Sydney M. Gordon

Residential environmental measurements in the national human exposure assessment survey (NHEXAS) pilot study in Arizona: preliminary results for pesticides and VOCs.

A major objective of the National Human Exposure Assessment Survey (NHEXAS) performed in Arizona was to conduct residential environmental and biomarker measurements of selected pesticides (chlorpyrifos, diazinon), volatile organic compounds (VOCs; benzene, toluene, trichloroethene, formaldehyde, 1,3-butadiene), and metals for total human exposure assessments. Both personal (e.g., blood, urine, dermal wipes, 24 h duplicate diet) and microenvironmental (e.g., indoor and outdoor air, house dust, foundation soil) samples were collected in each home in order to describe individual exposure via ingestion, inhalation, and dermal pathways, and to extrapolate trends to larger populations. This paper is a preliminary report of only the microenvironmental and dermal wipe data obtained for the target pesticides and VOCs, and provides comparisons with results from similar studies. Evaluations of total exposure from all sources and pathways will be addressed in future papers. The pesticides and VOCs all showed log-normal distributions of concentrations in the Arizona population sampled, and in most cases were detected with sufficient frequency to allow unequivocal description of the concentration by media at the 90th, 75th, and 50th (median) percentiles. Those combinations of pollutant and media, in which a large fraction of the measurements were below the detection limit of the analysis method used, included trichloroethene, 1,3-butadiene, and formaldehyde in outdoor air; chlorpyrifos and diazinon in outdoor air; and diazinon in dermal and window sill wipes. In general, indoor air concentrations were higher than outdoor air concentrations for all VOCs and pesticides investigated, and VOC levels were in good agreement with levels reported in other studies. In addition, the agreement obtained between co-located VOC samplers indicated that the low-cost diffusional badges used to measure concentrations are probably adequate for use in future monitoring studies. For the pesticides, the median levels found in indoor samples agreed well with other studies, although the levels corresponding to the upper 0.1–1% of the population were considerably higher than levels reported elsewhere, with indoor air levels as high as 3.3 and 20.5 µg/m3 for chlorpyrifos and diazinon, respectively. These data showed excellent correlation (Pearson and Spearman correlation coefficients of 0.998 and 0.998, respectively) between chlorpyrifos in indoor air and in the corresponding dermal wipes, and relatively poor correlation between chlorpyrifos in dust (µg/g or µg/m2) and dermal wipes (Pearson=0.055 µg/g and 0.015 µg/m2; Spearman=0.644 µg/g and 0.578 µg/m2). These data suggest the importance of dermal penetration of semi-volatiles as a route of residential human exposure.

Influence of tap water quality and household water use activities on indoor air and internal dose levels of trihalomethanes

Individual exposure to trihalomethanes (THMs) in tap water can occur through ingestion, inhalation, or dermal exposure. Studies indicate that activities associated with inhaled or dermal exposure routes result in a greater increase in blood THM concentration than does ingestion. We measured blood and exhaled air concentrations of THM as biomarkers of exposure to participants conducting 14 common household water use activities, including ingestion of hot and cold tap water beverages, showering, clothes washing, hand washing, bathing, dish washing, and indirect shower exposure. We conducted our study at a single residence in each of two water utility service areas, one with relatively high and the other low total THM in the residence tap water. To maintain a consistent exposure environment for seven participants, we controlled water use activities, exposure time, air exchange, water flow and temperature, and nonstudy THM sources to the indoor air. We collected reference samples for water supply and air (pre–water use activity), as well as tap water and ambient air samples. We collected blood samples before and after each activity and exhaled breath samples at baseline and postactivity. All hot water use activities yielded a 2-fold increase in blood or breath THM concentrations for at least one individual. The greatest observed increase in blood and exhaled breath THM concentration in any participant was due to showering (direct and indirect), bathing, and hand dishwashing. Average increase in blood THM concentration ranged from 57 to 358 pg/mL due to these activities. More research is needed to determine whether acute and frequent exposures to THM at these concentrations have public health implications. Further research is also needed in designing epidemiologic studies that minimize data collection burden yet maximize accuracy in classification of dermal and inhalation THM exposure during hot water use activities.

