Assessing the relationship between personal particulate and gaseous exposures of senior citizens living in Baltimore, MD

We conducted a multi-pollutant exposure study in Baltimore, MD, in which 15 non-smoking older adult subjects (> 64 years old) wore a multi-pollutant sampler for 12 days during the summer of 1998 and the winter of 1999. The sampler measured simultaneous 24-hr integrated personal exposures to PM2.5, PM10, SO4(2-), O3, NO2, SO2, and exhaust-related VOCs. Results of this study showed that longitudinal associations between ambient PM2.5 concentrations and corresponding personal exposures tended to be high in the summer (median Spearman's r = 0.74) and low in the winter (median Spearman's r = 0.25). Indoor ventilation was an important determinant of personal PM2.5 exposures and resulting personal-ambient associations. Associations between personal PM2.5 exposures and corresponding ambient concentrations were strongest for well-ventilated indoor environments and decreased with ventilation. This decrease was attributed to the increasing influence of indoor PM2.5 sources. Evidence for this was provided by SO4(2-) measurements, which can be thought of as a tracer for ambient PM2.5. For SO4(2-), personal-ambient associations were strong even in poorly ventilated indoor environments, suggesting that personal exposures to PM2.5 of ambient origin are strongly associated with corresponding ambient concentrations. The results also indicated that the contribution of indoor PM2.5 sources to personal PM2.5 exposures was lowest when individuals spent the majority of their time in well-ventilated indoor environments. Results also indicate that the potential for confounding by PM2.5 co-pollutants is limited, despite significant correlations among ambient pollutant concentrations. In contrast to ambient concentrations, PM2.5 exposures were not significantly correlated with personal exposures to PM2.5-10, PM2.5 of non-ambient origin, O3, NO2, and SO2. Since a confounder must be associated with the exposure of interest, these results provide evidence that the effects observed in the PM2.5 epidemiologic studies are unlikely to be due to confounding by the PM2.5 co-pollutants measured in this study.     

Laboratory and field evaluation of measurement methods for one-hour exposures to O3, PM2.5, and CO.

While researchers have linked acute (less than 12-hr) ambient O3, PM2.5, and CO concentrations to a variety of adverse health effects, few studies have characterized short-term exposures to these air pollutants, in part due to the lack of sensitive, accurate, and precise sampling technologies. In this paper, we present results from the laboratory and field evaluation of several new (or modified) samplers used in the "roll-around" system (RAS), which was developed to measure 1-hr O3, PM2.5, and CO exposures simultaneously. All the field evaluation data were collected during two sampling seasons: the summer of 1998 and the winter of 1999. To measure 1-hr O3 exposures, a new active O3 sampler was developed that uses two nitrite-coated filters to measure O3 concentrations. Laboratory chamber tests found that the active O3 sampler performed extremely well, with a collection efficiency of 0.96 that did not vary with temperature or relative humidity (RH). In field collocation comparisons with a reference UV photometric monitor, the active O3 sampler had an effective collection efficiency ranging between 0.92 and 0.96 and a precision for 1-hr measurements ranging between 4 and 6 parts per billion (ppb). The limits of detection (LOD) of this method were 9 ppb-hr for the chamber tests and approximtely 16 ppb-hr for the field comparison tests. PM2.5 and CO concentrations were measured using modified continuous monitors--the DustTrak and the Langan, respectively. A size-selective inlet and a Nafion dryer were placed upstream of the DustTrak inlet to remove particles with aerodynamic diameters greater than 2.5 microm and to dry particles prior to the measurements, respectively. During the field validation tests, the DustTrak consistently reported higher PM2.5 concentrations than those obtained by the collocated 12-hr PM2.5 PEM samples, by approximately a factor of 2. After the DustTrak response was corrected (correction factor of 2.07 in the summer and 2.02 in the winter), measurements obtained using these methods agreed well with R2 values of 0.87 in the summer and 0.81 in the winter. The results showed that the DustTrak can be used along with integrated measurements to measure the temporal and spatial variation in PM2.5 exposures. Finally, during the field validation tests, CO concentrations measured using the Langan were strongly correlated with those obtained using the reference method when the CO levels were above the LOD of the instrument [approximately 1 part per million (ppm)].     

Assessing the Relationship between Personal Particulate and Gaseous Exposures of Senior Citizens Living in Baltimore,MD

ABSTRACT

We conducted a multi-pollutant exposure study in Baltimore, MD, in which 15 non-smoking older adult subjects (>64 years old) wore a multi-pollutant sampler for 12 days during the summer of 1998 and the winter of 1999. The sampler measured simultaneous 24-hr integrated personal exposures to PM₂₅, PM₁₀, SO₄ ^2-, O₃, NO₂, SO₂, and exhaust-related VOCs.

