MEASUREMENT
ATMOSPHERIC
COMMON
OF
CONCENTRATIONS
HOUSEHOLD
A PILOT
ROBERT
G. LEWIS,
OF
PESTICIDES:
STUDY
ANDREW
E. B O N D
U.S. Environmental Protection Agency
Research Triangle Park, NC 27711, U.S.A.
DONALD
E. J O H N S O N ,
and J. P . H S U
Southwest Research Institute
San Antonio, T X 78284, U.S.A.
(Received April 1987)
Abstract. Air concentrations of 28 of the most c o m m o n l y used household pesticides were measured inside
nine h o m e s in Jacksonville, Florida, and compared with corresponding outdoor levels. The households
selected were sorted into three categories according to the degree o f pesticide indoor usage. Personal air
monitoring was also performed on one resident of each household by m e a n s of a portable sampler, which
was kept with the person at all times. Five of the pesticides were found in the air inside o f the majority
o f the homes at concentrations as high as 15 ~tg m - 3 (average concentrations, 12 ng m - 3 to 2.4 ~tg m - 3 .
Indoor levels were generally one to two orders of magnitude higher than surrounding outdoor air levels
and personal air measurements were within + 50~/0 of corresponding indoor values. All samples were
collected over 24-hr periods on polyurethane f o a m and analyzed by capillary column gas chromatography
with mass spectrometric a n d / o r electron capture detection.
1. Introduction
Many different kinds o f pesticides are commonly used in and around the home to
control pests ranging from termites to Japanese beetles and fungi to crabgrass.
Depending upon the manner in which they are used or applied, human exposure to
these pesticides may occur through respiration, ingestion, dermal absorption, or any
combination thereof. Very little human exposure data is available which can be used
to estimate potential health effects due to household pesticides or the relative
importance of the different routes of exposure. While occupational exposures to
airborne pesticides have been well documented (Wolfe, 1976; Bristol et al., 1984),
few studies have been conducted to determine typical air route exposures associated
with the use of home and garden pesticides (Lewis and Lee, 1976; Lewis and
MacLeod, 1982). Concern over the lack of information regarding non-occupational
exposures to pesticides prompted the passage of a congressional appropriations bill
in 1985 which provided funds for a total exposure assessment study by the U.S.
Environmental Protection Agency.
As a result, a study called the Non-occupational Pesticides Exposure Study
(NOPES) was designed around the concepts o f the Total Exposure Assessment
Methodology (TEAM) studies previously conducted by E P A (Ott, 1985; Ott et al.,
Environmental Monitoring and Assessment 10 (1988) 59-73.
9 1988 by Kluwer Academic Publishers.
60
ROBERT G. LEWIS ET AL.
1986). The primary objective of this study is to obtain an estimation of the cumulative
frequency distributions of non-occupational exposures to home and garden pesticides through the air, dermal, drinking water, and dietary routes. Secondary objectives are to (i) obtain an estimate of the relative importance of each route to the total
exposure, (ii) identify probable sources of the pesticides, and (iii) compare indoor
with outdoor air levels.
In preparation for the NOPES project, a pilot investigation encompassing nine
households was conducted during August 1985 in an urban-suburban area of the
southeastern United States (Jacksonville, Florida) selected on the basis of high
pesticide usage. The purpose of the pilot study was to select, validate and field-test
sampling methodologies and survey questionnaires to be used in a subsequent large
study covering 260 households in two cities.
Fixed-position indoor and outdoor and personal exposure (portable sampler) air
monitoring was performed at each of eight single-family dwellings and one apartment, which were classified on the basis of questionnaire results as low, medium,
or high pesticide usage households (three in each category). In addition, tap water
samples from each house were analyzed. A limited number of dermal exposure
measurements were made by analysis of pre-extracted white cotton gloves worn by
selected individuals during application of pesticides. Samples of each o f these media
were analyzed for each of the 33 chemicals listed in Table I. Included in this list are
28 pesticides which were selected on the basis of present-day or historical usage.
Three other high-use pesticides, glyphosate, acephate and p-dichlorobenzene, were
originally targeted for the study, but were dropped because of special sampling or
analytical requirements. The two pesticide metabolites or oxidation products (oxychlordane and heptachlor epoxide), a component of technical chlordane (trans-nonachlor), and two polychlorinated biphenyls (Aroclors | 1242 and 1260) were added
because they could be easily fitted into the monitoring and analytical scheme. In this
paper, only the air monitoring portion of the pilot study will be discussed.
