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 ------- 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% ------- (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. ------- 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 Official Business Penalty for Private Use $300 BULK RATE POSTAGE & FEES PAID EPA PERMIT NO. G-35 EPA/600/SR-97/059 ------- |