National Human Exposure Assessment Survey: analysis of exposure pathways and routes for arsenic and lead in EPA Region 5.

The National Human Exposure Assessment Survey (NHEXAS) Phase I field study conducted in EPA Region 5 (Great Lakes Area) provides extensive exposure data on a representative sample of approximately 250 residents of the region. Associated environmental media and biomarker (blood, urine) concentration data were also obtained for the study participants to aid in understanding of the relationships of exposures to both contaminant pathways and doses. Besides fulfilling the primary NHEXAS objectives, the NHEXAS data provided an opportunity to explore secondary usages, such as examining pathway to route of exposure relationships. A generic type of structural equation model was used to define the anticipated relationships among the various data types for both arsenic (As) and lead (Pb). Since, by design, only a few participants provided data for all sample types, implementing this model required that some media concentrations (outdoor air and soil) be imputed for subjects with missing information by using measurements collected in the same geographic area and time period. The model, and associated pairwise correlations, generally revealed significant but weak associations among the concentrations, exposures, and doses; the strongest associations occurred for the various air measurements (indoor versus outdoor and personal). The generally weak associations were thought to be partly due to the absence of complete coverage of nonresidential environmental media and to nonsynchronization of relevant measurement times and integration periods of collection across the various sample types. In general, relationships between the NHEXAS questionnaire data and the various concentration, exposure, and body-burden measures were also weak. The model results and the modeling exercise suggest several ways for optimizing the design of future exposure assessment studies that are aimed at supporting structural modeling activities.

Measurement of children's exposure to pesticides: analysis of urinary metabolite levels in a probability-based sample.

The Minnesota Children's Pesticide Exposure Study is a probability-based sample of 102 children 3-13 years old who were monitored for commonly used pesticides. During the summer of 1997, first-morning-void urine samples (1-3 per child) were obtained for 88% of study children and analyzed for metabolites of insecticides and herbicides: carbamates and related compounds (1-NAP), atrazine (AM), malathion (MDA), and chlorpyrifos and related compounds (TCPy). TCPy was present in 93% of the samples, whereas 1-NAP, MDA, and AM were detected in 45%, 37%, and 2% of samples, respectively. Measured intrachild means ranged from 1.4 microg/L for MDA to 9.2 microg/L for TCPy, and there was considerable intrachild variability. For children providing three urine samples, geometric mean TCPy levels were greater than the detection limit in 98% of the samples, and nearly half the children had geometric mean 1-NAP and MDA levels greater than the detection limit. Interchild variability was significantly greater than intrachild variability for 1-NAP (p = 0.0037) and TCPy (p < 0.0001). The four metabolites measured were not correlated within urine samples, and children's metabolite levels did not vary systematically by sex, age, race, household income, or putative household pesticide use. On a log scale, mean TCPy levels were significantly higher in urban than in nonurban children (7.2 vs. 4.7 microg/L; p = 0.036). Weighted population mean concentrations were 3.9 [standard error (SE) = 0.7; 95% confidence interval (CI), 2.5, 5.3] microg/L for 1-NAP, 1.7 (SE = 0.3; 95% CI, 1.1, 2.3) microg/L for MDA, and 9.6 (SE = 0.9; 95% CI, 7.8, 11) microg/L for TCPy. The weighted population results estimate the overall mean and variability of metabolite levels for more than 84,000 children in the census tracts sampled. Levels of 1-NAP were lower than reported adult reference range concentrations, whereas TCPy concentrations were substantially higher. Concentrations of MDA were detected more frequently and found at higher levels in children than in a recent nonprobability-based sample of adults. Overall, Minnesota children's TCPy and MDA levels were higher than in recent population-based studies of adults in the United States, but the relative magnitude of intraindividual variability was similar for adults and children.

An assessment of the data quality for NHEXAS--Part I: Exposure to metals and volatile organic chemicals in Region 5.