2. Methods
Two sampling systems were used in this study. For most o f the area sampling indoors
and outdoors and for all of the personal air monitoring, a low-volume (LV) sampler
developed by Lewis and MacLeod (1982) was employed. The components of the LV
sampler consisted of a constant-flow pump (Du Pont Model P-4000A or Alpha-l)
and a glass cartridge containing a 22-mm diameter x 7.6-cm long cylinder of polyurethane foam (PUF). In advance of the pilot study, 24-hr sampling efficiencies at
3.81min -1 were determined for each of the target chemicals at 0.01, 0.1 and
1.0 Ixg m - 3 of air by using the procedures of Lewis and MacLeod (1982). The overall
sampling and analytical efficiencies were 70-100070 for most of the compounds. PUF
plugs were spiked at two levels (550 g and 5500 ng per plug) with hexane solutions
of the chemicals, allowed to dry in a clean atmosphere for 1 hr, and extracted to
determine static recoveries. Collection efficiencies were determined by means of a
M E A S U R E M E N T OF A T M O S P H E R I C C O N C E N T R A T I O N S OF C O M M O N H O U S E H O L D PESTICIDES
61
TABLE I
Chemicals monitored
Compound
Type of
pesticide
Household uses leading to
potential human exposurea
Chlorpyrifos (Dursban |
Insecticide
Pentachlorophenol
Propoxur (Baygon|
Fungicide,
insecticide
Insecticide
Disinfectant,
fungicide
Insecticide
Control of mosquitos, cockroaches and
other household insects; turf and
ornamental insects; fire ants, termites, and
lice
Exterior wood preservative
Resmethrin
Insecticide
Dicofol
Insecticide
Captan
Fungicide
Carbaryl (Sevin |
Insecticide
Lindane (7-BHC)
Insecticide
Dichlorvos (DDVP)
Insecticide
2,4-D esters
Malathion
Herbicide
Insecticide
Permethrin (cis and trans)
Insecticide
Heptachlor
Aldrin
Dieldrin
Ronnel
Diazinon
Insecticide
Insecticide
Insecticide
Insecticide
Insecticide,
nematicide
Methoxychlor
Insecticide
Atrazine
Q-Hexachlorocyclohexane (ct-BHC)
Herbicide
Insecticide
Bendiocarb (Ficam|
Insecticide
Folpet
Fungicide
Chlordane
ortho-Phenylphenol
Subterranean termite control
Household disinfectant
Control of cockroaches, flies, mosquitos;
lawn and turf insects
Control of flying and crawling insects;
fabric protection; pet sprays and
shampoos; application on horses and in
horse stables; greenhouse use
Control of mites on fruit, vegetable, and
ornamental crops
Seed protectant; fungal control on fruits,
vegetables, and berries
Control of insects on lawns, ornamentals,
shade trees, vegetables, and pets
Seed treatment; insect control in soil, on
vegetables, ornamentals, and fruit and nut
trees
Household and public health insect control;
flea collars and no-pest strips
Postemergent weed control
Insect control on fruits, vegetables,
ornamentals and inside homes
Control of flies, mosquitos, ants,
cockroaches, garden insects
Subterranean termite control
Subterranean termite control
Subterranean termite control
Fly and cockroach control
Control of soil and household insects,
grubs and nematodes in turf; seed
treatment and fly control
Control of insects in garden, fruit, and
shade trees
Weed control
Manufacture and use discontinued in U.S.;
ubiquitous in air, residue from lindane
Household, ornamental, and turf insect
control
Fungus control on flowers, ornamentals,
seeds, plant beds; paints and plastics
62
ROBERTG. LEWISET AL.
