PM 2.5 pollution in a megacity of southwest China: source apportionment and implication

Abstract. Daily PM2.5 (aerosol particles with an aerodynamic diameter of less than 2.5 μm) samples were collected at an urban site in Chengdu, an inland megacity in southwest China, during four 1-month periods in 2011, with each period in a different season. Samples were subject to chemical analysis for various chemical components ranging from major water-soluble ions, organic carbon (OC), element carbon (EC), trace elements to biomass burning tracers, anhydrosugar levoglucosan (LG), and mannosan (MN). Two models, the ISORROPIA II thermodynamic equilibrium model and the positive matrix factorization (PMF) model, were applied to explore the likely chemical forms of ionic constituents and to apportion sources for PM2.5. Distinctive seasonal patterns of PM2.5 and associated main chemical components were identified and could be explained by varying emission sources and meteorological conditions. PM2.5 showed a typical seasonality of waxing in winter and waning in summer, with an annual mean of 119 μg m−3. Mineral soil concentrations increased in spring, whereas biomass burning species elevated in autumn and winter. Six major source factors were identified to have contributed to PM2.5 using the PMF model. These were secondary inorganic aerosols, coal combustion, biomass burning, iron and steel manufacturing, Mo-related industries, and soil dust, and they contributed 37 ± 18, 20 ± 12, 11 ± 10, 11 ± 9, 11 ± 9, and 10 ± 12%, respectively, to PM2.5 masses on annual average, while exhibiting large seasonal variability. On annual average, the unknown emission sources that were not identified by the PMF model contributed 1 ± 11% to the measured PM2.5 mass. Various chemical tracers were used for validating PMF performance. Antimony (Sb) was suggested to be a suitable tracer of coal combustion in Chengdu. Results of LG and MN helped constrain the biomass burning sources, with wood burning dominating in winter and agricultural waste burning dominating in autumn. Excessive Fe (Ex-Fe), defined as the excessive portion in measured Fe that cannot be sustained by mineral dust, is corroborated to be a straightforward useful tracer of iron and steel manufacturing pollution. In Chengdu, Mo / Ni mass ratios were persistently higher than unity, and considerably distinct from those usually observed in ambient airs. V / Ni ratios averaged only 0.7. Results revealed that heavy oil fuel combustion should not be a vital anthropogenic source, and additional anthropogenic sources for Mo are yet to be identified. Overall, the emission sources identified in Chengdu could be dominated by local sources located in the vicinity of Sichuan, a result different from those found in Beijing and Shanghai, wherein cross-boundary transport is significant in contributing pronounced PM2.5. These results provided implications for PM2.5 control strategies.

[1]  Renjian Zhang,et al.  Seasonal variations and chemical characteristics of sub-micrometer particles (PM1) in Guangzhou, China , 2012 .

[2]  F. Palmgren,et al.  Seasonal distribution of polar organic compounds in the urban atmosphere of two large cities from the North and South of Europe , 2007 .

[3]  D. Dockery,et al.  Health Effects of Fine Particulate Air Pollution: Lines that Connect , 2006, Journal of the Air & Waste Management Association.

[4]  S. Xie,et al.  Spatial and temporal variation of anthropogenic black carbon emissions in China for the period 1980–2009 , 2011 .

[5]  Roy M. Harrison,et al.  A Study of the Size Distributions and the Chemical Characterization of Airborne Particles in the Vicinity of a Large Integrated Steelworks , 2008 .

[6]  Sönke Szidat,et al.  Contributions of fossil fuel, biomass-burning, and biogenic emissions to carbonaceous aerosols in Zurich as traced by 14C , 2006 .

[7]  Jenise L. Swall,et al.  Determining the spatial and seasonal variability in OM/OC ratios across the US using multiple regression , 2010 .

[8]  J. Pinto,et al.  Spatial Variability of PM2.5 in Urban Areas in the United States , 2004, Journal of the Air & Waste Management Association.

[9]  Mar Viana,et al.  Speciation and sources of atmospheric aerosols in a highly industrialised emerging mega-city in central China. , 2006, Journal of environmental monitoring : JEM.

[10]  Stephen B. Reid,et al.  Toward Effective Source Apportionment Using Positive Matrix Factorization: Experiments with Simulated PM2.5 Data , 2010, Journal of the Air & Waste Management Association.

