globalchange  > 影响、适应和脆弱性
DOI: 10.1002/jgrd.50533
论文题名:
Detailed chemical characterization of unresolved complex mixtures in atmospheric organics: Insights into emission sources, atmospheric processing, and secondary organic aerosol formation
作者: Chan A.W.H.; Isaacman G.; Wilson K.R.; Worton D.R.; Ruehl C.R.; Nah T.; Gentner D.R.; Dallmann T.R.; Kirchstetter T.W.; Harley R.A.; Gilman J.B.; Kuster W.C.; De Gouw J.A.; Offenberg J.H.; Kleindienst T.E.; Lin Y.H.; Rubitschun C.L.; Surratt J.D.; Hayes P.L.; Jimenez J.L.; Goldstein A.H.
刊名: Journal of Geophysical Research Atmospheres
ISSN: 21698996
出版年: 2013
卷: 118, 期:12
起始页码: 6783
结束页码: 6796
语种: 英语
英文关键词: gas chromatography mass spectrometry ; secondary organic aerosol ; semivolatile organic compounds ; unresolved complex mixture ; urban emissions
Scopus关键词: Aerosols ; Air quality ; Climate change ; Gas chromatography ; Gas emissions ; Isomers ; Linear transformations ; Mass spectrometry ; Mathematical transformations ; Mixtures ; Organic compounds ; Paraffins ; Photooxidation ; Rate constants ; Gas chromatography-mass spectrometry ; Secondary organic aerosols ; Semivolatile organic compounds ; Unresolved complex mixtures ; Urban emissions ; Atmospheric chemistry ; aerosol ; air quality ; atmospheric chemistry ; chemical composition ; climate change ; gas chromatography ; hydroxyl radical ; ionization ; mass spectrometry ; photooxidation ; urban area ; urban atmosphere ; urban population ; volatile organic compound ; California ; Pasadena ; United States
英文摘要: Recent studies suggest that semivolatile organic compounds (SVOCs) are important precursors to secondary organic aerosol (SOA) in urban atmospheres. However, knowledge of the chemical composition of SVOCs is limited by current analytical techniques, which are typically unable to resolve a large number of constitutional isomers. Using a combination of gas chromatography and soft photoionization mass spectrometry, we characterize the unresolved complex mixture (UCM) of semivolatile aliphatic hydrocarbons observed in Pasadena, California (~16 km NE of downtown Los Angeles), and Bakersfield, California, during the California Research at the Nexus of Air Quality and Climate Change 2010. To the authors' knowledge, this work represents the most detailed characterization of the UCM in atmospheric samples to date. Knowledge of molecular structures, including carbon number, alkyl branching, and number of rings, provides important constraints on the rate of atmospheric processing, as the relative amounts of branched and linear alkanes are shown to be a function of integrated exposure to hydroxyl radicals. Emissions of semivolatile branched alkanes from fossil fuel-related sources are up to an order of magnitude higher than those of linear alkanes, and the gas-phase OH rate constants of branched alkanes are ~30% higher than their linear isomers. Based on a box model considering gas/particle partitioning, emissions, and reaction rates, semivolatile branched alkanes are expected to play a more important role than linear alkanes in the photooxidation of the UCM and subsequent transformations into SOA. Detailed speciation of semivolatile compounds therefore provides essential understanding of SOA sources and formation processes in urban areas. Key Points Previously unresolved organics are characterized by molecular structures. Branched alkanes play an important role in oxidation of SVOCs to form SOA. Composition of UCM provides constraints on rate of atmospheric processing. © 2013. American Geophysical Union. All Rights Reserved.
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/63655
Appears in Collections:影响、适应和脆弱性
气候减缓与适应

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作者单位: Department of Environmental Science, Policy and Management, University of California, Berkeley, CA, United States; Department of Chemical Engineering and Applied Chemistry, University of Toronto, 200 College St., Toronto, ON M5S 3E5, Canada; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, United States; Aerosol Dynamics Inc., Berkeley, CA, United States; Department of Chemistry, University of California, Berkeley, CA, United States; Department of Civil and Environmental Engineering, University of California, Berkeley, CA, United States; Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory, Berkeley, CA, United States; Cooperative Institute for Research in the Environmental Sciences, University of Colorado Boulder, Boulder, CO, United States; Chemical Sciences Division, NOAA, Boulder, CO, United States; National Exposure Laboratory, Office of Research and Development, U.S. Environmental Protection Agency, Research Triangle Park, NC, United States; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, University of North Carolina at Chapel Hill, Chapel Hill, NC, United States; Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, CO, United States

Recommended Citation:
Chan A.W.H.,Isaacman G.,Wilson K.R.,et al. Detailed chemical characterization of unresolved complex mixtures in atmospheric organics: Insights into emission sources, atmospheric processing, and secondary organic aerosol formation[J]. Journal of Geophysical Research Atmospheres,2013-01-01,118(12)
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