United States
Environmental Protection
Agency
Office of
Reseach and
Development
Environmental Monitoring
and Support Laboratory
Las Vegas, Nevada 89114
EPA-600/7-77-079
July 1977
CHARACTERIZATION OF
EMISSIONS FROM PLUTONIUM-
URANIUM OXIDE FUEL
FABRICATION
Interagency
Energy-Environment
Research and Development
Program Report
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RESEARCH REPORTING SERIES
Research reports of the Office of Research and Development, U.S. Environmental
Protection Agency, have been grouped into nine series. These nine broad cate-
gories were established to facilitate further development and application of en-
vironmental technology. Elimination of traditional grouping was consciously
planned to foster technology transfer and a maximum interface in related fields.
The nine series are:
1. Environmental Health Effects Research
2. Environmental Protection Technology
3. Ecological Research
4. Environmental Monitoring
5. Socioeconomic Environmental Studies
6. Scientific and Technical Assessment Reports (STAR)
7. Interagency Energy-Environment Research and Development
8. "Special" Reports
9. Miscellaneous Reports
This report has been assigned to the INTERAGENCY ENERGY-ENVIRONMENT
RESEARCH AND DEVELOPMENT series. Reports in this series result from the
effort funded under the 17-agency Federal Energy/Environment Research and
Development Program. These studies relate to EPA's mission to protect the public
health and welfare from adverse effects of pollutants associated with energy sys-
tems. The goal of the Program is to assure the rapid development of domestic
energy supplies in an environmentally-compatible manner by providing the nec-
essary environmental data and control technology. Investigations include analy-
ses of the transport of energy-related pollutants and their health and ecological
effects; assessments of, and development of, control technologies for energy
systems; and integrated assessments of a wide range of energy-related environ-
mental issues.
This document is available to the public through the National Technical Informa-
tion Service, Springfield, Virginia 22161.
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EPA-600/7-77-079
July 1977
CHARACTERIZATION OF EMISSIONS FROM
PLUTONIUM-URANIUM OXIDE FUEL FABRICATION
by
E. W. Bretthauer, A. J. Cvnraoings, and S. C. Black
Monitoring Systems Research and Development Division
Environmental Monitoring and Support Laboratory
Las Vegas, Nevada 89114
U.S. ENVIRONMENTAL PROTECTION AGENCY
OFFICE OF RESEARCH AND DEVELOPMENT
ENVIRONMENTAL MONITORING AND SUPPORT LABORATORY
LAS VEGAS, NEVADA 89114
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DISCLAIMER
This report has been reviewed by the Environmental Monitoring and Support
Laboratory-Las Vegas, U.S. Environmental Protection Agency, and approved for
publication. Approval does not signify that the contents necessarily reflect
the views and policies of the U.S. Environmental Protection Agency, nor does
mention of trade names or commercial products constitute endorsement or recom-
mendation for use.
ii
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FOREWORD
Protection of the environment requires effective regulatory actions which
are based on sound technical and scientific information. This information must
include the quantitative description and linking of pollutant sources, trans-
port mechanisms, interactions, and resulting effects on man and his environ-
ment. Because of the complexities involved, assessment of specific pollutants
in the environment requires a. total systems approach which transcends the media
of air, water, and land. The Environmental Monitoring and Support Laboratory-
Las Vegas contributes to the formation and enhancement of a sound integrated
monitoring data base through multidisciplinary, multimedia programs designed
to:
• develop and optimize systems and strategies for moni-
toring pollutants and their impact on the environment
• demonstrate new monitoring systems and technologies by
applying them to fulfill special monitoring needs of
the Agency's operating programs
This report describes efforts to develop optimized monitoring techniques
for measuring plutonium emissions from a mixed oxide fuel fabricating facility.
This report should be useful in the design of monitoring systems for similar
types of nuclear facilities. The users who should find this report of value
are the various regulatory agencies involved in standards setting and com-
pliance monitoring such as the Nuclear Regulatory Commission, U.S. Environ-
mental Protection Agency, U.S. Energy Research and Development Administration,
and the State and local agencies. Further information on this research may be
obtained from the Methods Development and Analytical Support Branch of this
Laboratory.
George B£ Morgan'
Director
Environmental Monitoring and Support Laboratory
Las Vegas
iii
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ABSTRACT
To develop accurate techniques for monitoring plutonium emissions from
plutonium-uranium oxide fuel fabrication facilities, knowledge of the appropriate
physical and chemical properties of the released plutonium are necessary. In-
stack, standard hi-vol, and special ultra-high volume air samplers were used
to collect particulate samples at the Babcock and Wilcox mixed oxide facility
in Parks Township, Pennsylvania.
The number of radioactive particles emitted, the particles sizes, and
plutonium and uranium isotopic content were determined. These characteristics
are used to propose an appropriate monitoring technique for plutonium for
facilities of this type.
iv
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CONTENTS
FOREWORD
ABSTRACT
LIST OF FIGURES AND TABLES
LIST OF ABBREVIATIONS
LIST OF SYMBOLS
ACKNOWLEDGMENTS
INTRODUCTION
CONCLUSION
RECOMMENDATIONS
METHODOLOGY
SAMPLING
ANALYSIS
ANALYTICAL RESULTS OF STACK SAMPLES AND CHARACTERIZATION
OF THE EMISSIONS ENTERING THE ENVIRONMENT
FISSIONABLE PARTICLE CHARACTERIZATION
NONFISSIONABLE PARTICLES
GROSS PLUTONIUM EMISSIONS
RESULTS OF ENVIRONMENTAL AIR ANALYSIS
PARTICLE CHARACTERIZATION
GROSS ACTINIDE ANALYSIS
REQUIREMENTS FOR MONITORING
REFERENCES
APPENDIX A. ENVIRONMENTAL SAMPLER DATA
APPENDIX B. USGS TOPOGRAPHIC MAP OF LEECHBURG, PA. AREA
APPENDIX C. RESULTS OF PLUTONIUM-238 and -239 ANALYSES
OF SOIL SAMPLES
APPENDIX D. RESULTS OF INDIVIDUAL PARTICLE ANALYSIS: STACK SAMPLES
APPENDIX E-l RESULTS OF GROSS ANALYSIS OF ENVIRONMENTAL SAMPLES
APPENDIX E-2 GROSS ISOTOPE LEVELS FROM MASSIVE AIR SAMPLES
APPENDIX F. RESULTS OF INDIVIDUAL PARTICLE ANALYSIS:
ENVIRONMENTAL AIR SAMPLES
APPENDIX G. PARTICLE PHOTOGRAPHS
v
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LIST OF FIGURES AND TABLES
Number Pag
FIGURES
1 Babcock and Wilcox process flow diagram for fuel 2
fabrication
2 Stack and high efficiency particulate air filter 7
arrangement
3 Stack sample port geometry 8
4 Mr and soil sampling locations 9
5 Size distribution of the fissionable particles 13
6 Equivalent size of PuO -tFO particles from 18
sample 43 based upon tracks
7 Predicted ground-level plume concentration 22
8a Plume concentration versus variable windspeed, 24
relative values.
8b Plume concentration versus variable crosswind 24
distance, relative values.
TABLES
1 Number of Particles Characterized in Each 12
Fission Track Group
2 Calculation of Plutonium Activity from Fission 15
Track Data from Half of Sample 43
3 Plutonium-239 Emission Summary 17
4 Equivalent Size of PuO —UO Particles from 18
Sample 43 x x
5 Atmospheric Turbulence Parameters 20
6 Key to Atmospheric Stability Categories 21
7 Ground-Level Plume Concentrations from 23
Dispersion Model
vi
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LIST OF ABBREVIATIONS
Abbreviations
Ar
BCL =r
em2 =
cm =
cm/s =
Ci
Ci/g---
Ci/ni =
DOP
dpm =
BMP =
fCi =
FeSO =
FT X =
ft . =
g
h
H2 =
H2° =
HEDL =
HEPA =
kg
km =
1
1/min =
m =
m/min =
micrometer m_ =
attocurie (10 = atto) mi?
argon Wo/h =
Battelle Columbus Laboratory m /min=
centimeter min =
square centimeters mm -
centimeters per second m/s =
curie N- =
curies per gram NaCl =
curies per cubic me.ter nCi =
dioctylphthalate ng =
disintegrations per minute NMD -
electron microgrphe NRC
femtocurie (10 = femto) 0 -
iron sulfates and sulfites pCi =
fissipn tracks pCi/g =
cubic feet Pu =
gram PuQ2 =
hour PuO =
hydrogen QA x -
water s =
Hanford Engineering and SEM =
Development Laboratory SiO =
high efficiency particulate TEMX =
air (filter)
kilogram TiO
kilometer U x =
liter U02
liters per minute UO =
meter x
meter per minute
square meters
cubic meters
cubic meters per hour
cubic meters per minute
minute
millimeter
meters per second
nitrogen
sodium chloride (salt)
nanocurie (10 = nano)
nanogram
Nuclear Materials Development
Nuclear Regulatory Commission
-12
= pico)
oxygen
picocurie (10
picocurie per gram
Plutonium
plutonium dioxide
Plutonium oxides
Quality Assurance
second
scanning electron microscope
silicon oxides
transmission electron micro-
scope
titanium oxides
uranium
uranium dioxide
uranium oxides
vii
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LIST OF SYMBOLS
Symbols
a
C-,
D
H
H
n.
r
t
acceleration due to gravity
percentage of cation number 1
percentage of cation number 2
percentage of cation number 3
apparent particle diameter
micrometers
aerodynamic diameter of.
particle, micrometers
inside stack diameter, meters
stack height, meters
effective stack height, meters
length, micrometers
index of refraction
particle density, grams per
cubic centimeter
air density, grams per cubic
centimeter
emission rate, particles per
second and/or particles per
cubic meter; flow rate, in /min
distance from center of sam-
pling tube to stack wall
thickness, micrometers
U
U)
X
y
a
a
n
X
ambient temperature, Kelvin
temperature of stack gas,
°Kelvin
time averaged wind velocity at
the height, H, meters per
second
stack gas velocity, meters per
second
width, micrometers
downwind distance, meters
crosswind distance, meters
vertical distance, meters
standard deviation of the time
averaged plume concentration
distributed in the crosswind
direction
standard deviation of the
time averaged plume concen-
tration distributed in the
vertical direction
density, grams per cubic
centimeter
density of cation number 1
density of cation number 2
density of cation number 3
viscosity of air, poise
ground-level concentration,
picocuries per cubic meter
and/or particles per cubic
meter
viii
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ACKNOWLEDGMENTS
The authors wish to thank the management of Babcock and Wilcox, espe-
cially Mr. Grant LaPier and Mr. David Ortz, for allowing the U.S. Environ-
mental Protection Agency (EPA) to conduct this study at the Babcock and
Wilcox mixed oxide fuel fabrication facility and for their assistance in
providing support in changing air filters and in providing meteorological
data. The authors would also like to thank the Hanford Engineering and
Development Laboratory, Westinghouse Corporation, particularly Mr. Robert
Smith, for providing use of their exhaust stack sampling ports.
The authors also wish to acknowledge the EPA's Office of Radiation
Programs, Mr. Donald W. Hendricfcs and Dr. Robertson Augustine; the Nuclear
Regulatory Commission, Mr. Bernard Weiss; and EPA's Region III Office,
Dr. Lee H. Bettenhausen for assisting with arrangements for conducting this
study.
ix
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INTRODUCTION
The objective of this research is to develop techniques for monitoring
plutonium emissions from mixed oxide fuel fabrication facilities. Appropriate
monitoring techniques and procedures for particulate plutonium emissions are
dependent upon a number of factors; among the most important are the physical
(size, shape, density, specific activity) and chemical properties of these
particulates. Additional factors which must be considered are the effects of
aging and climatic conditioning of individual particles containing plutonium
after their release into the environment. These factors led to a requirement
for sampling at and in the environs of a plutonium-uranium oxide fuel fab-
rication facility. At the inception of this research there were only two
facilities in the United States fabricating mixed plutonium-uranium oxide
fuels: Babcock and Wilcox, located in Pennsylvania, and Kerr-McGee, located
in Oklahoma. Each of these facilities had established a prototype production
line (using different chemical processes) for fabricating fuel for a breeder
reactor.
It was decided that the Babcock and Wilcox facility should be sampled
first because an intensive investigation by the Nuclear Regulatory Commission
(NRG) and certain other governmental bodies was being conducted at the Kerr-
McGee facility which precluded any sampling effort in the time frame allocated
to this research effort.
The Babcock and Wilcox mixed oxide facility, hereafter referred to as
the Plant, is one of three facilities located on 59 acres (23.9 hectare) of
land approximately 5 kilometers (km) northeast of Apollo, Pennsylvania. The
other two facilities are the Metals Complex and the Nuclear Materials Devel-
opment (NMD) Type II Plant. Specialty metals (but no nuclear materials) are
handled at the Metals Complex, and highly enriched uranium is processed in
the NMD Type II Plant.
Principal operations of the Plant include a glove box line for the
fabrication of finished rods, or pins, of mixed oxide pellets (plutonium
dioxide mixed with uranium dioxide), and a scrap recovery line that produces
purified plutonium nitrate solution from scrap materials. Plutonium nitrate
from the scrap recovery line is ultimately shipped from the Plant.
Five basic steps are used to produce finished fuel rods. Plutonium
dioxide powder undergoes several physical preparatory steps, and then is
blended with uranium dioxide. This mixed oxide powder is formed into high-
density pellets via a conventional pelletizing procedure. Finally, the
peletize,d mixed-oxide fuel is loaded into rods which, in turn, are welded,
inspected, washed, and loaded for shipment. A recycle line also exists,
whereby rejected pellets and/or powder can be worked back into the mixed
oxide line. The process is outlined in Figure 1.
Plutonium-bearing scrap, either from outside customers or from the
mixed oxide operations, is dissolved in a nitric acid/hydrofluoric acid
mixture. The resultant plutonium nitrate solution is purified by ion ex-
change columns, concentrated, collected in 10-liter (1) bottles, and stored
until ready for shipment.
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ro
uo2
V- BLEND-
JET MILL
SCREEN
Pu00
I2.
CALCINE
BALL MILL
1
SCREEN
170 MESH
1
V-BLEND
Tlm<-l».-IT TI
U(J2
_ TT TIT W»TT*
JET MILL
SCREEN
GREEN RECYCLE
ORGANIC REMOVAL
OXIDATION/REDUCTION
850° AIR/N2 -8% H^
BALL MILL
LOT V-BLEND* SAMPLE, Pu, IMPURITIES
| POWDER CHARACTERIZATION
ORGANIC ADDITION
SLUGGING
ION
GRANULATION & SCREEN
V-BL
-DIE LUBRICANT (STEROTEX)
END
SIEVE
100 MESH
V-BLEND
SINTERED RECYCLE
OXIDATION/REDUCTION
850? AIR/N0 -8% H.
BALL MILL
PRES
PRE-SINTER'
SINTER-—
V
A
-Ar + 8% H,
-Ar + 8% H,
Figure 1. Babcock and Wilcox process flow diagram for fuel fabrication.
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-DIMENSIONAL.
INSPECTION
_PELLET DENSITY
CHECKS
SAMPLE FOR Pu:;
ASSAY U ASSAY,
impurities, homo-
geneity, dimensions,
density, visual
CENTERLESS GRIND
(DRY)
LOT SAMPLING
COMPONENT-
"BAKE-OUT
ROD LOADING
DECONTAMINATE
WELDING
INCONEL REFLECTOR
-METTAOGRAPHY
WELD CHAMBER
GAS PURITY
.ality Assurance(QA)
GAS TAG
PUNCTURE
X-RAY *
-QA
CLADDING TUBE
FIRST END WELD
LOADING FUNNEL
MAKE UP
COMPONENT
-LOADING •«
TOPEND CAP
GAS TAG
PLENUM TUBES
SPRING INCONEL
REFLECTOR
-BOTTOM END
CAPS
RESIDUAL FLUORINE AND CHLORINE
FINAL CLEANING
AND PASSIVATION
FINAL COUNT
DIMENSIONAL., VISUAL
INSPECT QA
PACKAGE FOR
SHIPMENT
Figure 1. Babcock and Wilcox process flow diagram for fuel fabrication, (continued),
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The exhaust emissions from glove boxes (after initial high efficiency
particulate air (HEPA) filtration), hoods> etc., which are used in the prep-
aration of the fuel pins as well as emissions from an analytical laboratory,
cafeteria, and office area are all passed through prefilters and final HEPA
filters (Filter No. 7W-60NL-N2N2 manufactured by Flanders Filters, Inc.*)
before exhaustion into the atmosphere through a stack with an inside diameter
of 0.46 meter (m) at a velocity of 401 meters per minute (m/min). The Hanford
Engineering and Development Laboratory (HEDL), Westinghouse, Inc., and Bab-
cock and Wilcox had established sampling stations in the stack. HEDL and
Babcock and Wilcox engineers had determined stack velocities, sampling points,
and flow rates for isokinetic sampling both, upstream and downstream relative
to the final HEPA filter banks by a hot-wire anemometer technique. The
emissions from processing the plutonium-bearing scrap are not exhausted through
this stack.
