United States
                   Environmental Protection
                   Agency
National Exposure
Research Laboratory
Research Triangle Park, NC 27711
                   Research and Development
EPA/600/SR-97/059 September 1997
&EPA        Project Summary

                   Air Concentrations and  Inhalation
                   Exposure to Pesticides  in  the
                   Agricultural  Health  Pilot Study
                  John J. Streicher
                    The incidence of several types of can-
                  cers is higher among farmers than in
                  the general population—this despite
                  lower overall  mortality.  Occupational
                  agents responsible for these excess
                  cancers have not been definitively iden-
                  tified. The Agricultural Health  Study
                  seeks to identify and quantify pesticide
                  exposures to  farmers, indirect expo-
                  sures to their families, and  to assess
                  health risks. A 6-farm, exposure pilot
                  study implemented a total  exposure
                  assessment methodology, '-e-> multime-
                  dia transport and multi-pathway expo-
                  sure. Sampling design included air in-
                  halation, oral ingestion, and dermal ab-
                  sorption. This paper reports on the air
                  transport and inhalation exposures
                  monitored during  the exposure pilot
                  study.  Meteorological  data  were col-
                  lected from  an on-site three-meter
                  tower. Outdoor air was sampled on the
                  day of the pesticide application event,
                  and indoor air samples were collected
                  on three consecutive days centered on
                  the application day. Personal activity
                  logs, indicating time and location, were
                  maintained by participants during the
                  monitoring period.  Of 33 targeted pes-
                  ticides, 7 were applied on at least one
                  of the participant farms, 11 were de-
                  tected in the outdoor air near a farm
                  residence, and 17 were detected in farm
                  residence indoor air. Indoor concentra-
                  tions  of applied pesticides were de-
                  tected on 4 of the 6 farms, however
                  there is limited and  conflicting evidence
                  to support an exclusively outdoor air
                  source of indoor concentrations of ap-
                  plied pesticides. Indoor concentrations
                  of non-applied pesticides were  more
                  the rule than the exception. On 5 of the
 6 pilot-study farms, concentrations of
 non-applied pesticides were detected
 in the indoor air sample on at least one
 day. As expected, the applicator's in-
 halation exposure to applied pesticides
 is greater than that of any other family
 member on the day of application. For
 spouse and  children,  the  indoor mi-
 croenvironment contributed to inhala-
 tion exposure Of pesticides to a far
 greater extent than did the outdoor-on-
 farm microenvironment—even  on the
 day of application.
  This Project Summary was developed
 by  EPA's National Exposure Research
 Laboratory, Research Triangle Park, NC,
 to  announce key findings of  the re-
 search project that is fully documented
 in a separate report of the same title
 (see Project Report ordering informa-
 tion at back).

 Introduction
  The incidence of several types of can-
 cers is higher among farmers than in the
 general  population—this despite lower
 overall mortality.  Retrospective assess-
 ments of exposure to any suspected toxin
 are inadequate in determining environmen-
 tal  cause and health effect relationships.
 The Agricultural Health Study (AHS) is
 the first prospective study to evaluate the
 role of pesticides in cancer risks to farm-
 ers and their families. The AHS is a col-
 laborative effort of the  National  Cancer
 Institute, the U.S.  Environmental Protec-
 tion Agency, and the National Institute of
 Environmental Health Sciences. The study
 seeks to identify and quantify pesticide
 exposures to farmers, and indirect expo-
 sures to their families, and to assess long-
 term health risks.
                                                                   Printed on Recycled Paper

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  A total exposure assessment methodol-
ogy was incorporated in the design of a 6-
farm exposure pilot study, i.e., multimedia
transport and multi-pathway  exposure.
Thirty-three pesticides were targeted. Sam-
pling  design included air inhalation, oral
Ingestion, and dermal absorption. Media
and cohort monitoring were  chronologi-
cally centered around farm pesticide ap-
plication events.  Baseline  concentrations
of pesticides were considered in sampling
during a non-application (i.e., control) sea-
son, vs. the application season. This pa-
per reports on the air transport and inha-
lation exposures  monitored during the pi-
lot  study. Applicator, spouse, and  up to
two children participated from four Iowa
and two North Carolina farms.

