Hourly and daily patterns of particle-phase organic and elemental carbon concentrations in the urban atmosphere

Two semicontinuous elemental and organic carbon analyzers along with daily integrated samplers, which were used for laboratory elemental and organic carbon analysis, were operated to measure PM2.5 organic carbon (OC) and elemental carbon (EC) for the entire year of 2002 at the St. Louis Midwest Supersite. The annual-average denuded OC and EC concentrations were 3.88 and 0.7 microg/m3, respectively. A comparison of the 24-hr average denuded and undenuded OC measurements showed a positive bias for the undenuded OC measurement that was best represented by a positive intercept of 0.34 +/- 0.1 microg/m3 and a slope of 1.06 +/- 0.02, with an R2 of 0.91. The full year of daily EC and OC measurements was used to demonstrate that a one-in-six-day sampling strategy at this site accurately represents the annual average concentrations. Although fine particle OC concentrations did not correlate with day of the week, EC concentrations showed a significant weekly pattern, with the highest concentration during the middle of the workweek and the lowest concentration on Sundays. Hourly EC and OC measurements yielded average diurnal patterns for the EC to OC ratio that peaked during morning rush hour traffic on weekdays but not on weekends.     

Short-term temporal variation in PM2.5 mass and chemical composition during the Atlanta Supersite Experiment, 1999

Measurements in urban Atlanta of transient aerosol events in which PM2.5 mass concentrations rapidly rise and fall over a period of 3-6 hr are reported. The data are based on new measurement techniques demonstrated at the U.S. Environmental Protection Agency (EPA) Atlanta Supersite Experiment in August 1999. These independent instruments for aerosol chemical speciation of NO3-, SO4(2-), NH4+, and organic and elemental carbon (OC and EC), reconstructed the observed hourly dry PM2.5 mass to within 20% or better. Data from the experiment indicated that transient PM2.5 events were ubiquitous in Atlanta and were typically characterized by a sudden increase of EC (soot) and OC in the early morning or SO4(2-) in the late afternoon. The frequent temporal decoupling of these events provides insights into their origins, suggesting mobile sources in metro Atlanta as the main contributor to early morning PM2.5 and more regionally located point SO2 sources for afternoon PM2.5 events. The transient events may also have health implications. New data suggest that short-term PM2.5 exposures may lead to adverse health effects. Standard integrated filter-based techniques used in PM2.5 compliance monitoring networks and in most past PM2.5 epidemiologic studies collect samples over 24-hr periods and thus are unable to capture these transient events. Moreover, health-effects studies that focus on daily PM2.5 mass alone cannot evaluate the health implications of the unique and variable chemical properties of these episodes.     

Advances in integrated and continuous measurements for particle mass and chemical composition

Recent improvements in integrated and continuous PM2.5 mass and chemical measurements from the Supersite program and related studies in the past decade are summarized. Analytical capabilities of the measurement methods, including accuracy, precision, interferences, minimum detectable levels, comparability, and data completeness are documented. Upstream denuders followed by filter packs in integrated samplers allow an estimation of sampling artifacts. Efforts are needed to: (1) address positive and negative artifacts for organic carbon (OC), and (2) develop carbon standards to better separate organic versus elemental carbon (EC) under different temperature settings and analysis atmospheres. Advances in thermal desorption followed by gas chromatography/ mass spectrometry (GC/MS) provide organic speciation of approximately 130 nonpolar compounds (e.g., n-alkanes, alkenes, hopanes, steranes, and polycyclic aromatic hydrocarbons [PAHs]) using small portions of filters from existing integrated samples. Speciation of water-soluble OC (WSOC) using ion chromatography (IC)-based instruments can replace labor-intensive solvent extraction for many compounds used as source markers. Thermal gas-based continuous nitrate and sulfate measurements underestimate filter ions by 10-50% and require calibration against on-site filter-based measurements. IC-based instruments provide multiple ions and report comparable (+/-10%) results to filter-based measurements. Maintaining a greater than 80% data capture rate in continuous instruments is labor intensive and requires experienced operators. Several instruments quantify black carbon (BC) by optical or photoacoustic methods, or EC by thermal methods. A few instruments provide real-time OC, EC, and organic speciation. BC and EC concentrations from continuous instruments are highly correlated but the concentrations differ by a factor of two or more. Site- and season-specific mass absorption efficiencies are needed to convert light absorption to BC. Particle mass spectrometers, although semiquantitative, provide much information on particle size and composition related to formation, growth, and characteristics over short averaging times. Efforts are made to quantify mass by collocating with other particle sizing instruments. Common parameters should be identified and consistent approaches are needed to establish comparability among measurements.     

