Human exposure to volatile organic compounds: a comparison of organic vapor monitoring badge levels with blood levels

We undertook a study in Albany, New York, to investigate whether volatile organic compounds (VOCs) were measurable in the blood and in the breathing-zone air of people exposed to gasoline fumes and automotive exhaust. We sampled blood of 40 subjects, placed organic vapor badges on 40 subjects, and obtained personal breathing-zone samples from 24 subjects. We limited this analysis to 19 subjects who wore the organic vapor badges for at least 5 h. VOC levels, as determined by the organic vapor badges, were highly correlated with blood levels of these same compounds. Using detection in blood as the gold standard, we found the badges to be more sensitive than conventional charcoal tube samples in detecting low levels of methyl tert-butyl ether (0.60 vs 0.08), toluene (0.95 vs 0.64), and o-xylene (0.85 vs 0.64). In this study, organic vapor badges provided data on VOC exposure that correlated with blood assay results. These organic vapor badges might provide a convenient means of determining human exposure to VOCs in epidemiologic studies.     

Relationships of attached garage and home exposures to fuel type and emission levels of garage sources

Mobile source air toxics (MSAT) may pose an adverse health risk, especially in microenvironments with high exposures to vehicle exhaust or evaporative emissions. Although programs such as reformulated gasoline are intended to reduce the emissions of MSAT and ozone precursors, uncertainties remain regarding population exposures associated with both oxygenate-gasoline blends and conventional gasoline. Measurements were carried out in San Antonio, Texas under controlled conditions to establish relationships between vehicle tailpipe and evaporative emissions and concentration levels in a residence with an attached garage. This paper concentrates on the influence of vehicle type (sedan versus pickup truck), its operational mode (normal versus malfunction), and fuel type (conventional versus oxygenated) on the pollutant levels in the attached garage and adjacent room (kitchen).     

Gasoline vapor exposures at a high volume service station

Gasoline vapor concentrations were measured at a high volume service station for one week in May, 1983, for service station attendants, self-service customers and for various area locations. To facilitate the retention of highly volatile, low-molecular weight gasoline vapor components, 100/50 mg charcoal adsorption tubes were used with flow rates of 100 cc/min for long-term exposure samples and 900 cc/min for short-term exposures. Methylene chloride was selected as the desorption solvent. Desorbed hydrocarbons were analyzed and quantitated by capillary column gas chromatography using a flame ionization detector and a 0-100 degrees C temperature program. The data proved that the predominant ambient air hydrocarbons are those of C4 and C5 compounds. Monitoring results showed that the total gasoline vapor TWA exposures for service station attendants ranged from 0.6 to 4.8 ppm with a geometric mean of 1.5 ppm. Short-term personal samples collected while refueling ranged from not detectable to 38.8 ppm with a geometric mean of 5.8 ppm.     

Exposure to emissions from gasoline within automobile cabins.

Gasoline is emitted from automobiles as uncombusted fuel and via evaporation. Volatile organic compounds (VOC) from gasoline are at higher levels in roadway air than in the surrounding ambient atmosphere and penetrate into automobile cabins, thereby exposing commuters to higher levels than they would experience in other microenvironments. Measurements of VOC concentrations and carbon monoxide were made within automobiles during idling, while driving on a suburban route in New Jersey, and on a commute to New York City. Concentrations of VOC from gasoline were determined to be elevated above the ambient background levels in all microenvironments while VOC without a gasoline source were not. The variability of VOC concentrations with location within the automobile was determined to be smaller than inter-day variability during idling studies. VOC and carbon monoxide levels within the automobile cabin differed among the different routes examined. The levels were related to traffic density and were inversely related to driving speed and wind speed. Overall, daily VOC exposure for gasoline-derived compounds during winter commuting in New Jersey was estimated to range between 5 and 20% and constituted between 15 and 40% of an individual's daily exposure based on comparison to urban and suburban settings, respectively. VOC exposure during commuting in Southern California was estimated to range between 15 and 60%.     

