Chemical characterization and source apportionment of PM 2.5 in Beijing: seasonal perspective

Abstract. In this study, 121 daily PM2.5 (aerosol particle with aerodynamic diameter less than 2.5 μm) samples were collected from an urban site in Beijing in four months between April 2009 and January 2010 representing the four seasons. The samples were determined for various compositions, including elements, ions, and organic/elemental carbon. Various approaches, such as chemical mass balance, positive matrix factorization (PMF), trajectory clustering, and potential source contribution function (PSCF), were employed for characterizing aerosol speciation, identifying likely sources, and apportioning contributions from each likely source. Our results have shown distinctive seasonality for various aerosol speciations associated with PM2.5 in Beijing. Soil dust waxes in the spring and wanes in the summer. Regarding the secondary aerosol components, inorganic and organic species may behave in different manners. The former preferentially forms in the hot and humid summer via photochemical reactions, although their precursor gases, such as SO2 and NOx, are emitted much more in winter. The latter seems to favorably form in the cold and dry winter. Synoptic meteorological and climate conditions can overwhelm the emission pattern in the formation of secondary aerosols. The PMF model identified six main sources: soil dust, coal combustion, biomass burning, traffic and waste incineration emission, industrial pollution, and secondary inorganic aerosol. Each of these sources has an annual mean contribution of 16, 14, 13, 3, 28, and 26%, respectively, to PM2.5. However, the relative contributions of these identified sources significantly vary with changing seasons. The results of trajectory clustering and the PSCF method demonstrated that regional sources could be crucial contributors to PM pollution in Beijing. In conclusion, we have unraveled some complex aspects of the pollution sources and formation processes of PM2.5 in Beijing. To our knowledge, this is the first systematic study that comprehensively explores the chemical characterizations and source apportionments of PM2.5 aerosol speciation in Beijing by applying multiple approaches based on a completely seasonal perspective.

[1]  Bin Zhao,et al.  NO x emissions in China: historical trends and future perspectives , 2013 .

[2]  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 .

[3]  C. You,et al.  Seasonal and spatial variability of the organic matter-to-organic carbon mass ratios in Chinese urban organic aerosols and a first report of high correlations between aerosol oxalic acid and zinc , 2013 .

[4]  S. Pryor,et al.  Assessing the performance of Intergovernmental Panel on Climate Change AR5 climate models in simulating and projecting wind speeds over China , 2012 .

[5]  Xiuji Zhou,et al.  Characteristics of aerosols and mass closure study at two WMO GAW regional background stations in eastern China , 2012 .

[6]  H. Tian,et al.  Temporal trends and spatial variation characteristics of hazardous air pollutant emission inventory from municipal solid waste incineration in China. , 2012, Environmental science & technology.

[7]  Song Guo,et al.  Primary sources and secondary formation of organic aerosols in Beijing, China. , 2012, Environmental science & technology.

[8]  X. Querol,et al.  Hourly elemental concentrations in PM2.5 aerosols sampled simultaneously at urban background and road site , 2012 .

[9]  Kebin He,et al.  Policy: Cleaning China's air , 2012, Nature.

[10]  Renjian Zhang,et al.  Carbonaceous aerosols in China: top-down constraints on primary sources and estimation of secondary contribution , 2012 .

[11]  K. Yumimoto,et al.  Interannual variation in the fine-mode MODIS aerosol optical depth and its relationship to the changes in sulfur dioxide emissions in China between 2000 and 2010 , 2012 .

[12]  Xin Huang,et al.  A high‐resolution ammonia emission inventory in China , 2012 .

[13]  J. Hao,et al.  Chemical characteristics of size-resolved PM₂.₅ at a roadside environment in Beijing, China. , 2012, Environmental pollution.

[14]  N. Mahowald.  Aerosol Indirect Effect on Biogeochemical Cycles and Climate , 2011, Science.

[15]  Min Hu,et al.  Chemical characteristics of inorganic ammonium salts in PM 2.5 in the atmosphere of Beijing (China) , 2011 .

[16]  W. Nie,et al.  Semi-continuous measurement of water-soluble ions in PM2.5 in Jinan, China: Temporal variations and source apportionments , 2011 .

[17]  Z. Bai,et al.  Chemical composition of PM2.5 during winter in Tianjin, China , 2011 .

[18]  Yuan Cheng,et al.  The impact of the pollution control measures for the 2008 Beijing Olympic Games on the chemical composition of aerosols , 2011 .

