A TWENTY-SEVEN YEAR STUDY OF SELECTED LOS ALAMOS

ti&.
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LA-5148-MS
informal
UC-41
Report
& 48
ISSUED:
January
1973
Ioslalamos
scientific
Laboratory
of the University
LOS ALAMOS,
NEW
of California
MEXICO
87544
4\
A Twenty-Seven
Year
Los Alamos
Study
Plutonium
of Selected
Workers*
by
L. H. Hempelmann
**
C. R. Richmond
G. L. Voelz
Work
done by:
E. E. Campbell
W. D. h/10ss
P. N. Dean
D. F. Peterson
C. R. Richmond
J. W. Healy
L. H. Hempelmann
●
G. L. Voelz
*
H. O. Whipple
J. N. P. Lawrence
M. F. Milligan
●Work
supported
Research
●*Department
Rochester,
Contract
by the US AEC
AT-30-1
of Radiology,
Rochester,
New
Division
of Biomedical
(4284)
to the University
School
of Medicine
York.
and Environmental
of Rochester.
and Dentistry,
University
of
,,
I
..
TABLE OF CONTENTS
E&
iii
PREFACE
I.
INTRODUCTION
II.
SAFETY
III.
PLUTONIUM
CONCERNED
PROBLEMS
OPEIUTIONS
WITH PLUTONIUM
CAUSING
1
PROCESSING
5
HEAVY EXPOSURES
5
A.
Recovery
B.
Purification
Operation
8
c.
Fluorination
Operation
9
D.
Reduction
Iv.
EXPOSURE
v.
CLINICAL,
VI.
1
Operation
10
OF THE SUBJECTS
LABORATORY,
A.
Medical
B.
Plutonium
c.
Determination
D.
Chromosome
E.
Cytology
CONCLUDING
9
Operation
AND RADIOACTIVITY
12
OBSERVATIONS
12
Observationa
Body Burdens
by Urine Assay
13
in the Body by In Viz)o Measurements
15
as Determined
of Plutonium
18
Analysis
of Exfoliated
Bronchial
19
Cells
19
REMARKS
ACKNOWLEDGMENT S
19
REFERENCES
20
APPENDIX
A —
APPENDIX
B -- URINE ASSAY METROD AND ESTIMATION
APPENDIX
C -- MEDICAL
APPENDIX
D -- PADIATION
DECONTAMINATION
PROCEDURES
FOLLOW-UP
AND RESPIRATORS
OF PATIENT
DETEC310N
EQUIPMENT
USED AT LASL IN 1944
24
OF BODY BuRDEN
29
NO. 2
FOR IN VIVO MEASUREMENT
22
OF PLUTONIUM
31
...
., .
:’$”
.!.’
ii
PREFACE
This
Alsmos
report of the health
plutonium
Lsoghsm
workers
was inspired
and is dedicated
keen interest
of war-tine
is known
as one of the if not the world’s
nium biochemistry
and toxicity,
arose.
countries
whenever
Hia ultimate
toxicity
of plutonium
tion, he organized
subjects
authority
enthusiasm
been responsible
circulation
in these Newsletters
for the excellent
the UFPU Club members
of friendly
the humor
and
that haa
cooperation
classified
of
war-time
in plutonium
death.
In fact, en early
and a nmrber
reports
con-
of now de-
on plutonium
experiences
were with him at the time of the fatal plane
Although
Wright
interpretation
1972.
suffers
He kept in close touch with
interest
tinued until his untimely
cussions
of the
intense
draft of this manuscript
enormously
problems
of course, was the
It was undoubtedly
expressed
on pluto-
in man and, in this connec-
by periodic
UPPU Newsletters.
and,
as well as those
the UPPU Club composed
of this study.
the Club nembers
to everyone
plutonium
concern,
H.
Wright’s
he was the first to
be called upon by our government
of other
by Wright
to his memory.
in plutonium
Wright’s
Los
died before
he could write
of the present
to the report
of the subject
Although
data, he contributed
in the course of disduring
we are well
the authors have
report
of which
effort
to make the report
story, which
the winter
Wright’s
direct
tried to write
he would have been proud.
into a personal
it was to Wright,
mSUY of the anecdotes
of 1971-
aware that the study
greatly by not having
ticipation,
crash.
his
par-
a
In an
living
we have included
that Wright
loved
to tell.
in this study.
iii
A TWENTY-SEVEN
YEAR STUDY OF SELECTED
Compiled
L. H. Hempelmann,
LOS ALAMOS
and Written
C. R. Richmond,
PLUTONIUM
WORKERS
?
by
and G. L. Voelz
ABSTRACT
Twenty-five male subjects who worked with plutonium during World War II under extraordinarily crude working conditions have been follwed
medically for a period of 27 years.
Within the past year, 21 of these men have been examined at the Los Alamos Scientific LabIn addition to physical examinations and
oratory, and 3 more will be studied in 1973.
laboratory studies (complete blood count, blood chemtstry profile, and urinalysis), roentThe chromosomes of lymphocytes
genograma were taken of the chest, pelvis, knee, and teeth.
cultured from the peripheral blood and cells exfoliated from the pulmonary tract were also
Urine specimens assayed for plutonium gave a calculated current body burden
studied.
(excluding the lungs) ranging from O.005 to 0.42 l.ICi,and low-energy radiation emitted by
internally deposited trsnsuranic elements in the chest disclosed lung burdens probably of
less than approximately 0.01 LICi. To date, none of the medical findings in the group can
The bronchial cells of several
be attributed definitely to internally deposited plutonium.
of the subjects shcwed moderate to marked metaplastic change, but the significance of these
Diseases and physical changes characteristic
of a male population
changes is not clear.
Because of the small body burdens on the order
entering its sixth decade were observed.
of the maximum permissible level in these men so heavily exposed to plutonium compounds, we
conclude that the body has protective mechanisms which are effective in discriminating
This is presumagainst these materials following some types of occupational exposures.
Plutonium is more toxic than
ably explained by the insolubility of many of its compounds.
&
radium if deposited in certain body tissues, especially bone; however,
point of view, plutonium seems to be leas hazardous to handle.
I.
11.
INTRODUCTION
This is the story
heavily
Alsmos
exposed
Scientific
Mexico)
of hw
at what
Laboratory
ia now the Los
(at Los Alsmos,
in the days of the Manhattan
Project
World War II and of what has happened
the subsequent
jects
were
27 years.
of this study were
drafted
Engineering
Detachment
college
All were sent to Los Alamos
istry and Metallurgy
capacities,
Research
they were engaged
atomic bOmb.
of plutonim
for plutonium
ranged
Almost
during
Glenn Seaborg.
majors who
Division.
In an effort
In these
pluto-
of the first
all of these subjects
estimated
had body
from the urine assay
used at Los Alamos
before
element which
2
He was
of exposure
of plutonium
toxicity
caused bone
cancer
properties
in man after
in the radium
in the body.
about the biological
of plutonium
to avert another
in the 1920’s),
(and, hope-
disaster
dial painting
Seaborg
Berkeley,
1950 that
tion.
from 0.1 to 1.2 Ugl (0.006 to 0.08 I.ICi).
basic
of the Crocker
California,
Thanks
Radiation
industry
to Joseph
Laboratory
for biological
to Seaborg’s
facts related
such as
gave about 10 mg of pluto-
nium out of the first half gram produced
Hamilton
and
of the latter
quantities
to learn more
thereby
happened
to plutonium
aware of the similarity
properties
of microgram
and metabolic
fully,
danger
and of the extreme
Project.
in processing
and testing
radium
deposition
jobs in the Chem-
WITH PLUTONIUM
early in 1944 by its discoverer,
of the radioactive
to a Special
(Project Y) in 1944 or
technical
nium prior to fabrication
burdens
science
of the Manhattan
1945 and given various
was recognized
All but a few of the sub-
into the Army and assigned
The potential
New
to them in
CONCERNED
PROCESSING
25 young men were
to plutonium
SAFETY PROBLEMS
from the practical
foresightedness,
to the biology
in
experimentamany
of plutonium
1
.
.. . . .
.
,.
.,
were
known when
material
arrived
However,
ical hazards
them were
of plutonium
and to protect
different
matters.
could be established
in the radium dial paint plants,
of magnitude.
(Milligrams
plants were subjected
whereas
ties of plutonium
were
and metallurgical
manipulations.)
plutonium
was carried
and Metallurgy
Fig. 1).
effect
clothing
two changes
and surgical
on leaving
chemical
Chemistry
(see
put into
laundered
caps
the building);
attached
apprised
to surgical
and were
rare exceptions,
it was difficult
coveralls,
lurgists,
available
efforts
It is a matter of interest to modem
day plutonium
workers that the air entering the D Building was
cleansed of dust by electrostatic precipitation
methods.
However, air leaving the building was unfiltered for the most part, since few, if any, of
the exhausts even from plutonium-containing
hoods
had filters.
methods
Appendix
to the bes
the tension
and
of safety
i
rules.
of plutonium
first
chemists
and metal-
to live with what was
considered
levels were hampered
alpha counters
by
and continHov
had not yet been developed.
of the urgency
of the times, work
had to proceed,
primitive
A).
With
rules.
the first atomic
quantities
of monitoring
believably
fully
to avoid some shortcuts
to be safe contamination
ever, because
were
(as they were
cooperated
during
to Los Alamos
the fact that portable
with plutonium
i
and chem-
to sign a statement
and enforcement
uous air samplers
*
required
the workers
When milligram
Sometimes
All workers
of plutonium
of developing
the observation
canva:
(not made of stainless
feverish
weapons
system
system,
abide by the safety
activity
750
plutonium
rubberized
gloves).
although
became
(b) use of
with
of their ability,
areas with
(all persons
involving
to use a closed
they would
(Wilson
use of closed
dryboxes
of the hazards
then known)
saying
change of street
to the contaminated
per day of freshly
canvas bootees,
showered
in
All work with
regulations
procedures
possible,
steel in the early days).
quanti-
called “D Building”*
safety
(a) a complete
on entrance
in complex
out in the wooden
Building
Stringent
included
involved
kilogram
all chemical
ical hoods had to be used
by
to simple mechanical
at Los Alamos
gloves and respirators
and (c) whenever
sleeves
but
of radium
du~ing
rubber
was impractical
of
in the two cases differed
surgical
(at first, homemade
Safety
on the basis
problems
operations,
biolog-
against
experience
watch
of the
in the spring of 1944.
protection
many orders
,.
at Los Alamos
samples
to be aware of the potential
two entirely
regulations
,.
.,, .,
‘.., .,,
the first milligram
Because
and improvised
and decontamination
by today’s
stationary
were un-
standards
(see
counters
were
the
only means of detecting alpha particles from plutc
**
it was necessary to make “swipes” with
nium,
lightly
oiled
filter paper of the laboratory
faces considered
and to bring
hl.
Ii
portional
cident)
for counting.
on a daily basis
per laborato~).
(approximately
more
strips
in each laboratory
(6 swipes
,“
....
to the alpha proThis was done
(or after an ac-
containing
plutonium
Any “swiped”
6 x 6 in.) having
than 500 counts
sur-
likely to be contaminated
these paper
counter
systematically
most
per minute
area
an activity
of
required
..
**
.,
Fig. 1.
The original wooden D Building which housed
the chemists and metallurgists
in CMR
Division.
Note that the ~emical
hoods of
the laboratories on the first floor were
vented individually, usually without filtration.
There was a semi-portable
counter called Pluto
first available in March 1Q44, but it was very
bulky and its limlt of sensitivity was 5000 count
per tinute.
A more sensitive yet still cumbersom
counter called Supersnoop came into use in March
1945, but it was not until the instrument called
Eoppy became available in June 1945 that the monitoring situation really was under control.
Hand
counters were not available until October 1944,
when che first experimental models capable of
detecting 200 counts per minute were installed ic
the locker rooms.
,,1, >
.“*.
2
***
It is difficult to believe but,
~econt.mination.
~ecause of the bulkine~~ ad inconvenience
Of the
early
so-called
counters,
portable
the swipe tech-
nique of ~OnitOring was continued
oratories
absence
until June
first became
nostrils
avail~le
for radioactive
dusts
(the
‘n ‘he ‘all ‘f 1944)’ both
,,
worker were “swiped
with
rolled moistened
strips
of filter
at the end of the working
cidental
These
pulmOnary
samples
exposure
breakage
of safety
accidental
regulations
1945, kilogram
from the newly
operating
at Los Alamos
time portable
Hanford
air samplers
help with monitoring
lines in som
boxes,
(Fig. 2) ~d
equipment,
laboratories
positive-pressure
Fortunately,
were
masks,
most procedures
contin-
carried
to
of certain
including
also had been
Fig
A semi-portable
alpha counter called
“Supersnoop” used in early 1945.
2.
by this
available
and specially
were
to
and fabrication
for contamination
Operating
laboratories.
of plutonium
piles began
for processing
alpha counters
operating
Although
or
(e.g., hand con-
quantities
into the first atomic bombs.
UOUSly
inhalation
of the nostrils).
In April
arrive
the subject was questioned
about possible
tamination
in a stationary
If the nose swipe exceeded
counter.
