Major Source Categories for PM2.5 in Pittsburgh using PMF and UNMIX

An objective of the Pittsburgh Air Quality Study was to determine the major sources of PM2.5 in the Pittsburgh region. Daily 24-hour averaged filter-based data were collected for 13 months, starting in July 2001, including sulfate and nitrate data from IC analysis, trace element data from ICP-MS analysis, and organic and elemental carbon from the thermal optical transmittance (TOT) method and the NIOSH thermal evolution protocol. These data were used in two source-receptor models, Unmix and PMF. Unmix, which is limited to a maximum number of seven factors, resolved six source factors, including crustal material, a regional transport factor, secondary nitrate, an iron, zinc and manganese factor, specialty steel production and processing, and cadmium. PMF, which has no limit to the number of factors, apportioned the PM2.5 mass into ten factors, including crustal material, secondary sulfate, primary OC and EC, secondary nitrate, an iron, zinc and manganese factor, specialty steel production and processing, cadmium, selenium, lead, and a gallium-rich factor. The Unmix and PMF common factors agree reasonably well, both in composition and contributions to PM2.5. To further identify and apportion the sources of PM2.5, specific OC compounds that are known markers of some sources were added to the PMF analysis. The results were similar to the original solution, except that the primary OC and EC factor split into two factors. One factor was associated with vehicles as identified by the hopanes, PAH's, and other OC compounds. The other factor had strong correlations with the OC and EC ambient data as well as wood smoke markers such as levoglucosan, syringols, and resin acids.

[1]  P. Hopke,et al.  Comparative application of multiple receptor methods to identify aerosol sources in northern Vermont. , 2001, Environmental science & technology.

[2]  Glen R. Cass,et al.  Sources of fine organic aerosol. 2. Noncatalyst and catalyst-equipped automobiles and heavy-duty diesel trucks , 1993 .

[3]  C. Davidson,et al.  Modeling the diurnal variation of nitrate during the Pittsburgh Air Quality Study , 2004 .

[4]  J. Lewtas,et al.  Source apportionment of PM2.5 at an urban IMPROVE site in Seattle, Washington. , 2003, Environmental science & technology.

[5]  Long-Path Open-Path Fourier.  Compendium of Methods for the Determination of Toxic Organic Compounds in Ambient Air , 1999 .

[6]  J. Schauer,et al.  Source Apportionment of Wintertime Gas-Phase and Particle-Phase Air Pollutants Using Organic Compounds as Tracers , 2000 .

[7]  James J. Schauer,et al.  Source apportionment of airborne particulate matter using organic compounds as tracers , 1996 .

[8]  J. C. Cabada,et al.  Sources of Atmospheric Carbonaceous Particulate Matter in Pittsburgh, Pennsylvania , 2002, Journal of the Air & Waste Management Association.

[9]  P. Hopke,et al.  Analysis of ambient particle size distributions using Unmix and positive matrix factorization. , 2004, Environmental science & technology.

[10]  Cliff I. Davidson,et al.  Pittsburgh air quality study overview , 2004 .

[11]  P. Hopke,et al.  Source Identification of Atlanta Aerosol by Positive Matrix Factorization , 2003, Journal of the Air & Waste Management Association.

[12]  B. Simoneit,et al.  Biomass burning — a review of organic tracers for smoke from incomplete combustion , 2002 .

[13]  Cliff I. Davidson,et al.  Advanced factor analysis for multiple time resolution aerosol composition data , 2004 .

[14]  Michael J. Kleeman,et al.  Measurement of Emissions from Air Pollution Sources. 1. C1 through C29 Organic Compounds from Meat Charbroiling , 1999 .

[15]  Glen R. Cass,et al.  Sources of fine organic aerosol. 1. Charbroilers and meat cooking operations , 1991 .

[16]  J. Schauer,et al.  Source apportionment of PM2.5 in the Southeastern United States using solvent-extractable organic compounds as tracers. , 2002, Environmental science & technology.

[17]  P. Hopke,et al.  Application of PSCF and CPF to PMF-Modeled Sources of PM2.5 in Pittsburgh , 2006 .

[18]  Matthew P. Fraser,et al.  Source apportionment of fine particulate matter in Houston, TX, using organic molecular markers , 2003 .

[19]  D. Dockery,et al.  An association between air pollution and mortality in six U.S. cities. , 1993, The New England journal of medicine.

[20]  P. Hopke,et al.  Atmospheric aerosol over Vermont: chemical composition and sources. , 2001, Environmental science & technology.

[21]  P. Paatero,et al.  Atmospheric aerosol over Alaska: 2. Elemental composition and sources , 1998 .

[22]  Kuruvilla John,et al.  The Regional Nature of PM2.5 Episodes in the Upper Ohio River Valley , 2004, Journal of the Air & Waste Management Association.

[23]  P. Parekh.  A study of manganese from anthropogenic emissions at a rural site in the eastern United States , 1990 .

[24]  Allen L. Robinson,et al.  Photochemical oxidation and changes in molecular composition of organic aerosol in the regional context , 2006 .