Indoor/Outdoor relationships, trends, and carbonaceous content of fine particulate matter in retirement homes of the Los Angeles Basin

Hourly indoor and outdoor fine particulate matter (PM2.5), organic and elemental carbon (OC and EC, respectively), particle number (PN), ozone (O3), carbon monoxide (CO), and nitrogen oxide (NOx) concentrations were measured at two different retirement communities in the Los Angeles, CA, area as part of the Cardiovascular Health and Air Pollution Study. Site A (group 1 [G1]) was operated from July 6 to August 20, 2005 (phase 1 [P1]) and from October 19 to December 10, 2005 (P2), whereas site B (group 2 [G2]) was operated from August 24 to October 15, 2005 (P1), and from January 4 to February 18, 2006 (P2). Overall, the magnitude of indoor and outdoor measurements was similar, probably because of the major influence of outdoor sources on indoor particle and gas levels. However, G2 showed a substantial increase in indoor OC, PN, and PM2.5 between 6:00 and 9:00 a.m., probably from cooking. The contributions of primary and secondary OC (SOA) to measured outdoor OC were estimated from collected OC and EC concentrations using EC as a tracer of primary combustion-generated OC (i.e., "EC tracer method"). The study average outdoor SOA accounted for 40% of outdoor particulate OC (40-45% in the summer and 32-40% in the winter). Air exchange rates (hr(-1)) and infiltration factors (Finf; dimensionless) at each site were also determined. Estimated Finf and measured particle concentrations were then used in a single compartment mass balance model to assess the contributions of indoor and/or outdoor sources to measured indoor OC, EC, PM2.5, and PN. The average percentage contributions of indoor SOA of outdoor origin to measured indoor OC were approximately 35% (during G1P1 and G1P2) and approximately 45% (for G2P1 and G2P2). On average, 36% (G2P1) to 44% (G1P1) of measured indoor OC was composed of outdoor-generated primary OC.     

Multiple-year black carbon measurements and source apportionment using delta-C in Rochester, New York

Black carbon (BC), an important component ofthe atmospheric aerosol, has climatic, environmental, and human health significance. In this study, BC was continuously measured using a two-wavelength aethalometer (370 nm and 880 nm) in Rochester; New York, from January 2007 to December 2010. The monitoring site is adjacent to two major urban highways (I-490 and I-590), where 14% to 21% of the total traffic was heavy-duty diesel vehicles. The annual average BC concentrations were 0.76 microg/m3, 0.67 microg/m3, 0.60 microg/m3, and 0.52 microg/m3 in 2007, 2008, 2009, and 2010, respectively. Positive matrix factorization (PMF) modeling was performed using PM2.5 elements, sulfate, nitrate, ammonia, elemental carbon (EC), and organic carbon (OC) data from the US. Environmental Protection Agency (EPA) speciation network and Delta-C (UVBC370nm-BC880nm) data. Delta-C has been previously shown to be a tracer of wood combustion factor It was used as an input variable in source apportionment models for the first time in this study and was found to play an important role in separating traffic (especially diesel) emissions from wood combustion emissions. The result showed the annual average PM2.5 concentrations apportioned to diesel emissions in 2007, 2008, 2009, and 2010 were 1.34 microg/m3, 1.25 microg/m3, 1.13 microg/m3, and 0.97 microg/m3, respectively. The BC conditional probability function (CPF) plots show a large contribution from the highway diesel traffic to elevated BC concentrations. The measurements and modeling results suggest an impact of the US Environmental Protection Agency (EPA) 2007 Heavy-Duty Highway Rule on the decrease ofBC and PM2.5 concentrations during the study period.     

