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Pyrethroid insecticides are widely used to control insects in both agricultural and residential settings worldwide. Few data are available on the temporal variability of pyrethroid metabolites in the urine of non-occupationally exposed adults. In this work, we describe the study design and sampling methodology for the Pilot Study to Estimate Human Exposures to Pyrethroids using an Exposure Reconstruction Approach (Ex-R study). Two major objectives were to quantify the concentrations of several pyrethroid metabolites in bedtime, first morning void (FMV), and 24-h urine samples as concentration (wet weight), specific-gravity (SG) corrected, creatinine (CR) corrected, and excretion rate values for 50 Ex-R adults over a six-week monitoring period and to determine if these correction approaches for urine dilution reduced the variability of the biomarker levels. The Ex-R study was conducted at the United States Environmental Protection Agency's Human Studies Facility in Chapel Hill, North Carolina USA and at participants' homes within a 40-mile radius of this facility. Recruitment of participants and field activities occurred between October 2009 and May 2011. Participants, ages 19-50 years old, provided daily food, activity, and pesticide-use diaries and collected their own urine samples (bedtime, FMV, and 24-h) during weeks 1, 2, and 6 of a six-week monitoring period. A total of 2503 urine samples were collected from the study participants. These samples were analyzed for the pyrethroid metabolites 3-phenoxybenzoic acid (3-PBA), cis/trans-3-(2,2-dichlorovinyl)-2,2-dimethyl-cyclopropane carboxylic acid (cis/trans-DCCA), and 2-methyl-3-phenylbenzoic acid (MPA) using high performance liquid chromatography/tandem mass spectrometry. Only 3-PBA was frequently detected (>50%) in the adult urine samples. Median urinary 3-PBA levels were 0.88 ng/mL, 0.96 ng/mL-SG, 1.04 ng/mg, and 1.04 ng/min for concentration, SG-corrected, CR-corrected, and excretion rate values, respectively, across all urine samples. The results showed that median urinary 3-PBA concentrations were consistently the lowest in FMV samples (0.77 ng/mL, 0.68 ng/mL-SG, 0.68 ng/mg, and 0.58 ng/min) and the highest in 24-h samples (0.92 ng/mL, 1.06 ng/mL-SG, 1.18 ng/mg, and 1.19 ng/min) across all four methods. Intraclass correlation coefficient (ICC) estimates for 3-PBA indicated poor reproducibility (<0.22) for all urine sample types and methods over a day, week, and six weeks. Correcting for urine sample dilution, based on either SG, CR or urine output, introduced additional measurement variability both between- and within-individuals. These results indicate that a single measure of urinary 3-PBA was not sufficient to characterize average exposure regardless of sample type, correction method, and time frame of collection. In addition, the study results can be used to inform the design of exposure characterization strategies in relevant environmental epidemiology studies in the future., (Published by Elsevier Inc.)

This study examined the potential for pet dogs to be an important pathway for transporting diazinon residues into homes and onto its occupants following residential lawn applications. The primary objectives were to investigate the potential exposures of occupants and their pet dogs to diazinon after an application to turf at their residences and to determine if personal contacts between occupants and their pet dogs resulted in measurable exposures. It was conducted from April to August 2001 before the Agency phased out all residential uses of diazinon in December 2004. Six families and their pet dogs were recruited into the study. Monitoring was conducted at pre-, 1, 2, 4, and 8 days post-application of a commercial, granular formulation of diazinon to the lawn by the homeowner. Environmental samples collected included soil, indoor air, carpet dust, and transferable residues from lawns and floors. Samples collected from the pet dogs consisted of paw wipes, fur clippings, and transferable residues from the fur by a technician or child wearing a cotton glove(s). First morning void (FMV) urine samples were collected from each child and his/her parent on each sampling day. Diazinon was analyzed in all samples, except urine, by GC-MS. The metabolite 2-isopropyl-4-methyl-6-hydroxypyrimidine (IMPy) was analyzed in the urine samples by HPLC-MS/MS. Mean airborne residues of diazinon on day 1 post-application were at least six times higher in both the living rooms (235+/-267 ng/m(3)) and children's bedrooms (179+/-246 ng/m(3)) than at pre-application. Mean loadings of diazinon in carpet dust samples were at least 20 times greater on days 2, 4, and 8 post-application than mean loadings (0.03+/-0.04 ng/cm(2)) at pre-application. The pet dogs had over 900 times higher mean loadings of diazinon residues on their paws on day 1 post-application (88.1+/-100.1 ng/cm(2)) compared to mean loadings (<0.09 ng/cm(2)) at pre-application. The mean diazinon loadings on the fur clippings were at least 14 times higher on days 1, 2, 4, and 8 post-application than mean loadings (0.8+/-0.4 ng/cm(2)) at pre-application. For transferable residues from dog fur, the mean loadings of diazinon on the technician's cotton glove samples were the lowest before application (0.04+/-0.08 ng/cm(2)) and the highest on day 1 post-application (10.4+/-23.9 ng/cm(2)) of diazinon to turf. Urinary IMPy concentrations for the participants ranged from <0.3 to 5.5 ng/mL before application and <0.3-12.5 ng/mL after application of diazinon. The mean urinary IMPy concentrations for children or adults were not statistically different (p>0.05) at pre-application compared to post-application of diazinon to turf. The results showed that the participants and their pet dogs were likely exposed to low levels of diazinon residues from several sources (i.e., air, dust, and soil), through several pathways and routes, after lawn applications at these residences. Lastly, the pet dog appears to be an important pathway for the transfer and translocation of diazinon residues inside the homes and likely exposed occupants through personal contacts (i.e., petting).