[19]  Yang Yu,et al.  Dynamics and origin of PM2.5 during a three-year sampling period in Beijing, China. , 2011, Journal of environmental monitoring : JEM.

[20]  J. Chow,et al.  Stable carbon isotopes in aerosols from Chinese cities: Influence of fossil fuels , 2011 .

[21]  G. Gong,et al.  Effects of acidic processing, transport history, and dust and sea salt loadings on the dissolution of iron from Asian dust , 2010 .

[22]  Jing Zhao,et al.  Measurement of atmospheric hydrogen peroxide and organic peroxides in Beijing before and during the 2008 Olympic Games: Chemical and physical factors influencing their concentrations , 2010 .

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

[24]  D. Widory,et al.  Isotopes as tracers of sources of lead and strontium in aerosols (TSP & PM2.5) in Beijing , 2010 .

[25]  R. Mason,et al.  Global mercury emissions to the atmosphere from anthropogenic and natural sources , 2010 .

[26]  Wenying Chen,et al.  Clean coal technology development in China , 2010 .

[27]  Junji Cao,et al.  Chemical Characteristics of Fine Particles (PM1) from Xi'an, China , 2010 .

[28]  Youfei Zheng,et al.  Aerosol optical depth measurements in eastern China and a new calibration method , 2010 .

[29]  Alexis K.H. Lau,et al.  An intensive study of aerosol optical properties in Beijing urban area , 2009 .

[30]  Qiang Yao,et al.  Studies on formation and control of combustion particulate matter in China: A review , 2009 .

[31]  Xingying Zhang,et al.  Aerosol particles from dried salt-lakes and saline soils carried on dust storms over Beijing. , 2009 .

[32]  G. Carmichael,et al.  Asian emissions in 2006 for the NASA INTEX-B mission , 2009 .

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

[34]  L. Molina,et al.  Trace gas and particle emissions from domestic and industrial biofuel use and garbage burning in central Mexico , 2009 .

[35]  J. Tao,et al.  Effect of chemical composition of PM2.5 on visibility in Guangzhou, China, 2007 spring , 2009 .

[36]  Weijun Li,et al.  Observation of nitrate coatings on atmospheric mineral dust particles , 2008 .

[37]  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 .

[38]  Meinrat O. Andreae,et al.  Optical properties and chemical composition of the atmospheric aerosol in urban Guangzhou, China , 2008 .

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

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

[41]  Yu Song,et al.  Identifying anthropogenic and natural influences on extreme pollution of respirable suspended particulates in Beijing using backward trajectory analysis. , 2008, Journal of hazardous materials.

[42]  Shaodong Xie,et al.  Atmospheric Chemistry and Physics Discussions Interactive comment on “ Spatiotemporal variations of ambient PM 10 source contributions in Beijing in 2004 using positive matrix factorization ” , 2022 .

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

[44]  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 .

[45]  J. Ji,et al.  Dolomite as a tracer for the source regions of Asian dust , 2007 .

[46]  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.

[47]  Shaodong Xie,et al.  Source apportionment of PM2.5 in Beijing in 2004. , 2007, Journal of hazardous materials.

[48]  Toshinori Murayama,et al.  Nano-sized carbon black exposure exacerbates atherosclerosis in LDL-receptor knockout mice. , 2007, Circulation journal : official journal of the Japanese Circulation Society.

[49]  D. Eatough,et al.  Fine Particulate Chemical Composition and Light Extinction at Meadview, AZ , 2006, Journal of the Air & Waste Management Association.

[50]  H. Cachier,et al.  Geochemical perspectives from a new aerosol chemical mass closure , 2006 .

[51]  Min Shao,et al.  City clusters in China: air and surface water pollution , 2006 .

[52]  David G. Streets,et al.  Two‐decadal aerosol trends as a likely explanation of the global dimming/brightening transition , 2006 .

[53]  X. Querol,et al.  Identification and Chemical Characterization of Industrial Particulate Matter Sources in Southwest Spain , 2006, Journal of the Air & Waste Management Association.

[54]  Xiao-yan Tang,et al.  Seasonal pollution characteristics of organic compounds in atmospheric fine particles in Beijing. , 2006, The Science of the total environment.

[55]  Ying Wang,et al.  Chemical characteristics of PM2.5 and PM10 in haze-fog episodes in Beijing. , 2006, Environmental science & technology.