Results of this study showed that longitudinal associations between ambient PM_2.5 concentrations and corresponding personal exposures tended to be high in the summer (median Spearman's r = 0.74) and low in the winter (median Spearman's r = 0.25). Indoor ventilation was an important determinant of personal PM_2.5 exposures and resulting personal-ambient associations. Associations between personal PM₂₅ exposures and corresponding ambient concentrations were strongest for well-ventilated indoor environments and decreased with ventilation. This decrease was attributed to the increasing influence of indoor PM_{2 5} sources. Evidence for this was provided by SO₄ ^2-measurements, which can be thought of as a tracer for ambient PM₂₅. For SO₄ ^2-, personal-ambient associations were strong even in poorly ventilated indoor environments, suggesting that personal exposures to PM_2.5 of ambient origin are strongly associated with corresponding ambient concentrations. The results also indicated that the contribution of indoor PM_2.5 sources to personal PM_2.5 exposures was lowest when individuals spent the majority of their time in well-ventilated indoor environments.

Results also indicate that the potential for confounding by PM_2.5 co-pollutants is limited, despite significant correlations among ambient pollutant concentrations. In contrast to ambient concentrations, PM_2.5 exposures were not significantly correlated with personal exposures to PM_2.5-10, PM_2.5 of non-ambient origin, O₃, NO₂, and SO₂. Since a confounder must be associated with the exposure of interest, these results provide evidence that the effects observed in the PM_2.5 epidemiologic studies are unlikely to be due to confounding by the PM_2.5 co-pollutants measured in this study.     

Estimated hourly personal exposures to ambient and nonambient particulate matter among sensitive populations in Seattle, Washington

Epidemiological studies of particulate matter (PM) routinely use concentrations measured with stationary outdoor monitors as surrogates for personal exposure. Despite the frequently reported poor correlations between ambient concentrations and total personal exposure, the epidemiologic associations between ambient concentrations and health effects depend on the correlation between ambient concentrations and personal exposure to ambient-generated PM. This paper separates personal PM exposure into ambient and nonambient components and estimates the outdoor contribution to personal PM exposures with continuous light scattering data collected from 38 subjects in Seattle, WA. Across all subjects, the average exposure encountered indoors at home was lower than in all other microenvironments. Cooking and being at school were associated with elevated levels of exposure. Previously published estimates of particle infiltration (Finf) were combined with time-location data to estimate an ambient contribution fraction (alpha, mean = 0.66+/-0.21) for each subject. The mean alpha was significantly lower for subjects monitored during the heating season (0.55+/-0.16) than for those monitored during the nonheating season (0.80+/-0.17). Our modeled alpha estimates agreed well with those estimated with the sulfur-tracer method (slope = 1.08; R2 = 0.67). We modeled exposure to ambient and nonambient PM with both continuous light scattering and 24-hr gravimetric data and found good agreement between the two methods. On average, ambient particles accounted for 48% of total personal exposure (range = 21-80%). The personal activity exposure was highly influenced by time spent away from monitored microenvironments. The median hourly longitudinal correlation between central site concentrations and personal exposures was 0.30. Although both alpha and the nonambient sources influence the personal-central relationship, the latter seems to dominate. Thus, total personal exposure may be poorly predicted by stationary outdoor monitors, particularly among persons whose PM exposure is dominated by nonambient exposures, for example, those living in tightly sealed homes, those who cook, and children.     

Exposure of chronic obstructive pulmonary disease patients to particulate matter: relationships between personal and ambient air concentrations