Breath measurements as volatile organic compound biomarkers.

A brief review of the uses of breath analysis in studies of environmental exposure to volatile organic compounds (VOCs) is provided. The U.S. Environmental Protection Agencys large-scale Total Exposure Assessment Methodology Studies have measured concentrations of 32 target VOCs in the exhaled breath of about 800 residents of various U.S. cities. Since the previous 12-hr integrated personal air exposures to the same chemicals were also measured, the relation between exposure and body burden is illuminated. Another major use of the breath measurements has been to detect unmeasured pathways of exposure; the major impact of active smoking on exposure to benzene and styrene was detected in this way. Following the earlier field studies, a series of chamber studies have provided estimates of several important physiological parameters. Among these are the fraction, f, of the inhaled chemical that is exhaled under steady-state conditions and the residence times. tau i in several body compartments, which may be associated with the blood (or liver), organs, muscle, and fat. Most of the targeted VOCs appear to have similar residence times of a few minutes, 30 min, several hours, and several days in the respective tissue groups. Knowledge of these parameters can be helpful in estimating body burden from exposure or vice versa and in planning environmental studies, particularly in setting times to monitor breath in studies of the variation with time of body burden. Improvements in breath methods have made it possible to study short-term peak exposure situations such as filling a gas tank or taking a shower in contaminated water.

Monitoring methods for polycyclic aromatic hydrocarbons and their distribution in house dust and track-in soil

An analytical method was developed and employed to determine polycyclic aromatic hydrocarbons (PAH) in house dust and soil. The method was applied to the analysis of samples collected in an eight-home pilot study that was conducted in Columbus, OH, before and after the 1992/1993 heating season. The purpose of the study was to obtain concentration profiles of PAH in house dust and track-in soil, and to determine whether the track-in of outdoor soil contributes to PAH in house dust. A total of 19 PAH, ranging from naphthalene (2-ring) to coronene (7-ring), were monitored. The sums of concentrations of the 19 PAH ranged from 16 to 580 ppm (w/w) in house dust, from 58 to 5500 ppm in entryway soil, from 0.58 to 1200 ppm in pathway soil, and from 0.63 to 63 ppm in foundation soil. In general, the concentration trend was as follows : entryway soil > house dust > pathway soil > foundation soil. PAH levels in house dust and track-in soil were of the same order of magnitude before and after the heating season. In house dust samples, levels of most 4- to 6-ring PAH, the sums of the 19 PAH, and the sums of the PAH that are probable carcinogens correlated well (r > 0.90 at p < 0.001) with the corresponding levels in the entryway soil samples.

Design and sampling methodology for a large study of preschool children's aggregate exposures to persistent organic pollutants in their everyday environments.

Young children, because of their immaturity and their rapid development compared to adults, are considered to be more susceptible to the health effects of environmental pollutants. They are also more likely to be exposed to these pollutants, because of their continual exploration of their environments with all their senses. Although there has been increased emphasis in recent years on exposure research aimed at this specific susceptible population, there are still large gaps in the available data, especially in the area of chronic, low-level exposures of children in their home and school environments. A research program on preschool childrens exposures was established in 1996 at the USEPA National Exposure Research Laboratory. The emphasis of this program is on childrens aggregate exposures to common contaminants in their everyday environments, from multiple media, through all routes of exposure. The current research project, “Childrens Total Exposure to Persistent Pesticides and Other Persistent Organic Pollutants,” (CTEPP), is a pilot-scale study of the exposures of 257 children, ages 1½–5 years, and their primary adult caregivers to contaminants in their everyday surroundings. The contaminants of interest include several pesticides, phenols, polychlorinated biphenyls, polycyclic aromatic hydrocarbons, and phthalate esters. Field recruitment and data collection began in February 2000 in North Carolina and were completed in November 2001 in Ohio. This paper describes the design strategy, survey sampling, recruiting, and field methods for the CTEPP study.