Table I (continued)
Compound
Type of
pesticide
Householduses leading to
potential human exposurea
Chlorothalonil (Bravo|
Fungicide
Dacthal
Herbicide
Broad spectrum fungicide; wood
preservative; paint additive
Selectivepre-emergent weed control on
turf, ornamentals, and vegetable crops
Oxidation product of chlordane
Oxidation product of heptachlor
Component of chlordane
Use discontinued in U.S. after I972
Used in electrical transformers and
capacitors until 1976
Oxychlordane
Heptachlor epoxide
trans-Nonachlor
p,p'DDT
PCBs (Aroclors~ 1242 and 1260)
--
-
-Insecticide
-
-
a Source: Farm Chemicals Handbook, 1985, Meister Publishing Co., Willoughby, Ohio.
vapor generator (Lewis and MacLeod, 1982) where possible. For compounds which
could not be vaporized, dynamic retention efficiencies were determined by drawing
purified dry nitrogen through spiked P U F plugs for 24 hr. Previous studies by Lewis
and MacLeod (1982) have shown the latter to be good approximations of vaporphase collection efficiencies.
At selected households, a high-volume (HV) air sampler developed by Lewis et aL
(1977) was operated for 24-h periods at 2251 m i n - 1 in order to collect samples large
enough for exploratory investigations. This HV sampler was modified for indoor use
by placing the sampling module on a tripod and locating the p u m p outside the
dwelling (Wilson et al., 1985). The H V sampler was not evaluated for all of the
chemicals in Table I. However, it had been previously evaluated for several of these
compounds and others of similar chemical structure (Lewis et al., 1977).
The P U F plugs were precleaned by Soxhlet extraction with acetone followed by
5~ diethyl ether in hexane as previously described by Lewis et al. (1977), vacuum
dried, and loaded into the appropriate glass sampling cartridges under clean laboratory conditions. The cartridges were wrapped in hexane-rinsed aluminum foil and
stored in carefully cleaned glass jars padded with extracted P U F for transport to and
from the sampling sites in freezer chests cooled with dry ice. Exposed filters from
the HV samplers were also wrapped in prerinsed foil and placed in the jars with the
P U F cartridge. Disposable latex surgical gloves and prerinsed tongs were used for
handling the sampling cartridges when P U F plugs were loaded and unloaded in the
laboratory and for attaching them to the sampling systems in the field.
Three different sets o f ambient air samples were collected over 24-hr sampling
periods in each usage category. These are summarized in Table II. All sets included
a primary group of samples, comprising an inside LV sample (3.81min-1), an
outside LV sample (3.81 r a i n - 1), and a personal exposure (PE) sample (3.81 m i n - 1).
One house in each category was selected for a distributed air volume (DAV) set
(Walling, 1984), which consisted of two additional inside LV samples (1.2 and
2.01 r a i n - i), two additional outside LV samples (1.2 and 2.01 m i n - t), and inside and
MEASUREMENT
OF ATMOSPHERIC
CONCENTRATIONS
OF COMMON
HOUSEHOLD
PESTICIDES
63
TABLE II
Type and distribution of air samples
Sample type
Usage category (house number)
Low
Primary samples, LV (3.81min 1)
inside
outside
exposure
2
3
1
2
3
1
2
3
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
Replicate samples, LV (3.81min- J)
inside
outside
exposure
High-volume air samples (2251min-~)
inside
outside
inside, duplicate
outside, duplicate
High
1
Duplicate samples, LV (3.81min- J)
inside
outside
Distributed air volume samples
inside (1.21min- 1)
inside (2.01min- 1)
outside (1.21min- ~)
outside (2.01min- ~)
Medium
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
X
x
x
x
x
x
x
x
x
X
X
x
x
x
x
x
x
outside H V samples (2251 m i n - i ) . Duplicate (collocated) inside a n d outside H V air
samples were collected at the m e d i u m usage D A V house. The second h o u s e in each
usage category was picked for duplicate s a m p l i n g . Inside a n d o u t s i d e LV
(3.81 m i n - l) duplicate samples were collected s i m u l t a n e o u s l y with the p r i m a r y g r o u p
at these h o u s e h o l d s . T h e third house in each category was designated for replicate
s a m p l i n g , in which a second g r o u p o f samples was collected d u r i n g a s u b s e q u e n t
24-hr period at least 24 hr after the collection o f the p r i m a r y g r o u p o f samples.
I n d o o r air samples were collected in a n area o f high daily family activity, such as
a kitchen or f a m i l y r o o m . O u t d o o r air samples were collected in or a d j a c e n t to a n
area o f high-traffic o u t d o o r activity (e.g., o n a side p o r c h or patio).
