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1.
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.  相似文献   

2.
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.  相似文献   

3.
Compliance under the Regional Haze Rule of 1999 is based on Interagency Monitoring of Protected Visual Environments (IMPROVE) protocols for reconstructing aerosol mass and light extinction from aerosol chemical concentrations measured in the IMPROVE network. The accuracy, consistency, and potential biases in these formulations were examined using IMPROVE aerosol chemistry and light extinction data from 1988-1999. Underestimation of particulate matter with an aerodynamic diameter < 2.5 microm (PM2.5) by the IMPROVE mass reconstruction formula by 12%, on average, appears to be related to the exclusion of sodium, chlorine, and other elements and to artifacts associated with the measurement of organic carbon, but not to absorption of water by sulfates and nitrates on IMPROVE Teflon filters during weighing. Light scattering measured by transmissometry is not consistent with nephelometer scattering or single-scatter albedos expected for remote locations. Light scattering was systematically overestimated by 34%, on average, with the IMPROVE particle scattering (Bsp) reconstruction formula. The use of climatologically based hygroscopic growth factors f(RH) suggested for compliance with the Haze Rule contributes significantly to this overestimation and increases the amount of light extinction attributable to sulfates for IMPROVE samples between 1993 and 1999 by 5 percentage points.  相似文献   

4.
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.  相似文献   

5.
The [revised] IMPROVE Equation for estimating light extinction from aerosol chemical composition was evaluated considering new measurements at U.S. national parks. Compared with light scattering (Bsp) measured at seven IMPROVE sites with nephelometer data from 2003–2012, the [revised] IMPROVE Equation over- and underestimated Bsp in the lower and upper quintiles, respectively, of measured Bsp. Underestimation of the worst visibility cases (upper quintile) was reduced by assuming an organic mass (OM)/organic carbon (OC) ratio of 2.1 and hygroscopic growth of OM, based on results from previous field studies. This assumption, however, tended to overestimate low Bsp even more. Assuming that sulfate was present as ammonium bisulfate rather than as ammonium sulfate uniformly reduced estimated Bsp. The split-mode model of concentration- and size-dependent dry mass scattering efficiencies in the [revised] IMPROVE Equation does not eliminate systematic biases in estimated Bsp. While the new measurements of OM/OC and OM hygroscopicity should be incorporated into future iterations of the IMPROVE Equation, the problem is not well constrained due to a lack of routine measurements of sulfate neutralization and the water-soluble fraction of OM in the IMPROVE network.

Implications: Studies in U.S. national parks showed that aerosol organics contain more mass and absorb more water as a function of relative humidity than is currently assumed by the IMPROVE Equation for calculating chemical light extinction. Consideration of these results could significantly shift the apportionment of light extinction to water-soluble organic aerosols and therefore better inform pollution control strategies under the U.S. Environmental Protection Agency Regional Haze Rule.  相似文献   


6.
Speciated fine particulate matter (PM2.5) data collected as part of the Speciation Trends Network at four sites in the Midwest (Detroit, MI; Cincinnati, OH; Indianapolis, IN; and Northbrook, IL) and as part of the Interagency Monitoring of Protected Visual Environments program at the rural Bondville, IL, site were analyzed to understand sources contributing to organic carbon (OC) and PM2.5 mass. Positive matrix factorization (PMF) was applied to available data collected from January 2002 through March 2005, and seven to nine factors were identified at each site. Common factors at all of the sites included mobile (gasoline)/secondary organic aerosols with high OC, diesel with a high elemental carbon/OC ratio (only at the urban sites), secondary sulfate, secondary nitrate, soil, and biomass burning. Identified industrial factors included copper smelting (Northbrook, Indianapolis, and Bondville), steel/manufacturing with iron (Northbrook), industrial zinc (Northbrook, Cincinnati, Indianapolis, and Detroit), metal plating with chromium and nickel (Detroit, Indianapolis, and Bondville), mixed industrial with copper and iron (Cincinnati), and limestone with calcium and iron (Bondville). PMF results, on average, accounted for 96% of the measured PM2.5 mass at each site; residuals were consistently within tolerance (+/-3), and goodness-of-fit (Q) was acceptable. Potential source contribution function analysis helped identify regional and local impacts of the identified source types. Secondary sulfate and soil factors showed regional characteristics at each site, whereas industrial sources typically appeared to be locally influenced. These regional factors contributed approximately one third of the total PM2.5 mass, on average, whereas local mobile and industrial sources contributed to the remaining mass. Mobile sources were a major contributor (55-76% at the urban sites) to OC mass, generally with at least twice as much mass from nondiesel sources as from diesel. Regional OC associated with secondary sulfate and soil was generally low.  相似文献   

