Soils and dusts can act as sinks for semivolatile lipophilic organic compounds and children ingest relatively large amounts of both soils and dusts. Following intake, sorbed chemicals may desorb (mobilize) and become available for intestinal absorption (bioaccessible). When chemicals are not degraded in the digestive tract, mobilization can approximate bioaccessibility. Alternatively, when gastrointestinal degradation of mobilized chemicals does occur, it can be useful to separate mobilization from bioaccessibility. In this study we used synthetic digestive fluids in a sequential, three -compartment (saliva, gastric, and intestinal) in vitro assay to construct mobilization and bioaccessibility models for 16 pesticides (log Kow 2.5-6.8) sorbed to 32 characterized soils and house dusts. To address the potential loss of mobilized pesticides due to absorption, the assays were repeated using a solid phase sorbent (tenax) added to the digestive fluid immediately after addition of the intestinal fluid components. We found that pesticide mobilization was predicted by pesticide log Kow and the carbon content of the soils and dusts. Pesticide loss measurably reduced the bioaccessibility of most pesticides, and bioaccessibility was largely predicted by log Kow and pesticide loss rate constants. Introduction of the sink increased mobilization by x = 4 +/- 6% (soil) and x = 9 +/- 7% (dust) while bioaccessibility increases were x = 41 +/- 21% (soil) and x = 24 +/- 12% (dust). The physicochemical properties of the soils, dusts, and pesticides used in this study successfully predicted the in vitro mobilization and bioaccessibility of the pesticides. This suggests that modeling of pesticide mobilization and bioaccessibility could reduce uncertainty in exposure and risk assessments.
Per- and polyfluoroalkyl substances (PFAS) are regularly found in soils and dusts, both of which can be consumed by children at relatively high amounts. However, there is little data available to model the bioaccessibility of PFAS in soils and dusts when consumed or to describe how the physiochemical properties of PFAS and soils/dusts might affect bioaccessibility of these chemicals. Because bioaccessibility is an important consideration in estimating absorbed dose for exposure and risk assessments, in the current study, in vitro assays were used to determine bioaccessibility of 14 PFAS in 33 sets of soils and dusts. Bioaccessibility assays were conducted with and without a sink, which was used to account for the removal of PFAS due to their movement across the human intestine. Multiple linear regression with backward elimination showed that a segmented model using PFAS chain length, number of branches, and percent total organic carbon explained 78.0%-88.9% of the variability in PFAS bioaccessibility. In general, PFAS had significantly greater bioaccessibility in soils relative to dusts and the addition of a sink increased bioaccessibility in the test system by as much as 10.8% for soils and 20.3% for dusts. The results from this study indicate that PFAS bioaccessibility in soils and dusts can be predicted using a limited set of physical chemical characteristics and could be used to inform risk assessment models.
The Air Pollutants Exposure Model (APEX) is a stochastic population-based inhalation exposure model which (along with its earlier version called pNEM) has been used by the U.S. Environmental Protection Agency (EPA) for over 30 years for assessment of human exposure to airborne pollutants. This study describes the application of a variance decomposition-based sensitivity analysis using the Sobol method to elucidate the key APEX inputs and processes that affect variability in exposure and dose for the simulated population. Understanding APEX's sensitivities to these inputs helps not only the model user but also the EPA in prioritizing limited resources towards data-collection and analysis efforts for the most influential variables, in order to maintain the quality and defensibility of the simulation results. This analysis examines exposure to ozone of children ages 5-18 years. The results show that selection of activity diaries and microenvironmental parameters (including air-exchange rate and decay rate) are the most influential to estimated exposure and dose, their aggregate main-effect indices (MEIs) equaling 0.818 (out of a maximum of 1.0) for daily-average ozone exposure and 0.469 for daily-average inhaled ozone dose. The modeled person's home location, sampled from national Census data, has a modest influence on exposure (MEI = 0.079 for daily averages), while age, sex, and body mass, also sampled from Census and other survey data, have modest influences on inhaled dose (aggregate MEI = 0.307). The sensitivity analysis also plays a quality-assurance role by evaluating the sensitivities against our knowledge of the physical properties of the model.