I n d o o r s , all LV fixed-station samples were collected with intakes p o s i t i o n e d
h o r i z o n t a l l y at heights o f 1.0 to 1.6 m a b o v e the floor. O u t d o o r s , LV samples were
a t t a c h e d to v a r i o u s s u p p o r t s with intakes generally a b o u t 1.5 m a b o v e g r o u n d a n d
o r i e n t e d d o w n w a r d . T h e H V s a m p l e r i n t a k e was oriented u p w a r d a n d located 1.5 m
64
ROBERT G. LEWIS ET AL.
above the floor inside and 1.2 m above ground outside. Covers protected the HV
sampler intakes from dust-fall.
Personal monitors were carried by one resident of each household. During periods
of activity, this sampler was carried in a case with a shoulder strap so that the intake
was located at waist level and pointed behind the wearer. During periods o f inactivity
(i.e., when the person was not moving from room-to-room), the PE sampler may
have been located on a nearby table or counter top. The LV pumps were battery-operated only when carried on the person.
When duplicate or DAV samples were collected simultaneously with the primary
samples, LV samples were placed with a separation of 0.3 m. The inlets to the
cartridges were arranged such that sufficient distances were maintained between
sampler exhausts and inlets. HV air samplers in the DAV households were placed
in the same area as the LV samplers with a minimum separation of 2 m. Duplicate
HV samplers were separated by 1 m for the outdoor set and 2 m for the indoor set.
Exposed P U F plugs and filters were Soxhlet extracted together with 5% diethyl
ether in hexane following the general procedure of Lewis et al. (1977). The extracts
were reduced to 10 or 0.2 ml in Kuderna-Danish concentrators for analysis by gas
chromatography with electron capture detection (GC/ECD) or gas chromatographymass spectrometry (GC/MS), respectively. A 0.25-mm x 30-m DB-5 capillary column (0.25-1xm film thickness) with helium carrier gas (1 ml m i n - 1) was used for both
G C / E C D and G C / M S analyses. Temperature programming from 90 ~ (4min) to
270 ~ (4 ~ m i n - 1) for G C / E C D and 40 ~ (2 min) to 295 ~ (10 ~ m i n - l) for G C / M S
separated 32 of the 33 target compounds. Electron ionization MS with multiple ion
detection (MID) was used to confirm all compounds except chlordane and to
quantitate chlorpyrifos, which could not be separated from dacthal. An external
standard method was used for the quantitation of G C / E C D results. However,
quantitation with G C / M S / M I D was based on the use of two internal standards,
Dlo-phenanthrene and DiE-Chrysene. This analytical methodology was validated for
all of the compounds listed in Table I prior to collection of field samples. For this
purpose authentic reference standards obtained from the U.S. E P A Pesticides and
Industrial Chemical Repository, Research Triangle Park, North Carolina, were used.
Most of the chemicals could be quantitated at or below levels of 1 0 n g m - 3 in LV
samples and 1 n g m - 3 or below in HV samples.
The Du Pont sampling pumps were calibrated with a Du Pont calibrator pack
(Model P-2500B). The HV samplers were calibrated by means of a calibrated venturi
tube which was attached to the inlet. With two exceptions, an operational check and
a flow check were performed on each sampler at one time during the 24-hr sampling
period. In all cases, flows were checked at the end of each sampling period. In
addition, flow audits were conducted in the field by an independent team using two
laminar flow elements calibrated by the National Bureau of Standards (NBS). All
samplers in use during the audit period were found to be within + 507o of the set flow
rates.
Local barometric and ambient temperature values were obtained at 4-hr intervals
MEASUREMENT
OF ATMOSPHERIC
CONCENTRATIONS
OF COMMON
HOUSEHOLD
PESTICIDES
65
throughout the study period f r o m the National Weather Service. Barometric pressure
for a 24-hr sampling period was calculated by averaging the six values observed
during that period. Likewise, ambient air temperatures for outside air samples were
calculated f r o m the appropriate observations. Outdoor temperatures ranged f r o m
lows of 23-24 ~ to highs of 29-32 ~ during the study. Air temperatures for indoor
samples and exposure samples were dependent on air conditioning use and the
activity o f the monitored individual.
The nine domiciles monitored were selected f r o m a total of 38 screened and ranged
in type f r o m a mobile home to a t w o - b e d r o o m apartment to houses of up to 800 m 2
built on concrete slabs or over crawl spaces. The homes were distributed across three
U.S. census county divisions and were within 3 km of each other. A total of 74 air
samples were collected and analyzed along with six field b l a n k s . Some of these
samples a n d / o r aliquots of sample extracts were shared with a referee laboratory.