A National Human Exposure Assessment Survey (NHEXAS) was performed in U.S. Environmental Protection Agency (U.S. EPA) Region V, providing population-based exposure distribution data for metals and volatile organic chemicals (VOCs) in personal, indoor, and outdoor air, drinking water, beverages, food, dust, soil, blood, and urine. One of the principal objectives of NHEXAS was the testing of protocols for acquiring multimedia exposure measurements and developing databases for use in exposure models and assessments. Analysis of the data quality is one element in assessing the performance of the collection and analysis protocols used in NHEXAS. In addition, investigators must have data quality information available to guide their analyses of the study data. At the beginning of the program quality assurance (QA) goals were established for precision, accuracy, and method quantification limits. The assessment of data quality was complicated. First, quality control (QC) data were not available for all analytes and media sampled, because some of the QC data, e.g., precision of duplicate sample analysis, could be derived only if the analyte was present in the media sampled in at least four pairs of sample duplicates. Furthermore, several laboratories were responsible for the analysis of the collected samples. Each laboratory provided QC data according to their protocols and standard operating procedures (SOPs). Detection limits were established for each analyte in each sample type. The calculation of the method detection limits (MDLs) was different for each analytical method. The analytical methods for metals had adequate sensitivity for arsenic, lead, and cadmium in most media but not for chromium. The QA goals for arsenic and lead were met for all media except arsenic in dust and lead in air. The analytical methods for VOCs in air, water, and blood were sufficiently sensitive and met the QA goals, with very few exceptions. Accuracy was assessed as recovery from field controls. The results were excellent (> or = 98%) for metals in drinking water and acceptable (> or = 75%) for all VOCs except o-xylene in air. The recovery of VOCs from drinking water was lower, with all analytes except toluene (98%) in the 60-85% recovery range. The recovery of VOCs from drinking water also decreased when comparing holding times of < 8 and > 8 days. Assessment of the precision of sample collection and analysis was based on the percent relative standard deviation (% RSD) between the results for duplicate samples. In general, the number of duplicate samples (i.e., sample pairs) with measurable data were too few to assess the precision for cadmium and chromium in the various media. For arsenic and lead, the precision was excellent for indoor, and outdoor air (< 10% RSD) and, although not meeting QA goals, it was acceptable for arsenic in urine and lead in blood, but showed much higher variability in dust. There were no data available for metals in water and food to assess the precision of collection and analysis.

Particulate matter and manganese exposures in Indianapolis, Indiana.

