Secondary organic aerosol (SOA) yields from NO3 radical + isoprene based on nighttime aircraft power plant plume transects

被引:54
作者
Fry, Juliane L. [1 ]
Brown, Steven S. [2 ,5 ]
Middlebrook, Ann M. [2 ]
Edwards, Peter M. [2 ,3 ,4 ]
Campuzano-Jost, Pedro [3 ,5 ]
Day, Douglas A. [3 ,5 ]
Jimenez, Jose L. [3 ,5 ]
Allen, Hannah M. [6 ]
Ryerson, Thomas B. [2 ]
Pollack, Ilana [2 ,3 ,7 ]
Graus, Martin [3 ,8 ]
Warneke, Carsten [2 ,3 ]
de Gouw, Joost A. [3 ,5 ]
Brock, Charles A. [2 ]
Gilman, Jessica [2 ,3 ]
Lerner, Brian M. [2 ,3 ,9 ]
Dube, William P. [2 ,3 ]
Liao, Jin [2 ,3 ,10 ,11 ]
Welti, Andre [2 ,3 ,12 ]
机构
[1] Reed Coll, Dept Chem, Portland, OR 97202 USA
[2] NOAA, Chem Sci Div, Earth Syst Res Lab, Boulder, CO USA
[3] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
[4] Univ York, Dept Chem, Wolfson Atmospher Chem Labs, York, N Yorkshire, England
[5] Univ Colorado, Dept Chem, Boulder, CO 80309 USA
[6] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
[7] Colorado State Univ, Dept Atmospher Sci, Ft Collins, CO 80523 USA
[8] Univ Innsbruck, Dept Atmospher & Cryospher Sci, Innsbruck, Austria
[9] Aerodyne Res Inc, Billerica, MA USA
[10] Univ Space Res Assoc, Columbia, MD USA
[11] NASA, Goddard Space Flight Ctr, Atmospher Chem & Dynam Lab, Greenbelt, MD USA
[12] Leibniz Inst Tropospher Res, Dept Phys, Leipzig, Germany
关键词
SOUTHEASTERN UNITED-STATES; MASS-SPECTROMETER; NITROGEN-OXIDES; ISOPRENE OXIDATION; NITRATE RADICALS; AIRCRAFT; AIR; CHEMISTRY; PERFORMANCE; VOLATILITY;
D O I
10.5194/acp-18-11663-2018
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Nighttime reaction of nitrate radicals (NO3) with biogenic volatile organic compounds (BVOC) has been proposed as a potentially important but also highly uncertain source of secondary organic aerosol (SOA). The southeastern United States has both high BVOC and nitrogen oxide (NOx) emissions, resulting in a large model-predicted NO3-BVOC source of SOA. Coal-fired power plants in this region constitute substantial NOx emissions point sources into a nighttime atmosphere characterized by high regionally widespread concentrations of isoprene. In this paper, we exploit nighttime aircraft observations of these power plant plumes, in which NO3 radicals rapidly remove isoprene, to obtain field-based estimates of the secondary organic aerosol yield from NO3 + isoprene. Observed in-plume increases in nitrate aerosol are consistent with organic nitrate aerosol production from NO3 + isoprene, and these are used to determine molar SOA yields, for which the average over nine plumes is 9% (+/- 5 %). Corresponding mass yields depend on the assumed molecular formula for isoprene-NO3-SOA, but the average over nine plumes is 27% (+/- 14 %), on average larger than those previously measured in chamber studies (12 %-14% mass yield as Delta OA/Delta VOC after oxidation of both double bonds). Yields are larger for longer plume ages. This suggests that ambient aging processes lead more effectively to condensable material than typical chamber conditions allow. We discuss potential mechanistic explanations for this difference, including longer ambient peroxy radical lifetimes and heterogeneous reactions of NO3-isoprene gas phase products. More in-depth studies are needed to better understand the aerosol yield and oxidation mechanism of NO3 radical + isoprene, a coupled anthropogenic-biogenic source of SOA that may be regionally significant.
引用
收藏
页码:11663 / 11682
页数:20
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