CONCLUSION
The following conclusions concerning the character of the plutonium-
uranium stack emissions from a typical mixed Oxide fuel fabrication facility
can be made from this research:
1. Approximately 4.5 nanocuries (nCi) of plutonium-239 was emitted
into the atmosphere per kilogram (Teg) of plutonium fabricated into mixed oxide
fuel. This is equivalent to 0.15 nCi per fuel piii fabricated. The pluton-
ium-239 was being emitted into the atmosphere in the form of submicron par-
ticles with an aerodynamic mean diameter of 0.2 micrometer (HOD.) . Approx-
imately 300,000 particles were emitted into the. atmosphere per kilogram (kg)
of fuel fabricated or 10,000 particles per fuel pin fabricated. The average
activity of each particle emitted was 15.1 femtocurie (fCi). These particles
have been identified individually and as occlusions and inclusions in host
particles of feldspars, flyash, organic or carbonaceous materials. The
chemical form of the individual particles was plutonium-uranium oxide.
2. Plutonium-239 was being; emitted into the environment, although in
quantities too small to be detected by standard air monitoring techniques for
collection and gross alpha analysis of air samples. In addition, the amount
of uranium found in the environmental air samples tended to mask the small
amount of plutonium present when only gross alpha measurements were made.
3. Due to extraneous materials on stack sampling filters, particle
penetration into the filter, and isotope composition, direct alpha counting
of stack sampling filters may substantially underestimate the amount of plu-
tonium emitted into the environment. In this case, plutonium emissions were
estimated more than 60 percent low.
*This filter shows a retentivity of 99.. 97 percent by standard DOT? (dioctyl-
phthalate) test.
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4. Soil samples taken in the environs of the Plant indicated plutonium-
238 and/or -239 in concentrations ranging from less than 0.003 picocuries per
gram (pCi/g) to 0.3 pCi/g. These variable and relatively high levels preclude
soil sampling and analysis as an applicable monitoring technique.
RECOMMENDATIONS
The results of this study indicate that plutonium emissions from this type
of facility should be determined by sampling directly at the source. The source
can be considered as some point after the final stack filters and before
exhaustion into the atmosphere. Environmental air sampling, using samplers
capable of minimum sampling rates of 500 cubic meters per hour (m /h), should
be used as a check on the stack monitoring program.
Sampling programs near new sources of possible actinide pollution must
commence well in advance of establishment of any such sources. The prime
considerations here are:
a. A thorough study of existing actinides in the environment must be
made prior to the commencement of plant operation. The types of actinide
present, the isotopic composition and the amount present must be determined.
b. Typical meteorological conditions must be well established.
c. Realistic dispersion calculations, based on plant engineering design
and meteorological predictions, should be used to determine sampling sites
for maximum probability of pollutant collection.
d. The collection devices and medium used for stack monitoring must be
chosen to provide optimum sampling conditions (location in stack, flow rates).
e. Basic isotopic information is required to establish standard
analytical techniques for monitoring of routine samples. Therefore, periodic,
detailed analysis of particulate pollutants must be made to establish any
variations in isotopie composition or change in prefilter and final filter
efficiencies.
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METHODOLOGY
SAMPLING
Stack Sampling
The stack used to exhaust particulate matter from tue preparation of fuel
pins was sampled using the setup shown in Figure 2. Figure 3 shows the sample-
port geometry. The stack from the scrap processing area was not sampled
because it was not in operation during the sampling period. In brief, 47-
millimeter (mm) diameter Millipore type AA filters backed with Microsorban type
99/97 filters were exposed isokinetically to the stack emissions through sam-
pling tubes at flow rates of 19.8 liters/min (1/min) and 21.2 liters/min up-
stream and downstream of the HEPA filters, respectively. These samplers were
run continuously for the 86-day period from 5/15/75 to 8/9/75. The Millipore
filters have a pore diameter of approximately 0.8 micrometer. Microsorban
filter material has a retentivity greater than 99 percent for particles of
diameter greater than or equal to 0.3 micrometers.
The filters were removed by Babcock and Wilcox personnel after appropriate
instruction. Fuel fabrication operations were conducted for 51 days of the 86-
day sampling period (the Plant was not in operation on weekends or on May 29 or
August 5). During this 51-day production period, 103.8 kilograms of plutonium
(524.3 kilograms of mixed oxide fuel) and 3,034 fuel pins were produced. The
composition of the fuel, ratio of plutonium^239 to uranium-238, for May and
June was 24.2 percent and from July to August was 19.8 percent.
Environmental Air Sampling
The first phase of the environmental air sampling program was conducted
over the period from 5/14/75 to 8/14/75. Air samplers using_100-mm Microsorban
type 99/97 material and sampling at an average rate of 1.8 m /h were operated
at several locations in the environs of the Plant by Babcock and Wilcox person-
nel. Air sampling locations are shown in Figure 4. Appendix A contains a
table of sampling data. Meteorological data indicated that the prevalent winds
were to the north-northeast approximately 37 percent of the time during the
sampling period. This information was used to determine air sampling loca-
tions. Two samplers were located downwind of the stack; one was about 100
, meters from the stack while the second was about 900 meters further downwind.
A third sampler was located on the site of the cylinder storage area. A fourth
sampler, located 8 kilometers crosswind to the southeast and denoted as station
5, served as a background sampling location. Typical sampling times were 500
hours.
The second phase of the environmental sampling program used a massive
volume air sampler located near the cylinder storage area. The flow rate
through this sampler was approximately 1600 m /h. The particle collection was
by impaction and electrostatic precipitation. The sampler fractionated partic-
ulates into three size ranges: 1) less than 1.7 micrometers, 2) 1.7 to 3.5
micrometers, and 3) 3.5 to 20 micrometers. Aside from the obvious advantage of
-------
Endcap
Airflow
Upstream
sampler ports
0.69 m to center of manifold
HEPA filters
0.51 m~
/
/
n
To HEPA
filter bank
valve normally closed
ID
Downstream sampler ports
0.43 m to center of manifold
NOTE:
All major ducts
are 0.46-m In diameter
To blower and stack
Figure 2. Stack and high efficiency particulate air filter arrangement.
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~
0.46m
1
\=
Downstream
V
(m/min)
401
366
r
(cm)
1.38
2.48
Q*
(mVmin)
0.0189
0.0172
Filter:
Millipore AA/Microsorban
Rotameter
Vacuum
"Sampling Port inside diameter = 0.775cm System
Figure 3. Stack sample port geometry.
8
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85
#8
I Cylinder Storage '
i !
S = Soil Sample*
# = Air Samplers
I _J
\ r BCL
{
'
SI
S4
Parking Lot
S2 S9
#7
I
PLUTONIUM PLANT
l
Figure 4. Air and soil sampling locations,
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the high sampling rate, the particulates were collected free from any filter
matrix and in gram quantities (typical for a 7-day sampling period). This
sampler was operated for the 7-day period from 10/22/75 to 10/29/75. The Plant
was not operating during this period.
Soil Sampling
Soil samples were taken from several locations in the environs of the
Plant. The locations where the soil samples were taken are shown in Figure 4.
A topographic map of the general area is shown in Appendix B. A method devel-
oped by Johnson et al. (1975) was used for collecting the soil samples. John-
son's method requires 4 square meters (m ) of surface soil to be swept and
collected, however, this method was developed for desert and other relatively
arid and vegetation-free areas. The land area surrounding the Plant was
covered with grasses and commercial farm crops, thus a very limited area was
available for sampling via the Johnson technique. Soil was collected from a
drainage ditch near the Plant cylinder storage area, near the northeast fence
area, and from runoff silt deposited in the parking lot. Several other small
areas were sampled near the Plant; however, in these cases it was not possible
to sweep the full 4 m area. Soil samples were also obtained from three
upwind locations as well as two locations further downwind. The soils were
subsequently sieved and the 150-mierometer fraction was used for alpha spec-
"trometry analysis. The results of all soil analyses are shown in Appendix C.
ANALYSIS
Stack and Environmental Air Samples
A portion of each stack and air sample was soluBilized and analyzed by
mass spectrometry for isotopes of plutonium and uranium. Another portion of
each stack and air sample was taken for particle analysis. Particle analysis
was performed in two steps: (a) identification of radioactive particles, and
(b) detailed physical and chemical analysis of selected radioactive particles.
a. Identification of Radioactive Particles"—
This portion of the analysis consists of autoradiography by
photographic and/or track-etch techniques after neutron irradiation of the
filter to determine the total number of fissionable particles present per unit
sample area and the distribution of such particles according to activity levels.
(Becker 1969, Fleischer 1963, McCrone 1173).
b. Detailed Physical and Chemical Characterization'--
A portion of the sample was chosen and particles were separated
by chemical or physical means designed to preserve the integrity of any con-
tained particles. Individual -particles were examined to provide, in as much
detail as possible, the level of alpha activity per particle and an estimate
of the size ranges of the particles. Several particles in each size range
were then chosen for further study. Size and shape estimations and photo-
-------
graphs were made by optical or electron microscopy as appropriate to particle
size. The gross elemental composition of certain of these particles was de-
termined by electron microprobe analysis. Finally, mass spectrometric analysis
was used to determine isotopic composition of the plutonium or uranium present
on or in the particle. Analysis of non-fissionable particles was identical to
that of fissionable particles except that track-etch studies were not done.
ANALYTICAL RESULTS OF STACK SAMPLE AND CHARACTERIZATION
OF THE EMISIONS ENTERING THE ENVIRONMENT
The sample taken downstream of the final HEPA filter (sample 43) had a
gross alpha count of 190 disintegrations per minute (dpm) and the sample taken
upstream of the final HEPA filter (sample 44) had a gross alpha count of 1.2
x 10 dpm (these measurements were made by Babcock and Wilcox using an alpha
counter on the unprocessed samples and represents their standard analysis
technique). No further analyses of sample 44 were attempted because of the
high activity. The information below was obtained from sample 43.
FISSIONABLE PARTICLE CHARACTERIZATION
A variety of representative particles on sample 43 were characterized
by optical and electron microscopy. A significant number of these contained
small particles of PuO -UO attached to host particles containing aluminum,
silicon, iron, and oxygen. These host particles are either flyash or nat-
urally occurring feldspars. In most instances the PuO -UO inclusions were
too small to obtain any physical characteristics. Other PuO -UO particles
were associated with organic or carbonaceous material. The latter was most
probably of biological origin Ci.a., vegetative plant tissue).
Particle Selection
A total of 140 fissionable particles was optically characterized. These
included host particles that contained one or more fissionable inclusions or
occlusions. An attempt was made to optically characterize a representative
number of particles with less than 1000 fission tracks. A summary of the
optical measurements is presented in Appendix D-2.
11
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TABLE 1. NUMBER OF PARTICLES CHARACTERIZED IN EACH FISSION TRACK GROUP
Number of
Fission Track Range Particles Characterized
1
17
33
65
129
256
TOTAL
- 16
- 32
- 64
- 128
- 256
- 1000
>1000
21
20
20
21
27
24
7
140
Particle Size
The particle sizes were determined using an optical microscope. An
apparent diameter was calculated, using maximum dimensions, by the following
equation:
d = (I x w x t) (1)
Where the thickness could not be determined, it was estimated as one-half
width. In Appendix D-2 some sizes are recorded as zero because these particles
were less than 2 pm and thus too small to adequately characterize. A particle
size distribution of the 140 particles characterized in Appendix D-2 is pre-
sented in Figure 5. The median equivalent diameter, that diameter for which 50
percent of the particles measured are less than the stated size, was deter-
mined graphically as shown in Figure 5 . The median equivalent diameter was
1.75 um.
Particle Density
The particle densities, p, were calculated from the following equation
, (Larsen and Herman 1934) :
~^~ = P (2)
When the compound contains several cations, p becomes
pl Cl + P2 C2 + P3 C3
12
-------
O3
N
05
Percent less than stated size
30 40 50 60 70 80
Figure 5. Size distribution of the fissionable particles.
The elemental analysis determined by the electron microprobe (EMP) was
used as each C value. The p values were obtained from handbook tables cited
in Larsen and Herman (1934). Generally, the refractive index used was 1.52,
however, spme indices were determined optically. No refractive index greater
than 1.66 was determined optically.
The density of the particle was difficult to calculate in those instances
where the particle contained more than one optical portion. In those cases,
and particularly where oxides of iron, uranium, or plutonium were observed, the
density was estimated. Densities ranged from 1.0 to greater than 7.2 grams per
cubic centimeter (g/cm3). The density of all particles analyzed is given in
Appendix D-2.
13
-------
Electron Microprobe Analyses
The particles were analyzed using an Applied Research Laboratory's
electron microprobe (EMP). Generally, the major consituents of the nonfis-
sionable particles analyzed were iron, aluminum, oxygen, and silicon. The
fissionable particles usually contained U, Pu, and 0. The results are pre-
sented in Appendix D-3. Some of the particles were photomicrographed on the
scanning (SEM) or transmission electron microscope (TEM) .
Mass Spectrometric Analysis
The isotopic values of plutonium were determined by first using a low
filament temperature for ionization. The uranium isotopic values were then
determined using a higher filament temperature. Uranium-234 concentrations
were generally less than 0.007 percent, uranium-236 was not detectable in
most cases; any difference was assumed to be uranium-238. For the plutonium
isotopes present, plutonium-240 was approximately 11 percent, plutonium-241
approximately 1.5 percent, plutonium-242 approximately 0.2 percent, and plu-
tonium- 239 approximately 86 percent. A complete listing of the plutonium
and uranium isotopic values is presented in Appendices D-4 and D-5, respec-
tively. Appendix G contains various photomicrographs of selected particles.
NONFISSIONABLE PARTICLES
Optical Microscopy
Representative particulates selected from sample 43 were examined using
a polarizing microscope. Over 95 percent of the particulates consisted of
resinous vegetation material, carbon and unburned coal, and coal flyash in-
cluding black, brown, and clear flyash spheres. Trace materials (less than
1 percent) including oil soot, paint particulates, metal fragments, pollens,
fungal spores, corn starch, insect parts, salt (NaCl), feldspars, calcite,
nylon, rutile (TiO_) and asbestos were noted.
Electron Microprobe (EMP)
A small portion of the particulates was also examined using the EMP. A
large portion (greater than 25 percent) of the material consisted of carbon-
aceous or organic material. A significant number (10-20 percent) of oxidized
stainless steel particles was found in poorly defined form, possibly a hydrated
corrosion product. Other particles identified included SiO , feldspars,
aluminum silicates (some as flyash), gypsum, TiO , dolomiteXand FeSO .
14
-------
GROSS PLUTONIUM EMISSIONS
An estimation of the total plutonium entering the environment was made
using fission track, gross alpha and mass spectrometry data.
Gross Plutonium Emissions- Estimated from Fission Track Data
An estimation of total plutonium entering the environment from fission
track data from individual particles was obtained using the following in-
formation:
a. The plutonium-oxide. to uranium-oxide ratios of fissionable
particles as analyzed by EMJ? varied from 0 to 0.96.
b. Isotopically, the uranium was usually natural (0-72 percent
uranium-235).
c. Greater than 99 percent of the fission tracks observed were
calculated to originate from the plutonium portion of any mixed oxide particle
observed in this study (Hayden 1974, Nathans et al. 1974).
The fission track data from one-half of sample 43 and the above data
yield an estimate of the plutonium activity obtained as shown in Table 2.
Since the total dpm calculated in Table 2 was for half the sample, it
is estimated that the total filter had 2 x 29.25 *= 58.5 dpm of plutonium. The
resultant estimation of plutonium activity for the total sample is 88.9 dpm
when the calculations are made using the maximum number of tracks in each group
(i.e., 16 tracks in the 3-16 track group).
TABLE 2. CALCULATION OF PLUTONIUM ACTIVITY FROM FISSION
TRACK DATA FROM HALF OF SAMPLE 43
Fission Track
Star Range
(FT)
3 -
17 -
33 -
65 -
129 -
256 -
TOTAL
16
32
64
128
256
1000
>1000*
Median
Value
(FT)
10
25
49
97
196
628
4500*
Number
of Stars
Observed
991
1397
1240
527
196
77
11
4439 stars
Total
Fission
Tracks
9910
34925
60760
51119
37828
48356
49500
Pg
of
289J?u
5.
