Health effects of fine particulate air pollution: lines that connect.
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Biomedical subjects
Publications and source records attributed to George M Hidy.
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Deployment of continuous analyzers in the Southeastern Aerosol Research and Characterization Study (SEARCH) network began in 1998 and continues today as new technologies are developed. Measurement of fine particulate matter (PM2.5) mass is performed using a dried, 30 degrees C tapered element oscillating microbalance (TEOM). TEOM measurements are complemented by observations of light scattering by nephelometry. Measurements of major constituents include: (1) SO4(2-) via reduction to SO2; (2) NH4+ and NO3- via respective catalytic oxidation and reduction to NO, (3) black carbon (BC) by optical absorption, (4) total carbon by combustion to CO2, and (5) organic carbon by difference between the latter two measurements. Several illustrative examples of continuous data from the SEARCH network are presented. A distinctive composite annual average diurnal pattern is observed for PM2.5 mass, nitrate, and BC, likely indicating the influence of traffic-related emissions, growth, and break up of the boundary layer and formation of ammonium nitrate. Examination of PM2.5 components indicates the need to better understand the continuous composition of the unmeasured "other" category, because it contributes a significant fraction to total mass during periods of high PM2.5 loading. Selected episodes are presented to illustrate applications of SEARCH data. An SO2 conversion rate of 0.2%/hr is derived from an observation of a plume from a coal-fired power plant during early spring, and the importance of local, rural sources of NH3 to the formation of ammonium nitrate in particulate matter (PM) is demonstrated.
Measurements from sites of the Southeastern Aerosol Research and Characterization (SEARCH) program, made from 1998 to 2001, are used with a thermodynamic equilibrium model, Simulating Composition of Atmospheric Particles at Equilbrium (SCAPE2), to extend an earlier investigation of the responses of fine particulate nitrate (NO3-) and fine particulate matter (PM2.5) mass concentrations to changes in concentrations of nitric acid (HNO3) and sulfate (SO42-). The responses were determined for a projected range of variations of SO42- and HNO3 concentrations resulting from adopted and proposed regulatory initiatives. The predicted PM2.5 mass concentration decreases averaged 1.8-3.9 microg/m3 for SO42- decreases of 46-63% from current concentrations. Combining the S042- decrease with a 40% HNO3 decrease from current concentrations (approximating expected mobile-source oxides of nitrogen [NOx] reductions by 2020) yielded additional incremental reductions of mean predicted PM2.5 mass concentration of 0.2 microg/m3 for three nonurban sites and 0.8-1 microg/m3 for one nonurban and two urban sites. Increasing the HNO3 reduction to 55% (an estimate of adding Clear Skies Phase II NOx reductions) yielded additional incremental reductions of mean predicted PM2.5 mass concentration of 0-0.4 microg/m3. Because of the well-documented losses of particulate NO3- from Federal Reference Method (FRM) filters, only a fraction of these incremental changes would be observed.
The Southeastern Aerosol Research and Characterization Study (SEARCH) was implemented in 1998-1999 to provide data and analyses for the investigation of the sources, chemical speciation, and long-term trends of fine particulate matter (PM2.5) and coarse particulate matter (PM10-2.5) in the Southeastern United States. This work is an initial analysis of 5 years (1999-2003) of filter-based PM2.5 and PM10-2.5 data from SEARCH. We find that annual PM2.5 design values were consistently above the National Ambient Air Quality Standards (NAAQS) 15 microg/m3 annual standard only at monitoring sites in the two largest urban areas (Atlanta, GA, and North Birmingham, AL). Other sites in the network had annual design values below the standard, and no site had daily design values above the NAAQS 65 microg/m3 daily standard. Using a particle composition monitor designed specifically for SEARCH, we found that volatilization losses of nitrate, ammonium, and organic carbon must be accounted for to accurately characterize atmospheric particulate matter. In particular, the federal reference method for PM2.5 underestimates mass by 3-7% as a result of these volatilization losses. Organic matter (OM) and sulfate account for approximately 60% of PM2.5 mass at SEARCH sites, whereas major metal oxides (MMO) and unidentified components ("other") account for > or = 80% of PM10-2.5 mass. Limited data suggest that much of the unidentified mass in PM10-2.5 may be OM. For paired comparisons of urban-rural sites, differences in PM2.5 mass are explained, in large part, by higher OM and black carbon at the urban site. For PM10, higher urban concentrations are explained by higher MMO and "other." Annual means for PM2.5 and PM10-2.5 mass and major components demonstrate substantial declines at all of the SEARCH sites over the 1999-2003 period (10-20% in the case of PM2.5, dominated by 14-20% declines in sulfate and 11-26% declines in OM, and 14-25% in the case of PM10-2.5, dominated by 17-30% declines in MMO and 14-31% declines in "other"). Although declining national emissions of sulfur dioxide and anthropogenic carbon may account for a portion of the observed declines, additional investigation will be necessary to establish a quantitative assessment, especially regarding trends in local and regional emissions, primary carbon emissions, and meteorology.
