.04
27
None
—
—
---
—
—
Total, pCi/l
0.013
D.013
See footnotes to Appendix D.11.
-------
APPENDIX D.13
Estimate of ,31l Concentrations in Thyroids of McDonald Heifers
Fresh
Cumulative
Depn.,
Depn.,a
Daily uptake
131l in Thyroids
pC i /hi2
pCi/mz
by thyroid,b
as of July 10,c
Date
(D)
(C.)
pCi
pCi
June 9
0.059
9
0.082
0.141
11-12
0.254
0.347
Cows placed in pasture on June 16
16
—
0.198
1.78
0.17
17
—
0.174
1.58
0.16
18
—
0.153
1.38
0.16
19
—
0.132
1.19
0.15
20
—
0.114
1.03
0.14
21
0.027\
0.167
1.50
0.23
21
0. 039 f
22
—
0.145
1.31
0.22
23
—
0.127
1.14
0.21
24
0.138
0.248
2.23
0.46
25
m a* •»
0.216
1.93
0.44
26
0.047
0.236
2.12
0.53
27
0.382
0.5B8
5.29
1.46
20
0.206
0.718
6.46
1.96
29
—
0.625
5.63
1.89
30
—
0.546
4.91
1.83
July 1
0.086
0.560
5.04
2.07
2
—
0.487
4.38
1.99
3
0.0711
0.598
5.38
2.69
3
0.102J
4
—
0.520
4.68
2.58
5
0.059
0.514
4.62
2.82
6
—
0.447
4.02
2.71
7
m m m
0.390
3.51
2.61
Total
27.5
aEnvi ronmentaI = 5 days.
bCow effectively grazes 45 m2 grass/day [Koranda]; 20% of intake goes to
thyroid [Garner]; values are 45 x 0.2 x Cg.
^Biological 7^ ¦ 7 days.
-------
RADIOLOGICAL SURVEILLANCE STUDIES AT A BOILING WATTO NUCLEAR
POWER REACTOR. B. Kahn, R. L. Blanchard, H. L. Krieger, H. E,
Kolde, D, B. Smith, A. Martin, S. Gold, W. J, Averett, W. L.
Brinck, and G. J. Karches; Feb. 1970; EER 70-1; DER, EPH, HEW.
Radionuclides in water, gases, and airborne particles were
measured at the Dresden Nuclear ft>wer Station and in its environ-
ment in order to provide the technical basis for surveillance
programs at nuclear power stations. Concentrations of radio-
nuclides in the primary coolant and the off-gas were determined
on several occasions; at the same time, radioxenon concentrations
and external radiation exposures were measured near the plume
within 1 to 2 km of the stack, and the radionuclide content of
effluent water was measured near the point of discharge. Samples
of food, feed, and water from the immediate environment were
also analyzed for specific radionuclides. Results of radionuclide
analyses and radiation exposure calculations are presented, and
analytical techniques for measuring radionuclides at low concen-
trations and in complex mixtures are indicated.
KEY WM6:
Miclear
Rawer
Radiological
SurveiIlance
Radionuclide
Analysis
Radiation
Exposure
Reactor
Effluents
RADIOLOGICAL SURVEILLANCE STUDIES AT A BOILING WATEH NUCLEAR
POWER REACTOR. B. Kahn, R. L Blanchard, H. L. Krieger, H. E.
Kolde, D. B. Smith, A, Martin, S. Gold, W. J, Averett, W. L.
Brinck, and G. J. Karches; Feb. 1970; ETO 70-1; DER, EPH, DO,
Radionuclides in water, gases, and airborne particles were
measured at the Dresden Nuclear Power Station and in its environ-
ment in order to provide the technical basis for surveillance
programs at nuclear power stations. Concentrations of radio-
nuclides in the primary coolant and the off-gas were determined
on several occasions; at the same time, radioxenon concentrations
and external radiation exposures were measured near the plume
within 1 to 2 km of the stack, and the radionuclide content of
effluent water was measured near the point of discharge. Sanples
of food, feed, and water from the immediate environment were
also analyzed for specific radionuclides. Results of radionuclide
analyses and radiation exposure calculations are presented, and
analytical techniques for measuring radionuclides at low concen-
trations and in complex mixtures are indicated.
KEY WHS:
Nuclear
Fbwer
Radiological
Surveillance
Radionuclide
Analysis
Radiation
Esqposure
Reactor
Effluents
RADIOLOGICAL SURVEILLANCE STUDIES AT A ROILING WATER NUCLEAR
POWER REACTOR. B. Kahn, R. L. Blanchard, H. L. Krieger, H, E.
Kolde, D. B> Smith, A. Martin, S. Gold, W. J. Averett, W. L.
Brinck, and G. J. Karches; Feb. 1970; HP 70-1; DER, EPH, MW.
Radionuclides in water, gases, and airborne particles were
measured at the Dresden Nuclear fewer Station and in its environ-
ment in order to provide the technical basis for surveillance
programs at nuclear power stations. Concentrations of radio-
nuclides in the primary coolant and the off-gas were determined
on several occasions; at the same time, radioxenon concentrations
and external radiation exposures were measured near the plume
within 1 to 2 km of the stack, and the radionuclide content of
effluent water was measured near the point of discharge. Sanples
of food, feed, and water from the immediate environment were
also analyzed for specific radionuclides. Results of radionuclide
Analyses and radiation exposure calculations are presented, and
analytical techniques for measuring radionuclides at low concen-
trations and in complex mixtures are indicated.
KEY VOTE:
Nuclear
Rjwer
Radiological
Surveillance
Radionuclide
Analysis
Radiation
Eiposure
Reactor
Effluents
------- |