Changes in breath trihalomethane levels resulting from household water-use activities

Common household water-use activities such as showering, bathing, drinking, and washing clothes or dishes are potentially important contributors to individual exposure to trihalomethanes (THMs), the major class of disinfection by-products of water treated with chlorine. Previous studies have focused on showering or bathing activities. In this study, we selected 12 common water-use activities and determined which may lead to the greatest THM exposures and result in the greatest increase in the internal dose. Seven subjects performed the various water-use activities in two residences served by water utilities with relatively high and moderate total THM levels. To maintain a consistent exposure environment, the activities, exposure times, air exchange rates, water flows, water temperatures, and extraneous THM emissions to the indoor air were carefully controlled. Water, indoor air, blood, and exhaled-breath samples were collected during each exposure session for each activity, in accordance with a strict, well-defined protocol. Although showering (for 10 min) and bathing (for 14 min), as well as machine washing of clothes and opening mechanical dishwashers at the end of the cycle, resulted in substantial increases in indoor air chloroform concentrations, only showering and bathing caused significant increases in the breath chloroform levels. In the case of bromodichloromethane (BDCM), only bathing yielded a significantly higher air level in relation to the preexposure concentration. For chloroform from showering, strong correlations were observed for indoor air and exhaled breath, blood and exhaled breath, indoor air and blood, and tap water and blood. Only water and breath, and blood and breath were significantly associated for chloroform from bathing. For BDCM, significant correlations were obtained for blood and air, and blood and water from showering. Neither dibromochloromethane nor bromoform gave measurable breath concentrations for any of the activities investigated because of their much lower tap-water concentrations. Future studies will address the effects that changes in these common water-use activities may have on exposure.

The National Human Exposure Assessment Survey (NHEXAS) study in Arizona—introduction and preliminary results

The objective of the National Human Exposure Assessment Survey (NHEXAS) in Arizona is to determine the multimedia distribution of total human exposure to environmental pollutants in the classes of metals, pesticides, and volatile organic compounds (VOCs) for the population of Arizona. This was accomplished by studying a probability-based sample of the total population in Arizona with a nested design for the different stages of sampling (954 Stage I, 505 Stage II, and 179 Stage III participants). This report compares the study population demographics with those from the U.S. Census and provides preliminary data on the distributions of the example pollutant for each class, lead for metals, chlorpyrifos for pesticides, and benzene for metals. The probability-based sample age and gender demographics compare reasonably well with the Census data (1990 Census and 1996 Census Estimate). The race/ethnicity compared less well with 21% Hispanics in the 1996 Census Estimate and 42% Hispanics in the entire NHEXAS-Arizona sample and 30% Hispanics as Stage III participants for this study. The chemical analyses of the various media (yard soil, foundation soil, house dust, indoor air, outdoor air, drinking water, food, and beverage) show generally low levels of the representative pollutants. The 50th percentiles of the distributions are generally near or below the analytical detection limits, and applicable Federal action limits were rarely exceeded.

Evaluations of primary metals from NHEXAS Arizona: Distributions and preliminary exposures

NHEXAS AZ is a multimedia, multipathway exposure assessment survey designed to evaluate metals and other analytes. This paper reports the analyte-specific concentration distributions in each of the media examined (air, soil, house dust, food, beverage, and water), for various methodologies used (inductively coupled plasma-atomic emission spectroscopy and hydride generation-atomic absorption spectroscopy). Results are reported for the five primary metals (Pb, As, Cd, Cr, and Ni). Ingestion was the most important pathway of exposure. Metal concentrations in air were very low (ng/m3) and found only above the 90th percentile. Metals were commonly found in house dust and soil. Exposure transfer coefficients minimize the importance of this component for those over the age of 6 years. When ranked by exposure, food, beverage, and water appeared to be the primary contributors of metal exposure in NHEXAS AZ. For instance, at the 90th percentile, Pb was undetected in air, found at 131 and 118 µg/m3 in floor dust and soil, respectively, and measured at 16 µg/kg in food, 7.1 µg/kg in beverage, and 2.0 and 1.3 µg/l in drinking and tap water, respectively. We calculated preliminary estimates of total exposure (µg/day) for each participant and examined them independently by age, gender, and ethnicity as reported by the subjects in the NHEXAS questionnaire. At the 90th percentile for Pb, total exposures were 64 µg/day across all subjects (n=176); adult men (n=55) had the greatest exposure (73 µg/day) and children (n=35) the least (37 µg/day). Hispanics (n=54) had greater exposure to Pb (68 µg/day) than non-Hispanics (n=119; 50 µg/day), whereas non-Hispanics had greater exposure for all other metals reported. These results have implications related to environmental justice. The NHEXAS project provides information to make informed decisions for protecting and promoting appropriate public health policy.