Mot time-series studies of particulate air pollution and acute health outcomes assess exposure of the study population using fixed-site outdoor measurements. To address the issue of exposure misclassification, we evaluate the relationship between ambient particle concentrations and personal exposures of a population expected to be at risk of particle health effects. Sampling was conducted within the Vancouver metropolitan area during April-September 1998. Sixteen subjects (non-smoking, ages 54-86) with physician-diagnosed chronic obstructive pulmonary disease (COPD) wore personal PM2.5 monitors for seven 24-hr periods, randomly spaced approximately 1.5 weeks apart. Time-activity logs and dwelling characteristics data were also obtained for each subject. Daily 24-hr ambient PM10 and PM2.5 concentrations were measured at five fixed sites spaced throughout the study region. SO4(2-), which is found almost exclusively in the fine particle fraction and which does not have major indoor sources, was measured in all PM2.5 samples as an indicator of accumulation mode particulate matter of ambient origin. The mean personal and ambient PM2.5 concentrations were 18 micrograms/m3 and 11 micrograms/m3, respectively. In analyses relating personal and ambient measurements, ambient concentrations were expressed either as an average of the values obtained from five ambient monitoring sites for each day of personal sampling, or as the concentration obtained at the ambient site closest to each subject's home. The mean personal to ambient concentration ratio of all samples was 1.75 (range = 0.24 to 10.60) for PM2.5, and 0.75 (range = 0.09 to 1.42) for SO4(2-). Regression analyses were conducted for each subject separately and on pooled data. The median correlation (Pearson's r) between personal and average ambient PM2.5 concentrations was 0.48 (range = -0.68 to 0.83). Using SO4(2-) as the exposure metric, the median r between personal and average ambient concentrations was 0.96 (range = 0.66 to 1.0). Use of the closest ambient site did not improve the median correlation of the group for either PM2.5 or SO4(2-). All pooled analyses resulted in lower correlation coefficients than the median correlation coefficient of individual regressions. Personal SO4(2-) was more highly correlated with all ambient measures than PM2.5. Inclusion of time-activity and dwelling characteristics data did not result in a useful predictive regression model for PM2.5 personal exposure, but improved the model fit from simply regressing against ambient concentration (R2 = 0.27). The model for SO4(2-) was predictive (R2 = 0.82), as personal exposures were largely explained by ambient levels. These results indicate a relatively low correlation between personal exposure and ambient PM2.5 that is not improved by assigning exposure to the closest ambient monitor. The correlation between personal exposure and ambient concentration is high, however, when using SO4(2-), an indicator of accumulation mode particulate matter of ambient origin.     

The Steubenville Comprehensive Air Monitoring Program (SCAMP): analysis of short-term and episodic variations in PM2.5 concentrations using hourly air monitoring data

One-hour average ambient concentrations of particulate matter (PM) with an aerodynamic diameter < 2.5 microm (PM2.5) were determined in Steubenville, OH, between June 2000 and May 2002 with a tapered element oscillating microbalance (TEOM). Hourly average gaseous copollutant [carbon monoxide (CO), sulfur dioxide (SO2), nitrogen oxide (NOx), and ozone (O3)] concentrations and meteorological conditions also were measured. Although 75% of the 14,682 hourly PM2.5 concentrations measured during this period were < or = 17 microg/m3, concentrations > 65 microg/m3 were observed 76 times. On average, PM2.5 concentrations at Steubenville exhibited a diurnal pattern of higher early morning concentrations and lower afternoon concentrations, similar to the diurnal profiles of CO and NO(x). This pattern was highly variable; however, PM2.5 concentrations > 65 microg/m3 were never observed during the mid-afternoon between 1:00 p.m. and 5:00 p.m. EST. Twenty-two episodes centered on one or more of these elevated concentrations were identified. Five episodes occurred during the months June through August; the maximum PM2.5 concentration during these episodes was 76.6 microg/m3. Episodes occurring during climatologically cooler months often featured higher peak concentrations (five had maximum concentrations between 95.0 and 139.6 microg/m3), and many exhibited strong covariation between PM2.5 and CO, NO(x), or SO2. Case studies suggested that nocturnal surface-based temperature inversions were influential in driving high nighttime concentrations of these species during several cool season episodes, which typically had dramatically lower afternoon concentrations. These findings provide insights that may be useful in the development of PM2.5 reduction strategies for Steubenville, and suggest that studies assessing possible health effects of PM2.5 should carefully consider exposure issues related to the intraday timing of PM2.5 episodes, as well as the potential for toxicological interactions among PM2.5, and primary gaseous pollutants.     