The MTBE air concentrations in the cabin of automobiles while fueling.

Methyl tertiary-butyl ether (MTBE) is the most commonly used oxygenated compound added to gasoline to reduce ambient carbon monoxide levels. Complaints about perceived MTBE exposures and adverse health symptoms have been registered in several states, including New Jersey (NJ). Fueling automobiles is the activity thought to cause the highest environmental MTBE exposures. The current study was conducted to determine the MTBE concentrations inside automobile cabins during fueling, which represents the peak exposure that can occur at full service gasoline service stations, such as those that exist in NJ. Air samples were collected at service stations located on the NJ and PA turnpikes from March 1996 to July 1997 during which the MTBE content in gasoline varied. A bimodal distribution of MTBE concentrations was found in the cabin of the cars while fueling. The median MTBE, benzene and toluene in cabin concentrations were 100, 5.5 and 18 ppb, respectively, with the upper concentrations of the distribution exceeding 1 ppm for MTBE and 0.1 ppm for benzene and toluene. The highest in cabin concentrations occurred in a car that had a malfunctioning vapor recovery system and in a series of cars sampled on an unusually warm, calm winter day when the fuel volatility was high, the evaporation maximal and the dispersion by wind minimal. The in-cabin concentrations were typically higher when the car window was opened during the entire fueling process. Thus, exposure to MTBE during fueling can be reduced by properly maintaining the integrity of the fuel system and keeping the windows closed during fueling.     

Assessing total exposures to gasoline vapor using the source exposure model.

Recent developments in source apportionment modeling of volatile organic compounds (VOCs) include receptor modeling (RM) applications to "total" (indoor and outdoor) exposure assessment for source of VOC. Source fingerprints are available for major VOC sources such as gasoline vapor, automobile exhaust, refinery emissions, cleaning solvent vapors, printing inks, and waste-water treatment facilities. The relative proportion of each VOC species in the source fingerprint enables the RM method, through a least squares analysis, to identify each source's presence and quantify its contribution to ambient air concentrations. Sampling periods and locations may be selected to represent microenvironmental exposures. Receptor modeling has direct applicability to determining the relative contribution of gasoline vapors to VOC exposures in the general population.     

Customer exposure to gasoline vapors during refueling at service stations

Gasoline is a volatile complex mixture of hydrocarbon compounds that is easily vaporized during handling under normal conditions. Modern reformulated gasoline also contains oxygenates to enhance octane number and reduce ambient pollution. This study measured the difference in the exposure of customers to gasoline and oxygenate vapors during refueling in service stations with and without vapor recovery systems. Field measurements were carried out at two self-service stations. One was equipped with Stage I and the other with Stage II vapor recovery systems. At Stage I stations there is vapor recovery only during delivery from road tanker, and at Stage II stations additional vapor recovery during refueling. The exposure of 20 customers was measured at both stations by collecting air samples from their breathing zone into charcoal tubes during refueling with 95-octane reformulated gasoline. Each sample represented two consecutive refuelings. The samples were analyzed in the laboratory by gas chromatography using mass-selective detection for vapor components. The Raid vapor pressure of gasoline was 70 kPa and an oxygen content 2 wt%. Oxygenated gasoline contained 7 percent methyl tert-butyl ether (MtBE) and 5 percent methyl tert-amyl ether (MtAE). The geometric mean concentrations of hydrocarbons (C3-C11) in the customers' breathing zone was 85 mg/m3 (range 2.5-531 mg/m3) at the Stage I service station and 18 mg/m3 (range < 0.2-129 mg/m3) at the Stage II service station. The geometric mean of the exposure of customers to MtBE during refueling at the Stage I service station was 15.3 mg/m3 (range 1.8-74 mg/m3), and at the Stage II service station 3.4 mg/m3 (range 0.2-16 mg/m3). The differences in exposure were statistically significant (p < 0.05). The mean refueling times were 57 seconds (range 23-207) at the Stage I and 66 seconds (range 18-120) at the Stage II station. The measurements were done on consecutive days at the various service stations. The temperature ranged from 10 to 17 degrees C, and wind velocity was 2-4 m/s. The climatic conditions were very similar on the measurement days. Based on this study it was found that the Stage II vapor recovery system reduces gasoline emission considerably. The exposure level of customers at the Stage II station during refueling was circa 20-25 percent of the exposure at the Stage I service station when conditions were equal and no other confounding factors such as leaks or spills were present.     