Source apportionment of airborne particulate matter in Southeast Texas using a source-oriented 3D air quality model

A nested version of the source-oriented externally mixed UCD/CIT model was developed to study the source contributions to airborne particulate matter (PM) during a two-week long air quality episode during the Texas 2000 Air Quality Study (TexAQS 2000). Contributions to primary PM and secondary ammonium sulfate in the Houston–Galveston Bay (HGB) and Beaumont–Port Arthur (BPA) areas were determined.The predicted 24-h elemental carbon (EC), organic compounds (OC), sulfate, ammonium ion and primary PM_2.5 mass are in good agreement with filter-based observations. Predicted concentrations of hourly sulfate, ammonium ion, and primary OC from diesel and gasoline engines and biomass burning organic aerosol (BBOA) at La Porte, Texas agree well with measurements from an Aerodyne Aerosol Mass Spectrometer (AMS).The UCD/CIT model predicts that EC is mainly from diesel engines and majority of the primary OC is from internal combustion engines and industrial sources. Open burning contributes large fractions of EC, OC and primary PM_2.5 mass. Road dust, internal combustion engines and industries are the major sources of primary PM_2.5. Wildfire dominates the contributions to all primary PM components in areas near the fires. The predicted source contributions to primary PM are in general agreement with results from a chemical mass balance (CMB) model. Discrepancy between the two models suggests that further investigations on the industrial PM emissions are necessary.Secondary ammonium sulfate accounts for the majority of the secondary inorganic PM. Over 80% of the secondary sulfate in the 4 km domain is produced in upwind areas. Coal combustion is the largest source of sulfate. Ammonium ion is mainly from agriculture sources and contributions from gasoline vehicles are significant in urban areas.     

Improving source apportionment of fine particles in the eastern United States utilizing temperature-resolved carbon fractions

The objectives of this study were to examine the use of carbon fractions to identify particulate matter (PM) sources, especially traffic-related carbonaceous particle sources, and to estimate their contributions to the particle mass concentrations. In recent studies, positive matrix factorization (PMF) was applied to ambient fine PM (PM2.5) compositional data sets of 24-hr integrated samples including eight individual carbon fractions collected at three monitoring sites in the eastern United States: Atlanta, GA, Washington, DC, and Brigantine, NJ. Particulate carbon was analyzed using the Interagency Monitoring of Protected Visual Environments/Thermal Optical Reflectance method that divides carbon into four organic carbons (OC): pyrolized OC and three elemental carbon (EC) fractions. In contrast to earlier PMF studies that included only the total OC and EC concentrations, gasoline emissions could be distinguished from diesel emissions based on the differences in the abundances of the carbon fractions between the two sources. The compositional profiles for these two major source types show similarities among the three sites. Temperature-resolved carbon fractions also enhanced separations of carbon-rich secondary sulfate aerosols. Potential source contribution function analyses show the potential source areas and pathways of sulfate-rich secondary aerosols, especially the regional influences of the biogenic, as well as anthropogenic secondary aerosol. This study indicates that temperature-resolved carbon fractions can be used to enhance the source apportionment of ambient PM2.5.     

Contribution of primary and secondary sources to organic aerosol and PM2.5 at SEARCH network sites

Chemical tracer methods for determining contributions to primary organic aerosol (POA) are fairly well established, whereas similar techniques for secondary organic aerosol (SOA), inherently complicated by time-dependent atmospheric processes, are only beginning to be studied. Laboratory chamber experiments provide insights into the precursors of SOA, but field data must be used to test the approaches. This study investigates primary and secondary sources of organic carbon (OC) and determines their mass contribution to particulate matter 2.5 microm or less in aerodynamic diameter (PM2.5) in Southeastern Aerosol Research and Characterization (SEARCH) network samples. Filter samples were taken during 20 24-hr periods between May and August 2005 at SEARCH sites in Atlanta, GA (JST); Birmingham, AL (BHM); Centerville, AL (CTR); and Pensacola, FL (PNS) and analyzed for organic tracers by gas chromatography-mass spectrometry. Contribution to primary OC was made using a chemical mass balance method and to secondary OC using a mass fraction method. Aerosol masses were reconstructed from the contributions of POA, SOA, elemental carbon, inorganic ions (sulfate [SO4(2-)], nitrate [NO3-], ammonium [NH4+]), metals, and metal oxides and compared with the measured PM2.5. From the analysis, OC contributions from seven primary sources and four secondary sources were determined. The major primary sources of carbon were from wood combustion, diesel and gasoline exhaust, and meat cooking; major secondary sources were from isoprene and monoterpenes with minor contributions from toluene and beta-caryophyllene SOA. Mass concentrations at the four sites were determined using source-specific organic mass (OM)-to-OC ratios and gave values in the range of 12-42 microg m(-3). Reconstructed masses at three of the sites (JST, CTR, PNS) ranged from 87 to 91% of the measured PM2.5 mass. The reconstructed mass at the BHM site exceeded the measured mass by approximately 25%. The difference between the reconstructed and measured PM2.5 mass for nonindustrial areas is consistent with not including aerosol liquid water or other sources of organic aerosol.     