The 1999 Fresno particulate matter exposure studies: comparison of community, outdoor, and residential PM mass measurements

Two collaborative studies have been conducted by the U.S. Environmental Protection Agency (EPA) National Exposure Research Laboratory (NERL) and National Health and Environmental Effects Research Laboratory to determine personal exposures and physiological responses to particulate matter (PM) of elderly persons living in a retirement facility in Fresno, CA. Measurements of PM and other criteria air pollutants were made inside selected individual residences within the retirement facility and at a central outdoor site on the premises. In addition, personal PM exposure monitoring was conducted for a subset of the participants, and ambient PM monitoring data were available for comparison from the NERL PM research monitoring platform in central Fresno. Both a winter (February 1-28, 1999) and a spring (April 19-May 16, 1999) study were completed so that seasonal effects could be evaluated. During the spring study, a more robust personal exposure component was added, as well as a more detailed evaluation of physical factors, such as air-exchange rate, that are known to influence the penetration of particles into the indoor environment. In this paper, comparisons are made among measured personal PM exposures and PM mass concentrations measured at the NERL Fresno Platform site, outside on the premises of the retirement facility, and inside selected residential apartments at the facility during the two 28-day study periods. The arithmetic daily mean personal PM2.5 exposure during the winter study period was 13.3 micrograms/m3, compared with 9.7, 20.5, and 21.7 micrograms/m3 for daily mean overall apartment, outdoor, and ambient (i.e., platform) concentrations, respectively. The daily mean personal PM2.5 exposure during the spring study period was 11.1 micrograms/m3, compared with 8.0, 10.1, and 8.6 micrograms/m3 for the daily mean apartment, outdoor, and ambient concentrations, respectively.     

The Steubenville comprehensive air monitoring program (SCAMP): associations among fine particulate matter, co-pollutants, and meteorological conditions

We determined 24-hr average ambient concentrations of PM2.5 and its ionic and carbonaceous components in Steubenville, OH, between May 2000 and May 2002. We also determined daily average gaseous co-pollutant concentrations, meteorological conditions, and pollen and mold spore counts. Data were analyzed graphically and by linear regression and time series models. Multiple-day episodes of elevated fine particulate matter (PM2.5) concentrations often occurred during periods of locally high temperature (especially during summer), high pressure, or low wind speed (especially during winter) and generally ended with the passage of a frontal system. After removing autocorrelation, we observed statistically significant positive associations between concentrations of PM2.5 and concentrations of CO, NOx, and SO2. Associations with NOx and CO exhibited significant seasonal dependencies, with the strongest correlations during fall and winter. NOx, CO, SO2, O3, temperature, relative humidity, and wind speed were all significant predictors of PM2.5 concentration in a time-series model with external regressors, which successfully accounted for 79% of the variance in log-transformed daily PM2.5 concentrations. Coefficient estimates for NOx and temperature varied significantly by season. The results provide insight that may be useful in the development of future PM2.5 reduction strategies for Steubenville. Additionally, they demonstrate the need for PM epidemiology studies in Steubenville (and elsewhere) to carefully consider the potential confounding effects of gaseous co-pollutants, such as CO and NOx, and their seasonally dependent associations with PM2.5.     

Personal exposure to fine particulate matter in elderly subjects: relation between personal, indoor, and outdoor concentrations

The time-series correlation between ambient levels, indoor levels, and personal exposure to PM2.5 was assessed in panels of elderly subjects with cardiovascular disease in Amsterdam, the Netherlands, and Helsinki, Finland. Subjects were followed for 6 months with biweekly clinical visits. Each subject's indoor and personal exposure to PM2.5 was measured biweekly, during the 24-hr period preceding the clinical visits. Outdoor PM2.5 concentrations were measured at fixed sites. The absorption coefficients of all PM2.5 filters were measured as a marker for elemental carbon (EC). Regression analyses were conducted for each subject separately, and the distribution of the individual regression and correlation coefficients was investigated. Personal, indoor, and ambient concentrations were highly correlated within subjects over time. Median Pearson's R between personal and outdoor PM2.5 was 0.79 in Amsterdam and 0.76 in Helsinki. For absorption, these values were 0.93 and 0.81 for Amsterdam and Helsinki, respectively. The findings of this study provide further support for using fixed-site measurements as a measure of exposure to PM2.5 in epidemiological time-series studies.     

Personal exposure levels and microenvironmental concentrations of formaldehyde and acetaldehyde in the Helsinki metropolitan area, Finland

Personal 48-hr exposures to formaldehyde and acetaldehyde of 15 randomly selected participants were measured during the summer/autumn of 1997 using Sep-Pak DNPH-Silica cartridges as a part of the EXPOLIS study in Helsinki, Finland. In addition to personal exposures, simultaneous measurements of microenvironmental concentrations were conducted at each participant's residence (indoor and outdoor) and workplace. Mean personal exposure levels were 21.4 ppb for formaldehyde and 7.9 ppb for acetaldehyde. Personal exposures were systematically lower than indoor residential concentrations for both compounds, and ambient air concentrations were lower than both indoor residential concentrations and personal exposure levels. Mean workplace concentrations of both compounds were lower than mean indoor residential concentrations. Correlation between personal exposures and indoor residential concentrations was statistically significant for both compounds. This indicated that indoor residential concentrations of formaldehyde and acetaldehyde are a better estimate of personal exposures than are concentrations in ambient air. In addition, a time-weighted exposure model did not improve the estimation of personal exposures above that obtained using indoor residential concentrations as a surrogate for personal exposures. Correlation between formaldehyde and acetaldehyde was statistically significant in outdoor microenvironments, suggesting that both compounds have similar sources and sinks in ambient urban air.     

