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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress Appendix C Detailed Assessment of Particulate Matter Research Progress In this appendix, the committee reviews progress made in implementing the particulate matter (PM) research portfolio from 1998 (the year in which the portfolio was first recommended by the committee) until the middle of 2002. Some additional updating was done over the next year as this report was written. The focus of the committee’s evaluation has been research funded by the U.S. Environmental Protection Agency (EPA) with additional consideration of other funding organizations in the United States and abroad. The committee’s evaluative approach is described in Chapter 2. Table 1-3 in Chapter 1 summarizes the levels of funding allocated to the 10 categories of research recommendations by this committee. For each of the 10 topics in the research portfolio, the committee considers the state of understanding at the end of 1997 and the types of research projects started shortly thereafter. The committee also considers what has been learned since 1997 as well as the scientific value and decisionmaking value of that evidence. In addition, the committee discusses information expected to become available in the near future from ongoing research, major remaining uncertainties, and remaining tasks. RESEARCH TOPIC 1 OUTDOOR MEASURES VERSUS ACTUAL HUMAN EXPOSURES What are the quantitative relationships between concentrations of particulate matter and gaseous copollutants measured at stationary outdoor air-monitoring sites, and the contributions of these concentrations to actual
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress personal exposures, especially for potentially susceptible subpopulations and individuals? Introduction Compliance with the National Ambient Air Quality Standards (NAAQS) for particulate matter (PM) is ascertained by measuring ambient concentrations of PM at monitoring sites. With regard to the health effects of air pollution, the risks depend on personal exposure—that is, the exposures received by people in the various specific places, conceptualized as microenvironments, where they spend time. Total personal exposure represents the time-weighted average of particle concentrations in the microenvironments where people spend their time. Exposures to particles generated by outdoor sources take place not only outside but also in indoor environments where the particles penetrate. Indoor particle sources, such as cigarette smoking, thus might contribute substantially to total personal exposure to particles. Research carried out in regard to this topic addresses the relationship of monitoring data for ambient air with personal exposures to PM and gaseous copollutants. Data on this relationship are needed not only for healthy people but also for those persons who are particularly susceptible to air pollution and at greatest risk for experiencing adverse effects. Such persons are referred to collectively as a “susceptible subpopulation” and are further addressed under topic 8 later in this chapter. State of Understanding in 1997 Before 1997, the majority of time-series analyses of morbidity and mortality data relied on ambient air pollution concentrations as measures of exposure. A critical assumption of these investigations was that ambient PM concentrations serve as surrogates of corresponding personal exposures to ambient particles. Previous findings from personal monitoring studies suggested that human exposures differ from ambient concentrations due to the contributions of microenvironmental sources (Dockery and Spengler 1981; Ozkaynak et al. 1993; Ozkaynak et al. 1996a). In addition, most of these investigations found statistically insignificant and weak associations between personal exposures and ambient concentrations when assessed cross-sectionally (that is, at different locations). However, these conclusions were based on a small number of studies that were originally designed
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress to determine population exposure distributions rather than to examine the strength of association between personal exposures and ambient concentrations, particularly, over time. To address this knowledge gap, the National Research Council (NRC) recommended that further research be conducted to characterize longitudinal personal exposures to PM2.5, including their relationship to ambient PM2.5 and other pollutants (NRC 1998). For these longitudinal studies, groups of individuals would be measured at successive points in time to examine the relationship between their exposures and the corresponding ambient concentrations over time. This recommendation was based on findings from previous studies showing stronger correlations for data analyzed longitudinally rather than cross-sectionally (Lioy et al. 1990; Janssen et al. 1997). Additional objectives of these studies included (1) identifying factors, such as PM spatial and temporal variability, season, meteorology, time-activity patterns, and building characteristics, potentially influencing the observed relationships; (2) recruiting individuals susceptible to the effects of PM exposures, such as chronic obstruction pulmonary disease (COPD) patients, persons with cardiovascular disease or hypertension, older persons, persons with asthma, and children; (3) determining the fraction of ambient particles to which humans are exposed (henceforth, attenuation factor) and investigating its variability across different