The Southeastern Aerosol Research and Characterization Study: Part 1—Overview

Abstract

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.     

The Southeastern Aerosol Research and Characterization Study: Part II. Filter-based measurements of fine and coarse particulate matter mass and composition

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.     

The Southeastern Aerosol Research and Characterization Study: part 1--Overview

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.     

The Aerosol Research and Inhalation Epidemiology Study (ARIES): PM2.5 mass and aerosol component concentrations and sampler intercomparisons

The Aerosol Research and Inhalation Epidemiology Study (ARIES) was designed to provide high-quality measurements of PM2.5, its components, and co-varying pollutants for an air pollution epidemiology study in Atlanta, GA. Air pollution epidemiology studies have typically relied on available data on particle mass often collected using filter-based methods. Filter-based PM2.5 sampling is susceptible to both positive and negative errors in the measurement of aerosol mass and particle-phase component concentrations in the undisturbed atmosphere. These biases are introduced by collection of gas-phase aerosol components on the filter media or by volatilization of particle phase components from collected particles. As part of the ARIES, we collected daily 24-hr PM2.5 mass and speciation samples and continuous PM2.5 data at a mixed residential-light industrial site in Atlanta. These data facilitate analysis of the effects of a wide variety of factors on sampler performance. We assess the relative importance of PM2.5 components and consider associations and potential mechanistic linkages of PM2.5 mass concentrations with several PM2.5 components. For the 12 months of validated data collected to date (August 1, 1998-July 31, 1999), the monthly average Federal Reference Method (FRM) PM2.5 mass always exceeded the proposed annual average standard (12-month average = 20.3 +/- 9.5 micrograms/m3). The particulate SO4(2-) fraction (as (NH4)2SO4) was largest in the summer and exceeded 50% of the FRM mass. The contribution of (NH4)2SO4 to FRM PM2.5 mass dropped to less than 30% in winter. Particulate NO3- collected on a denuded nylon filter averaged 1.1 +/- 0.9 micrograms/m3. Particle-phase organic compounds (as organic carbon x 1.4) measured on a denuded quartz filter sampler averaged 6.4 +/- 3.1 micrograms/m3 (32% of FRM PM2.5 mass) with less seasonal variability than SO4(2-).     

Air quality measurements for the aerosol research and inhalation epidemiology study

Measurements of pollutant gases, airborne particulate matter mass and composition, and meteorology have been made at a core site near downtown Atlanta, GA, since August 1998 in support of the Aerosol Research and Inhalation Epidemiology Study (ARIES). This site is one of eight in the Southeastern Aerosol Research and Characterization network. The measurement objective is to provide a long-term, multivariate dataset suitable for investigating statistical associations of respiratory and cardiovascular disease with airborne particulate matter composition, meteorology, and copollutant gases through epidemiologic modeling. Measurements are expected to continue through 2010. Ancillary multiyear measurements at additional sites in the Atlanta metropolitan area and in short-term exposure assessments have been used to estimate the exposure/measurement error associated with using data from a central site to approximate human exposures for the entire area. To date, 13-, 25-, and 53-month air quality datasets have been used in epidemiologic analyses.     

Effects of instrument precision and spatial variability on the assessment of the temporal variation of ambient air pollution in Atlanta, Georgia

Data from the U.S. Environmental Protection Agency Air Quality System, the Southeastern Aerosol Research and Characterization database, and the Assessment of Spatial Aerosol Composition in Atlanta database for 1999 through 2002 have been used to characterize error associated with instrument precision and spatial variability on the assessment of the temporal variation of ambient air pollution in Atlanta, GA. These data are being used in time series epidemiologic studies in which associations of acute respiratory and cardiovascular health outcomes and daily ambient air pollutant levels are assessed. Modified semivariograms are used to quantify the effects of instrument precision and spatial variability on the assessment of daily metrics of ambient gaseous pollutants (SO2, CO, NOx, and O3) and fine particulate matter ([PM2.5] PM2.5 mass, sulfate, nitrate, ammonium, elemental carbon [EC], and organic carbon [OC]). Variation because of instrument imprecision represented 7-40% of the temporal variation in the daily pollutant measures and was largest for the PM2.5 EC and OC. Spatial variability was greatest for primary pollutants (SO2, CO, NOx, and EC). Population-weighted variation in daily ambient air pollutant levels because of both instrument imprecision and spatial variability ranged from 20% of the temporal variation for O3 to 70% of the temporal variation for SO2 and EC. Wind     