[56]  Peter Wåhlin,et al.  Characterisation of traffic-generated particulate matter in Copenhagen , 2006 .

[57]  Xiangao Xia,et al.  Variation of column‐integrated aerosol properties in a Chinese urban region , 2006 .

[58]  Iddi S. N. Mkilaha,et al.  Mechanisms of fine particulates formation with alkali metal compounds during coal combustion , 2006 .

[59]  Yu Song,et al.  Source apportionment of PM2.5 in Beijing by positive matrix factorization , 2006 .

[60]  J. Chow,et al.  Seasonal variations and mass closure analysis of particulate matter in Hong Kong. , 2006, The Science of the total environment.

[61]  Yong-liang Ma,et al.  Concentration and chemical characteristics of PM2.5 in Beijing, China: 2001-2002. , 2006, The Science of the total environment.

[62]  S. Y. Ryu,et al.  Size-resolved source apportionment of ambient particles by positive matrix factorization at Gosan background site in East Asia , 2006 .

[63]  Roy M Harrison,et al.  Trace metal concentrations and water solubility in size-fractionated atmospheric particles and influence of road traffic. , 2006, Environmental science & technology.

[64]  Fabienne Maignan,et al.  Simulation of the mineral dust emission frequencies from desert areas of China and Mongolia using an aerodynamic roughness length map derived from the POLDER/ADEOS 1 surface products : Quantifying the radiative and biogeochemical impacts of mineral dust , 2005 .

[65]  Y. Tsai,et al.  PM2.5 aerosol water content and chemical composition in a metropolitan and a coastal area in southern Taiwan , 2005 .

[66]  W. Malm,et al.  Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study , 2005 .

[67]  Ying Wang,et al.  The ion chemistry and the source of PM2.5 aerosol in Beijing , 2005 .

[68]  J. Diamond,et al.  China's environment in a globalizing world , 2005, Nature.

[69]  J. Hao,et al.  Air pollutants contribution and control strategies of energy-use related sources in Beijing , 2005 .

[70]  F. Duan,et al.  Seasonal characteristics of biomass burning contribution to Beijing aerosol , 2005 .

[71]  Weihong Qian,et al.  Regional trends in recent precipitation indices in China , 2005 .

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

[73]  Jinbin Cao,et al.  The transport pathways and sources of PM10 pollution in Beijing during spring 2001, 2002 and 2003 , 2004 .

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

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

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

[77]  P. Buseck,et al.  Atmospheric tar balls: Particles from biomass and biofuel burning , 2003 .

[78]  Renjian Zhang,et al.  Analysis on the chemical and physical properties of particles in a dust storm in spring in Beijing , 2003 .

[79]  F. Duan,et al.  Atmospheric aerosol concentration level and chemical characteristics of water-soluble ionic species in wintertime in Beijing, China. , 2003, Journal of environmental monitoring : JEM.

[80]  C. Chan,et al.  Size distributions and formation of ionic species in atmospheric particulate pollutants in Beijing, China: 1-inorganic ions , 2003 .

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

[82]  Philip K. Hopke,et al.  Recent developments in receptor modeling , 2003 .

[83]  P. Hopke,et al.  Comparison of hybrid receptor models to locate PCB sources in Chicago , 2003 .

[84]  Min Hu,et al.  Seasonal variation of ionic species in fine particles at Qingdao, China , 2002 .

[85]  Kebin He,et al.  URBAN AIR POLLUTION IN CHINA: Current Status, Characteristics, and Progress , 2002 .

[86]  Kebin He,et al.  The water-soluble ionic composition of PM2.5 in Shanghai and Beijing, China , 2002 .

[87]  Risto Hillamo,et al.  Organic and black carbon in PM2.5 and PM10: 1 year of data from an urban site in Helsinki, Finland , 2002 .

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

[89]  Weihong Qian,et al.  Variations of the Dust Storm in China and its Climatic Control , 2002 .

[90]  Yuanhang Zhang,et al.  DIURNAL VARIATIONS OF AEROSOL CHEMICAL COMPOSITIONS AND RELATED GASEOUS POLLUTANTS IN BEIJING AND GUANGZHOU , 2002, Journal of Environmental Science and Health. Part A: Toxic/Hazardous Substances and Environmental Engineering.

[91]  Ronald W. Williams,et al.  Personal exposures to PM2.5 mass and trace elements in Baltimore, MD, USA , 2001 .

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

[93]  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.

