Source and formation of secondary particulate matter in PM2.5 in Asian continental outflow

[1] Fifty-five 48-h PM2.5 samples were collected from March 2003 to January 2004 at Changdao, a resort island in Bohai Sea/Yellow Sea in Northern China. Sulfate, nitrate and ammonium accounted for 54 ± 9% of the PM2.5 mass concentration (annual average 47 μg m−3) while organic matter and K+ contributed to 27 ± 7% and 7 ± 7% of the total mass, respectively. The ratios of SO42− to NO3− mass concentrations could be divided into two regimes and demarcated at nitrate concentration of 5 μg m−3. In the low NO3− regime, NO3−, SO42− and EC were well correlated to K+, and the estimated contributions of NO3−, SO42− and EC from biomass burning were 50 ± 27%, 38 ± 24% and 47 ± 27%, respectively. These correlations substantially decreased in the high NO3− regime reflecting fossil fuel combustion and formation of ammonium nitrate and the estimated contributions of NO3−, SO42− and EC from biomass burning were 16 ± 12%, 28 ± 18% and 27 ± 16%, respectively. In most samples, the equivalent ratios of total anion to total cation concentrations were greater than unity, suggesting that the aerosols were acidic. When [H+] > 0, a moderately good linear correlation of the estimated aerosol acidity [H+] with the water-soluble organic carbon (WSOC) was observed with R2 = 0.70 and an increase of [H+] by 100 neq m−3 would increase 1.2 μg m−3 WSOC in PM2.5. When [H+] > 0, an increase of [H+] by 100 neq m−3 would increase 1.4 μg m−3 of secondary organic carbon (SOC) in PM2.5. Moreover, the correlation analysis result suggested that 60% of the estimated SOC (on average) in PM2.5 were water-soluble.

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

[2]  Tao Wang,et al.  Characteristics of summertime PM2.5 organic and elemental carbon in four major Chinese cities: Implications of high acidity for water-soluble organic carbon (WSOC) , 2011 .

[3]  H. L. Miller,et al.  Climate Change 2007: The Physical Science Basis , 2007 .

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

[5]  Erik Swietlicki,et al.  Organic aerosol and global climate modelling: a review , 2004 .

[6]  N. Takegawa,et al.  Seasonal and diurnal variations of organic carbon in PM2.5 in Beijing and the estimation of secondary organic carbon , 2009 .

[7]  Jing Chen,et al.  A study of air pollution of city clusters , 2011 .

[8]  M. Uematsu,et al.  Numerical study of the atmospheric input of anthropogenic total nitrate to the marginal seas in the western North Pacific region , 2007 .

[9]  K. Kawamura,et al.  Seasonal changes in the distribution of dicarboxylic acids in the urban atmosphere , 1993 .

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

[11]  John P. Burrows,et al.  Global budgets of atmospheric glyoxal and methylglyoxal, and implications for formation of secondary organic aerosols , 2007 .

[12]  J. Prospero,et al.  Long-Range Atmospheric Transport of Soil Dust from Asia to the Tropical North Pacific: Temporal Variability , 1980, Science.

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

[14]  X. Yao,et al.  Sources, compositions, and distributions of water‐soluble organic nitrogen in aerosols over the China Sea , 2010 .

[15]  A. Wexler,et al.  Size distributions of particulate sulfate, nitrate, and ammonium at a coastal site in Hong Kong , 1999 .

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

[17]  Barry J. Huebert,et al.  A large organic aerosol source in the free troposphere missing from current models , 2005 .

[18]  Paulo Artaxo,et al.  Chemical composition of aerosol particles from direct emissions of vegetation fires in the Amazon Basin: water-soluble species and trace elements , 2000 .

[19]  Comment on "Atmospheric particulate matter pollution during the 2008 Beijing Olympics". , 2009, Environmental science & technology.

[20]  Hilkka Timonen,et al.  Sources of organic carbon in fine particulate matter in northern European urban air , 2008 .

[21]  M. Uematsu,et al.  Chemical characteristics of aerosols transported from Asia to the East China Sea: an evaluation of anthropogenic combined nitrogen deposition in autumn , 2005 .

