Biomonitoring of 2,4-dichlorophenoxyacetic acid exposure and dose in farm families.

OBJECTIVE: We estimated 2,4-dichlorophenoxyacetic acid (2,4-D) exposure and systemic dose in farm family members following an application of 2,4-D on their farm. METHODS: Farm families were recruited from licensed applicators in Minnesota and South Carolina. Eligible family members collected all urine during five 24-hr intervals, 1 day before through 3 days after an application of 2,4-D. Exposure profiles were characterized with 24-hr urine 2,4-D concentrations, which then were related to potential predictors of exposure. Systemic dose was estimated using the urine collections from the application day through the third day after application. RESULTS: Median urine 2,4-D concentrations at baseline and day after application were 2.1 and 73.1 microg/L for applicators, below the limit of detection, and 1.2 microg/L for spouses, and 1.5 and 2.9 microg/L for children. The younger children (4-11 years of age) had higher median post-application concentrations than the older children (> or = 12 years of age) (6.5 vs. 1.9 microg/L). The geometric mean systemic doses (micrograms per kilogram body weight) were 2.46 (applicators), 0.8 (spouses), 0.22 (all children), 0.32 (children 4-11 years of age), and 0.12 (children > or = 12 years of age). Exposure to the spouses and children was primarily determined by direct contact with the application process and the number of acres treated. Multivariate models identified glove use, repairing equipment, and number of acres treated as predictors of exposure in the applicators. CONCLUSIONS: We observed considerable heterogeneity of 2,4-D exposure among farm family members, primarily attributable to level of contact with the application process. Awareness of this variability and the actual magnitude of exposures are important for developing exposure and risk characterizations in 2,4-D-exposed agricultural populations.

Chlorpyrifos exposure in farm families: results from the farm family exposure study.

We used urinary biological monitoring to characterize chlorpyrifos (O,O-diethyl-O-(3,5,6-trichloro-2-pyridinyl) phosphororthioate) exposure to farm family members from Minnesota and South Carolina who participated in the Farm Family Exposure Study. Five consecutive 24-h urine samples were obtained from 34 families of licensed pesticide applicators 1 day before through 3 days after a chlorpyrifos application. Daily 3,5,6-trichloro-2-pyridinol (TCP) urinary concentrations characterized exposure profiles of the applicator, the spouse, and children aged 4-17 years. Self-reported and observed determinants of exposure were compared to the maximum postapplication TCP concentration. All participants had detectable (> or = 1 microg/l) urinary TCP concentrations at baseline. Applicators' peak TCP levels occurred the day after the application (geometric mean (GM) = 19.0 microg/l). Postapplication TCP change from baseline in the spouses and children was negligible, and the only reliable predictor of exposure was assisting with the application for children aged 12 years and older. The applicators' exposure was primarily influenced by the chemical formulation (GM = 11.3 microg/l for granular and 30.9 microg/l for liquid), and the number of loads applied. Repairing equipment, observed skin contact, and eating during the application were moderately associated TCP levels for those who applied liquid formulations. Estimated absorbed doses (microg chlorpyrifos/kg bodyweight) were calculated based on TCP excretion summed over the 4 postapplication days and corrected for pharmacokinetic recovery. The GM doses were 2.1, 0.7, and 1.0 microg/kg bodyweight for applicators, spouses, and children, respectively. Chlorpyrifos exposure to farm family members from the observed application was largely determined by the extent of contact with the mixing, loading, and application process.

Exposure misclassification in studies of agricultural pesticides: insights from biomonitoring.

BACKGROUND: Epidemiologists often assess lifetime pesticide exposure by questioning participants about use of specific pesticides and associated work practices. Recently, Dosemeci and colleagues proposed an algorithm to estimate lifetime average exposure intensity from questionnaire information. We evaluated this algorithm against measured urinary pesticide concentrations for farmers who applied glyphosate (n = 48), 2,4-D (n = 34), or chlorpyrifos (n = 34). METHODS: Algorithm scores were calculated separately based on trained field observers' and farmers' evaluations of application conditions. Statistical analyses included nonparametric correlations, assessment of categorical agreement, and categorical evaluation of exposure distributions. RESULTS: Based on field observers' assessments, there were moderate correlations between algorithm scores and urine concentrations for glyphosate (r = 0.47; 95% confidence interval [CI] = 0.21 to 0.66) and 2,4-D (0.45; 0.13 to 0.68). Correlations were lower when algorithm scores were based on participants' self-reports (for glyphosate, r = 0.23 [CI = -0.07 to 0.48]; for 2,4-D, r = 0.25 [-0.10 to 0.54]). For chlorpyrifos, there were contrasting correlations for liquid (0.42; 0.01 to 0.70) and granular formulations (-0.44; -0.83 to 0.29) based on both observers' and participants' inputs. Percent agreement in categorical analyses for the 3 pesticides ranged from 20% to 44%, and there was appreciable overlap in the exposure distributions across categories. CONCLUSIONS: Our results demonstrate the importance of collecting type of pesticide formulation and suggest a generic exposure assessment is likely to result in appreciable exposure misclassification for many pesticides.

Implications for epidemiologic research on variation by pesticide in studies of farmers and their families.

Epidemiologic studies rely on participants' recall to classify their exposure to specific pesticides. As exposure classification evolves, an important issue is whether the recall of pesticide application details can be used to derive measures of exposure intensity or cumulative exposure. A preliminary analysis of biomonitoring data for farmers before, during, and after a pesticide application suggests variation for different pesticides in the proportion with detectable urinary concentrations, urinary levels, and patterns of uptake and elimination. These findings, and the limited predictive modeling done to date, suggest that chemical-specific differences need to be considered in exposure classification schemes. An analysis of biomonitoring data for farm spouses and children found few with appreciable changes in the urinary concentration after a pesticide application. These findings point to the need to validate assumptions about exposures in studies of people who are not directly involved in pesticide application.