7.
The U.S. Department of Energy Gasoline/Diesel PM Split Study examined the sources of uncertainties in using an organic compound-based chemical mass balance receptor model to quantify the contributions of spark-ignition (SI) and compression-ignition (CI) engine exhaust to ambient fine particulate matter (PM2.5). This paper presents the chemical composition profiles of SI and CI engine exhaust from the vehicle-testing portion of the study. Chemical analysis of source samples consisted of gravimetric mass, elements, ions, organic carbon (OC), and elemental carbon (EC) by the Interagency Monitoring of Protected Visual Environments (IMPROVE) and Speciation Trends Network (STN) thermal/optical methods, polycyclic aromatic hydrocarbons (PAHs), hopanes, steranes, alkanes, and polar organic compounds. More than half of the mass of carbonaceous particles emitted by heavy-duty diesel trucks was EC (IMPROVE) and emissions from SI vehicles contained predominantly OC. Although total carbon (TC) by the IMPROVE and STN protocols agreed well for all of the samples, the STN/IMPROVE ratios for EC from SI exhaust decreased with decreasing sample loading. SI vehicles, whether low or high emitters, emitted greater amounts of high-molecular-weight particulate PAHs (benzo[ghi]perylene, indeno[1,2,3-cd]pyrene, and coronene) than did CI vehicles. Diesel emissions contained higher abundances of two- to four-ring semivolatile PAHs. Diacids were emitted by CI vehicles but are also prevalent in secondary organic aerosols, so they cannot be considered unique tracers. Hopanes and steranes were present in lubricating oil with similar composition for both gasoline and diesel vehicles and were negligible in gasoline or diesel fuels. CI vehicles emitted greater total amounts of hopanes and steranes on a mass per mile basis, but abundances were comparable to SI exhaust normalized to TC emissions within measurement uncertainty. The combustion-produced high-molecular-weight PAHs were found in used gasoline motor oil but not in fresh oil and are negligible in used diesel engine oil. The contributions of lubrication oils to abundances of these PAHs in the exhaust were large in some cases and were variable with the age and consumption rate of the oil. These factors contributed to the observed variations in their abundances to total carbon or PM2.5 among the SI composition profiles.  相似文献   

8.
In an effort to better quantify wintertime particulate matter (PM) and the contribution of wood smoke to air pollution events in Fresno, CA, a field campaign was conducted in winter 2003-2004. Coarse and fine daily PM samples were collected at five locations in Fresno, including residential, urban, and industrial areas. Measurements of collected samples included gravimetric mass determination, organic and elemental carbon analysis, and trace organic compound analysis by gas chromatograph mass spectrometry (GC/MS). The wood smoke tracer levoglucosan was also measured in aqueous aerosol extracts using high-performance anion exchange chromatography coupled with pulsed amperometric detection. Sample preparation and analysis by this technique is much simpler and less expensive than derivatized levoglucosan analysis by GC/MS, permitting analysis of daily PM samples from all five of the measurement locations. Analyses revealed low spatial variability and similar temporal patterns of PM2.5 mass, organic carbon (OC), and levoglucosan. Daily mass concentrations appear to have been strongly influenced by meteorological conditions, including precipitation, wind, and fog events. Fine PM (PM2.5) concentrations are uncommonly low during the study period, reflecting frequent precipitation events. During the first portion of the study, levoglucosan had a strong relationship to the concentrations of PM2.5 and OC. In the later portion of the study, there was a significant reduction in levoglucosan relative to PM2.5 and OC. This may indicate a change in particle removal processes, perhaps because of fog events, which were more common in the latter period. Combined, the emissions from wood smoke, meat cooking, and motor vehicles appear to contribute approximately 65-80% to measured OC, with wood smoke, on average, accounting for approximately 41% of OC and approximately 18% of PM2.5 mass. Two residential sites exhibit somewhat higher contributions of wood smoke to OC than other locations.  相似文献   