populations, seasons, climates, and home characteristics; and (4) examining relationships between personal exposures to particles and gases and their respective ambient concentrations and investigating the role of gaseous copollutants in studies of PM health effects. What Has Been Learned? Numerous PM exposure assessment studies were conducted in various locations in the United States with different climatic conditions and air pollution mixtures, including Atlanta, Baltimore, Boston, Fresno, Los Angeles, New York, Research Triangle Park, Seattle, Steubenville, and St. Louis. Support for these studies was provided by EPA, the Health Effects Institute, the Electric Power Research Institute (EPRI), the California Air Resources Board, the U.S. Department of Energy, the Ohio Coal Development Office, and the American Petroleum Institute. Studies were also conducted in Europe and South America. Although the exposure assessment studies were undertaken independently by several universities and research organizations, similar sampling and measurement approaches were
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress adopted with the goal of generating comparable data sets. Collectively, several hundred participants were monitored during periods ranging from 1 to 12 days, generating approximately 20,000-30,000 personal, indoor, outdoor, and ambient samples. The results from the longitudinal PM exposure studies have already yielded new understanding of PM exposure concentrations and factors influencing these exposures and will continue to be critical in the evolution of the PM exposure assessment field. From 1998 to 2002, more than 40 peer-reviewed papers have been published in scientific journals. Approximately 50 references of the PM criteria document (EPA 2002a) were included in Chapter 5. Topics covered ranged from associations between personal exposures and ambient concentrations (referred to as personal-ambient associations) to quantifying statistical models of exposure and field-method evaluation. During 1997-2002, a series of longitudinal PM panel studies were conducted. The field operations and laboratory-analysis components of these investigations have been completed; however, data analysis is still under way for many of these studies. Summarized below are the major findings obtained from analyses of the collected data. Relationship Between Personal Exposures and Ambient Concentrations Below, the term concentration will be used to refer to measurements obtained from stationary monitors in different microenvironments, such as indoors, outside a home, and at centrally located outdoor sites, whereas the term exposure will be used to refer to personal exposure measurements. Results from the recent panel studies support the hypothesis that ambient PM2.5 concentrations are significant predictors of corresponding personal exposures over time for cohorts of children, older persons, and persons with COPD (Ebelt et al. 2000; Evans et al. 2000; Rojas-Bracho et al. 2000; Sarnat et al. 2000, 2001; Williams et al. 2000a,b; Rodes et al. 2001). Several longitudinal exposure assessment studies measured personal PM10 exposures and reported weaker personal-ambient associations than between those for PM2.5 (Evans et al. 2000; Rojas-Bracho et al. 2000; Williams et al. 2000a; Chang and Suh 2003). Subject-specific correlation coefficients showed considerable interpersonal variability, from nonsignificant to values approaching unity (Rojas-Bracho et al. 2000; Williams et al. 2000a; Wallace et al. 2002). Home air exchange rate (AER) as well as AER surrogates, such as air conditioning
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress use, open window status, season and climatic conditions, were found to be important factors explaining variability in the strength of the correlations (Long et al. 2001a; Howard-Reed et al. 2002; Wallace et al. 2002). Personal-ambient associations were found to be stronger for participants residing in homes with high AERs (Rojas-Bracho et al. 2000; Sarnat et al. 2000). The strength of the personal-ambient associations for PM2.5 and PM10 increased as the number of repeated measures per individual increased from a few days up to 15 days (Williams et al. 2000a). Several monitoring studies have investigated the spatial variability of ambient PM concentrations. Studies conducted in eastern locations, such as Boston, New York, Philadelphia, Atlanta, and Research Triangle Park, found that ambient PM2.5 concentrations are homogeneously distributed throughout these metropolitan areas, as shown by high cross-city PM2.5 correlations (Wilson and Suh 1997; Lippmann et al. 2000; Williams et al. 2002). In contrast, monitoring studies of coarse particle concentrations have shown considerable spatial heterogeneity (Burton et al. 1996; Evans et al. 2000; Chang and Suh, 2003; Goswami et al. 2002; Zhu et al. 2002). Greater variability in PM2.5 concentrations was observed in two western U.S. cities, Los Angeles and Seattle. In Los Angeles, PM2.5 concentrations measured at coastal monitoring sites were significantly lower than those measured inland (Chang and Suh 2003). Likewise, results from an exposure study in Seattle showed that PM2.5 concentrations decreased with increasing elevation (Goswami et al. 2002). Despite those findings, the generally strong personal-ambient PM2.5 correlations reported in the longitudinal exposure assessment studies downplay the importance of spatial variability of ambient PM2.5 as a modifier of personal-ambient relationships (Wilson and Suh 1997). There is also evidence that