气候变化领域集成服务门户(CCPortal): On the sources and sinks of atmospheric VOCs: an integrated analysis of recent aircraft campaigns over North America

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DOI	10.5194/acp-19-9097-2019
	On the sources and sinks of atmospheric VOCs: an integrated analysis of recent aircraft campaigns over North America
	Chen X.; Millet D.B.; Singh H.B.; Wisthaler A.; Apel E.C.; Atlas E.L.; Blake D.R.; Bourgeois I.; Brown S.S.; Crounse J.D.; De Gouw J.A.; Flocke F.M.; Fried A.; Heikes B.G.; Hornbrook R.S.; Mikoviny T.; Min K.-E.; Müller M.; Andrew Neuman J.; O'sullivan D.W.; Peischl J.; Pfister G.G.; Richter D.; Roberts J.M.; Ryerson T.B.; Shertz S.R.; Thompson C.R.; Treadaway V.; Veres P.R.; Walega J.; Warneke C.; Washenfelder R.A.; Weibring P.; Yuan B.
发表日期	2019
ISSN	16807316
起始页码	9097
结束页码	9123
卷号	19 期号:14
英文摘要	We apply a high-resolution chemical transport model (GEOS-Chem CTM) with updated treatment of volatile organic compounds (VOCs) and a comprehensive suite of airborne datasets over North America to (i) characterize the VOC budget and (ii) test the ability of current models to capture the distribution and reactivity of atmospheric VOCs over this region. Biogenic emissions dominate the North American VOC budget in the model, accounting for 70 % and 95 % of annually emitted VOC carbon and reactivity, respectively. Based on current inventories anthropogenic emissions have declined to the point where biogenic emissions are the dominant summertime source of VOC reactivity even in most major North American cities. Methane oxidation is a 2× larger source of nonmethane VOCs (via production of formaldehyde and methyl hydroperoxide) over North America in the model than are anthropogenic emissions. However, anthropogenic VOCs account for over half of the ambient VOC loading over the majority of the region owing to their longer aggregate lifetime. Fires can be a significant VOC source episodically but are small on average. In the planetary boundary layer (PBL), the model exhibits skill in capturing observed variability in total VOC abundance (R2Combining double low line0.36) and reactivity (R2Combining double low line0.54). The same is not true in the free troposphere (FT), where skill is low and there is a persistent low model bias (ĝ1/4 60 %), with most (27 of 34) model VOCs underestimated by more than a factor of 2. A comparison of PBL : FT concentration ratios over the southeastern US points to a misrepresentation of PBL ventilation as a contributor to these model FT biases. We also find that a relatively small number of VOCs (acetone, methanol, ethane, acetaldehyde, formaldehyde, isoprene + oxidation products, methyl hydroperoxide) drive a large fraction of total ambient VOC reactivity and associated model biases; research to improve understanding of their budgets is thus warranted. A source tracer analysis suggests a current overestimate of biogenic sources for hydroxyacetone, methyl ethyl ketone and glyoxal, an underestimate of biogenic formic acid sources, and an underestimate of peroxyacetic acid production across biogenic and anthropogenic precursors. Future work to improve model representations of vertical transport and to address the VOC biases discussed are needed to advance predictions of ozone and SOA formation. © Author(s) 2019.
语种	英语
scopus关键词	aircraft emission; annual variation; atmospheric transport; concentration (composition); data set; integrated approach; seasonal variation; source apportionment; volatile organic compound; North America
来源期刊	Atmospheric Chemistry and Physics
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/144276
作者单位	Department of Soil, Water, and Climate, University of Minnesota, Minneapolis-Saint Paul, MN, United States; NASA Ames Research Center, Moffett Field, CA, United States; Institute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, 6020, Austria; Department of Chemistry, University of Oslo, Oslo, Norway; Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, United States; Department of Atmospheric Sciences, Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL, United States; Department of Chemistry, University of California, Irvine, Irvine, CA, United States; Chemical Sciences Division, NOAA Earth System Research Laboratory, Boulder, CO, United States; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, United States; Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, United States; Institute of Arctic a...
推荐引用方式 GB/T 7714	Chen X.,Millet D.B.,Singh H.B.,et al. On the sources and sinks of atmospheric VOCs: an integrated analysis of recent aircraft campaigns over North America[J],2019,19(14).
APA	Chen X..,Millet D.B..,Singh H.B..,Wisthaler A..,Apel E.C..,...&Yuan B..(2019).On the sources and sinks of atmospheric VOCs: an integrated analysis of recent aircraft campaigns over North America.Atmospheric Chemistry and Physics,19(14).
MLA	Chen X.,et al."On the sources and sinks of atmospheric VOCs: an integrated analysis of recent aircraft campaigns over North America".Atmospheric Chemistry and Physics 19.14(2019).