Highly time-resolved chemical characterization of atmospheric submicron particles during 2008 Beijing Olympic Games using an Aerodyne High-Resolution Aerosol Mass Spectrometer

被引:260
作者
Huang, X. -F. [1 ]
He, L. -Y. [1 ]
Hu, M. [2 ]
Canagaratna, M. R. [3 ]
Sun, Y. [4 ]
Zhang, Q. [4 ]
Zhu, T. [2 ]
Xue, L. [1 ]
Zeng, L. -W. [1 ]
Liu, X. -G. [2 ]
Zhang, Y. -H. [2 ]
Jayne, J. T. [3 ]
Ng, N. L. [3 ]
Worsnop, D. R. [3 ]
机构
[1] Peking Univ, Shenzhen Grad Sch, Sch Environm & Energy, Key Lab Urban Habitat Environm Sci & Technol, Shenzhen, Peoples R China
[2] Peking Univ, Coll Environm Sci & Engn, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100871, Peoples R China
[3] Aerodyne Res Inc, Billerica, MA 01821 USA
[4] Univ Calif Davis, Dept Environm Toxicol, Davis, CA 95616 USA
基金
美国国家科学基金会; 中国国家自然科学基金;
关键词
POSITIVE MATRIX FACTORIZATION; PARTICULATE ORGANIC-MATTER; SOURCE APPORTIONMENT; MEXICO-CITY; EMISSIONS; AMBIENT; URBAN; PM2.5; VOLATILITY; COMPONENTS;
D O I
10.5194/acp-10-8933-2010
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
As part of Campaigns of Air Quality Research in Beijing and Surrounding Region-2008 (CAREBeijing-2008), an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed in urban Beijing to characterize submicron aerosol particles during the time of 2008 Beijing Olympic Games and Paralympic Games (24 July to 20 September 2008). The campaign mean PM1 mass concentration was 63.1 +/- 39.8 mu g m(-3); the mean composition consisted of organics (37.9%), sulfate (26.7%), ammonium (15.9%), nitrate (15.8%), black carbon (3.1%), and chloride (0.87%). The average size distributions of the species (except BC) were all dominated by an accumulation mode peaking at about 600 nm in vacuum aerodynamic diameter, and organics was characterized by an additional smaller mode extending below 100 nm. Positive Matrix Factorization (PMF) analysis of the high resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., hydrocarbon-like (HOA), cooking-related (COA), and two oxygenated organic aerosols (OOA-1 and OOA-2), which on average accounted for 18.1, 24.4, 33.7 and 23.7% of the total organic mass, respectively. The HOA was identified to be closely associated with primary combustion sources, while the COA mass spectrum and diurnal pattern showed similar characteristics to that measured for cooking emissions. The OOA components correspond to aged secondary organic aerosol. Although the two OOA components have similar elemental (O/C, H/C) compositions, they display differences in mass spectra and time series which appear to correlate with the different source regions sampled during the campaign. Back trajectory clustering analysis indicated that the southerly air flows were associated with the highest PM1 pollution during the campaign. Aerosol particles in southern airmasses were especially rich in inorganic and oxidized organic species. Aerosol particles in northern airmasses contained a large fraction of primary HOA and COA species, probably due to stronger influences from local emissions. The lowest concentration levels for all major species were obtained during the Olympic game days (8 to 24 August 2008), possibly due to the effects of both strict emission controls and favorable meteorological conditions.
引用
收藏
页码:8933 / 8945
页数:13
相关论文
共 64 条
  • [1] 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
    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.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (17) : 6633 - 6653
  • [2] O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry
    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.
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (12) : 4478 - 4485
  • [3] Elemental analysis of organic species with electron ionization high-resolution mass spectrometry
    Aiken, Allison. C.
    DeCarlo, Peter F.
    Jimenez, Jose L.
    [J]. ANALYTICAL CHEMISTRY, 2007, 79 (21) : 8350 - 8358
  • [4] Identification of the mass spectral signature of organic aerosols from wood burning emissions
    Alfarra, M. Rami
    Prevot, Andre S. H.
    Szidat, Sonke
    Sandradewi, Jisca
    Weimer, Silke
    Lanz, Valentin A.
    Schreiber, Daniel
    Mohr, Martin
    Baltensperger, Urs
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2007, 41 (16) : 5770 - 5777
  • [5] Characterization of urban and rural organic particulate in the lower Fraser valley using two aerodyne aerosol mass spectrometers
    Alfarra, MR
    Coe, H
    Allan, JD
    Bower, KN
    Boudries, H
    Canagaratna, MR
    Jimenez, JL
    Jayne, JT
    Garforth, AA
    Li, SM
    Worsnop, DR
    [J]. ATMOSPHERIC ENVIRONMENT, 2004, 38 (34) : 5745 - 5758
  • [6] Quantitative sampling using an Aerodyne aerosol mass spectrometer - 2. Measurements of fine particulate chemical composition in two U.K. cities
    Allan, JD
    Alfarra, MR
    Bower, KN
    Williams, PI
    Gallagher, MW
    Jimenez, JL
    McDonald, AG
    Nemitz, E
    Canagaratna, MR
    Jayne, JT
    Coe, H
    Worsnop, DR
    [J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D3)
  • [7] Quantitative sampling using an Aerodyne aerosol mass spectrometer - 1. Techniques of data interpretation and error analysis
    Allan, JD
    Jimenez, JL
    Williams, PI
    Alfarra, MR
    Bower, KN
    Jayne, JT
    Coe, H
    Worsnop, DR
    [J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D3)
  • [8] A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data
    Allan, JD
    Delia, AE
    Coe, H
    Bower, KN
    Alfarra, MR
    Jimenez, JL
    Middlebrook, AM
    Drewnick, F
    Onasch, TB
    Canagaratna, MR
    Jayne, JT
    Worsnop, DR
    [J]. JOURNAL OF AEROSOL SCIENCE, 2004, 35 (07) : 909 - 922
  • [9] [Anonymous], ATMOS CHEM PHYS DISC
  • [10] Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer
    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.
    [J]. MASS SPECTROMETRY REVIEWS, 2007, 26 (02) : 185 - 222