Carbonaceous aerosol characteristics in outdoor and indoor environments of Nanchang, China, during summer 2009

A study of carbonaceous aerosol was initiated in Nanchang, a city in eastern China, for the first time. Daily and diurnal (daytime and nighttime) PM2.5 (particulate matter with aerodynamic diameter < or =2.5 microm) samples were collected at an outdoor site and in three different indoor environments (common office, special printing and copying office, and student dormitory) in a campus of Nanchang University during summer 2009 (5-20 June). Daily PM10 (particulate matter with aerodynamic diameter < or =10 microm) samples were collected only at the outdoor site, whereas PM2.5 samples were collected at both indoor and outdoor sites. Loaded PM2.5 and PM10 samples were analyzed for organic and elemental carbon (OC, EC) by thermal/optical reflectance following the Interagency Monitoring of Protected Visual Environments-Advanced (IMPROVE-A) protocol. Ambient mass concentrations of PM10 and PM2.5 in Nanchang were compared with the air quality standards in China and the United States, and revealed high air pollution levels in Nanchang. PM2.5 accounted for about 70% of PM10, but the ratio of OC and EC in PM2.5 to that in PM10 was higher than 80%, which indicated that OC and EC were mainly distributed in the fine particles. The variations of carbonaceous aerosol between daytime and nighttime indicated that OC was released and formed more rapidly in daytime than in nighttime. OC/EC ratios were used to quantify secondary organic carbon (SOC). The differences in SOC and SOC/OC between daytime and nighttime were useful in interpreting the secondary formation mechanism. The results of (1) OC and EC contributions to PM2.5 at indoor sites and the outdoor site; (2) indoor-outdoor correlation of OC and EC; (3) OC-EC correlation; and (4) relative contributions of indoor and outdoor sources to indoor carbonaceous aerosol indicated that OC indoor sources existed in indoor sites, with the highest OC emissions in I2 (the special printing and copying office), and that indoor EC originated from outdoor sources. The distributions of eight carbon fractions in emissions from the printer and copier showed obviously high OC1 (>20%) and OC2 (approximately 30%), and obviously low EC1-OP (a pyrolyzed carbon fraction) (<10%), when compared with other sources.     

Sources of atmospheric carbonaceous particulate matter in Pittsburgh,Pennsylvania

The organic carbon (OC)/elemental carbon (EC) tracer method is applied to the Pittsburgh, PA, area to estimate the contribution of secondary organic aerosol (SOA) to the monthly average concentration of organic particulate matter (PM) during 1995. An emissions inventory is constructed for the primary emissions of OC and EC in the area of interest. The ratio of primary emissions of OC to those of EC ranges between 2.4 in the winter months and 1.0 in the summer months. A mass balance model and ambient measurements were used to assess the accuracy of the emissions inventory. It is estimated to be accurate to within 50%. The results from this analysis show a strong monthly dependence of the SOA contribution to the total organic PM concentration, varying from near zero during winter months to as much as 50% of the total OC concentration in the summer.     

Hourly measurements of fine particulate sulfate and carbon aerosols at the Harvard-U.S. Environmental Protection Agency Supersite in Boston

Hourly concentrations of ambient fine particle sulfate and carbonaceous aerosols (elemental carbon [EC], organic carbon [OC], and black carbon [BC]) were measured at the Harvard-U.S. Environmental Protection Agency Supersite in Boston, MA, between January 2007 and October 2008. These hourly concentrations were compared with those made using integrated filter-based measurements over 6-day or 24-hr periods. For sulfate, the two measurement methods showed good agreement. Semicontinuous measurements of EC and OC also agreed (but not as well as for sulfate) with those obtained using 24-hr integrated filter-based and optical BC reference methods. During the study period, 24-hr PM2.5 (particulate matter [PM] < or = 2.5 microm in aerodynamic diameter) concentrations ranged from 1.4 to 37.6 microg/m3, with an average of 9.3 microg/m3. Sulfate as the equivalent of ammonium sulfate accounted for 39.1% of the PM2.5 mass, whereas EC and OC accounted for 4.2 and 35.2%, respectively. Hourly sulfate concentrations showed no distinct diurnal pattern, whereas hourly EC and BC concentrations peaked during the morning rush hour between 7:00 and 9:00 a.m. OC concentrations also exhibited nonpronounced, small peaks during the day, most likely related to traffic, secondary organic aerosol, and local sources, respectively.     

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.     