50 counts per minute,
carefully
day or if at****
wss suspected”
were also counted
alpha particle
air
urine
assay method
this allowed
plutonium
pounds
for plutonium
crude estimates
to be made
in the lung).
4
had been developed;
of the body burdens
(not including
However,
insoluble
of
com-
even with improvements
made
imprOved.
out in dry–
some work had to be done in open hoods
(Fig. 3).
This was particularly
of the Recovery
so diverse
were
in the
of each plutonium
routinely
paper
1945.
of air samplers
in some lab-
Similarly,
Group,
and unstandardized
totally
true in the case
the activities
inoperable. 3
of which were
that closed
Also by March
systems
1945, a
***
The swipe technique ~asured
only alpha particleemitting materials not fixed to the surface.
Oil
on the filter paper used for surface swipes probably
decreased so~what
the treasurable alpha activity.
The moistened paper strips wed
for nose counts were
dried before counting; consequently,
the measured
activity was probably ~re
accurate than that of
the oiled swipes.
The geomtry
of the stationary
proportional
counter was relatively good, approaching 50 percent.
In contrast to poorly fixed radio- o
activity measured by the swipe technique, portable
counters developed later measured fixed as well as
unfixed radioactive contamination with a rather
poor geometry (10 to 15 percent).
****
The nose counts and air counts (at first one
sampler in the most hazardous laboratory) were bv
..
–,
no means accurate measures of exposure of personnel.
At best, they were merely crude indications that
permissible contaminatio~
levels had been exceeded
or that safety regulations might
have been violated.
Fig. 3.
One of the steps in the purification
operation performed in an open chemical hood.
The operator is wearing the standard protective clothing and respirator (Wilson
750) .
,
3
. .
in monitoring
deplorable
after
techniques,
by present-day
working
initial bomb processing
August
conditions
standards.
were
Fortunately,
was completed
1946, all work with plutonium
20
I
Odginolcountz
in
was sharply
-–J~
curtailed
until
the new and greatly
ities at DP Site in Los Alamos
September
To illustrate
a few almost
various
reports
the maximum
plutonium
-, .
,MaithÒ
the degree
in D Building
present
oratories
were opened
facil-
in
1946.
laboratories
per minute
improved
random
issued
in D Building
isotope
experiences
at the time.
and minimum
correspond
of contamination
“swipe”
taken from
Table
counts
in March
to 0.007
mixture
of
in 1944 and 1945, we will
1944
[500 counts
Pg or 0.0004
of that ti=;
I shows
in all lab-
Pci of
note the
I
,
~~fter
t
,
!
deconf:minatlon
~he percent
of laboratories
WI,Lci) radioactivity
in June and July 1944 in
levels
(ss measured
.~eru above 5000 counts per minute
>W
or were between
Table
and 5000 counts per minute.
l,i~llnose counts
~hree chemists
but below
1945, 1243 “hOt”
mostly
Group
number
were
of decontamination
procedures
1980, 3489 (of which
reader
cOunters,
In June, July, and August
per minute),
worked
with
monitoring
overtime
1945, the
however,
were
out
30,000
Lest
cOunts
the
lax or care-
to maintain
the safety
41 persons
standards
Pressures
available.
to
factory,
safety measures
admittedly
in March
Metallurgy
Division,
periods,
of plutonium.
the staff worked
Fortunately,
unsatis-
OPERATIONS
CAUSING
HEAVY
EXPOSURES
Twenty-three
of the 25 living exposed sub******
Plutojects
worked in four operating groups:
nium Purification
orination
metal),
(wet chemistry),
(dry chemistry),
and Plutonium
Plutonium
Plutonium
Recovery.
Because
was by far the most hazardous,
described
first.
and Metallurgy
mitted
as well
Research
in 1944 and 1945
as references
much of the material
interviews
12-hour
(mny
A.
it will be
Divisions
sub-
still classified),
3 and 5, are the source
in this section.
with the subjects
Extensive
and their
monitors,
of
supervisors,
provided
sup-
Fourteen
body burdens
Operation
between
March
worked
in the recovery
1944 and September
1946.
shifts
A suite of three laboratories
laboratory
pressure)
D-117.
These
steel hoods
were equipped
masks were not entirely
satisfactory
personnel
contamination.
Kennedy-Hinch
included
airborne
in protecting
made mask
Group
residues;
crucibles
washings
scraps,
composed
shavings,
and
of various
materials
materials
spills
materials;
graphite
and drybox
and chemical
tions
(supematant
of PuF G; absorbent
taminated
considerable
materials
for processing
analysis;
ing basic procedure
good protec-
steps in the wet purifica-
metallic
used in the reduction
After
Not until
(called the
radioactivity.
from various
tion of plutonium;
air
after its designers)
analytical
trimmings;
with
was there comparatively
to the Recovery
solutions)
Although
positive-pressure
The types of plutonium-containing
submitted
had
*******-
mask,
was developed,
tion against
a specially
the
of the ordinary
used in D-117.
available
from airborne
(main-
laboratories
instead
hoods previously
July 1945, when
7 days a
had replaced
lines, the commercially
of the 25 subjects with measurable
of plutoniu
to handle
peak work
in use in an annex of the old D
used to wipe up accidental
information.
Recovery
operation
the last
began
Building.
open stainless
and
During
were
of the Chemistry
and Health
as well as with the health
plementary
reports
(to
Reduction
operation
Monthly
Flu-
of increased
by this time new laboratory
two of these laboratories
PLUTONIUM
III.
first with
of plutonium;
facilities
chemical
of the times.
and sub-
by the Chemistry
the Laboratory
quantities
and
metal.
1945, as a result
kilogram
single
or
to the +4
Group dealt
being processed
tained under reduced
the bomb were so great that work had to pro-
ceed using the best, although
to plutonium
and later with gram amounts
quantities
week.
that a large, well-
staff of approximately
the crude mthods
build
were decon-
plutonium
for fluorination
In 1944, the Recovery
milligram
76o exceeded
think that the operations
reduction
in any
procedures
or lost as contamination,
the recovered
valence state suitable
sequent
left behind
or operational
accidentally
(b) converting
responsi-
of the then priceless
which had been either
of the experimental
spots,
carried
and 5347, respectively.
less, h< should be advised
trained
In April
with the follnwing
(a) recovery
plutonium
spilled
of
consistently
50 counts per minute).
by pOrtable
the
(other nose
(over 500 counts per minute)
detected
taminated.
II shows
(over 50 counts per minute)
in the Recovery
counts of these men not included were
,,osltiW
by swipes)
This group was charged
bilities:
and other con-
tubes used in oxygen
hood sweepings.
experimentation,
was adapted
(see Fig. 5)********:
the follow-
for recovery
(a) soluble
opera-
salts of
*******
******
These men were the charter members of the UpPU
Club formed by Wright Langham when this study began
in the early 1950’s.
In essence, the acronym represents the phrase “you excrete plutonim.”
The
name was originally IPPU, but Langham decided this
was too per~Onal.
The late Joseph W. Kennedy
CMR Division.
was the leader of
*******
It should be mentioned that not all of the
recovered plutonium went through the entire procedure.
Depending upon the chemical nature and purity
of the plutonium being recovered, various steps of
the total procedure were omitted.
,.
5
TA8LE
EXAMPLES
OF SUBJECTS
11
WITH NOSE COUNTS
ABOVE
a
Date
Nose CountS
Date
——
Nose COuntSa
50 CO~TS
PERMI~E
Subject
subject
6
7
9
10
11
12
13
14
16
17
23
25
8-17-45
20
23
24
acounts
b
-144
188
207
717-408
174-113
73-27
196-172
421-41
122-107
138-129
62-22
101-67
250-87
930-82
272-174
163-43
267-131
177-118
170-165
504-416
246-514
720-501
2559-3111
199-150
320-200
126-78
608-94
68-50
217-182
336-316
394-182
324-182=
218-122
486-152
128-108
92-56
520-394
1096-329=
64-80
1oo-80
100-60
148-130=
96-76
100-96
70-66
64-52
696-90
144-48
88-26
76-60
per minute
Only one nostril
cAccidental
6
Of activity
swabbed.
exposure
suspected.
5
6
7
9
10
11
12
14
16,
17
18
19
23
24
25
26
8-13-45
20
27
9-12-45
14
17
5- 8-46
6-17-46
swiped
No. 9
No. 8
6- 2-45
4
5
6
7
9
11
12
13
14
15
16
18
19
20
22
23
7- 2-45
4
175
199
207
4-17-44b
28
7-19-44
IO-12-44
11- 7-44
12-29-44
4-20-45
5- 8-45
15
16
18
19
21
22
29
31
6- 4-45
5
6
7
9
14
15
16
18
19
20
23
25
26
27
7- 2-45
4
5
..
S&ject
No. 5
Nose CountSa
Date
88-26
216-100
231-213
20-60
291-201
286-89
1181-323
454-385
1107-1292
509-229
623-560
1208-680
146-92
928-615
1506-1009
1898-1100
90-23
400-274
164-170
236-9 7C
324-126
198-118C
338-278
268-72
1016-694
484-304
2s0-247
198-166
356-328
364-328
462-410
752-545
179-183=
941-243
898-816
322-160
166-154
768-652
124-56
202-100
300-136
106-78
165-107
136-72
52-825
168-401
from each nOstril”
6-28-45
29
30
7- 2-45
3
6
9
10
11
23
25
30
31
8- 2-45
3
4
6
3727146
562-98
698-66&
70-64
208-140
112-80
1164-608
608-626=
57-50
879-706
838-842
1296-306=
2.64-408
3040-464
2086-482
8976-5180
660-204
674-530
3922-1752
,,
as the peroxide
of H O . The plutonium
22
(4 valence state)
by addition
oxide was converted
to nitrate
and was given to the Dry Chemistry
orination.
Group
for flu-
Late in 1944, the dilute supernatant
“w,
solutions
s,!’..!
Am..
M,C+Y.,C.1 1
were
reduced with
treatneot with A1(OH)3.
S02 and precipitated
In December
process was turned over to another
by
1944, this
group
(~-lo).
Iwo,
I
d 6,..,
I sol’.
In retrospect,
J
?,<mmtes
MM.OH
m *S*
E..
1
greatest
1
w dPvO.!.8W-’.’-d
-.LG
n.a.,Tc.
.,v..
F..
.wzr.1~
1
added
it may be reasoned
exposures
occurred
(with vigorous
tions of plutonyl
Although
stirring)
nitrate
this procedure
hood in 3-liter
(1 to 40 grams per liter).
cooled beakers,
~h’
RIO,
pii’q..w
[
I
J
Mo.sa,m!a
P“-:i-,
(lhQ
N&O.
S.r,,
rm,..! 1:
.-.P.
‘‘N’”NEa-
[
[PwOH).
.lZr.Th)
H0;
‘i
NLMo,
P“%--C*,U,Th,Zrl
‘O’” -
(
handled.)
-
f
P“D,-.
.(&L<Th2d
1
qp-TfpEm%%-Rwp
.
‘i
GGm
c+3-
10%lfmalmm-
procedure,
wearing
of high nose counts
in-
step was added to
but this also coincided
amounts
-b
Pdfl.
aoan
—1.
The addition
of dilute
supematant
of plutonium
in
being
of NaOH to the large vats
solution
liter) also caused heavy
spattering.
Because
(0.1 to 1.0 gram per
fogging
and occasionally
of the size of the 50-liter
Fy:J.
containers,
this procedure
open laboratories
3
Flow sheet for the recovery operation.
This gi=s
the general outline of the
procedures used, but each individual
recovery operation required special conditions.
Fig. 5.
out by workers
(The number
creased sharply when the peroxide
the recovery
into the air
and May 1945, this pro-
1
8*.,9,4,,
rkbalk?.)1
my.
respirators.
out in an open
there was consider-
of droplets
In April
time with the increasing
mk:3P#
[
the hood.
cedure was often carried
Wo,
to high concentra-
was carried
able fizzing and discharge
outside
that the
in step e when H202 was
without
cheorlcal steps which
were
concentrating
benefit
caused
dilute
ashing combustible
especially
was carried
of hoods.
airborne
solutions
materials;
those involving
out in the
Other
contamination
by boiling;
and fusion procedures,
sodium peroxide
plus
carbon or persulfate.
As might be expected,
plutonium
salts
were dissolved
directly
(oxides or carbides)
acid after persulfate
nium was precipitated
nium hydroxide
itated
digsolved
fusion;
with NaOH or ~40H;
(d) plutonium
HN03 and oxidized
in HC1; insoluble
were
or carbonate
was dissolved
as the oxalate
agents;
&SO
in HNO
3
in the presence
that used in the purification
(steps d and e) , which
nitrate)
of reducing
involved
similar
to
during the closing
contributed
of these occurred
batch
purified
plutonium
3.6-gram
aliquot
placed
into ether and
state and precipitated
was being
of plutonyl
processed.
and the concentrated
solution
was
auction,
from the contaminated
from the floor.
to Soxhlet
spilled
rebroke
on the floor.
by mechanical
plutonium
asphalt
extrac-
the thimble
aspirated
and the remaining
An initial
in solution,
As it was being
the glass tray supporting
The spilled material
the first 8-gram
at that time) of
nitrate
prior
in an oven.
undoubtedly
The most dramatic
supply
in a glass thimble
extraction
and
entire
the Recovery
which
in May 1944 when
(the world’s
of
that prevailed
days of the war,
to the exposures.
tion, was heated
iodide
in the atmosphere
and fatigue
Group had its share of accidents
moved,
and (f) after April
was extracted
tension,
described
of ammonium
reduction with
to the tetravalent
in
state by treat-
process
the presence
as the oxalate;
1945, the plutonium
reduced
(in
and subsequent
precipitation
(c) pluto-
oxalate was redissolved
to the hexavalent
from acid solution
(b) pluto-
and precip-
ment with Na8r0 ~; (e) ether extraction
Inter
in
excitemnt,
was recovered
tile slabs torn up
When recovered
and purified,
this
7
. .< .. .