Personal, indoor, and outdoor VOC exposures in a probability sample of children

As part of the Minnesota Children's Pesticide Exposure Study we measured volatile organic compound (VOC) concentrations in a probability sample of households with children. The 6-day average concentrations for 10 common VOCs were obtained in urban and nonurban residences twice during this multiphase study: screening-phase indoor measurements were collected in 284 households, and in the intensive-phase matched outdoor (O), indoor (I), and personal (P) measurements were collected in a subset (N=72) of the screened households. Screening-phase households with smokers had significantly higher concentrations of benzene and styrene compared to nonsmoking households; households with an attached garage had significantly higher levels of benzene, chloroform, styrene, and m/p- and o-xylene compared to households without an attached garage; and nonurban residences, which had a greater prevalence of smokers and attached garages, had significantly higher 1,1,1-trichloroethane, styrene, and toluene and significantly lower tetrachloroethylene concentrations compared to urban households. The screening-phase weighted distributions estimate the mean and variability in indoor VOC concentrations for more than 45,000 households with children in the census tracts sampled. Overall, median indoor concentrations of most VOCs measured in this study were similar to or lower than indoor levels measured previously in the United States. Intensive-phase outdoor VOC concentrations were generally lower than other major metropolitan areas, but urban concentrations were significantly higher than nonurban concentrations for all compounds except 1,1,1-trichloroethylene. A consistent pattern of P>I>O was observed for nine of 10 VOCs, with 1,1,1-trichloroethylene (I>P>O) being the only exception to this pattern. For most children, the indoor at-home microevironment was strongly associated with personal exposure after controlling for important covariates, but the ratio of median to upper bound exposures was smaller than that observed in studies of adults. There are relatively little data on VOC exposures in children, so these results are useful for estimating the central tendency and distribution of VOC exposures in locations where children spend a majority of their time.     

Toxicokinetics of human exposure to methyl tertiary-butyl ether (MTBE) following short-term controlled exposures.

Methyl tertiary-butyl ether (MTBE) is an oxygenated compound added to gasoline to improve air quality as part of the US Federal Clean Air Act. Due to the increasing and widespread use of MTBE and suspected health effects, a controlled, short-term MTBE inhalation exposure kinetics study was conducted using breath and blood analyses to evaluate the metabolic kinetics of MTBE and its metabolite, tertiary-butyl alcohol (TBA), in the human body. In order to simulate common exposure situations such as gasoline pumping, subjects were exposed to vapors from MTBE in gasoline rather than pure MTBE. Six subjects (three females, three males) were exposed to 1.7 ppm of MTBE generated by vaporizing 15 LV% MTBE gasoline mixture for 15 min. The mean percentage of MTBE absorbed was 65.8 +/- 5.6% following exposures to MTBE. The mean accumulated percentages expired through inhalation for 1 and 8 h after exposure for all subjects were 40.1% and 69.4%, respectively. The three elimination half-lives of the triphasic exponential breath decay curves for the first compartment was 1-4 min, for the second compartment 9-53 min, and for the third compartment 2-8 h. The half-lives data set for the breath second and blood first compartments suggested that the second breath compartment rather than the first breath compartment is associated with a blood compartment. Possible locations for the very short breath half-life observed are in the lungs or mucous membranes. The third compartment calculated for the blood data represent the vessel poor tissues or adipose tissues. A strong correlation between blood MTBE and breath MTBE was found with mean blood-to-breath ratio of 23.5. The peak blood TBA levels occurred after the MTBE peak concentration and reached the highest levels around 2-4 h after exposures. Following the exposures, immediate increases in MTBE urinary excretion rates were observed with lags in the TBA excretion rate. The TBA concentrations reached their highest levels around 6-8 h, and then gradually returned to background levels around 20 h after exposure. Approximately 0.7-1.5% of the inhaled MTBE dose was excreted as unchange urinary MTBE, and 1-3% was excreted as unconjugated urinary TBA within 24 h after exposure.     