[94]  Jimin Sun,et al.  Spatial and temporal characteristics of dust storms in China and its surrounding regions, 1960-1999 : Relations to source area and climate , 2001 .

[95]  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.

[96]  A. Cecinato,et al.  Organic aerosols in urban and waste landfill of Algiers metropolitan area: occurrence and sources. , 2001, Environmental science & technology.

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

[98]  G. Oberdörster,et al.  Pulmonary effects of inhaled ultrafine particles , 2000, International archives of occupational and environmental health.

[99]  Daizhou Zhang,et al.  Nitrate and sulfate in individual Asian dust-storm particles in Beijing, China in Spring of 1995 and 1996 , 1999 .

[100]  P. Paatero,et al.  Application of positive matrix factorization in source apportionment of particulate pollutants in Hong Kong , 1999 .

[101]  Dorothy K. Hall,et al.  The aerosol at Barrow, Alaska: long-term trends and source locations , 1999 .

[102]  Richard Arimoto,et al.  Dust emission from Chinese desert sources linked to variations in atmospheric circulation , 1997 .

[103]  J. Schwartz,et al.  Is Daily Mortality Associated Specifically with Fine Particles? , 1996, Journal of the Air & Waste Management Association.

[104]  Judith C. Chow,et al.  Descriptive analysis of PM2.5 and PM10 at regionally representative locations during SJVAQS/AUSPEX , 1996 .

[105]  D. Dockery,et al.  Particulate air pollution as a predictor of mortality in a prospective study of U.S. adults. , 1995, American journal of respiratory and critical care medicine.

[106]  Judith C. Chow,et al.  Temporal and spatial variations of PM2.5 and PM10 aerosol in the Southern California air quality study , 1994 .

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

[108]  H. Cachier,et al.  Influence of biomass burning on equatorial African rains , 1991, Nature.

[109]  J H Seinfeld,et al.  Urban Air Pollution: State of the Science , 1989, Science.

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

[111]  Renjian Zhang,et al.  Characterization and Source Apportionment of PM2.5 in an Urban Environment in Beijing , 2013 .

[112]  Renjian Zhang,et al.  Characterization of Atmospheric Organic and Elemental Carbon of PM2.5 in a Typical Semi-Arid Area of Northeastern China , 2012 .

[113]  J. Chow,et al.  Carbonaceous and Ionic Components of Atmospheric Fine Particles in Beijing and Their Impact on Atmospheric Visibility , 2012 .

[114]  Yan Feng,et al.  Air Pollution, Greenhouse Gases and Climate Change: Global and Regional Perspectives , 2009 .

[115]  Yaping Zhang,et al.  Source apportionment of lead-containing aerosol particles in Shanghai using single particle mass spectrometry. , 2009, Chemosphere.

[116]  Ming Fang,et al.  Managing air quality in a rapidly developing nation : China , 2009 .

[117]  Hui Yuan,et al.  Long-term monitoring and source apportionment of PM2.5/PM10 in Beijing, China. , 2008, Journal of environmental sciences.

[118]  S. Schneider,et al.  Climate Change 2007 Synthesis report , 2008 .

[119]  C. Chan,et al.  Air pollution in mega cities in China , 2008 .

[120]  K. Ho,et al.  Carbonaceous aerosols in PM10 and pollution gases in winter in Beijing. , 2007, Journal of environmental sciences.

[121]  Pushpam Kumar.  Agriculture (Chapter8) in IPCC, 2007: Climate change 2007: Mitigation of Climate Change. Contribution of Working Group III to the Fourth assessment Report of the Intergovernmental Panel on Climate Change , 2007 .

[122]  Binyu Wang,et al.  Air quality during the 2008 Beijing Olympic Games , 2007 .

[123]  Xiaohong Yao,et al.  Sampling artifacts of acidity and ionic species in PM2.5. , 2004, Environmental science & technology.

[124]  M. Lazaridis,et al.  Chemical composition of size-resolved atmospheric aerosols in the eastern Mediterranean during summer and winter , 2003 .

[125]  G. Mininni,et al.  Behaviour of Cd, Cr, Mn, Ni, Pb, and Zn in sewage sludge incineration by fluidised bed furnace. , 2003, Waste management.

[126]  H. Barnes,et al.  An instrument for measuring the liquid water content of aerosols , 1997 .

[127]  D. Dockery,et al.  Acute respiratory effects of particulate air pollution. , 1994, Annual review of public health.