A Matrix has recently been presented as a tool to assist in the translation of epidemiology literature for the needs of risk assessment. The Matrix is an approach to bridge the epidemiology-risk assessment gap and includes nine risk assessor “asks” of epidemiology studies. The Matrix is designed to facilitate awareness about how choices regarding a study's design, analyses and reporting can enhance the use of epidemiology data for risk assessment, and ultimately public health decision-making. In this paper, a case study of the Matrix is presented to (i) demonstrate how a selected body of epidemiology literature can be described in a risk assessment context using the elements of the Matrix, and (ii) assess the clarity and utility of the Matrix. This was conducted by reviewing 14 epidemiologic studies used in the US National Ambient Air Quality Standards Integrated Science Assessment for Oxides of Nitrogen for evaluating the nine elements outlined in the Matrix. The Matrix performed well in characterizing the needs of risk assessors in the areas of hazard identification, exposure assessment, and dose-response assessment. The case study revealed areas in which more precise word choices within the Matrix may improve the characterization of translational needs in epidemiology literature; recommendations for modifications to the Matrix are made. The case study findings indicate that there are opportunities for risk assessors and epidemiologists to collaborate to facilitate the use of epidemiology research for public health decision-making.
Soils are sorbents for many organic compounds and children consume relatively large amounts of soil. To improve the estimated health risks from this exposure pathway, we examined the role of co-ingested foods in determining the post-ingestion bioaccessibility (mobilization) of 18 polychlorinated biphenyls (PCBs) sorbed to 10 characterized soils. The bioaccessibility test system (DIN 19738, 2004) was an in vitro, 3-compartment, digestive tract containing salts, protein, and bile. Each soil was fortified with PCBs, then, digestive fluids appropriate to each compartment, were added sequentially. Next, digestive fluid and soil were seperated and PCB concentrations in both media were measured. This complete test system was then reduced to assess contributions of individual endogenous digestive fluid constituents (water, salts, pancreatin, bile, and mucin) and representative foods: protein (bovine serum albumin (BSA)), sugar (glucose), and fat (oleic acid). Then, the influence of increasing concentrations of BSA, glucose, and oleic acid was evaluated (individually) complete test systems. In a subset of the samples, solid phase microextraction (SPME) was used to measure freely dissolved PCBs. Across all treatments, percent soil organic carbon was the most influential bioaccessibility determinant, accounting for ≥87% of the explained variation. When evaluated individually, pancreatin, mucin, BSA, bile, and oleic acid each effectively increased PCB bioaccessibility and reduced freely dissolved PCB concentrations. This suggests competitive sorption of PCBs by organic constituents of the digestive constituents. Without sink material, intra-PCB mobilization differences were observed as freely dissolved PCB concentrations inversely correlated (p < 0.05) with their respective log Kow's. When added to the complete digestive fluid, increasing oleic acid mass increased PCB bioaccessibility (p < 0.05), while adding more BSA or glucose did not (p > 0.05). This indicates that fat intake may be the sole consideration needed when modeling dietary contributions to bioaccessibility of soil sorbed PCBs.
This paper describes an operational evaluation of the US Environmental Protection Agency's (EPA) Air Pollution Exposure Model (APEX). APEX simulations for a multipollutant ambient air mixture, i.e. ozone (O3), carbon monoxide (CO), and particulate matter 2.5 microns in diameter or less (PM2.5), were performed for two seasons in three study areas in central Los Angeles. APEX predicted microenvironmental concentrations were compared with concentrations of these three pollutants monitored in the Exposure Classification Project (ECP) study during the same periods. The ECP was designed expressly for evaluating exposure models and measured concentrations inside and outside 40 microenvironments. This evaluation study identifies important uncertainties in APEX inputs and model predictions useful for guiding further exposure model input data and algorithm development efforts. This paper also presents summaries of the concentrations in the different microenvironments.