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.     

Personal exposure meets risk assessment: a comparison of measured and modeled exposures and risks in an urban community

Human exposure research has consistently shown that, for most volatile organic compounds (VOCs), personal exposures are vastly different from outdoor air concentrations. Therefore, risk estimates based on ambient measurements may over- or underestimate risk, leading to ineffective or inefficient management strategies. In the present study we examine the extent of exposure misclassification and its impact on risk for exposure estimated by the U.S. Environmental Protection Agency (U.S. EPA) Assessment System for Population Exposure Nationwide (ASPEN) model relative to monitoring results from a community-based exposure assessment conducted in Baltimore, Maryland (USA). This study is the first direct comparison of the ASPEN model (as used by the U.S. EPA for the Cumulative Exposure Project and subsequently the National-Scale Air Toxics Assessment) and human exposure data to estimate health risks. A random sampling strategy was used to recruit 33 nonsmoking adult community residents. Passive air sampling badges were used to assess 3-day time-weighted-average personal exposure as well as outdoor and indoor residential concentrations of VOCs for each study participant. In general, personal exposures were greater than indoor VOC concentrations, which were greater than outdoor VOC concentrations. Public health risks due to actual personal exposures were estimated. In comparing measured personal exposures and indoor and outdoor VOC concentrations with ASPEN model estimates for ambient concentrations, our data suggest that ASPEN was reasonably accurate as a surrogate for personal exposures (measured exposures of community residents) for VOCs emitted primarily from mobile sources or VOCs that occur as global "background" source pollutant with no indoor source contributions. Otherwise, the ASPEN model estimates were generally lower than measured personal exposures and the estimated health risks. ASPEN's lower exposures resulted in proportional underestimation of cumulative cancer risk when pollutant exposures were combined to estimate cumulative risk. Median cumulative lifetime cancer risk based on personal exposures was 3-fold greater than estimates based on ASPEN-modeled concentrations. These findings demonstrate the significance of indoor exposure sources and the importance of indoor and/or personal monitoring for accurate assessment of risk. Environmental health policies may not be sufficient in reducing exposures and risks if they are based solely on modeled ambient VOC concentrations. Results from our study underscore the need for a coordinated multimedia approach to exposure assessment for setting public health policy.     

Customer exposure to MTBE, TAME, C6 alkyl methyl ethers, and benzene during gasoline refueling.

We studied customer exposure during refueling by collecting air samples from customers' breathing zone. The measurements were carried out during 4 days in summer 1996 at two Finnish self-service gasoline stations with "stage I" vapor recovery systems. The 95-RON (research octane number) gasoline contained approximately 2.7% methyl tert-butyl ether (MTBE), approximately 8.5% tert-amyl methyl ether (TAME), approximately 3.2% C6 alkyl methyl ethers (C6 AMEs), and 0.75% benzene. The individual exposure concentrations showed a wide log-normal distribution, with low exposures being the most frequent. In over 90% of the samples, the concentration of MTBE was higher (range <0.02-51 mg/m3) than that of TAME. The MTBE values were well below the short-term (15 min) threshold limits set for occupational exposure (250-360 mg/m3). At station A, the geometric mean concentrations in individual samples were 3.9 mg/m3 MTBE and 2. 2 mg/m3 TAME. The corresponding values at station B were 2.4 and 1.7 mg/m3, respectively. The average refueling (sampling) time was 63 sec at station A and 74 sec at station B. No statistically significant difference was observed in customer exposures between the two service stations. The overall geometric means (n = 167) for an adjusted 1-min refueling time were 3.3 mg/m3 MTBE and 1.9 mg/m3 TAME. Each day an integrated breathing zone sample was also collected, corresponding to an arithmetic mean of 20-21 refuelings. The overall arithmetic mean concentrations in the integrated samples (n = 8) were 0.90 mg/m3 for benzene and 0.56 mg/m3 for C6 AMEs calculated as a group. Mean MTBE concentrations in ambient air (a stationary point in the middle of the pump island) were 0.16 mg/m3 for station A and 0.07 mg/m3 for station B. The mean ambient concentrations of TAME, C6 AMEs, and benzene were 0.031 mg/m3, approximately 0.005 mg/m3, and approximately 0.01 mg/m3, respectively, at both stations. The mean wind speed was 1.4 m/sec and mean air temperature was 21 degreesC. Of the gasoline refueled during the study, 75% was 95 grade and 25% was 98/99 grade, with an oxygenate (MTBE) content of 12.2%.     