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.     

Fine and coarse particulate matter chemical characterization in a heavily industrialized city in central Mexico during Winter 2003

This paper presents the results of the first reported study on fine particulate matter (PM) chemical composition at Salamanca, a highly industrialized urban area of Central Mexico. Samples were collected at six sites within the urban area during February and March 2003. Several trace elements, organic carbon (OC), elemental carbon (EC), and six ions were analyzed to characterize aerosols. Average concentrations of PM with aerodynamic diameter of less than 10 microm (PM10) and fine PM with aerodynamic diameter of less than 2.5 microm (PM2.5) ranged from 32.2 to 76.6 [g m(-3) and 11.1 to 23.7 microg m(-3), respectively. OC (34%), SO4= (25.1%), EC (12.9%), and geological material (12.5%) were the major components of PM2.5. For PM10 geological material (57.9%), OC (17.3%), and SO4= (9.7%) were the major components. Coarse fraction (PM,, -PM2.5), geological material (81.7%), and OC (8.6%) were the dominant species, which amounted to 90.4%. Correlation analysis showed that sulfate in PM2.5 was present as ammonium sulfate. Sulfate showed a significant spatial variation with higher concentrations to the north resulting from predominantly southwesterly winds above the surface layer and by major SO2 sources that include a power plant and refinery. At the urban site of Cruz Roja it was observed that PM2.5 mass concentrations were similar to the submicron fraction concentrations. Furthermore, the correlation between EC in PM2.5 and EC measured from an aethalometer was r(2) = 0.710. Temporal variations of SO2 and nitrogen oxide were observed during a day when the maximum concentration of PM2.5 was measured, which was associated with emissions from the nearby refinery and power plant. From cascade impactor measurements, the three measured modes of airborne particles corresponded with diameters of 0.32, 1.8, and 5.6 microm.     

PM source identification at Sunland Park, New Mexico, using a simple heuristic meteorological and chemical analysis

The causes for evening low-wind PM10 and PM2.5 peaks at Sunland Park, NM, were investigated by using wind sector analysis and by assessing relationships between PM loadings and meteorological parameters through canonical ordination analysis. Both PM10 and PM2.5 concentrations during the evening hours accounted for approximately 50% of their respective 24-hr averages, and the PM10 was mainly composed of coarse material (PM10-2.5 amounted to 77% of PM10). A wind sector analysis based on data from three surface meteorological monitoring stations in the region narrowed the potential source region for PM10 and PM2.5 to an area within a few kilometers south of Sunland Park. Canonical ordination analysis confirmed that the peak frequently occurred under stable conditions with weak southerly winds. Chemical analyses of PM showed that elemental and organic carbon (EC and OC, respectively) dominate PM2.5 and inorganic elements dominate PM10-2.5. The combined data for EC/OC, geologic elements, and various trace elements indicate that under low wind and stable conditions, traffic-related PM emissions (motor vehicle exhausts and re-suspended road dust) from the south of the site are the most likely sources for the evening PM10 and PM2.5 peaks.     

Multi-year hourly PM2.5 carbon measurements in New York: Diurnal,day of week and seasonal patterns