[11]  F. Bardelli,et al.  Speciation of Sb in airborne particulate matter, vehicle brake linings, and brake pad wear residues , 2013 .

[12]  W. Malm,et al.  Spatial and seasonal trends in particle concentration and optical extinction in the United States , 1994 .

[13]  J. Chow,et al.  Lead concentrations in fine particulate matter after the phasing out of leaded gasoline in Xi'an, China , 2012 .

[14]  Xiaoyuan Yan,et al.  Bottom-up estimate of biomass burning in mainland China. , 2006 .

[15]  G. Cao,et al.  Inventory of black carbon and organic carbon emissions from China , 2006 .

[16]  Xiaoye Zhang,et al.  Carbonaceous aerosol composition over various regions of China during 2006 , 2008 .

[17]  D. Gomez,et al.  Antimony: a traffic-related element in the atmosphere of Buenos Aires, Argentina. , 2005, Journal of environmental monitoring : JEM.

[18]  Min Shao,et al.  Characteristics of particulate carbon emissions from real-world Chinese coal combustion. , 2008, Environmental science & technology.

[19]  Xiaohui Xu,et al.  Fine particulate air pollution and daily mortality in Shenyang, China. , 2011, The Science of the total environment.

[20]  Meinrat O. Andreae,et al.  Aerosol cloud precipitation interactions. Part 1. The nature and sources of cloud-active aerosols , 2008 .

[21]  Yan‐jing Chen,et al.  Pb–Sr–Nd isotope constraints on the fluid source of the Dahu Au–Mo deposit in Qinling Orogen, central China, and implication for Triassic tectonic setting , 2012 .

[22]  Z. Bai,et al.  Characterization of Atmospheric Organic Carbon and Element Carbon of PM2.5 and PM10 at Tianjin, China , 2010 .

[23]  Y. Qin,et al.  Spatial and temporal variation of anthropogenic black carbon emissions in China for the period 1980–2009 , 2011 .

[24]  Hsi-Hsien Yang,et al.  Profiles of PAH emission from steel and iron industries. , 2002, Chemosphere.

[25]  E. Vermote,et al.  The MODIS Aerosol Algorithm, Products, and Validation , 2005 .

[26]  Xiaoqiu Chen,et al.  Seasonal variations and chemical compositions of PM2.5 aerosol in the urban area of Fuzhou, China , 2012 .

[27]  Yuan Cheng,et al.  Dust storms come to Central and Southwestern China, too: implications from a major dust event in Chongqing , 2009, Atmospheric Chemistry and Physics.

[28]  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.

[29]  Peter Wåhlin,et al.  A European aerosol phenomenology—1: physical characteristics of particulate matter at kerbside, urban, rural and background sites in Europe , 2004 .

[30]  S. Liu,et al.  High wintertime particulate matter pollution over an offshore island (Kinmen) off southeastern China: An overview , 2010 .

[31]  Eiliv Steinnes,et al.  Carbonaceous aerosols in Norwegian urban areas , 2009 .

[32]  Kebin He,et al.  The characteristics of PM2.5 in Beijing, China , 2001 .

[33]  Renjian Zhang,et al.  Chemical characterization and source apportionment of PM 2 . 5 in Beijing : seasonal perspective , 2013 .

[34]  M. Claeys,et al.  Improved method for quantifying levoglucosan and related monosaccharide anhydrides in atmospheric aerosols and application to samples from urban and tropical locations. , 2002, Environmental science & technology.

[35]  Martin Gysel,et al.  Chemical characterisation of PM2.5, PM10 and coarse particles at urban, near-city and rural sites in Switzerland , 2005 .

[36]  Jiming Hao,et al.  Anthropogenic atmospheric emissions of antimony and its spatial distribution characteristics in China. , 2012, Environmental science & technology.

[37]  Leiming Zhang,et al.  Uncertainty assessment of current size-resolved parameterizations for below-cloud particle scavenging by rain , 2010 .

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

[39]  P. Hopke,et al.  Atmospheric Chemistry and Physics Source apportionment of PM 2 . 5 in Seoul , Korea , 2009 .

[40]  J. Hao,et al.  Trend and characteristics of atmospheric emissions of Hg, As, and Se from coal combustion in China, 1980–2007 , 2010 .

[41]  Åke Sjödin,et al.  Metal emissions from road traffic and the influence of resuspension: results from two tunnel studies , 2002 .