specific sizes or components of PM2.5, especially those associated with mobile-source emissions (for example, elemental carbon and ultrafine particles), might exhibit a greater degree of spatial variability and, correspondingly, weaker personal-ambient correlations (EPA 2002b). Pellizari et al. (1999), using a probability sample study design, showed that the mass fraction of PM2.5 manganese (a gasoline additive in Canada) varied spatially across the Toronto metropolitan area, significantly altering the observed personal-ambient correlations. Ultrafine ratios outside and inside homes were noted to be highly variable in Fresno homes, and local outdoor combustion sources were noted to contribute highly to this variability (Lawless et al. 2001; Vette et al. 2001). Ultrafine particle concentrations were shown to be highest near highways in Los Angeles and to drop to background concentrations within 300 meters (m)
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress of the highway (Zhu et al. 2002). Therefore, personal-ambient relationships for specific particle components and size fractions are expected to differ from those observed for PM2.5. This hypothesis should be investigated in future studies, as suggested by research topic 2. Collectively, the panel studies, which were performed on various cohorts (several hundred individuals) and cities across different seasons, showed that there were varying degrees of association between personal exposures and ambient concentrations for the measured individual, with almost half of the associations being nonsignificant. In general, the percentage of participants with significant associations for PM10 was less than that for PM2.5 (Sarnat et al. 2000; Williams et al. 2000a,b). The personal-ambient associations involving exposures to particles primarily of ambient origin (SO42) were shown to be consistently stronger and less variable than those found for PM2.5 (Ebelt et al. 2000; Sarnat et al. 2000; Landis et al. 2001; Brown et al. 2003). These findings highlight the influence of nonambient PM2.5 contributions on personal exposures and the weakening effect of these contributions on associations of personal exposures with corresponding ambient PM2.5 concentrations (Rea et al. 2001). Indoor Concentrations Individuals spend their time in a variety of microenvironments, such as the home, workplace, school, in transport media, and outdoors. To date, however, most microenvironmental studies have focused on ambient and residential microenvironments. For that reason, this discussion focuses on the residential and outdoor environments; for simplicity, the terms indoor and ambient will be used to refer to these two microenvironments, respectively. Studies referenced in this discussion used measurements conducted either outside homes (outdoor concentrations) or at a centrally located fixed site (ambient concentrations). For brevity, the term ambient concentrations will be used for both ambient and outdoor concentrations. Near-real-time PM2.5 indoor and personal measurements have highlighted the importance of microenvironmental PM sources (Abt et al. 2000; Howard-Reed et al. 2000; Long et al. 2000; Rea et al. 2001; Vette et al. 2001). However, there is no evidence that indoor exposures have a strong effect on personal-ambient relationships. This lack of effect may be explained by the patterns of contributions of indoor sources to personal exposures to particles. Although indoor source use may be intermittent, the daily patterns of use are relatively consistent. Therefore, when indoor PM-
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress source contributions are averaged over repeated 24-hour (hr) sampling periods, they add only a small fraction to total PM2.5 exposure variability for a particular person over time. That result might not be true for locations where ambient concentrations are very low or individuals are heavily exposed to specific microenvironmental sources (for example, cigarette smoking). Particles of indoor origin can be produced either by combustion sources, such as cooking or gas phase reactions (mostly ultrafine particles), or by mechanical processes, such as vacuuming, sweeping, or dusting (mostly coarse particles). In contrast, most particles of ambient origin found indoors are present in the accumulation mode, because the penetration of ultrafine and coarse particles is considerably lower than that of particles in the accumulation mode (Long et al. 2001a; Vette et al. 2001). The fraction of ambient particles that penetrates indoors varies considerably (from approximately 0.3 to 1.0), and it increases with the home AER (Sarnat et al. 2002). The infiltration efficiency in 44 homes in Seattle varied from about 0.3 to 1.0 and was a function of AER (Allen et al. 2003; Wallace et al. 2004). In addition, the average infiltration factor for 294 homes of inner-city children with asthma in several U.S. cities was found to be 0.50 (Wallace et al. 2003). Finally, the relative impact of ambient and indoor sources has also been shown to depend strongly on the home AER and removal processes, such as filtration by forced air heating, ventilation, or air-conditioning or by independent air cleaners (Rodes et al. 1998). Impact of Ambient Concentrations on Personal Exposures Until recently, the variability in personal PM exposures was considered to be primarily due to the contributions from microenvironmental sources; all PM particles of ambient origin were also considered to penetrate indoors. There is now strong evidence, however, that a substantial fraction of this variability is due to the impact of ambient sources on the indoor environments and, subsequently, on personal exposures (Landis et al. 2001; Williams et al. 2002). The fraction of ambient PM concentrations to which individuals are exposed (attenuation factor) has been shown to vary considerably. For example, in Baltimore during the summer, the estimated average attenuation factor for two investigated cohorts (children and older persons) was 0.48, which was substantially lower than that estimated for Boston during the same season and for the same cohorts (0.81). The average attenuation factor for these cohorts during the winter-