Air and Inhalation Exposure
Monitoring Procedures
  The assessment of direct inhalation ex-
posure of the applicator during application
events (handling,  mixing, and  loading
(HML) operations; as well as actual pesti-
cide application) required concurrent sam-
pling  of the applicator's breathing  zone.
Assessment  of indirect inhalation  expo-
sures, as may be accrued by all family
members from breathing  indoor or out-
door air contaminated with fugitive pesti-
cides,  required sampling  of indoor and
outdoor air. All  samples  were collected
with a polyurethane foam (PUF) and quartz
pre-filter cartridge with a size-selective im-
pactor at cartridge inlet which removed
particles greater than 2.5 micrometers in
diameter.
  A five-day sampling strategy was chro-
nologically centered on  the  day of a
planned application event,  hereafter syn-
onymous  with "day 3". The first and fifth
days were directed toward  setup and dis-
assembly of monitoring equipment.  Dur-
ing the second, or pre-application day, an
indoor air sample was collected. During
the application day, indoor and  outdoor
air  samples were collected, as  well as
personal air samples from  the applicator.
During the fourth, or post-application day,
an  indoor air sample was collected. Par-
ticipants' activity  logs recorded the time,
location, and  activity  of the  applicator,
spouse, and one or two children, during
days 2, 3, and 4.
  A personal  air sampler  measured the
applicator's exposure to pesticides by in-
halation during HML and  application ac-
tivities. A 3.8 L/min air sample was drawn
through an inlet tubing positioned within
the applicator's breathing zone. A meteo-
rological monitoring tower  collected wind
speed, wind  direction, temperature, and
relative humidity data at 3 meters above
ground level. Outdoor air  pesticide con-
centrations sampled at the residences on
the application day were expected to cor-
relate with pesticide spray drift during ap-
plication if meteorological  conditions  fa-
vored such  transport.  The indoor  air
samples, collected on days 2, 3, and 4, in
conjunction with participant activity logs,
provided data for  indirect exposure as-
sessment of  all  family members. A non-
application season  indoor air sample pro-
vided indication of baseline concentrations
and chronic exposure. Indoor and outdoor
samples were 24-hour averages; applicator
personal air samples were collected over the
duration of the activity of interest—either HML
or application.

Modeling Initiative
  The contribution of modeling in this study
was to estimate potential  peak outdoor
concentrations under hypothetical  near
worst case conditions.  The selection of
application events suitable to a physically
based model simulation was based  on
both model capability and data limitations.
Each simulated  case adheres  to  actual
pesticide amounts applied and rate of ap-
plication. However, meteorological condi-
tions were a conservative composite of
measured variables,  and concentrations
are  calculated at  plume centerline (i.e.,
assuming wind direction is directly from
application field to monitor). Meteorologi-
cal data are  reported for selected farms
concurrent with  monitored application
events.
  The AgDRIFT model was initially devel-
oped to assess  off-target drift deposition
rates of water-based aerial pesticide ap-
plications.  It   can  also calculate plume
centerline concentrations needed in the
assessment of inhalation exposure. At the
model's core  is a Lagrangian treatment of
dispersion, tracking each nozzle stream
of droplets through  a flow field.  AgDRIFT
incorporates  source constructs such  as
nozzle type, flow rates, and drop size dis-
tribution. Environmental variables having
greatest impact on transport—wind speed,
temperature,  and  relative  humidity—are
incorporated  in  AgDRIFT's calculations.
AgDRIFT was deemed  suitable to simu-
late  ground boom  sprayer  drift, provided
several extrinsic source parameters are
appropriately  assigned.
  The application of the AgDRIFT model
to ground  boom spraying  was accom-
plished by the appropriate setting of vari-
ous emission  and dispersion variables. The
objective of the modeling exercise was to
provide conservative assessments  of
downwind concentrations of applied pesti-
cides for an averaging time typical of ap-
plication duration. The actual application
rate (pounds active ingredient applied per
acre and per unit time) was adhered to in
the calculations.  Model simulations were
consistent with measured values of wind
speed during actual application periods.
Quantitative  details of pesticide applica-
tion are reported, including pesticide iden-
tification, amount of active ingredient, to-
tal volume of liquid mixture  applied,  the
concentration, acreage of application, ap-
plication rate, duration of the application,
and  distance to  the receptor (i.e., farm
house). Additionally, the  model  estimate
of worst case peak concentration at the
receptor is  reported, as  is the  '24-hour
averaged" model calculation, and finally
the measured 24-hour average concen-
tration.  Figures  illustrate modeled peak
one-hour concentration, at nominal adult
breathing height (1.5 m), as a function of
downwind distance.