[42]  Min Hu,et al.  Anthropogenic Calcium Particles Observed in Beijing and Qingdao, China , 2005 .

[43]  Judith C. Chow,et al.  Characteristics of carbonaceous aerosol in Pearl River Delta Region, China during 2001 winter period , 2003 .

[44]  Andrea Pozzer,et al.  Interactive comment on “A high-resolution emission inventory of primary pollutants for the Huabei region, China” by B. Zhao et al , 2011 .

[45]  K. He,et al.  Characteristics of PM 2.5 speciation in representative megacities and across China , 2011 .

[46]  K. H. Wedepohl,et al.  The Composition of the Continental Crust , 1995 .

[47]  Donald F. Gatz,et al.  Toxic trace elements in urban air in Illinois , 1990 .

[48]  X. Querol,et al.  Natural and Anthropogenic Contributions to PM10 and PM2.5 in an Urban Area in the Western Mediterranean Coast , 2008 .

[49]  Ernie Weijers,et al.  Source apportionment and spatial variability of PM2.5 using measurements at five sites in the Netherlands , 2011 .

[50]  H. Hansson,et al.  Speciation and origin of PM10 and PM2.5 in selected European cities , 2004 .

[51]  M. Sugiyama,et al.  Atmospheric bulk deposition of soluble phosphorus in Ashiu Experimental Forest, Central Japan: source apportionment and sample contamination problem , 2005 .

[52]  C. Perrino,et al.  Source characterization of fine and coarse particles at the East Mediterranean coast , 2008 .

[53]  Maria Ascensão Trancoso,et al.  Source apportionment of fine and coarse particulate matter in a sub-urban area at the Western European Coast , 2005 .

[54]  Shih-Chieh Hsu,et al.  Long‐range southeastward transport of Asian biosmoke pollution: Signature detected by aerosol potassium in Northern Taiwan , 2009 .

[55]  P. Espen,et al.  Single particle characterization of spring and summer aerosols in Beijing : Formation of composite sulfate of calcium and potassium , 2005 .

[56]  R. Rudnick,et al.  Composition of the Continental Crust , 2014 .

[57]  Gregg Marland,et al.  China: Emissions pattern of the world leader in CO2 emissions from fossil fuel consumption and cement production , 2008 .

[58]  Judith C. Chow,et al.  Spatial and seasonal distributions of carbonaceous aerosols over China , 2007 .

[59]  S. Masunaga,et al.  Characterization of PM2.5, PM2.5-10 and PM>10 in ambient air, Yokohama, Japan , 2010 .

[60]  W. Malm,et al.  Determination of levoglucosan in biomass combustion aerosol by high-performance anion-exchange chromatography with pulsed amperometric detection , 2006 .

[61]  Byung-Wook Kang,et al.  Chemical characteristics of principal PM2.5 species in Chongju, South Korea , 2001 .

[62]  C. You,et al.  Seasonal and spatial variability of the OM/OC mass ratios and high regional correlation between oxalic acid and zinc in Chinese urban organic aerosols , 2013 .

[63]  B. Turpin,et al.  Identification of secondary organic aerosol episodes and quantitation of primary and secondary organic aerosol concentrations during SCAQS , 1995 .

[64]  P. Hopke,et al.  Major Source Categories for PM2.5 in Pittsburgh using PMF and UNMIX , 2006 .

[65]  S. Liu,et al.  Water‐soluble species in the marine aerosol from the northern South China Sea: High chloride depletion related to air pollution , 2007 .

[66]  Tong Yu,et al.  Identification and estimate of biomass burning contribution to the urban aerosol organic carbon concentrations in Beijing , 2004 .

[67]  R. Draxler HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) Model access via NOAA ARL READY Website , 2010 .

[68]  J. Schwartz,et al.  Association of fine particulate matter from different sources with daily mortality in six U.S. cities. , 2000, Environmental health perspectives.

[69]  A. Nenes,et al.  ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K + –Ca 2+ –Mg 2+ –NH 4 + –Na + –SO 4 2− –NO 3 − –Cl − –H 2 O aerosols , 2007 .

[70]  Rajasekhar Balasubramanian,et al.  Comprehensive characterization of PM2.5 aerosols in Singapore , 2003 .

[71]  Chung-Chi Chen,et al.  A super Asian dust storm over the East and South China Seas: Disproportionate dust deposition , 2013 .