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress time season for Baltimore and Boston were similar, 0.23 and 0.27, respectively (Brown et al. 2003). Analysis of similar data sets from different locations will probably provide more information about the variability of this factor and the parameters influencing its variability (that is, home ventilation characteristics and time-activity patterns) (Rodes et al. 2001). Finally, future studies should focus on characterizing attenuation factors for specific PM components and size fractions (research topic 2). Particles of Ambient and Indoor Origin Associations have been found between mortality and morbidity outcomes and corresponding ambient PM concentrations, suggesting an adverse effect of exposures to ambient PM. However, studies have suggested that PM of indoor origin might be associated with adverse effects (Drumm et al. 1999; Long et al. 2001b). These studies point to the need for a comprehensive assessment of exposures to particles of both ambient and indoor origin, in part to make possible the assessment of the individual effects of both particle types. The relative contributions of ambient and indoor PM sources to personal exposures were investigated in recent studies using different approaches. For example, sulfate was used as a tracer of ambient PM (Wilson and Suh, 1997; Ebelt et al. 2000; Oglesby et al. 2000; Sarnat et al. 2000; Landis et al. 2001). Although sulfate is a suitable tracer for the accumulation mode, it might overestimate the penetration of ambient ultrafine and coarse particles indoors. Alternatively, statistical methods based on the regression of personal exposures or indoor air concentrations on ambient concentrations have also been used (Ott et al. 2000; Wallace and Ott 2002). Cohort Effect When the longitudinal exposure studies were initiated, personal exposures to PM were hypothesized to differ by subpopulation because of time-activity differences. The EPA National Exposure Research Laboratory (NERL) measured PM2.5 exposures of two distinct subpopulations living within the Research Triangle Park (RTP) region of North Carolina (Williams et al. 2002). A total of 38 participants were monitored (a cohort of 30 nonsmoking, hypertensive African-Americans living in a low-to-moderate
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress socioeconomic status neighborhood of Raleigh and a multiracial cohort of 8 individuals with implanted cardiac defibrillators from Chapel Hill) (Wallace et al. 2004). Contrary to expectations that the multiracial cohort with implanted cardiac defibrillators might be more sedentary than the hypertensive African-American cohort, analysis of the time-activity patterns did not show statistically significant differences between the two groups. Considerable intracohort variability was found, however, in the duration and location of activities conducted. Brown et al. (2003) found no differences in exposures to PM2.5 of ambient origin among the investigated cohorts of children, COPD patients, and healthy older citizens living in Baltimore and Boston. Personal PM2.5 exposures were measured for 56 subjects living in Baltimore and 43 subjects living in Boston. The Baltimore study investigated 20 healthy senior citizens, 21 schoolchildren, and 15 individuals with COPD. The Boston study investigated 20 healthy older citizens and 23 schoolchildren. (Brown et al. 2003). Using mixed models, the study had personal exposures regressed on the corresponding outdoor concentrations. Both city and season were found to have an effect on the regression intercept (mostly nonambient exposures) and slope (attenuation factor). Similar to the RTP study, no cohort effect on the regression intercepts or slopes was found. These findings were somewhat unexpected considering the hypothesized differences in cohort activities and time spent outdoors during the 24-hr sampling periods. Exposures to Gaseous Copollutants In several longitudinal panel studies, simultaneous 24-hr personal PM2.5, ozone (O3), sulfur dioxide (SO2), and nitrogen dioxide (NO2) exposures and corresponding ambient concentrations were measured using a personal multipollutant sampler. The findings of these studies suggest that personal PM2.5 exposures and corresponding ambient concentrations were correlated, and personal O3, SO2, and NO2 exposures were not correlated with their respective ambient concentrations (Sarnat et al. 2001). In contrast, PM2.5 personal exposures were correlated with O3 and NO2 ambient concentrations. Similar results using different sampling methods were observed in the Baltimore and RTP panel studies (Williams et al. 2000c; Vette et al. 2002). These results suggest that using ambient gaseous concentrations in multipollutant health-effects models along with PM2.5 might not be appropriate, since the ambient gaseous and PM2.5 concentrations are serving as surrogates for PM2.5 exposures.