Individual and population exposures to gasoline.

Gasoline is a complex mixture of many constituents in varying proportions. Not only does the composition of whole gasoline vary from company to company and season to season, but it changes over time. The composition of gasoline vapors is dominated by volatile compounds, while "gasoline" in groundwater consists mainly of water-soluble constituents. Hydrocarbons, including alkanes, alkenes, and aromatics, make up the large majority of gasoline, but other substances, such as alcohols, ethers, and additives, may also be present. Given this inability to define "gasoline,h' exposures to individual chemicals or groups of chemicals must be defined in a meaningful exposure assessment. An estimated 111 million people are currently exposed to gasoline constituents in the course of refueling at self-service gasoline stations. Refueling requires only a few minutes per week, accruing to about 100 min per year. During that time, concentrations in air of total hydrocarbons typically fall in the range 20-200 parts per million by volume (ppmV). Concentrations of the aromatic compounds benzene, toluene, and xylene rarely exceed 1 ppmV. Some liquid gasoline is also released, generally as drops less than 0.1 g each, but with enough larger spills to raise the average loss per gallon dispensed to 0.23 g for stations with conventional nozzles and 0.14 g per refueling for stations with vapor recovery nozzles (Stage II controls). Some skin exposure may occur from these spills but the exposure has not been quantified. Two major types of vehicular emissions have been studied. Evaporative emissions include emissions while the vehicle is driven (running losses), emissions after the engine has been shut off but is still warm (hot soak), and emissions during other standing periods (diurnal) emissions. These evaporative emissions are dominated by the more volatile gasoline components. Tailpipe emissions include some unreacted gasoline constituents as well as products of combustion (including chemicals identical to some of the original constituents of the gasoline) and a variety of hydrocarbons and related compounds. Running losses are reported to fall in the range of 0.2 to 2.8 g of total hydrocarbons per mile driven, while benzene evaporative emissions range from 0.002 to 0.007 g/mile. Benzene levels inside travelling vehicles have been reported to average about 13 ppbV in Los Angeles. Tailpipe emissions amount to 0.3 to 1.0 g/mile of total hydrocarbons; emissions of benzene, polycylic aromatic hydrocarbons, and 1,3-butadiene have been reported to range from 0.015 to 0.04 g/mile, 0.00025 to 0.00046 g/mile, and 0.001 to 0.005 g/mile, respectively.(ABSTRACT TRUNCATED AT 400 WORDS)     

Personal exposure to benzene from fuel emissions among commercial fishers: comparison of two-stroke, four-stroke and diesel engines

Commercial fishers are exposed to unburned hydrocarbon vapors and combustion products present in the emissions from their boat engines. The objective of this study was to measure personal exposure to benzene as a marker of fuel exposure, and to predict exposure levels across categories of carbureted two-stroke, four-stroke and diesel engines. A self-monitoring approach, employing passive monitors, was used to obtain measurements of personal exposure to benzene over time. Mixed-effect linear regression models were used to predict exposure levels, identify significant effects and determine restricted maximum likelihood estimates for within- and between-person variance components. Significant fixed effects for engine type and refueling a car or truck were identified. After controlling for refueling, predicted benzene exposure levels to fishers on boats equipped with two-stroke, four-stroke and diesel engines were 58.4, 38.9 and 15.7 microg/m3, respectively. The logged within-person variance component was 1.43, larger than the between-person variance component of 1.13, indicating that the total variation may be attributable to monitor placement, environmental conditions and other factors that change over time as well as differences between individual work practices. The health consequences of exposure to marine engine emissions are not known. The predicted levels are well below those at which health effects have been attributed, however.     