9.
Fine particulate matter (PM2.5) samples were simultaneously collected on Teflon and quartz filters between February 2010 and February 2011 at an urban monitoring site (CAMS2) in Dhaka, Bangladesh. The samples were collected using AirMetrics MiniVol samplers. The samples on Teflon filters were analyzed for their elemental composition by PIXE and PESA. Particulate carbon on quartz filters was analyzed using the IMPROVE thermal optical reflectance (TOR) method that divides carbon into four organic carbons (OC), pyrolized organic carbon (OP), and three elemental carbon (EC) fractions. The data were analyzed by positive matrix factorization using the PMF2 program. Initially, only total OC and total EC were included in the analysis and five sources, including road dust, sea salt and Zn, soil dust, motor vehicles, and brick kilns, were obtained. In the second analysis, the eight carbon fractions (OC1, OC2, OC3, OC4, OP, EC1, EC2, EC3) were included in order to ascertain whether additional source information could be extracted from the data. In this case, it is possible to identify more sources than with only total OC and EC. The motor vehicle source was separated into gasoline and diesel emissions and a fugitive Pb source was identified. Brick kilns contribute 7.9 μg/m3 and 6.0 μg/m3 of OC and EC, respectively, to the fine particulate matter based on the two results. From the estimated mass extinction coefficients and the apportioned source contributions, soil dust, brick kiln, diesel, gasoline, and the Pb sources were found to contribute most strongly to visibility degradation, particularly in the winter.

Implications: Fine particle concentrations in Dhaka, Bangladesh, are very high and cause significant degradation of urban visibility. This work shows that using carbon fraction data from the IMPROVE OC/EC protocol provides improved source apportionment. Soil dust, brick kiln, diesel, gasoline, and the Pb sources contribute strongly to haze, particularly in the winter.  相似文献   

10.
Seasonal elemental carbon (EC) and organic carbon (OC) concentration levels in PM2.5 samples collected in Milan (Italy) are presented and discussed, enriching the world-wide database of carbonaceous species in fine particulate matter (PM). High-volume PM2.5 sampling campaigns were performed from August 2002 through December 2003 in downtown Milan at an urban background site. Compared to worldwide average concentrations, in Milan warm-season OC and both warm- and cold-season EC are relatively low; conversely, cold-season OC concentrations are rather high. Consequently, high values for the OC/EC ratio are observed, especially in the winter period. The relation between OC/EC ratio values and wind direction is investigated, pointing out that the highest ratios are associated to winds blowing from those nearby areas where wood consumption for domestic heating is larger. Information on the OC partitioning between its primary and secondary fraction are derived by means of the EC-tracer method and principal component analysis. In the warm-season, OC is mainly of secondary origin, secondary organic aerosol (SOA) accounting for about 84% of the particulate organic matter and 25–28% of the PM2.5 mass. For the cold season the full application of the EC-tracer method was not possible and the primary organic aerosol deriving from traffic could only be estimated. However, principal component analysis (PCA) suggest a prevailing primary origin for OC, thus raising the attention on space heating emissions, and on wood combustion in particular, for air quality control. The role of traffic emissions on PM2.5 concentration levels, as a primary source, are also assessed: EC and primary organic matter from traffic account for a warm-season 30% and a cold-season 7% of the total carbon in PM2.5, that is for about 10% and 6% of PM2.5 mass, respectively. This latter small primary contribution estimated for the cold-season points out that stationary sources, which were not thought to play a significant role on PM concentration levels, may conversely be as much responsible for ambient particulate pollution.  相似文献   

11.
Evaporative loss of particulate matter (with aerodynamic diameter < 2.5 microm, [PM2.5]) ammonium nitrate from quartz-fiber filters during aerosol sampling was evaluated from December 3, 1999, through February 3, 2001, at two urban (Fresno and Bakersfield) and three nonurban (Bethel Island, Sierra Nevada Foothills, and Angiola) sites in central California. Compared with total particulate nitrate, evaporative nitrate losses ranged from < 10% during cold months to > 80% during warm months. In agreement with theory, evaporative loss from quartz-fiber filters in nitric acid denuded samplers is controlled by the ambient nitric acid-to-particulate nitrate ratio, which is determined mainly by ambient temperature. Accurate estimation of nitrate volatilization requires a detailed thermodynamic model and comprehensive chemical measurements. For the 14-month average of PM2.5 acquired on Teflon-membrane filters, measured PM2.5 mass was 8-16% lower than actual PM2.5 mass owing to nitrate volatilization. For 24-hr samples, measured PM2.5 was as much as 32-44% lower than actual PM2.5 at three California Central Valley locations.  相似文献   