The distribution of PM(2.5) and manganese (Mn) personal exposures was determined over a 4-month period in Indianapolis, IN, at a time when the gasoline additive, methylcyclopentadienyl manganese tricarbonyl (MMT), was not being used. The data collection period coincided with the data collection period in the Toronto, ON, study, where MMT had been used as a gasoline additive for over 20 years. The inferential or target population consisted of noninstitutionalized residents of the Indianapolis area during the monitoring period (from May 1996 through August 1996) who were at least 16 years old. The survey instruments used in this study (and also in Toronto) included a household screener form (HSF), a study questionnaire (SQ), and a time and activity questionnaire (TAQ). The SQ was administered to elicit information about the participant and his/her activities, occupation, and surroundings that might be relevant to his/her exposure to particles and Mn. In addition to the personal particulate matter (PM) and elemental 3-day monitoring, 240 participants completed a TAQ on a daily basis during the actual monitoring period. Also, a subset of participants had 3-day outdoor and indoor stationary monitoring at their home (approximately 58 observations), and sampling was conducted at a fixed site (approximately thirty-three 3-day observations). The quality of data was assessed and compared to the Toronto study in terms of linearity of measurement, instrument and method sensitivity, measurement biases, and measurement reproducibility. Twenty-six of the sample filters were subjected to two analyses to characterize the within-laboratory component of precision in terms of relative standard deviations (RSDs). The median RSD for Mn was 8.7%, as compared to 2.2% for Toronto. The quality assurance (QA) laboratory exhibited a clear positive bias relative to the primary laboratory for Al and Ca, but no systematic difference was evident for Mn. A high interlaboratory correlation (>0.99) was also attained for Mn. Mean field blank results for PM and Mn were 0.87 microg/m(3) and 0.71 ng/m(3), respectively, which were comparable to the Toronto study. The median RSDs for colocated fixed site and residential samples ranged from 2.2% to 9.0% for PM and from 8.8% to 15.3% for Mn, which were close to those observed in Toronto. For the PM(10), the 90th percentile indoors was 124 microg/m(3) compared with 54 microg/m(3) outdoors. This pattern was even more pronounced for the PM(2.5) data (90th percentiles of 92 microg/m(3) indoors vs 30 microg/m(3) outdoors). Personal PM(2.5) was somewhat higher than the indoor levels, but the percentiles seemed to follow the more highly skewed pattern of the indoor distribution. This difference was largely due to the presence of some smokers in the sample; e.g., exclusion of smokers led to a personal exposure distribution that was more similar to the outdoor distribution. The estimated 90th percentile for the nonsmokers' personal exposures to PM was 43 microg/m(3) compared with 84 microg/m(3) for the overall population. In general, the Indianapolis PM levels of a given type and cut size were somewhat higher than the levels observed in Toronto, e.g., the median and 90th percentile for the personal PM(2.5) exposures were 23 and 85 microg/m(3), respectively, in Indianapolis, while in Toronto, the corresponding percentiles were 19 and 63 microg/m(3). The cities' distributions of the proportion of the PM(10) mass in the 2.5-microm fraction appeared similar for the residential outdoor data (medians of 0.67 and 0.65 for Indianapolis and Toronto, respectively, and 90th percentiles of 0.83 for both cities). For the indoor data, Indianapolis tended to have a larger portion of the mass in the fine fraction (median of 0.80 compared to 0.70 for Toronto). Unlike the PM, the Indianapolis indoor Mn concentration levels were substantially lower than the outdoor levels for both PM sizes, and the median personal levels for Mn in PM(2.5) appeared to fall between the median indoor and outdoor levels. The personal Mn exposure distributions exhibited more skewness than the indoor or outdoor distributions (e.g., the means for the personal, indoor, and outdoor distributions were 7.5, 2.6, and 3.5 ng/m(3), respectively, while the medians were 2.8, 2.2, and 3.2 ng/m(3), respectively). At least a substantial portion of the high end of the personal exposure distribution appeared to be associated with occupational exposures to Mn. In general, the Mn levels in both cut sizes in Indianapolis were approximately 5 ng/m(3) smaller than those in Toronto (e.g., the estimated median and mean levels for personal Mn exposures in PM(2.5) were 2.8 and 7.5 ng/m(3), respectively, in Indianapolis, but were 8.0 and 13.1 ng/m(3) in Toronto). For the nonoccupational subgroups with no exposure to smoking and no subway riders in the two cities, the medians (2.6 ng/m(3) in Indianapolis and 7.8 ng/m(3) in Toronto) were similar to those for the overall populations, but the means were substantially smaller (3.1 ng/m(3) in Indianapolis and 9.2 ng/m(3) in Toronto). The median proportion of Mn in the fine fraction (relative to the PM(10) Mn) for Indianapolis was 0.39 for outdoors and 0.55 for indoors; these ratios were somewhat smaller than the corresponding Toronto medians (0.52 and 0.73). The study found high correlations for particulates and Mn between personal exposures and indoor concentrations, and between outdoor and fixed site concentrations, and low correlations of personal and indoor levels with outdoor and fixed site levels. The pattern was similar to that observed for Toronto, but slightly more pronounced. The PM(10) Mn concentrations (log scale) generally exhibited stronger associations among these various measures than the PM(2.5) Mn concentrations. Comparisons of the particulate distributions between PTEAM (Riverside, CA) and the Indianapolis and Toronto studies were also made.

Quantitative analysis of children's microactivity patterns: The Minnesota Children's Pesticide Exposure Study.

The National Human Exposure Assessment Survey (NHEXAS)/Minnesota Children's Pesticide Exposure Study (MNCPES) was a population-based study designed to characterize children's exposure to residential pesticides and to evaluate the contribution of residential and children's activities to children's exposure. Families of 168 children were surveyed for residential use of pesticides and children's activities. From these homes, families of 102 children between the ages of 3 and 13 years participated in a week-long intensive exposure study. Of the 102 children, 19 children were videotaped for four consecutive hours in their normal daily activities. The survey responses indicated that the youngest children were more likely to exhibit behaviors that would foster exposure to environmental contaminants. Comparison of questionnaire responses indicated that the videotaped subsample was representative of the exposure study population. The microactivities of the videotaped children that might contribute to their exposure via ingestion or dermal routes were quantified. Hand-to-mouth and object-to-mouth activities were observed most frequently among the youngest children. The youngest children were also most likely to be barefoot both indoors and outside. Gender differences were found in mouthing behavior and the proportion of observed time spent outdoors.

Design strategy for assessing multi-pathway exposure for children: the Minnesota Children's Pesticide Exposure Study (MNCPES).