,.
.,
material
was combined
plutonium,
was placed
the hydroxide,
While being
spilling
into the centrifuge
into the centrifuge
recovered
tion.
*********
Better
washing
Surprisingly,
made, but it will be SO=
the in-
be appreciably
protective
studies
to these spectacular
there were also occasional
(up to 50 liters)
of dilute
trated
.,
solutions
plutonium
were handled
objects;
case, the excised
carrying
tissues
contained
One other man burned
activity.
out the carbon-sodium
of a new
the ventilation,
installa
The situation
sinks, etc.
is st
however.”
All 14 subjects were
steel
indicated
removed
in the summe
that their body burdens
or had exceeded
in each
the then maximum
(7 counts per minute
little radio-
suggesting
his hand while
perOxide
with a nu
1945 from this type of work because
cut their hands
fortunately,
the haza
(5
concen-
in stainless
Four of the 14 subjects
hoods .)
with contaminated
solution
(The smaller
critical,
time before
are be
except by the use of be
such as installation
on improving
incr~
quickly.
of product
CM-1 has helped
devices.
of foot-pedal
accidents,
spills of large volumes
to 10 mg) onto the floor.
reduced
of improvements
very little plutO-
is being
must be obtained
in the handling
was
nium was lost in these two accidents.
In addition
The air pressure
respirators
Improvements
with a dilute acid sol*-
“
but an in,
by cM-12 has failed to show appreciab:
contamination.
cup and
The plutonium
itself.
once again by repeatedly
side of the centrifuge
tigation
in the form of
in a centrifuge tube.
*********
the tube broke,
centrifuged,
the sample
tion of the air lines was suspected,
with more newly purified
and the 8-gram sample,
fusiOn
B.
were
approac
permissible
per 24-hour urine
a body burden
Purification
urine assz
1
specime
of 1 lJg or 0.06 xi).
Operation
procedure.
Aa might be expected,
spring
and summer
caused
exposures
during
great concern
Three of our subjects
the late
about the
Division.
health
of these workers.
from the Monthly
The following
istry and Metallurgy
Progress
excerpt
Division
is
for May 1945 (issued
produced
Because
impurities
in the recovery
much worse
to the great increase
being processed.
chemistzy
Because
shutdown
is
counts
on removing
as well as increase
,“
....
every effort
the health
altered
.,.
,
.- ..
.
hold-
situation.
Forced air respirathey have not
the nose counts yet.
Contamina-
*********
The reason for the accidents presumably was
the unsuspected radiation-induced
fragility of the
glass vessels used in these procedures.
It was
believed that alpha particles alone would not affect
the glass, but irradiation by neutrons arising from
interaction of alpha particles with boron in Pyrex
glass had not been anticipated.
**********
There is a story that great difficulty was
encountered in the fluorination of this ill-fated
batch of plutonium.
We have not been able to verify
this .
8
slurry
containers
diluted
received
in 160-gram
from Hanford
(cut), assayed,
considerable
On the average,
was
lots
dissolved,
and transferred
difficulty)
(some
into a closed s
these preliminary
3.3 days.
The following
ried out:
(a) reducing
iodide;
,,.
metals
is being msde to
tors have been put into use, although
materially
contaminating
of this situation
with
improve
this
of recovery will essentially
shut down purification,
up of product,
(see next section),
The flow sheet used in the purification
3
tion
until July 1945 is shown in Fig. 6. P1
mtal
and because
that nonuet
due
of product which
The trend in 24-hour urine
upward.
it was believed
procedures
nium nitrate
is definitely
the plut,
labor-
in the past month
in amount
methods
could best be removed by subsequen
concentrated
atories has become
by wet chemical
by the piles in Oak Ridge and later
Hanford.
situation
Re:
Report of the Chem-
June 1, 1945):
“The health
in the Puri”
and Metallurgy
This group was given the responsib-
of purifying
taken
worked
tion Group in the Chemistry
solving
plutonium
and dissolving
ing plutonyl
nitrate
nitrate;
nitrate
iodide
with
This product,
took
were
then
(or PUV1) nitrat
(b) precipitating PU1ll oxalate
VI
with bromate and nitric
ing amzenium
late.
procedures
PUIV
as Pu
(c) precipitating
acetate
steps
as sodium
in HN03;
and d
acid;
plutony
(d) ether ext
from the acid solution
and (e) reducing
and precipitating
recovered
pluton
as the
in about 97 pe
yield, was given to the Fluorination
reification of plutonium
c
Group.
in this form continue
;-
blowing
at an open-faced
the room, the subject
This man is well
off-scale.
;ed.
ionization
a body burden
I
chamber
across
could cause the needle
tO go
today and did not have
of plutonium as measured
***********
by older
urine assay methods.
;
can
c.
Fluorination
Operation
!r
Three of the subjects
with measurable
body bur-
on this operation.
Their
!r
dens of plutonium
worked
)d,
job was to convert
plutonium
oxalate
(prepared by
m
the Purification
[
to oxide and then to flu-
I
I
..’,”
30,
..No,
ml.,mn
oride prior to reduction
1
nr”m”.
W,*
to the metallic
state.
,.1
l..-
“L*
N.vd,qn,o,l,
N.N03
-u,-.
HC2.30>
the spring and s~r
~
plutonium
of 1945, these men handled
in batches
of 160 grams and worked
in
Pm
[
shifts around the clock.
.
“No,
mu,a.1
Slurries
du, m
. WI, N03
%
!1s
?“02,.0312
.!.”
-1.
6 in the wet purification
!-.
[
into platinum
1
i%.t.wx!
PV021N0312
.
“,
.
H2C204
1.1.
of plutonium
oxalate
(from step 5 or
procedure)
were poured
E,,.sc!m”
R**
1
f.1,x!.vih1C2H51#
H~
boats
furnace within
and oxidized
by baking
The uncovered
a hood.
in a tube
boats,
contain-
-,.,,0,!
ing oxide in the form of a light green powder,
balance
,,
%Ezt:
,
the room to an ordinary
also in a hood.
After
boats were
Y
two large hoods with sliding
3
Flow sheet for the purification
operation.
out in D Building
until September
1945.
Y
this group handled
160-gram
batches
w
of plutonium
a-
in June,
hazards
totaling
the Recovery
cipitates)
ardized
1945, 5.69 kg
end 9.2 kg in August,
in the presence
of hydrogen
fluoride
fluoride
was weighed
The nature
supematsnt
of the operations
solutions
from pre-
was such that they were quickly
and carried
out in relatively
stand–
simple
closed
m.
The body burdens
systems .
of the 3 subjects
in
t
this group were
the Recovery
consequently
Group.
th
sures did occur.
10 mg of plutonium
In August
chloride
ploded while being opened
the face and mouth
lower than those in
Nevertheless,
accidental
finally was poured
and passed
expo-
1944, a vial containing
on to
the
Reduction
the form of oxalate,
occurred
Further
when the wooden
Fortunately,
such as dropping
with
powder
Group.
operadust in
Some expo-
or fluoride,
while
pro-
covered,
to plutonium
plutonium
always worn.
(i.e., by scrubbing
etc.).
oxide,
occurred
the powdered
tors were
tetrafluoride
in the fluorination
tion could have been exposed
weighing
gas and oxygen.
and, if the con-
into a glass container,
The 3 men working
sure presumably
in one of
the fluorination
Plutonium
cedure was repeated.
the
were not as great as those in
Group.
(mainly decanting
s
4.9 kg in May
6.13 kg in July,
to personnel
these
glass doors and fired
version was not satisfactory,
c
Although
being weighed,
carried back to a tube furnace
The plutonium
be carried
analytical
~
ch
Fig. 6.
were
-b,-
carried across
m
In
U,on”ow”t
N, C2M30=
If
Group)
they were
carrying
even though
exposure
or
respira-
could have
hoods were decontaminated
scouring
agents,
there were no serious
painting,
accidents
a boat in the open laboratory.
in the +4 state ex-
and heavily
of a young
chenrst.
the skin of the face was thoroughly
contaminated
Although
scrubbed
and
D.
Reduction
Operation
Three of the subjects
reduction
operation.
worked
in the metal
They developed
the methods
of
in-
the mouth
thoroughly
washed
tion of the face (estimated
out, heavy
contanrina-
plutonium
fluoride
to the metal, which was
to be 1 pg) persisted
***********
for several
days.
air,
it
was
estimated
tion
in
the mouth was of the order of 10 Dg.
t
reducing
From the ionization
of expired
that the level of contaminaBy
According to the most recent analysis by
J. Lawrence, this man does have a measurable body
He is not but should be a
burden of plutonium.
member of the UPPU Club.
——
then fabricated
into the shapes needed
in the early
were supposed
in quanti-
such a confined
the welded
atomic bombs.
Before plutonium
ties, preliminary
uranium
became
experiments
and other retallic
tors soon learned
other metallic
~tals
halides
on a small scale,
plutonium
with
were
tended to remain
than to form well
(Since the melting
separation
overheated,
out to enable
achieved
container.
plutonium
buttons
the
from the slag was first
metal
bomb” nmthod.
lithium
in a refractory
PuC13
This was welded
centrifuge,
rotated.
in favor of the “stat:
was discontinued
which
Good cohesive
it was easier,
suits
than the centrifugal
The principle
in the stationar}
calcium
in refractory
On heating
the bomb a strongly
tion of iodine
occurred,
efficiency.
war.
ried out in dryboxes.
All loading
on, disassembly
earlier
Iv.
Because
bomb.
were
small-scale
operations
a
t;
t.
wer,
the lid was bol
Moreover,
experiments.
body burden
during
A
than in
the well
fc
less dusty than those it
who developed
EXPOSURE
plutonium
of th’e bomb was easier
products
measurable
slag.
2
ignition
This became
and unloading
case of the welded
metallurgist
and the plutonium
to the charge helped
of reducing
steel bomb
exothermic/ther
from the fluid CaF
in an all-
reaction
liners made of elect rica
in argon-filled
to 11OO”C
of the bombs
method.
of PuF 4 and metal
method
were
to the
and gave better
employed
standard
May 26, 1944 (Fig. 7).
and unloading
quicker,
method was to pack a mixture
and 1–1/2 in. in
buttons
1944, thi
had been developed
where
collection
The first 500-mg metallic button of
5
almost pure plutonium
was made by this method on
loading
method
improved
electrically
body burder
In September
of argon in a
soon obtained.
Although
both have measurable
************
plutonium.
reaction
shut and placed
heated
per m-
This metallurgic:
clearly
steel bomb about 1 in. in diameter
graphite
his assistant
the n,
was 11,900 counts
the work was carr:
reduction
oxide
out in the op,
in which
separated
beryllium
carried
contaminated.
the “cen-
in an atmosphere
height.
and the laboratory
or PuF4, mixed with
cone-shaped
were
fused MgO contained
into the tip of a
to saw op
On at least two occas
On one of these occasions,
on was heavily
to be
bombs,
space.
procedures
laboratory.
bomb” method,
reac-
experiments
This was called
trifugal
while being
of
by the use of centrifugal
force to throw the molten
liner, was placed
While
causing
scale in stationary
of plutonium
cone-shaped
point
at this time, the reaction
on a larger
successfully
earth
mtal
the refractories.)
carried
or alkaline
certain
out in dry
steel bomb was difficult
count of one operator
and
slag rather
“buttens.”
was unknown
produced
The opera-
of plutonium
alkali
the reduced
vessels were considerably
tions with
carried out using
easy but that, when operating
the cindery
consolidated
were
“stand-ins.”
that reduction
was relatively
mixed with
available
to have been carried
Nevertheless,
this method
does hav
of plutonium.
OF THE SUBJECTS
By March 1945, the plutonium urinary assay
6
had been developed to the point where i(
method
could be applied
assay system
‘t,
..
I
.,
.-
Fig. 7.
10
A 500-mg metallic
plutonium.
button
of almost pure
to the plutonium
had to be extremely
workers.
sensitive,
The
as c
************
The contamination occurred during p
aration of the metallic button mentioned above.
Unbeknown to their supervisors, these workers b{
the reduction at midnight.
The next morning th(
plutonium button in an-appropriate
container wa>
allegedly found on the desk of Dr. Cyril Smith,
Associate Leader of CMR Division, and extensive
contamination had occurred throughout the labor:
and adjacent hallways.
The workers were nowher(
around but were finally located in the bar of tl
La Fonda Hotel in Santa Fe, where they were celf
brating their success in reducing plutonium by :
technique they had developed.
~-,. .,,, -.,.
