VOC emissions, evolutions and contributions to SOA formation at a receptor site in eastern China

被引:238
作者
Yuan, B. [1 ]
Hu, W. W. [1 ]
Shao, M. [1 ]
Wang, M. [1 ]
Chen, W. T. [1 ]
Lu, S. H. [1 ]
Zeng, L. M. [1 ]
Hu, M. [1 ]
机构
[1] Peking Univ, Coll Environm Sci & Engn, State Joint Key Lab Environm Simulat & Pollut Con, Beijing 100871, Peoples R China
关键词
SECONDARY ORGANIC AEROSOL; POLYCYCLIC AROMATIC-HYDROCARBONS; MEXICO-CITY; RURAL SITE; PHOTOOXIDATION; OXIDATION; PARTICLES; ALKANES; OUTFLOW; RATIOS;
D O I
10.5194/acp-13-8815-2013
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Volatile organic compounds (VOCs) were measured by two online instruments (GC-FID/MS and PTR-MS) at a receptor site on Changdao Island (37.99 degrees N, 120.70 degrees E) in eastern China. Reaction with OH radical dominated chemical losses of most VOC species during the Changdao campaign. A photochemical-age-based parameterization method is used to calculate VOC emission ratios and to quantify the evolution of ambient VOCs. The calculated emission ratios of most hydrocarbons agree well with those obtained from emission inventory data, but determined emission ratios of oxygenated VOCs (OVOCs) are significantly higher than those from emission inventory data. The photochemical-age-based parameterization method is also used to investigate primary emissions and secondary formation of organic aerosol. The primary emission ratio of organic aerosol (OA) to CO is determined to be 14.9 mu g m(-3) ppm(-1), and secondary organic aeorosols (SOA) are produced at an enhancement ratio of 18.8 mu g m(-3) ppm(-1) to CO after 50 h of photochemical processing in the atmosphere. SOA formation is significantly higher than the level determined from VOC oxidation under both high-NOx (2.0 mu g m(-3) ppm(-1) CO) and low-NOx conditions (6.5 mu g m(-3) ppm(-1) CO). Polycyclic aromatic hydrocarbons (PAHs) and higher alkanes (>C10) account for as high as 17.4% of SOA formation, which suggests semi-volatile organic compounds (SVOCs) may be a large contributor to SOA formation during the Changdao campaign. The SOA formation potential of primary VOC emissions determined from field campaigns in Beijing and Pearl River Delta (PRD) is lower than the measured SOA levels reported in the two regions, indicating SOA formation is also beyond explainable by VOC oxidation in the two city clusters.
引用
收藏
页码:8815 / 8832
页数:18
相关论文
共 69 条
[1]   Chemical evolution of volatile organic compounds in the outflow of the Mexico City Metropolitan area [J].
Apel, E. C. ;
Emmons, L. K. ;
Karl, T. ;
Flocke, F. ;
Hills, A. J. ;
Madronich, S. ;
Lee-Taylor, J. ;
Fried, A. ;
Weibring, P. ;
Walega, J. ;
Richter, D. ;
Tie, X. ;
Mauldin, L. ;
Campos, T. ;
Weinheimer, A. ;
Knapp, D. ;
Sive, B. ;
Kleinman, L. ;
Springston, S. ;
Zaveri, R. ;
Ortega, J. ;
Voss, P. ;
Blake, D. ;
Baker, A. ;
Warneke, C. ;
Welsh-Bon, D. ;
de Gouw, J. ;
Zheng, J. ;
Zhang, R. ;
Rudolph, J. ;
Junkermann, W. ;
Riemer, D. D. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (05) :2353-2375
[2]   Atmospheric degradation of volatile organic compounds [J].
Atkinson, R ;
Arey, J .
CHEMICAL REVIEWS, 2003, 103 (12) :4605-4638
[3]   Organic aerosol formation in urban and industrial plumes near Houston and Dallas, Texas [J].