[22]  T. Kirchstetter,et al.  Water-soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution and Distribution , 2003 .

[23]  Shao-Meng Li,et al.  Reactive uptake of pinonaldehyde on acidic aerosols , 2006 .

[24]  C. Carlson,et al.  Sources of Organic Carbon to Coral Reef Flats , 2013 .

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

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

[27]  H. Takada,et al.  Seasonal variations of sulfate, carbonaceous species (black carbon and polycyclic aromatic hydrocarbons), and trace elements in fine atmospheric aerosols collected at subtropical islands in the East China Sea , 2004 .

[28]  Tsz Yan Ling,et al.  Comparison of thermodynamic predictions for in situ pH in PM2.5 , 2006 .

[29]  G. Shaw,et al.  The Asian source of Arctic haze bands , 1977, Nature.

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

[31]  R. Duce,et al.  Atmospheric non‐sea‐salt sulfate, nitrate and methanesulfonate over the China Sea , 1996 .

[32]  M. Zheng,et al.  Biomass burning impact on PM 2.5 over the southeastern US during 2007: integrating chemically speciated FRM filter measurements, MODIS fire counts and PMF analysis , 2010 .

[33]  Min Hu,et al.  Mixture of sulfate and nitrate in coastal atmospheric aerosols: individual particle studies in Qingdao (36°04′N, 120°21′E), China , 2000 .

[34]  Yong-liang Ma,et al.  Ambient organic carbon to elemental carbon ratios: Influences of the measurement methods and implications , 2011 .

[35]  M. Birch Analysis of carbonaceous aerosols: interlaboratory comparison. , 1998, The Analyst.

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

[37]  Tao Wang,et al.  Summertime PM 2.5 ionic species in four major cities of China: nitrate formation in an ammonia-deficient atmosphere , 2008 .

[38]  Acid-catalyzed condensed-phase reactions of limonene and terpineol and their impacts on gas-to-particle partitioning in the formation of organic aerosols. , 2010, Environmental science & technology.

[39]  K. Demerjian,et al.  Aerosol chemical composition in New York state from integrated filter samples: Urban/rural and seasonal contrasts , 2004 .

[40]  G. Carmichael,et al.  Characteristics and Influence of Biosmoke on the Fine-Particle Ionic Composition Measured in Asian Outflow during the Transport and Chemical Evolution Over the Pacific (TRACE-P) Experiment , 2003 .

[41]  C. Medaglia,et al.  A Numerical Study , 2005 .

[42]  C. Chan,et al.  Characterization of dicarboxylic acids in PM2.5 in Hong Kong , 2004 .

[43]  D. Allen,et al.  Estimates of heterogeneous formation of secondary organic aerosol during a wood smoke episode in Houston, Texas , 2007 .

[44]  C. Chan,et al.  Accretion reactions of octanal catalyzed by sulfuric acid: product identification, reaction pathways, and atmospheric implications. , 2008, Environmental science & technology.

[45]  P. Mulawa,et al.  P API reference , 2003 .

[46]  C. Chan,et al.  Properties of organic matter in PM2.5 at Changdao Island, China - A rural site in the transport path of the Asian continental outflow , 2007 .

[47]  John H. Seinfeld,et al.  the Creative Commons Attribution 3.0 License. Atmospheric Chemistry , 2008 .

[48]  Xin Yang,et al.  A laboratory study of agricultural crop residue combustion in China: Emission factors and emission inventory , 2008 .

[49]  R. Hillamo,et al.  Ion balances of size-resolved tropospheric aerosol samples: implications for the acidity and atmospheric processing of aerosols , 2001 .

[50]  C. Chan,et al.  Evidence of high PM2.5 strong acidity in ammonia-rich atmosphere of Guangzhou, China: Transition in pathways of ambient ammonia to form aerosol ammonium at [NH4+]/[SO42–] = 1.5 , 2011 .

[51]  J. Seinfeld,et al.  Coupling Thermodynamic Theory with Measurements to Characterize Acidity of Atmospheric Particles , 1993 .