20.
35.
30.
22.
28.
29.
83
54
74
07
25
44
12
dpm dpm/
of particle
239Pu (x 10~3)
1.
3.
6.
5.
3.
4.
4.
29.
00
50
07
11
79
83
95
25
1.
2.
4.
9.
190.
620.
4500.
dpm
0
5
9
7
0
0
0
*Assuming maximum star as 10,000 tracks
15
-------
Total emission calculations were made as follows:
Stack diameter = 0.46 m
Area = 0.17 m2
Exit velocity = 401 m/min
Stack emission rate, Q = 0.17 m2 x 401 m/min = 68.1,;m3/min
Stack sampler rate = 19.82 liter/min = 0.0198 m3/mln
Therefore, total emission rate = 68.1/0.0198 = 3439 times
the sampler rate.
Assuming sample 43 contains 58.5 dpm plutonium Cfrom above) and that the
sample was taken isokinetically, then the total plutonium particulate alpha
activity emitted from the stack during the sampling period was 58.5 x 3439 =
201,200 dpm or 2.0 x 1Q5 dpm/2.22 x 103 dpm/nCi = 90.1 nCi. Since the sampling
period was 86 days, this represents 1.05 nCi of plutonium emitted per day using
the median value from Table 2 or 1.60 nCi using the maximum value.
Gross Plutonium Emissions Estimated from Gross Alpha Count
The data from gross alpha counting by Babcock and Wilcox were also used
to calculate the gross plutonium-239 emitted from the stack. The calculation
was as follows:
The gross alpha count on sample 43 was 19-0 dpm. Therefore, 190 xt 3439 =
6.5 x 105 or 293 nCi emitted in 86 days or 3.41 nCi/day.
Gross Plutonium Emissions Estimated from Mass Speetrometry Data
The total nanograms (ng) of plutonium on the sample, as determined by mass
spectrometry analysis of one-quarter of the sample, was 1.78 nanograms. Ad-
justing for the contribution of plutonium-240, there was 170 dpm/ng of total
plutonium. Therefore, the plutonium disintegration rate of this filter was
170 x 1.78 = 303 dpm = 136 pCi or 1.58 pCi/day. The total effluent was 3439
x 1.58 = 5.43 nCi/day or 9.2 nCi/workday. Of the three techniques used to
calculate plutonium emissions, the latter would be expected to provide the
most accurate information. The number of plutonium particles in the Plant
emissions per day can be calculated as follows: From Table 2, 4500 particles
per half sample or 9,000 particles were found in the 86-day sample. Since the
volume ratio (stack/sample) was 3439, the stack, particles emission rate is
then C9000/86) x 3439 = 3.6 x 105 particles per sample day or 6.07 x 10s par-
.ticles per workday (7 particles/s). As calculated above, 136 pCi in 9,000
particles was emitted, implying an average activity of 15.1 fCi/particle.
Given the plutonium-239 emission rate of 5.43 nCi of gross plutonium per
sampling day and 3.6 x 10s particles per sampling day, we can summarize the
emitted plutonium-239 in the following manner: (following page)
16
-------
TABLE 3. PLUTONIUM-239 MISSION SUMMARY
Total (nCi)
Particulate
Per
Work
Day
9.20
6.07 x 10s
Per
Sampling
Day
5.43
3.6 x 10s
Per
kg of Fuel
Fabricated
4.51
2.99 x 10s
Per
Fuel
Pin
0.15
1.02 x 10"
The aerodynamic size of the emitted particles can be calculated as
follows:
Particles larger than about a micrometer in diameter settle in air
at velocities approximated by Stokes1 Law (U.S. DHEW, 1969)
V = a x d2(P - P )/18n (4)
JL £•
The expression is true only for spheres. An upper limit to its ap-
plicability is set when a certain settling velocity is reached and the particle
generates a significant wake. The lower limit is reached when the particles
become small, around 1 ym, so air resistance is no longer continuous but is
rather the result of individual collisions with air molecules. Under these
conditions the particles "slip" between molecules and Stokes' equation under-
estimates their falling velocity.
In the case of nonspherical particles, substitution of V, a, P., P?, and
n in the above equation leads to a fictitious diameter, d , which is known as
the 'aerodynamic* diameter.
If the density, P_, is unknown, it may arbitrarily be assigned a value
of 1 g/cm3. In this case d is no longer Stokes' diameter but rather the
"reduced sedimentation diameter." An example is: 1-um sphere of lead or
PuO? - UO- (50:50) with a density of 11 g/cm3 has a reduced sedimentation
diameter of =3.3 urn. The settling velocity is now increased from 2 x 10 2 cm/s
to 2 x 10"1 cm/s. Conversely, a large (greater than 6 urn) host particle with a.
density of 2 to 3 g/cm3 with a 1-um Pud -UO inclusion has its "reduced sedi-
mentation diameter" altered by 5 percent; therefore, there is no noticeable
change in the settling velocity.
*
A calculation was made to determine the equivalent particle size of the
PuO -UO particles found in sample 43. This equivalent particle size is based
upon the fission track distribution and is presented in Table 4; the data from
Table 4 are plotted in Figure 6. The median equivalent diameter (Figure 6)
is near 0.2 urn. This is significant in that half of the equivalent diameter
particles of PuO -UO may be a pulmonary hazard if these particles exist in a
free, unattachedxstate.
17
-------
TABLE 4. EQUIVALENT SIZE OF PuO -UO PARTICLES FROM SAMPLE 43
Fission
Star Range
(Tracks)
3 -
17 -
33 -
65 -
129 -
256 -
TOTALS
16
32
64
128
255
1000
>1000
Tracks
(Avg.)
10
25
25
97
193
628
4500*
Equivalent
Particle
Size (urn)
0.14
0.19
0.24
0.29
0.37
0.54
1.05
Number
of
Particles
991
1397
1240
527
196
77
11
4439
Percent
of
Total
22.3
31.5
27.9
11.9
4.4
1.7
0.2
99.9
Cumulative
Percent
22.3
53.8
81.7
93.6
98.0
99.7
99.9
*Assuming maximum star as 10,000 tracks
Percent less then stated size
20 30 40 SO 60 70
Figure 6. Equivalent size of PuO —UO particles from sample 43 based' upon
_j_ - • m -' 3t 2£ •.'•'*
tracks.
18
-------
RESULTS OF ENVIRONMENTAL AIR ANALYSIS
PARTICLE CHARACTERIZATION
Examination of a large number of particles from environmental air
samples has shown the presence of various isotopes of uranium; however, no
plutonium particles were found. The uranium isotopes and their percentages
are listed in Appendix F.
GROSS ACTINIDE ANALYSIS
Appendix E-l contains results of gross analysis by mass spectrometric
techniques for six environmental air samples. The total grams of uranium per
filter is one the order of 10 7 and is predominately uranium-235 and uranium-
238. The total grams of plutonium per filter ranges from less than 10 12 to
2 x 10 12 with isotopic compositions of plutonium-239 in the 50 to 80 isotope-
percent range and plutonium-240 in the 0 to 27 isotope-percent range. Plu-
tonium-241 was present in one sample at 23 isotope-percent. The specific
activity of plutonium-239 is 6.13 x 10 2 Ci/g. The average activity collected,
assuming 1 x 10 12g of plutonium at an 80 percent concentration for the 239
isotope, is (6.13 x 10~2Ci/g) x CO.80) = C4.9 x 10"1" Ci) = 49 fCi. Sampling
times ran from 137 to 676 hours. The average sample collection time was 500
hours at a rate of 1.8 m3/h.
Therefore, for an average sampled air volume of 500 x 1.8 = 900 m3, the
average ground-level concentration of plutonium was:
4.9 x IQ'1* curies/900 m3 * 5.4 x 10~17 Ci/m3 = 54 aCi/m3
Appendix E-2 contains gross levels of various uranium and plutonium
isotopes as a function of size fraction.
REQUIREMENTS FOR MONITORING
The establishment of an environmental sampling methodology is dependent
upon knowledge of the pollutant concentration in the surrounding area. A
major source of pollutant entry into the environment from the Plant is assumed
to be the exhaust stack utilized for the production of finished fuel rods.
Estimations of the stack plume concentration at ground level are dependent
upon a number of factors.
i
These factors can be classed under three general headings, and are:
1. Process factors
Emission rate
Temperature of emission products
Form of emission products, i.e., dust, fumes, mist, spray, etc.
19
-------
- Concentration of emission products
- Particle size distribution and terminal velocity
- Agglomerating characteristics
- Chemical properties
Source factors
- Stack height
- Stack diameter and exit configuration
- Stack velocity
- Relationship of stack to surroundings
Meteorological factors
- Wind speed and direction
- Temperature and humidity
- Atmospheric stability
- Topographic effects
The basic formula for plume dispersions assumes a Gaussian diffusion
model (Turner 1970). This model is described by
Equation (5) has found widespread acceptance even though more exotic
models have been developed. The critical factors of this model are the stand-
ard deviations of plume concentration, a and a . These factors are dependent
upon atmospheric turbulence and most commonly based on the Pasquill typing
scheme (Pasquill 1961) and are classed from "very unstable" to "very stable".
The general acceptance of this typing scheme has caused considerable effort to
be expended in the development of usable formulation of the deviation param-
aters (Smith 1951; Turner 1964; Briggs 1969). The values recently developed
by Briggs (1974) as quoted by Gifford (1976) are used for calculations of
emissions from the Babeoek and Wilcox stack. These parameters are shown in
Table 5.
TABLE 5. ATMOSPHERIC TURBULENCE PARAMETERS
Pasquill
Type
A '
B
C
D
E
F
0
y
(m)
0.22x(l + O.OOOlx)"^
0.16x(l + O.OOOlx) jj
O.llx(l + O.OOOlx) 2
0.08x(l + O.OOOlx) i
0.06x(l + O.OOOlx) ^
0.04x(l + O.OOOlx) 2
(m)
0.20x
0.12x
0.08x(l +
0.06x(l +
0.03x(l +
0.016x(l+
-k
0.0002x) I*
O.OOlSx) **
0.0003x) |
O.OOOSx)
Note: Values quoted are
for op-en country conditions \
7ith 10* < x
< 10*m.
20
-------
The key to the stability types is given in Table 6.
Surface Wind
Speed (at 10 m) ,
m/s
<2
2 to
3 to
5 to
>6
3
5
6
Day
Night
Incoming Solar Radiation Thinly Overcast
Strong
A
A, B
B
C
C
Moderate
A, B
B
B, C
C, D
D
Slight
B
C
C
D
D
°f <3/8
^4/8 Low Cloud Cloud
E
D
D
D
F
E
D
D
Note: The neutral class, D, should be assumed for overcast conditions during
day or night.
The meteorological conditions observed at the Plant location during the
months of May to August limits the consideration of stability classes to A, B
and D.
The major concern here is the prediction of maximum plume concentration
values and locations of the maximums. The involvement of the a's with x and
the multiplicity of exponential functions of x make this procedure complex for
the general case. The diffusion equation is reduced in complexity by restrict-
ing calculations to ground level (z = 0) and along the plume centerline (y = 0) .
When this is done, equation (5) reduces to
H> -
y z
The variation of a is related through the square root function of x for
all classes of stability\ Rather than perform the differentiation of equation
(5) and performing the hand calculation, it is much simpler to allow a computer
to calculate values of xOO and to plot equation (6) for the various stability
classes.
Figure 7 shows a plot of downwind ground-level concentrations for the
plume. The calculation is based on the following assumptions:
1. The stack gas exit velocity was constant at 6.68 meters
per second (m/s) .
2. The temperature of emission products was the same as
ambient temperature.
3. The particulate emission products had an effective diameter
of less than 20 v.m.
21
-------
H
&
H-
O
rt-
(D
D.
fl
&
to i
to H
3
(D
H
V
H
8
o
n>
PI
rt
&
.00
40.00
80.00 120.00 160.00 200.00
DOWNWIND DISTANCE, M (x 101)
240.00
280.00
320.00
-------
4. The stack height was 10.7 m.
5. The stack diameter was 0.46 m.
6. The wind speed averaged 1.6 m/s* over the months of May- August.
7. The wind direction was constant during the calculation period.
8. The effects of surrounding building and topography were
considered negligible.
9. No corrections made for humidity and temperature variations.
10. The particle emission rate was 7 particles /s.
11. The effective stack height was 15.6 m.
12. The turbulence values were those shown in Table 5.
13. The plume was nonhuoyant with neither washout nor dilution.
The effective stack height, H , used for the calculation is as
follows (Briggs 1969): e
C7)
Table 7 is a tabulation of stability class and the resulting values
of maximum concentrations and distance? as calculated from equation C6) .
TABLE 7. GROUND-LEVEL PLUME CONCENTRATIONS FROM DISPERSION MODEL
Stability
Class
A
B
C
D
E
F
max \iax
Cm) Cparticles/m3 * 10~3)
60
90
140
200
400
825
6.1
5.1
4.9
4.5
3.1
2.2
\iax
(pCi/m3 x 10~s)
9.2
7.7
7.4
6.8
4.7
3.3
Note: a (x) and a (x) values for x<100 m are linear extrapolations of
tXe values quoted in Table 5.
Air Volume Requirements
*
The total volume of air to be sampled in order to measure a minimum de-
tectable activityt of 0.1 pCi for plutonium-239-, using an approximate value
for the smallest Y , is:
uiax
*The quality of the measurements is suspect due to location of meteorological
instrumentation with respect to the stack location and surrounding buildings.
tGenerally accepted for total dissolution isotopic analysis by alpha spectrometer.
23
-------
Volume =0.1 pCi/4.0 x 10~3 pCi/m3 = 2500 m3
An additional factor of wind variation raises this minimum value. Due
to variation in wind directions at the Plant, the samples were downwind of
the stack approximately 37 percent of the time. Therefore, (the minimum vol-
ume of the sampled air calculated by the preceding equation would have to be
multiplied by 1/0.37 to account for wind variation. This gives a minimum
quantity of 6, 760 m3 of air which must be sampled to measure minimum detectable
activity. If we make the assumption that the plume width is typically 22.5
degrees (Briggs 1974), and also, that the wind pattern is uniformly distributed
around the other 15 compass points during the remaining 63 percent of the time,
we can see that for sampling points at other locations it would be necessary to
collect approximately 59,500 m3 of air to reach the minimum detectable levels
for plutonium.
It should be noted that the simplifying assumptions used in the basic
concentration calculation are applicable only for an ideal source and tend to
maximize the concentrations. Real conditions as they pertain to fabrication
processes and individual sources, as well as environmental and meteorological
factors (washout, dilution, terrain, building, etc.), would tend to further
reduce ground-level concentrations. For instance, Figures 8a and 8b are plots
of the basic diffusion equation of Figure 7 with variations in the parameters
of windspeed and crosswind distance, respectively; the variation parameter in
these figures increases in value in the positive direction of the third axis.
From these figures, it can be seen that any or all of these factors can reduce
the ground-level concentration at downwind distances.
CONCENTWTJON
WINOSPEED
CONCENTRHTIOM
CROSSVIND DISTANCE
Figure 8a. Plume concentration versus Figure 8b. Plume concentration versus
variable windspeed, relative values. variable crosswind distance, relative
values.
24
-------
Pasquill (1974) and Weber (1976) report an error analysis of the
diffusion equation. The results of errors introduced by uncertainties in
H, a and a (Briggs1 error analysis on Table 5 values is not available)
have led them to predict a net root-mean-square error of 49 percent.
A variety of air samplers using some form of filter material as a
collections medium are available. Such samplers typically operate in the
0.14 to 2.24 m3/min (5 to 80 ft3/min) range. With this type of sampler,
minimum sampling times vary from 2 to 31 days for an 'in-plume1 sample of
the required 6,760 m3 of air. A realistic sampling period of 24 hours
would require a sampler rate of 280 m3/h.
25
-------
REFERENCES
Becker, K. 1969. "Alpha Particle Registration in Plastics and its Application
for Radon and Neutron Personnel Dosimeters." Health Physios, pp. 16 & 113;
Pergammon Press.
Briggs, G. A. 1969. "Plume Rise." U. S. Atomic Energy Commission Office
of Information Services, TID 25075.
Briggs, G. A. 1974. "Diffusion Estimation for Small Environs." Environmental
Research Laboratories, Air Resources Atmospheric Turbulence and Diffusion
Laboratory 1973 Annual Report, U.S. Atomic Energy Commission Report No.
ATDL-106, NOAA.