The potential exposures of 127 preschool children to the pyrethroid insecticides, cis- and trans-permethrin, in their everyday environments were examined. Participants were recruited randomly from 127 homes and 16 daycare centers in six Ohio (OH) counties. Monitoring was performed over a 48-h period at the children's homes and/or daycare centers. Samples collected included soil, carpet dust, indoor air, outdoor air, diet, hand wipes, surface wipes, transferable residues, and urine. The environmental samples were analyzed for the cis and trans isomers of permethrin, and the urine samples were analyzed for the pyrethroid urinary metabolite, 3-phenoxybenzoic acid (3-PBA), by gas chromatography/mass spectrometry. The isomers were detected most often in the dust (100%) and hand wipe (>78%) samples collected at both homes and daycare centers. The median levels of cis-permethrin (470 and 1010 ng/g) were higher than the median levels of trans-permethrin (344 and 544 ng/g) in the dust samples at both the children's homes and daycare centers, respectively. In the children's hand wipe samples, the median levels of cis- and trans-permethrin were similar, ranging from 0.03 to 0.04 ng/cm(2), at both locations. The urinary metabolite 3-PBA was detected in 67% of the children's urine samples. The median urinary 3-PBA concentration for the children was 0.3 ng/mL, and the maximum value for one child was 33.8 ng/mL. The primary route of the children's exposure to the combined isomers was through dietary ingestion, followed by indirect ingestion. In addition, our calculated aggregate absorbed doses of permethrin accounted for about 60% of the excreted amounts of 3-PBA found in the children's urine. In conclusion, these children were potentially exposed to low levels of permethrin from several sources, and through several pathways and routes.

The Children's Total Exposure to Persistent Pesticides and Other Persistent Organic Pollutants (CTEPP) study investigated the potential exposures of 257 preschool children, ages 1 1/2-5 yr, and their primary adult caregivers to more than 50 anthropogenic chemicals. Field sampling took place in selected counties in North Carolina (NC) and Ohio (OH) in 2000-2001. Over a 48-h period in each child's daycare center and/or home, food, beverages, indoor air, outdoor air, house dust, soil, participants' hand surfaces and urine were sampled. Additional samples-transferable residues, food preparation surface wipes, and hard floor surface wipes-were collected in the approximately 13% of the homes that had pesticide applications within the 7 days prior to field sampling. Three phenols were among the measured chemicals: pentachlorophenol (PCP), bisphenol-A [2,2-bis(4-hydroxyphenyl)propane], and nonylphenol (4-n-nonylphenol). Nonylphenol (NP) was detected in less than 11% of the samples in any medium. Among samples that were collected at all participants' homes and daycare centers, PCP was detected in >50% of indoor air, outdoor air, house dust, and urine samples; bisphenol-A (BPA) was detected in >50% of indoor air, hand wipe, solid food, and liquid food samples. The concentrations of the phenols in the sampled media were measured, and the children's potential exposures and potential absorbed doses resulting from intake through the inhalation, dietary ingestion, and indirect ingestion routes of exposure were estimated. The children's potential exposures to PCP were predominantly through inhalation: 78% in NC and 90% in OH. In contrast, their potential exposures to BPA were predominantly through dietary ingestion: 99%, for children in both states. The children's estimated exposures to PCP, calculated from the amounts excreted in their urine, exceeded their estimated maximum potential intake, calculated from the multimedia PCP concentrations, by a factor greater than 10. This inconsistency for PCP highlights the need for further research on the environmental pathways and routes of PCP exposure, investigation of possible exposures to other compounds that could be metabolized to PCP, and on the human absorption, metabolism, and excretion of this phenol over time periods longer than 48 h.