Mass Spectral Analysis of Organic Aerosol Formed Downwind of the Deepwater Horizon Oil Spill: Field Studies and Laboratory Confirmations

被引：39

作者：

Bahreini, R. ^{[1
,2
]}

Middlebrook, A. M. ^{[2
]}

Brock, C. A. ^{[2
]}

de Gouw, J. A. ^{[1
,2
]}

McKeen, S. A. ^{[1
,2
]}

Williams, L. R. ^{[3
]}

Daumit, K. E. ^{[4
]}

Lambe, A. T. ^{[3
,5
]}

Massoli, P. ^{[3
]}

Canagaratna, M. R. ^{[3
]}

Ahmadov, R. ^{[1
,2
]}

Carrasquillo, A. J. ^{[4
]}

Cross, E. S. ^{[4
]}

Ervens, B. ^{[1
,2
]}

Holloway, J. S. ^{[1
,2
]}

Hunter, J. F. ^{[4
]}

Onasch, T. B. ^{[3
,5
]}

Pollack, I. B. ^{[1
,2
]}

Roberts, J. M. ^{[2
]}

Ryerson, T. B. ^{[2
]}

Warneke, C. ^{[1
,2
]}

Davidovits, P. ^{[5
]}

Worsnop, D. R. ^{[3
]}

Kroll, J. H. ^{[4
,6
]}

机构：

[1] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA

[2] NOAA, Div Chem Sci, Earth Syst Res Lab, Boulder, CO USA

[3] Aerodyne Res Inc, Billerica, MA 01821 USA

[4] MIT, Dept Civil & Environm Engn, Cambridge, MA 02139 USA

[5] Boston Coll, Dept Chem, Chestnut Hill, MA 02167 USA

[6] MIT, Dept Chem Engn, Cambridge, MA 02139 USA

来源：

ENVIRONMENTAL SCIENCE & TECHNOLOGY | 2012年 / 46卷 / 15期

基金：

美国国家科学基金会;

关键词：

ELEMENTAL COMPOSITION; HYDROCARBON-LIKE; SECONDARY; EMISSIONS; OXIDATION; AMBIENT; INLET; SOA; SEMIVOLATILE; SPECTROMETRY;

D O I：

10.1021/es301691k

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

In June 2010, the NOAA WP-3D aircraft conducted two survey flights around the Deepwater Horizon (DWH) oil spill. The Gulf oil spill resulted in an isolated source of secondary organic aerosol (SOA) precursors in a relatively clean environment. Measurements of aerosol composition and volatile organic species (VOCs) indicated formation of SOA from intermediate-volatility organic compounds (IVOCs) downwind of the oil spill (Science 2011, 331, doi 10.1126/science.1200320). In an effort to better understand formation of SOA in this environment, we present mass spectral characteristics of SOA in the Gulf and of SOA formed in the laboratory from evaporated light crude oil. Compared to urban primary organic aerosol, high-mass-resolution analysis of the background-subtracted SOA spectra in the Gulf (for short, "Gulf SOA") showed higher contribution of CxHyO+ relative to CxHy+ fragments at the same nominal mass. In each transect downwind of the DWH spill site, a gradient in the degree of oxidation of the Gulf SOA was observed: more oxidized SOA (oxygen/carbon = O/C similar to 0.4 was observed in the area impacted by fresher oil; less oxidized SOA (O/C similar to 0.3), with contribution from fragments with a hydrocarbon backbone, was found in a broader region of more-aged surface oil. Furthermore, in the plumes originating from the more-aged oil, contribution of oxygenated fragments to SOA decreased with downwind distance. Despite differences between experimental conditions in the laboratory and the ambient environment, mass spectra of SOA formed from gas-phase oxidation of crude oil by OH radicals in a smog chamber and a flow tube reactor strongly resembled the mass spectra of Gulf SOA (r(2) > 0.94). Processes that led to the observed Gulf SOA characteristics are also likely to occur in polluted regions where VOCs and IVOCs are coemitted.

引用

页码：8025 / 8034

页数：10

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