Fleischer, R. L., P. B. Price, R. M. Walker. 1963. "Nuclear Tracks in Solids,"
Applied Physios Letters, 3, No. 2, pp. 28.
Gifford, F. A. 1976. "Turbulence Typing Scheme: A Review." Niidlear Safety,
Vol. 1, pp. 68-86.
Hayden, J. A. 1974. "Characterization of Environmental Plutonium by Nuclear
Track Techniques". Conference of Atmospheric-Surface Exchange of par-
ticulate and Gaseous Pollutants, Richland, Wash.
Johnson, C. J., G. Lucas, J. Connor, R. Tidhall and A. Hazle. 1975. "Evalua-
tion of Contamination of the Soil by Windblown Dust Containing Plutonium
and Its Degradation Products." Memo to Jefferson County Commissioners of
the Colorado State Department of Health, May 1, 1975.
Larsen, E. S. and H. Berman. 1934. "The Microscopic Determination of the
Nonopaque Minerals," second ed., Geological Survey Bull. No. 848, U.S.
Government Print Office, Washington, D.C. pp. 30-32.
McCrone, W. C. 1973. "Particle Atlas," second edition, Ann Arbor Scientific
Publications Inc.; Ann Arbor, Michigan.
Nathans, M. W., R. Rhinehart, W. Holland. 1974. "Methods of Analysis Useful
in the Study of Alpha-Emitting and Fissionable Material-Containing Par-
ticles," Conference of Atmospheric-surface Exchange of Particulate and
Gaseous Pollutants, Richland, Washington.
Pasquill, F. 1961. "The Estimation of the Dispersion of Windborne Material."
Meteorological Magazine, 90:33-49.
26
-------
Pasquill, F. 1974. "Atmospheric Diffusion," second ed., J. Wiley and Sons,
New York.
Smith, M. E. 1951. "The Forecasting of Micrometeorological Variables."
Meteorological Monographs, ^: 50-55.
Turner, D. B. 1964. "A Diffusion Model for an Urban Area." Journal of
Applied Meteorology, _3CD:83-91.
Turner, D. B. 1970. "Workbook of Atmospheric Dispersion Estimates."
U.S. Department of Health, Education, and Welfare, PB191482.
U.S. Department of Health, Education, and Welfare CDHEW). 1969. "Air
Quality Criteria for Particulate Matter." Washington, D.C. January
1969. pp. 5-7.
Weber, A. H. 1976. "Atmospheric Dispersion Parameters in Gaussian Plume
Modeling, Part I." U.S. Environmental Protection Agency Report
No. EPA-600/4-76-030a.
27
-------
APPENDIX A. ENVIRONMENTAL SAMPLER DATA.
Sample No.
41
42
45
46
47
48
49
50
51
52
53
54
55
56
57
58
59
60
61
62
Sampling Dates
(Start & Stop)
05/14/75
05/14/75
05/15/75
05/15/75
05/20/75
05/23/75
05/29/75
06/02/75
06/02/75
06/09/75
05/30/75
06/26/75
06/26/75
06/26/75
06/26/75
07/18/75
07/18/75
07/18/75
07/18/75
10/22/75
- 06/02/75
- 05/23/75
- 05/20/75
- 05/15/75
- 06/20/75
- 05/30/75
- 06/26/75
- 06/26/75
- 06/26/75
- 06/26/75
- 06/09/75
- 07/18/75
- 07/18/75
- 07/18/75
- 07/18/75
- 08/04/75
- 08/04/75
- 08/04/75
- 08/04/75
- 10/29/75
Run Time Bab cock & Wilcox
(hrs.) Locations (See Fig. 4)
457
216
109
3
320
137
676
674
675
478
191
529
529
529
532
410
410
409
404
165
7
8
V
5
V
5
8
7
5
5
5
V
7
8
5
Metals
7
8
5
BCL
28
-------
APPENDIX B. USGS TOPOGRAPHIC MAP OF LEECHBURG, PA. AREA.
\ \ -V • •• • '"
i \ M'. • ;. •' Gforgetown "
\ 'A |l» . ' /•
•/T \Park
N
V-AI-LEiiHENY
.Gas Wen
1009
use*
Dump
Well
A,tpo<1
Babcock and Wilcox Plant
y
'Ht
Scale: 1" = 0. 62 km
29
-------
APPENDIX C. RESULTS OF PLUTONIUM-238 AND -239 ANALYSES OF SOIL SAMPLES.
Sample
Number
NUMEC #1-1
NUMEC #1-2
NUMEC #2-1
NUMEC #2-2
NUMEC #4-1
NUMEC #4-2
NUMEC #5-1
NUMEC #5-2
NUMEC #6-1
NUMEC #6-2
NUMEC #7-1
NUMEC #7-2
NUMEC #8-1
NUMEC #8-2
NUMEC #9-1
NUMEC #9-2
Total Dry
Weight (g)
9.91
10.001
9.996
9.973
9.981
10.001
3.966
3.949
4.983
4.975
4.998
4.917
4.996
4.991
5.411
4.600
pCi/g
238^
Pu
0.02 ± 0.017
0.009 ± 0.004
0.016 ± 0.007
0.003
0.014
0.024 ± 0.006
0.043 ± 0.023
0.005
0.026 ± 0.008
0.012 ± 0.008
0.018 ± 0.008
2.12 ± 0.20
0.120 ± 0.024
2.28 ± 0.180
0.007
0.276 ± 0.041
239,,
Pu
0.157 ± 0.020
0.29 ± 0.035
0.064 ± 0.015
0.025 ± 0.001
0.229 ± 0.075
0.518 ± 0.050
0.156 ± 0.048
0.180 ± 0.033
0.006
0.002
0.006
0.008 ± 0.006
0.008 ± 0.006
0.12
0.004
0.020 ± 0.009
30
-------
APPENDIX D. RESULTS OF INDIVIDUAL PARTICLE ANALYSIS; STACK SAMPLE.
CONTENTS
Page
D-l Terminology Definitions and Cross Reference 31
D-2 Optical Measurements of Particles; Stack Sample
D-3 Particle Constitution by BMP; Stack Sample
D-4 Mass Spectrometry Results for Plutonium
D-5 Mass Spectrometry Results for Uranium
31
-------
APPENDIX D-l. TERMINOLOGY DEFINITIONS AND CROSS REFERENCE
Heading Description
Identification (I.D.) The 3-digit number associated with the
sample number is the particle number. When
two particles are shown, this means that
the two separate particles indicated were
attached to each, other.
Color Transmitted color observed with an opti-
cal microscope.
MCC Particle Classification Code
1 Needles or rods
2 Flat
4 High Index (n>1.52)
8 Birefringent
16 Colored
32 Opaque
A single particle is optically character-
ized using the above 6-digit code. The
binary numbers above the blocks are used
additive to describe a particle.
Example: Code = 28. The particle is
colored and birefringent and has a high
refractive index; 16+8+4 = 28.
A code of 100 means no morphology measure-
ments were made.
Tracks This is the number of fission tracks re-
corded in Lexan with a 9 x 1014 neutron x
volume x time thermal neutron fluence.
One picogram of 239Pu produces approximat-
ely 1700 tracks. Where 1001 tracks are
indicated this means greater than 1000
tracks.
32
-------
APPENDIX D-l. TERMINOLOGY DEFINITIONS AND CROSS REFERENCE (continued;
Size
Optical measurements in micrometers.
Weight
Comments
Isotopic Distribution
of Uranium
Isotopic Distribution
of Plutonium
Elemental Concentrations
,1/3
Size = (length x width x thickness)'
where thickness is arbitrarily assigned
a value of one-half the width when it
cannot be determined.
Values shown are in equivalent femtograms
of plutonium as calculated from the number
of fission tracks observed. One should
recognize that in most cases, no pluton-
ium was observed.
This represents the best possible identi-
fication of the particle based on an eval-
uation of all of the measurements made on
that particle.
Density of particle from refraction esti-
mates.
The values and their corresponding stand-
ard deviations shown are in isotope-percent
for the nuclide indicated. No 233U was ob-
served in any of the particles. Missing
information indicates that the number of
counts collected was too low to make an
isotopic measurement.
Same as for uranium except the isotopes
indicated are plutonium. A search was
made for plutonium in all of the particles
analyzed by mass spectrometry; only those
which had positive indications of pluton-
ium are listed in these tables. Pluton-
ium-238 was not measured because of the
238U interference.
The weight percent of the elements indi-
cated as measured by the electron micro-
probe. The elements are all assumed to
be oxides, i.e., the oxygen values are
calculated—not measured. Those elements
without a weight % indicated are all <1%
concentration.
33
-------
TABLE D-l. CROSS REFERENCE BETWEEN SAMPLE NUMBER AND SAMPLE LOCATION.
EPA No.
41
42
45
46
47
48
49
49 Top*
50
51
52
53
54
55
56
57
43
44
58
59
60
61
BCL 62-1 3.5-15 urn
BCL 62-2 1.7-3.5 ym
BCL 62-3 <1.7 ym
Location
Restaurant
Drum Storage
Veados Home
Gum Corner
Veados Home
Gum Corner
Drum Storage
Drum Storage
Restaurant
Veados Home
Gum Corner
Gum Corner
Veados Home
Restaurant
Drum Storage
Gum Corner
Stack Downstream
Stack Upstream
Metals Building
Restaurant
Drum Storage
Gum Corner
Drum Storage
Drum Storage
Drum Storage
7
8
V
5
V
5
8
8
7
V
5
5
V
7
8
5
6
7
8
5
8
8
8
*Sample split into two parts.
34
-------
APPENDIX D-2. OPTICAL MEASUREMENTS OF PARTICLES: STACK SAMPLE.
IDENTIFICATION
EPA
SPA
EPA
ePA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
KPA
EPA
£PA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
cPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
4J
4.)
43
43
43
43
43
43
43
43
43
43
4j
43
43
43
43
4}
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
201
202
203
204
205
206-
501
552
503
504
505
506
507
508
509
510
511
5I2A5I3
5I3B5I2
5I4A5I5
5151)514
5I6A5I7
5171)516
518
5|y
520A52I
521H520
522
523A524
524HS23
525
526
527
528
529A530
530B529
53IA5.12
532B53I
513
534A53V
535 AS 36
536B535
537A538
538B537
53VB534
540A54I
54IB540
542A543
S43B542
544
545A546
5461)545
547
548A54V
S49B548
550A551
55 IB 550
55 2 A 553
553U"i52
554
555
556
557A55R
558B557
559A560
56OH55V
56 1 A590
562
563A564
564B563
565
566
567A568
568B567
569A570
570B569
57 1 A57Z
572B57I
573A574
574d573
iJOLOH
DIIOWN
I) H(MN
YELUM
YELLOW
YELLOW
IIHOHN
YELLOW
YEULOH
YKLLOrf
YELLOW
BROWN
BROWN
YELLO.I
BROWN
ORANGE
ORANGE
ORANGE
ORANGE
YELLOW
Yh'LLOl*
YELLOW
YELLOW
OPAQUE
OPAQUE
OPAQUE
ORANGE
HKOMN
OKKRN
YELLOW
OPAOUH
OPAOUE
OPAOUE
OPAOUE
OPAOUE
OPAOUE
OPAOUE
YELLOW
NO COLOR
HHOrffl
YELLOW
OHANGE
NO COLOR
ORANGE
YriLLOW
OWAVOE
ORANGE
ORANGE
ORAMGE
ORANGE
ORAMGE
OHANl/E
YELLOW
ORANGE
ORANGE
ORANGE
YELLOW
YELLOW
YELLOW
ORANGE
YELLOW
YELLOW
YELLOW
ORANGE
ORANGE
ORANGE
YELLOW
YELLOW
OPAOUE
YELLOW
YELLOW
ORANGE
YELLOW
ORANGE
ORANGE
ORANGE
YELLOW
MCC
48
4R
48
21
28
IOO
28
IOO
IOO
3?
32
32
32
32
32
32
ion
0
20
I6
16
n
16
IOO
16
16
100
16
16
IOO
IOO
16
IOO
100
16
IOO
16
100
?0
16
24
IOO
16
IOO
IOO
16
IOO
16
IOO
IOO
16
IOO
20
16
100
16
IOO
16
IOO
16
16
16
16
IOO
16
IOO
32
16
16
IOO
16
16
16
IOO
16
IOO
16
IOO
16
IOO
TRACKS
0.
0.
0.
0.
O.
600.
175.
50.
40.
200.
175.
200.
375.
275.
200.
200.
1001.
0.
IOOI.
0.
450.
0.
1/5.
150.
175.
O.
30O.
300.
0.
500.
HO.
800.
400.
300.
0.
2-10.
0.
200.
350.
0.
O.
150.
0.
ISO.
150.
0.
23.
0.
150.
23.
0.
45.
32.
0.
14.
0.
50.
0.
55.
250.
16.
32.
0.
19.
0.
25.
0.
27.
0.
40.
16.
16.
0.
40.
0.
13.
0.
4O.
0.
30.
SUE
14.9
II. 0
21.1
A. 6
8.5
0.
2.6
0.
0.
.0
.0
.0
.0
.0
.0
.0
.6
11.4
1.0
15.2
2.2
13.5
2.4
0.
5.0
15. b
0.
3.2
6.2
0.
0.
1.8
0.
1.0
13.0
0.
7.5
0.
1.5
13.5
12. H
0.
3.8
0.
0.
10.5
0.
ll.fi
0.
0.
4.8
0.
5.4
6.6
0.
4.2
0.
14.9
0.
5.0
17.0
7.0
11.5
0.
30.4
0.
7.2
7.5
16.5
0.
16.5
11.5
18.0
0.
10.0
0.
4.3
0.
0.6
0.
WEIGHT comENrs
0
0
0
0
0
35?
102
2V
23
117
102
117
?20
161
117
117
> 5R8
0
> 5>W
0
264
O
102
88
102
0
176
176
0
294
47
470
2Jb
176
0
164
0
117
205
0
0
H8
0
SH
SB
U
13
0
SB
13
0
26
IU
0
H
0
2V
0
32
147
4
18
0
II
0
14
O
15
0
23
9
9
0
23
O
7
O
23
0
17
WOX
7N '(ETAL
7.N METAL
KK7O3 LOSr
PU PRESENT
Pi; PHEScNI
UOX + PUOX
UOX * PJOX
SI OX
UOX » PUOX
UOX » PUOX
LOST ON TeM
LOST ON TRM
LObT ON TKM
SI OX
UOX * PUOX
UOX » PUOX
PU PRESENT
PU PRtSENT
HFOX
UOX » PUOX
UOX » i-JOX
5 ALPHA 1HACKS
STAINLESS STEEL -OX
LOST
UOX * PUOX
ALSIOX
UOX » PUOX
UOX » PUOX
UOX + PUOX
siox
UOX » PUOX
PU PRbSENF
TUNGSTEN
PU PRESENf
SIOX
UOX * PUOX
STAINLESS STEEL-OX
SIOX
LOST
PU PRESENT
LOST
PU -PRcStNT
ORGANIC
SI OX
PU PRESENf
PU PHcStNT
TUNGSTEN
PU PRESENT
35
-------
APPENDIX D-2. OPTICAL MEASUREMENTS OF PARTICLES: STACK SAMPLE. (continued)
IDENTIFICATION
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
4J
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
575
576A577
577B576
578A57V
579B578
58O
581
532
583
584
335
586
537A5E)8
538BS37
58V
5VOB56I
7fl|
732
703
704
705
706
707
708C715
739
710
711
7I2A724
713
714
7I5E70H
7I6E703
7 1 7E708
718
719
720A723
721
7?2
7238720
7 2487 12
725D7 33
726
727
728D72V
72VE728
730E728
731E72H
732E728
733E725
734E725
735
736
737
73H
739
740
741
742
743
7 1407 48
745
746
747
748E744
749
750
75IA7SH
752
753
754
755D7H6
756
757D783
758
759
760
741
76?