Ingestion of soils and house dusts is an important pathway for children's exposure to sorbed organic pollutants such as polychlorinated biphenyls (PCBs). To reduce the uncertainty of the exposure estimates, it is important to understand the extent to which chemicals desorb and become bioaccessible following ingestion. In this study we use a three compartment in vitro digestive system to model the role of soil and house dust physicochemical properties on the post ingestion bioaccessibility of PCBs. Matched pairs (n = 37) of soil and dust were characterized for percent carbon and nitrogen, pH, moisture content, and particle size distribution. They were then fortified with a mixture of 18 PCBs and processed through the assay. The percent bioaccessibility of each PCB was calculated, then modeled using individual PCB log Kow values and the soil and dust properties. The bioaccessibility of the PCBs in soil (x̄ = 65 ± 16%) was greater (p < 0.001) than that of the PCBs in house dust (x̄ = 36 ± 14%). In the soil model, carbon was the sole statistically significant predictive (p ≤ 0.05) variable, while in house dust, both carbon and clay content were statistically significant (p ≤ 0.05) predictors.
This paper describes a new regression modeling approach to estimate on-road nitrogen dioxide (NO 2 ) and oxides of nitrogen (NO X ) concentrations and near-road spatial gradients using data from a near-road monitoring network. Field data were collected in Las Vegas, NV, at three monitors sited 20, 100, and 300 m from Interstate-15 between December 2008 and January 2010. Measurements of NO 2 and NO X were integrated over 1-h intervals and matched with meteorological data. Several mathematical transformations were tested for regressing pollutant concentrations against distance from the roadway. A logit-ln model was found to have the best fit ( R 2 = 94.7 %) and also provided a physically realistic profile. The mathematical model used data from the near-road monitors to estimate on-road concentrations and the near-road gradient over which mobile source pollutants have concentrations elevated above background levels. Average and maximum on-road NO 2 concentration estimates were 33 and 105 ppb, respectively. Concentration gradients were steeper in the morning and late afternoon compared with overnight when stable conditions preclude mixing. Estimated on-road concentrations were also highest in the late afternoon. Median estimated on-road and gradient NO 2 concentrations were lower during summer compared with winter, with a steeper gradient during the summer, when convective mixing occurs during a longer portion of the day. On-road concentration estimates were higher for winds perpendicular to the road compared with parallel winds and for atmospheric stability with neutral-to-unstable atmospheric conditions. The concentration gradient with increasing distance from the road was estimated to be sharper for neutral-to-unstable conditions when compared with stable conditions and for parallel wind conditions compared with perpendicular winds. A regression of the NO 2 /NO X ratios yielded on-road ratios ranging from 0.25 to 0.35, substantially higher than the anticipated tailpipe emissions ratios. The results from the ratios also showed that the diurnal cycle of the background NO 2 /NO X ratios were a driving factor in the on-road and downwind NO 2 /NO X ratios.
The impact of climate change on human and environmental health is of critical concern. Population exposures to air pollutants both indoors and outdoors are influenced by a wide range of air quality, meteorological, behavioral, and housing-related factors, many of which are also impacted by climate change. An integrated methodology for modeling changes in human exposures to tropospheric ozone (O 3 ) owing to potential future changes in climate and demographics was implemented by linking existing modeling tools for climate, weather, air quality, population distribution, and human exposure. Human exposure results from the Air Pollutants Exposure Model (APEX) for 12 US cities show differences in daily maximum 8-h (DM8H) exposure patterns and levels by sex, age, and city for all scenarios. When climate is held constant and population demographics are varied, minimal difference in O 3 exposures is predicted even with the most extreme demographic change scenario. In contrast, when population is held constant, we see evidence of substantial changes in O 3 exposure for the most extreme change in climate. Similarly, we see increases in the percentage of the population in each city with at least one O 3 exposure exceedance above 60 p.p.b and 70 p.p.b thresholds for future changes in climate. For these climate and population scenarios, the impact of projected changes in climate and air quality on human exposure to O 3 are much larger than the impacts of changing demographics. These results indicate the potential for future changes in O 3 exposure as a result of changes in climate that could impact human health.