Protocols for the particulate matter (PM) National Ambient Air Quality Standards (NAAQS), and the Regional Haze Rule (RHR) give two complementary definitions for "natural" background airborne particle concentrations in the United States. The definition for the NAAQS derives largely from reported annual averages, whereas the definition for the RHR takes into account the frequency of occurrence of a range of visibility conditions estimated using fine particle composition. These definitions are simple, static representations of background or "unmanageable" aerosol conditions in the United States. An accumulation of data from rural-remote sites representing global conditions indicates that the airborne particle concentrations are highly variable. Observational campaigns show weather-related variations, including incidents of regional or intercontinental transport of pollution that influence background aerosol levels over midlatitude North America. Defining a background in North America based on long-term observations relies mainly on the remote-rural IMPROVE network in the United States, with a few additional measurements from Canada. Examination of the frequency of occurrence of mass concentrations and particle components provides insight not only about annual median conditions but also the variability of apparent background conditions. The results of this analysis suggest that a more elaborate approach to defining an unmanageable background could improve the present approach taken for information input into the U.S. regulatory process. An approach interpreting the continental gradients in fine PM (PM2.5) concentrations and composition may be warranted.
An experimental design is described to estimate the fraction of secondary fine particle from the biogenic component of volatile organic compounds (VOCs) in the atmosphere using radiocarbon isotopic abundance ratios. The method distinguishes between "modern" carbon (C), and "old" C of primary and secondary origins based on three components, condensed-phase organic carbon (OC), semi-volatile particulate compounds (SVOCs), and VOCs. The method depends on interpretation of diurnal and seasonal variation in OC, SVOC, and VOC concentrations. Sampling employs a filter-denuder unit, which collects the three C components for isotopic analysis. The samples are collected repetitively for a daily sequence of the same hourly intervals covering diurnal periods with similar meteorological conditions. Collected C is thermally treated to separate OC from black carbon on filters and VOCs or SVOCs from adsorbents, with all four fractions individually oxidized to carbon dioxide to determine the radiocarbon content by accelerator mass spectrometry. Using C isotope abundance, the data are interpreted for fractions of primary modern C and secondary modern C as estimated from averaging diurnal and seasonal variations in the concentration data. As support for interpretation, samples of OC, SVOCs, and VOCs would be analyzed for speciation to identify source indicator species present.
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A thermodynamic equilibrium model, Simulating Composition of Atmospheric Particles at Equilibrium (SCAPE2), was used to investigate the response of fine particulate NO3(-) to changes in concentrations of HNO3, NH3, and SO4(2-) in the southeastern United States. The data consisted of daily, 24-hr time resolution measurements from the Aerosol Research Inhalation Epidemiology Study (ARIES) Jefferson Street (Atlanta) site and five other sites of the Southeastern Aerosol Research and Characterization Project (SEARCH). Reductions of total NH3 (gas-phase NH3 plus particulate NH4(+)), total NO3(-) (HNO3 plus particulate NO3(-)), SO4(2-), or combined total NO3(-) (HNO3 plus particulate NO3(-)) with SO4(2-) were used to estimate the effects of changing emission levels. The conversion of SO2 to SO4(2-) and NO2 to HNO3 involves additional nonlinear reactions not incorporated into the model. For all sites, fine particulate NO3(-) concentrations decreased in response to reductions of either NH3 or total NO3(-), but the particulate NO3(-) decreases were greater for the NH3 reductions than for the total NO3(-) reductions. Particulate NO3(-) concentrations increased in response to reductions of SO4(2-). For the combined reduction (total NO3(-) plus SO4(2-)), the resulting particulate NO3(-) concentrations were on average no different than the base-case NO3(-) levels. Measurements of fine particulate NO3(-) and HNO3 support the modeling conclusions and indicate that particulate NO3(-) formation is limited by the availability of NH3 at most times at all SEARCH sites.
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This paper presents an overview of a major, long-term program for tropospheric gas and aerosol research in the southeastern United States. Building on three existing ozone (O3)-focused research sites begun in mid-1992, the Southeastern Aerosol Research and Characterization Study (SEARCH) was initiated in mid-1998 as a 7-year observation and research program with a broader focus including aerosols and an expanded geographical coverage in the Southeast. The monitoring network comprises four urban-rural (or urban-suburban) site pairs at locations along the coast of the Gulf of Mexico and inland, including two moderately sized and two major urban areas (Pensacola, FL; Gulfport, MS; Atlanta, GA; and Birmingham, AL). The sites are equipped with an extensive suite of instruments for measuring particulate matter (PM), gases relevant to secondary O3 and the production of secondary aerosol particles, and surface meteorology. The measurements taken to date have added substantially to the knowledge about the temporal behavior and geographic variability of tropospheric aerosols in the Southeast. Details are presented in four papers to follow.