12.
The primary emission source contributions to fine organic carbon (OC) and fine particulate matter (PM2.5) mass concentrations on a daily basis in Atlanta, GA, are quantified for a summer (July 3 to August 4, 2001) and a winter (January 2-31, 2002) month. Thirty-one organic compounds in PM2.5 were identified and quantified by gas chromatography/mass spectrometry. These organic tracers, along with elemental carbon, aluminum, and silicon, were used in a chemical mass balance (CMB) receptor model. CMB source apportionment results revealed that major contributors to identified fine OC concentrations include meat cooking (7-68%; average: 36%), gasoline exhaust (7-45%; average: 21%), and diesel exhaust (6-41%; average: 20%) for the summer month, and wood combustion (0-77%; average: 50%); gasoline exhaust (14-69%; average: 33%), meat cooking (1-14%; average: 5%), and diesel exhaust (0-13%; average: 4%) for the winter month. Primary sources, as well as secondary ions, including sulfate, nitrate, and ammonium, accounted for 86 +/- 13% and 112 +/- 15% of the measured PM2.5 mass in summer and winter, respectively.  相似文献   

13.
Han Y  Cao J  An Z  Chow JC  Watson JG  Jin Z  Fung K  Liu S 《Chemosphere》2007,69(4):526-533
The IMPROVE thermal/optical reflectance (TOR) method, commonly used for EC quantification in atmospheric aerosols, is applied to soils and sediments and compared with a thermochemical method commonly applied to these non-atmospheric samples. TOR determines elemental carbon (EC) by an optical method, but it also yields thermally defined EC fractions in a 2% O2/98% He oxidizing atmosphere at 550 degrees C (EC1), 700 degrees C (EC2), and 800 degrees C (EC3). Replicate TOR TC, OC, and EC values exhibited precisions of approximately +/-10% as determined from multiple analyses of the same samples. EC abundances relative to total mass concentrations were within the ranges reported by other methods for diesel exhaust soot, n-hexane soot, wood and rice chars, and coals, as well as for environmental matrices. A direct comparison with the chemothermal (CTO) method of Gustafson et al. for ten soil and sediment samples demonstrated that almost all of the OC and EC1 are eliminated, as is part of the EC2. The CTO soot carbon is bounded by the EC3 and EC2+EC3 fractions of the IMPROVE TOR analysis. It might be possible to adjust these fractions to obtain better agreement between atmospheric aerosol and soil/sediment analysis methods. Given its linking the EC measurement in the atmosphere to sediments, the TOR method will not only provide useful information on the explanation and comparison between different environmental matrices, but also can be used to derive information on global cycling of EC.  相似文献   

14.
Systematic measurement of fine particulate matter (aerodynamic diameter less than 2.5 microm [PM2.5]) mass concentrations began nationally with implementation of the Federal Reference Method (FRM) network in 1998 and 1999. In California, additional monitoring of fine particulate matter (PM) occurred via a dichotomous sampler network and several special studies carried out between 1982 and 2002. The authors evaluate the comparability of FRM and non-FRM measurements of PM2.5 mass concentrations and establish conversion factors to standardize fine mass measurements from different methods to FRM-equivalent concentrations. The authors also identify measurements of PM2.5 mass concentrations that do not agree with FRM or other independent PM2.5 mass measurements. The authors show that PM2.5 mass can be reconstructed to a high degree of accuracy (r2 > 0.9; mean absolute error approximately 2 microg m(-3)) from PM with an aerodynamic diameter < or =10 microm (PM10) mass and species concentrations when site-specific and season-specific conversion factors are used and a statewide record of fine PM mass concentrations by combining the FRM PM2.5 measurements, non-FRM PM2.5 measurements, and reconstructions of PM2.5 mass concentrations. Trends and spatial variations are evaluated using the integrated data. The rates of change of annual fine PM mass were negative (downward trends) at all 22 urban and 6 nonurban (Interagency Monitoring of Protected Visual Environments [IMPROVE]) monitoring locations having at least 15 yr of data during the period 1980-2007. The trends at the IMPROVE sites ranged from -0.05 to -0.25 microg m(-3) yr(-1) (median -0.11 microg m(-3) yr(-1)), whereas urban-site trends ranged from -0.13 to -1.29 microg m(-3) yr(-1) (median -0.59 microg m(-3) yr(-1)). The urban concentrations declined by a factor of 2 over the period of record, and these decreases were qualitatively consistent with changes in emissions of primary PM2.5 and gas-phase precursors of secondary PM. Mean PM2.5 mass concentrations ranged from 3.3 to 7.4 microg m(-3) at IMPROVE sites and from 9.3 to 37.1 microg m(-3) at urban sites.  相似文献   