Carbonaceous aerosol over a Pinus taeda forest in Central North Carolina,USA

Organic aerosol is the least understood component of ambient fine particulate matter (PM_2.5). In this study, organic and elemental carbon (OC and EC) within ambient PM_2.5 over a three-year period at a forested site in the North Carolina Piedmont are presented. EC exhibited significant weekday/weekend effects and less significant seasonal effects, in contrast to OC, which showed strong seasonal differences and smaller weekend/weekday effects. Summer OC concentrations are about twice as high as winter concentrations, while EC was somewhat higher in the winter. OC was highly correlated with EC during cool periods when both were controlled by primary combustion sources. This correlation decreased with increasing temperature, reflecting higher contributions from secondary organic aerosol, likely of biogenic origin. PM_2.5 radiocarbon data from the site confirms that a large fraction of the carbon in PM_2.5 is indeed of biogenic origin, since modern (non-fossil fuel derived) carbon accounted for 80% of the PM_2.5 carbon over the course of a year. OC and EC exhibited distinct diurnal profiles, with summertime OC peaking in late evening and declining until midday. During winter, OC peaked during the early morning hours and again declined until midday. Summertime EC peaked during late morning hours except on weekends. Wintertime EC often peaked in late PM or early AM hours due to local residential wood combustion emissions. The highest short term peaks in OC and EC were associated with wildfire events. These data corroborate recent source apportionment studies conducted within 20 km of our site, where oxidation products of isoprene, α-pinene, and β-caryophyllene were identified as important precursors to organic aerosols. A large fraction of the carbon in rural southeastern ambient PM_2.5 appears to be of biogenic origin, which is probably difficult to reduce by anthropogenic controls.     

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.     

Fine particulate matter source apportionment for the Chemical speciation Trends Network site at Birmingham, Alabama, using Positive Matrix Factorization

The Positive Matrix Factorization (PMF) receptor model version 1.1 was used with data from the fine particulate matter (PM2.5) Chemical Speciation Trends Network (STN) to estimate source contributions to ambient PM2.5 in a highly industrialized urban setting in the southeastern United States. Model results consistently resolved 10 factors that are interpreted as two secondary, five industrial, one motor vehicle, one road dust, and one biomass burning sources. The STN dataset is generally not corrected for field blank levels, which are significant in the case of organic carbon (OC). Estimation of primary OC using the elemental carbon (EC) tracer method applied on a seasonal basis significantly improved the model's performance. Uniform increase of input data uncertainty and exclusion of a few outlier samples (associated with high potassium) further improved the model results. However, it was found that most PMF factors did not cleanly represent single source types and instead are "contaminated" by other sources, a situation that might be improved by controlling rotational ambiguity within the model. Secondary particulate matter formed by atmospheric processes, such as sulfate and secondary OC, contribute the majority of ambient PM2.5 and exhibit strong seasonality (37 +/- 10% winter vs. 55 +/- 16% summer average). Motor vehicle emissions constitute the biggest primary PM2.5 mass contribution with almost 25 +/- 2% long-term average and winter maximum of 29 +/- 11%. PM2.5 contributions from the five identified industrial sources vary little with season and average 14 +/- 1.3%. In summary, this study demonstrates the utility of the EC tracer method to effectively blank-correct the OC concentrations in the STN dataset. In addition, examination of the effect of input uncertainty estimates on model results indicates that the estimated uncertainties currently being provided with the STN data may be somewhat lower than the levels needed for optimum modeling results.     

Fine particulate matter and visibility in the Lake Tahoe Basin: chemical characterization, trends, and source apportionment

Speciated PM2.5 (particulate matter with an aerodynamic diameter相似文献   

Source apportionment of fine particles at urban background and rural sites in the UK atmosphere

Airborne fine particulate matter (PM_2.5) has been collected at two sites in the West Midlands conurbation, UK, representing urban background and rural locations. Chemical analyses have been carried out for major anions, trace metals, total OC and EC, and for individual organic marker species including n-alkanes, hopanes, PAHs, organic acids and sterols. Source apportionment has been conducted using both a pragmatic mass closure model and the US EPA chemical mass balance (CMB) model. The pragmatic mass closure model is well able to account for the measured PM_2.5 mass in terms of chemical/source components, and the chemical mass balance model has been used to apportion the carbonaceous component of the aerosol. The dominant components of PM_2.5 at both sites are secondary inorganic (sulphate and nitrate) and carbonaceous particles. The CMB model shows the latter to arise mainly from road traffic sources, with smaller contributions from vegetative detritus, wood smoke, natural gas, coal, and dust/soil. The CMB model also identifies an important component of the organic aerosol not associated with these primary sources, which correlates very strongly with secondary organic aerosol estimated from the OC/EC ratio. The split between different automotive source types does not relate well to UK emission inventories, and may indicate that CMB source profiles from North American studies and different carbon analysis protocols may lead to erroneous conclusions.     