763
764
COLOR
ORANGE
YELLOW
YELLOW
BROrtN
BROrtN
BROrtil
ORANGE
GREEN"
RROrtN
YELLOrt
YELLOrt
YELLOrt
iJHOBN
8RIMN
•tHOtlN
BROWN
iiVOMN
BROWN
HROnN
BROrtN
UHOHN
YELLOrt
YELLOrt
YELLOW
YELLOrt
HHOWN
ORANGE
ORANGE
ORANGE
ilKOHN
ORANGE
ORANGE
BROWN
BROHN
BHOHN
HROWN
ORANGE
ORANGE
BROWN
BROWN
URUIIN
YELLOrt
YELLOW
ORANGE
OPAQUE
ORANGE
ORANGE
YELLOW
YELLOW
ORANGE
YELLOrt
YELLOrt
YELLOH
YELLOrt
YELLOW
BROWN
ORANGE
YELLOW
YELLOW
KHOrtN
BROWS
ORANGE
ORANGE
BROWN
ORANGE
YELLOW
ORA'IGE
YELLOW
HROrtN
ORANGE
ORANGE
OHANGE
ORANGE
ORANGE
ORANGE
ORANGE
bHONN
HROWN
HROWN
YELLOW
RROrtN
YELLOrt
YELLOW
YELLOW
BROrtN
HRDrtN
URUrtN
YELLOrt
BHOJ1N
KPUWN
YELLOW
ORANGE
YELLOW
ORANGE
Yf-ULO.1
BROrtN
YELLOW
ORANGE
YELLOrt
ORANGE
ORANGE
»CC
IOO
16
ino
16
IOO
ino
ino
IOO
inn
32
IOO
100
16
IOO
ir»
100
100
IOO
ion
IOO
28
28
28
28
?H
2*
2fl
78
78
28
28
78
20
20
20
28
20
20
28
20
24
20
78
ino
ino
IOO
ino
too
ino
28
28
28
24
28
78
IOO
2S
28
28
IOO
28
2*
28
IOO
28
28
28
28
28
inn
28
28
IOO
78
28
28
IOO
IOO
TRACKS
ISO.
0.
7O.
0.
80.
16.
60.
80.
70.
IOO.
14.
70.
O.
I2O.
32.
50.
inni.
350.
5TO.
tool.
150.
V5.
275.
4OO.
200.
H5.
S5.
0.
300.
1001.
4 no.
4 no.
4TO.
ISO.
HO.
inni.
375.
400.
1001.
200.
130.
275.
175.
350.
0.
0.
0.
0.
0.
0.
47.
47.
85.
VA.
27.
17.
6.
120.
13.
0.
| ,
13.
14.
9.
14.
240.
n.
HO.
725.
2V.
14.
I2O.
60.
72.
6O.
51.
120.
160.
15.
30.
SI-IE
6.0
14.5
0.
5.3
0.
0.
0.
0.
0.
0.
0.
3.5
0.
0.
0.
0.
0.
0.
0.
8.6
3.7
3.5
4.0
10. 0
3.5
3.5
2.7
3.5
1.5
2.0
3.5
0.
12.0
6.5
7.5
14. O
H.O
0.
O.
3.7
R.n
2.3
4.0
0.
0.
0.
0.
O.
0.
14.0
9.5
8.0
6.5
13.5
7.0
5.3
3.7
19.0
4.0
5.0
5.5
3.7
1.7
0.
10. 5
2.5
7.5
4.8
5.5
8.0
0.
4.7
7.5
0.
5.0
5.3
1.7
0.
O.
HEIGHT COMMENTS
»8
0 STAINLESS STEEL-OX
41 PU PRESENT
0
47 PU PRESENT
y PU PRESENT
35
47
41 PU PRESENT
58
8
41
0 STAINLESS STEEL-OX
70 PU PRESENT
IH PU PRESENT
2v UOX * PUOX
> 588 PU PRESENT
203 PU PRESENT
294 PU PRESENT
> 5< 5HH LOST
235 FEOX
235 SIOX
235 UOX
*8 PU PRESENT
105 ORGANIC
> 5R8 STAINLESS STEEL
220 PU PRESENT
235 PU PRESENT
> 58« PUOX * UOX
117 PUOX * UOX
16
161
102
205
0
0
0
0
0
O
27
24 PU PRESENT
5O PU PRESENT
56 SIOX
15 PU PRESENT
10 ORGANIC
3
70 PU PRESENT
7
3 LOST
0
7
8 ORGANIC
5 STAINLESS STEEL -OX
8 PU PRESENT
141 PU PRESENT
0 FEOX
47 PU PRESENT
132 PU PRESENT
17 FE.ALSIOX
8 ORGANIC
70 PU PRcSENT
35 ORGANIC
42 PU PRESENT
35 PU PRESENT
30 Pl> PRESENT
70 LOST
94 LOST
8 PU PRESENT
17 PU PRESENT
36
-------
APPENDIX D-2. OPTICAL MEASUREMENTS OF PARTICLES: STACK SAMPLE. (concluded)
OPTICAL WEHSU'JbMEMTJ
IDENHNKATION
bPA
cPA
EPA
r-PA
EPA
KPA
tPA
tPA
EPA
EPA
KPA
cPA
EPA
CPA
bPA
bPA
EPA
EPA
fc/A
EPA
EPA
ifPA
tPA
EPA
EPA
43
43
43
4}
43
43
43
43
43
43
43
43
43
4J
43
43
43
43
43
43
43
43
4]
43
43
Tib
7(S6
Ifil
7-SR
7rtv
770
771
772
773
774
775
77A
777A7-I,'
77H
77v
7 HO
7H1
712
713E757
7M4E7*> ?
7S5E757
y.-kst-yw
M7
718H7-5I
7HVH77V
cnuw nee rnACXs
iiHiinn
iiR()Ji'4
HRCIHI
OII/MJGK
YHU-Ot
UHANU?
OHANJE
UhANGK
ilttOhN
(Jf?AMGF
ORANuR
OlMNOc
YEU.IW
YEIJ.OH
YHLl.nn
YKI.UM
OMA'JG1*
YELLOW
Yuf-I.O'^
(HA'JUk
YELL0.1
UROIIN
YEU.ON
(IRA«IGc
YELLOW
YELLIH
HWO.«I
IIKDUN
24
IOO
IOO
?4
100
24
100
2H
2B
100
24
2R
21
10"
?•*
7H
100
?H
7S
IOO
100
2H
24
IOO
IOO
1 10.
70.
45.
I/.
22.
•S2.
2V.
40.
44.
12.
10.
2^ .
o.
31 .
1 ^ .
32.
13.
13.
0.
0.
0.
14.
120.
VS.
Mb.
SIZh rfEIOHT OOMMENfS
7.0
0.
0.
A.O
O.
5.2
0.
7.5
h.T
0.
A.O
V..T
3.7
0.
v.b
4.5
0.
9.0
4.5
0.
0.
0.
7.2
0.
0.
64 PU PHI: SENT
41
?6 PU PHcitNf
10 (WJANIC
12
3A PU PRESENT
I /
23 PU
2'J
bfFEL-OX
HU
PU PHESSNT
5
17
0 hi-OX
11 PU PRcSEl.T
Irt PU PBuSEliT
Y PU PUcab'f.T
7 PU PHcShNf
o STAItlLESo STEEL-DX
0 il^.'ANIv.1
0 0')>MNIC
70 (WJAN 1C
•55 U')X + P0()'(
H U(!X « r-U»X
37
-------
APPENDIX D-3. PARTICLE CONSTITUTION BY ELECTRON MICROPROBE, STACK SAMPLE.
IDENTIFICATION ELEMENTAL CONCENTRATION WT.Z ELEMENTS < 1.0%
EPA 43 201 W7g,021
EPA 43 202 ZN90,09 FE
EPA 43 203 ZN95,03.3,P1.7
EPA 43 205 048,SI23,FE13,AL8.7,S2.2,
MG1.8,NA1.4,PB1.2,P1 .0
EPA 43 501 051,SI36,AL7,FE4.7,K1.1 TI
EPA 43 504 U50,PU38,012
EPA 43 505 U50,PU38,012
EPA 43 50S 5147,053
ITOA AI *o,-7 U50,PU38,012
U50,PU38,012
5153,046 FE
049,SI29,K10,AL8,FE4.5 NA,CA,CR,MG,NI
U43,PU40,017
049,SI33,AL9,NA8 FE
4,5 D1Y U43,PU40,017
43 519 050,SI27,AL16,FE5,K2.0 MG,TI,CA
AT cofli FE56,033,CR4.2,SI3.7,NI2.3
U43,PU40,017
FE52,032,CR10,N3.9,MN1.5 SI,S,NA,CL
FE47,039,SI8,CR2.9,AL2.1 TI,CA,NA
U56,PU27,017
FE49,CR15,NI5,030,MN1
U55,PU30,015
052,SI44,FE1.8,AL1.0
051,SI30,FE9,AL4.6,K2.6,NA2.0
U51,PU32,017
W99
EPA 43 507
EPA 43 508
EPA 43 512
EPA 43 514
EPA 43 515
EPA 43 516
EPA 43 517
EPA
EPA 43 520
EPA 43 521
EPA 43 522
EPA 43 523
EPA 43 524
EPA 43 526
EPA 43 528
EPA 43 540 052,5144.FE1.8.AL1.0 K
EPA 43 542
EPA 43 543
EPA 43 545
EPA 43 547
EPA 43 548
EPA 43 550 047,5128 ,K 13, AL9,FE2.5 ' NA
EPA 43 552 053,5143,CL1 .8,NA1 .3 FE
EPA 43 553
047,5128 ,K 13, AL9,FE2.5
053,SI43,CL1.8,NA1.3
U52,PU31,017
EPA 43 554 FE50,030,CR9,NI6,CL1.7,51.0 NA
EPA 43 555 053,5146 FE,AL,P,MG,W
EPA 43 557 040, FE31,5117,CR3.9, AL3.4, NA
Nil.5,51.1
047.SI21.FEU.AL9.S4.4.NA1
EPA 43 559
v-r^ **£i&*v*yt^4.* •)\si\ve*'y nt-t w 0 —g m i~* r\
Nil.5,51.1
047,SI21,FE14,AL9,S4.4,NA1.0 MG,P,T]
38
-------
APPENCIX D-3. PARTICLE CONSTITUTION BY ELECTRON MICROPROBE, STACK SAMPLE.
(continued)
ELEMENTAL CONCENTRATION Wl
043,FE22,SI18,K4.9,AL4.3,
S2.4,CR1.9,NI1.4,NA1.1
FE42,037,SI12,CR2.0,AL1.7,
K1.6
C83.05.FE7.6.SI2.2.CR1.0
IDENTIFICATION ELEMENTAL CONCENTRATION WT.Z ELEMENTS < 1.07.
EPA 43 561
EPA 43 563 FE42,037,SI12,CR2.0,AL1.7, P,NI,S,NA
K1.6
EPA 43 565 C83,05,FE7.6,SI2.2,CR1.0 K,NI,AL,TI,SN,
P,S,CL,NA
EPA 43 566 TI39,039,FE17,313.4 AL,K
EPA 43 567 053,5147 FE
EPA 43569 041 ,FE33,3121 ,CR2.0,NI 1 .0 S,AL,CL,i1N
EPA 43 571 W99 FE,AL
EPA 43 573 045,3129,FE19,K1.1 CR,NI,P,NA,AL,
CA,S
EPA 43 575 048,SI29,AL10,FE7,TI3.0 K,CA
EPA 43 576 FE40,033,CR 12,NI6,SI5 ,P1.0 MN,S
EPA 43 578 FE48,033,314.2,CR3.7,NI2.2, MN,TI
NA1 .7,CL1 .6,S1.2,K1.2,CU1.0
EPA 43 584 045,3132,K21,FE1.1
EPA 43 587 FE43,032,CR11,NI5,TI3.2,SI1.8,
SI 2
EPA 43 590 U53,PU30,017
EPA 43 705 052,3143,FE3.9
EPA 43 706 053,3146 AL
EPA 43 707 C83,011,AL3.4,SI2.6 V,MG
EPA 43 708 050,3126,AL22,FE1.1 MG
EPA 43709 C72,021,SI4,FE1.4,AL1.0 P
EPA 43 710 051,5I36,AL11,NA2.3 K
EPA 43 711 C92,07 SI,NA,P,CL
EPA 43 712 052,3141,AL5,FE1.1
EPA 43 713 U59,022,SI19 AL
EPA 43 715 FEG7,032 SI
EPA 43 716 054,SI43,AL2.4 NA
EPA 43 717 U83,017
EPA 43 718 050,SI29,FE10,AL9,S1.8 K,CA,MG
EPA 43 719 C95,313.5,01.4 FE,K,AL
EPA 43 720 FE50,033,CR10,NI3.4,31.0 CL,SI,MN
EPA 43 721 045,SI27,FE20,AL3.3,GR1.7, NI,TI,P
K 1 ?
EPA 43 722 050,5129, AL12,K 6, FE2.2 GA,MG
EPA 4*3 723 PU65,U23,012
EPA 43 724 PU43,U41,015
39
-------
APPENDIX D-3. PARTICLK CONSTITUTION BY ELECTRON MICROPROBE, STACK SAMPLE.
(concluded)
IDENTIFICATION
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
43 735
43 73S
43 737
43 738
43 739
43 740
43 741
43 743
43 745
43 747
43 748
43 750
43 751
43 752
43 753
43 754
43 755
43 757
43 758
43 760
43 765
43 768
43 770
43 772
43 773
43 775
43 776
43 777
43 779
ELEMENTAL CONCENTRATION WT.%
041,FE37,SI11,AL5,P3.6,K2.2
045,SI16,TI13,AL12,FE10,K2.5,
NA1.7
051,SI34,AL8,FE5,K1.5
SI42,053,FE5
047,SI22,AL16,FE8,K5
C98,01.8
049,SI29,AL13,FE7,MG1.6
044,FE25,SI19,AL8,CR2.0,K1.8
FE49,035,SI8,CA3.5,AL1 .7,
MN1.5
C99
FE47,CR13,035,NI5
045,SI20,AL16,FE9,K8
FE65,032
046,8125, FE13,AL9,K2. 4, Nil. 4,
CR1.2,NA1.1
049,SI23,AL2l,FE6,K1.6
048,SI25,AL18,FE7
C99
C99
045,FE20,SI20,AL10,K2.0,CR1.0
047,SI31,FE12,AL4.7,K2.5
045,SI28,FE20,AL2.1
C99
047,M018,SI14,S12,CU6,TI2.9
040,FE28,SI16,CR5,AL4.5,NI3.0,
K2.6
FE46,032,CR18,NI4.1
053,3144, FE1. 9
FE47,037,SI10,K4.9
FE65,030,CL5
038,FE35,SI10,CR4.1,NA3.2,
ELEMENTS < 1.07.
NA,S,CR,CA,PB
P,NI
AL
NA
FE,P,NA,S
TI,K
P,NI,S,MG,TI
P,MG,K
FE,0
MN
MG
SI,AL
FE,AL,SI
FE,SI,TI
AL,K
S
K2.2,AL2.0,P1.8,S1.6,NI1,
FE45,034,CR9,SI7,NI3.0
049,SI33,K11,AL5,NA1.9
FE49,033,CR8,SI3.8,NI3.2i
AL1.1
C99
C99
C99
096,02.1,SI 1.
U46,PU37,017
U46,PU37,017
<\ £-..£., nL*C-.*V , J 1 »O fj 1«O,1VX 1 • 1
EPA 43 780 FE45,034,CR9,SI7,NI3.0 MN,S
EPA 43 782 049,SI33,K11,AL5,NA1.9 FE
EPA 43 783 FE49,C --------
AL1.1
EPA 43 784 C99
EPA 43 785 C99
EPA 43 786 C99
EPA 43 787 C96,02.1,SI1.5 CA
EPA 43 788 U46.PU37.017
EPA 43 789
40
-------
APPENDIX D-4. MASS SPECTROMETRY RESULTS FOR PLUTONIUM.
IDENTIFICATION #240
EPA
EPA
EPA
EPA
EPA
EPA
HP A
HP A
EPA
EPA
EPA
EPA
HP A
EPA
EPA
HP A
EPA
EPA
EPA
HP A
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
206
502
504
505
507
508
513
515
516
518
519
521
523
543
544
547
551
554
560
564
565
568
570
574
577
579
580
583
588
539
590
701
702
703
704
705
706
7t)8
709
710
712
1.490
1.433
0.
1.719
1.670
1.400
0.
1 .780
2.381
0.858
0.
.240
.743
.268
.349
.301
).
0.
.527
).589
.309
.546
. 167
.922
.819
0.942
.374
.816
.726
2.319
.544
.463
.517
.990
.071
.939
.192
.517
.443
.266
.789
ISOTOPIC
+SD ?<241
0.043
0.054
0. (
0.047
0.062
0.250
0.
0.077
0.074
0.260
0. (
0.062
0.056
0.050
0.192
0. 135
.416
.348
D.
.358
.453
.764
T.
.473
.865
.426
D.
.374
.357
.450
.396
.427
0. 0.
0. 0.
