Insights on organic aerosol aging and the influence of coal combustion at a regional receptor site of central eastern China

被引：142

作者：

Hu, W. W. ^{[1
,3
]}

Hu, M. ^{[1
]}

Yuan, B. ^{[1
]}

Jimenez, J. L. ^{[3
,4
]}

Tang, Q. ^{[1
]}

Peng, J. F. ^{[1
]}

Hu, W. ^{[1
]}

Shao, M. ^{[1
]}

Wang, M. ^{[1
]}

Zeng, L. M. ^{[1
]}

Wu, Y. S. ^{[1
]}

Gong, Z. H. ^{[1
,2
]}

Huang, X. F. ^{[1
,2
]}

He, L. Y. ^{[1
,2
]}

机构：

[1] Peking Univ, Coll Environm Sci & Engn, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100871, Peoples R China

[2] Peking Univ, Shenzhen Grad Sch, Sch Environm & Energy, Key Lab Urban Habitat Environm Sci & Technol, Shenzhen 518055, Peoples R China

[3] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA

[4] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA

来源：

ATMOSPHERIC CHEMISTRY AND PHYSICS | 2013年 / 13卷 / 19期

基金：

中国国家自然科学基金;

关键词：

RESOLVED CHEMICAL-CHARACTERIZATION; POLYCYCLIC AROMATIC-HYDROCARBONS; URBAN SUPERSITE T0; PEARL RIVER DELTA; NEW-YORK-CITY; HIGH-RESOLUTION; SOURCE APPORTIONMENT; MASS-SPECTROMETER; SOA FORMATION; RURAL SITE;

D O I：

10.5194/acp-13-10095-2013

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

In order to understand the aging and processing of organic aerosols (OA), an intensive field campaign (Campaign of Air Pollution at Typical Coastal Areas IN Eastern China, CAPTAIN) was conducted March-April at a receptor site (a Changdao island) in central eastern China. Multiple fast aerosol and gas measurement instruments were used during the campaign, including a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) that was applied to measure mass concentrations and non-refractory chemical components of submicron particles (PM1nr). The average mass concentration of PM1(PM1nr+black carbon) was 47 +/- 36 mu g m(-3) during the campaign and showed distinct variation, depending on back trajectories and their overlap with source regions. Organic aerosol (OA) is the largest component of PM1 (30%), followed by nitrate (28%), sulfate (19%), ammonium (15%), black carbon (6%), and chloride (3%). Four OA components were resolved by positive matrix factorization (PMF) of the high-resolution spectra, including low-volatility oxygenated organic aerosol (LV-OOA), semi-volatile oxygenated OA (SV-OOA), hydrocarbon-like OA (HOA) and a coal combustion OA (CCOA). The mass spectrum of CCOA had high abundance of fragments from polycyclic aromatic hydrocarbons (PAHs) (m/z 128, 152, 178, etc.). The average atomic ratio of oxygen to carbon in OA (O/C) at Changdao was 0.59, which is comparable to other field studies reported at locations downwind of large pollution sources, indicating the oxidized nature of most OA during the campaign. The evolution of OA elemental composition in the van Krevelen diagram (H/C vs. O/C) showed a slope of -0.63; however, the OA influenced by coal combustion exhibits a completely different evolution that appears dominated by physical mixing. The aging of organic aerosols vs. photochemical age was investigated. It was shown that OA/Delta CO, as well as LV-OOA/Delta CO and SV-OOA/Delta CO, positively correlated with photochemical age. LV-OOA accounted for 73% of the OA secondary formation (SOA) in the oldest plumes (photochemical age of 25 h). The kOH at Changdao, by assuming SOA formation and aging as a first-order process proportional to OH, was calculated to be 5.2x10(-12) cm(3) molec.(-1) s(-1), which is similar to those determined in recent studies of polluted air in other continents.

引用

页码：10095 / 10112

页数：18

共 62 条

[1] Mexico city aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) - Part 2: Analysis of the biomass burning contribution and the non-fossil carbon fraction [J].

Aiken, A. C. ;

de Foy, B. ;

Wiedinmyer, C. ;

DeCarlo, P. F. ;

Ulbrich, I. M. ;

Wehrli, M. N. ;

Szidat, S. ;

Prevot, A. S. H. ;

Noda, J. ;

Wacker, L. ;

Volkamer, R. ;

Fortner, E. ;

Wang, J. ;

Laskin, A. ;

Shutthanandan, V. ;

Zheng, J. ;

Zhang, R. ;

Paredes-Miranda, G. ;

Arnott, W. P. ;

Molina, L. T. ;

Sosa, G. ;

Querol, X. ;

Jimenez, J. L. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (12) :5315-5341

[2] Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) - Part 1: Fine particle composition and organic source apportionment [J].