A study of the association between daily mortality and ambient air pollutant concentrations in Pittsburgh, Pennsylvania

We have studied the possible association of daily mortality with ambient pollutant concentrations (PM10, CO, O3, SO2, NO2, and fine [PM2.5] and coarse PM) and weather variables (temperature and dew point) in the Pittsburgh, PA, area for two age groups--less than 75, and 75 and over--for the 3-year period of 1989-1991. Correlation functions among pollutant concentrations show important seasonal dependence, and this fact necessitates the use of seasonal models to better identify the link between ambient pollutant concentrations and daily mortality. An analysis of the seasonal model results for the younger-age group reveals significant multicollinearity problems among the highly correlated concentrations of PM10, CO, and NO2 (and O3 in spring and summer), and calls into question the rather consistent results of the single- and multi-pollutant non-seasonal models that show a significant positive association between PM10 and daily mortality. For the older-age group, dew point consistently shows a significant association with daily mortality in all models. Collinearity problems appear in the multi-pollutant seasonal and non-seasonal models such that a significant, positive PM10 coefficient is accompanied by a significant, negative coefficient of another ambient pollutant, and the identity of this other pollutant changes with season. The PM2.5 data set is half that of PM10. Identical-model runs for both data sets reveal instability in the pollutant coefficients, especially for the younger age group. The concern for the instability of the pollutant coefficients due to a small signal-to-noise ratio makes it impossible to ascertain credibly the relative associations of the fine- and coarse-particle modes with daily mortality. In this connection, we call for caution in the interpretation of model results for causal inference when the models use fully or partially estimated PM values to fill large data gaps.     

Personal exposures to particles and their relationships with personal activities for chronic obstructive pulmonary disease patients living in Boston

An exposure study of 18 subjects with chronic obstructive pulmonary disease (COPD) living in the Boston, MA, area was conducted. The objective was to examine determinants of personal exposures to particulate matter (PM) with aerodynamic diameters of less than 2.5 microm (PM2.5), less than 10 microm (PM10), and between 2.5 and 10 microm (PM2.5-10). In a previous publication, the analyses of the longitudinal individual-specific relationships among indoor, outdoor, and personal levels showed that the relationships varied by subject and by particle size fraction. In the present paper, statistical and physical models were used to examine personal PM2.5, PM10, and PM2.5-10 exposure covariates. Results indicated that time-weighted indoor concentrations were significant predictors of personal PM2.5, PM10, and PM2.5-10 exposures. Also, time-weighted outdoor concentrations, time spent near smokers, and time spent during transportation were important predictors for PM2.5 but not for personal PM2.5-10 exposures. In turn, time spent cleaning contributed to all size-fraction personal exposures, whereas cooking affected only personal PM2.5-10 exposures. The findings showed that the relationship between personal PM2.5 exposures and the corresponding ambient concentrations was influenced by home air exchange rates (or by ventilation status). Because the particle properties or components causing the health effects are unknown, it is not certain to what extent the risk posed by ambient particles can be reduced by controlling any one of these factors.     