Although children are exposed to a variety of environmental hazards, including pesticides, there is a scarcity of information available to estimate exposures realistically. This article reports on one of the first attempts to measure multi-pathway pesticide exposures in a population-based sample of urban and non-urban children. A design strategy was developed to assess multi-pathway pesticide exposures in children using personal exposure measurements in combination with complimentary measurements of biological markers of exposure, concentrations in relevant environmental media, and time spent in important microenvironments and participating in exposure-related activities. Sample collection and analysis emphasized measurement of three insecticides (i.e., chlorpyrifos, diazinon, and malathion) and one herbicide (i.e., atrazine). These compounds were selected because of their frequent use, presence in multiple environmental media, expected population exposures, and related hazard/toxicity. The study was conducted during the summer of 1997 in Minnesota and involved a stratified sample of households with children ages 3-12 years. Participants resided in either (a) the cities of Minneapolis and St. Paul (urban households), or (b) Rice and Goodhue Counties just south of the metropolitan area (non-urban households). Results from a residential inventory documenting storage and use of products containing the target pesticides were used to preferentially select households where children were likely to have higher exposures. The study successfully obtained pesticide exposure data for 102 children, including measurements of personal exposures (air, hand rinse, duplicate diet), environmental concentrations (residential indoor/outdoor air, drinking water, residential surfaces, soil), activity patterns (obtained by questionnaire, diary, videotaping), and internal dose (metabolites in urine).

Measurement of multi-pollutant and multi-pathway exposures in a probability-based sample of children: practical strategies for effective field studies.

The purpose of this manuscript is to describe the practical strategies developed for the implementation of the Minnesota Children's Pesticide Exposure Study (MNCPES), which is one of the first probability-based samples of multi-pathway and multi-pesticide exposures in children. The primary objective of MNCPES was to characterize children's exposure to selected pesticides through a combination of questionnaires, personal exposure measurements (i.e., air, duplicate diet, hand rinse), and complementary monitoring of biological samples (i.e., pesticide metabolites in urine), environmental samples (i.e., residential indoor/outdoor air, drinking water, dust on residential surfaces, soil), and children's activity patterns. A cross-sectional design employing a stratified random sample was used to identify homes with age-eligible children and screen residences to facilitate oversampling of households with higher potential exposures. Numerous techniques were employed in the study, including in-person contact by locally based interviewers, brief and highly focused home visits, graduated subject incentives, and training of parents and children to assist in sample collection. It is not feasible to quantify increases in rates of subject recruitment, retention, or compliance that resulted from the techniques employed in this study. Nevertheless, results indicate that the total package of implemented procedures was instrumental in obtaining a high percentage of valid samples for targeted households and environmental media.

Factors influencing total dietary exposures of young children.

A deterministic model was developed to identify the critical input parameters needed to assess dietary intakes of young children. The model was used as a framework for understanding the important factors in data collection and data analysis. Factors incorporated into the model included transfer efficiencies of pesticide from surfaces to food, transfer efficiencies of pesticide from surfaces to hands to food, and more accurate microactivity data related to contact frequency for the three variables of interest--hands, surfaces, and food. Results from range-finding measurements of transfer efficiencies using an aqueous pesticide solution of a mixture of malathion, diazinon, and chlorpyrifos sprayed on the surfaces indicate that a higher pesticide transfer occurred from hard surfaces to food (hardwood, plastic), with low transfer from soft surfaces (carpet, cloth). Six children, all less than 4 years old, were videotaped to obtain realistic contact frequency and times for the interaction of hands, surfaces, and foods during eating meals and snacks while in their homes or day care centers. The time range of eating events varied from about 2 to 55 min, with an average of about 20 min. The average number of contact frequencies between food and hands was 19 times for each eating event, with a range of 10-40. Contacts between the surface and hand were about the same as the food and hands. Contacts between foods and surfaces ranged from 0 to 32, but only five or less of the contacts per eating event were associated with surfaces other than eating utensil. The children's microactivity data collected during the eating events, together with the laboratory results from the transfer studies, were provided as input into a Monte Carlo simulation of the dietary ingestion model. Simulation results indicate that children's handling of the food could contribute 20-80% of the total dietary intake of pesticides. Dietary exposure due to residues in the food before handling accounted for 16% and 47%, respectively, of the total mean intake from simulations for a child's consumption of an apple or banana. These results indicated that transfer efficiencies for foods on various surfaces typically found in homes as well as children's hand contacts with the food and surfaces are important as determinants of dietary exposure.

Collecting urine samples from young children using cotton gauze for pesticide studies.