PM2.5 carbon measurements in two urban areas: Seoul and Kwangju,Korea

24-h PM_2.5 carbonaceous samples were collected between 27 November and 9 December 1999 in Seoul, and between 7 and 20 June 2000 in Kwangju to investigate characteristics of carbonaceous species, and the relationship between elemental carbon (EC) and Aethalometer-based black carbon (BC) measurements. 5-min PM_2.5 BC and criteria air pollutant data were also measured using the Aethalometer and ambient air monitoring system. The PM_2.5 samples were analyzed for EC and OC using a selective thermal manganese dioxide oxidation (TMO) method. The daily average EC and OC concentrations in Seoul were higher in the winter than in the summer (Atmos. Environ. 35 (2001a) 657). It was found that difference between ambient BC levels in the two cities was not directly proportional to the population ratio (∼8) or diesel traffic ratio (∼5.9) since particulate matter or BC concentration is strongly influenced by a result of varying traffic and meteorological conditions at the site. Using the primary OC/EC ratio approach, the results suggest that most of the measured OC in Kwangju is of primary origin during the summer. In Seoul, the observed OC includes additional secondary organic aerosol during the wintertime conditions. The relationship between the 24-h TMO-EC and Aethalometer BC measurements in PM_2.5 reflected very good agreement for the two urban sites, with correlation coefficients of R²=0.99 and 0.92, and BC/EC slopes of 0.93 and 1.07, respectively. It was found that comparing TMO-EC to BC at a different location in Korea, a different scaling factor was needed.     

Seasonal and spatial trends in the sources of fine particle organic carbon in Israel,Jordan, and Palestine

A study of carbonaceous particulate matter (PM) was conducted in the Middle East at sites in Israel, Jordan, and Palestine. The sources and seasonal variation of organic carbon, as well as the contribution to fine aerosol (PM_2.5) mass, were determined. Of the 11 sites studied, Nablus had the highest contribution of organic carbon (OC), 29%, and elemental carbon (EC), 19%, to total PM_2.5 mass. The lowest concentrations of PM_2.5 mass, OC, and EC were measured at southern desert sites, located in Aqaba, Eilat, and Rachma. The OC contribution to PM_2.5 mass at these sites ranged between 9.4% and 16%, with mean annual PM_2.5 mass concentrations ranging from 21 to 25 ug m^?3. These sites were also observed to have the highest OC to EC ratios (4.1–5.0), indicative of smaller contributions from primary combustion sources and/or a higher contribution of secondary organic aerosol. Biomass burning and vehicular emissions were found to be important sources of carbonaceous PM in this region at the non-southern desert sites, which together accounted for 30%–55% of the fine particle organic carbon at these sites. The fraction of measured OC unapportioned to primary sources (1.4 μgC m^?3 to 4.9 μgC m^?3; 30%–74%), which has been shown to be largely from secondary organic aerosol, is relatively constant at the sites examined in this study. This suggests that secondary organic aerosol is important in the Middle East during all seasons of the year.     

Characterization of PM(2.5) collected during broadcast and slash-pile prescribed burns of predominately ponderosa pine forests in northern Arizona

Prescribed burning, in combination with mechanical thinning, is a successful method for reducing heavy fuel loads from forest floors and thereby lowering the risk of catastrophic wildfire. However, an undesirable consequence of managed fire is the production of fine particulate matter or PM(2.5) (particles ≤2.5 μm in aerodynamic diameter). Wood-smoke particulate data from 21 prescribed burns are described, including results from broadcast and slash-pile burns. All PM(2.5) samples were collected in situ on day 1 (ignition) or day 2. Samples were analyzed for mass, polycyclic aromatic hydrocarbons (PAHs), inorganic elements, organic carbon (OC), and elemental carbon (EC). Results were characteristic of low intensity, smoldering fires. PM(2.5) concentrations varied from 523 to 8357 μg m(-3) and were higher on day 1. PAH weight percents (19 PAHs) were higher in slash-pile burns (0.21 ± 0.08% OC) than broadcast burns (0.07 ± 0.03% OC). The major elements were K, Cl, S, and Si. OC and EC values averaged 66 ± 7 and 2.8 ± 1.4% PM(2.5), respectively, for all burns studied, in good agreement with literature values for smoldering fires.     