Results and Discussion
  Indoor and outdoor monitored concentra-
tions of all detected pesticides are presented
by farm, for both control (non-application) sea-
son, and application season. Indoor concen-
trations  of an applied or residual  pesticide
were higher on the application day than con-
terminous days on Iowa farm #1 (dicamba),
Iowa farm #2 (metolachlor), and  Iowa farm #3
(alachlor; second application season). How-
ever, the cases observed in the pilot study do
nor strongly support a conclusion that outdoor
air (exclusively) is the source of indoor con-
centrations of applied/residual pesticides.
  The time,  location, and  activity of study
participants were  recorded by the partici-
pants during days 2, 3, and 4. These activ-
ity logs were reviewed with respect to par-
ticipant location (and activity, in the case of
HML  or application). To assess exposure
to detected pesticides, participant location
was partitioned by characterized  microen-
vironments (indoors; outdoors on farm; or
performing  HML/application activity),  and
time-in-microenvironment  exposure  was
accumulated within 24-hour periods.
  Applicator exposures represented the pre-
ponderance of the applied pesticide inhala-
tion exposure of any family member on any
AHS farm on the day of application. Appli-
cators generally used no  respiratory  pro-
tection during HML  or application activity.
Not surprisingly, HML and application  ac-
tivities accounted for  nearly all of  the
applicator's day 3 exposure to the applied
pesticide. Applicator exposure from HML/
application activity is presented as a  per-
centage of day 3 total exposure. Applicator
exposure during HML/application  activities
accounted for between 80% (alachlor on
North Carolina  farm #1) and  100%

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(dicamba and 2,4-D butoxy ethyl ester on
Iowa farm #2) of applicator day 3 expo-
sure to applied pesticides. A summary of
applicators'  day 3 HML/application—re-
lated dose was also calculated with an
estimated 25 liters  per minute [L/min]
breathing rate.
   Inhalation exposures of all family mem-
bers on the  application day were calcu-
lated to assess relative exposure of appli-
cator,  spouse,  and children. Application
day air pathway exposures are presented
by farm, applied  pesticide,  family mem-
ber,  and by microenvironment.  The data
are presented to permit attribution of a
family  member's exposure to each of the
three designated microenvironments (i.e.,
HML/application activities,  outdoors on
farm, and  indoors).  When  personal air
samples distinguished multiple  HML/ap-
plication activities, separate exposures are
calculated. The final column  in each table
provides the sum of exposures accrued in
all microenvironments on the application
day, by family member and applied pesti-
cide.
  The indoor microenvironment is unique
in its contribution to pesticide exposure of
all study participants via the air pathway.
Time-activity logs indicated that all partici-
pating  family members at all farms spent
an average in excess of 8 hours per day
indoors, over the  three-day period. In all
cases  except Iowa farm #4, concentra-
tions of at least one pesticide being ap-
plied, or found as residue within the appli-
cation  mixture, were measured indoors
during  the three-day monitoring period.
Numerous examples of non-applied, non-
ambient (no  detectable outdoor concen-
tration), pesticides  were  found  to  be
present in indoor air samples. Indeed, in-
door concentrations of non-applied pesti-
cides were the rule more than the excep-
tion.
   Indoor air exposures and  inhalation
doses  of all  indoor detected pesticides—
regardless of their known  origin on the
farm, are presented for all participants, by
farm, pesticide, and  day. The three-day
exposure sum,  as well as a mean daily
indoor inhalation dose, is also calculated
in the final columns of each table. A rest-
ing breathing rate of 10 L/min was applied
to exposure sums in calculating inhalation
dose.

