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
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
收藏
页码:10095 / 10112
页数:18
相关论文
共 62 条
[41]   Ozonolysis of α-pinene at atmospherically relevant concentrations:: Temperature dependence of aerosol mass fractions (yields) [J].
Pathak, Ravi K. ;
Stanier, Charles O. ;
Donahue, Neil M. ;
Pandis, Spyros N. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2007, 112 (D3)
[42]   Diurnal variations of ambient particulate wood burning emissions and their contribution to the concentration of Polycyclic Aromatic Hydrocarbons (PAHs) in Seiffen, Germany [J].
Poulain, L. ;
Iinuma, Y. ;
Mueller, K. ;
Birmili, W. ;
Weinhold, K. ;
Brueggemann, E. ;
Gnauk, T. ;
Hausmann, A. ;
Loeschau, G. ;
Wiedensohler, A. ;
Herrmann, H. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (24) :12697-12713
[43]   Rethinking organic aerosols: Semivolatile emissions and photochemical aging [J].
Robinson, Allen L. ;
Donahue, Neil M. ;
Shrivastava, Manish K. ;
Weitkamp, Emily A. ;
Sage, Amy M. ;
Grieshop, Andrew P. ;
Lane, Timothy E. ;
Pierce, Jeffrey R. ;
Pandis, Spyros N. .
SCIENCE, 2007, 315 (5816) :1259-1262
[44]   Aerosol mass spectrometer constraint on the global secondary organic aerosol budget [J].
Spracklen, D. V. ;
Jimenez, J. L. ;
Carslaw, K. S. ;
Worsnop, D. R. ;
Evans, M. J. ;
Mann, G. W. ;
Zhang, Q. ;
Canagaratna, M. R. ;
Allan, J. ;
Coe, H. ;
McFiggans, G. ;
Rap, A. ;
Forster, P. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (23) :12109-12136
[45]   Highly time- and size-resolved characterization of submicron aerosol particles in Beijing using an Aerodyne Aerosol Mass Spectrometer [J].
Sun, Junying ;
Zhang, Qi ;
Canagaratna, Manjula R. ;
Zhang, Yangmei ;
Ng, Nga L. ;
Sun, Yele ;
Jayne, John T. ;
Zhang, Xiaochun ;
Zhang, Xiaoye ;
Worsnop, Douglas R. .
ATMOSPHERIC ENVIRONMENT, 2010, 44 (01) :131-140
[46]   Characterization of the sources and processes of organic and inorganic aerosols in New York city with a high-resolution time-of-flight aerosol mass apectrometer [J].
Sun, Y. -L. ;
Zhang, Q. ;
Schwab, J. J. ;
Demerjian, K. L. ;
Chen, W. -N. ;
Bae, M. -S. ;
Hung, H. -M. ;
Hogrefe, O. ;
Frank, B. ;
Rattigan, O. V. ;
Lin, Y. -C. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (04) :1581-1602
[47]   Temperature dependence of secondary organic aerosol formation by photo-oxidation of hydrocarbons [J].
Takekawa, H ;
Minoura, H ;
Yamazaki, S .
ATMOSPHERIC ENVIRONMENT, 2003, 37 (24) :3413-3424
[48]  
Turpin BJ, 2001, AEROSOL SCI TECH, V35, P602, DOI 10.1080/02786820152051454
[49]   Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data [J].
Ulbrich, I. M. ;
Canagaratna, M. R. ;
Zhang, Q. ;
Worsnop, D. R. ;
Jimenez, J. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (09) :2891-2918
[50]   Global tropospheric NO2 column distributions:: Comparing three-dimensional model calculations with GOME measurements [J].
Velders, GJM ;
Granier, C ;
Portmann, RW ;
Pfeilsticker, K ;
Wenig, M ;
Wagner, T ;
Platt, U ;
Richter, A ;
Burrows, JP .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2001, 106 (D12) :12643-12660