:ybo>
from animal
>pen
~ ~xiw
Ision
I Jg) would
lpen
plutonim
experiments
pe~ssible
minu
~~ay
the bodies
his
mmbers
or oftener.
. .
that a person with
counts per minute
specimn).
Nevertheless,
had actually
the
been deposited
on March
of the Recovery
.-...
in
Group were assayed
To the consternation
of
monthly
of everyone,
,. .*-.
suggesting
,,
...
. .
the
. ..
. ., .,,.,
that the body burdens
urine collation
to minimize
designed
decreased
precipitously.
Table
of body burdens
of plutonium
swipes
III shows early
as well as the number
(over 50 counts per minute)
ity of all high nose counts
Although
the correlation
(see
of the urine samples
estimates
assays,
contamination
had been perfected
B), the radioactivity
were
When a system of
levels.
based
on
of high nose
and total activ6
for each subject.
between
e poi
radioactivity
of the initial
24-hour urine samples
high nose counts and body burden
r re-
waa of the order of hundreds
of counts per minute,
the 11 persons
TA8LE
of plutonium
many times the acceptable
urine
11, 1944, urine samples
-.
Appendix
first hope Of estimating
our
..
of the urine specimens
or
of our workers.
Beginning
tions
✎✍ .--$-J
✍✍✍✍✍
only 5 x 10
gave us
~thOd
how much plutonium
ens c
suggested
per day (7 alpha
50 pg per 24-hour
ist ~
✎✎ ✍✍✌✌
body burden (at chat time
-5
Ug (50 P13) of
excrete
nose
ried
✎✌✎✌✌✎✎✎
●✚✍✍✎✎✎✎✎
✎✎✍
✎
the number
of
is not good, 8 of
with more than 20 high nose counts
111
?y bo]
RESULTS
OF URINE ASSAYS
AND NOSE SWAB COUNTS
CONDUCTED
ON
dlic
LoS ALANOS
PLUTONIUM
OPERATORS
SHOWING
POSITIVE
EXPOSURE
:ally
Ibs.
Subject
Numbe ra
Average
Date of Exposure
Estimated Body
Burden (Pg + 50%)
Total Number
High Nose Swebs
Total Activity inb
High Nose Swsbs (cpm)
:rmic
1944
0.5
2
Late
1944
0.1 - 0.5
3
May 1945
1.2
1
Addiand
-
1.0
Late
m met
lC
11,606
3C
29o
37
4,267
the
4
June 1945
1.2
2.4
14,968
the
5
June 1945
1.2
55
27,246
re ca]
6
June
1.0
32
8,859
1945
lted
7
June 1945
1.0
28
15,699
I the
8
J&e
1945
0,7
60
36,407
fused
9
July 1945
1.0
22
39,778
.n
10
July
1945
0.8
24
5,334
;, the
11
July 1946
0.4
6
Ive a
12
July 1945
0.4
23
8,607
13
July
1945
0.3
8
2,016
16
July 1945
0.1
4
5,403
17
August
1945
0.7
14
7,762
18
August
1945
0.6
9
6,429
19
August
1945
0.5
8
2,266
20
August
1945
0.3
6,
2,417
21
August
1945
0.3
28
7,470
22
August
1945
0.3
22
11,688
23
September
1945
0.3
8
2,541
24
September
1945
0.1
8
5,107
25
September
1945
0.1
8
4,984
26
October
1945
0.3
3
478
27
October
1945
0.3
11
Y
it
2
data
prep>egan
Ie
3s
?atory
aSubject Nos. 14 and 15 were dropped beca~e
of the death of one subject
low body burden of the other as determined by modern asaay techniques.
18,342
of coronary
heart
disease
and the
:e
:he
.ea
b
This column waa added to the table given in reference
(both nostrils).
c
Incomplete
records were
available
for these
6 and represent
the sum of all high nose COUnts
cases.
11
had a body burden
3 in 11 persons
of 0.5 Pg Or mOre coqared
with lower
of the 8 persons with
10,000
Furthermore,
levels.
CLINICAL,
v.
with
OBSERVATIONS
6
total nose counts exceeding
Nedical
A.
Observations
were in the former group.
counts per minute
In the early
In Fig. 8 the urine
counts,
1950’s it was thought
had measurable
counts per month
in the Recovery
Group are correlated
from the series
of plutonium
processed
and protective
methodology,
1953, a program
men
in 6 subjects
for periodic
every
of nose swipes,
suggesting
to airborne
2 years was planned.
the level of body burden
and physical
by the urine radioactivity
bloo
and alkaline
p
urinalysis,
and stool examination
The following
roentgenograme
for
were
in the nose, but this is not surpristaken:
ing in view of the crudeness
of the nose
lateral
and the inevitable
skull, PA chest, AF pelvis,
R
count
.Icnee and elbow,
technique
complete
phosphorus
and
cult blood.
total activity
examination,
calcium,
of plutophatase,
nium as indicated
inter
is no corcount, blood
between
This included
considerable
There
plutonium.
stu
by a high
history
relation
of the:
Energy Cormuis
At first, a very thorough
was established.
exposure
examination
(financed by the U. S. Atomic
(Nos. 3, 4, 5, 6, 9, =d
17); in each case, the rise was preceded
activity
and one other died.
meas-
There was a sharp rise in plutonium
ures used.
excretion
as a result of the use ~
with the
more reliable
amount
acco
of the time, but 3 have bet
of 8 sub -
of exposure
dropped
jects
body burdens
of the
and the total activity
to the assay methods
high nose
that 29
the number
radioactivity,
tonium workers
of high nose
AND RADIOACTIVITY
LABORATORY,
false positives
lateral
of foot, AP of foot, an
due
dental
films of right teeth.
to contamination.
In 1953 and again in 1955, 22 and 25 subje
Maxinwmpermwsible
:=
subject ● 4
7+
i~
2 ~
(9171
1=E
9 +5+
(93S0) (2418)
levalfwurtna
——
MoxmwmpwmmsWe
I
I
1
18 -*2~7~
1
[2+
J
16 -No
I
further exposura
I
Ievel for wind
Subject
●6
E 10*
O
-+K-l ~10
(75)
10
—————
_____
+11 ~
(2S90)
_
5
1
1
Moxlmum permms!ble Ievelfuurma
?N
\
z
\ 15
0
Subject #17
Maximum
10
15
I
I
—__
level for 4urma
)
I
Moxlmumpermmsiblo
:-
t
-%
10
1
I
No further OXPO$W*
.“
5
,
I
No
furher
s.xposuro
(466)
Urlrm counts
———-—
=-----
~w
1
Moumum Derm#ssible level fwurma
4+l~l+14~8+Nofurther
exposure
::::\
4-14+?—
(7090)
permisslblo level
---------
5!
--
‘:::
-
Sept. Oet
Nov.
~
‘=:
5
~Moximum
permissible level for urmo
~:
Moxdmum pormlsslble level for Urine
March
April
May
June
July
1945
Fig. 8.
Aug.
Sept.
Oct. NOV.
March
April
Moy
June
July
Aug.
1945
Graphs for 9 subjects showing the urine count , number of high nose counts per month, and total
radioactivity of nasal swipes per xmnth (parenthetical figures) from Marth to November 1945.
Tt.
amount of plutonium handled by the Recovery Group and the protective measures used are shown in
the last graph of the second chart.
~ :,,,,6.
.
12
of the series , respectively,
29 PIII
:cordin
been
;e of
There were no significant
ion.
,nis, but ~om
.,
appeared
was expressed
However,
rovntgenogr=.
Of the sa~
considered
was
find–
Iission
After
limits.
reviewing
1956, it was decided
tween examinations
to increase
completely
program
the interval
in
be-
to 5 years and, on the advice of
Christiansen
of the University
of Utah,
:erval
.ood
! phos )r oc -
to reduce
the number
All 25 of the men
of x-rays.
were examined ,by their fam.ilY physici~s
in 19613~
17 in 1966, and 24 in 1970.
In late 1971 and early
1972, 21 of the 25 sub-
for a complete
observation
study in-
estimates
in Appendix
evolution
IV.
period
Because
separation
nium body burden.
changed
radio-
radiometric
for estimation
meas-
of the pluto-
(1972) version
—Body Burden
of
—From urine &tal-
code7 was used to estimate
urine assays for plutonium, in Vivo measure239
Pu in the chest, pulmonary cytology,
for
of the
of urine collection,
The current
(~lutonium
to be the best value
LP of
more knowhave
description
of plutonium,
urements , and the bases
ysis)
(1953-
were made, we have pre-
B a detailed
of the methods
chemical
as
since 1953 when the first reasonably
the PUQFUA
.e
jects came to Los Alamos
the 20-year
sophisticated
sented
Itudy
Dr. William
by Urine
of plutonium
ledge has been gained and techniques
normal
the experiwntd
of body burden
1972) are shown in Table
In
:hese
as Determined
by assay of the urine of the subjects
made during
age, this
to be within
Body Burdens
The estimates
determined
in the
after careful comparison
IIOI=S1 male subjects
witIl
medical
Plutonium
U
Energy
about what
to be an excess of bone islands
observation
i.
~oncem
B.
by
with the U. S. Atomic
p}]ysicians =sociated
cu~iss
were examined
what is considered
for the body burden
of the
cluding
and
ments
and chromosome
The mdical
analyses.
TABLE
PLUTONIUM
examination
BODY BURDEN
IV
ESTIMATES
FOR UPPU
SUBJEGTSa
jects
consisted
historv
alysis
of the following
and physical,
and blood
complete
chemistry
phatase,
cholesterol,
protein,
albumin,
(alkaline
A/G ratio,
glucose
Case
Code
count, urin-
profiles
globulin,
were
blood
total bilirubin,
SGOT, LDH, creatinine,
Roentgenograma
complete
procedures :
phos-
1
0.03 - 0.06
total
2
0.006 - 0.032
total lipid,
3
0.08
4
0.08
5
6
BUN, and urea).
also taken of the chest, peltis,
and teeth.
Except
for the ailments
in a group of men mostly
all subjects
examined
One man had a coronary
and was well
that one would
in their early
were
in remarkably
occlusion
compensated,
inal group died in 1959 of a coronaxy
Another
had a hamartoma
removed
wfthout
C and section
chest wall
(regional
fourth had a partial
ulcer.
Several
at age 38.
of the
lymph nodes were negative).
gastrectomy
All En
working,
most as successful
executives.
No roentgenographic
changes
A
for a bleeding
and one had gout.
and uoderate
were
actively
in the lungs or
The lsmina dura of the jaws
(which show the first changes
in one edentuloua
of the orig-
in 1971 (see Appendix
obesity,
doses of plutonium)
good health.
A third had a uelsnoma
had mild hypertension
bones were apparent.
fi’fties,
of the lung surgically
complication
V. C).
expect
but had recovered
and another
in beagles
19531
given toxic
19576
19627
1972
0.01
0.206
0.07
0.13
0.42
0.08
0.14
0.26
0.08
0.07
0.14
0.18
0.06
0.06
0.07
0.14
7
0.06
0.06
0.O8
0.15
8
0.04
0.04
0.05
0.11
0.03 - 0.06
0.03
9
0.06
0.06
0.11
0.11
10
0.05
0.05
0.03
0.10
11
0.03
0.02
0.03
0.05
12
0.03
0.02
0.02
0.12
13
0.02
0.02
0.04
0.035
16
0.006
0.006
0.002
0.03
17
0.04
0.04
0.09
0.13
18
0.04
0.04
0.04
0,10
19
0.03
0.03
0.06
0.02
20
0.02
0.02
0.02
0.05
21
0.02
0.02
0.03
0.04
22
0.02
0.02
0.02
0.05
23
0.02
0.02
0.04
0.04
24
0.006
0.006
0.01
0.03
25
0.006
0.006
0.01
0.01
26
0.02
0.02
0.03
0.006
27
0.02
0.02
0.03
0,05
were intact in all cases except
subject.
%licrocurie
~ approximately
50 percent.
13
-—
!
/
,dical
TABLE V
The
ESTIMATED
ACCUMULATED
AVEf@GE
ORGAN DOSES
EXPOSED
FOR pER.sOf’Js
..
BY INHALATION~~
TO PLUTONIUM
.e
,na1
TirE.
sin CC
Estimated Exposure
(MPL)b
ExpOsure
(years)
1.4
6.7
37
80
24
1.4
6.7
37
m
24
1.6
7.6
42
90
24
1.8
8.6
47
100
24
2.0
9.6
53
110
24
2.3
11.0
61
130
24
2.5
12.0
66
140
24
3.3
16.0
87
190
24
3.4
16.0
90
190
95
200
24
as
the
is
Accumulated Average Organ Dosea
Lung (rads)
(rads)
Liver (rads)
Bone
odel
gham
rtain
ve ror
24
3.6
17.0
23
1.1
5.0
28
63
23
1.1
5.0
28
63
as
1ter
hhese
values are being brought
of a future report.
b
One maximum
permissible
level
using the latest values
up-to-date
This is a subject
for the body burden.