0.259 2.363
0.099
0.123
0. 113
0.167
0.099
0.075
0.072
0.095
0.124
0.073
0.228
0.080
0.049
0.053
0.075
0.054
0.069
0.070
0.044
0.053
0.064
0.054
.536
.461
.518
.487
.337
.215
.439
.404
.483
.335
.250
.499
.427
.426
.356
.504
.359
..557
.423
.579
.420
.422
DISTRIBUTION OF
+SD
0.010
0.012
0.
0.010
0.015
0.071
0.
0.019
0.020
0.066
0.
0.015
0.013
0.012
0.048
0.034
0.
0.
0.087
0.026
0.031
0.029
0.043
0.023
0.016
0.018
0.023
0.031
0.017
0.051
0.020
0.011
0.012
0.017
0.013
0.016
0.018
0.010
0.013
0.016
0.013
%242
0.200
0.217
0.
0.215
0.211
0.299
0.
0.210
0.226
0.208
0.
0.221
0.215
0.222
0.221
0.236
0.
0.
0.751
0.200
0.243
0.218
0 . 224
0.224
0.224
0.225
0.233
0.207
0 . 226
0.200
0.210
0 . 220
0.211
0.207
0.222
0.219
0.191
0.210
0.21 1
0.208
0.208
PLUTON
+5D
0.003
0 . 004
0.
0.003
0.004
0.028
0.
0.006
0 . 005
0.021
0.
0.005
0.004
0 . 003
0.017
O.D12
0.
0.
0.047
0.008
0.01 1
0 . 009
0.014
0.008
0.006
0.006
o.ooa
O.dIO
0.006
0.017
0.006
0.003
0 . 004
0.005
0.004
0.005
0.005
0.003
0.004
0.005
0.004
IUW
%239
36.894
87.003
00.000
86.708
80.666
86.536
00 . 000
86.5-38
85.52d
87.507
no. ooo
87.165
So. 635
87.060
87.035
87.037
no . ooo
00.000
•'-35.35y
87.675
86.y'37
86. 7M
87.123
80.51 H
86.742
87.393
86.990
86.494
86.713
86.232
86.747
86.391
86.847
86.44H
87.203
86.432
87.060
86.850
86.767
87.107
Ro.582
+SD
0.047
0.057
0.
J.050
0.066
0.262
0.
O.081
•0.079
0.270
0.
0.065
O.OD9
u.053
0. 1 yy
0. 140
0.
3.
0.2HO
0. 103
0. 12H
0. I1H
0. 174
0.102
0.078
J.076
O.oyy
Q.12y
0.077
0.234
U.OH4
v;.:>52
>).056
0.079
»j..)57
J.072
0.074
u.')48
o.Ob 6
0.06H
0.057
41
-------
APPENDIX D-4. MASS SPECTROMETRY RESULTS FOR PLUTONIUM. (concluded)
IDENTIFICATION .'S240
EPA
EPA
EPA
EPA
EPA
EPA
tPA
EPA
EPA
EPA
EPA
EPA
HP A
EPA
niPA
EPA
cPA
.EPA
EPA
:-:PA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
-'PA
EPA
EPA
.-:PA
EPA
EPA
EPA
EPA
SPA
EPA
EPA
EPA
SPA
EPA
EPA
EPA
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
4J
43
43
713
718
719
720
721
722
723
736
737
738
739
742
743
747
749
7oO
752
753
755
756
757
758
759
760
763
764
765
767
768
770
772
773
774
776
778
779
780
7H1
782
7'53
784-
/85
788
1.055
1.681
0.852
0.
1.281
2.519
0.942
1.211
2.415
1.523
1 . 359
0.
1 .062
2.100
1.387
1.992
1 .494
1.782
0.
1 . 607
1.713
1.932
1.855
1 . 354
1 . 485
2.073
1.972
1.787
1 . 308
1.782
1.668
2.J73
1.599
1.590
1.651
2.271
2.630
1 . 6VO
1.215
0.
0.
1 . 627
1.627
789 10.847
ISOTOPIC
+SD S241
0.167
0.071
0.136
0.
0.071
0.296
0.038
0.132
0.079
0.078
0.153
0.
0.252
0.203
0.152
0.069
0.052
0. 165
0. (
0.086
0.193
0.068
0.066
0.018
0.138
0. 170
0.086
0.147
0.214
0.145
0.085
0.279
0.194
0.208
0. 112
0.170
0. 166
0.142
0.268
.557
.383
.571
3.
.457
.386
.473
.466
.247
.446
.499
).
.347
.509
.383
.301
.366
.360
).
.356
.621
.388
.456
. 40'?
. 462
.387
.254
.338
.349
.380
.411
.376
.471
.330
.377
.526
.135
.364
.156
0. 0.
0. 0.
0.085 1.539
0.069 1.426
0.092 1.529
DISTRIBUTION OF
+SD
0.044
0.017
0.037
0.
0.017
0.070
0.009
0.034
0.017
0.019
0.039
0.
0.062
0.051
0.037
0.016
0.012
0.040
0.
0.020
0.051
0.016
0.016
0.022
0.035
0.041
0.019
0.035
0.052
0.035
0.020
0.067
0.050
0.050
0.027
0.042
0.035
0.034
0.062
0.
0.
0.021
0.016
0.024
35242
0.209
0.212
0.231
0.
0.217
0.224
0.220
0.214
0.205
0.215
0.236
0.
0.214
0.243
0.209
0.193
0.202
0.225
0.
0.226
0.207
0.213
0.210
0.206
0.246
0.214
0.214
0.232
0.238
0.241
0.195
0.214
0.285
0.217
0.229
0.21 1
0.239
0.235
0.237
0.
0.
0.212
0.206
0.271
PLUTONIUM
+SD
0.014
0.005
0.012
0.
0.005
0.024
0.002
0.011
0.006
0.006
0.014
0.
0.020
0.018
0.013
0.005
0.003
0.014
0.
0.007
0.016
0.005
0.005
0.007
0.012
0.014
0.006
0.012
0.019
0.012
U.006
0.025
0.020
0.017
U.009
0.013
0.013
0.013
0.025
0.
0.
0.007
0.005
0.008
5K239
87 . 1 79
86.724
87.346
00.000
87.044
85.871
87.365
87.109
86.133
86.816
86.406
00.000
87.376
86.149
86.521
86.514
86.938
36.632
00.000
86.811
86.459
86.467
86.479
87.031
86.807
86.327
86.559
86.642
87.105
86.597
86.726
86.037
86.645
86.864
86.743
85 . 99 1
85.996
86.710
87.392
00.000
00.000
86.621
86.741
87.353
+SD
0.174
0.075
0.143
0.
0.074
0.305
0.042
0.137
0.082
0.082
0.160
0.
0.260
0.211
0.157
0.072
0.056
0.171
0.
0.090
0.201
0.071
0.070
0 . 092
0.1 44
0.176
0.089
0.152
0.222
0. 150
0.088
0.289
0.203
0.215
0. 116
0.176
0. 171
0.147
0.277
0.
0.
0.089
0.072
0.096
42
-------
APPENDIX D-5. MASS SPECTROMETRY RESULTS FOR URANIUM
i*d:i
i:PA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
h'PA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA.
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
CATION
2J6
501
502
503
504
505
506
507
508
513
b!5
516
518
519
521
522
523
525
526
528
533
541
543
544
546
547
549
551
553
554
555
•558
560
564
565
566
568
570
572
574
575
'.'.234
O.OOb
0.
0.
0.
0.
0.
0.
0.005
0.
0.
0.
0.
0.011
0.
0.005
0.
0.006
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
I
*jn •
o.ooo
{).
0.
0.
0.
0.
0.
o.oro
0.
0.
0.
0.
0.001
0.
0.000
0.
0.001
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
fiOTOPIC
3235
0.703
3.5°-^
0.
0.
0.
0.721
0.
0.719
0.
0.
0.
0.
I .I9y
0.
0.735
0.
0.735
0.
0.
0.
0.
0.
0.744
0.
0.
0.605
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.794
0.
nidTRIiJUTIOil OF
+sn
0 . 009
0. 101
0.
0.
0.
0 . 00V
0.
0 . 003
0.
0.
0.
0.
0.0)5
0.
0.007
0.
0.010
0.
0.
0.
0.
0.
0.017
0.
0.
0.020
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.024
0.
•;236
o.ooi
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
URA'4IU'/
+sn
0.000
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
V238
99.291
96.412
00.000
oo.ooo
no. ooo
99.279
00.000
9V . 276
00.000
00.000
oo.ooo
00.000
98.790
00.000
99.260
00.000
99.259
00.000
00 . 000
00.000
00 . 000
00.000
99.256
00.000
00.000
99.395
00.000
00.000
00.000
oo.ooo
00.000
00.000
00.000
00.000
oo.ooo
00.000
00.000
oo.ooo
00 . 000
99.206
oo.ooo
+SD
0.009
0.115
0.
0.
*0.
0.010
0.
O.OO8
0.
0.
0.
0.
0.015
0.
0.007
0.
0.0)0
0.
0.
0.
0.
0.
0.017
0.
0.
0.022
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.02b
0.
43
-------
APPENDIX D-5. MASS SPECTROMETRY RESULTS FOR URANIUM. (continued)
IDENTIFICATION
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
577
579
580
581
582
583
584
585
586
588
589
590
701
702
703
704
705
706
707
708
709
710
711
712
713
718
719
720
721
723
735
736
737
738
739
740
741
742
743
745
746
%234
0.
0.
0.
0.
0.005
0.
0.
0.
0.
0.
0.
0.
0.005
0.
0.
0.005
0.005
0.007
0.
0.005
0.
0.006
0.
0.005
0.
0.
0.
0.
0.362
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
+SD
0.
0.
0.
0.
0.001
0.
0.
0.
0.
0.
0.
0.
0.000
0.
0.
0.000
0.000
0.001
0.
0.000
0.
0.001
0.
0.001
0.
0.
0.
0.
0.004
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
ISOTOPIC
%235
0.705
0.714
0.727
0.721
0.732
0.735
0.
0.
0.7J1
0.672
0.
0.733
0.725
0.754
0.728
0.728
0.708
0.727
0.
0.730
0.
0.710
0.
0.708
0.
1.083
0.832
3.914
35.587
0.691
U.
0.742
0.728
0.
0.
0.
0.
0.
0.
0.
0.
DISTRIBUTION OF
+SD
0.016
0.015
0.021
0.013
0.008
0.013
0.
0.
0.013
0.015
0.
0.015
0.008
0.014
0.014
0.008
0.010
0.015
0.
0.008
0.
0.012
0.
0.012
0.
0.023
0.020
0.104
0.098
0.015
0.
0.020
0.015
0.
0.
0.
0.
0.
0.
0.
0.
*236
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.001
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.078
0.006
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
URANIUM
+SD
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.000
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.002
0.001
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
%238
99.295
99.286
99.273
99.279
99.263
99.265
00.000
00.000
99.289
99.328
00.000
99.267
99.271
99.246
99.272
99.267
99.285
99.266
00.000
99.264
00.000
99.285
00.000
99.286
00.000
98.917
99.168
96.086
63.974
99.303
00.000
99.258
99.272
00.000
00.000
00.000
00.000
00.000
00.000
00.000
00.000
+SD
0.016
0.015
10.022
0.013
0.009
0.014
0.
0.
0.014
0.015
0.
0.015
0.008
0.015
0.014
0.008
0.010
0.015
0.
0.008
0.
0.012
0.
0.012
0.
0.023
0.020
0.105
0.099
0.016
0.
0.021
0.015
0.
0.
0.
0.
».o.
0.
0.
0.
44
-------
APPENDIX D-5. MASS SPECTROMETRY RESULTS FOR URANIUM. (concluded)
IDENTIFICATION %234
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
43
43
43
43
43
43
43
4.3
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
43
747
748
749
750
752
753
754
755
756
757
758
759
760
763
764
765
766
767
768
769
770
771
772
773
774
775
776
778
779
780
781
782
783
784
785
786
787
788
789
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
+SD
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
ISOTOPIC
•K235
0.
0.
0.
0.698
0.701
0.
0.
0.
0.696
0.
0.720
0.741
0.
0.
0.
0.713
0.
0.710
0.
0.
0.688
0.
0.
0.
0.
0.
0.
0.
0.660
0.
0.
0.
0.
0.
0.
0.
0.
0.754
0.
DISTRIHUTION OF URANIUM
+SD
0.
0.
0.
0.017
0.021
0.
0.
0.
0.016
0.
0.015
0.022
0.
0.
0.
0.017
0.
0.021
0.
0.
0.017
0.
0.
0.
0.
0.
0.
0.
0.021
0.
0.
0.
0.
0.
0.
0.
0.
0.017
0.
'".236
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
+SD
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
%238
00.000
00.000
00.000
99.302
99.299
00.000
00.000
00.000
99.304
00.000
99.280
99.259
00.000
00.000
00.000
99.287
00.000
99.290
00.000
00.000
99.312
00.000
00.000
00.000
00.000
00.000
00.000
00.000
99.340
00.000
00.000
00.000
00.000
00.000
00.000
00.000
00.000
99.246
00.000
+SD
0.
0.
0.
0.017
0.021
0.
0.
0.
0.016
0.
0.016
0.023
0.
0.
0.
0.017
0.
0.021
0.
0.
0.017
0.
0.
0.
0.
0.
0.
0.
0.022
0.
0.
0.
0.
0.
0.
0.
0.
0.017
0.
45
-------
APPENDIX E-l. RESULTS OF GROSS ANALYSIS OF ENVIRONMENTAL SAMPLES.
Gross analysis of environmental air samples to date gives the following
values of collected actinides as determined by mass spectrometry.
Sample No.
Plutonium
Uranium
49
50
51
52
55
62-1
62-2
62-3
-13
<5.8 x 10 g/sample
—12
<1.1 x 10 g/sample
—12
<2.4 x 10 g/sample
—13
<7.6 x 10 g/sample
— 12
<1.0 x 10 g/sample
— 12
48.0 x 10 g/g particulate
-12
92.0 x 10 g/g particulate
-12
67.0 x 10 g/g partieulate
4.47 x io~ g/sample
2.86 x 10~ g/sample
3.59 x lo~ g/sample
4.9 x 10~ g/g particulate
4.6 x 10 g/g particulate
-6
2.7 x 10 g/g particulate
Below minimum detectable level
-------
APPENDIX E-2. GROSS ISOTOPE LEVELS FROM MASSIVE AIR SAMPLES.*
Sample 62-1
0. 2624 g total weight
3.5-20 ym size range
Isotope Concentration
(yCi/ml)
239Pu 2.
Pu 1.
2^Pu 7.
U 8.
U 2.
U 1 .
61
31
75
22
86
71
x 10-18
x 10-18
x 10-17
x 10-18
x 10-19
x 10-2°
Percent of
Total Wt.
86.8
11.8
1.4
0.0266
2.69
0.0054
Sample 62-2
0.2131 g total weight
1.7-3.5 ym size range
Concentration
(yCi/ml)
3
2
2
2
7
2
.98
.10
.59
.29
.38
.39
x 10-18
x 10-18
x 10-16
x 10-18
x ID"19
x ID'20
Percent of
Total Wt.
84.9
12.1
3.0
0.0333
3.09
0.0099
Sample 62-3
1.1523 g total weight
<1.7 ym size range
Concentration
(yCi/ml)
1.59
8.10
6.13
3.16
1.10
7.36
x 10-17
x 10-18
x 10-16
x 10-17
x 10-18
x 10-2°
Percent of
Total Wt.
86.4
11.8
1.8
0.0422
4.12
0.0097
Specific
Activity
(Ci/g)
6.14 x lo"2
2.27 x lo~
1.13 x lo2
6.19 x lo~3
2.14 x lo"6
6.34 x 10~5
*Data reduced from gross values tabulated in Appendix E-l.
-------
APPENDIX F-l. OPTICAL MEASUREMENTS: ENVIRONMENTAL AIR SAMPLES.
IDENFIFICATION COLOR
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
bPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
42
42
42
£?
42
42
42
42
42
42
42
42
42
42
42
50
50
50
50
50
50
50
50
50
50
101
102
103
104
105
106
107
108
0V
10
1 1
12
13
14
15
201
202
203
501A502
502B501
503
504
b05
506
507
508
50V
510
5I1A512
51 285 11
201
501
502 ORANGE
113A504
504B503
505C50V
506A507
507B5O6
508
50yE505
5 1 OE505
70IA704 BROWN
702 YELLOW
703 BROWN
704B701
701 BROWN
702 BROWN
703 BROWN
704
705
706 BROWN
707
708
70V
7IOA7I6 BROWN
YELLOW
YELLOW
GREEN
NO COLOR
NO COLOR
NO COLOR
YELLOW
OPAOUH
YELLOW
YELLOW
ORANGE
OPAQUE
ORANGE
NO COLOR
YELLOW
YELLOW
YELLOW
YELLOW
YELLOW
YELLOW
YELLOW
BROWN
YELLOW
YELLOW
YELLOW
YELLOW
YELLOW
YELLOW
MCC
100
100
100
100
100
16
100
16
16
100
100
100
100
100
100
10
10
a
20
100
100
32
16
100
100
100
24
20
32
20
8
17
24
17
100
100
16
100
100
16
16
?8
28
28
100
28
28
23
100
100
28
mo
100
100
28
TRACKS
200.