Roadside particulate air pollution in Bangkok

Airborne fine particles of PM(2.5-10) and PM2.5 in Bangkok, Nonthaburi, and Ayutthaya were measured from December 22, 1998, to March 26, 1999, and from November 30, 1999, to December 2, 1999. Almost all the PM10 values in the high-polluted (H) area exceeded the Thailand National Ambient Air Quality Standards (NAAQS) of 120 microg/m3. The low-polluted (L) area showed low PM10 (34-74 microg/m3 in the daytime and 54-89 microg/m3 at night). PM2.5 in the H area varied between 82 and 143 microg/m3 in the daytime and between 45 and 146 microg/m3 at night. In the L area, PM2.5 was quite low both day and night and varied between 24 and 54 microg/m3, lower than the U.S. Environmental Protection Agency (EPA) standard (65 microg/m3). The personal exposure results showed a significantly higher proportion of PM2.5 to PM10 in the H area than in the L area (H = 0.80 +/- 0.08 and L = 0.65 +/- 0.04). Roadside PM10 was measured simultaneously with the Thailand Pollution Control Department (PCD) monitoring station at the same site and at the intersections where police work. The result from dual simultaneous measurements of PM10 showed a good correlation (correlation coefficient: r = 0.93); however, PM levels near the roadside at the intersections were higher than the concentrations at the monitoring station. The relationship between ambient PM level and actual personal exposures was examined. Correlation coefficients between the general ambient outdoors and personal exposure levels were 0.92 for both PM2.5 and PM10. Bangkok air quality data for 1997-2000, including 24-hr average PM10, NO2, SO2, and O3 from eight PCD monitoring stations, were analyzed and validated. The annual arithmetic mean PM10 of the PCD data at the roadside monitoring stations for the last 3 years decreased from 130 to 73 microg/m3, whereas the corresponding levels at the general monitoring stations decreased from 90 to 49 microg/m3. The proportion of days when the level of the 24-hr average PM10 exceeded the NAAQS was between 13 and 26% at roadside stations. PCD data showed PM10 was well correlated with NO2 but not with SO2, suggesting that automobile exhaust is the main source of the particulate air pollution. The results obtained from the simultaneous measurement of PM2.5 and PM10 indicate the potential environmental health hazard of fine particles. In conclusion, Bangkok traffic police were exposed to high levels of automobile-derived particulate air pollution.     

Predicting particulate (PM10) personal exposure distributions using a random component superposition statistical model

This paper presents a new statistical model designed to extend our understanding from prior personal exposure field measurements of urban populations to other cities where ambient monitoring data, but no personal exposure measurements, exist. The model partitions personal exposure into two distinct components: ambient concentration and nonambient concentration. It is assumed the ambient and nonambient concentration components are uncorrelated and add together; therefore, the model is called a random component superposition (RCS) model. The 24-hr ambient outdoor concentration is multiplied by a dimensionless "attenuation factor" between 0 and 1 to account for deposition of particles as the ambient air infiltrates indoors. The RCS model is applied to field PM10 measurement data from three large-scale personal exposure field studies: THEES (Total Human Environmental Exposure Study) in Phillipsburg, NJ; PTEAM (Particle Total Exposure Assessment Methodology) in Riverside, CA; and the Ethyl Corporation study in Toronto, Canada. Because indoor sources and activities (smoking, cooking, cleaning, the personal cloud, etc.) may be similar in similar populations, it was hypothesized that the statistical distribution of nonambient personal exposure is invariant across cities. Using a fixed 24-hr attenuation factor as a first approximation derived from regression analysis for the respondents, the distributions of nonambient PM10 personal exposures were obtained for each city. Although the mean ambient PM10 concentrations in the three cities varied from 27.9 micrograms/m3 in Toronto to 60.9 micrograms/m3 in Phillipsburg to 94.1 micrograms/m3 in Riverside, the mean nonambient components of personal exposures were found to be closer: 52.6 micrograms/m3 in Toronto; 52.4 micrograms/m3 in Phillipsburg; and 59.2 micrograms/m3 in Riverside. The three frequency distributions of the nonambient components of exposure also were similar in shape, giving support to the hypothesis that nonambient concentrations are similar across different cities and populations. These results indicate that, if the ambient concentrations were completely controlled and set to zero in all three cities, the median of the remaining personal exposures to PM10 would range from 32.0 micrograms/m3 (Toronto) to 34.4 micrograms/m3 (Phillipsburg) to 48.8 micrograms/m3 (Riverside). The highest-exposed 30% of the population in the three cities would still be exposed to 24-hr average PM10 concentrations of 47-74 micrograms/m3; the highest 20% would be exposed to concentrations of 56-92 micrograms/m3; the highest 10% to concentrations of 88-131 micrograms/m3; and the highest 5% to 133-175 micrograms/m3, due only to indoor sources and activities. The distribution for the difference between personal exposures and indoor concentrations, or the "personal cloud," also was similar in the three cities, with a mean of 30-35 micrograms/m3, suggesting that the personal cloud accounts for more than half of the nonambient component of PM10 personal exposure in the three cities. Using only the ambient measurements in Toronto, the nonambient data from THEES in Phillipsburg was used to predict the entire personal exposure distribution in Toronto. The PM10 exposure distribution predicted by the model showed reasonable agreement with the PM10 personal exposure distribution measured in Toronto. These initial results suggest that the RCS model may be a powerful tool for predicting personal exposure distributions and statistics in other cities where only ambient particle data are available.     