15.
This study evaluates the effect of retrofit closed crankcase ventilation filters (CCFs) and diesel oxidation catalysts (DOCs) on the in-cabin air quality in transit-style diesel school buses. In-cabin pollution levels were measured on three buses from the Pueblo, CO District 70 fleet. Monitoring was conducted while buses were driven along their regular routes, with each bus tested three times before and three times after installation of control devices. Ultrafine number concentrations in the school bus cabins were 33–41% lower, on average, after the control devices were installed. Mean mass concentrations of particulate matter less than 2.5 μm in diameter (PM2.5) were 56% lower, organic carbon (OC) 41% lower, elemental carbon (EC) 85% lower, and formaldehyde 32% lower after control devices were installed. While carbon monoxide concentrations were low in all tests, mean concentrations were higher after control devices were installed than in pre-retrofit tests. Reductions in number, OC, and formaldehyde concentrations were statistically significant, but reductions in PM2.5 mass were not. Even with control devices installed, during some runs PM2.5 and OC concentrations in the bus cabins were elevated compared to ambient concentrations observed in the area. OC concentrations inside the bus cabins ranged from 22 to 58 μg m?3 before and 13 to 33 μg m?3 after control devices were installed. OC concentrations were correlated with particle-bound organic tracers for lubricating oil emissions (hopanes) and diesel fuel and tailpipe emissions (polycyclic aromatic hydrocarbons (PAH) and aliphatic hydrocarbons). Mean concentrations of hopanes, PAH, and aliphatic hydrocarbons were lower by 37, 50, and 43%, respectively, after the control devices were installed, suggesting that both CCFs and DOCs were effective at reducing in-cabin OC concentrations.  相似文献   

16.
Abstract

In an effort to better quantify wintertime particulate matter (PM) and the contribution of wood smoke to air pollution events in Fresno, CA, a field campaign was conducted in winter 2003–2004. Coarse and fine daily PM samples were collected at five locations in Fresno, including residential, urban, and industrial areas. Measurements of collected samples included gravimetric mass determination, organic and elemental carbon analysis, and trace organic compound analysis by gas chromatograph mass spectrometry (GC/MS). The wood smoke tracer levoglucosan was also measured in aqueous aerosol extracts using high-performance anion exchange chromatography coupled with pulsed amperometric detection. Sample preparation and analysis by this technique is much simpler and less expensive than derivatized levoglucosan analysis by GC/MS, permitting analysis of daily PM samples from all five of the measurement locations. Analyses revealed low spatial variability and similar temporal patterns of PM2.5 mass, organic carbon (OC), and levoglucosan. Daily mass concentrations appear to have been strongly influenced by meteorological conditions, including precipitation, wind, and fog events. Fine PM (PM2.5) concentrations are uncommonly low during the study period, reflecting frequent precipitation events. During the first portion of the study, levoglucosan had a strong relationship to the concentrations of PM2.5 and OC. In the later portion of the study, there was a significant reduction in levoglucosan relative to PM2.5 and OC. This may indicate a change in particle removal processes, perhaps because of fog events, which were more common in the latter period. Combined, the emissions from wood smoke, meat cooking, and motor vehicles appear to contribute ~65–80% to measured OC, with wood smoke, on average, accounting for ~41% of OC and ~18% of PM2.5 mass. Two residential sites exhibit somewhat higher contributions of wood smoke to OC than other locations.  相似文献   