To estimate pesticide exposure, urine samples are often needed to analyze pesticide metabolites. However, this is difficult for children wearing diapers because simple and feasible techniques suitable for field collection are not available. The objectives of this study were to test the validity of using cotton gauze pad as a medium for collecting urine samples from young children and to examine the stability of the recoveries for creatinine and pesticide metabolites over 24 h. Urine spiked with a pesticide and four metabolites, 2,4-dichlorophenoxyacetic acid (which is mainly eliminated from urine unchanged), 3-phenoxybenzoic acid (metabolite for synthetic pyrethroids), atrazine mercapturate (metabolite for atrazine), malathion dicarboxylic acid (metabolite for malathion), and 2-isopropyl-4-methyl-6-hydroxypyrimidine (metabolite for diazinon) was added to the gauze pads and kept in jars at 37 degrees C in a water bath. Urine was expressed from the gauze pads immediately and after 1, 2, 4, 8, and 24 h, then analyzed. The recoveries, calculated as the percentage of concentration in expressed urine divided by that of the control urine sample, were within a range of 70-130%. The metabolite and creatinine concentrations did not change with time in either expressed urine samples or controls. The results suggest that cotton gauze pad is a promising candidate for collecting urine samples from young children wearing diapers for studies in which these five urinary pesticide metabolites are to be analyzed.

Dietary exposure of children in lead-laden environments.

Children are the most susceptible population to lead exposure because of three interacting factors; they have more opportunity for contact with lead sources due to their activities, lead absorption occurs more readily in a child compared to an adult, and the child's development is more vulnerable to lead than adults. Low levels of lead in the blood have been shown to cause adverse health effects; the level of concern for children is currently 10 microg/dl. The contribution of dietary exposure of lead to increased blood lead levels (PbB) is not well characterized. This study was conducted to measure potential dietary lead intakes of children 2 to 3 years of age who live in homes contaminated with environmental lead. Objectives were to estimate lead intakes for children consuming food in contaminated environments, recognizing unstructured eating patterns and to investigate if correlations exist between daily dietary exposure and measured PbB. Dietary exposure was evaluated by collecting samples that were typical of the foods the young children ate in their homes. A 24-h duplicate of all foods plus sentinel foods, i.e., individual items used to represent foods contaminated during handling, were collected from 48 children. Ten homes were revisited to obtain information on the variation in daily dietary intakes. Drinking water was evaluated both as part of the segregated beverage sample composite and by itself. Additional information collected included lead concentrations from hand wipes, floor wipes, and venous blood, and questionnaire responses from the caregiver on activities potentially related to exposure. Activities and hygiene practices of the children and contamination of foods in their environment influences total dietary intake. Estimated mean dietary intakes of lead (29.2 microg Pb/day) were more than three times the measured 24-h duplicate-diet levels (8.37 microg Pb/day), which were almost six times higher than current national estimates (1.40 microg Pb/day). Statistically significant correlations were observed between floor wipes and foods contacting contaminated surfaces, hand wipes and foods contacting contaminated hands and surfaces, and hand wipes and floor wipes. This study indicates that the dietary pathway of exposure to lead is impacted by eating activities of children living in lead-contaminated environments and that analysis of foods themselves is not enough to determine excess dietary exposures that are occurring.

Sampling design, response rates, and analysis weights for the National Human Exposure Assessment Survey (NHEXAS) in EPA region 5.

For the Phase I field test of the National Human Exposure Assessment Survey (NHEXAS) in U.S. Environmental Protection Agency (EPA) Region 5, this paper presents the survey sampling design, the response rates achieved, and the sample weighting procedure implemented to compensate for unit nonresponse. To enable statistically defensible inferences to the entire region, a sample of about 250 members of the household population in EPA Region 5 was selected using a stratified multistage probability-based survey sampling design. Sample selection proceeded in four nested stages: (1) sample counties; (2) area segments based on Census blocks within sample counties; (3) housing units (HUs) within sample segments; and (4) individual participants within sample households. Each fourth-stage sample member was asked to participate in 6 days of exposure monitoring. A subsample of participants was asked to participate in two rounds of longitudinal follow-up data collection. Approximately 70% of all sample households participated in household screening interviews in which rosters of household members were developed. Over 70% of the sample subjects selected from these households completed the Baseline Questionnaire regarding their demographic characteristics and potential for exposures. And, over 75% of these sample members went on to complete at least the core environmental monitoring, including personal exposures to volatile organic compounds (VOCs) and tap water concentrations of metals. The sample weighting procedures used the data collected in the screening interviews for all household members to fit logistic models for nonresponse in the later phases of the study. Moreover, the statistical analysis weights were poststratified to 1994 State population projections obtained from the Bureau of the Census to ensure consistency with other statistics for the Region.

National Human Exposure Assessment Survey (NHEXAS): distributions and associations of lead, arsenic and volatile organic compounds in EPA region 5.

