Abstract
To provide additional insight into factors affecting exposure to airborne particulate matter and the resultant health effects, we developed a method to estimate the ambient and nonambient components of total personal exposure. The ambient (or outdoor) component of total personal exposure to particulate matter (PM) (called ambient exposure) includes exposure to the ambient PM concentration while outdoors and exposure while indoors to ambient PM that has infiltrated indoors. The nonambient component of total personal exposure to PM (called nonambient exposure) refers to exposure to PM generated by indoor sources and an individual's personal activity. We used data collected from a personal monitoring study in Vancouver, Canada to demonstrate the methodology. In this study, ambient PM2.5 exposure was 71% of the measured ambient PM2.5 concentration and was responsible for 44% of the measured total personal PM2.5 exposure. Regression analysis of the pooled data sets for ambient and total exposure against outdoor concentrations yielded similar slopes (0.76 for ambient and 0.77 for total) but a higher coefficient of determination for ambient exposure (R2=0.62) than for total exposure (R2=0.072). As expected, the nonambient exposure was not related to the ambient concentration (R2<10−6). For longitudinal analyses of the relationship between measured personal exposure and ambient concentrations for individual subjects, the correlation of total personal exposure with ambient concentration yielded values of Pearson's r from 0.83 to −0.68 with an average of 0.36. The relationship was statistically significant for only five of the 16 subjects. In contrast, the correlation of the estimated ambient exposure with ambient concentration yielded values of Pearson's r from 0.92 to 0.77 with an average of 0.88; 14 were significant. An example, taken from an epidemiologic analysis using the exposure data from this paper, demonstrates the usefulness of separating total exposure into its ambient and nonambient components.
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Acknowledgements
The collection of the data that are analyzed in this manuscript was supported in part by a research grant from the British Columbia Lung Association and by an Infrastructure Program (Center for Health and Environment Research) award from the Michael Smith Foundation for Health Research. Portions of this work were first reported at the Annual Conference of the International Society of Exposure Assessment, Charleston, SC, November 4–8, 2001 (Wilson and Brauer, 2001).
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This paper has been reviewed in accordance with U.S. Environmental Protection Agency policy and approved for publication. However, the views expressed are those of the authors and do not necessarily reflect the views or policies of the Environmental Protection Agency. Mention of trade names or commercial products does not constitute endorsement or recommendation for use.
Appendices
Appendix A1. Summary of notation, symbols, definitions, and equations
Exposure and Concentration Variables
- T :
-
total personal exposure as measured by a monitor worn by an individual
- N :
-
nonambient exposure, that is, the component of total exposure due to indoor sources, while indoors, plus “personal cloud” or personal-activity sources, while indoors or outdoors
- A :
-
ambient exposure, that is, exposure to ambient particles, while outdoors, plus exposure, while indoors, to particles that have infiltrated from outdoors to indoors
- C :
-
ambient concentration, as measured at a community monitoring site or the average of several community monitoring sites
- C ai :
-
concentration of ambient PM infiltrated indoors from outdoors
- C in :
-
concentration of PM in indoor air
- F INF :
-
Cai/C=pa/(a+k)=infiltration factor
- α :
-
A/C=y+(1-y) {pa/(a+k)}=attenuation factor
Mass Balance Equation and Derived Equations
Parameters Used in the Mass Balance Equation
Superscripts used to identify size fractions or chemical components
Thus, C2.5 refers to the ambient concentration of PM2.5 and AijSO4 2.5 would refer to the ambient exposure to sulfate in PM2.5. As in this study sulfate was only measured in PM2.5, we simplify the notation so that refers to ambient exposure to sulfate in PM2.5.