(MPL) = 0.04 pCi.
ing
hort
e
b-
ts
these studies
has been
sity of Utah Medical
carried out at the Univer12
On December 1, 1952,
School.
below
point has not been accepted
for 6 groups of about
The first animal
of an osteogenic
m
These
group.
sarcoma
to die in July 1956
was in the highest
In 1961, an osteosarcoma
occurred
dose
verse biological
at the then lowest
effects
have
to predict
(e.g., practical
levels of injected
been proven unequivocally
14
nuclides.
no adthreshold)
plutonium.
by everyone
This
and has not
for alpha-emitting
radio-
in a
c.
beagle
certain
observations
investigators
2.9 pCi per kg body weight
12 dogs each.
ver,
is reduced.
numerous
the first group of 6 beagles were injected (IV) with
239
Injected doses ranged from 0.016 to
Pu citrate.
g-
J-
injected
prompted
Determination
of Plutonium
in the Body by In
dose (0.016 VCi per kg),
Vivo Measurements
and since then several
lower dose groups have been
added to the experiment.
0.00064
1.
The lowest dose group,
‘s.
VCi per kg, corresponds
roughly
to the msx-
Plutonium
most recent
in the Chest Cavity.
(late 1971-early
During
1972) medical
the
examina-
ie1s
imum permissible
occupational
body burden
(0.04 pCi)
tions at Los Alsmos,
amount
in man.
of plutonium
estimates
were made
of the
in the lung and respiratory
lote
To date, the 0.016
interest,
Lnce
giving
I.ICiper kg dose level is of
as 4 dogs have developed
a tumor incidence
age time from injection
was 9.9 years,
osteosarcomas ,
of 33 percent.
to death
and the average
The aver-
for these animals
skeletal
dose from
lymph nodes
counter
(see Appendix
of detectors
x-rays
of each subject
emerging
were made
D).
in position
using
Figure
sn in tivo lung
9 shows the pair
for counting
from the chest.
of the liver region
the low-energy
Measurements
in several
also
subjects
7tes
injection
to death was estimated
and of the hands
to be about
of persons
known
to have had skin
age
80 cads 13 (a more recent estimate
suggests
50 rads).
osteosarcomas
wounds
about
contaminated
by plutonium.
The minimum
de-
Sher
We do not know whether
be produced
at dose levels
lnwer than 0.016
and can only await the outcome
experiment.
incidence
to develop
However,
decreases
will
vCi/kg
of this important
we do know that the tumr
and the time required for tumors
increases as the amount of plutonium
tectable
with
activity
(MDA) for human
the LASL detectors
eters such as body build
measured
param-
and chest thickness.
average MOA for a 2000-second
counting
7 nCi if one uses the 95 percent
For the 68 percent
subjects
varies with several
confidence
An
time is about
confidence
level.
level and a similar
less than 200 rads, are below
which
caused adverse
experiments
colleagues
using beagles.
12 years following
239
PU02 .
is essen
exposure
Fig. 9.
The {n tiuo counter with detectors
tion for counting the chest.
counting
time, the comparable
in posi-
value is about 3.5 n-
Ci.
Positive
counts were
These
sons measured.
ranging
95 percent
chest burden
confidence
jects with positive
(at the 68 percent
level.
For reference,
the maximum
permissible
burden
will deliver
lung, assuming
throughout
Seven of the 14 sub–
lung burden
about
this
15 rem per year to the
of energy
the organ.
qualitative
statements
of subject
likely
exposure
received
approximately
Subject
10 nCi.
in the Recovery
burden
o~ about
Group,
values
are not surprising,
These
8 nCi.
of plutonium
as a function
The cumulative
the estimates
Nos.
oxide, were
4 and 9, who
each had a chest
relatively
small
in view of the kncwn
from the lung to other
of time following
radiation
of some of our subjects
level,
Nos. 1 and 2, who most
to plutonium
worked
translocation
confidence
can be made about
For example,
of lung burdens
viously
for occupational
indefinitely,
distribution
the chest measurements.
tissues
to have
of from 7
10 nCi is about 2/3 of
If maintained
uniform
chest
and may be considered
If one uses the 68 percent
certain
in no case
the MOA at the
chest burdens
to 10.nCi.
(16 nCi).
exceed
level of confidence)
significant
workers
chest burdens
chest counts had estimated
of 7 nCi or greater
statistically
for 14 of 21 per-
However,
from 3 to about 10 nCi.
did the estimated
burdens
obtained
counts suggested
doses
inhalation.
to the lungs
have been estimated
by Langham 11 (Table V).
The values,
preall
effects
For example,
at Battelle-Northwest
lung effects below
interpre
the lowest dose:
biological
seen i
Bair
have not obst
about 2000 rads in dogs 10
doses
?
~
een in
Bair and
observed
s 10 to
posure
to
st be
ncidence
~dl iwl.,nt tumors and pulmonary
11
estimated
;IIman, Langham
was approximately
of subject No. 2. Table. VI shows results
239PU
239PU
of analyses for
The concentration of
as inducing
17
sclerosis .
I,,,,ti
~~ ,1completely
empirical
1,.
v, 1 “at or above which
m~~ ensue
100 rads to the
judgment
biological
the same in the tumor and lung
239
Pu in bone
the concentration of
tissue, while
as to a
was approximately
consequences
in a small pOpulati On Of ~ifited distribu-
observed
with the experimental
PU02 by inhalation,
at Battelle–Northwest
t-CPort that the plutonium
content
established
of the thoracic
was about the same as that
lvmph nodes of beagles
tissue,
findings
relative
to that in lung tissue
function
of time following
a homogeneous
lung and lymph nodes and a total
31 organ,
Y) percent
imated
AL
,Ibout
of the initial
10
years
fOll OWing exposure,
tained about 12 percent
the lungs con-
and the thoracic
lymph nodes
distribution
1000 grams and respiratory
20 grams,
increases
as a
lung weight
of
lymph node weight
of
the total plutonium
burden
and respiratory
lymph nodes
roughly
divided between
equally
in lymph nodes
If one assumes
exposure.
239
Pu
throughout
the
of
lunX tissue and thoracic
contained about
239
PU02 .
alveolar-deposited
to
It is well
above.
that the concentration
loped lung
lymph nodes
concentration,
is consistent
in dogs exposed
as mentioned
veOlar-
; dog lung,
o! Lt]e entire
The highest
half.
in the lymph node
lung tissue about 5 years following
16
At this time, both
J + ingle inhalation exe Osure.
Iis amount
in
., ,,eJr$ ~~ ~]ccupational exposure)
Park and co-workers
available
of plutonium
the lungs in this study was made on the operative
~cnt
ti on.”
nal data
measurement
specimens
.:,jepe[,
plutonium
o lower
The only direct
of the distribution of dose in time,
‘“
~,, -u+t ~rcept ~ dOse Of 75 rads (accumulated over
of the lungs
is approximately
8 nCi
lung and lymph node.
For reference,
loodless
about 4(J percent of the initial alveolar-deposited
239
From these data, we might expect a signif1’UO
2“
icant fraction of the original lung burden of our
lung of case No. 2 (estimated
by tissue
human
be 3.85 nCi) is approximately
550 times contempo-
. mean
nodes many years after exp Osure tO Plut Onium Ofide.
rary total lung burdens
,el that
however,
States exposed
mg
know whether
,me.,
(about
,th in
subjects
to be present
one must exercise
in the thoracic
caution,
the translocation
lymph
as we do not
and man or whether
ion equiv-
the rates observed
nal lung
dens would be realistic
e, is
velopment
deposits in man.
Although a single measurement
239
Pu in the chest of subjects exposed 27 to
not to
28 years ago is of little help in obtaining
For
ated to
estimates
periodic
for beagles
measurements
with
for smatk?r
of the current
lymph node tissue,
of
accurate
similar
counting.
Figure
plutonium
particle
examined
9e un-
periodic
ature
jects, we would have more confidence
30ut
mates of the chest burden.
Had repeated,
been made on the present
weapons tests.
Estimates
239
Pu of subject No. 2,
from analysis
are in reasonable
distribution
sub–
2.
in a section
agreement
based
(a
on chest–
of a
of lymph node re–
of other
in the lymph node tissue
a very nonuniform
from plutonium
Plutonium
.
of lung and
Observations
No. 2.
particles
indicate
from plutonium
10 shins an autoradiograph
moved from subject
changes
the chest.
in the
assay to
in the United
resulting
factor of about 2) with estimates
data on temporal
individuals
of
on extrapolation
plutonium
of plutonium
measurements
based
alveolar
exposed
re, the
within
large lung bur–
recently
hen the
by atmospheric
of the chest burden
of plutonium
in humans
to fallout
initial
chest burdens,
on several
have yielded
dispersed
rates of plutonium
oxide are the same for the beagle
the total amount
radiation
dose-
particulate.
in Other Tissues.
Because
we
in our estihave no reliable
calibration
system
for plutonium
16) conTABLE VI
3 burden
PLUTONIUM-239
~dents
17
llev
Tissue
Wet Weight
(grams)
CONTENT
OF TISSUES
Volume
IWMOVED
of Solution
(ml)
FHOM PATIENT
NO. 2 IN MAY 1971a
~dpm per ml)
PlutOnium-239
(dpm per gram)
(pCi per gram)
)plasms
Lu” g
70.85
100
6.o1
8.48
3.85
ty in-
lymph node
1.25
25
22.55
451.00
205.00
: control
Ilamartoma
0.77
25
0.23
7.47
3.40
20.00
100
0.71
3.55
1.61
Mosk!ffect
Rib
a
~ifter ashing and dissolution
of tissue.
17
studied
well
in persons
exposed
as to a variety
cyclamates,
effects
to ionizing
of exogenous
caffeine,
of elements
and LSD.
radiat
agents such
More recently
such as cadmium
that are
vironmental
pollutants suspected of contribut
18
disease
have been studied.
Radiat
to human
induced
human
chromosome
been used to estimate
.people
involved
whole-body
aberration
radiation
yields
ha
doses receive
in radiation accidents involv
60C0 19
to
Similar studi(
exposure
also been performed
on peripheral
blood
leuco,
obtained from subjects exposed years ago to T1
20,21
trast;
the element 232Th decays through
6 alpha
and 4 beta disintegrations
90 percent
with high LET alpha rays).
Fig. 10.
Autoradiograph
of lung section of subject
No. 2 showing a radioactive particle.
ucts deposit
sequently
in the liver of human
quantitative
in several
within
persons
“the observations
cannot be measured
Plutonium
by the in oivo
Traces
of plutonium
the hands
of several
to have hand wounds
nium in 1944 or 1945.
located
we can make no
concerning
who were measured.
technique.
tected by counting
known
subjects,
statements
the bone
counting
were de-
observation
that the subject
Of interest
erroneously
that the wound was on the other hand.
the skin overlying
grossly normal
the active
except
to make additional
site appears
for minimal
measurements
of this deposit
in the future.
D.
Analysis
Chromosome
During
the 1971–1972
samples were
obtained
studies
techniques.
scaling.
visit
to the LASL, blood
chromosome
techniques
banding
group for chro-
were
to add newly
found
developed
During
recent years,
been directed
ipheral blood.
rations
18
considerable
at the effects
agents on chromosomes
in human
peripheral
interest
of various
of lymphocytes
The induction
analyzed;
many of these patients were exposed
22,23
War II.
In both Thorotrast and
to World
dium patients,
leukocytes
has
stressing
in the per-
of chromosomal
marked
might
aber-
has been
of blood
lymphocytes
of radium have been
excesses
of chromosome
a
reported.
Because
of observations
expect
of chronic
to plutonium
to observe
lympho
oxide aerosols,
chrOmOsome
dsmage
o:
in 1:
cytes of exposed
plutonium workers.
This obse:
24
tion led Dolphin
to investigate the possibil:
of chromosomal
obtained
aberrations
from workers
exposed
workers
in lymphocyte
in England
to plutonium.
8 plutonium
knwn
He compared
cultu~
to have
the findings
who had been exposed
14 rads of external
to plu
irradiation
over
year period
with workers
irradiation
only and found that the dicentric
of lymphocytes
accounted
other
who had received
of the plutonium
case in which
a plutonium
indicated
lymphocyte
series
of the patient.
chromosomes
worker
was foun(
to have 10 to 20 times the p<
after an inhalation
a variety
y
could b.
radiation dose re24
Dolphin
also cites an
level of plutonium
analysis
workers
exter
for by the external
by chest–counting,
3 years
when the group is next studied.
pr
and c
the chromosomes
missible
to our procedures
daughter
is exhaled,
with body burdens
ceived by the workers.
established
no abnormalities
we plan
We plan
Radium
thoron
Finally,
nium plus
from the UPPU
in these subjects,
to be
on and observations
using standardized,
Although
thought
At present,
(:
is associat
both bone and lung tissue are irradi
in dogs exposed
is the
to 208Pb
energy
patients
with pluto-
The site was precisely
to be 5.3 —
+ 0.4 nCi.
in bone,
rations were
subjects
while working
in one case (subject No. 1) and the amount
estimated
mosome
of the radiation
minimal
in the lung about
accident.
radia~ion
Chromosoc
damage
to t
even at a high level of exposL
Other
obtained
investigators
from uranium
of stressing
agents,
are studyir
miners
exposec
including
radiati
adiatio
such a
are en
ributin~
~diatio]
1s have
:eived E
lvolving
)tudies
.eucocyt
to Thor
ugh
Pb (abol
ociated
er prodand conrradiate
{tes of
been
~sed pri
and ralme aber.
mphopen]
S, one
in lymph
observability
Jltures
have bee
dings in
3
plutOa
7-
ZXterual
:ic yield
!ld be
Ie re!s anfound ,
he perUt
mos ome
to the
xposure
udying
Josed to
iiation,
their emplo~enc.
when
obtained
ently,
lver
during
~aution
interpreting
from chromosome
aberraCfO~
cannOt
accumulated
dose because
the lymphocyte.