The National Human Exposure Assessment Survey (NHEXAS) Phase I field study conducted in EPA Region 5 provides extensive exposure data on approximately 250 study participants selected via probability sampling. Associated environmental media and biomarker (blood, urine) concentration data were also obtained to aid in the understanding of relationships of the exposures to both contaminant sources and doses. Distributional parameters for arsenic (As), lead (Pb), and four volatile organic compounds (VOCs)--benzene, chloroform, tetrachloroethylene, and trichloroethylene--were estimated for each of the relevant media using weighted data analysis techniques. Inter-media associations were investigated through correlation analysis, and longitudinal correlations and models were used to investigate longitudinal patterns. Solid food appeared to be a major contributor to urine As levels, while Pb levels in household (HH) dust, personal air, and beverages all were significantly associated with blood Pb levels. Relatively high (>0.50) longitudinal correlations were observed for tap water Pb and As, as compared to only moderate longitudinal correlations for the personal air VOCs.

Analysis of mercury in hair of EPA region V population.

A scoping study, the National Human Exposure Assessment Survey (NHEXAS) was conducted in EPA Region V from July 1995 to May 1997. This probability-based population study provided an opportunity to examine the mercury levels in 182 participants who provided hair samples. A sensitive analytical procedure based on atomic fluorescence spectrometry was developed and evaluated for the analysis of Hg in approximately 5 mg of human hair. The correlation coefficient (r), the precision, and bias were 0.9983, < or = 1.6%, and < or = 8%, respectively, for standard curves in the hair matrix. The method detection limit (MDL), recovery of Hg in a certified sample (NIES-13), precision (% RSD) for duplicate extract analysis, and precision for duplicate sample analysis averaged 12 ppb (range 4 to 22 ppb), 100 +/- 3% (N=27), 4.6 +/- 2.8 (N=18), and 12.5 +/- 7.4 (N=17), respectively, over the 7 to 8 months of sample analysis. The low MDL yielded 95% of the samples with measurable values, permitting the entire distribution of Hg levels to be characterized. Comparison of annualized Hg distribution in hair with and without background correction revealed a negligible bias on the distribution (1.47% at the 90th percentile). Also, a comparison of the unweighted and nonannualized weighted Hg levels throughout the percentile distribution indicated a small deviation in the upper tail (95th percentile) and is attributable to the small sample size (N=182). The mean, median, and maximum of the annualized Hg levels in hair were 287, 204, and 3505 ppb, respectively. The 75th percentiles were 335 and 368 ppb for the weighted annualized and unweighted distributions, respectively. The percent of individuals in three age categories (0-24, 25-49, and 50 years and older) who exceeded the 75th percentile showed a linear increase with age. Males (N=81) had 10% and 20% lower mean levels than females (N=101) for unweighted and annualized weighted Hg data, respectively. The application of this methodology for characterizing hair Hg levels in fish-eating populations is discussed.

Population-based dietary intakes and tap water concentrations for selected elements in the EPA region V National Human Exposure Assessment Survey (NHEXAS).

A National Human Exposure Assessment Survey (NHEXAS) field study was performed in U.S. Environmental Protection Agency (EPA) Region V, providing population-based exposure distribution data for selected elements in several personal, environmental, and biological media. Population distributions are reported for the 11 elements that were measured in water and dietary samples. Dietary intakes and home tap water concentrations of lead, arsenic, and cadmium were further examined for intermedia associations, for differences between dietary exposure for adults and children, and to estimate the proportion of the population above health-based reference values (dietary) or regulatory action levels or maximum contaminant levels (water). Water lead and arsenic concentrations were significantly associated with dietary intake. Intake of all elements was higher from solid foods than from liquid foods (including drinking water). Dietary intakes of Pb, As, and Cd were greater than those calculated for intake from home tap water or inhalation on a microg/day basis. Median dietary intakes for the Region V population for Pb, As, and Cd were 0.10, 0.13, and 0.19 microg/kg bw/day, respectively. While Pb, As, and Cd concentrations in the foods consumed by 0 to 6-year-old children were similar to or lower than those for adults, dietary intakes calculated on a body weight basis were 1.5 to 2.5 times higher for young children. Intrapersonal intake differences accounted for most of the variance in short-term (daily) dietary intakes for Pb and As, while interpersonal differences accounted for more of the intake variance for Cd. Only small percentages of the population exceeded health-based intake reference values or concentrations equal to regulatory levels in water for Pb, As, and Cd.