Validity of ambient levels of fine particles as surrogate for personal exposure to outdoor air pollution--results of the European EXPOLIS-EAS Study (Swiss Center Basel)

To evaluate the validity of fixed-site fine particle levels as exposure surrogates in air pollution epidemiology, we considered four indicator groups: (1) PM2.5 total mass concentrations, (2) sulfur and potassium for regional air pollution, (3) lead and bromine for traffic-related particles, and (4) calcium for crustal particles. Using data from the European EXPOLIS (Air Pollution Exposure Distribution within Adult Urban Populations in Europe) study, we assessed the associations between 48-hr personal exposures and home outdoor levels of the indicators. Furthermore, within-city variability of fine particle levels was evaluated. Personal exposures to PM2.5 mass were not correlated to corresponding home outdoor levels (n = 44, rSpearman (Sp) = 0.07). In the group reporting neither relevant indoor sources nor relevant activities, personal exposures and home outdoor levels of sulfur were highly correlated (n = 40, rSp = 0.85). In contrast, the associations were weaker for traffic (Pb: n = 44, rSp = 0.53; Br: n = 44, rSp = 0.21) and crustal (Ca: n = 44, rSp = 0.12) indicators. This contrast is consistent with spatially homogeneous regional pollution and higher spatial variability of traffic and crustal indicators observed in Basel, Switzerland. We conclude that for regional air pollution, fixed-site fine particle levels are valid exposure surrogates. For source-specific exposures, however, fixed-site data are probably not the optimal measure. Still, in air pollution epidemiology, ambient PM2.5 levels may be more appropriate exposure estimates than total personal PM2.5 exposure, since the latter reflects a mixture of indoor and outdoor sources.     

Laboratory and Field Evaluation of Measurement Methods for One-Hour Exposures to O3, PM25, and CO

ABSTRACT

While researchers have linked acute (less than 12-hr) ambient O₃, PM₂₅, and CO concentrations to a variety of adverse health effects, few studies have characterized short-term exposures to these air pollutants, in part due to the lack of sensitive, accurate, and precise sampling technologies. In this paper, we present results from the laboratory and field evaluation of several new (or modified) samplers used in the “roll-around” system (RAS), which was developed to measure 1-hr O₃, PM₂₅, and CO exposures simultaneously. All the field evaluation data were collected during two sampling seasons: the summer of 1998 and the winter of 1999.

To measure 1-hr O₃ exposures, a new active O₃ sampler was developed that uses two nitrite-coated filters to measure O₃ concentrations. Laboratory chamber tests found that the active O₃ sampler performed extremely well, with a collection efficiency of 0.96 that did not vary with temperature or relative humidity (RH). In field collocation comparisons with a reference UV photometric monitor, the active O₃ sampler had an effective collection efficiency ranging between 0.92 and 0.96 and a precision for 1-hr measurements ranging between 4 and 6 parts per billion (ppb). The limits of detection (LOD) of this method were 9 ppb-hr for the chamber tests and ~16 ppb-hr for the field comparison tests.

PM_2.5 and CO concentrations were measured using modified continuous monitors—the DustTrak and the Langan, respectively. A size-selective inlet and a Nafion dryer were placed upstream of the DustTrak inlet to remove particles with aerodynamic diameters greater than 2.5 um and to dry particles prior to the measurements, respectively. During the field validation tests, the DustTrak consistently reported higher PM_2.5 concentrations than those obtained by the collocated 12-hr PM_{2 5} PEM samples, by approximately a factor of 2. After the DustTrak response was corrected (correction factor of 2.07 in the summer and 2.02 in the winter), measurements obtained using these methods agreed well with R² values of 0.87 in the summer and 0.81 in the winter. The results showed that the DustTrak can be used along with integrated measurements to measure the temporal and spatial variation in PM_{2 5} exposures. Finally, during the field validation tests, CO concentrations measured using the Langan were strongly correlated with those obtained using the reference method when the CO levels were above the LOD of the instrument [~1 part per million (ppm)].     

