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7 Distribution of Pesticide Residues in Human Body Tissues from Montgomery County, Ohio M A R Y L . S C H A F E R and J E P T H A E . C A M P B E L L Milk and Food Research, Robert A. Taft Sanitary Engineering Center, Public Health Service, U.S. Department of Health, Education, and Welfare, Cincinnati, Ohio
Blood,
omental fat, and organs of 19 cadavers,
accidental Southern using
deaths Ohio,
during
1964-65
body
All samples
burden
equipped
contained
of these
two
range from 22 to 300 mg. Eighteen ranging from
of from
the
cadavers
2 to 31 p.p.m..
observed
between
other 18
In
capture The
total
estimated
to
was present in the
fat.
contained
was blood
concentrations
and fat concentrations index,
fat and blood assays.
as a member
hydrocarbons electron
plus DDE.
compounds
A correlation
a blood assay of 94 p.p.b. rejected
DDT
Over 95%
2 to 58 p.p.b.
with
from County,
were assayed for chlorinated
gas chromatographs
detectors.
resulting
in Montgomery
ranging
R2, of 0.77
One
cadaver
and fat assay of 5.4 p.p.m.
of the population
represented
was with was
by
the
cadavers.
our laboratory studies on catfish (4), measurable concentrations of endrin were observed in the blood of those exposed to endrin.
With
exposure levels sufficiently high to cause death, there was a significent increase in blood endrin concentrations. Richardson (I)
In 1964
Brown, Hunter, and
reported a correlation between the levels of dieldrin in
blood and clinical signs of poisoning in humans and suggested the usefulness of the blood test to diagnose marginal exposure.
The present
investigation was undertaken to determine the relationship between the levels of D D T in blood and the total body burden of humans, so that the total body burden for this pesticide may be estimated from analysis of blood. In an attempt to study this relationship in persons subjected to 89 Rosen and Kraybill; Organic Pesticides in the Environment Advances in Chemistry; American Chemical Society: Washington, DC, 1966.
90
ORGANIC
PESTICIDES I N T H E E N V I R O N M E N T
normal environmental exposures, cadavers resulting from accidental deaths were used. A total of 19 cadavers from Montgomery County, Southern Ohio, was studied. They included six females and 13 males ranging between 18 and 76 years of age. The tissues and body fluids that were assayed included blood, omental fat, liver, kidney, brain, heart, and gut. A l l samples were assayed according to the method developed i n our laboratories ( 6 ) . After saponification of the fat, the pesticides were extracted into hexane. Since D D T is quantitatively dehydrohalogenated to D D E during alkaline hydrolysis, all results reported as D D E are the sum of D D T plus D D E . The hexane extracts were resolved and assayed in gas chromatographs equipped with electron capture detectors. In addition to columns packed with D o w 11 plus E p o n coated on Fluoropak 80, at least one replicate from each sample was assayed on a column packed with 3 % Q F - 1 on anakrom A B S . This latter column showed excellent resolution for dieldrin and D D E , as shown i n Figure 1.
I
I
I
I
I
I
I
I
I
I
I
I
Electron capture 5ft.x '/4inch, 3%QF-1 on 50/60 onokrom ABS Column temp: I58 C Injection temp : I85 C Ν £ flow rote : 88 ml /min. Injection volume : 5μΙ hexane solution
Detector Column
ioh-
#
9
20
0.24 Ng ALDRIN
Κ 30 Ζ
2
0.6 Ng 0.6 Na DDE DIELDRIN
UJ40 OC
Hi 50 Ο OC
0.6 Ng ENDRIN
ο
«60 70
90j
I
I
1
I
I
1
8
I
I
I
12
I
I
1
16
1
1 I
20
RETENTION TIME, min. Figure 1.
Chromatograph of standard solution of pesticides
Rosen and Kraybill; Organic Pesticides in the Environment Advances in Chemistry; American Chemical Society: Washington, DC, 1966.
7.
SCHAFER
A N D
91
Distnbution in Human Tissues
C A M P B E L L
Duplicate 10-gram blood samples for each cadaver were saponified and assayed. The concentrations of D D E ranged from 2 to 94 p.p.b. Chromatographs of the two extreme values are shown i n Figure 2. A d d i I
I
I
I
I
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I
I
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I
I
I
5jil Hexane extract (5mg Whole blood)
RETENTION TIME,min. Figure 2.
Chromatograph of hexane extracts of whole blood
tional studies to confirm the identity of the D D E peak included the use of a thin layer chromatographic technique (7) and the comparison of the retention times for the hexane extracts of the blood sample and a standard solution of D D E on two additional column packings i n which Apiezon L and a mixture of Q F - 1 plus X E 60 were used as liquid phases. For recovery studies, one of the duplicate samples from each of two cadavers was contaminated with sufficient D D T to produce a concentration of 40 p.p.b. Assuming 100% recovery of the added D D T , the duplicates agreed within the standard deviation observed for replicates of samples. This was less than 350/1000. Portions of omental fat were rendered on a steam bath and 0.5- to 1.0-gram portions of the rendered fat were assayed. F o r recovery studies, two of the four replicate fat samples from one cadaver were contaminated with sufficient D D T to produce a concentration of 2 p.p.m. Assuming
Rosen and Kraybill; Organic Pesticides in the Environment Advances in Chemistry; American Chemical Society: Washington, DC, 1966.