Outdoor, indoor, and personal exposure to VOCs in children

We measured volatile organic compound (VOC) exposures in multiple locations for a diverse population of children who attended two inner-city schools in Minneapolis, Minnesota. Fifteen common VOCs were measured at four locations: outdoors (O), indoors at school (S), indoors at home (H), and in personal samples (P). Concentrations of most VOCs followed the general pattern O approximately equal to S < P less than or equal to H across the measured microenvironments. The S and O environments had the smallest and H the largest influence on personal exposure to most compounds. A time-weighted model of P exposure using all measured microenvironments and time-activity data provided little additional explanatory power beyond that provided by using the H measurement alone. Although H and P concentrations of most VOCs measured in this study were similar to or lower than levels measured in recent personal monitoring studies of adults and children in the United States, p-dichlorobenzene was the notable exception to this pattern, with upper-bound exposures more than 100 times greater than those found in other studies of children. Median and upper-bound H and P exposures were well above health benchmarks for several compounds, so outdoor measurements likely underestimate long-term health risks from children's exposure to these compounds.     

Relationships among personal, indoor, and outdoor fine and coarse particle concentrations for individuals with COPD

This study characterizes the personal, indoor, and outdoor PM2.5, PM10, and PM2.5-10 exposures of 18 individuals with chronic obstructive pulmonary disease (COPD) living in Boston, MA. Monitoring was performed for each participant for six consecutive days in the winters of 1996 or 1997 and for six to twelve days in the summer of 1996. On each day, 12-h personal, indoor, and outdoor samples of PM2.5 and PM10 were collected simultaneously. Home characteristic information and time-activity patterns were also obtained. Personal exposures were higher than corresponding indoor and outdoor concentrations for all particle measures and for all seasons, except for winter indoor PM2.5-10 levels, which were higher than personal and outdoor levels. Higher personal exposures may be due to the proximity of the individuals to particle sources, such as cooking and cleaning. Indoor concentrations were associated with both outdoor concentrations and personal exposures (as determined by individual least square regression analyses), with associations strongest for PM2.5. Indoor PM2.5 concentrations were significantly associated with outdoor and personal levels for 12 and 15 of the 17 individuals, respectively. Both the strength and magnitude of the associations varied by individual. Also, personal PM2.5, but not PM2.5-10, exposures were associated with outdoor levels, with 10 of the 17 subjects having significant associations. The strength of the personal-outdoor association for PM2.5 was strongly related to that for indoor and outdoor levels, suggesting that home characteristics and indoor particulate sources were key determinants of the personal-outdoor association for PM2.5. Air exchange rates were found to be important determinants of both indoor and personal levels. Again, substantial interpersonal variability in the personal-outdoor relationship was found, as personal exposures varied by as much as 200% for a given outdoor level.     