[52]  J. Brook,et al.  Identification of the major sources contributing to PM2.5 observed in Toronto. , 2003, Environmental science & technology.

[53]  Shuxiao Wang,et al.  Particulate and trace gas emissions from open burning of wheat straw and corn stover in China. , 2007, Environmental science & technology.

[54]  R. Duce,et al.  Input of atmospheric trace elements and mineral matter to the Yellow Sea during the spring of a low‐dust year , 1992 .

[55]  Zhaoyan Liu,et al.  Asian dust transported one full circuit around the globe , 2009 .

[56]  Jian-hua Chen,et al.  Study on acidity and acidic buffering capacity of particulate matter over Chinese eastern coastal areas in spring , 2006 .

[57]  B. Zielińska,et al.  Emissions of levoglucosan, methoxy phenols, and organic acids from prescribed burns, laboratory combustion of wildland fuels, and residential wood combustion. , 2007, Environmental science & technology.

[58]  Y. Rudich,et al.  Low molecular weight organic acids in aerosol particles from Rondônia, Brazil, during the biomass-burning, transition and wet periods , 2004 .

[59]  E. Edgerton,et al.  Searching for evidence of acid-catalyzed enhancement of secondary organic aerosol formation using ambient aerosol data , 2009 .

[60]  Kwon-Ho Lee,et al.  Impact of the smoke aerosol from Russian forest fires on the atmospheric environment over Korea during May 2003 , 2004 .

[61]  Alexandre Caseiro,et al.  Chemical characterisation of fine particle emissions from wood stove combustion of common woods growing in mid-European Alpine regions , 2008 .

[62]  Yele Sun,et al.  The variation of characteristics and formation mechanisms of aerosols in dust, haze, and clear days in Beijing , 2006 .

[63]  M. Shao,et al.  Source profiles of particulate organic matters emitted from cereal straw burnings. , 2007, Journal of environmental sciences.

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

[65]  Min Hu,et al.  When aerosol sulfate goes up, so does oxalate: implication for the formation mechanisms of oxalate. , 2005, Environmental science & technology.

[66]  Xinming Wang,et al.  The influence of temperature and aerosol acidity on biogenic secondary organic aerosol tracers: Observations at a rural site in the central Pearl River Delta region, South China , 2011 .

[67]  J. A. de Gouw,et al.  No evidence for acid‐catalyzed secondary organic aerosol formation in power plant plumes over metropolitan Atlanta, Georgia , 2007 .

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

[69]  Allen L. Robinson,et al.  Levoglucosan stability in biomass burning particles exposed to hydroxyl radicals , 2010 .

[70]  Shu Tao,et al.  Atmospheric particulate matter pollution during the 2008 Beijing Olympics. , 2009, Environmental science & technology.

[71]  J. Chow,et al.  Characterization of chemical species in PM2.5 and PM10 aerosols in Hong kong , 2003 .

[72]  C. Chan,et al.  Inter-particle and gas-particle interactions in sampling artifacts of PM2.5 in filter-based samplers , 2005 .

[73]  D. C. Snyder,et al.  Insights into the Origin of Water Soluble Organic Carbon in Atmospheric Fine Particulate Matter , 2009 .

[74]  Naoki Kaneyasu,et al.  Chemical forms and sources of extremely high nitrate and chloride in winter aerosol pollution in the Kanto Plain of Japan , 1999 .

[75]  T. Takemura,et al.  Seasonal variation of levoglucosan in aerosols over the western North Pacific and its assessment as a biomass-burning tracer , 2010 .

[76]  A. G. Allen,et al.  Influence of agricultural biomass burning on aerosol size distribution and dry deposition in southeastern Brazil. , 2005, Environmental science & technology.

[77]  C. Simpson,et al.  Emission factors of PAHs, methoxyphenols, levoglucosan, elemental carbon and organic carbon from simulated wheat and Kentucky bluegrass stubble burns , 2007 .

[78]  D O U G L A,et al.  A Case Study of Urban Particle Acidity and Its Influence on Secondary Organic Aerosol , 2007 .

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