Exogenous and endogenous determinants of blood trihalomethane levels after showering.

Background We previously conducted a study to assess whether household exposures to tap water increased an individual’s internal dose of trihalomethanes (THMs). Increases in blood THM levels among subjects who showered or bathed were variable, with increased levels tending to cluster in two groups. Objectives Our goal was to assess the importance of personal characteristics, previous exposures, genetic polymorphisms, and environmental exposures in determining THM concentrations in blood after showering. Methods One hundred study participants completed a health symptom questionnaire, a 48-hr food and water consumption diary, and took a 10-min shower in a controlled setting. We examined THM levels in blood samples collected at baseline and 10 and 30 min after the shower. We assessed the significance of personal characteristics, previous exposures to THMs, and specific gene polymorphisms in predicting postshower blood THM concentrations. Results We did not observe the clustering of blood THM concentrations observed in our earlier study. We found that environmental THM concentrations were important predictors of blood THM concentrations immediately after showering. For example, the chloroform concentration in the shower stall air was the most important predictor of blood chloroform levels 10 min after the shower (p < 0.001). Personal characteristics, previous exposures to THMs, and specific polymorphisms in CYP2D6 and GSTT1 genes were significant predictors of both baseline and postshowering blood THM concentrations as well as of changes in THM concentrations associated with showering. Conclusion The inclusion of information about individual physiologic characteristics and environmental measurements would be valuable in future studies to assess human health effects from exposures to THMs in tap water.

Increases in tobacco exposure biomarkers measured in non-smokers exposed to sidestream cigarette smoke under controlled conditions

National surveys of the exposure of non-smokers to secondhand smoke based on serum cotinine analyses have consistently identified certain groups within the population including children, males and non-Hispanic Blacks as having relatively greater exposure. Although these differences in mean serum cotinine concentrations probably represent differences in exposure of individuals in their daily lives, it is also possible that metabolic or other differences in response might influence the results. To better define the nature of those findings, we have examined the response of 40 non-smokers including both men and women and African-Americans and whites to sidestream (SS) cigarette smoke generated by a smoking machine under controlled conditions. In this study, participants were exposed to aged, diluted SS smoke (ADSS) generated in an environmental chamber with a mean air nicotine concentration of 140 μg m−3 and 8.6 ppm CO for 4 h. Salivary cotinine was measured every 30 min, and serum cotinine samples were taken prior to, and 2 h after exposure. Urinary nicotine metabolites and NNAL, a tobacco-specific nitrosamine, and 4-aminobiphenyl (4-AB) haemoglobin adducts were also measured prior to and 2 h following the exposure. Under these uniform, controlled conditions, we found a similar response to ADSS smoke exposure among all the participants. In all cases a significant increase in biomarker concentration was noted following exposure, and the short-term increases in salivary cotinine concentration were quite similar at approximately 12 pg ml−1 min−1 among the groups. In this small study, no significant differences by gender or race were seen in the mean increases observed in cotinine, NNAL or 4-AB adducts following 4 h of exposure. Thus, our results are most consistent with a relatively uniform response in tobacco biomarker concentrations following short-term exposure to ADSS tobacco smoke, and suggest that biomarker measurements are capable of effectively indicating increases in exposure among groups of non-smokers.