All samples were kept at temperatures below 4 ~ f r o m immediately after collection
until they were analyzed (including during shipment). All samples were extracted
within 14days and analyzed within 21 days of collection. The percent relative
standard deviation between duplicate samples collected in the field was in the 20
to 30070 range.
3. Results
There were no consistent differences in measured air concentrations f r o m simultaneous LV samples collected at 3.8, 2.0 and 1.21 m i n - l , indicating that none of the
pesticides collected broke through the PUF. Concentration values were usually very
similar at the three sampling rates (_+ 10O7o); however, differences of an order of
magnitude occurred occasionally, but in no predictable manner. As expected, somewhat fewer c o m p o u n d s were detected in samples collected at 1.21 m i n - 1. A few more
compounds were detected indoors by the H V sampler, usually at low concentrations.
M a n y more compounds were measurable in the air out-of-doors (again, usually at
lower concentrations) when the H V sampler was used. The LV sampling rate of
3.81 m i n - 1 appeared to be well-suited for indoor and personal exposure measurements.
O f the 33 pesticides and related chemicals listed in Table I, a total of 24 were
detected in the indoor air samples collected. Concentrations ranged f r o m 1.7 ng m - 3
to 15.0 ~tg m - 3 . Not detected in any indoor air sample were permethrin, resmethrin,
carbaryl, 2,4-D esters, atrazine, dacthal, and PCBs. A s u m m a r y of positive findings
is given in Table III. O u t d o o r air levels were generally much lower than indoor air
levels, ranging f r o m < 1.0 ng m - 3 to 410 ng m - 3. Personal exposure measurements
ranged f r o m < 1 0 n g m -3 to 8.8~tgm -3.
The pesticides present and their concentrations in the ambient outdoor air differed
greatly f r o m one household to another. When the LV samplers were used, only two
or three pesticides could be measured in the outdoor air. However, an average of
14 to 15 were quantifiable with the H V sampler. There was no evidence of a c o m m o n
66
ROBERT G. LEWIS ET AL.
TABLE III
Summary of pesticides found in air
Pesticides
Chlorpyrifos
Diazinon
Chlordane
Propoxur
Heptachlor
trans-Nonachlor
Lindane
Heptachlor epoxide
Aldrin
o-Phenylphenol
Dieldrin
Captan
Folpet
Oxychlordane
Malathion
Bendiocarb
a-BHC
Ronnel
Chlorothalonil
Pentachlorophenol
Dichlorvos
Dicofol
Methoxychlor
p p '-DDT
cis-Permethrin
trans-Permethrin
Number of households at which detected in air
Ir~doors
Outdoors
Respiratory
9
8
7
7
7
6
6
6
6
5
5
5
5
5
4
3
3
3
3
2
1
1
1
1
0
0
7
7
3
4
5
3
2
2
4
4
4
2
4
2
2
1
2
1
3
1
1
2
1
0
1
1
8
6
6
6
6
5
3
3
3
4
5
4
4
1
1
4
3
3
1
0
1
0
0
0
l
0
background profile for outdoor air throughout the overall study area or within given
neighborhoods. Therefore, it may not be valid to use one outdoor air sample to
represent a cluster of homes. Ideally, comparisons of indoor with outdoor air quality
should be made only for a given household and immediately adjacent property. It
should be noted that in this study outdoor samples were collected on patios or
porches to better reflect outdoor exposures around the household. Consequently,
some of the compounds found in these samples may have been emitted from inside
the home.
The average number of target pesticides found in the air inside the three households
considered to have high pesticide usage was 11, compared to an average of seven in
the medium-usage and five in the low-usage dwellings. As m a n y as 20 pesticides were
identified in the air of one high-usage household.