Multi-year hourly measurements of PM_2.5 elemental carbon (EC) and organic carbon (OC) from a site in the South Bronx, New York were used to examine diurnal, day of week and seasonal patterns. The hourly carbon measurements also provided temporally resolved information on sporadic EC spikes observed predominantly in winter. Furthermore, hourly EC and OC data were used to provide information on secondary organic aerosol formation. Average monthly EC concentrations ranged from 0.5 to 1.4 μg m^?3 with peak hourly values of several μg m^?3 typically observed from November to March. Mean EC concentrations were lower on weekends (approximately 27% lower on Saturday and 38% lower on Sunday) than on weekdays (Monday to Friday). The weekday/weekend difference was more pronounced during summer months and less noticeable during winter. Throughout the year EC exhibited a similar diurnal pattern to NO_x showing a pronounced peak during the morning commute period (7–10 AM EST). These patterns suggest that EC was impacted by local mobile emissions and in addition by emissions from space heating sources during winter months. Although EC was highly correlated with black carbon (BC) there was a pronounced seasonal BC/EC gradient with summer BC concentrations approximately a factor of 2 higher than EC. Average monthly OC concentrations ranged from 1.0 to 4.1 μg m^?3 with maximum hourly concentrations of 7–11 μg m^?3 predominantly in summer or winter months. OC concentrations generally correlated with PM_2.5 total mass and aerosol sulfate and with NO_x during winter months. OC showed no particular day of week pattern. The OC diurnal pattern was typically different than EC except in winter when OC tracked EC and NO_x indicating local primary emissions contributed significantly to OC during winter at the urban location. On average secondary organic aerosol was estimated to account for 40–50% of OC during winter and up to 63–73% during summer months.     

Driver exposure to particulate matter in Bangkok

The aims of this study were to determine the particulate matter with aerodynamic diameters > or = 2.5 microm (PM2.5) and 2.5-10 microm (PM10-2.5) exposure levels of drivers and to analyze the proportion of elemental carbon (EC) and organic carbon (OC) in PM2.5 in Bangkok, Thailand. Four bus routes were selected. Measurements were conducted over 10 days in August (rainy season) 2008 and 8 days in January (dry season) 2009. The mean PM2.5 exposure level of the Tuk-tuk drivers was 86 microg/m3 in August and 198 microg/m3 in January. The mean for the non-air-conditioned bus drivers was 63 microg/m3 in August and 125 microg/m3 in January. The PM2.5 and PM10-2.5 exposure levels of the drivers in January were approximately twice as high as those in August. The proportion of total carbon (TC) in PM2.5 to the PM2.5 level in August (0.97 +/- 0.28 microg/m3) was higher than in January (0.65 +/- 0.13 microg/m3). The proportion of OC in the TC of the PM2.5 in August (0.51 +/- 0.08 microg/m3) was similar to that in January (0.65 +/- 0.07 microg/m3). The TC exposure by PM25 in January (81 +/- 30 microg/m3) remained higher than in August (56-21 microg/m3). The mean level of OC in the PM2.5 was 29 +/- 13 microg/m3 in August and 50 +/- 24 microg/m3 in January. In conclusion, the PM exposure level in Bangkok drivers was higher than that in the general environment, which was already high, and it varied with the seasons and vehicle type. This study also demonstrated that the major component of the PM was carbon, likely derived from vehicles.     

Chemical characterization and factor analysis of PM2.5 in two sites of Monterrey, Mexico

The Monterrey Metropolitan Area (MMA) has shown a high concentration of PM2.5 in its atmosphere since 2003. The contribution of possible sources of primary PM2.5 and its precursors is not known. In this paper we present the results of analyzing the chemical composition of sixty 24-hr samples of PM2.5 to determine possible sources of PM2.5 in the MMA. The samples were collected at the northeast and southeast of the MMA between November 22 and December 12, 2007, using low-volume devices. Teflon and quartz filters were used to collect the samples. The concentrations of 16 airborne trace elements were determined using x-ray fluorescence (XRF). Anions and cations were determined using ion chromatography. Organic carbon (OC) and elemental carbon (EC) were determined by thermal optical analysis. The results show that Ca had the maximum mean concentration of all elements studied, followed by S. Enrichment factors above 50 were calculated for S, Cl, Cu, Zn, Br and Pb. This indicates that these elements may come from anthropogenic sources. Overall, the major average components of PM2.5 were OC (41.7%), SO4(2-) (22.9%), EC (7.4%), crustal material (11.4%), and NO3- (12.6%), which altogether accounted for 96% of the mass. Statistically, we did not find any difference in SO4(2-) concentrations between the two sites. The fraction of secondary organic carbon was between 24% and 34%. The results of the factor analysis performed over 10 metals and OC and EC show that there are three main sources of PM2.5: crustal material and vehicle exhaust; industrial activity; and fuel oil burning. The results show that SO4(2-), OC, and crustal material are important components of PM2.5 in MMA. Further work is necessary to evaluate the proportion of secondary inorganic and organic aerosol in order to have a better understanding of the sources and precursors of aerosols in the MMA.     