17.
To investigate the chemical characteristics of fine particles in the Sihwa area, Korea, atmospheric aerosol samples were collected using a dichotomous PM10 sampler and two URG PM2.5 cyclone samplers during five intensive sampling periods between February 1998 and February 1999. The Inductively Coupled Plasma (ICP)-Atomic Emission Spectrometry (AES)/ICP-Mass Spectrometry (MS), ion chromatograph (IC), and thermal manganese dioxide oxidation (TMO) methods were used to analyze the trace elements, ionic species, and carbonaceous species, respectively. Backward trajectory analysis, factor analysis, and a chemical mass balance (CMB) model were used to estimate quantitatively source contributions to PM2.5 particles collected in the Sihwa area. The results of PM2.5 source apportionment using the CMB7 receptor model showed that (NH4)2SO4 was, on average, the major contributor to PM2.5 particles, followed by nontraffic organic carbon (OC) emission, NH4NO3, agricultural waste burning, motor vehicle emission, road dust, waste incineration, marine aerosol, and others. Here, the nontraffic OC sources include primary anthropogenic OC emitted from the industrial complex zone, secondary OC, and organic species from distant sources. The source impact of waste incineration emission became significant when the dominant wind directions were from southwest and west sectors during the sampling periods. It was found that PM2.5 particles in the Sihwa area were influenced mainly by both anthropogenic local sources and long-range transport and transformation of air pollutants.  相似文献   

18.
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.  相似文献   

19.
Thermally derived carbon fractions including organic carbon (OC) and elemental carbon (EC) have been reported for the U.S. Interagency Monitoring of PROtected Visual Environments (IMPROVE) network since 1987 and have been found useful in source apportionment studies and to evaluate quartz-fiber filter adsorption of organic vapors. The IMPROVE_A temperature protocol defines temperature plateaus for thermally derived carbon fractions of 140 degrees C for OC1, 280 degrees C for OC2, 480 degrees C for OC3, and 580 degrees C for OC4 in a helium (He) carrier gas and 580 degrees C for EC1, 740 degrees C for EC2, and 840 degrees C for EC3 in a 98% He/2% oxygen (O2) carrier gas. These temperatures differ from those used previously because new hardware used for the IMPROVE thermal/optical reflectance (IMPROVE_TOR) protocol better represents the sample temperature than did the old hardware. A newly developed temperature calibration method demonstrates that these temperatures better represent sample temperatures in the older units used to quantify IMPROVE carbon fractions from 1987 through 2004. Only the thermal fractions are affected by changes in temperature. The OC and EC by TOR are insensitive to the change in temperature protocol, and therefore the long-term consistency of the IMPROVE database is conserved. A method to detect small quantities of O2 in the pure He carrier gas shows that O2 levels above 100 ppmv also affect the comparability of thermal carbon fractions but have little effect on the IMPROVE_TOR split between OC and EC.  相似文献   

20.
Ambient particulates of PM2.5 were sampled at three sites in Kaohsiung, Taiwan, during February and March 1999. In addition, resuspended PM2.5 collected from traffic tunnels, paved roads, fly ash of a municipal solid waste (MSW) incinerator, and seawater was obtained. All the samples were analyzed for twenty constituents, including water-soluble ions, organic carbon (OC), elemental carbon (EC), and metallic elements. In conjunction with local source profiles and the source profiles in the model library SPECIATE EPA, the receptor model based on chemical mass balance (CMB) was then applied to determine the source contributions to ambient PM2.5. The mean concentration of ambient PM2.5 was 42.69-53.68 micrograms/m3 for the sampling period. The abundant species in ambient PM2.5 in the mass fraction for three sites were OC (12.7-14.2%), SO4(2-) (12.8-15.1%), NO3- (8.1-10.3%), NH4+ (6.7-7.5%), and EC (5.3-8.5%). Results of CMB modeling show that major pollution sources for ambient PM2.5 are traffic exhaust (18-54%), secondary aerosols (30-41% from SO4(2-) and NO3-), and outdoor burning of agriculture wastes (13-17%).  相似文献   

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