Use of a continuous nephelometer to measure personal exposure to particles during the U.S. Environmental Protection Agency Baltimore and Fresno Panel studies

In population exposure studies, personal exposure to PM is typically measured as a 12- to 24-hr integrated mass concentration. To better understand short-term variation in personal PM exposure, continuous (1-min averaging time) nephelometers were worn by 15 participants as part of two U.S. Environmental Protection Agency (EPA) longitudinal PM exposure studies conducted in Baltimore County, MD, and Fresno, CA. Participants also wore inertial impactor samplers (24-hr integrated filter samples) and recorded their daily activities in 15-min intervals. In Baltimore, the nephelometers correlated well (R2 = 0.66) with the PM2.5 impactors. Time-series plots of personal nephelometer data showed each participant's PM exposure to consist of a series of peaks of relatively short duration. Activities corresponding to a significant instrument response included cooking, outdoor activities, transportation, laundry, cleaning, shopping, gardening, moving between microenvironments, and removing/putting on the instrument. On average, 63-66% of the daily PM exposure occurred indoors at home (about 2/3 of which occurred during waking hours), primarily due to the large amount of time spent in that location (an average of 72-77%). Although not a reference method for measuring mass concentration, the nephelometer did help identify PM sources and the relative contribution of those sources to an individual's personal exposure.     

Concentrations of mobile source air pollutants in urban microenvironments

Human exposures to criteria and hazardous air pollutants (HAPs) in urban areas vary greatly due to temporal-spatial variations in emissions, changing meteorology, varying proximity to sources, as well as due to building, vehicle, and other environmental characteristics that influence the amounts of ambient pollutants that penetrate or infiltrate into these microenvironments. Consequently, the exposure estimates derived from central-site ambient measurements are uncertain and tend to underestimate actual exposures. The Exposure Classification Project (ECP) was conducted to measure pollutant concentrations for common urban microenvironments (MEs) for use in evaluating the results of regulatory human exposure models. Nearly 500 sets of measurements were made in three Los Angeles County communities during fall 2008, winter 2009, and summer 2009. MEs included in-vehicle, near-road, outdoor, and indoor locations accessible to the general public. Contemporaneous 1- to 15-min average personal breathing zone concentrations of carbon monoxide (CO), carbon dioxide (CO₂), volatile organic compounds (VOCs), nitric oxide (NO), nitrogen oxides (NO_x), particulate matter (<2.5 μm diameter; PM_2.5) mass, ultrafine particle (UFP; <100 nm diameter) number, black carbon (BC), speciated HAPs (e.g., benzene, toluene, ethylbenzene, xylenes [BTEX], 1,3-butadiene), and ozone (O₃) were measured continuously. In-vehicle and inside/outside measurements were made in various passenger vehicle types and in public buildings to estimate penetration or infiltration factors. A large fraction of the observed pollutant concentrations for on-road MEs, especially near diesel trucks, was unrelated to ambient measurements at nearby monitors. Comparisons of ME concentrations estimated using the median ME/ambient ratio versus regression slopes and intercepts indicate that the regression approach may be more accurate for on-road MEs. Ranges in the ME/ambient ratios among ME categories were generally greater than differences among the three communities for the same ME category, suggesting that the ME proximity factors may be more broadly applicable to urban MEs.

Implications:Estimates of population exposure to air pollutants extrapolated from ambient measurements at ambient fixed site monitors or exposure surrogates are prone to uncertainty. This study measured concentrations of mobile source air toxics (MSAT) and related criteria pollutants within in-vehicle, outdoor near-road, and indoor urban MEs to provide multipollutant ME measurements that can be used to calibrate regulatory exposure models.     

Subgroups exposed to systematically different elemental compositions of PM2.5

Identification of exposure subgroups is important for both health-based assessments where health effects are linked to the elemental composition of PM_2.5 mixture to which participants are exposed, and for development of population exposure models where population exposures to PM_2.5 mass are modeled generally using fixed site ambient monitoring. Here we demonstrate that workplace sources dominate PM_2.5 mass in the upper end of the distribution for EXPOLIS participants in Athens, Basel, Helsinki and Oxford, resulting in poor performance of models that use ambient concentrations to predict exposures when predicting higher exposures, where adverse health impacts would be more likely. Further, since different microenvironments reflect differing contributions from local PM_2.5 sources, personal PM_2.5 exposures for participants whose exposures are dominated by different microenvironments show systematically different elemental personal compositions. Perhaps a more significant complication for epidemiologic associations is that the proportion of participants whose exposures are dominated by each microenvironment varies across the exposure distribution to PM_2.5. Participants exposed predominantly in the outdoor or personal microenvironments are a greater fraction of the lower end of the PM_2.5 exposure distribution while participants with dominant workplace environments are a greater fraction of the upper end of the distribution, with corresponding differences in elemental compositions of PM_2.5 exposures across the exposure distribution.