Applicator exposure to acetochlor based on biomonitoring.

Biomonitoring was used to assess the combined dermal, oral, and inhalation exposure associated with the agricultural use of Harness Plus, an emulsifiable concentrate formulation of the herbicide acetochlor. Twenty Spanish farmers handled and applied acetochlor to maize in the spring of 2003, following the product label recommendations. Open- and closed-cabin applications were equally represented. Urine was collected during six consecutive days, starting the day prior to application. Daily composites were analyzed for 2-ethyl-6-methyl-aniline, a common chemophore representing the major urinary acetochlor metabolites. All applicators showed detectable concentrations in urine after application. Although, the open-cabin applicators treated fewer hectares, they showed significantly higher exposure compared to the closed-cabin applicators (average exposure: 0.004 and 0.002 mg/kg bw/day, respectively). Linear regression analysis suggested that untracked incidents had a significant impact on the total exposure. Other events that may have contributed to the observed exposure are repair of faulty equipment, accidental spillages, splashes, and inadequate use of protective gloves. The average margins of exposure (MOE) for farmers ranged from 23,000 (open cabin) to about 44,000 (closed cabin). For professional applicators the MOEs were 10-fold lower. These MOEs clearly indicate that no adverse health effects should be expected from agricultural acetochlor applications.

Exposure to sulfosulfuron in agricultural drainage ditches: field monitoring and scenario-based modelling.

Field monitoring and scenario-based modelling were used to assess exposure of small ditches in the UK to the herbicide sulfosulfuron following transport via field drains. A site in central England on a high pH, clay soil was treated with sulfosulfuron, and concentrations were monitored in the single drain outfall and in the receiving ditch 1 km downstream. Drainflow in the nine months following application totalled 283 mm. Pesticide lost in the first 12.5 mm of flow was 99% of the total loading to drains (0.5% of applied). Significant dilution was observed in the receiving ditch and quantifiable residues were only detected in one sample (0.06 microg litre(-1)). The MACRO model was evaluated against the field data with minimal calibration. The parameterisation over-estimated the importance of macropore flow at the site. As a consequence, the maximum concentration in drainflow (2.3 microg litre(-1)) and the total loading to drains (0.76 g) were over-estimated by factors of 2.4 and 5, respectively. MACRO was then used to simulate long-term fate of the herbicide for each of 20 environmental scenarios. Resulting estimates for concentrations of sulfosulfuron in a receiving ditch were weighted according to the prevalence of each scenario to produce a probability distribution of daily exposure.

Fractal-based scaling and scale-invariant dispersion of peak concentrations of crop protection chemicals in rivers.

A new regulatory approach is needed to characterize peak pesticide concentrations in surface waters over a range of watershed scales. Methods now in common use rely upon idealized edge-of-field scenarios that ignore scaling effects. Although some watershed-scale regulatory models are available, their complexity generally prevents them from being used duringthe pesticide registration decision process, even though nearly all exposure to both humans and aquatic organisms can occur only at this scale. The theory of fractal geometry offers a simpler method for addressing this regulatory need. Mandelbrot described rivers as "space-filling curves" (Mandelbrot, B. B. The Fractal Geometry of Nature; Freeman: New York, 1983), a class of fractal objects implying two useful properties we exploit in this work. The first is a simple power-law relationship in which log-log plots of maximum daily concentrations as a function of watershed area tend to be linear with a negative slope. We demonstrate that the extrapolation of such plots down to smaller watersheds agrees with edge-of-field concentrations predicted using the Pesticide Root Zone Model, but only when the modeling results are properly adjusted for use intensity within the watershed. We also define a second useful property, "scale-invariant dispersion", in which concentrations are well described by a single analytical solution to the convective--dispersion equation, regardless of scale. Both of these findings make it possible to incorporate the effect of watershed scale directly into regulatory assessments.

Glyphosate biomonitoring for farmers and their families: results from the Farm Family Exposure Study.

Glyphosate is the active ingredient in Roundup agricultural herbicides and other herbicide formulations that are widely used for agricultural, forestry, and residential weed control. As part of the Farm Family Exposure Study, we evaluated urinary glyphosate concentrations for 48 farmers, their spouses, and their 79 children (4-18 years of age). We evaluated 24-hr composite urine samples for each family member the day before, the day of, and for 3 days after a glyphosate application. Sixty percent of farmers had detectable levels of glyphosate in their urine on the day of application. The geometric mean (GM) concentration was 3 ppb, the maximum value was 233 ppb, and the highest estimated systemic dose was 0.004 mg/kg. Farmers who did not use rubber gloves had higher GM urinary concentrations than did other farmers (10 ppb vs. 2.0 ppb). For spouses, 4% had detectable levels in their urine on the day of application. Their maximum value was 3 ppb. For children, 12% had detectable glyphosate in their urine on the day of application, with a maximum concentration of 29 ppb. All but one of the children with detectable concentrations had helped with the application or were present during herbicide mixing, loading, or application. None of the systemic doses estimated in this study approached the U.S. Environmental Protection Agency reference dose for glyphosate of 2 mg/kg/day. Nonetheless, it is advisable to minimize exposure to pesticides, and this study did identify specific practices that could be modified to reduce the potential for exposure.