92
ORGANIC
PESTICIDES
IN
T H E ENVIRONMENT
100% recovery of the added D D T , the four replicates agreed within the standard deviation for replicates of samples, w h i c h was less than 100/ 1000. The concentrations of D D E found i n these samples ranged from 2 to 31 p.p.m. The data for blood and fat are summarized i n Table I. Table I. D D T plus D D E in Human Tissue No. of Persons
Blood, p.p.b.
Fat, p.p.m.
5 9 4 ]
< 5 5-20 28-58 94
2.2- 4.7 3.3-13.8 9.4-31.0 5.4
Data for individual cadavers, along with the available personal history, are given i n Table II. Cadaver 19, with the high blood level and low fat level, obviously is different from the remaining samples.
H e was a
supervisor or a foreman at a manufacturing plant, white, 64 years old, and weighed 200 pounds.
H e apparently blacked out while driving a
car, ran off the roadway, and struck a power pole. There were no skid
Table II. Personal
Occupation Teacher Bank teller Retired Unknown Unknown Dentist Retired Teacher Unknown Housewife Housewife Housewife Construction worker Foundry employee Unknown Unknown Garbage collector Cement worker Factory foreman
Coroner's Statement
Cause of Death Suicide Suicide Natural causes Homicide Accidental Unknown Natural causes Natural causes Homicide Traffic accident Traffic accident Homicide Suicide Traffic accident " Homicide Traffic accident * Natural causes Homicide Traffic accident · ·
Gun shot Gun shot Heart condition Carbon monoxide Multiple degenerative diseases Influenza
α
6
Carbon monoxide
Heart condition c
" Driver of car that caused accident. Passenger in car involved in accident. Lived 3 days after accident. b c
Rosen and Kraybill; Organic Pesticides in the Environment Advances in Chemistry; American Chemical Society: Washington, DC, 1966.
7.
SCHAFER
A N D
C A M P B E L L
Distnbution in Human Tissues
93
marks. H e lived 3 days after the accident. The pathological findings referred to small bowel hemorrhage. During the early spring of 1964, blood samples from 25 employees at Taft Center were assayed using the procedure described above. Blood samples from 20 employees of the Lower Mississippi River Project, P H S , D H E W , 16 located in Baton Rouge, L a . , and four in Memphis, Tenn., were assayed in 1965-6. A l l samples contained detectable concentrations of D D T plus D D E . A comparison of the data for these groups with those from Montgomery County is shown in Table III. Fortunately, blood assays were obtained on five of the individuals from Baton Rouge in M a y 1965 and again in January 1966. For four of these individuals with assays in the range of 21 to 30 p.p.m. D D T plus D D E , the samples taken 7 months apart agreed within the precision of the method. One individual with a blood concentration of 40 p.p.b. in M a y 1965 showed a significant decrease to 19 p.p.b. in January 1966. The mean concentrations of D D T plus D D E in the omental fat, 5.1 p.p.m., and the average value, 9.0 p.p.m., are less than the mean storage level of 12.7 p.p.m. reported for the U.S. population in 1961-2 by Quinby History of Subjects Cadaver No. 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19
Blood, p.p.b. 2 2 3 3 4 8 8 9 11 13 13 15 17 20 28 34 44 58 94
Fat, p.p.m. 2.4 2.9 2.3 4.7 2.2 3.3 4.6 3.5 7.1 5.0 5.5 5.3 13.8 6.0 23.4 9.4 31.0 30.2 5.4
Age
Sex
Ht., In.
Wt., Lb.
Rate
40 18 76 34 56 32 72 25 35 41 52 31 47 40 28 21 38 48 64
F F F M M M M M M F F F M M M M M M M
68 63 58 73 70 72 70 70 75 63 62 63 68 72 link. 70 68 72 73
140 110 145 180 170 180 150 260 190 130 135 95 145 180 Unk. 205 150 150 200
W W W N W w w w N W w N W w N W N N W
Rosen and Kraybill; Organic Pesticides in the Environment Advances in Chemistry; American Chemical Society: Washington, DC, 1966.
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ORGANIC
PESTICIDES IN
T H EE N V I R O N M E N T
et al. ( 5 ) . However, these workers reported data of samples assayed by a colorimetric procedure which according to Dale and Quinby (2) shows incorrectly high values as compared to those obtained with gas chromatographic procedures. Table III. Frequency Distribution of D D T Concentration in Human Blood from Four Geographic Locations Blood, (P.P.B.)
Montgomery County, Ohio
