Source Apportionment Of Ambient Particulate Matter Research Articles

Ambient particulate matter source apportionment using receptor modelling in European and Central Asia urban areas

This work presents the results of a PM2.5 source apportionment study conducted in urban background sites from 16 European and Asian countries. For some Eastern Europe and Central Asia cities this was the first time that quantitative information on pollution source contributions to ambient particulate matter (PM) has been performed. More than 2200 filters were sampled and analyzed by X-Ray Fluorescence (XRF), Particle-Induced X-Ray Emission (PIXE), and Inductively Coupled Plasma Mass Spectrometry (ICP-MS) to measure the concentrations of chemical elements in fine particles. Samples were also analyzed for the contents of black carbon, elemental carbon, organic carbon, and water-soluble ions. The Positive Matrix Factorization receptor model (EPA PMF 5.0) was used to characterize similarities and heterogeneities in PM2.5 sources and respective contributions in the cities that the number of collected samples exceeded 75. At the end source apportionment was performed in 11 out of the 16 participating cities. Nine major sources were identified to have contributed to PM2.5: biomass burning, secondary sulfates, traffic, fuel oil combustion, industry, coal combustion, soil, salt and “other sources”. From the averages of sources contributions, considering 11 cities 16% of PM2.5 was attributed to biomass burning, 15% to secondary sulfates, 13% to traffic, 12% to soil, 8.0% to fuel oil combustion, 5.5% to coal combustion, 1.9% to salt, 0.8% to industry emissions, 5.1% to “other sources” and 23% to unaccounted mass. Characteristic seasonal patterns were identified for each PM2.5 source. Biomass burning in all cities, coal combustion in Krakow/POL, and oil combustion in Belgrade/SRB and Banja Luka/BIH increased in Winter due to the impact of domestic heating, whereas in most cities secondary sulfates reached higher levels in Summer as a consequence of the enhanced photochemical activity. During high pollution days the largest sources of fine particles were biomass burning, traffic and secondary sulfates.

Roadside measurements of size-segregated particulate organic compounds near gasoline and diesel-dominated freeways in Los Angeles, CA

Individual organic compounds such as hopanes and steranes (originating in lube oil) and selected polycyclic aromatic compounds (PAHs) (generated via combustion) found in particulate emissions from vehicles have proven useful in source apportionment of ambient particulate matter (PM). Detailed information on the size-segregated (ultrafine and accumulation mode) chemical characteristics of organic PM during the winter season originating from a pure gasoline traffic freeway (CA-110), and a mixed-fleet freeway with the highest fraction of heavy-duty diesel vehicles in the state of California (I-710) is reported in this study. Hopanes and steranes as well as high molecular weight PAHs such as benzo(ghi)perylene (BgP) and coronene levels are found comparable near these freeways, while elemental carbon (EC) and lighter molecular weight PAHs are found much elevated near I-710 compared to CA-110. The roadway organic speciation data presented here are compared with the emission factors (EFs) measured in the Caldecott tunnel, Berkeley, CA [Phuleria, H.C., Geller, M.D., Fine, P.M., Sioutas, C., 2006. Size-resolved emissions of organic tracers from light- and heavy-duty vehicles measured in a California roadway tunnel. Environmental Science and Technology 40, 4109–4118] for light-duty vehicles (LDVs) and heavy-duty vehicles. Very good agreement is observed between CA-110 measurements and LDV EFs as well as I-710 measurements and corresponding reconstructed EFs from Caldecott tunnel for hopanes and steranes as well as heavier PAHs such as BgP and coronene. Our results, therefore, suggest that the EFs for hopanes and steranes obtained in tunnel environments, where emissions are averaged over a large vehicle-fleet, enable reliable source apportionment of ambient PM, given the overall agreement between the roadway vs tunnel concentrations of these species.

Determination of Single Particle Mass Spectral Signatures from Light-Duty Vehicle Emissions

In this study, 28 light-duty gasoline vehicles (LDV) were operated on a chassis dynamometer at the California Air Resources Board Haagen-Smit Facility in El Monte, CA. The mass spectra of individual particles emitted from these vehicles were measured using aerosol time-of-flight mass spectrometry (ATOFMS). A primary goal of this study involves determining representative size-resolved single particle mass spectral signatures that can be used in future ambient particulate matter source apportionment studies. Different cycles were used to simulate urban driving conditions including the federal testing procedure (FTP), unified cycle (UC), and the correction cycle (CC). The vehicles were selected to span a range of catalytic converter (three-way, oxidation, and no catalysts) and engine technologies (vehicles models from 1953 to 2003). Exhaust particles were sampled directly from a dilution and residence chamber system using particle sizing instruments and an ATOFMS equipped with an aerodynamic lens (UF-ATOFMS) analyzing particles between 50 and 300 nm. On the basis of chemical composition, 10 unique chemical types describe the majority of the particles with distinct size and temporal characteristics. In the ultrafine size range (between 50 and 100 nm), three elemental carbon (EC) particle types dominated, all showing distinct EC signatures combined with Ca, phosphate, sulfate, and a lower abundance of organic carbon (OC). The relative fraction of EC particle types decreased as particle size increased with OC particles becoming more prevalent above 100 nm. Depending on the vehicle and cycle, several distinct OC particle types produced distinct ion patterns, including substituted aromatic compounds and polycyclic aromatic hydrocarbons (PAH), coupled with other chemical species including ammonium, EC, nitrate, sulfate, phosphate, V, and Ca. The most likely source of the Ca and phosphate in the particles is attributed to the lubricating oil. Significant variability was observed in the chemical composition of particles emitted within the different car categories as well as for the same car operating under different driving conditions. Two-minute temporal resolution measurements provide information on the chemical classes as they evolved during the FTP cycle. The first two minutes of the cold start produced more than 5 times the number of particles than any other portion of the cycle, with one class of ultrafine particles (EC coupled with Ca, OC, and phosphate) preferentially produced. By number, the three EC with Ca classes (which also contained OC, phosphate, and sulfate) were the most abundant classes produced by the nonsmoking vehicles. The smoker category produced the highest number of particles, with the dominant classes being OC comprised of substituted monoaromatic compounds and PAHs, coupled with Ca and phosphate, thus suggesting used lubricating oil was associated with many of these particles. These studies show, by number, EC particles dominate gasoline emissions in the ultrafine size range particularlyforthe lowest emitting newer vehicles, suggesting the EC signature alone cannot be used as a unique tracer for diesels. This represents the first report of high time- and size-resolved chemical composition data showing the mixing state of nonrefractory elements in particles such as EC for vehicle emissions during dynamometer source testing.