Pyrethroid insecticides are used extensively in agriculture, and they, as well as their environmental degradates, may remain as residues on foods such as fruits and vegetables. Since pyrethroid degradates can be identical to the urinary markers used in human biomonitoring, it is important to understand the contribution of these degradates when studying sources of human pyrethroid exposure. We modified the widely used Quick Easy Cheap Effective Rugged Safe (QuEChERS) method to measure several current-use pyrethroids (cis/trans-permethrin, cypermethrin, deltamethrin, esfenvalerate, bifenthrin, cyfluthrin, and cyhalothrin) and their environmental degradation products (3-PBA, cis/trans-DCCA, 4-F-3-PBA, DBCA, and MPA) in selected fresh fruits and vegetables. Using fortified samples, we determined extraction efficiencies from: tomatoes, oranges (whole, peeled, and rind), grapes, apples, bananas (peeled and rind only), onions, lettuce, green peppers, carrots and broccoli. For a subset of these food items (apples, grapes, tomatoes, lettuce and banana peel), we also established limits of detection (MDLs) and quantitation (MQLs). Each sample was homogenized (1kg) then spiked with the target pyrethroids and their degradation products. Sub-samples (15g) were extracted with acetonitrile, then salted out and partitioned with NaCl and MgSO4. The extract was divided and further cleaned using solid phase extraction (SPE) cartridges containing either graphitized non-porous carbon (pyrethroids) or C18 (degradation products). Sample analysis was via liquid chromatography/tandem mass spectrometry (LC-MS/MS). Considering the mean recoveries each of the 14 analytes in all 13 matrices: 42% of the recoveries were ≥90%, 70% were ≥80%, and 90% were ≥70%. All MDL's were less than 100ng/kg, except 3-PBA (132ng/kg, tomato), MPA (129ng/kg, tomato), and trans-permethrin (141ng/kg, banana peel). We then applied the method to non-spiked samples (subset of 5 for which the MDLs/MQLs had been determined) collected weekly for four weeks from local supermarkets. At least one pyrethroid was present in measureable concentrations in all matrices except banana peels. In contrast, the only degradation products detected were cis/trans-DCCA, in one lettuce sample.
For children, ingestion of soils and house dusts can be an important exposure pathway for regulated organic compounds. Following ingestion, the extent to which compounds desorb and become bioaccessible is a critical determinant of systemic adsorption. We characterized the physicochemical properties of 37 soil and house dust pairs collected during a national survey of United States homes. For each sample, we measured the bioaccessibility of fipronil, a phenylpyrazole insecticide using an in vitro, three- compartment digestive system, then modeled the physicochemical predictors of fipronil bioaccessibility. The properties of the soils and dusts were not correlated and percent carbon was the only significant predictor of bioaccessibility for both soils (p<0.001) and dusts (p<0.001). The carbon content of the soils (3.1±2.4%) was lower than that of the dusts (18.6±6.9%) Due to the lower carbon content, soil sorbed fipronil was more bioaccessible than dust sorbed fipronil. However, the slope of the bioaccessibility carbon regression line was steeper for the soils than for the house dusts. This suggested that, for soils having carbon percentages greater than those in this study, fipronil bioaccessibility may be less than that of house dusts having equal carbon content.
Epidemiologic studies of air pollution have traditionally relied upon surrogates of personal pollutant exposures, such as ambient concentration measurements from fixed-site pollutant monitors. This study evaluates the performance of alternative measured and modeled exposure metrics for multiple particulate and gaseous pollutants, in the context of different epidemiologic studies performed by EPA, Rutgers/Rochester/LBNL and Emory/Georgia Tech researchers. Alternative exposure estimation approaches used, included: central site or interpolated monitoring data, regional pollution levels based on measurements or models (CMAQ) and local scale (AERMOD) air quality models, hybrid models, statistically blended modeling and measurement data, concentrations adjusted by home infiltration rates based on LBNL algorithms, and population human exposure (SHEDS and APEX) model predictions. The Emory/Georgia Tech team examined the acute morbidity effects of ambient traffic-related pollutants (CO, NOx, PM2.5 and PM2.5 EC) and ozone using time series analyses of emergency department (ED) visits and case-crossover analysis of implantable cardioverter defibrillator (ICD) detected ventricular arrhythmias in Atlanta, GA. The Rutgers/Rochester/LBL team examined the associations between PM2.5 mass and its species with myocardial infarction (case-crossover study) and adverse birth outcomes (cohort study) in New Jersey. Initially, the various exposure indicators/metrics were compared in terms of their ability to characterize the spatial and temporal variations of multiple ambient air pollutants across the different study areas. These metrics were then used to examine associations between ambient air pollution and adverse health effects. Next, pollutant–specific relative risks (RRs) obtained from epidemiologic analyses of the alternative exposure metrics were evaluated against those obtained from using a conventional approach (i.e., central site data alone). Pollutant and metric dependent exposure prediction differences were found in some cases, indicating a non-uniform exposure prediction error structure across pollutants. Results suggest the need for additional refinements to methods used to estimate exposures in support of different types of air pollution epidemiologic studies.