Hcwever,
One must use
quantitatively
analysis,
results
as the number
continue
of
tO ‘nCrease ‘ith ‘he
of che finite life span of
For long periods
of
assistance
in the in vim
Flynn, M.D., for medical
for assistance
D. Meyer
chest measurements;
examinations;
in administrative
arrangements;
for his help in recalling
tions and health
safety procedures
P.
exposure
c. w. Mays and T. F. Dougherty,
12.
“prOgress
the Beagle, Studies at the University of
Utah, ” Health Phys. 22, 793 (1972).
13.
C. W. Mays, G. N. Taylor, W. S. S. Jee, a
“Speculated Risk to Bone
~~v~~ ~~~h;i$~~,”
Health Phys. 19, 601 (
14.
C. W. Mays and R. D. Lloyd, “Bone Sarco~
Incidence vs. Alpha Particle Dose, in Rad
biology of Plutonium, B. J. Stover and~
Jee, Eds. (The J. W. Press, University of
Salt Lake City, Utah, 1972), p. 409.
15.
W. J. Bair, “Inhalation of Radionuclides
in Inhalation Carcinogen
Carcinogenesis,”
M. G. Hanna, Jr., P. Nettesheim, and J. R
Gilbert, Eds. (U. S. Atomic Energy Commis
Division of Technical Information, Washin
D. C., April 1970), AEC Symposium Series
p. 77.
16.
J. F. Park, W. J. Bair, and R. H. Busch,
“Progress in Beagle Dog Studies with Tran:
uranium Elements at Battelle-Northwest,”
Health Phys. ~,
803 (1972).
O. Johnson
and
condi–
in the early
days.
REFERENCES
1.
W. H. Langham and J. B. Storer, Eds., “knual
Report of the Biomedical Research Group of the
Health Division, 1952,” Los Alamos Scientific
Laboratory report LA-1537 (June 1953), P. 8.
2.
G. T. Seaborg, “Health Hazards in Working with
Plutonium,” Memorandum to R. S. Stone, report
MUS-GTS-399
(January 5, 1944).
3.
“The Chemistry of Plutonium,” LOS AhIK@
Scientific Laboratory Technical Series report LA1100 (1947), downgraded to Confidential
in
1959.
4.
W. H. Langham, “Determination
of Plutonium in
Human Urine,” Los Alamos Scientific Laboratory
report LAMS-603 (December 1947); also U. s.
Atomic Energy Commission report MDDC-1555,
Technical Information Division, Oak Ridge,
Tennessee (March 1945).
5.
6.
C. S. Smith, “Plutonium Metallurgy at Los
Alamos during 1943 to 1945,” in The Mtal
Plutonium, A. S. Coffinberry and W. N. Miner,
Eds. (University of Chicago Press, Chicago,
Ill. , 1961), Chap. IV, p. 30.
L. H. Hempelmann and W. H. Lsngham, “Determination of Systemically Deposited Plutonium
in Laboratory Personnel and a Simple Qualitative Test for Exposure to Airborne Radioactive Material” (U. S. Atomic Energy Comnd.ssion, Technical Information Service, Oak
Ridge, Tennessee, December 1953), rePOrt
AECU-2633.
7.
J. N. P. Lawrence, “PUQFUA, An IBM 704 Code
for Computing Plutonium Body Burdens,”
Health Phys. ~, 61 (1962).
8.
J. N. P. Lawrence, “PUQFUA:
An IBM-704
FORTRAN Code for Determining Plutonium Body
Burden from Urine Assays,” Los Alamos Scientific Laboratory report LA-2329 (April
1960) .
9.
W. H. Langham, “Physiology and TOXiCOlOgy
Plutonium-239
and Its Industrial Medical
trol,” Health Phys. ~, 172 (1959).
10.
W. H. Langham, J. N. P. Lawrence, J. McClelland and L. H. Hempelmann, “The Los Alsmos
Scientific Laboratory’s Experience with Plutonium in Man, ” Health Phys. ~, 753 (1962) .
11.
17.
18.
Y. Shiraishi, H. Kurahaahi, and T. H. Yos~
“Chromosomal Aberrations in Cultured Hums
Leukocytes Induced by Cadmium Sulfide,” P]
Japan Acad. &,
133 (1972).
19.
J. G. Brewen, R. J. Preston, and L. G. Lit
Human Chronmsom
field, “Radiation-Induced
Aberration Yields following an Accidental
Whole-Body Exposure to 60co Y-RSYS,” Radi:
RSS. Q,
647 (1972).
20.
M. L. Janower, O. S. Miettinen, and M. J.
Flynn, “Effects of Long-Term Thorotrast Ex
sure,” Radiology ~,
13 (1972).
21.
P. Fischer, E. Golob, E. Kunze-Muehl,
and
Muellner, “Chromosome Aberrations in Perso
with Thorium Dioxide Burdens,” in Human
Radiation Cytogenetics,
H. J. Evans, W. M.
Court-Brown, and A. S. McLesn, Eds. (North
Holland Publishing Company, Amsterdam, and
J. Wiley and Sons, Inc., New York, 1967),
p. 194.
22.
R. Tuscany and J. M~ller, “Chromasomsl Stu
of Bone Marrow and Periph
Carrying Body Burdens of ‘$t?~~dg~~;r’
Human Radiation Cytogenetics, H. J. Evans,
W. M. Court-Brown,
and A. S. McLean, Eds.
(North-Holland Publishing Company, Amaterd
and J. Wiley and Sons, Inc., New York, 196
p. 203.
23.
J. T. Boyd, W. M. Court-Bru.m, G. E. Woodc~
and J. Vennart, “Relationship between Exte:
Radiation Exposure and Chromosome Aberratic
among Luminous Dial Painters,” in Human Ra{
tion Cytogenetics,
H. J. Evans, W. M. Court
Brown, an d A. S. McLean, Eds. (North-Holla
Publishing Company, Amsterdam, and J. Wile:
and Sons, Inc., New York, 1967), p. 208.
Of
Con-
W. H. Lsngham, “Biological Considerations
of
Nonnuclear Incidents Involving Nuclear Warheads,” J. F. Becker, Ed., University of
California Radiation Laboratory report UCRL50639 (April 1969).
,,239PU
: Problems of Its
Y. I. Moskalev,
Biological Effect,” Health Phys. ~,
723
(1972) .
20
,:.‘
!,
gress in
y of
,;. X. Dolphin, “The Biological Problems in the
radiological Protection of Workers EWosed
CO
239pu,!~ Health Phys. Q,
549 (1971).
*e, and
Bone and
501 (1970).
‘;. saccomanno,
R. P. Saunders,
O. Auerbach, M. Kuschner, and P. A. Beckler,
“Cancer of the Lung:
The Cytology of Sputum
prior to the Development of Carcinoma,” Acts
Cytol. ~, 413 (1965).
V. E. Archer,
rcoma
1 Radiold~.
S.
:y of Utah,
togenesis,
.
J. R.
~
maniasion,
ffihington,
.ies 18,
ch ,
Trans-
t,”
Its
723
Yosida,
Human
9“ Proc.
LittleX.ome
ztal
Radiation
s
J.
;t Expo-
and T.
?ersons
4orthand
;7),
Study
I Persons
k, “ in
,ans,
ids.
terdam,
1967) ,
,
‘oodcock,
External
rat ions
n Radia–
Court olland
Wiley
8.
;
1
;
f
I
;
21
APPENDIX
DECONTAMINATION
The following
Clinton
is an excerpt
Laboratories,
Knoxville,
PROCEDURES
from a Secret
Tennessee,
A
AND RESPIRATORS
letter written
USED AT LASL IN 1944
by L. H. Hempelmann
dated July 20, 1944, which
describes
to Dr. Robert
S. Ston(
decontamination
proced(
end respirators:
“1. Decontamination
A.
Procedures:
Floors:
A special corp of janitors assigned to these laboratories spend all their
time on this iob. Thev work under the supervision of a head Ianitor and a
In order to get good res-dts end to keep the-floor counts low, it
“laboratorian~”
is necessary for the floors to be covered with a smooth hard surface of wax.
There
does not seem to be much difference in the kinds of wax that we used so we have
Our present
settled on the water-soluble
floor wax supplied by the janitor service.
floors are made up of some asphalt tiles knoun by the trade name of “Mastic.”
In
so~ new laboratories we plan to use a smooth asphalt surface with an MgO base.
1, Routine Cleansing:
All floors are mopped once a day; floors of hot
laboratories are mopped twice a day or oftener.
They are wet mopped
with a good lather of Ivory soap, followed closely with a dry (wrong
It is essential that the janitors be meticulously careful
out) mop.
The results are better if the wash
about covering the entire floor.
By this method it has been posand rinsing water be kept separate.
In our “hottest”
sible to keep the floor counts in most labs below 100.
laboratories,
the counts are always below 500. We are now using some
detergents in an effort to obtain better results.
2.
B.
c.
22
This is done by a trained decontaminaDecontamination
after Spillage:
The floor is fi~st mopped with Ivo&
soap.
The wax is then
tion squad.
removed with boiling hot water, followed by kerosene and steel wool.
The floor is then painted with two coats of any thick paint which will
stick to the surface.
Desk Tops of Laboratory Benches:
Every working surface is covered with a smooth
Porous surfaces are covered with enamel paint before
surface preferably glass.
they are used for work.
If they are contaminated by accident, an effort is made
to seal them in the material by painting rather then to remove the contaminated
In the case of the lab benches made of “Kemrock” (the
part of the desk top.
ordinary black surface made by the Kewaunne Mfg. Co., Adrian, Mich.) the surface
responds to ordinary methods of decontamination
although it appears to be porous.
The same company puts out a surface paint of the same material, called “Kemrock
Wipe Coat,” which can be used to paint over contaminated surfaces.
1.
Routine Cleaning:
Smoth
surfaces can be quite successfully decontaminated by wiping with a clean cloth wet with spindle oil. An
excess of oil is used and this is followed by a clean dry cloth.
The
secret of the successful use of this method is to change cloths very
The surface count is usually reduced below 50 per minute
frequently.
by this method.
2.
Decontamination
after Spillage (or after contamination from droplets
First wipe the surface with 1 & HC1 solution
produced by evaporation):
followed by dry rag, then clean with oiled rag as above.
Rends : Before starting work, spread thin coating of spindle oil over both hands;
this must be done very carefully.
Decontaminate
gloves before removing them;
remove gloves using surgical technique so as not to touch outside surface with
henda,
Apply coat of West’s Sulfo snap to hands, moisten with water and lather,
rinse; repeat with Sulfo soap and finally wash with Ivory soap.
A-
- --
●
----
The success of this =thod
depends upon how well directions are followed particIt
ularly insofar as spindle oil is reapplied after each washing of the hands.
has been our ewerience
that it is usually possible to reduce the hand counts to
a few hundred or less by =ans
of this method.
D.
A 10 percent solution of the detergent “aerosol” is used
Gloves and Respirators:
Other detergents do not seem to work as
for decontamination
of rubber articles.
The solution containing acetic acid formerly used by us has been discontinued
well.
because the acid tended to injure the rubber and was hard on the skin if not properly
removed.
The gloves are washed every day (after one wearing).
They are rubbed and
This is quite time consuming as about
swished aromd
in the solution until clean.
two minutes iS required for each glove (we hope
to cut this down by getting each
The rubber respirator faceperson to decontaminate his own gloves after wearing).
pieces are cleaned once a week if their count is over 50.
E.
This is cleaned by running each piece of glassware through the following
Glassware:
solutions:
1. water
2. Ivory soap water followed by rinsing
3. cleaning solution followed by rinsing
4. Ivory soap and water followed by rinsing
5. distilled water
Popham says that the results seem to be satisfactory but he will not guarantee them.
Not very much work has been done on this problem.
F.
Tools : Can be decontaminated
and clean frequently.
Stone,
cocedure:
]eir
it
fiere
‘esent
In
2.
t 1!
en
with
an oiled
rag as described
above.
Use clean cloths
Most of the respirators
Masks’: We have used only Wilson respirators and positive pressure masks.
put out by this company have filter pads which are satisfactory for this type of dust.
Their
chief disadvantage is in their failure to fit properly but we have found that one of the following three types will fit just about any type of face:
200L, 5L and 750. We are careful to fit
As far as the positive pressure masks
each mask to the person before letting them go into use.
are concerned we have not tried the A.M.S. type because they did not appear as satisfactory as
We have modified the masks by putting on
the Wilson type as described in their catalogues.
softer tubing onto the facepiece since there were some complaints about the stiff tubing supplied
by the company and by placing the filters on the wall rather than on the belts.
The tubes are
fastened to the belts to avoid the masks being jerked off the faces of the men if the tubing gets
caught.