Aiken, A. C. ;

Salcedo, D. ;

Cubison, M. J. ;

Huffman, J. A. ;

DeCarlo, P. F. ;

Ulbrich, I. M. ;

Docherty, K. S. ;

Sueper, D. ;

Kimmel, J. R. ;

Worsnop, D. R. ;

Trimborn, A. ;

Northway, M. ;

Stone, E. A. ;

Schauer, J. J. ;

Volkamer, R. M. ;

Fortner, E. ;

de Foy, B. ;

Wang, J. ;

Laskin, A. ;

Shutthanandan, V. ;

Zheng, J. ;

Zhang, R. ;

Gaffney, J. ;

Marley, N. A. ;

Paredes-Miranda, G. ;

Arnott, W. P. ;

Molina, L. T. ;

Sosa, G. ;

Jimenez, J. L. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (17) :6633-6653

[3] O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry [J].

Aiken, Allison C. ;

Decarlo, Peter F. ;

Kroll, Jesse H. ;

Worsnop, Douglas R. ;

Huffman, J. Alex ;

Docherty, Kenneth S. ;

Ulbrich, Ingrid M. ;

Mohr, Claudia ;

Kimmel, Joel R. ;

Sueper, Donna ;

Sun, Yele ;

Zhang, Qi ;

Trimborn, Achim ;

Northway, Megan ;

Ziemann, Paul J. ;

Canagaratna, Manjula R. ;

Onasch, Timothy B. ;

Alfarra, M. Rami ;

Prevot, Andre S. H. ;

Dommen, Josef ;

Duplissy, Jonathan ;

Metzger, Axel ;

Baltensperger, Urs ;

Jimenez, Jose L. .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (12) :4478-4485

[4] Contributions from transport, solid fuel burning and cooking to primary organic aerosols in two UK cities [J].

Allan, J. D. ;

Williams, P. I. ;

Morgan, W. T. ;

Martin, C. L. ;

Flynn, M. J. ;

Lee, J. ;

Nemitz, E. ;

Phillips, G. J. ;

Gallagher, M. W. ;

Coe, H. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (02) :647-668

[5] Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer [J].

Canagaratna, M. R. ;

Jayne, J. T. ;

Jimenez, J. L. ;

Allan, J. D. ;

Alfarra, M. R. ;

Zhang, Q. ;

Onasch, T. B. ;

Drewnick, F. ;

Coe, H. ;

Middlebrook, A. ;

Delia, A. ;

Williams, L. R. ;

Trimborn, A. M. ;

Northway, M. J. ;

DeCarlo, P. F. ;

Kolb, C. E. ;

Davidovits, P. ;

Worsnop, D. R. .

MASS SPECTROMETRY REVIEWS, 2007, 26 (02) :185-222

[6] Chase studies of particulate emissions from in-use New York City vehicles [J].

Canagaratna, MR ;

Jayne, JT ;

Ghertner, DA ;

Herndon, S ;

Shi, Q ;

Jimenez, JL ;

Silva, PJ ;

Williams, P ;

Lanni, T ;

Drewnick, F ;

Demerjian, KL ;

Kolb, CE ;

Worsnop, DR .

AEROSOL SCIENCE AND TECHNOLOGY, 2004, 38 (06) :555-573

[7] Elemental composition and oxidation of chamber organic aerosol [J].

Chhabra, P. S. ;

Ng, N. L. ;

Canagaratna, M. R. ;

Corrigan, A. L. ;

Russell, L. M. ;

Worsnop, D. R. ;

Flagan, R. C. ;

Seinfeld, J. H. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (17) :8827-8845

[8] Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies [J].

Cubison, M. J. ;

Ortega, A. M. ;

Hayes, P. L. ;

Farmer, D. K. ;

Day, D. ;

Lechner, M. J. ;

Brune, W. H. ;

Apel, E. ;

Diskin, G. S. ;

Fisher, J. A. ;

Fuelberg, H. E. ;

Hecobian, A. ;

Knapp, D. J. ;

Mikoviny, T. ;

Riemer, D. ;

Sachse, G. W. ;

Sessions, W. ;

Weber, R. J. ;

Weinheimer, A. J. ;

Wisthaler, A. ;

Jimenez, J. L. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (23) :12049-12064

[9] Budget of organic carbon in a polluted atmosphere: Results from the New England Air Quality Study in 2002 [J].

de Gouw, JA ;

Middlebrook, AM ;

Warneke, C ;

Goldan, PD ;

Kuster, WC ;

Roberts, JM ;

Fehsenfeld, FC ;

Worsnop, DR ;

Canagaratna, MR ;

Pszenny, AAP ;

Keene, WC ;

Marchewka, M ;

Bertman, SB ;

Bates, TS .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2005, 110 (D16) :1-22

[10] Organic Aerosols in the Earth's Atmosphere [J].

De Gouw, Joost ;

Jimenez, Jose L. .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2009, 43 (20) :7614-7618

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