UNLABELLED:National surveys of United States households and child care centers have demonstrated that pyrethroids are widely distributed in indoor habited dwellings and this suggests that co-exposure to multiple pyrethroids occurs in nonoccupational settings. The purpose of this research was to use an environmentally relevant mixture of pyrethroids to assess their cumulative effect on motor activity and develop kinetic profiles for these pyrethroids and their hydrolytic metabolites in brain and blood of rats. Rats were dosed orally at one of two levels (1.5× or 5.0× the calculated dose that decreases rat motor activity by 30%) with a mixture of cypermethrin, deltamethrin, esfenvalerate, cis-/trans-permethrin, and β-cyfluthrin in corn oil. At 1, 2, 4, 8, or 24h after dosing, the motor activity of each animal was assessed and the animals sacrificed. Concentrations of pyrethroids in brain and blood, and the following metabolites: cis-/trans-dichlorovinyl-dimethylcyclopropane-carboxylic acid, 3-phenoxybenzoic acid, 3-phenoxybenzyl alcohol, 4-fluoro-3-phenoxybenzoic acid, and cis-dibromovinyl-dimethylcyclopropane-carboxylic acid were determined using liquid chromatography tandem mass spectrometry (LC-MS/MS). Using this pyrethroid mixture in rats, the results suggest there is greater metabolism of trans-permethrin prior to entering the systemic circulatory system. All pyrethroids had tissue half-lives (t1/2) of less than 5h, excepting esfenvalerate in brain. At early time points, relative pyrethroid brain concentrations approximated their dose mixture proportions and a sigmoidal Emax model described the relationship between motor activity decrease and total pyrethroid brain concentration. In blood, the t1/2's of the cyclopropane metabolites were longer than the phenoxybenzoic metabolites. However, relative to their respective precursors, concentrations of the phenoxybenzoic acids were much higher than concentrations of the cyclopropane metabolites. Brain concentrations of all metabolites were low relative to blood concentrations. This implies limited metabolite penetration of the blood-brain barrier and little metabolite formation within the brain. IN CONCLUSION:toxicokinetic differences between the pyrethroids did not appear to be important determinants of their relative potency and their effect on motor activity was consistent with a pyrethroid dose additive model.
Measurements from central site (CS) monitors are often used as estimates of exposure in air pollution epidemiological studies. As these measurements are typically limited in their spatiotemporal resolution, true exposure variability within a population is often obscured, leading to potential measurement errors. To fully examine this limitation, we developed a set of alternative daily exposure metrics for each of the 169 ZIP codes in the Atlanta, GA, metropolitan area, from 1999 to 2002, for PM2.5 and its components (elemental carbon (EC), SO4), O3, carbon monoxide (CO), and nitrogen oxides (NOx). Metrics were applied in a study investigating the respiratory health effects of these pollutants. The metrics included: (i) CS measurements (one CS per pollutant); (ii) air quality model results for regional background pollution; (iii) local-scale AERMOD air quality model results; (iv) hybrid air quality model estimates (a combination of (ii) and (iii)); and (iv) population exposure model predictions (SHEDS and APEX). Differences in estimated spatial and temporal variability were compared by exposure metric and pollutant. Comparisons showed that: (i) both hybrid and exposure model estimates exhibited high spatial variability for traffic-related pollutants (CO, NOx, and EC), but little spatial variability among ZIP code centroids for regional pollutants (PM2.5, SO4, and O3); (ii) for all pollutants except NOx, temporal variability was consistent across metrics; (iii) daily hybrid-to-exposure model correlations were strong (r>0.82) for all pollutants, suggesting that when temporal variability of pollutant concentrations is of main interest in an epidemiological application, the use of estimates from either model may yield similar results; (iv) exposure models incorporating infiltration parameters, time-location-activity budgets, and other exposure factors affect the magnitude and spatiotemporal distribution of exposure, especially for local pollutants. The results of this analysis can inform the development of more appropriate exposure metrics for future epidemiological studies of the short-term effects of particulate and gaseous ambient pollutant exposure in a community.
