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DOI10.1029/2020JD032553
Global Atmospheric Budget of Acetone: Air-Sea Exchange and the Contribution to Hydroxyl Radicals
Wang S.; Apel E.C.; Schwantes R.H.; Bates K.H.; Jacob D.J.; Fischer E.V.; Hornbrook R.S.; Hills A.J.; Emmons L.K.; Pan L.L.; Honomichl S.; Tilmes S.; Lamarque J.-F.; Yang M.; Marandino C.A.; Saltzman E.S.; de Bruyn W.; Kameyama S.; Tanimoto H.; Omori Y.; Hall S.R.; Ullmann K.; Ryerson T.B.; Thompson C.R.; Peischl J.; Daube B.C.; Commane R.; McKain K.; Sweeney C.; Thames A.B.; Miller D.O.; Brune W.H.; Diskin G.S.; DiGangi J.P.; Wofsy S.C.
发表日期2020
ISSN2169897X
卷号125期号:15
英文摘要Acetone is one of the most abundant oxygenated volatile organic compounds (VOCs) in the atmosphere. The oceans impose a strong control on atmospheric acetone, yet the oceanic fluxes of acetone remain poorly constrained. In this work, the global budget of acetone is evaluated using two global models: CAM-chem and GEOS-Chem. CAM-chem uses an online air-sea exchange framework to calculate the bidirectional oceanic acetone fluxes, which is coupled to a data-oriented machine-learning approach. The machine-learning algorithm is trained using a global suite of seawater acetone measurements. GEOS-Chem uses a fixed surface seawater concentration of acetone to calculate the oceanic fluxes. Both model simulations are compared to airborne observations from a recent global-scale, multiseasonal campaign, the NASA Atmospheric Tomography Mission (ATom). We find that both CAM-chem and GEOS-Chem capture the measured acetone vertical distributions in the remote atmosphere reasonably well. The combined observational and modeling analysis suggests that (i) the ocean strongly regulates the atmospheric budget of acetone. The tropical and subtropical oceans are mostly a net source of acetone, while the high-latitude oceans are a net sink. (ii) CMIP6 anthropogenic emission inventory may underestimate acetone and/or its precursors in the Northern Hemisphere. (iii) The MEGAN biogenic emissions model may overestimate acetone and/or its precursors, and/or the biogenic oxidation mechanisms may overestimate the acetone yields. (iv) The models consistently overestimate acetone in the upper troposphere-lower stratosphere over the Southern Ocean in austral winter. (v) Acetone contributes up to 30–40% of hydroxyl radical production in the tropical upper troposphere/lower stratosphere. ©2020. American Geophysical Union. All Rights Reserved.
英文关键词acetone; air-sea exchange; HOx radicals; machine learning
语种英语
来源期刊Journal of Geophysical Research: Atmospheres
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/185882
作者单位Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, United States; Now at Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO, United States; Now at Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, United States; School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, United States; Department of Atmospheric Science, Colorado State University, Fort Collins, CO, United States; Climate and Global Dynamics, National Center for Atmospheric Research, Boulder, CO, United States; Plymouth Marine Laboratory, Plymouth, United Kingdom; Forschungsbereich Marine Biogeochemie, GEOMAR, Helmholtz-Zentrum für Ozeanforschung Kiel, Kiel, Germany; Department of Earth System Science, University of California, Irvine, CA, United States; Department of Chemistry, Schmid College of Science and Technology, Chapman University, Orange, CA, United State...
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Wang S.,Apel E.C.,Schwantes R.H.,et al. Global Atmospheric Budget of Acetone: Air-Sea Exchange and the Contribution to Hydroxyl Radicals[J],2020,125(15).
APA Wang S..,Apel E.C..,Schwantes R.H..,Bates K.H..,Jacob D.J..,...&Wofsy S.C..(2020).Global Atmospheric Budget of Acetone: Air-Sea Exchange and the Contribution to Hydroxyl Radicals.Journal of Geophysical Research: Atmospheres,125(15).
MLA Wang S.,et al."Global Atmospheric Budget of Acetone: Air-Sea Exchange and the Contribution to Hydroxyl Radicals".Journal of Geophysical Research: Atmospheres 125.15(2020).
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