Bahreini, R. ;
Ervens, B. ;
Middlebrook, A. M. ;
Warneke, C. ;
de Gouw, J. A. ;
DeCarlo, P. F. ;
Jimenez, J. L. ;
Brock, C. A. ;
Neuman, J. A. ;
Ryerson, T. B. ;
Stark, H. ;
Atlas, E. ;
Brioude, J. ;
Fried, A. ;
Holloway, J. S. ;
Peischl, J. ;
Richter, D. ;
Walega, J. ;
Weibring, P. ;
Wollny, A. G. ;
Fehsenfeld, F. C. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2009, 114
[4]   Carbonyl and nitrogen dioxide emissions from gasoline- and diesel-powered motor vehicles [J].
Ban-Weiss, George A. ;
Mclaughlin, John P. ;
Harley, Robert A. ;
Kean, Andrew J. ;
Grosjean, Eric ;
Grosjean, Daniel .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (11) :3944-3950
[5]   Measurements of volatile organic compounds at a suburban ground site (T1) in Mexico City during the MILAGRO 2006 campaign: measurement comparison, emission ratios, and source attribution [J].
Bon, D. M. ;
Ulbrich, I. M. ;
de Gouw, J. A. ;
Warneke, C. ;
Kuster, W. C. ;
Alexander, M. L. ;
Baker, A. ;
Beyersdorf, A. J. ;
Blake, D. ;
Fall, R. ;
Jimenez, J. L. ;
Herndon, S. C. ;
Huey, L. G. ;
Knighton, W. B. ;
Ortega, J. ;
Springston, S. ;
Vargas, O. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (06) :2399-2421
[6]   Secondary organic aerosol from biogenic VOCs over West Africa during AMMA [J].
Capes, G. ;
Murphy, J. G. ;
Reeves, C. E. ;
McQuaid, J. B. ;
Hamilton, J. F. ;
Hopkins, J. R. ;
Crosier, J. ;
Williams, P. I. ;
Coe, H. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (12) :3841-3850
[7]   Secondary organic aerosol formation from photooxidation of naphthalene and alkylnaphthalenes: implications for oxidation of intermediate volatility organic compounds (IVOCs) [J].
Chan, A. W. H. ;
Kautzman, K. E. ;
Chhabra, P. S. ;
Surratt, J. D. ;
Chan, M. N. ;
Crounse, J. D. ;
Kuerten, A. ;
Wennberg, P. O. ;
Flagan, R. C. ;
Seinfeld, J. H. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (09) :3049-3060
[8]   Organic Aerosol Formation Downwind from the Deepwater Horizon Oil Spill [J].
de Gouw, J. A. ;
Middlebrook, A. M. ;
Warneke, C. ;
Ahmadov, R. ;
Atlas, E. L. ;
Bahreini, R. ;
Blake, D. R. ;
Brock, C. A. ;
Brioude, J. ;
Fahey, D. W. ;
Fehsenfeld, F. C. ;
Holloway, J. S. ;
Le Henaff, M. ;
Lueb, R. A. ;
McKeen, S. A. ;
Meagher, J. F. ;
Murphy, D. M. ;
Paris, C. ;
Parrish, D. D. ;
Perring, A. E. ;
Pollack, I. B. ;
Ravishankara, A. R. ;
Robinson, A. L. ;
Ryerson, T. B. ;
Schwarz, J. P. ;
Spackman, J. R. ;
Srinivasan, A. ;
Watts, L. A. .
SCIENCE, 2011, 331 (6022) :1295-1299
[9]   Sources of particulate matter in the northeastern United States in summer: 1. Direct emissions and secondary formation of organic matter in urban plumes [J].
de Gouw, J. A. ;
Brock, C. A. ;
Atlas, E. L. ;
Bates, T. S. ;
Fehsenfeld, F. C. ;
Goldan, P. D. ;
Holloway, J. S. ;
Kuster, W. C. ;
Lerner, B. M. ;
Matthew, B. M. ;
Middlebrook, A. M. ;
Onasch, T. B. ;
Peltier, R. E. ;
Quinn, P. K. ;
Senff, C. J. ;
Stohl, A. ;
Sullivan, A. P. ;
Trainer, M. ;
Warneke, C. ;
Weber, R. J. ;
Williams, E. J. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2008, 113 (D8)
[10]   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