Reducing the environmental impact of coal-washing practice in Australia

All Australian coal for export is washed — that is, the low-grade high-ash material is separated out and disposed of at the washery site. The coarse rejects are generally placed in embankments and the tailings are pumped into settling ponds. These methods of waste disposal can create environmental problems. In addition, they represent a significant energy loss, because about one-third of the waste material is combustible and is thus a potentially valuable source of energy. Laboratory studies at the CSIRO Division of Fossil Fuels at North Ryde, New South Wales, have shown that energy can be successfully recovered from washery wastes by the process of fluidized-bed combustion. A pilot fluidized-bed combustor, with a capacity of 2 tonnes/hour, is undergoing prolonged trial at the Clutha washery near Camden, New South Wales, in a joint project between the Joint Coal Board and CSIRO. The results from the pilot plant tests have provided the basis for a conceptual design and feasibility study for a full-scale tailings treatment plant. This study has indicated that fluidized-bed combustion:

1. offers an environmentally attractive and economically competitive alternative to the disposal of tailings in settling ponds, and
2. can be used to generate large quantities of energy from the wastes, reducing the energy lost in coal washing from around 16% to 6% of the coal mined.

     

The Southeastern Aerosol Research and Characterization Study,Part 3: Continuous Measurements of Fine Particulate Matter Mass and Composition

Abstract

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 (PM_2.5) mass is performed using a dried, 30 °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 PM_2.5 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 PM_2.5 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 PM_2.5 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.     

The Aerosol Research and Inhalation Epidemiology Study (ARIES): PM25 Mass and Aerosol Component Concentrations and Sampler Intercomparisons

ABSTRACT

The Aerosol Research and Inhalation Epidemiology Study (ARIES) was designed to provide high-quality measurements of PM₂₅, its components, and co-varying pollutants for an air pollution epidemiology study in Atlanta, GA.

Air pollution epidemiology studies have typically relied on available data on particle mass often collected using filter-based methods. Filter-based PM_2.5 sampling is susceptible to both positive and negative errors in the measurement of aerosol mass and particle-phase component concentrations in the undisturbed atmosphere. These biases are introduced by collection of gas-phase aerosol components on the filter media or by volatilization of particle phase components from collected particles. As part of the ARIES, we collected daily 24-hr PM_2.5 mass and speciation samples and continuous PM_2.5 data at a mixed residential-light industrial site in Atlanta. These data facilitate analysis of the effects of a wide variety of factors on sampler performance. We assess the relative importance of PM_2.5 components and consider associations and potential mechanistic linkages of PM_2.5 mass concentrations with several PM_2.5 components.

For the 12 months of validated data collected to date (August 1, 1998-July 31, 1999), the monthly average Federal Reference Method (FRM) PM_{2 5} mass always exceeded the proposed annual average standard (12-month average = 20.3 ± 9.5 ug/m³). The particulate SO₄ ^2- fraction (as (NH₄)₂SO₄) was largest in the summer and exceeded 50% of the FRM mass. The contribution of (NH₄)₂SO₄ to FRM PM_2.5 mass dropped to less than 30% in winter. Particu-late NO₃ ^- collected on a denuded nylon filter averaged 1.1 ± 0.9 ug/m³. Particle-phase organic compounds (as organic carbon × 1.4) measured on a denuded quartz filter sampler averaged 6.4 ± 3.1 ug/m³ (32% of FRM PM_{2 5} mass) with less seasonal variability than SO₄ ^2-.     

Air Quality Measurements for the Aerosol Research and Inhalation Epidemiology Study

Abstract

Measurements of pollutant gases, airborne particulate matter mass and composition, and meteorology have been made at a core site near downtown Atlanta, GA, since August 1998 in support of the Aerosol Research and Inhalation Epidemiology Study (ARIES). This site is one of eight in the Southeastern Aerosol Research and Characterization network. The measurement objective is to provide a long-term, multivariate dataset suitable for investigating statistical associations of respiratory and cardiovascular disease with airborne particulate matter composition, meteorology, and copollutant gases through epidemiologic modeling. Measurements are expected to continue through 2010. Ancillary multiyear measurements at additional sites in the Atlanta metropolitan area and in short-term exposure assessments have been used to estimate the exposure/measurement error associated with using data from a central site to approximate human exposures for the entire area. To date, 13-, 25-, and 53-month air quality datasets have been used in epidemiologic analyses.