Size-resolved aerosol chemistry on Whistler Mountain, Canada with a high-resolution aerosol mass spectrometer during INTEX-B

被引:86
作者
Sun, Y. [1 ]
Zhang, Q. [1 ]
Macdonald, A. M. [2 ]
Hayden, K. [2 ]
Li, S. M. [2 ]
Liggio, J. [2 ]
Liu, P. S. K. [2 ]
Anlauf, K. G. [2 ]
Leaitch, W. R. [2 ]
Steffen, A. [2 ]
Cubison, M. [3 ]
Worsnop, D. R. [4 ]
van Donkelaar, A. [5 ]
Martin, R. V. [5 ]
机构
[1] SUNY Albany, Atmospher Sci Res Ctr, 251 Fuller Rd, Albany, NY 12203 USA
[2] Environm Canada, Toronto, ON, Canada
[3] Univ Colorado, Boulder, CO USA
[4] Aerodyne Res Inc, Billerica, MA 01821 USA
[5] Dalhousie Univ, Halifax, NS, Canada
关键词
OXYGENATED ORGANIC AEROSOLS; BEAM WIDTH PROBE; AMBIENT AEROSOL; AIR-POLLUTION; HYDROCARBON-LIKE; FINE PARTICLES; TRANSPORT; ASIA; EMISSIONS; SPECIATION;
D O I
10.5194/acp-9-3095-2009
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the peak of Whistler Mountain (2182 m above sea level), British Columbia, from 19 April to 16 May 2006, as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign. The mass concentrations and size distributions of non-refractory submicron particle (NR-PM1) species (i.e., sulfate, nitrate, ammonium, chloride, and organics) were measured in situ at 10-min time resolution. The HR-ToF-AMS results agreed well with collocated measurements. The average concentration of non-refractory submicron particulate matter (NR-PM1; 1.9 mu g m(-3)) is similar to those observed at other remote, high elevation sites in North America. Episodes of enhanced aerosol loadings were observed, due to influences of regional and trans-Pacific transport of air pollution. Organics and sulfate were the dominant species, on average accounting for 55% and 30%, respectively, of the NR-PM1 mass. The average size distributions of sulfate and ammonium both showed an accumulation mode peaking at similar to 500 nm in vacuum aerodynamic diameter (D-va) while those of organic aerosol (OA) and nitrate peaked at similar to 300 nm. The size differences suggested that sulfate and OA were mostly present in external mixtures from different source origins. We also quantitatively determined the elemental composition of OA using the high resolution mass spectra. Overall, OA at Whistler Peak was highly oxygenated, with an average organic-mass-to-organic-carbon ratio (OM/OC) of 2.28 +/- 0.23 and an atomic ratio of oxygen-to-carbon (O/C) of 0.83 +/- 0.17. The nominal formula for OA was C1H1.66N0.03O0.83 for the entire study. Two significant trans-Pacific dust events originated from Asia were observed at Whistler Peak during this study. While both events were characterized with significant enhancements of coarse mode particles and mineral contents, the composition and characteristics of NR-PM1 were significantly different between them. One trans-Pacific event occurred on 15 May 2006, during which ammonium sulfate contributed >90% of the total NR-PM1 mass. This event was followed by a high OA episode likely associated with regional emissions. In total, three enhanced regional OA events, each of which lasted 2 3 days, were observed during this study. In contrast to the two dust events, the regional OA events were generally characterized with higher OA/sulfate ratio, less oxidized OA, and lower OM/OC ratio.
引用
收藏
页码:3095 / 3111
页数:17
相关论文
共 61 条
[1]   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
[2]   Elemental analysis of organic species with electron ionization high-resolution mass spectrometry [J].
Aiken, Allison. C. ;
DeCarlo, Peter F. ;
Jimenez, Jose L. .
ANALYTICAL CHEMISTRY, 2007, 79 (21) :8350-8358
[3]   Characterization of urban and rural organic particulate in the lower Fraser valley using two aerodyne aerosol mass spectrometers [J].
Alfarra, MR ;
Coe, H ;
Allan, JD ;
Bower, KN ;
Boudries, H ;
Canagaratna, MR ;
Jimenez, JL ;
Jayne, JT ;
Garforth, AA ;
Li, SM ;
Worsnop, DR .
ATMOSPHERIC ENVIRONMENT, 2004, 38 (34) :5745-5758
[4]   Submicron aerosol composition at Trinidad Head, California, during ITCT 2K2: Its relationship with gas phase volatile organic carbon and assessment of instrument performance [J].
Allan, JD ;
Bower, KN ;
Coe, H ;
Boudries, H ;
Jayne, JT ;
Canagaratna, MR ;
Millet, DB ;
Goldstein, AH ;
Quinn, PK ;
Weber, RJ ;
Worsnop, DR .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2004, 109 (D23) :1-16
[5]   Quantitative sampling using an Aerodyne aerosol mass spectrometer - 1. Techniques of data interpretation and error analysis [J].
Allan, JD ;
Jimenez, JL ;
Williams, PI ;
Alfarra, MR ;
Bower, KN ;
Jayne, JT ;
Coe, H ;
Worsnop, DR .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D3)
[6]   A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data [J].
Allan, JD ;
Delia, AE ;
Coe, H ;
Bower, KN ;
Alfarra, MR ;
Jimenez, JL ;
Middlebrook, AM ;
Drewnick, F ;
Onasch, TB ;
Canagaratna, MR ;
Jayne, JT ;
Worsnop, DR .
JOURNAL OF AEROSOL SCIENCE, 2004, 35 (07) :909-922
[7]   Interference of organic signals in highly time resolved nitrate measurements by low mass resolution aerosol mass spectrometry [J].
Bae, Min-Suk ;
Schwab, James J. ;
Zhang, Qi ;
Hogrefe, Olga ;
Demerjian, Kenneth L. ;
Weimer, Silke ;
Rhoads, Kevin ;
Orsini, Doug ;
Venkatachari, Prasanna ;
Hopke, Philip K. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2007, 112 (D22)
[8]   Design and operation of a pressure-controlled inlet for airborne sampling with an aerodynamic aerosol lens [J].
Bahreini, Roya ;
Dunlea, Edward J. ;
Matthew, Brendan M. ;
Simons, Craig ;
Docherty, Kenneth S. ;
DeCarlo, Peter F. ;
Jimenez, Jose L. ;
Brock, Charles A. ;
Middlebrook, Ann M. .
AEROSOL SCIENCE AND TECHNOLOGY, 2008, 42 (06) :465-471
[9]   Atmospheric organochlorine pesticides in the western Canadian Arctic: Evidence of transpacific transport [J].
Bailey, R ;
Barrie, LA ;
Halsall, CJ ;
Fellin, P ;
Muir, DCG .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2000, 105 (D9) :11805-11811
[10]   Particle characteristics following cloud-modified transport from Asia to North America -: art. no. D23S26 [J].
Brock, CA ;
Hudson, PK ;
Lovejoy, ER ;
Sullivan, A ;
Nowak, JB ;
Huey, LG ;
Cooper, OR ;
Cziczo, DJ ;
de Gouw, J ;
Fehsenfeld, FC ;
Holloway, JS ;
Hübler, G ;
Lafleur, BG ;
Murphy, DM ;
Neuman, JA ;
Nicks, DK ;
Orsini, DA ;
Parrish, DD ;
Ryerson, TB ;
Tanner, DJ ;
Warneke, C ;
Weber, RJ ;
Wilson, JC .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2004, 109 (D23) :1-17