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress How Much Has Uncertainty Been Reduced? Over the past 6 years, PM exposure assessment studies of healthy and susceptible individuals have been conducted. During this period, significant progress has been made in reducing methodological uncertainties in the assessment of gravimetric PM mass (Allen et al. 1999; Lawless and Rodes 1999) and in the PM monitoring methods used in personal exposure assessment (Williams et al. 2000b; Demokritou et al. 2001). Studies characterizing exposure among sensitive populations, in particular, directly addressed a major research need identified by this committee. The results show that the relationship between personal exposures and ambient concentrations varies considerably both within and between the measured cohorts. The observed dissimilarities among individuals were attributed to differences in home characteristics, which likely vary by season and region, and, to a lesser extent, time-activity patterns and microenvironmental sources. Although analysis is still being conducted to examine potential cohort-specific exposure patterns, results to date do not indicate significant differences in PM2.5 exposures among the cohorts (Brown et al. 2003; Wallace et al. EPA, unpublished material, 2003; Williams et al. 2002). Despite the interpersonal differences observed within each of the investigated panels, significant associations between personal and ambient concentrations were found for approximately one-half of the measured individuals ( Sarnat et al. 2001; Liu et al. 2003). Although these results are based on a small number of individuals who might not be representative of the entire population, they suggest that the use of PM2.5 concentrations as a surrogate of population exposures is a reasonable and scientifically sound assumption. However, the conclusions drawn for PM2.5 might not be applicable to other particle-size fractions, such as ultrafine and coarse particles, and particle components (for example, elemental carbon, metals, and organic compounds). Future research, outlined in research topic 2, will focus on the exposure assessment of different particle-size fractions and constituents. As mentioned above, considerable intrapersonal and interpersonal variability was reported in the relationships between personal PM2.5 exposures and corresponding ambient concentrations. In the past, these differences were attributed to the impact of microenvironmental sources. However, the recent findings provide compelling evidence that the fraction of ambient particles penetrating indoors might be highly variable, thus weakening personal-ambient associations. The recent studies suggest that the
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Research Priorities for Airborne Particulate Matter: IV - Continuing Research Progress fraction of ambient particles affecting personal exposures varies by location and season, especially in cities where distinct seasonal weather patterns exist. Therefore, it is reasonable to assume that differences in observed risks in multicity epidemiological studies can be attributable, in part, to corresponding differences in the contributions of ambient PM sources to personal PM exposures (Janssen et al. 2002). Emerging information from multipollutant exposure studies suggests that ambient concentrations of gaseous pollutants, such as O3, SO2, and nitrogen oxides (NOx), in some U.S. cities are associated with personal PM2.5 exposures and not with personal exposures to the gases themselves (Williams et al. 2000d; Sarnat et al. 2001; Brown et al. 2003; Vette et al. 2002;). (No results are available for carbon monoxide (CO), however, because short-term or continuous personal exposure measures are not available for this pollutant gas.) Therefore, a number of ambient gaseous copollutants might be surrogates of fine-particle personal exposures and not confounders of associations of PM with outcome measures. This information is relevant to the development of multivariate statistical models that include PM and other pollutants and also to the interpretation of model findings. This methodological issue receives further consideration in research topic 10. Synthesis The longitudinal exposure assessment studies conducted during the past 6 years have provided support for findings reported in the time-series epidemiological studies that use ambient concentrations as surrogates of personal exposures. For about half the measured individuals, ambient concentrations were shown to be significantly correlated with corresponding personal exposures. Scientific Value The design and execution of the longitudinal exposure assessment studies were largely successful. These investigations comprised measurements of different cohorts living in a variety of climates and locales and exposed to varying levels of ambient pollutants. The information obtained from these studies has enhanced the understanding of the relationship
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Representative terms from entire chapter: