GSTDTAP  > 地球科学
DOI10.5194/acp-17-8725-2017
Glyoxal yield from isoprene oxidation and relation to formaldehyde: chemical mechanism, constraints from SENEX aircraft observations, and interpretation of OMI satellite data
Miller, Christopher Chan1; Jacob, Daniel J.1,2; Marais, Eloise A.1; Yu, Karen2; Travis, Katherine R.2; Kim, Patrick S.1; Fisher, Jenny A.3,4; Zhu, Lei2; Wolfe, Glenn M.5,6; Hanisco, Thomas F.5; Keutsch, Frank N.2,7; Kaiser, Jennifer2,8; Min, Kyung-Eun9,10,13; Brown, Steven S.10,11; Washenfelder, Rebecca A.9,10; Abad, Gonzalo Gonzalez12; Chance, Kelly12
2017-07-18
发表期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
ISSN1680-7316
EISSN1680-7324
出版年2017
卷号17期号:14
文章类型Article
语种英语
国家USA; Australia; South Korea
英文摘要

Glyoxal (CHOCHO) is produced in the atmosphere by the oxidation of volatile organic compounds (VOCs). Like formaldehyde (HCHO), another VOC oxidation product, it is measurable from space by solar backscatter. Isoprene emitted by vegetation is the dominant source of CHOCHO and HCHO in most of the world. We use aircraft observations of CHOCHO and HCHO from the SENEX campaign over the southeast US in summer 2013 to better understand the CHOCHO time-dependent yield from isoprene oxidation, its dependence on nitrogen oxides (NOx equivalent to NO + NO2), the behavior of the CHOCHO-HCHO relationship, the quality of OMI CHOCHO satellite observations, and the implications for using CHOCHO observations from space as constraints on isoprene emissions. We simulate the SENEX and OMI observations with the Goddard Earth Observing System chemical transport model (GEOS-Chem) featuring a new chemical mechanism for CHOCHO formation from isoprene. The mechanism includes prompt CHOCHO formation under low-NOx conditions following the isomerization of the isoprene peroxy radical (ISOPO2). The SENEX observations provide support for this prompt CHOCHO formation pathway, and are generally consistent with the GEOS-Chem mechanism. Boundary layer CHOCHO and HCHO are strongly correlated in the observations and the model, with some departure under low-NOx conditions due to prompt CHOCHO formation. SENEX vertical profiles indicate a free-tropospheric CHOCHO background that is absent from the model. The OMI CHOCHO data provide some support for this free-tropospheric background and show southeast US enhancements consistent with the isoprene source but a factor of 2 too low. Part of this OMI bias is due to excessive surface reflectivities assumed in the retrieval. The OMI CHOCHO and HCHO seasonal data over the southeast US are tightly correlated and provide redundant proxies of isoprene emissions. Higher temporal resolution in future geostationary satellite observations may enable detection of the prompt CHOCHO production under low-NOx conditions apparent in the SENEX data.


领域地球科学
收录类别SCI-E
WOS记录号WOS:000405773900001
WOS关键词SOUTHEAST UNITED-STATES ; OZONE MONITORING INSTRUMENT ; AEROSOL EXTINCTION ; ORGANIC AEROSOL ; IN-SITU ; NITRATE CHEMISTRY ; TRANSPORT MODEL ; NORTH-AMERICA ; GLOBAL-SCALE ; EMISSIONS
WOS类目Environmental Sciences ; Meteorology & Atmospheric Sciences
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
引用统计
文献类型期刊论文
条目标识符http://119.78.100.173/C666/handle/2XK7JSWQ/17283
专题地球科学
作者单位1.Harvard Univ, Dept Earth & Planetary Sci, 20 Oxford St, Cambridge, MA 02138 USA;
2.Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA;
3.Univ Wollongong, Sch Chem, Wollongong, NSW, Australia;
4.Univ Wollongong, Sch Earth & Environm Sci, Wollongong, NSW, Australia;
5.NASA, Goddard Space Flight Ctr, Atmospher Chem & Dynam Lab, Greenbelt, MD USA;
6.Univ Maryland Baltimore Cty, Joint Ctr Earth Syst Technol, Baltimore, MD 21228 USA;
7.Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA;
8.Univ Wisconsin Madison, Dept Chem, Madison, WI USA;
9.Univ Colorado Boulder, Cooperat Inst Res Environm Sci, Boulder, CO USA;
10.NOAA, Earth Syst Res Lab, Chem Sci Div, Boulder, CO USA;
11.Univ Colorado, Dept Chem & Biochem, Campus Box 215, Boulder, CO 80309 USA;
12.Harvard Smithsonian Ctr Astrophys, 60 Garden St, Cambridge, MA 02138 USA;
13.Gwangju Inst Sci & Technol, Sch Earth Sci & Environm Engn, Gwangju, South Korea
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GB/T 7714
Miller, Christopher Chan,Jacob, Daniel J.,Marais, Eloise A.,et al. Glyoxal yield from isoprene oxidation and relation to formaldehyde: chemical mechanism, constraints from SENEX aircraft observations, and interpretation of OMI satellite data[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2017,17(14).
APA Miller, Christopher Chan.,Jacob, Daniel J..,Marais, Eloise A..,Yu, Karen.,Travis, Katherine R..,...&Chance, Kelly.(2017).Glyoxal yield from isoprene oxidation and relation to formaldehyde: chemical mechanism, constraints from SENEX aircraft observations, and interpretation of OMI satellite data.ATMOSPHERIC CHEMISTRY AND PHYSICS,17(14).
MLA Miller, Christopher Chan,et al."Glyoxal yield from isoprene oxidation and relation to formaldehyde: chemical mechanism, constraints from SENEX aircraft observations, and interpretation of OMI satellite data".ATMOSPHERIC CHEMISTRY AND PHYSICS 17.14(2017).
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