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.     

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.     

Sampling artefacts,concentration and chemical composition of fine water-soluble organic carbon and humic-like substances in a continental urban atmospheric environment

Water-soluble organic carbon (WSOC) and atmospheric humic-like substances (HULIS) were investigated for urban PM2.5-fraction aerosol samples, which were collected with the tandem filter method on quartz fibre filters over a non-heating spring season. Sampling artefacts were of importance for all organic chemical fractions, and the back-to-front-filter concentration ratios were on average 28% for WSOC and 17% for HULIS and organic carbon (OC). The difference in the ratios indicates that the water-soluble organics play a more important role in adsorptive artefacts than the organic matter (OM) in general. The results emphasize the need for an appropriate sampling and/or correction method for measuring particulate organic substances in urban environments. The corrected atmospheric concentration of HULIS, obtained by subtracting the back-filter from the front-filter data, was on average 2 μg m⁻³; which represented 6% of the mean PM2.5 particulate mass, and it made up 45% of the secondary OC. The HULIS carbon accounted for 20% of the OC and 62% of the WSOC, while WSOC made up 32% of OC. The major element composition of HULIS, expressed in molar ratios, was C:H:O:N=22:32:10:1. The molar H/C ratio of 1.49 implies the presence of unsaturated organic compounds, although these were depleted in comparison with rural aerosol or standard fulvic acids. The molar O/C ratio of 0.47 indicates the existence of oxygenated functional groups; comparison to rural aerosol suggests that the (fresh) urban-type aerosol is less oxidized (and, therefore, less water soluble as well) than the rural one. The OM/OC mass conversion factor for the isolated (water-soluble) HULIS was derived to be 1.81. It was inferred from comparisons with published data that there are substantial differences in abundance and chemical composition of HULIS for different environments.     

Elemental and organic carbon in urban canyon and background environments in Budapest,Hungary

As part of an international research project, aerosol samples were collected by several filter-based devices on Nuclepore polycarbonate membrane, Teflon membrane and quartz fibre filters over separate daylight periods and nights, and on-line aerosol measurements were performed by TEOM and aethalometer within an urban canyon (kerbside) and at a near-city background site in Budapest, Hungary from 23 April–5 May 2002. Aerosol masses in PM2.0, PM10–2.0, PM2.5, PM10 size fractions and of TSP were determined gravimetrically; atmospheric concentrations of organic (OC) and elemental carbon (EC) for PM2.5 (or PM2.0), PM10 fractions and for TSP were measured by thermal–optical transmission method. Repeatability of the mass determination by Nuclepore filters seems to be 5–6%. Collections on Teflon filters yielded smaller mass on average by 8(±12)% than that for the Nuclepore filters. Quartz filters overestimated the PM10 mass in comparison with the Nuclepore filters due primarily to sampling artefacts on average by 10(±16)% at the kerbside. Tandem filter set-ups were utilised for correcting the sampling artefacts for OC by subtraction method. At the kerbside, the aerosol mass was made up on average of 35(±4)% of organic matter (OM) in the PM10 fraction, while the contribution of OM to the PM2.5 mass was 43(±9)%. At the background, OM also accounted for 43(±13)% of the PM2.0 mass. On average, EC made up 14(±6)%, 7(±2)% and 4.5(±1.1)% of the mass in the PM2.5, PM10 fractions and TSP, respectively, at the kerbside; while its contribution was only 2.1(±0.5)% in the PM2.0 fraction in the near-city background. Temporal variability for PM mass, OC and EC concentrations was related to road traffic, local meteorology and long-range transport of air masses. It was concluded that a direct coupling between the atmospheric concentration levels and vehicle circulation can be identified within the urban canyon, nevertheless, the local meteorology in particular and long-range transport of air masses have much more influence on the air quality than changes in the source intensity of road traffic. Concentration ratios of OC/EC were evaluated, and the amount of secondary organic aerosol (SOA) was estimated by using EC as tracer for the primary OC emissions. Mean contribution and standard deviation of the SOA to the OM in the PM2.5 size fraction at the kerbside over daylight periods and nights were of 37(±18) and 46(±16)%, respectively.     

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.     

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.     

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     

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.