Appendix B1. Quality assurance
Data Collection
Three PM samplers were used in the Vancouver panel study, personal exposure monitors (PEM), Harvard Impactors, and the Tapered Element Oscillating Microbalance (TEOM). Prior to the Vancouver panel study, collocation and intercomparison experiments were made with the PEM and the Harvard Impactors. The results indicated that the PEMs gave readings that were on average 1.5 μg/m3 higher than the Harvard Impactors but that this difference was less than the difference between collocated PEMS (mean difference of 2.3 μg/m3). Therefore, no adjustments were made to the values measured in the study. Other studies have also found higher values for the PEMs, especially for intercomparisons conducted indoors (Williams et al., 2000a, 2000b; Weisel et al., 2005). These differences may be related to differences in the loss of ammonium nitrate and semi-volatile organic compounds due to evaporation during sampling. The PEM has a lower face velocity and pressure drop across the filter and, therefore, would be expected to retain more of the semi-volatile components. The observation from an intercomparison of PM10 monitors (Thomas et al., 1993) that PEMs gave median PM10 concentrations that were approximately 9% higher than the dichotomous sampler and 16% higher than the high-volume sampler are consistent with this explanation. Other studies have examined the agreement among the PEM, the Harvard Impactor, and the Federal Reference Method for PM2.5 and measured the precision of the PEM and the Harvard Impactor (Babich et al., 2000; Liu et al, 2003; Williams et al, 2000b, 2000c). There do not appear to be any intercomparisons of the TEOM with PEMs, but the TEOM is classified as an equivalent method for PM10. In general, while exposure analysts have been concerned with the differences among the various PM monitors, they have concluded that the measurements are adequate to conduct reliable exposure studies.
Data Analysis
The Vancouver study had monitoring data from five sites in the neighborhood in which the subjects lived. It was necessary to decide whether to use the ambient concentration data from the monitoring site closest to each subject's home or to use the value obtained by averaging the concentrations data from all five sites. The closest site would not be the most representative site if the site, but not the subject's home, were impacted by a local source. Averaging across five sites would also reduce the effect of a measurement error at the closest site. Therefore, both possibilities were examined.
The initial simple least squares regression analysis of T2.5 vs. C2.5 for the entire data set yields an ā of 0.32 for the closest sites and an ā of 0.52 for the average of five sites. Both values of ā seem unreasonably low for PM2.5 for the summer–fall period for subjects who mostly kept their windows open. These values were also low compared to the ā obtained from the regression of against . Two additional regression models, which gave less weight to points farthest from the regression line, were tried. They gave increased values for ā, but lower and unrealistic values for N. Therefore, some quality control checks on the data (Cj and Tij) were performed. As a point with a high T and a low C, or a point with a low T and a high C, would unduly reduce the value of α obtained from the regression, the distribution of Tij/Cj was examined. Two high values were found that were well outside the distribution of the remaining points. After removing these outliers, the simple least squares regression of Tij against the average Cij yielded ā=0.77, in good agreement with ā=0.74 from the regression of against and the ā=0.75 obtained from the average of the individual sulfate . However, even with the outliers deleted, the slope obtained from the regression with the closest site was too low (ā=0.56). Therefore, it was decided to use the average of the five monitoring sites in the further analysis of the data. Table B1 shows the results of the four regression analyses. If the interest is in obtaining a meaningful ā and N from a regression analysis, it will be necessary to check for and, if necessary, remove points that are clearly outside the distribution. However, if the interest is in determining if C is an adequate surrogate for T, the outliers should be kept in the analysis unless it can be shown that they are owing to error rather than unusually large nonambient exposures.
The average of the ambient concentrations from the five sites was used for the statistical analyses and discussion in this paper. However, in estimating values for use in the epidemiologic analysis (Ebelt et al., 2005), we performed some additional adjustments in order to obtain the most appropriate values for each individual subject. For two subjects, values were mostly greater than 1, and the regression of vs. gave a positive intercept, suggesting an indoor source of sulfate. We could not identify, however, any sources of indoor sulfate based on time-activity data. In future studies, it would be useful to check for possible indoor sources such as use of ultrasonic humidifiers, matches, kerosene heaters, inhalers using medications in the form of sulfates, or placing the personal sampler where it would be exposed to particles from evaporation of droplets from showering. For the two subjects with a positive intercept, the average , as given by the slope of vs. for each individual, was used. In both cases, the regression of on yielded a high correlation and, therefore, a reliable value of . The values of were then multiplied by the corresponding daily C2.5 value to obtain Aij2.5 (Eq. (A.5)), followed by estimation of Nij2.5 using Eq. (A.4). An additional 11 values of were >1. For these cases, the was replaced by the average of the other daily values of for the subject.
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Wilson, W., Brauer, M. Estimation of ambient and non-ambient components of particulate matter exposure from a personal monitoring panel study. J Expo Sci Environ Epidemiol 16, 264–274 (2006). https://doi.org/10.1038/sj.jes.7500483
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DOI: https://doi.org/10.1038/sj.jes.7500483
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