The most commonly encountered pesticides are shown in Table IV. The concentrations of these five pesticides were generally about one order of magnitude higher
M E A S U R E M E N T OF A T M O S P H E R I C C O N C E N T R A T I O N S OF C O M M O N H O U S E H O L D PESTICIDES
67
TABLE IV
Summary of positive findings for most prevalent pesticides
Pesticide
Air concentration, Ixgm-3
Indoor
Outdoor
Personal
exposure
Chlorpyrifos
range
meana
positiveb
0.014 to 15
2.4
9 of 9
0.009 to 0.30
0.063
7 of 9
0.056 to 8.8
2.2
8 of 9
Diazinon
range
mean
positive
0.030 to 8.8
1.4
8 of 9
0.004 to 0.41
0.097
7 of 9
0.035 to 5.1
1.3
6 of 9
Chlordane
range
mean
positive
0.078 to 1.7
0.64
7 of 9
0.036 to 0.2t
0.082
3 of 9
0.063 to 4.2
0.83
6 of 9
Propoxur
range
mean
positive
0.019 to 0.66
O.16
7 of 9
0.001 to 0.020
0.007
4 of 9
0.013 to 0.60
O.14
6 of 9
Heptachlor
range
mean
positive
0.012 to 0.36
0.18
7 of 9
0.009 to 0.059
0.025
5 of 9
0.012 to 0.23
0.088
6 of 9
a Arithmetic mean value of all positive measurements.
b Number of dwellings of 9 monitored for which at least one sample contained detectable levels of the
indicated pesticide.
t h a n those o f a n y other pesticide f o u n d in the same samples. I n d o o r air levels were
a l m o s t always o n e to two orders o f m a g n i t u d e higher t h a n o u t d o o r levels. These same
pesticides have been previously reported at similar i n d o o r air c o n c e n t r a t i o n s in other
investigations (Leidy et al., 1985; Leidy a n d W r i g h t , 1987; Lewis a n d M a c L e o d ,
1982; W r i g h t et al., 1981; W r i g h t a n d Leidy, 1982).
I n the m a j o r i t y o f cases, the same pesticides that were f o u n d to be the most
prevalent in i n d o o r air were also identified in a n i n d e p e n d e n t survey to be ingredients
o f pesticidal p r o d u c t s f o u n d at the h o u s e h o l d or used b y the o c c u p a n t s or recently
applied by professional pest c o n t r o l operators. T h e c o m p o s i t i o n o f the air inside each
dwelling a p p e a r e d to have its o w n characteristic profile i n terms o f identity a n d levels
o f the pesticides present. T h e r e was r e m a r k a b l y little d a y - t o - d a y v a r i a t i o n in the
c o m p o s i t i o n o f either the i n d o o r air o r p e r s o n a l exposure samples.
O f the n i n e s t u d y homes, seven were k n o w n to have b e e n treated for termites, six
w i t h i n the past o n e to five years. Six received p r o f e s s i o n a l i n d o o r pest t r e a t m e n t s
o n a regular basis (as o f t e n as m o n t h l y ) a n d all had inventories o f pesticidal p r o d u c t s
which were used in a n d a r o u n d the h o u s e h o l d s b y the o c c u p a n t s .
I n general, the p r e s a m p l i n g pesticide use survey d a t a a n d m o n i t o r i n g results agreed
well. T h e o c c u r r e n c e a n d c o n c e n t r a t i o n s o f pesticides were usually f o u n d to be
68
ROBERT G. LEWIS ET AL.
highest at those households designated high-use f r o m the survey and lowest at those
designated low-use. The bar graphs presented in Figure 1 show the mean air concentrations of the five most prevalent pesticides according to household use classification. The propoxur data for the low-use households is biased by high measurements obtained at one household at which the insecticide was used during the
monitoring period. The relatively high mean heptachlor concentrations for the
medium-use households are also the result of high measurements at a single home.
This house had been recently treated with the termiticide Termide | Heptachlor is
the m a j o r single active ingredient and one of the most volatile components of
Termide | Specific measurements obtained at the two households which showed the
m a x i m u m and minimum occurrence and concentration levels are given in Tables V
and VI.
With few exceptions, the personal exposure samples exhibited the same profiles
as those of the resident households. For specific pesticides, personal exposure
measurements were generally within _.+50~ of the corresponding indoor air measurements. In every PE air sample obtained, at least two-thirds of the pesticides found
were also present in the corresponding indoor air samples. As can be seen f r o m the
data presented in Table VII, an average of 81 ~ of the total personal air exposures
of the participants could be attributed to breathing the air within their homes.