Variability of environmental exposures to volatile organic compounds

Although studies of occupational exposure to volatile organic compounds (VOCs) often partition variability across groups, and between and within persons, those of environmental exposure to VOCs have not involved such partitioning. Using data from the Environmental Protection Agency's total exposure assessment methodology (TEAM) studies, we partitioned exposure variability across cities, and between and within persons for nine VOCs. The estimated variance components decreased in the order: within-person > between-person > across city. Despite their smaller magnitudes, estimates of between-person and across-city variance components were sufficiently large to provide reasonable contrast for informative epidemiology studies of most VOCs. Estimates of between-person variance components for environmental VOCs were similar to those published for occupational VOCs (groups defined by job and factory). However, estimates of within-person variance components were much greater for environmental VOCs, probably due to the greater diversity of locations (including the workplace) visited by the general public over time. For benzene and perchloroethylene, we used a simple model to calculate numbers of personal measurements required to relate the exposure level to health outcome statistically. About 10 times more personal measurements would be required to investigate perchloroethylene exposure as compared to benzene exposure; this disparity reflects the greater within-subject variability of perchloroethylene data compared to benzene data. We conclude that variability should be partitioned for environmental VOC exposures in much the same manner as for occupational exposures. There should be sufficient variability in the levels of most VOCs across cities and between subjects to provide reasonable contrast for informative epidemiology studies, as we illustrate for exposures to benzene. Yet, epidemiologists should be wary of investigating environmental VOCs without preliminary data with which to estimate the variance structure of exposure variables.     

Determinants of exposure to volatile organic compounds in four Oklahoma cities

To begin to develop generalized models for estimating personal exposure to ambient air pollutants within diverse populations, the design of the Oklahoma Urban Air Toxics Study incorporated eight dichotomous macroenvironmental and household factors that were hypothesized to be potential determinants of exposure. Personal, indoor, and outdoor samples of volatile organic compounds (VOCs) were collected over 24-h monitoring periods in 42 households, together with activity diaries and data on the participants' residences. The distributions of the VOC concentrations were moderately to highly left-censored, and were mostly bimodal. The ATSDR minimal risk level (MRL) was exceeded in a small number of the samples. Personal and indoor concentrations tended to be higher than outdoor concentrations, indicating that indoor exposures were dominated by indoor sources. However, indoor concentrations were not correlated with the permeability of the residence, suggesting that the observed indoor concentrations reflected mostly localized, short-term emissions. The influence of the eight dichotomous factors and of the presence of an attached garage was evaluated using the Wilcoxon rank-sum test and by comparison of "excursion fractions", that is, the fractions of each distributions exceeding 10% of the MRL. Dry weather and absence of children in the household were found to be associated with higher exposures in personal or indoor exposures. Given the small sample size, it is possible that these factors were confounded with unidentified household characteristics or activities that were the true determinants of exposure.     

Environmental and biological monitoring of benzene during self-service automobile refueling

Although automobile refueling represents the major source of benzene exposure among the nonsmoking public, few data are available regarding such exposures and the associated uptake of benzene. We repeatedly measured benzene exposure and uptake (via benzene in exhaled breath) among 39 self-service customers using self-administered monitoring, a technique rarely used to obtain measurements from the general public (130 sets of measurements were obtained). Benzene exposures averaged 2.9 mg/m(3) (SD = 5.8 mg/m(3); median duration = 3 min) with a range of < 0.076-36 mg/m(3), and postexposure breath levels averaged 160 microg/m(3) (SD = 260 microg/m(3)) with a range of < 3.2-1,400 microg/m(3). Log-transformed exposures and breath levels were significantly correlated (r = 0.77, p < 0.0001). We used mixed-effects statistical models to gauge the relative influences of environmental and subject-specific factors on benzene exposure and breath levels and to investigate the importance of various covariates obtained by questionnaire. Model fitting yielded three significant predictors of benzene exposure, namely, fuel octane grade (p = 0.0011), duration of exposure (p = 0.0054), and season of the year (p = 0.032). Likewise, another model yielded three significant predictors of benzene concentration in breath, specifically, benzene exposure (p = 0.0001), preexposure breath concentration (p = 0.0008), and duration of exposure (p = 0.038). Variability in benzene concentrations was remarkable, with 95% of the estimated values falling within a 274-fold range, and was comprised entirely of the within-person component of variance (representing exposures of the same subject at different times of refueling). The corresponding range for benzene concentrations in breath was 41-fold and was comprised primarily of the within-person variance component (74% of the total variance). Our results indicate that environmental rather than interindividual differences are primarily responsible for benzene exposure and uptake during automobile refueling. The study also demonstrates that self-administered monitoring can be efficiently used to measure environmental exposures and biomarkers among the general public.