National human exposure assessment survey (NHEXAS): exploratory survey of exposure among population subgroups in EPA Region V.

The National Human Exposure Assessment Survey (NHEXAS) provides a rich database of exposure and environmental measurements for persons living in EPA Region V (Great Lakes). Demographics (e.g., gender, minority status, age, income, and year home built) between U.S. Census data and the overall Region V sample were compared and showed good agreement. This representative sample was used to conduct an exploratory investigation of selected subpopulations that might exhibit higher exposures, on average, to volatile organic chemicals (VOCs) such as benzene, chloroform, etc.; inspirable particles; and metals (e.g., lead, arsenic, etc.) than the general population in Region V. Means and medians were the metrics of comparison. Personal air exposures for p-dichlorobenzene were significantly higher in adults (> 21 years old) than in children (1-14 years old) (median: below detection limit vs. 0.87 microgram/m3, p = 0.0005), while a trend toward higher levels of arsenic exposure in children than adults was observed (median: 1.13 vs. 0.8 ng/m3, p = 0.083). A trend towards higher personal air exposure to lead for minorities vs. nonminorities was evident (median: 26 vs. 12 ng/m3, p = 0.066), but personal exposure to 1,1,1-trichloroethane tended to be higher in nonminorities (mean: 22 vs. 3.7 micrograms/m3, p = 0.081). Dietary exposure to arsenic from solid foods was significantly higher in adults than children (mean: 21 vs. 7.1 micrograms/kg, p = 0.0001; median: 10 vs. 5.6 micrograms/kg, p = < 0.001), and for cadmium it was higher for nonminorities than minorities (median: 18 vs. 15 micrograms/kg, p = 0.023). In contrast, the dietary intake for arsenic, which is based on body weight, was significantly higher in children than adults (mean: 1.72 vs 1.38 micrograms/kg-1 day-1, p = < 0.0001; median 1.02 vs. 0.83, p = < 0.0001). Dietary exposure to chromium in beverages tended to be higher in minorities than nonminorities (median: 16 vs. 13 micrograms/kg, p = 0.017). Lead levels in surface dust wipes tended to increase with the age of the home (mean: 128 micrograms/g in homes built since 1980 to 1075 micrograms/g in homes built before 1940; median: 93 to 236 micrograms/g, respectively). These findings were consistent with the observation that for persons living in older homes personal air exposures to lead are elevated compared to persons living in recently built homes (median: 12 ng/m3 in homes built since 1980, vs. 24 ng/m3 in homes built before 1940, p = 0.043).

Uptake and decay of volatile organic compounds at environmental concentrations: application of a four-compartment model to a chamber study of five human subjects.

Five subjects were exposed to nine volatile organic compounds (VOCs) at concentrations that can be encountered in everyday life. Breath samples were collected during a 10-h uptake phase and a 24-h decay phase. It was possible to determine four distinct slopes in the decay curve for each chemical. The distribution in the body and residence times in different tissues were calculated using a linear four-compartment mass-balance model. The model was used to predict breath concentrations for two subjects in a second chamber experiment including the same nine VOCs, representing three chemical classes (aromatic, aliphatic, and chlorinated compounds). Predicted values were generally within 25% of those observed, suggesting that the model parameters calculated here could be useful in estimating exposure and body burden to other VOCs in these three classes. Median residence times for the nine VOCs ranged from 3-12 min for compartment 1 (metabolizing); 0.3-2 h for compartment 2; 2-5 h for compartment 3; and 1-4 d for compartment 4. The fraction of the parent compound exhaled at equilibrium was estimated to range from 0.06-0.16 for four aromatic compounds and decane; 0.22-0.23 for trichloroethylene and dichloromethane; 0.35 for hexane; and 0.88 for 1,1,1-trichloroethane. Limited blood measurements were obtained for six of the nine VOCs in two subjects simultaneously with the breath samples over four-hour decay periods. Blood/breath ratios agreed well between the two subjects, but were higher than human blood/air partition coefficients reported in subjects exposed to high concentrations. This observation is consistent with results from other studies at relatively low concentrations.

Testing duplicate diet sample collection methods for measuring personal dietary exposures to chemical contaminants.