TABLE V
Comparison of indoor, outdoor and personal exposure air samples from one high-use household
Pesticide
Air concentration, I.tgm -a
Indoor
Chlorpyrifos
Diazinon
Chlordane
o-Phenylphenol
Heptachlor
trans-Nonachlor
Aldrin
Captan
Ronnel
Dieldrin
Oxychlordane
Heptachlor epoxide
Propoxur
Lindane
ct-BHC
Folpet
a
Outdoor
Personal
day 1
day 2
day 1
day 2
day 1
day 2
15.0
3.2
1.7
0.39
0.16
0.10
0.055
0.037
0.037
0.035
0.033
0.031
0.046
0.012
ND
ND
6.6
1.6
1.7
0.37
0.20
0.17
0.061
0.072
0.047
0.040
0.039
0.037
0.019
ND
ND
ND
0.075
ND
0.064
ND a
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
0.016
0.160
0.047
0.044
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
0.018
5.8
1.0
0.640
0.110
0.084
0.034
0.023
0.019
0.021
0.011
0.026
0.024
ND
ND
0.012
0.190
8.8
2.1
0.65
0.50
0.042
0.039
0.026
0.028
ND
0.015
0.050
0.047
0.021
ND
ND
0.023
Not detected at ca. O.OlOixgm 3.
M E A S U R E M E N T OF A T M O S P H E R I C C O N C E N T R A T I O N S OF C O M M O N H O U S E H O L D PESTICIDES
69
The personal air monitoring data was more difficult to relate to potential exposures
associated with reported applications of pesticidal products. This may be due to the
fact that there was very little activity o f this type during the study period. OnIy one
person reported that he applied pesticides while wearing the monitor. In this case,
elevated levels of the pesticides dichlorvos and propoxur were found on the gloves
he wore, but only dichlorvos was found to be elevated in the PE air sample
5.0
4"5 i
9
Z
0
O
3.5
CHLORPYR|FOS
~'~LOW
]MEDIUM
RHIGH
F- 3.0
<[
I.- 2.5
70 2.0
0
0 1.5
Z
<
~ 1.0
IE
0.5
OUTDOOR
INDOOR
EXPOSURE
SAMPLE TYPE
4.0
DIAZINON
3.5 -
[]LOW
3.0 --
[]MEDIUM
[]HIGH
O 2.51
F<
n*
,~, 2.0
Z 1.5
0
~ 1.0
IE
0.5
OUTDOOR
INDOOR
SAMPLETYPE
F i g . 1.
EXPOSURE
70
ROBERT G. LEWIS ET AL.
CHLORDANE
~ILow
m
1.5
{
--
NMED'OM
IHIGH
9
0
Z
0
Z
0.5
--
OUTDOOR
INDOOR
SAMPLETYPE
EXPOSURE
INDOOR
EXPOSURE
PROPOXUR
~JLOW
~. 0"4r
]MEDIUM
Z
[]HIGH
0.3
Z
~Z 0.2 0
Z
0.1--
i
|
!
OUTDOOR
~
SAMPLETYPE
{
HEPTACHLOR
0.3 -- F'TLOW
N"EO'O"
IHIGH
O
~
0,2--
5
Z
0
0 0.1
Z
O
OUTDOOR
,INDOOR
EXPOSURE
SAMPLETYPE
Fig. 1. D i s t r i b u t i o n o f m e a n c o n c e n t r a t i o n s o f the five m o s t p r e v a l e n t pesticides f o u n d in o u t d o o r ,
i n d o o r a n d p e r s o n a l e x p o s u r e s a m p l e s b y p r e d e t e r m i n e d o v e r a l l pesticides u s a g e c a t e g o r y . M e a n v a l u e s
c a l c u l a t e d f r o m results o f all s a m p l e s i n c l u d i n g n o n d e t e c t a b l e m e a s u r e m e n t s .
MEASUREMENT OF ATMOSPHERIC CONCENTRATIONS OF COMMON HOUSEHOLD PESTICIDES
71
TABLE VI
Comparison of indoor, outdoor and personal exposure air samples from one low-use household
Pesticide
Air concentrations, pg m - 3
Indoor
Chlorpyrifos
Propoxur
Chlordane
Diazinon
Heptachlor
Heptachlor epoxide
Folpet
Lindane
trans-Nonachlor
Oxychlordane
ct-BHC
Captan
Outdoor
Personal
day 1
day 2
day 1
day 2
day I
1.0
0.92
0.32
0.28
0.043
0.014
ND
0.015
ND
ND
ND
ND
0.21
0.065
ND
ND
0.013
ND
0.082
0.064
0.013
0.010
0.065
0.016
ND ~
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
0.043
ND
ND
ND
ND
0.021
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
day 2
0.56
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
a Not detected at ca. 0.010~tgm -3.