5000.
300.
450.
150.
700.
830.
150.
2800.
3000.
2700.
1000.
3000.
4000.
3500.
0.
0.
0.
50.
0.
40.
30.
30.
25.
35.
35.
40.
40.
0.
24.
0.
vo.
40.
0.
60.
0.
0.
35.
20.
45.
45.
0.
50.
45.
18.
38.
130.
175.
10.
17.
350.
25.
16.
14.
0.
SIZE
0.
0.
0
0
0.
t.
0.
0.
1 .
0.
0.
0.
0.
0
0.
15.
12
7.
2.
0.
0.
9.
5.
0.
0.
0
15.
2.
5.
2.
13.
IV.
19.
2.
0.
0.
2.
0.
0.
35
13
7
18
4
0
5
10
2
0
0
2
0
0
0
5
»
»
»
6
0
5
0
5
3
0
0
6
1
0
0
0
5
5
7
5
0
.0
.0
0
.3
i
.2
.0
.8
i
.5
»
•
.0
COMMENTS
LOST
GYPSUW
GYPSUM
GYPSUM
UOX
7.IRCON
FEOX
KFESI308
ORGANIC
LOST
ORGANIC
ORGANIC
ORGANIC
ORGANIC
ORGANIC
FEOX
NBOX
48
-------
APPENDIX F-l. OPTICAL MEASUREMENTS: ENVIRONMENTAL AIR SAMPLES. (continued)
IDENTIFICATION
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
bO 711
50 712
50 713
50 714
50 715
50 71 687 10
54 20IA202
54 202B20I
54 203
54 204D205
54 205E204
55 I01A102
55 I02B101
55 103
55 104
5b 105
55 106
55 107
55 108
55 109
55 HO
55 201
55 202
55 203
55 204
55 205
55 206
55 207
55 208A20V
55 209B208
55 2IOC2M
55 2IIE2IO
55 212
55 213
55 214
55 215E2IO
55 701
55 702
55 703
56 201
56 202
56 203
56 204
56 205
56 206
56 207
56 208
56 209
56 210
56 211*
56 212
56 213
56 214
56 215
57 201
57 203
57 204
57 205
57 206
COLOR
YFiLLOW
BROWN
BROWN
YELLOW
GREEN
GREEN
ORANGH
BROWN
GREY
YELLOW
YELLOW
YELLOW
GREY
ORANGE
BROWN
YELLOW
YELLOW
YELLOW
GREEN
OPAQUE
OPAQUE
GREY
BROWN
BROWN
YELLOW
ORANGE
Yt£LLOW
OPAOUH:
GREY
OPAQUR
ORANGE
OPAQUH
bROWN
OPAQUE
GRH:EN
OPAQUE
BROWN
BROWN
BROWN
BROWN
OPAQUE
GRREN
OPAOUS
OPAQUE
OPV3UE
RED
BROWN
OPAOUE
OPAQUE
OPAOUE
BROWN
OPAQUE
OPAOUE
HED
NO COLOR
NO COLOR
MCC
100
20
28
28
28
100
100
32
48
20
100
?4
20
28
28
100
100
100
100
too
28
100
100
100
32
24
32
mo
28
32
100
3?
100
24
3?
24
22
22
28
100
100
100
32
16
32
32
32
28
29
32
32
100
50
28
48
48
28
8
8
TRACKS
42.
160.
20.
26.
42.
22.
50.
50.
50.
0.
140.
0.
1001.
1001 .
1001 .
1001.
1001.
1001 .
1001.
1001.
1001.
300.
400.
500.
500.
100.
150.
350.
0.
190.
350.
175.
175.
200.
250.
175.
999V.
9999.
9999.
400.
300.
300.
150.
250.
12b.
125.
200.
400.
250,
140.
225.
125.
150.
300.
0.
0.
0.
0.
0.
SIZE
0.
6.8
5.8
8.0
9.0
0.
3.7
1.2
9.6
6.8
0.
5.6
1.8
6.5
6.5
0.
0.
0.
0.
0.
4.8
0.
0.
0.
1.V
A. 5
1.0
0.
7.5
1.3
20.6
4.8
0.
2.1
1 .3
21.8
7.0
1 1 .0
4.7
0.
0.
0.
1 .6
3.7
6.8
1.9
2.3
2.3
28.0
1 .8
4.8
0.
4.3
4.2
15. 0
10.0
10.2
32.0
17.5
CO«MENT
LOST
UOX
CARBON
UOX
UOX
NliOX* UOX
ORGANIC
LOST
LOST
U308
U02
U02
Ht£S2. (PYRITE)
LObT
UOX
ORGANIC
LOST
U03
LOST
ORGANIC
FE203
GYPSUW
GYPSUM LOST
49
-------
APPENDIX F-l. OPTICAL MEASUREMENTS: ENVIRONMENTAL AIR SAMPLES. (continued)
IDENTIFICATION COLOR MCC TRACKS
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
57
57
57
57
57
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
58
53
58
58
58
58
58
58
58
59
59
59
59
59
59
59
59
59
bV
59
59
59
59
69
59
5P
59
59
59
59
59
5V
207C209 YELLOW
208C210
209E207
2 1 OE208
2 1 1 E208
201 BROWN
202
203
204
205
206
207
208
209
210
2 1 1 BROWN
212
213
214
215
216
217D218
218E2I7
219
220
221
222
223
224
225
226D227
227E226
228
229 ORANGE
230 RED
231
232E217
233E226
201
202D203 MED
203E202
204E202
205
206A2I3
207
208 OHANGh
20V ORANGE
210 04ANJP
211
212
2I3B206
214
215
216
217
2I8A219
2I9B213
220A221
221 8220
222 A 223
223A224
BROWN
BROWN
OPAQUE
GREY
NO COLOR
NO COLOR
OPAQUt
OPAQUE
OPAQUP
BWOWN
GREY
OPAQUE
OPAQUE
ORANGE
OPAOUE
RED
OPAOUE
OPAOUE
OPAOUE
OPAOUE
OPAOUE
OPAOUE
OPAOUE
OPAQUE
OPAOUE
OPAQUE
OPAOUE
OPAOUE
OPAOUE
BROWN
BROWN
ORANGE
OPAOUE
OPAOUE
OPAOUE
OPAOUE
BROWN
OPAOUE
OPAOUE
OPAQUE
ORANGE
•OPAOUE
GRHY
GREY
BROHN
OPAOUE
NO COLOR
OPAQUE
NO COLOR
NO COLOR
GREY
NO COLOR
17
20
32
100
100
24
8
9
32
32
32
28
24
32
32
28
32
28
32
32
32
32
32
100
32
32
32
32
32
32
32
48
28
28
28
48
32
48
32
28
ioo
100
32
28
48
16
16
?o
100
100
ino
100
ion
32
100
16
32
0
8
24
16
0.
0.
0.
0.
0.
0.
0.
0.
1001.
100.
100.
80.
125.
125.
140.
1000.
300.
200.
350.
150.
200.
1001 .
750.
45.
100.
40.
65.
42.
1001 .
110.
1001 .
600.
1001 .
150.
1001.
300.
1000.
500.
500.
0.
0.
0.
1001.
0.
150.
90.
120.
500.
125.
200.
1000.
250.
45.
125.
100.
125.
125.
125.
125.
0.
0.
SIZE
7.0
28.0
4.3
0.
0.
22.0
35.0
9.8
9.6
3.4
2.8
1.8
4.1
1 .5
3.8
5.8
3.0
3.2
6.1
4.2
3.6
11.8
5.0
0.
21.0
0.
0.
0.
17.5
1.3
18.2
9.8
10.8
5.5
1.1
4.8
6.8
8.4
5.9
7.8
1.4
2.9
1.6
1.3
4.5
1.4
1.3
4.4
0.
0.
0.
0.
0.
1.3
0.
11.2
1.2
7.5
2.0
3.4
13.2
COMMENTS
CARBON
CARBON
UOX
UOX
LOST
GYPSUM LOST
UOX
FEOX
ZROX
UOX
U308 + U02 LOST
UOX
UOX
LOST
UOX + NBOX
U03
U02
U02
U03
U02 + U308
U03
LOST
LOST
UOX + NBOX
ALSIOX
U02
UOX
UOX
LOST
UOX
ORGANIC
SI OX
ORGANIC
50
-------
APPENDIX F-l. OPTICAL MEASUREMENTS: ENVIRONMENTAL AIR SAMPLES. (concluded)
IDENTIFICATION COLOR MCC TRACKS
EPA
EPA
EPA
EPA
HP A
EPA
EPA
tPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
61
61
61
61
61
61
61
61
61
61
61
61
61
61
61
61
61
59
59
59
59
5V
60
60
60
60
60
60
60
60
60
60
60
60
60
60
60
60
61
61
61
61
205
206C207
207E206
208A209 ORANGE
209H208
2IOA211 ORANGE
2 11 82 II 0
2 1 2 BROWN
213
214
215
216
217
213
219
220
22IE206 GREEN
224B223
225
226
227E202
228B222
201
202
203
204
205
206
207
208
209
210 BROWN
211
212
2I3A216 GREY
2UA215 GREY
2I5B214
2I6B213
201
202
203
204
OPAQUE
OPAQUE
BROWN
OPAOUt
BROrtN
OPAQUE
ORANGE
OPAQUE
GREY
OPAQiJH
OPAQUE
NO COLOR
OPAQUE
YELLOW
NO COLOR
GRHEN
GREEN
OPAQUE
OPAQUE
OPAQUE
OPAQUE
OPAQUE
3?
100
32
16
3?
16
32
?4
32
100
IQO
mo
100
ino
100
ion
2H
3?
100
100
100
mo
32
100
100
100
100
100
100
100
32
100
100
100
24
16
32
100
32
32
32
32
35.
87.
0.
0.
1001.
150.
150.
150.
150.
300.
300.
850.
350.
50.
200.
700.
H7.
500.
90.
150.
1001 .
125.
150.
?oo.
150.
500.
250.
500.
40.
110.
200.
1001 .
100.
1001.
0.
0.
300.
1001 .
23.
33.
44.
58.
517.E COMMENTS
0.
5.0
1.2 LOST
8.5 ORGANIC
0. UOX
9.9 ORGANIC
0.
0.
0.
0.
0.
0.
0.
0.
0.
0. SOLUBLE UtUSIJV!
3.d
2.0
0.
0.
?.0 UOX + 7H
0. UOX
0.
0.
0.
0.
0.
0.
0.
0.
1.2
0.
0.
0.
26.5
9.5 ORGANIC
4.1
5.0 UOX + 7.R
0.
0.
0.
1 .0
51
-------
APPENDIX F-2. PARTICLE CONSTITUTION BY EMP: ENVIRONMENTAL AIR SAMPLES.
IDENTIFICATION ELEMENTAL CONCENTRATION WT.Z ELEMENTS < 1.0Z
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
41
41
41
41
41
41
41
41
41
42
42
4O
<-
42
42
42
42
42
53
53
50
5tJ
53
53
53
53
53
54
54
201
232
233
531
534
525
539
510
511
201
501
503
509
510
721
722
703
721
702
703
70S
71i?
712
713
714
71 1
231
K33
048,CA27,S24
C A 70, 029
04$ ,C A3 1,523
U32,017
047,SI24,ALll,FEia,K3.1,Si:.0,
NA1.3.CL1.0
050,SI25,AL22,FE2.5
ZR41,038,SI18,FE1.4,Yl.l
FE<7,332,S1.2
FE54,033,K5,S3.1,NA2.1,SI1.8
04S,SI33,K15,AL4.5,FE2.7
C88, 04. 5, FE2. 1,512.1, ALLS,
51.0.
CP9,08,SL2.4
C89,04.7,P2.ltSl.8,FEU5
CS9,013,SI9,S4.2,FE3.2,K1 .9,
AL1 .5
C91,04.3,SI1.5,FE1.3,TI1.3
043,FE18,SI1S1AL14,K5,MG2.8,
Til. 2
C81,013,5I3.6,AL2.4
047,SI23,AL15,FE?,K4.1,S1.7,
FES5, 032 ,5 1.1, SI 1.3
NB65,033,FEl.'>,:n .5^(1.0
045, SI 18, FE1 1 , US, ,^7,54.4,
K.:.3,TI2.1,NA::.3
0-12,?R.14,S1S,SI9,NA4.9,FE1.5,
?1. 4
049,SIf;7,AL9,PB4.9,Si:.9,K;:.7,
HA?..5,FE1.4
051,SI33,AL12,K3.5
019, 5131 ,FE12,ALS,S 1.3
HC3,017
051,SI31,ALlf?,FE1.5
C7"S,ni2,Sl9,AL1.8,FE1.3
SI
SI,FE
SI
TI,MG
CA,TI,MG,K
P, AL,HF,CA,S,
F
ZR,CL,Sl,NA
BA.NA
NA,K,CL
FE.AL
ZN,CL,SI,AL,-.1G,
K
PB,ZN,NA,P,MG,
CA,CL
CL,AL,S,P,NA,
MG,CA
S,FE,NA,MG,CAt
K
P
AL,ZN
!"JG, TI ,NA
NA,P
CA,MG
K,S
52
-------
APPENDIX F-2. PARTICLE CONSTITUTION BY EMP: ENVIRONMENTAL AIR SAMPLES.
(continued)
IDENTIFICATION
EPA
EPA
EPA
EPA
ZPA
EPA
HPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
SPA
SPA
EPA
CPA
EPA
EPA
H?A
EPA
EPA
EPA
EPA
EPA
EPA
54 204
54 205
55 101
55 102
55 133
55 134
55 204
55 £08
55 731
55 702
55 703
5$ 208
5S 209
57 j>01
57 203
57 204
57 205
57 207
57 208
57 210
57 211
58 210
58 211
58 i:l2
58 213
58 215
58 2K
50 225
^o rlflo
jf j t~t **f~t
59 235
59 2<5S
59 23?
59 i',P9
59 213
ELEMENTAL CONCENTRATION WT.%
049,SI33,FE10,K3.8,AL3.0
1183,017
047, SI 17,AL16,FE15,CA4.2
U83,017
NS37,U34, 02S,FE1.0fSl .0
053,SiaS,AL21,NA1.3
C97,01.i,?B1.3
048,SI2S,AL1 7,FE$,CA1.5
(JS7,ZR13,0<5,FE3*9
U73,ZR15,03.3,FE4.8,P2.4,
SI. 2
S60,FE40
1)31,018,511.2
FE55,031,PB8,S4.2,CL1.5
C'74,SI12,07,AL4.1,K1'..5
C86,OS,r>I3«fl,Sc:.5,FEl .8
FES9,030
045,CA33,S22
C90,07,9ia.7
C91, 05,513. 4
U83, 017
IJ83,017
DR3,ai7
FE59,032,SI2.2,U2.0,CL1.6,
SI .4,NA1 .2
ZR73,029
U83,017
1)83,017
(J83,017
U73,NB13,01S
043,CA39,St 1 1 ,S5,K2.0,FE1 .5,
ALl.l
!K3,MBf;0,017
AL23, 3124,053
1)83,017
IJ83,017
U83,017
ELEMENTS < 1 .02
P,S
Mfi
PB,SI,ZR
TI
SI,FE,S,NA
K,TI,MG
NA
NA
S,CA, FE
K,AL,PB,CA,MG,
NA
S,SI
PB,FE,S,AL,TI,
P,K
AL,FE,S,PB,P
SI
CR
U,SN
FE
FE.NI
NI
FE
NA,P
CF?,MN,FE
53
-------
APPENDIX F-2. PARTICLE CONSTITUTION BY BMP; ENVIRONMENTAL AIR SAMPLES.