We have still not been able to put the positive pressure masks in general usage because
of the crowded conditions in our laboratories .
The Eastman masks which I described to you over the telephone appear to be the most satisfactory of all, but have not been well tested.
If you see them and consider having some made
up we would be very interested in placing an order at the same time.”
Declassified by L. M. Redman
(September
11, 1972)
23
APPENDIX
URINE ASSAY METHOD
URINE
SAMPLE
B
OF BODY BURDEN
AND ESTIMATION
COLLECTION
TABLE
Beginning
were
in January
collected
from plutonium
that measurement
yield
of plutonium
results which
snd/or
intake
workers
on a 24-hour basis
suggested
contamination.
contamination,
a Health
to
1944, a pto-
from analysis
massive
Each employee
granted
10.1
2.2
4.3
3
41.6
4
16.1
3.4
of urine
c
2.8
0.1
c
17.8
5
30.6
2.2
20.0
2.2
of such
Paas Ward was established
Hospital
heavily
ing to the hospital,
During
this time,
in the spring
exposed
2 days off with
of Sample (cp
In Hospitz
6
Average
in the Los Alamos
SANPLE
“clean”
artifactual
the possibility
OF COLLECTING
FOUND IN THE URINE
Place of Collection
At Homea
~—
urine samples were
in so-called
occasional
To minimize
to exposure
By March
of plutonium.
areas, but the data derived
samples
in the hope
could be related
OF METHOD
ON COUNTS
in the urine might
cedure had been adopted whereby
collected
EFFECT
1944, spot urine samples
I
of 1945.
to plutonium
full pay* prior
where he stayed
an uncontaminated
waa
to report-
for 24 hours.
aSsmples collected at home were 2 overnight vo
collected by the individual after thorough bat
and washing of hands.
or minimally
b
contaminated
using
24-hour
all practical
procedures
tamination.
Upon entering
men showered
and changed
which were worn
to minimize
the Health
into hospital
throughout
I shows the rather striking
for urinary
6 subjects
who
collected
and in the hospital.
inally presented
excretion
~ot
in June
Lsngham
1945.
ss@e
differences
in
follow-up.
both at home
at a plutonium
conference in May 1945 and documented in a report
*
Employees, particularly
those in military service,
were forever grateful to Lsnghsm for the 2-day leave
away from the ‘Will,” as the mesa was called.
**
Langham’s favorite story had to do with the enormous quantities of urine passed by many of the
plutonium workers while in the hospital ward.
The
subj ects, usually G. 1.’s, were able to obt~n
beer
from the nearby PX by some means and drank this in
substantial quantities,
Fortunately, plutonium output is independent of quantity of urine.
According
to Langham, the champion was a man nicknamed Pias
Porter (not his real name).
1
unfortunately,
cont~nation
forgotten
during
periodically
and accidents
Also
of interest
on the then current
0.5 count per minute
ute.
table
gives some inform
(per 24 hours)
of
and recove~
In the c
as counts per II
of the proportional
used at the time is uncertain
proached
(Table 1
urine blanks
often presented
The efficiency
an,
of data.
for the urine essay procedure.
days, data were
expo:
and Thule),
is another
average
of
has beeI
(e.g., operational
such as Palomares
from the same report,l which
values
this problem
collection
has led to misinterpretation
The data are shcun as orig-
by Wright
in UPPU
period.
collecting
of plutonium
urine samples
the
pajamas,
gloves were used while
**
the urine specimens.
Table
con-
Pass Ward,
the collection
White mortician’s
recorded
Samples collected in hospit~
were 24-hour sa
collected under the rigorous hospital plan aft
2-day leave from the ‘TIill.”
urine sample was collected
counte
but probably
ap-
50 percent.
In an effort
to minimize
costs, the procec
was modified
in 1947 to eliminate
pass period,
but the employee
the 2-day hec
still reported
., ,
24
‘,,
. .i’
tc
TABLE II
~;COLTRy
>,>,
&,L.
r !if
DeK,,-:.,,,,tlIJ115
_.
._...—:.
oF ~NOwN ,If40L?iTS
(JF PLUTONIUM
Nature
Blanks
88-1oo
11
Hock urine solution
10.0
93
85-101
1:
Kegular
urine
10.0
88
73-104
Regular urine
4.5
95
81-105
1’:1s.Ward
for sample
In a fur-
collection.
ther it tort LO redllce cOsts,
the Health
v.lk ,]lulisll~.,1
in 1951, and employees
p=s
were
Ward
to ,vll,[t
It home 2 morning
and 2 evening
i!ls:!<
. Tt]c,sesamples were pooled
CIIL,
“k,
quivalc,nt”’ 24-hour
met~l
kit was
tained
2.2
2.2
three
which
The metal kits proved
unsanitary.
and the concept
bottles
three
fore , a disposable
l-pint bottles
statistical
collected.
voided
over
collected
24-hour
a
period
This
been
CS been
collected
constancy
), and this
in special
able II)
nformation
of
containers
with
excretion.
change in procedure
have
time marks
for greater
plutonium
afforded
per minute.
separation
corrections
and
electronic
per sample
to disintegrations
in dis–
can be realisper minute
per
CliJv.
This
equipment
resulted
procedure.
In
by TTA extrac-
measurement
is made
film counting.
The
recoveries
of
of O.OO7 + 0.005 dis-
A somewhat
procedure
change was substituted
expressed
sensitivity
plutonium
with blanks
has
by volume
the
the measured
is separated
track alpha)
procedure
70 —
+ 17 percent
chemical
of urine.
in 1957 of the Hanford
(nuclear
Hanford
on urine
eliminating
did not alter
tion, and the final radiometric
integration
Informa-
plutonium,
earth phos-
or blanks.
this method,
by NTA
tech–
of 67 —
+
of 0.15 ~ 0.1 disintegra-
large volumes
of such timed samples
so that results
corrected
samples
to learn more about the
specific
per minute
collected
co-precipitation
recoveries
was used directly
to evaporate
recoveries
82 —
+ 19 percent
In 1955, an alkaline
The desire
urine
fluoride
to concentrate
in adoption
is used today.
nonro”tine
to apply
tically
ecovery
procedure
made it possible
integrations
the
represent
urinary
from analysis
gravity
by snal–
from that time
was
By 1949, the serial bismuth
phate precipitation
four
with an iron–
of 0.69 +
— 0.53 disintegra-
20 percent with blanks
need
data
recovery
with blanks
tion per minute.
suggests
of 22 —
+ 4 hours, when
collection
of plutonium
tion gained
obtained
Existing
complex.
that plutonium
nique was in use, affording
samples
1958; a
by co-extraction
phosphate-lanthanum
There-
is not necessarily
samples
on the lids in an effort
exposures
in January
to be
4 void-
kit containing
by this means
sample
Since 1969, occasional
.em of
discarded
of collecting
cardboard
The pooled
correctly.
each kit con-
eventually
cupferride
tion per minute.
A reusable
were
review of the results
that a “true”
vOid-
proved unacceptable.
was introduced
ysis of samples
mr samples
in after a
the employee;
bottles,
after use.
in~s In
&t voidings
3h bathing
furnished
l-pint
separated
associated
and considered
urine sample.
plutonium
suggest
asked
2.2
0.1
(0-1.2 Cpm)
0.5 cpm)
94
Health
3.4
(average
29.2
)
4.3
Spread
(%)
!lock urine sOlutiOn
MPLE
:*
0.0
urine)
smLEs
Recovery
(%)
Amount of Spike
(cpm)
of Samples
(regular
FROM RECLJLAR AND MocK ~INE
utilizing
in 1963.
capable
simpler
radio-
anion ex-
Introduction
of pulse-height
of
‘
dis-
crimination
made it possible in 1967 to include a
236
Pu as a tracer or yield-determiner.
242
236
In June 1972,
Pu waa substituted for
Pu to
step utilizing
reduce the background
in the 238Pu and 239-240Pu
the early
regions .
per mini
counter
y ap-
ay
METHOD
OF URINARY
ASSAY
F{)R PI.UTONIW
overall
recovery
in use today,
affords
an
of fIO 3 20 percent as determined
236
242
with
Pu (or
Pu) .
by internal
spiking
RAOIOMETRIC
tLEASUREf.fENT
1
~
:
procedure
RAOIOCI{EMICAL SEPARATION
The procedure,
i
health
I
ted to the
I
To the best of our knowledge,
19LL, urine samples were
as of January
ashed and the alpha activ2
ity
of the ash was measured
directly.
Hmever,
we
kr]uw t!lat in 1945 urine samples were ashed and the
The measuring
flow proportional
device
used in 1944 was a gas
alpha counter
of unknown
efficiency
25
a background
with
of approximately
minute.
Simpson
acquired
in May 1945, were
an efficiency
gas flow proportional
operated
of 48 to 50 percent
counters,
chiefly
copper
with
and a background
lining the counting
self with electrolytic
background
body content
counters,
originally
Modifications
of about 1 count per minute.
have been written
30 counts per
of these
chamber
foil, reduced
to 0.15 —
+ 0.1 count per minute.
it-
with backgrounds
NTA procedure,
counting
in January
of microscopic
detection.
with an efficiency
procedure
cent confidence
From April
cient with a background
Acquisition
about
alpha spectrometry
In addition
trometry
cedure
to techniques
allows one to
236PU
238PU
of
,
,
counting,
neutron
neutrons
are used to produce
usually
in a thick plastic
supporting
the plutonium-containing
areaa of the plastic
equation
content.
The power
acterized
from industrial
pwer
Although
Urine
plutonium.
information
fission
The
sample.
are then etched
26
FROM BIOASSAY
recent
is available
for rates of urinary
a’
patients
an
that either
functio:
excretion
patt
data were obtained
for excretion
Use of power
functions
some
periods
based
specific
and urinary
tion in man given plutonium
on t:
expres:
plus fecal ex
citrate
over a per
of 5 years:
ERU = 0.002 t4”74
ERU+
and
where
f = O.OO8
ERU and ER
injected
U+f
dose excreted
(Eq .
t4”94,
(Eq .
improve-
computer
represent
the fraction
of
per day and t the days f
lowing exposure.
Following
a single
one can estimate
exposure
the body burden
from measurement
at a known
tim
(Q) at time of
of a 24-hour urine
at a later time (t).
SF
Using Eq. 1
the relation
TECHNIQUES
of internally
times,
More recent
exponential
latter data give the following
pro-
material
assay data are used as the basis
In more
the amount and re
suggest
most of the human
cha
can
in terms of sensitivity.
the body burden
functions
compartments.
or multiple
rate to b
ing the first 140 days after injection,
to 5 years.
La
is often used to
can be used to fit the observed
exposure
determining
function
exposures
function
men collected
OF BODY BURDEN
excretion
by both decreasing
rate from various
this system is said to offer a considerable
ESTINATES
in 1945.5
a simple power ’funct
a set of exponential
can be quantitated by use of optical means or spark
3
counters.
Although not in wide use at present,
ment over others
injection
to relate urinary
approximate
of short
In the lat-
irradiation.
fragments,
damaged
plutonium
mod
were given plutoniu
data to derive
such as alpha spec-
also in the urine by a track”etch
following
ter system,
In use
which
isotopes
and proportional
be measured
and a back-
system with electronic
capability,
measure simultaneously
239-240PU
~d 242PU
,
equip–
1967; the proce-
count per minute.
is an 8-detector
data processing
effi-
count per
of 27 percent
of human subjects
These persons
yses of the data from the original
of all samples by
after January
an efficiency
ground of O.OO4 ~ 0.003
presently
(50 per–
of alpha spectrometric
in 1966 led to measurement
dure yields
The
counters
of 0.01 —
+ 0.006
from studies
citrate by intravenous
count
45 percent
tained
used these
1966 to
scintillation
were
ar
at least in part, upon the systemic
the
level) of about 0.05 disintegra-
1967, zinc sulfide
minute.
limit
in the early days, the procedures
The
of electronic
of 0.005
had a sensitivity
were used; these devices
ment
instead
of 50 percent.
tion per minute per sample.
January
1957, involved
This gave a background
per minute
overall
tracks
practiced
expectancy.
efficiency
of about 0.1 count per minute.
adopted
of computerizes
or to hand calculations
elimination developed by Langham and c
4
This model was derived from data ob
leagues.
1957, were sup-
49 percent
to
to the convenience
wh~
and analysis
urinary
in continuous
at 48
However,
reduction
based,
in 1952 by four NMC gas flow proportional
operating
one resorts
the
plemented
counters
at a given time after contaminate
or at the time of contamination.
These
counters,
use until
to relate urine assay data t
ERU = U/Q,
(Eq.
for
deposited
programs
where U is the amount
24-hour urine
sample
of plutonium
measured
at time t, then
in
data to t
clearance
(Eq. 4)
Q = 500 utO” ’4.
