Insights into the chemistry of new particle formation and growth events in Pittsburgh based on aerosol mass spectrometry

被引:207
作者
Zhang, Q
Stanier, CO
Canagaratna, MR
Jayne, JT
Worsnop, DR
Pandis, SN
Jimenez, JL [1 ]
机构
[1] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
[2] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA
[3] Carnegie Mellon Univ, Dept Chem Engn, Pittsburgh, PA 15213 USA
[4] Aerodyne Res Inc, Billerica, MA 01821 USA
关键词
D O I
10.1021/es035417u
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
New particle formation and growth events have been observed in several urban areas and are of concern due to their potential negative effects on human health. The main purpose of this study was to investigate the chemistry of ultrafine particles during the growth phase of the frequently observed nucleation events in Pittsburgh (similar to100 events per year) and therefore infer the mechanisms of new particle growth in the urban troposphere. An Aerodyne aerosol mass spectrometer (AMS) and two SMPS systems were deployed at the U.S. EPA Pittsburgh Supersite during September 2002. Significant nucleation events were observed in 3 out of the 16 days of this deployment, including one of the 10 strongest nucleation events observed in Pittsburgh over a period of 15 months. These events appear to be representative of the climatology of new particle formation and growth in the Pittsburgh region. Distinctive growth of sulfate, ammonium, organics, and nitrate in the ultrafine mode(33-60nm in a vacuum aerodynamic diameter or similar to18-33 nm in physical diameter) was observed during each of these three events, with sulfate always being the first (and the fastest) species to increase. Ultrafine ammonium usually increased 10-40 min later than sulfate, causing the ultrafine mode particles to be more acidic during the initial stages of the nucleation events. Significant increase of ultrafine organics often happened after 11:00 a.m., when photochemistry is more intense. This observation coupled with a parallel increase of ultrafine m/z 44, a mass fragment generally representative of oxygenated organic compounds, indicates that secondary organic species contribute significantly to the growth of particles at a relatively later time of the event. Among all these four species, nitrate was always a minor component of the ultrafine particles and contributed the least to the new particle growth.
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页码:4797 / 4809
页数:13
相关论文
共 52 条
[1]   Disproportionate impact of particulate emissions on global cloud condensation nuclei concentrations [J].
Adams, PJ ;
Seinfeld, JH .
GEOPHYSICAL RESEARCH LETTERS, 2003, 30 (05)
[2]   Observations of new particle formation in urban air [J].
Alam, A ;
Shi, JP ;
Harrison, RM .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D3)
[3]  
ALFARRA MR, IN PRESS ATMOS ENV
[4]   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)
[5]   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
[6]  
Baron P.A., 2001, AEROSOL MEASUREMENT, V2nd
[7]   Atmospheric particle number size distribution in central Europe: Statistical relations to air masses and meteorology [J].
Birmili, W ;
Wiedensohler, A ;
Heintzenberg, J ;
Lehmann, K .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2001, 106 (D23) :32005-32018
[8]   Ultrafine particles in the atmosphere: introduction [J].
Brown, LM ;
Collings, N ;
Harrison, RM ;
Maynard, AD ;
Maynard, RL .
PHILOSOPHICAL TRANSACTIONS OF THE ROYAL SOCIETY OF LONDON SERIES A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES, 2000, 358 (1775) :2563-2565
[9]   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
[10]   Ultrafine (nanometre) particle mediated lung injury [J].
Donaldson, K ;
Li, XY ;
MacNee, W .
JOURNAL OF AEROSOL SCIENCE, 1998, 29 (5-6) :553-560