(continued)
IDENTIFICATION ELEMENTAL CONCENTRATION WT.Z ELEMENTS < 1 ,0Z
EPA 59 218 C99 0,5,CL,NA,CA,
SI
EPA 59 220 053,5145 K,NA,FE
EPA 59 222 C8S, 08,514.4, AL1.0 KA,S
EPA 59 223 051,5143,CAS
EPA 59 227 fJ74,014,ZRI2
EPA 59 228 1183,017
EPA S3 213 051,SI2S,AL2Z,ZN1.3,TIl.a FE.NA
EPA «0 214 C93,03.9,512.8 AL.ZN.TI
EPA 613 216 U74,014,Z^12
EPA SI 22C C95,OJ.5,P1.3 FE, <;L,NA,S, SI,
K,CL
EPA SI 209 IH?3,017
EPA SI 210 C8?,OS,SI2.3,?C1.5,AL1.3 NA,K,3
EPA 61 •££.{ 049,SI36,FE3.2,K3.2,AL2.7,
PB1.6,S1.S
54
-------
APPENDIX F-2.
PARTICLE CONSTITUTION BY BMP: ENVIRONMENTAL AIR SAMPLES
(concluded)
IDENTIFICATION ELEMENTAL CONCENTRATION WT.Z
BCLS2
BCLS2
BCL62
BCLS2
BCLS2
201
202
203
204
205
C88,010,SI1.7
04S,AL20,SI19,K12,FE1.8,NA1.
039 ,FE27,TI 16,519, AL5,K 1.1
050(SI38,FE4.1,AL2.2,NA2.1
037,K24,SI17,CL5,NA4.2,FE4.1
BCLS2 1 20S
BCL62 1 207
BCL62 1 208
BCLS2 1 212
BCLS2 1 213
BCLS2 2 202
BCL62 2 203
BCLS2 2 205
BCL62 Z 206
BCLS2 2 207
BCL62 2 208
BCLS2 2 209
BCL62 2 210
BCL62 3 20S
C A2
C90,07,SI1.5,S1.1
04S,SI25,AL12,NA6,CA4.6,FE3.5,
MN1.1,K1.0
043,FE27fSI17,NA6,AL5
U83,017
U83,017
C77,013fFESfAL3.2,SI1.9,CA1.0
FE38,032,CL13,313.8,33.1,
CA2.4,AL2.0,TI1.8,P1.2,NA1.0
040,FE27,SI9,AL5,P4.8,S2.5,
PB2.1,CA1.7,NA1.7,MG1.S,CL1.4
044,SI15,FE11,AL9,S6,CAS,
K2.3,PB2.2,F1.4,NA1.2
CS7f019,SIS,AL3.6,FE3.5
050,SI33,AL5,K3.1,FE2.9,S2.5
FE44,034,NI8,SI6,S2.2,AL2.1,
CL1.5
U83,017
C90,05,FE3.3,AL1.4
ELEMENTS < 1.0Z
CA,FE,AL,NA,S
NA.MG.CA
CL,K,MGtS
AL,CA,TI,FE,BA,
NA
CR
SfCA,TI
ZR
NA,K,S
MN,K,MG,PB
TI
TI,MG,P
S,NA,K,TI,CA,
MGfPB,P,MN
CA,TI,PB,NA
NA,MN,CU,PB,Kt
P,TI
S,NA,P,CA,SI,
U
55
-------
APPENDIX F~3.
URANIUM ISOTOPES FROM MASS SPECTROMETRY RESULTS,
ENVIRONMENTAL AIR SAMPLES
IDENTIFICATION X234
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
•EPA
EPA
EPA
EPA
EPA
EPA
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
41
42
42
42
42
42
42
42
50
50
50
50
50
50
54
54
55
55
55
55
55
55
55
55
101
102
103
104
105
106
107
108
110
111
112
501
503
504
505
508
509
512
501
504
508
509
510
701
702
701
704
705
707
713
716
201
204
102
104
106
107
108
202
204
205
0.521
0.523
0.510
0.517
0.489
0.511
0.514
0.520
0.519
0.523
0.520
0.001
0.025
0.
0.001
0.022
0.006
0.
0.
0.394
0.016
0.025
0.
0.016
0.
0.015
0.
0.017
0.013
0.
0.015
0.
0.061
0.018
0.016
0.
0.327
0.280
0.096
0.260
0.338
+SD
0.004
0.004
0.005
0.004
0.005
0.004
0.004
0.005
0.004
0.005
0.004
0.000
0.001
0.
0.000
0.001
0.000
0.
0.
0.037
0.001
0.001
0.
0.001
0.
0.001
0.
0.001
0.001
0.
0.001
0.
0.001
0.000
0.000
0.
0.005
0.005
0.004
0.021
0.025
ISOTOPIC
%235
49.762
49.850
49.462
49.413
46.683
49.069
49.513
49.778
49.813
49.505
49.702
0.236
2.656
0.
0.231
2.510
0.726
0.
0.
45.191
1.976
3.022
0.
1.989
0.
1.957
2.133
2.111
2.238
0.
2.090
0.
6.393
2.046
2.004
7.281
32.938
27.944
8.064
23.796
37.775
DISTRIBUTION OF
+SD %236
0.106
0.105
0.106
0.104
0.105
0.105
0.105
0.111
0.105
0.108
0.106
0.003
0.020
0.
0.003
0.017
0.008
0.
0.
0.503
0.018
0.025
0.
0.015
0.
0.015
0.039
0.025
0.022
0.
0.023
0.
0.030
0.014
0.013
0.054
0.092
0.109
0.056
0.340
0.372
0.075
0.075
0.075
0.075
0.069
0.074
0.073
0.073
0.077
0.076
0.075
0.004
0.002
0.
0.005
0.011
0*
0.
0.
0.153
0.
0.013
0.
0.
0.
0.009
0.
0.010
0.
0.
0.009
0.
0.021
0.011
0.001
0.
0.091
0.069
0.
0.
0.097
URANIUM
+SD X238
0.001
0.001
0.001
0.001
0.001
0.001
0.001
0.001
0.001
0.001
0.001
0.000
0.000
0.
0.000
0.001
0.
0.
0.
0.030
0.
0.001
0.
0.
0.
0.000
0.
0.001
0.
0.
0.001
0.
0.001
0.000
0.000
0.
0.002
0.003
0.
0.
0.018
49.642
49.552
4V. 953
49.995
52.759
50.346
49.900
49.629
49.592
49.896
49.704
99.759
97.317
00.000
99.763
97.458
99.268
00.000
00.000
54.262
98.009
96.940
00.000
97.994
00.000
98.018
97.867
97.861
97.748
00.000
97.886
00.000
93.525
97.925
97.980
92.719
66.644
71.706
91.840
75.943
61.791
+SD
0.106
0.104
0.107
0.105
0.105
0.105
0.105
0. Ill
0.104
0.108
0.106
0.003
0.020
0.
0.003
0.017
0.008
0.
0.
0.506
0.018
0.025
0.
0.016
0.
0.015
0.040
0.025
0.022
0.
0.023
0.
0.031
0.014
0.013
0.054
0.093
0.109
0.057
0.341
0.374
56
-------
APPENDIX F-3.
URANIUM ISOTOPES FROM MASS SPECTROMETRY RESULTS,
ENVIRONMENTAL AIR SAMPLES, (continued)
IDENTIFICATION X234
EPA
EPA
EPA
EPA
EPA
hPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EPA
EAP
EAP
EAP
EAP
EAP
EAP
EAP
55
55
56
56
56
56
56
56
56
56
56
57
57
57
58
58
58
58
58
58
58
58
58
58
58
58
58
58
59
59
59
59
59
59
60
61
61
61
61
61
61
207
209
201
202
203
204
207
208
209
211
213
207
209
210
204
205
206
208
209
210
213
215
216
220
221
222
223
225
205
208
209
216
•219
221
211
201
203
205
212
213
214
0.001
0.
0.024
0.026
0.019
0.035
0.
0.033
0.19t
0.
0.021
0.030
0.027
0.029
0.001
0.001
0.
0.
0.
0.001
0.005
0.001
0.001
0.001
0.001
0.001
0.001
0.
0.427
0.
0.021
0.023
0.
0.
0.025
0.
0.018
0.016
0.022
0.510
0.091
+SD
0.000
0.
0.001
0.001
0.000
0.001
0.
0.001
0.018
0.
0.001
0.001
0.001
0.001
0.000
0.000
0.
0.
0.
0.000
0.000
0.000
0.000
0.000
0.000
0.000
0.000
0.
0.043
0.
0.001
0.001
0.
0.
0.001
0.
0.001
0.001
0.000
0.005
0.001
ISOTOPIC
X235
0.228
0.
2.718
2.985
2.280
3.329
0.720
3.351
21.681
0.
2.547
3.365
3.342
3.361
0.231
0.218
0.208
0.256
0.
0.229
0.724
0.230
0.231
0.236
0.242
0.236
0.228
0.
44.522
0.
2.556
2.722
0.
0.
2.879
0.701
2.959
2.402
2.557
48.855
9.249
DISTRIBUTIONS
+SD
0.003
0.
0.017
0.016
0.014
0.023
0.021
0.016
0.384
0.
0.017
0.016
0.020
0.017
0.002
0.003
0.005
0.005
0.
0.003
0.006
0.002
0.002
0.003
0.004
0.003
0.003
0.
0.309
0.
0.017
0.014
0.
0.
0.015
0.010
0.017
0.016
0.014
0.112
0.032
X236
0.003
0.
0.008
0.018
0.007
0.044
0.
0.045
0.031
0.
0.004
0.008
0.008
0.008
0.005
0.003
0.003
0.004
0.
0.005
0.
0.004
0.005
0.006
0.006
0.005
0.005
0.
0.
0.
0.003
0.004
0.
0.
0.017
0.
0.016
0.010
0.013
0.11 I
0.026
URANIUM
•fSD
0.000
0.
0.000
0.000
0.000
0.001
0.
0.001
0.010
0.
0.000
0.000
0.000
0.000
0.000
0.000
0.000
0.000
0.
0.000
0.
0.000
0.000
0.000
0.000
0.000
0.000
0.
0.
0.
0.000
0.000
0.
0.
0.001
0.
0.001
0.001
0.000
0.002
0.001
X238
99.768
00.000
97.251
96.971
97.694
96.592
99.280
96.570
78.098
00.000
97.429
9/5.597
96.623
96.602
99.764
99.778
99.789
99.741
00.000
99.766
99.271
99.765
99.763
99.757
99.751
99.758
99.766
00.000
55.051
00.000
97.419
97.251
00.000
00.000
97.079
99.299
97.008
97.573
97.409
50.524
90.634
+SD
0.003
0.
0.017
0.016
0.014
0.023
0.022
0.017
0.384
0.
0.017
0.016
0.020
0.017
0.002
0.003
0.005
0.005
0.
0.003
0.006
0.003
0.002
0.003
0.004
0.003
0.003
0.
0.310
0.
0.017
0.014
0.
0.
0.015
0.011
0.017
0.016
0.014
0.113
0.032
57
-------
APPENDIX F-3.
URANIUM ISOTOPES FROM MASS SPECTROMETRY RESULTS,
ENVIRONMENTAL AIR SAMPLES. (concluded)
IDENTIFICATION JS234
EAP 61 218 0.296
EAP 61 220 0.335
EAP 61 221 0.021
ISOTOPIC DISTRIBUTION OF URANIUM
+SD %235 +SD S236 +5D %238
0.003 28.616
0.004 34.162
0.000 2.572
0.078 0.077 0.001 71.011
0.098 0.088 0.002 65.416
0.013 0.005 0.000 97.402
+SD
0.079
0.098
0.014
ISOTOPIC DISTRIBUTION OF URANIUM
IDENTIFICATION %234
3CL62
BCL62
BCL62
BCL62
BCL62
BCL62
BCL62
BCL62
+SD %235
+SD S236
+SD 5S238
+SD
1
1
1
2
2
2
3
3
207
209
213
201
208
214
203
204
0.125
0.032
0.038
0.039
0.079
0.009
0.037
0.012
0.011
0.002
0.000
0.005
0.001
0.007
0.001
0.000
11.743
4.040
4.030
3.976
7.822
2.716
4.003
1.650
0.657
0.018
0.011
0.070
0.099
0.087
0.012
0.040
0.035
0.
0.004
0.005
0.021
0.
0.004
0.009
0.007
0.002
O.OOO
0.004
0.000
0.005
0.000
0.000
88.098
95.928
95.929
95.981
92.078
97.275
95.955
98.329
0.653
0.018
0.011
0.075
0.100
0.096
0.012
0.041
58
-------
APPENDIX G. PARTICLE PHOTOGRAPHS
CONTENTS
Page
Explanation of Electron Microprobe(EMP) Imaging 60
Figure Gl. Particle V000864-702(B) 61
Figure G2. Particle V000867-514, 515 62
Figure G3. Particle V000867-712, 724 63
Figure G4. Particle V000867-720, 723 64
59
-------
EXPLANATION OF ELECTRON MICROPROBE (BMP) IMAGING
Electron images and X-ray images of the particle were recorded photo-
graphically to determine the spatial distribution of several elements in the
specimen. The black and white photographs (3 in each case) were then photo-
graphed on a Polaroid qolor print using the additive color separation process
with the three primary color filters. The color composition is interpreted in
the following manner:
Where red and green overlap: YeJLlow will be recorded
Where red and blue overlap: Magenta will be recorded
Where green and blue overlap: Cyan will be recorded
Where red, green and blue overlap: White will be recorded
60
-------
Figure Gl-A. Particle V000864-
702(B); photomicrograph.
Figure Gl-B. particle V000864-
702(B); TEM* photograph
Figure Gl-C. Particle V000864-
702(B); EMP Scan. Red: Zr; Blue:
U; Green: Fe
*Transmission Electron Microscope
61
-------
Figure G2-A. Particle V000867-
514, 515. Photomicrograph
Figure G2-B. Particle V000867-
514, 515. TEM photograph
Figure G2-C. Particle V000867-
514, 515. BMP Scan. Red: Pu;
Green: Fe; Blue: U
62
-------
Figure G3-A. Particle V000867-
712, 724. Photomicrograph
Figure G3-B. Particle V000867-
712, 724. TEM photograph
Figure G3-C. Particle V000867-
712, 724. EMP Scan. Red: Pu;
Green: Si; Blue: U
63
-------
Figure G4-A. Particle V000867-
720, 723. Photomicrograph
Figure G4-B. Particle V000867-
720, 723. Scan. SEM*
Figure G4-C. Particle V000867-
720, 723. EMP Scan. Red: Pu;
Green: Si; Blue: U
*Scanning Electron Microscope
64
-------
TECHNICAL REPORT DATA
(Please read Instructions on the reverse before completing)
1. REPORT NO.
EPA-600/7-77-079
3. RECIPIENT'S ACCESSION-NO.
4. TITLE AND SUBTITLE
CHARACTERIZATION OF EMISSIONS FROM PLUTONIUM-
URANIUM OXIDE FUEL FABRICATION
5. REPORT DATE
July 1977
6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
E. W. Bretthauer, A. J. Cummings and S. C. Black
8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
Environmental Monitoring and Support Laboratory
Office of Research and Development
U.S. Environmental Protection Agency
Las Vegas. Nevada 89114
10. PROGRAM ELEMENT NO.
INE625
11. CONTRACT/GRANT NO.
12. SPONSORING AGENCY NAME AND ADDRESS
U.S. Environmental Protection Agency-Las Vegas,
Office of Research and Development
Environmental Monitoring and Support Laboratory
Las Vegas, Nevada 89114
13. TYPE OF REPORT AND PERIOD COVERED
14. SPONSORING AGENCY CODE
EPA/600/07
15. SUPPLEMENTARY NOTES
16. ABSTRACT
To develop accurate monitoring techniques for the radioactive emissions
from new types of nuclear facilities, it is necessary to characterize those
emissions as completely as possible. The first facility selected was a mixed-
oxide fuel fabrication plant. In-stack, standard hi-vol, and special ultra-
high volume air samplers were used to collect particulate samples at the
Babcock and Wilcox plant in Parks Township, Pennsylvania.
The number of radioactive particles emitted, the particle sizes, plutonium
and uranium isotopic content, and the concentration of other materials were
determined. These characteristics are used to propose an appropriate air-
monitoring technique for facilities of this type.
7.
KEY WORDS AND DOCUMENT ANALYSIS
DESCRIPTORS
b. IDENTIFIERS/OPEN ENDED TERMS C. COSATI Field/Group
Isotopes
Nuclear power plants
Particle physics
Plutonium
Radiation chemistry
Radioactivity
Uranium
Plutonium-Uranium Oxide
Babcock & Wilcox
Fuel fabrication
04A
07E
18B
18E
18H
20H
8. DISTRIBUTION STATEMENT
RELEASE TO PUBLIC
19. SECURITY CLASS (ThisReport)
UNCLASSIFIED
21. NO. OF PAGES
76
20. SECURITY CLASS (Thispage)
UNCLASSIFIED
22. PRICE
EPA Form 2220-1 (9-73)
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