TABLE VII
Summary of pesticide air exposures attributable to household indoor air
Use
category
Household
number
Number of target
compounds in
personal air
Number (%) of compounds
also in indoor air
High
1
2
3 (day 1)
3 (day 2)
14
10
14
14
11
7
12
12
(79)
(70)
(86)
(86)
Medium
1
2
3 (day 1)
3 (day 2)
13
2
6
6
11
2
4
5
(85)
(100)
(67)
(83)
Low
1
2
3 (day 1)
3 (day 2)
7
7
1
2
5
6
1
2
(71)
(86)
(100)
(100)
(0.29 Ixg m - 3 vs nondetectable in the indoor air sample). In another case, however,
the presence of relatively high propoxur levels in indoor and personal exposure
samples collected at one low-use home were later attributed to an unreported use of
that insecticide during the monitoring period. Two participants spent about 30 min
each working in their gardens, but no significant differences between their PE and
72
ROBERT G. LEWIS ET AL.
corresponding indoor air samples were detected. In two other cases, PE air levels
of chlorpyrifos were significantly higher than corresponding indoor air levels for
persons with pets known to be treated with this insecticide for flea and tick control.
It should also be emphasized that, since the PE samplers were operated for 24 hr,
the quantities of pesticides collected during short exposure periods would be greatty
diluted by relatively clean air sampled for the remaining time.
4. Conclusions
The pilot study showed that the LV sampling system operated at 3.81min and
associated analytical methodology were effective for monitoring all of the pesticides
of interest. In the pilot study area, indoor and personal exposure air concentrations
were generally large enough to be reliably measured with a 12-hr sample, rather than
the 24-hr sample taken. The very good agreement between residential fixed-station
indoor air monitoring and personal air exposure monitoring in this study probably
resulted because the participants spent unusually large proportions of the time inside
their homes. Separate 12-hr daytime and nighttime samples should provide a better
indication of the proportion of the exposure between home and workplace for the
average family member. However, the additional costs involved, especially for
analyses, would likely reduce the size of a given study (in this case, the full NOPES
project), and the additional information would not be essential to determination of
chronic air route exposures.
The results of the pilot study showed that the numbers and concentrations of
pesticides in residential indoor air were higher than those in the immediately
surrounding outdoor air. They also demonstrated the reliability of the field survey
and questionnaire process in stratifying the households by degree of pesticide usage.
The absence in air of the popular pesticide carbaryl may be explained by its low
volatility and the relative difficulty in analyzing samples for this compound. The
nondetectability of polychlorinated biphenyls (<0.1 ggm -3) appears to be in
contrast with previous findings (MacLeod, 1981), and may reflect current trends.
However, PCB-specific cleanup methodology was not used and GC/MS confirmation was not feasible.
The overall conduct of the pilot study was relatively trouble-free. The portable
(LV) samplers were unobtrusive and provided an adequate sample size for GC/MS
analysis. The Du Pont sampling pumps were very reliable in operation and afforded
precise flow control.
Acknowledgement
The authors wish to thank H. J. Schattenberg, H. G. Wheeler, J. H. Brewer, H.
J. Harding and D. E. Camann of Southwest Research Institute for sampling and
analysis assistance; F. W. Immerman, D. Jackson, R. W. Whitmore and K. Inglis
M E A S U R E M E N T OF A T M O S P H E R I C C O N C E N T R A T I O N S OF C O M M O N H O U S E H O L D PESTICIDES
73
of Research Triangle Institute, Research Triangle Park, NC, for designing
questionnaires and conducting household surveys; W. F. Barnard of the U.S.
Environmental Protection Agency, Research Triangle Park, NC, for performing
field audits; H. L. Crist of EPA for preparing quality assurance materials; R. G.
Haines of the PLM Company, Orange Park, FL, for assistance in household
selection; and G. G. Akland of EPA for overall guidance.
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Disclaimer
Although the research described in this article was funded wholly or in part by the U.S. Environmental
Protection Agency through Contract 68-02-3745, it does not necessarily reflect the views of the Agency,
and no official endorsement should be inferred. Mention of trade names or commercial products does
not constitute endorsement or recommendation for use.