Understanding the longitudinal properties of the time spent in different locations and activities is important in characterizing human exposure to pollutants. The results of a four-season longitudinal time-activity diary study in eight working adults are presented, with the goal of improving the parameterization of human activity algorithms in EPA’s exposure modeling efforts. Despite the longitudinal, multi-season nature of the study, participant non-compliance with the protocol over time did not play a major role in data collection. The diversity ( D )—a ranked intraclass correlation coefficient (ICC)— and lag-one autocorrelation ( A ) statistics of study participants are presented for time spent in outdoor, motor vehicle, residential, and other-indoor locations. Day-type (workday versus non-workday, and weekday versus weekend), season, temperature, and gender differences in the time spent in selected locations and activities are described, and D & A statistics are presented. The overall D and ICC values ranged from approximately 0.08–0.26, while the mean population rank A values ranged from approximately 0.19–0.36. These statistics indicate that intra-individual variability exceeds explained inter-individual variability, and low day-to-day correlations among locations. Most exposure models do not address these behavioral characteristics, and thus underestimate population exposure distributions and subsequent health risks associated with environmental exposures.
Due to extensive use, human exposure to multiple pyrethroid insecticides occurs frequently. Studies of pyrethroid neurotoxicity suggest a common mode of toxicity and that pyrethroids should be considered cumulatively to model risk. The objective of this work was to use a pyrethroid mixture that reflects human exposure to common pyrethroids to develop comparative toxicokinetic profiles in rats, and then model the relationship between brain concentration and motor activity. Data from a national survey of child care centers were used to make a mixture reflecting proportions of the most prevalent pyrethroids: permethrin, cypermethrin, β-cyfluthrin, deltamethrin, and esfenvalerate. The mixture was administered orally at one of two concentrations (11.2 and 27.4 mg/kg) to adult male rats. At intervals from 1 to 24h, motor activity was assessed and the animals were sacrificed. Pyrethroid concentrations were measured in the blood, liver, fat, and brain. After controlling for dose, there were no differences in any tissue concentrations, except blood at the initial time point. Elimination half-lives for all pyrethroids in all tissues were < 7h. Brain concentrations of all pyrethroids (when cis- and trans-permethrin were pooled) at the initial time point were proportional to their relative doses. Decreases in motor activity indicated dose additivity, and the relationship between pyrethroid brain concentration and motor activity was described by a four-parameter sigmoidal Emax model. This study links environmental data with toxicokinetic and neurobehavioral assays to support cumulative risk assessments of pyrethroid pesticides. The results support the additive model of pyrethroid effect on motor activity and suggest that variation in the neurotoxicity of individual pyrethroids is related to toxicodynamic rather than toxicokinetic differences.