Summary and Conclusions
  Of the 33  targeted pesticides, 7 were
applied on at least one of the participant
farms,  11 were detected in the outdoor air
near a farm residence, and  17  were de-
tected in farm residence indoor air.
  The pesticide applicator was usually ex-
posed  to the applied pesticide(s) during
HML and application activities. An excep-
tion  was found on  Iowa farm #4,  where
pyrethrins  and piperonyl ;butoxide were
applied but their presence in personal air
samples was not  detected. While the
applicator's inhalation exposure to applied
pesticides occurs almost exclusively dur-
ing  HML/application activities (at least
80%),  exposure to  non-applied (fugitive)
pesticides does  occur  during time spent
outdoors on the farm, and even more so
during time spent indoors.
  Outdoor concentrations  of pesticides
applied using a ground boom sprayer were
detected (stationary point measurement)
at significant concentrations (265  ng/m3
alachlor, 24-hour average, on North Caro-
lina farm #1) when wind direction favored
such transport. The converse is not sup-
ported, however, as outdoor concentra-
tions of atrazine were  detected on Iowa
farm #3 even though wind direction never
favored source-to-receptor transport dur-
ing HML or application  activities. Outdoor
concentrations of non-applied pesticides
were detected on 5 of the 6 farms. The
highest 24-hour outdoor concentration of
any non-applied pesticide was 26.3 ng/m3
metolachlor on Iowa farm #3 during the
first  application  season,  although
metolachlor was found  residual within the
applied pesticide mixture. The highest 24-
hour outdoor concentration  of any non-
applied, non-residual pesticide was 18.7
ng/m3 alachlor, also detected on Iowa farm
#3 during the first application  season. Pes-
ticide application events can substantially
increase outdoor concentrations directly
downwind—to levels exceeding typical ap-
plicator personal air concentration  during
handling, mixing, and  loading. Elevated
outdoor pesticide concentrations were not,
however, clearly related to indoor concen-
trations on farms monitored in this study.
  Indoor concentrations of applied pesti-
cides were detected (stationary point mea-
surement) on 4 of the  6 farms, although
one  case (metolachlor  on Iowa farm #2)
confirmed detection during the control sea-
son as well. Indoor concentrations of an
applied or residual pesticide were  higher
on the application day than conterminous
days on Iowa farm #1 (dicamba), Iowa
farm #2 (metolachlor),  and  Iowa farm #3
(alachlor; second application  season).
However, the cases observed in the pilot
study do not strongly  support a conclu-
sion  that outdoor air (exclusively)  is the
source of indoor concentrations of applied/
residual pesticides. Indoor concentrations
of non-applied pesticides were more the
rule than the exception. On 5 of the  6 pilot
study farms, concentrations of non-applied
pesticides were detected on at least one
day.  In  most  cases,  applicator/spouse
questionnaires  relating to historical use of
such pesticides could not confirm usage.
  The applicator's inhalation exposure to
applied pesticides is greater than that of
any other family member on the day of
application (calculated exposures indicated
applicator inhalation exposure to be at
least  a factor  of 5  times greater). This
elevated exposure is attributable to HML/
application activities. Non-applicator fam-
ily members can be exposed indirectly to
applied (and  non-applied)  pesticides dur-
ing time spent indoors or outdoors on  the
farm.  For spouse and children, the indoor
microenvironment contributed to inhalation
exposure of  pesticides to a far greater
extent than did the  outdoor-on-farm  mi-
croenvironment—even on  the day.pf^ap-,
plication. On two" of six farms, miean daily
indoor inhalation dose  for a spouse  or
child was calculated to be  on the order of
micrograms—comparable to  doses  re-
ceived by an applicator during an applica-
tion (although toxicological response and
health risk cannot be presumed to be  the
same). This importance of the indoor  mi-
croenvironment to an individual's  total in-
halation exposure is attributable  to sev-
eral factors. Firstly, the time spent indoors
(over  the course of 24 hours) exceeded
time spent outdoors on the farm. Chronic
exposure to pesticides found in farm resi-
dence indoor air can be comparable, in
cumulative inhaled dose, to exposures  ac-
crued by applicators during pesticide ap-
plications. Secondly,  pesticide concentra-
tions were generally higher indoors than
outdoors (of  20 comparisons that could
be  made, 14 pesticides had higher 24-
hour indoor concentrations; only 6 had
higher 24-hour  outdoor concentrations).
Thirdly, the indoor microenvironment con-
tained a greater number of detected pesti-
cides  than outdoors (17  different pesti-
cides . were detected in indoor samples;
11 were detected in outdoor samples).

Disclaimers
  This paper has been reviewed in accor-
dance with the United States Environmen-
tal  Protection Agency's peer review and
administrative review policies for approval
for  presentation and  publication. Mention
of trade  names or commercial products
does not constitute endorsement or rec-
ommendation for use. The information in
this document  has  been funded by  the
National Institutes of Health and the United
States Environmental Protection  Agency.
It has been subject to review by the Na-
tional  Cancer Institute and National Insti-
tute of Environmental  Health Sciences and
approved for publication.

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    The EPA author, John J. Streicher, who is on assignment from the National
     Oceanic and Atmospheric Administration, U.S. Department of Commerce, isalso
     the EPA Project Officer (see below)
    The complete report, entitled  "Air Concentrations and Inhalation Exposure to
     Pesticides in the Agricultural Health PilotStudy," (Order No. PB97-196109; Cost:
           $25.00, subject to change) will be available only from:
           National Technical Information Service
           5285 Port Royal Road
        •   Springfield, VA 22161
           Telephone: 703-487-4650
    The EPA Project Officer can be contacted at:
           National Exposure Research Laboratory
           U.S.  Environmental Protection Agency
           Research Triangle Park, NC 27711
United States
Environmental Protection Agency
Center for Environmental Research Information
Cincinnati, OH 45268

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