Characterization of particulate matter for three sites in Kuwait

Many studies have shown strong associations between particulate matter (PM) levels and a variety of health outcomes, leading to changes in air quality standards in many regions, especially the United States and Europe. Kuwait, a desert country located on the Persian Gulf, has a large petroleum industry with associated industrial and urban land uses. It was marked by environmental destruction from the 1990 Iraqi invasion and subsequent oil fires. A detailed particle characterization study was conducted over 12 months in 2004-2005 at three sites simultaneously with an additional 6 months at one of the sites. Two sites were in urban areas (central and southern) and one in a remote desert location (northern). This paper reports the concentrations of particles less than 10 microm in diameter (PM10) and fine PM (PM2.5), as well as fine particle nitrate, sulfate, elemental carbon (EC), organic carbon (OC), and elements measured at the three sites. Mean annual concentrations for PM10 ranged from 66 to 93 microg/m3 across the three sites, exceeding the World Health Organization (WHO) air quality guidelines for PM10 of 20 microg/m3. The arithmetic mean PM2.5 concentrations varied from 38 and 37 microg/m3 at the central and southern sites, respectively, to 31 microg/m3 at the northern site. All sites had mean PM2.5 concentrations more than double the U.S. National Ambient Air Quality Standard (NAAQS) for PM2.5. Coarse particles comprised 50-60% of PM10. The high levels of PM10 and large fraction of coarse particles comprising PM10 are partially explained by the resuspension of dust and soil from the desert crust. However, EC, OC, and most of the elements were significantly higher at the urbanized sites, compared with the more remote northern site, indicating significant pollutant contributions from local mobile and stationary sources. The particulate levels in this study are high enough to generate substantial health impacts and present opportunities for improving public health by reducing airborne PM.     

Characterization of carbonaceous species of ambient PM2.5 in Beijing, China

One-week integrated fine particulate matter (i.e., particles <2.5 microm in diameter; PM2.5) samples were collected continuously with a low-flow rate sampler at a downtown site (Chegongzhuang) and a residential site (Tsinghua University) in Beijing between July 1999 and June 2000. The annual average concentrations of organic carbon (OC) and elemental carbon (EC) at the urban site were 23.9 and 8.8 microg m(-3), much higher than those in some cities with serious air pollution. Similar weekly variations of OC and EC concentrations were found for the two sampling sites with higher concentrations in the winter and autumn. The highest weekly variations of OC and EC occurred in the winter, suggesting that combustion sources for space heating were important contributors to carbonaceous particles, along with a significant impact from variable meteorological conditions. High emissions coupled with unfavorable meteorological conditions led to the max weekly carbonaceous concentration the week of November 18-25, 1999. The weekly mass ratios of OC:EC ranged between 2 and 4 for most samples and averaged 2.9, probably suggesting that secondary OC (SOC) is present most weeks. The range of contemporary carbon fraction, based on the C14 analyses of eight samples collected in 2001, is 0.330-0.479. Estimated SOC accounted for approximately 38% of the total OC at the two sites. Average OC and EC concentrations at Tsinghua University were 25% and 18%, respectively, higher than those at Chegongzhuang, which could be attributed to different local emissions of primary carbonaceous particles and gaseous precursors of SOC, as well as different summer photochemical intensities between the two locations.     

Current status of air quality models for particulate matter.

The current status of the mathematical modeling of atmospheric particulate matter (PM) is reviewed in this paper. Simulating PM requires treating various processes, including the formation of condensable species, the gas/ particle partitioning of condensable compounds, and in some cases, the evolution of the particle size distribution. The algorithms available to simulate these processes are reviewed and discussed. Eleven 3-dimensional (3-D) Eulerian air quality models for PM are reviewed in terms of their formulation and past applications. Results of past performance evaluations of 3-D Eulerian PM models are presented. Currently, 24-hr average PM2.5 concentrations appear to be predicted within 50% for urban-scale domains. However, there are compensating errors among individual particulate species. The lowest errors tend to be associated with SO4(2-), while NO3-, black carbon (BC), and organic carbon (OC) typically show larger errors due to uncertainties in emissions inventories and the prediction of the secondary OC fraction. Further improvements and performance evaluations are recommended.     