PP-29-117 Background/Aims: Surveys in the United States have repeatedly demonstrated the presence and co-occurrence of various pyrethroid pesticides in residences and daycare facilities. Since pyrethroids co-occur and have similar modes of action, pharmacokinetic models will be better informed if data are derived from studies using chemical mixtures. The objective of this research was to develop and apply methods with sufficient sensitivity to determine tissue clearance profiles for a mixture of pyrethroids. Methods: The pyrethroids selected for the mixture (cis- and trans-permethrin, cyfluthrin, cypermethrin, deltamethrin, and esfenvalerate) and their relative proportions in the dosing solution were based on the distribution of pyrethroid residues measured in a nationally representative probability study of 168 child care centers. The pyrethroids were administered orally in a corn oil vehicle to adult male Long-Evans rats. Animals received either a high or low concentration dose and were sacrificed at 1, 2, 4, 8, or 24 hours after dosing. Tissue concentrations in brain, subcutaneous fat, liver, and whole blood were determined. Two replicates of each sample were analyzed to evaluate method reproducibility. Results: There was little variability associated with the replicate tissue results compared with results from different animals at the same dose and time point. The limit of quantitation for all pesticides in all tissues was less than 3 ηg/g and this sensitivity allowed the determination of elimination rate constants for all pyrethroids in blood and brain except the low dose esfenvalerate. Elimination rate constants were also calculated for cis-permethrin, cypermethrin, deltamethrin, and esfenvalerate in liver. The half-life of all pyrethroids in blood, liver, and brain was less than 6 hours while the fat functioned effectively as a storage compartment. Conclusion: The use of empirically based chemical mixtures to determine clearance estimates is feasible and may provide an effective way to relate laboratory kinetic data to human exposure.
Background and Aims: Epidemiological studies of air pollution have traditionally relied upon surrogates of personal exposures, such as ambient concentration measurements from central-site monitoring stations. This study examines the spatial and temporal variations of alternative measured and modeled exposure metrics for multiple pollutants (i.e., particulate matter, elemental carbon, sulfates, nitrogen oxides, carbon monoxide and ozone), developed and applied within an epidemiological study in a large US metropolitan area. Methods: Several tiers of exposure metrics for ambient traffic-related and regional pollutants were used for predicting health impacts of ambient air quality and population exposures on daily ZIP code level emergency department (ED) visits in Atlanta, GA for the period 1999-2002. The approaches included central site or interpolated monitoring data, regional pollution levels based on measurements or models (CMAQ) and local scale (AERMOD) air quality models, hybrid models, statistically blended modeling and measurement data, concentrations adjusted by home infiltration rates based on LBL algorithms utilizing information on housing stock and meteorology, and the population human exposure (SHEDS and APEX) model predictions. Results: The various exposure metrics were compared in their ability to characterize the spatial and temporal variations of multiple ambient air pollutants across the study area. These metrics were then used to examine associations between ambient air pollution and acute morbidity. The pollutant–specific relative risks (RRs) obtained from epidemiological analyses of the alternative exposure metrics were compared to those obtained from using a conventional approach (i.e., central site data alone). Both pollutant and metric dependent differences were found suggesting a complex exposure prediction error structure among the pollutants studied. Conclusions: Our results suggest the need for case-specific enhancements for future exposure assessments in conjunction with different types of individual or multipollutant air pollution epidemiologic study designs.
Urinary metabolites of pyrethroid pesticides have been used as biomarkers to estimate human exposure to the parent insecticide. It is important to establish whether these markers are present in environments or media to which humans are exposed routinely. Failure to account for the contribution of pre-existing markers to urinary concentrations could result in risk assessments that overestimate exposure. The purpose of this study was to quantify the concentrations of 13 selected pyrethroid pesticides and their degradation products in samples of indoor dust that had been collected in vacuum cleaner bags during the children's total exposure to persistent pesticides and other persistent organic pollutants (CTEPP) study of homes and day cares in North Carolina and Ohio. Sieved contents of 85 vacuum cleaner bags were analyzed, and permethrin was found in all samples. Sixty-nine samples contained at least one additional pyrethroid, but none contained more than five pyrethroids in detectable concentrations. Resmethrin, prallethrin, and fenpropathrin were not detected in any samples, while 36 contained phenothrin. The median concentration of permethrin in the samples was 1454 ng/g of dust. Excluding permethrin, pyrethroid concentrations were typically less than or equal to 100 ng/g of dust. The majority of degradates were present in more than half of the dust samples, usually at concentrations of less than or equal to 100 ng/g of dust. For those pyrethroids with a characteristic oxydibenzene group, the cyclopropane degradates were present at higher concentrations than the corresponding benzoic acid moieties. Using urinary concentrations of these metabolites to model human exposure to the parent pyrethroids, may over-estimate risk due to the presence of pre-existing degradates in dust.