Dietary ingestion may be a significant pathway of human exposure to many potentially toxic chemicals. The U.S. Environmental Protection Agency-National Human Exposure Laboratory has made the development of methods for measuring personal dietary exposures a high priority for its dietary exposure research program. Of particular interest was the testing of methods that could be applied in the general population as one component of multipathway exposure measurement studies. This paper describes a controlled pilot study that was conducted to evaluate procedures for collecting and processing duplicate diet samples. Nine adult and three child participants volunteered to provide dietary information for 28 days, and duplicate portions of all foods consumed daily for seven consecutive days. Sample collection procedures were evaluated for participant collection and segregation of solid and liquid foods, and for identification and separation of high-fat and low-fat foods. Methods for compositing and homogenizing mixed diet samples were tested. Food records and questionnaires were tested to document the collected food and to evaluate procedures for assessing dietary changes and collection bias. Participant time and monetary needs were evaluated along with the approach for training and providing support to study participants. Participants were able to collect 96% of the meals they consumed, even with 33% of the meals consumed away from home. Food consumed in social settings was the most difficult to collect, and participants were unable or unwilling to collect foods in some social settings. Noncollection of meals and food items increased after the third day of collection. Mixed diet samples were successfully homogenized, with 1%-11% mean relative standard deviations for moisture, fat, protein, and ash analysis in replicate sample aliquots. The laboratory-measured caloric content of collected foods was an average of 12% (range: -24% to 36%) lower than estimates of energy intake using a food diary and 16% lower than estimated energy expenditure values.

Mutagens from heated Chinese and U.S. cooking oils.

BACKGROUND: The lung cancer incidence in Chinese women is among the highest in the world, but tobacco smoking accounts for only a minority of the cancers. Epidemiologic investigations of lung cancer among Chinese women have implicated exposure to indoor air pollution from wok cooking, where the volatile emissions from unrefined cooking oils are mutagenic. PURPOSE: This study was conducted to identify and quantify the potentially mutagenic substances emitted from a variety of cooking oils heated to the temperatures typically used in wok cooking. METHODS: Several cooking oils and fatty acids were heated in a wok to boiling, at temperatures (for the cooking oils) that ranged from 240 degrees C to 280 degrees C (typical cooking temperatures in Shanghai, China). The oils tested were unrefined Chinese rapeseed, refined U.S. rapeseed (known as canola), Chinese soybean, and Chinese peanut in addition to linolenic, linoleic, and erucic fatty acids. Condensates of the emissions were collected and tested in the Salmonella mutation assay (using Salmonella typhimurium tester strains TA98 and TA104). Volatile decomposition products also were subjected to gas chromatography and mass spectroscopy. Aldehydes were detected using high-performance liquid chromatography and UV spectroscopy. RESULTS: 1,3-Butadiene, benzene, acrolein, formaldehyde, and other related compounds were qualitatively and quantitatively detected, with emissions tending to be highest for unrefined Chinese rapeseed oil and lowest for peanut oil. The emission of 1,3-butadiene and benzene was approximately 22-fold and 12-fold higher, respectively, from heated unrefined Chinese rapeseed oil than from heated peanut oil. Lowering the cooking temperatures or adding an antioxidant, such as butylated hydroxyanisole, before cooking decreased the amount of these volatile emissions. Among the individual fatty acids tested, heated linolenic acid produced the greatest quantities of 1,3-butadiene, benzene, and acrolein. Separately, the mutagenicity of individual volatile emission condensates was correlated with linolenic acid content (r = .83; P = .0004). Condensates from heated linolenic acid, but not linoleic or erucic acid, were highly mutagenic. CONCLUSIONS: These studies, combined with experimental and epidemiologic findings, suggest that high-temperature wok cooking with unrefined Chinese rapeseed oil may increase lung cancer risk. This study indicates methods that may reduce that risk. IMPLICATIONS: The common use of wok cooking in China might be an important but controllable risk factor in the etiology of lung cancer. In the United States, where cooking oils are usually refined for purity, additional studies should be conducted to further quantify the potential risks of such methods of cooking.

Recent advances in measuring exhaled breath and estimating exposure and body burden for volatile organic compounds (VOCs).

An improved portable breath measurement method has been developed that allows 1-min sampling times. The equipment has been successfully tested in field and chamber studies. Results of these studies suggest that breath levels following known exposures are predictable and reproducible across a small number of volunteers. The residence times in the body and the distribution in body compartments of several common air toxics have been determined. A simple four-compartment linear model is capable of fitting the observed data. The main parameters of the model include the fraction f of the parent compound exhaled under steady-state conditions and the residence times tau i, in the tau ith compartment. The values of these parameters for several VOCs and for the four body compartments (blood, vessel-rich tissues, vessel-poor tissues, and fat) are provided.