Chemical composition of PM10 and PM2.5 collected at ground level and 100 meters during a strong winter-time pollution episode in Xi'an, China

An intensive sampling of aerosol particles from ground level and 100 m was conducted during a strong pollution episode during the winter in Xi'an, China. Concentrations of water-soluble inorganic ions, carbonaceous compounds, and trace elements were determined to compare the composition of particulate matter (PM) at the two heights. PM mass concentrations were high at both stations: PM10 (PM with aerodynamic diameter < or =10 microm) exceeded the China National Air Quality Standard Class II value on three occasions, and PM2.5 (PM with aerodynamic diameter < or =2.5 microm) exceeded the daily U.S. National Ambient Air Quality Standard more than 10 times. The PM10 organic carbon (OC) and elemental carbon (EC) were slightly lower at the ground than at 100 m, both in terms of concentration and percentage of total mass, but OC and EC in PM2.5 exhibited the opposite pattern. Major ionic species, such as sulfate and nitrate, showed vertical variations similar to the carbonaceous aerosols. High sulfate concentrations indicated that coal combustion dominated the PM mass both at the ground and 100 m. Correlations between K+ and OC and EC at 100 m imply a strong influence from suburban biomass burning, whereas coal combustion and motor vehicle exhaust had a greater influence on the ground PM. Stable atmospheric conditions apparently led to the accumulation of PM, especially at 100 m, and these conditions contributed to the similarities in PM at the two elevations. Low coefficient of divergence (CD) values reflect the similarities in the composition of the aerosol between sites, but higher CDs for fine particles compared with coarse ones were consistent with the differences in emission sources between the ground and 100 m.     

Chemical composition of post-harvest biomass burning aerosols in Gwangju, Korea

The main objective of this study was to investigate the chemical characteristics of post-harvest biomass burning aerosols from field burning of barley straw in late spring and rice straw in late fall in rural areas of Korea. A 12-hr integrated intensive sampling of particulate matter (PM) with an aerodynamic diameter less than or equal to 10 microm (PM10) and PM with an aerodynamic diameter less than or equal to 2.5 microm (PM2.5) biomass burning aerosols had been conducted continuously in Gwangju, Korea, during two biomass burning periods: June 4--15, 2001, and October 8--November 14, 2002. The fine and coarse particles of biomass burning aerosols were analyzed for mass and ionic, elemental, and carbonaceous species. The average fine and coarse mass concentrations of biomass burning aerosols were, respectively, 129.6 and 24.2 microg/m3 in June 2001 and 47.1 and 33.2 microg/m3 in October--November 2002. An exceptionally high PM2.5 concentration of 157.8 microg/m3 was observed during biomass burning events under stagnant atmospheric conditions. In the fine mode, chlorine and potassium were unusually rich because of the high content of semi-arid vegetation. Both organic carbon (OC) and elemental carbon increased during the biomass burning periods, with the former exhibiting a higher abundance. PM from the open field burning of agricultural waste has an adverse impact on local air quality and regional climate.     

Improving Source Apportionment of Fine Particles in the Eastern United States Utilizing Temperature-Resolved Carbon Fractions

Abstract

The objectives of this study were to examine the use of carbon fractions to identify particulate matter (PM) sources, especially traffic‐related carbonaceous particle sources, and to estimate their contributions to the particle mass concentrations. In recent studies, positive matrix factorization (PMF) was applied to ambient fine PM (PM_2.5) compositional data sets of 24‐hr integrated samples including eight individual carbon fractions collected at three monitoring sites in the eastern United States: Atlanta, GA, Washington, DC, and Brigantine, NJ. Particulate carbon was analyzed using the Interagency Monitoring of Protected Visual Environments/Thermal Optical Reflectance method that divides carbon into four organic carbons (OC): pyrolized OC and three elemental carbon (EC) fractions. In contrast to earlier PMF studies that included only the total OC and EC concentrations, gasoline emissions could be distinguished from diesel emissions based on the differences in the abundances of the carbon fractions between the two sources. The compositional profiles for these two major source types show similarities among the three sites. Temperature‐resolved carbon fractions also enhanced separations of carbon‐rich secondary sulfate aerosols. Potential source contribution function analyses show the potential source areas and pathways of sulfate‐rich secondary aerosols, especially the regional influences of the biogenic, as well as anthropogenic secondary aerosol. This study indicates that temperature‐resolved carbon fractions can be used to enhance the source apportionment of ambient PM_2.5.