[72]  Alexis K.H. Lau,et al.  Seasonal characteristics and regional transport of PM2.5 in Hong Kong , 2005 .

[73]  J. C. Galloo,et al.  PM10 metal concentrations and source identification using positive matrix factorization and wind sectoring in a French industrial zone , 2010 .

[74]  Y. Tsai,et al.  Size-Resolved Anhydrosugar Composition in Smoke Aerosol from Controlled Field Burning of Rice Straw , 2009 .

[75]  Shaocai Yu,et al.  A performance evaluation of the 2004 release of Models-3 CMAQ , 2006 .

[76]  Hairong Tao,et al.  The characteristics of carbonaceous species and their sources in PM2.5 in Beijing , 2004 .

[77]  David G. Streets,et al.  Primary anthropogenic aerosol emission trends for China, 1990–2005 , 2011 .

[78]  J. Watson Visibility: Science and Regulation , 2002, Journal of the Air & Waste Management Association.

[79]  H. Puxbaum,et al.  A highly resolved anion-exchange chromatographic method for determination of saccharidic tracers for biomass combustion and primary bio-particles in atmospheric aerosol , 2009 .

[80]  M. Legrand,et al.  Chemical composition of atmospheric aerosols during the 2003 summer intense forest fire period , 2008 .

[81]  P. Butelli,et al.  Major chemical components of PM2.5 in Milan (Italy) , 2005 .

[82]  G. Dongarrà,et al.  Mass levels, crustal component and trace elements in PM10 in Palermo, Italy , 2007 .

[83]  Jun Li,et al.  Characteristics of organic and elemental carbon in PM2.5 samples in Shanghai, China , 2009 .

[84]  Haizhen Yang,et al.  Concentration and chemical composition of PM2.5 in Shanghai for a 1-year period , 2003 .

[85]  S. Liu,et al.  A criterion for identifying Asian dust events based on Al concentration data collected from northern Taiwan between 2002 and early 2007 , 2008 .

[86]  J. Pacyna,et al.  An assessment of global and regional emissions of trace metals to the atmosphere from anthropogenic sources worldwide , 2001 .

[87]  S. Taylor Trace element abundances and the chondritic Earth model , 1964 .

[88]  Renjian Zhang,et al.  Chemical composition of PM2.5 in an urban environment in Chengdu, China:Importance of springtime dust storms and biomass burning , 2013 .

[89]  James J. Schauer,et al.  Characterization of organic aerosols emitted from the combustion of biomass indigenous to South Asia , 2003 .

[90]  A. S. Shannigrahi,et al.  Fossil and non-fossil sources of organic carbon (OC) and elemental carbon (EC) in Göteborg, Sweden , 2008 .

[91]  Jinsheng Chen,et al.  Chemical compositions and extinction coefficients of PM2.5 in peri-urban of Xiamen, China, during June 2009–May 2010 , 2012 .

[92]  S. Machemer Characterization of airborne and bulk particulate from iron and steel manufacturing facilities. , 2004, Environmental science & technology.

[93]  Dongfang Wang,et al.  Characterization of soil dust aerosol in China and its transport and distribution during 2001 ACE‐Asia: 1. Network observations , 2003 .

[94]  Ji-ti Zhou,et al.  Regional characteristics of sulfur and lead isotope ratios in the atmosphere at several Chinese urban sites. , 2001, Environmental science & technology.

[95]  X. Tie,et al.  Water-soluble ions in atmospheric aerosols measured in Xi'an, China: Seasonal variations and sources , 2011 .

[96]  Judith C. Chow,et al.  The IMPROVE_A Temperature Protocol for Thermal/Optical Carbon Analysis: Maintaining Consistency with a Long-Term Database , 2007, Journal of the Air & Waste Management Association.

[97]  Renjian Zhang,et al.  Impact of PM2.5 chemical compositions on aerosol light scattering in Guangzhou — the largest megacity in South China , 2014 .

[98]  王汝荣 European cities , 2022 .

[99]  M. Andreae,et al.  Emission of trace gases and aerosols from biomass burning , 2001 .

[100]  Kirk R. Smith,et al.  Implications of changes in household stoves and fuel use in China , 2004 .

[101]  Philip B. Russell,et al.  ACE-ASIA Regional Climatic and Atmospheric Chemical Effects of Asian Dust and Pollution , 2004 .