[25]  R. K. Larsen,et al.  Source apportionment of polycyclic aromatic hydrocarbons in the urban atmosphere: a comparison of three methods. , 2003, Environmental science & technology.

[26]  Christopher G. Nolte,et al.  Levoglucosan, a tracer for cellulose in biomass burning and atmospheric particles , 1999 .

[27]  J. Chow,et al.  PM2.5 chemical source profiles for vehicle exhaust, vegetative burning, geological material, and coal burning in Northwestern Colorado during 1995. , 2001, Chemosphere.

[28]  B. Simoneit.  A review of biomarker compounds as source indicators and tracers for air pollution , 1999, Environmental science and pollution research international.

[29]  P. Paatero.  Least squares formulation of robust non-negative factor analysis , 1997 .

[30]  Philip K. Hopke,et al.  A graphical diagnostic method for assessing the rotation in factor analytical models of atmospheric pollution , 2005 .

[31]  J. Schauer,et al.  Source reconciliation of atmospheric gas-phase and particle-phase pollutants during a severe photochemical smog episode. , 2002, Environmental science & technology.

[32]  J. C. Cabada,et al.  Positive and Negative Artifacts in Particulate Organic Carbon Measurements with Denuded and Undenuded Sampler Configurations Special Issue of Aerosol Science and Technology on Findings from the Fine Particulate Matter Supersites Program , 2004 .

[33]  Glen R. Cass,et al.  SOURCES OF FINE ORGANIC AEROSOL. 3. ROAD DUST, TIRE DEBRIS, AND ORGANOMETALLIC BRAKE LINING DUST: ROADS AS SOURCES AND SINKS , 1993 .

[34]  R. Burnett,et al.  Lung cancer, cardiopulmonary mortality, and long-term exposure to fine particulate air pollution. , 2002, JAMA.

[35]  Barbara J. Turpin,et al.  Species Contributions to PM2.5 Mass Concentrations: Revisiting Common Assumptions for Estimating Organic Mass , 2001 .

[36]  J. Schauer,et al.  Measurement of emissions from air pollution sources. 4. C1-C27 organic compounds from cooking with seed oils. , 2002, Environmental science & technology.

[37]  Apportionment of Ambient Primary and Secondary PM2.5 During a 2001 Summer Intensive Study at the NETL Pittsburgh Site Using PMF2 and EPA UNMIX , 2006 .

[38]  B. Simoneit,et al.  Organic Matter of the Troposphere-II. Natural Background of biogenic lipid matter in aerosols over the rural western United States ††Contribution No. 2088: Institute of Geophysics and Planetary Physics, University of California at Los Angeles. , 2007 .

[39]  A. Robinson,et al.  Mass balance closure and the federal reference method for PM2.5 in Pittsburgh, Pennsylvania , 2004 .

[40]  C. Davidson,et al.  Determination of trace elements in ambient aerosol samples , 2005 .

[41]  R. L. Bennett,et al.  Compositions of particles from selected sources in Philadelphia for receptor modeling applications. , 1988, JAPCA.

[42]  J. Chow,et al.  Northern Front Range Air Quality Study Final Report Volume B: Source Measurements , 1998 .

[43]  Allen L. Robinson,et al.  Positive and Negative Artifacts in Particulate Organic Carbon Measurements with Denuded and Undenuded Sampler Configurations Special Issue of Aerosol Science and Technology on Findings from the Fine Particulate Matter Supersites Program , 2004 .

[44]  P. Paatero,et al.  Positive matrix factorization: A non-negative factor model with optimal utilization of error estimates of data values† , 1994 .

[45]  P. Paatero,et al.  Analysis of different modes of factor analysis as least squares fit problems , 1993 .

[46]  Andrey Khlystov,et al.  Light scattering by fine particles during the Pittsburgh Air Quality Study: measurements and modeling , 2004 .

[47]  Glen R. Cass,et al.  Sources of fine organic aerosol. 4. Particulate abrasion products from leaf surfaces of urban plants , 1993 .

[48]  B. Simoneit.  Organic matter of the troposphere—III. Characterization and sources of petroleum and pyrogenic residues in aerosols over the western united states , 1984 .

[49]  A. Robinson,et al.  Spatial Variations of PM2.5 During the Pittsburgh Air Quality Study , 2004 .

[50]  G. Cass,et al.  Mathematical modeling of atmospheric fine particle‐associated primary organic compound concentrations , 1996 .

[51]  R. Henry.  History and fundamentals of multivariate air quality receptor models , 1997 .

[52]  R. Bautista.  Processing to obtain high-purity gallium , 2003 .

[53]  B. Simoneit,et al.  Application of Molecular Marker Analysis to Vehicular Exhaust for Source Reconciliations , 1985 .

[54]  Allen L Robinson,et al.  Source apportionment of molecular markers and organic aerosol. 3. Food cooking emissions. , 2006, Environmental science & technology.

[55]  Allen L. Robinson,et al.  Ambient measurements of metal-containing PM2.5 in an urban environment using laser-induced breakdown spectroscopy , 2004 .