:amination
ter, whethe
S&stitution
Iterized da
of knmn
values
ures are
!nic model
~.c.,
m and
as
COl-
data ob-
total-body
Illws
comt
rate,
he body burden
(QR) at any time t following
may be calculated
lamination
coefficient
lutonium
uts as a summation
te to bod~
iw
sed to
eleased
ona char-
Iepend on manY
ecent anal
multiple
in evaluating
,urcs has been the problem
and rele~
re–
organs
human
of rese~Oirs
(not bone)
to the circulatory
expo-
eposited
either the
he body via urinav
in Other tissues
may be described
as the sum of
is relative
to elapsed
lung rather
than time since inhalation.
are obtained
u
= 0.002
is QO
e ‘At (R-
f o
t)-0”74dt.
(Eq. 7)
is subsequently
and ultimately
continuous
Unfortunately,
lost from
release
for individual
values
expansion
of the exponential
term and solving until
tained dur
lized by Healy,7 has been built into models by
8,9
The rate of
everal groups Of investigators.
(1) rate of transfer
periods U1
rinary
(As), and (2) rate of loss via ciliary
ed on the
hronfcally
of plutonium
can be estimated
the series
first form-
in persons
from Eqs. 1
me~hsnisms
nd 2 by summation of individual
administrations.
as i.
seal excre
ealy ’s model regards
insoluble
excretion
r a period
lum in the lung as a reservoir
~rmal body metabolism
lutonium
(Eq. 1
(Eq. 2
yet continually
into the bloodstream.
regarding
IY Portion
of the lung or body;
Lcles translocated
the position
:ovided the rate of solution
~ days fol
fstemic circulation
lrine spec]
lgEq.
1 SI
fractional
the
into
assumes
model
develOped
assumed
expressions
circulation
clearance
that As was the same
were derived
and for the amount
after initial
for fecal
of plutonium
1 shrws the calculated
in blood.
relation
between
I
,rlSYSTEMIC E XFOSURE MOOEL
—Y=0.00ST-0.74
to-~ .
\
LUNG EXPOSURE MODEL
~
:
+
z
~
1U
~
x
w
IO-4~
----
.-
Oo&L’[R-tr0.74
----- k,=O.01
(1/2.69
--0--k,
\
j
Eu=0.002ks
----”
-+
.
OAYS)
=0.00 I(T/2 =693 DAYS)
~
10-S-
clearance
E
>
of an
,O-*
lount (Q ) of insoluble
o
plutonium
is:
Q = Q. e-~t.
(Eq. 3)
\
(Eq. 5)
10-~
!00
Ired in a
rate
G
~
(Q) in the lung at time t follow-
Ig acute deposition
Healy
L
par-
The model
the systemic
transfer
of two components:
into the systemic
in
removal per unit time frOm the
Ing and then utilizes
? Langham. 10
The quantity
therefore,
is theasme.
Similar
Figure
of plutonium
and entry
(A).
The overall
to be composed
releasing
ss those in the lung,
?tion of t’
time of
from
from the lung to lymph nodes
thave in the same manner
Iown time,
pluto-
The model has no
WMtraints
constant
isolated
converges.
(A) was thought
and must
of k, R, and t by
ound plutonium into the body
fluids,
of
Eq. 7 is not integrable
be solved
on pattern
relatively
after inhala-
form.
The concept of slow,
expressic
from the
Using R
(Eu) is:
functions
exposed
(t)
R
E
the
and fecal excretion.
or fecal excretion
Time
time since transfer
rate
is
shown in Eq. 1,
rates from each increment.
system at rates that
plutonium
transferred
to the function
tion, the excretion
that are slowly
(Eq. 6)
that each increment
as the time urine samples
of PlutO-
OdY, particle size, and physiochemical
ents and
trans-
as:
Q. e-At.
the total excretion
in-
fsctors such as location within
his SIOWly translocated
is
according
the excretion
process.
r functiol
in various
Assuming
excreted
by using the total
and assuming
A major difficulty
Langh,
a =
Similarly,
,eated exposure
f short li
5.5
burden
or activity).
~ss,
circulation
for t and u
at time
one to estimate
,f ,,xpOsure in the same units that are used for U
Aations
One can then describe
mechanisms.
fer to the systemic
,e overall
elimination
Ith solubilization
rculation
rate (X) actually
and tranafer
and discharge
from the lung by Ciliary
lot
TIME AFTER EXPOSURE
represents
to the systemic
10’
Fig. 1.
10’
104
u
I&
(CAYS)
Fractional urinary excretion as a function
of time after acute exposure based on the
systemic and lung exposure models.
27
predicted
*
urinary
rate
excretion
and time, assuming
various
rates of exponential clearance from a non11
systemic reservoir.
The solid line represents the
systemic
which
exposure
model
is the basis
model. ‘2’13
(e.g.,
systemic
half times),
27 years
following
industrial
closely
exposure.
exposures
during employment,
excretion
to about
to
curves which
plutonium
are
body
for persons with
who somtimes
only at relatively
and the
It is important
for estimating
In real life, except
burdens.
urinary
corresponds
that these are idealized
used as the bases
times
the lung model
model both yield similar
at 104 days, which
appreciate
tained
of the PUQFDA computational
Even for slow lung clearance
693-day
values
from the lung)
(no transfer
can be followed
urine samples
infrequent
can be obThis
times.
iS
also true in the case of some UPPU Club members who,
although
atively
exposed
in 1944 or 1945, provided
few urine samples
27 years.
to estimate
To date, the number
body burdens
study have ranged
REFERENCES
2.
3.
4.
5,
6.
W. Lsngham
rel-
the intervening
of urine samples
for the subjects
and E.
used
of this
from 5 to 125 for different
viduals.
1.
during
indi-
—
ium Lung
nd. Hyg.
termination
surements Of ‘
ent of Radio.’
—.
mic Energy
~
603.
i
APPENDIX
C
\
“Evaluation
g Systemic
. ~,
58
MEDICAL
{
‘
FOLLOW-UP
!;,.xi[lllillx
in tf,e spring of 1942, patient No. 2
The Applica.’
Determinati~
vas ,.xpos,IdLO uranium halides while attempting to
opes,” Brit.
rt V.
rcd!lc,,(]r.]nl~lm
tl,trafluoride to the metallic state.
P1lL [:!!IC‘~<,.:, one of several
erties of
urden in
ty in Man
y, Vienna,
th{, 1’~)1 xr~~ip, wOrked
nonmilitary
at LOS Alamoa
members
from February
He subsequently
19h~4, L();,(,x,,st16, 1944.
worked
otb~,r ins~.Jll.ltions where he was not exposed
rwiluacc
M-73 4
nium Body
mos Sci (April
was ,Ixpos,.
d 10
nium
powder
wictl
at
chlo-
in hot-pressing
ura-
workc.ciWILII c:lta]ytic agents but had no significant
704 Code
nas”
expusure
exposrd
chlorine,
arsenic,
as well aa compounds
mater-ials were weighed
in the open in crucibles
ti]at were evacuated
and then fired.
were
the benefit
opened without
boxes .
In 1960, he worked
with
a vacuum system but probably
toxic materials.
in
the
to
dcL(!ct
Since
manufacture
cadmium
or dryselenite
was not exposed
in 1969 confirmed
no Jetcctable
examination
lesion was noted
A previous
196(1 !Iad been normal.
used
in 1966, a
The follow-up
in size.
examination
consultation
pllvslci,ins, the individual
0! [l)..AE(:’s Division
pO[ilIIL
4 hospital
~
was
admitted
doubled
of about
between
attending
concerned,
and staff
of Biology
United
During
dov.,, !),.IJ,*Ssubjected
tests verified
ography
indicated
or deposition
sion since
perform
and Medicine,
States
CO a series
several
of diagnostic
lesion
Fiber-optic
growth.
changes
findings
located
of
in the
indi-
in the lung within
Cytological
small
study
by pinch biopsy was also neg-
no intrusion
insufflation
radi-
on the bronchial
1
tree
defects.
of the demonstrable
1965, the attending
lobectomy,
of the tumor and regional
growth of the lephysicians
Histological
lung, regional
for radioactive
assay and radiographic
Histologically,
the neoplasm
cells.
nodes were perfectly
signs of cellular
laboratories
studies.
embryonic
and epi-
the regional
normal histologically
damage
despite
benign
cells)
adult cartilaginous
Interestingly,
and
lymph
was a classical
from residual
considerable
to
sections
lymph nodes were made,
and bone were sent to several
(derived
decided
and on MSy 17, 1971, the
of the tumor, normal
thelial
from
Tomo-
bronchoscopy
right lower lobe was removed.
containing
speci-
could be compat-
the previous
of the tantalum
a simple
Patient
the
for further
the following
which
bronchial
simple
obtained
Results
and brush
in cells exfoliated
(to about 3 mm).
ative.
based on
lymph
with no
the relatively
high
radioactivity.
on May 4, 1971, to a large
in tb,. eastern
di,]p:>os
tic st,,dies.
diameter
washings,
process
cated no abnormal
cytoland lung
There were some indications
tree.
demarcated,
hamartoma
showed
In a roentgenogram
in size and then had an outside
Following
made in
the lung abnotncality which
change
graphic
a well
sputum
bronchoscopy,
examinations
ible with an underlying
nodes,
in the right
chest roentgenogram
tak..n in ?larch 1971, the lesion had nearly
,
to
instruments
the bronchial
samples
the medical
coin-sized
luwer llm~.
5 (m.
in
1965, he haa been involved
electronic
bronchoscopic
Because
hydrocarbons.
During
small,
of
The crucibles
of hoods
function,
nxms showed no metaplasia
of specimens
of
Very often these
and antimony.
sputum,
pulmonary
inaufflation,
Cytological
tomography.
bronchioles
In 1954, he was
10 toxic chemicals.
to so(iium vapors
tests including
o13Y, tantalum
right lower lung.
In 1952, he
I]ardening agents.
NO. 2
of an inflammatory
to
oxide and beryllium
I>c, ryllium
[n 1948, tw was engaged
rfd{,.
3s
Hm.rever, late in 1946, he
fmat<rials .
iv~,
of
OF PATIENT
returned
No. 2 is currently
to Los Alamos with
UFPU group
for additional
in good health
other members
study in November
We believe
it is worthwhile
is concern
and interest
to point
1971.
out that there
for these subjects
though uany years have passed
and
of the
even
since they worked
with
I
29
plutonium.
Perhaps
patient
pie, as approximately
his 6-month
30
28 years have elapsed
involvement
days of the Manhattan
No. 2 is a good exam-
with plutonium
Project.
since
during
This. kind of
the
information,
experience
even though very limited,
of the most relevant
ing value judgments
formulating
where
inadequate
risk evaluationa.
is human
kind for establi
data exist
is human
jr establish.
Ita exist
fOr
i
APPENDIX
RADIATION
DETECTION
EQUIPI+ZNT FOR IN VIVO ~ASUREMENT
rh~ three foil Owing types of radiation
lny, ,,lu;pment
are
currentlyused to
6
; qll.111(
![.;Of plutonium i.n the bOdy:
detect-
estimate
(1)
the
proportional
i’
~o,,,,L,r,.:
(2)
thin
sOdim
iOdide
crystals
and
dual
Al-
~
OU,i
IIHnIItiide;
and (3) Cesium iodide cwstals.
)
tht,t,s,h
thi>s~
instruments
are Often called “lung”
co(lr~t,,r::
, they cannOt distinguish
between
ac( iv,.!~:~terialsin the pulmonary
ad
#uL..
IrlIn effort tO
thickness.
Each detector
coincidence
system,
background
energy
tis-
partic-
ilar MDA values
ities
occupational
ni!ml or ton~aminsnt
fonm>d
bv
d(~cay
of
rays
from
plutO-
241m
radionuclides such aa
241p”
The radiation energies
.
roughly
techniques
Measurements
counting
from 241Pu and the 60-Kev
must b,> differentiated
gamma ray from
241ti
also emitted by
MDA’s
the commonly
burden,
chest
Livermore
in the range of
accepted
one must
16-nCi
carefully
thickness.
are used for this purpose
esti-
Ultrasonic
at LASL.
must be made also in “low-background”
chambers
constructed
of massive
iron
shielding.
REFERENCE
‘1’llv
system used at the Los Alsmos
Scientific
1.
to measurein ViVO deposits of plutonium
In our s,,bjects is comprised
of two combined
tals , Nal backed by a 50-ImIICSI
which
lung
at other facil-
from those given off by
plut unl,,m.
Laboracon
the body
The MDA at the 95 per–
at the Lawrence
To achieve
mate an individual’s
Lx-rays
241
Am.
x-rays
of
from higher-
from within
have been obtained
one-third
of great(,st interest are the 17- to 20-Kev uranium
Lw-energy
scatter
originating
(for example,
mens,lrt, L(,w-t,nergy
gamma
as an anti-
in a suppression
and in the local environment.
ul.]rly in [be hilar lymph nodes, an intraesophogeal
1
All of these instruments
prut,,.is t,,,in~developed.
or
functions
resulting
caused by Compton
radiations
Laboratory).
x-rays
OF PLUTONIUM
cent confidence level for this system averages about
239
Pu for a 30-minute counting period.
7 nCi
Sim-
radio-
lymphatic
plutonium,
localize
D
crystal,
1s about 125 mm in diameter
crys-
K. L. Swinth, J. F. Park, and P. J. Moldofsky,
“Counting Plutonium in the Tracheobronchial
Lymph Nodes,” Health Phys. Q,
899 (1972).
each of
and 3 mm in
\lh
.. \
31
..?