DOI: 10.1002/2017JD027403
Scopus记录号: 2-s2.0-85041048325
论文题名: Observations and Explicit Modeling of Summertime Carbonyl Formation in Beijing: Identification of Key Precursor Species and Their Impact on Atmospheric Oxidation Chemistry
作者: Yang X. ; Xue L. ; Wang T. ; Wang X. ; Gao J. ; Lee S. ; Blake D.R. ; Chai F. ; Wang W.
刊名: Journal of Geophysical Research: Atmospheres
ISSN: 2169897X
出版年: 2018
卷: 123, 期: 2 起始页码: 1426
结束页码: 1440
语种: 英语
英文关键词: atmospheric oxidation chemistry
; carbonyls
; master chemical mechanism
; precursor species
; secondary formation
Scopus关键词: acetone
; atmospheric chemistry
; carbonyl compound
; chemical pollutant
; hydrocarbon
; identification key
; isoprene
; model validation
; oxidation
; ozone depletion
; photochemistry
; radical
; volatile organic compound
; Beijing [China]
; China
英文摘要: Carbonyls are an important group of volatile organic compounds (VOCs) that play critical roles in tropospheric chemistry. To better understand the formation mechanisms of carbonyl compounds, extensive measurements of carbonyls and related parameters were conducted in Beijing in summer 2008. Formaldehyde (11.17 ± 5.32 ppbv), acetone (6.98 ± 3.01 ppbv), and acetaldehyde (5.27 ± 2.24 ppbv) were the most abundant carbonyl species. Two dicarbonyls, glyoxal (0.68 ± 0.26 ppbv) and methylglyoxal (MGLY; 1.10 ± 0.44 ppbv), were also present in relatively high concentrations. An observation-based chemical box model was used to simulate the in situ production of formaldehyde, acetaldehyde, glyoxal, and MGLY and quantify their contributions to ozone formation and ROx budget. All four carbonyls showed similar formation mechanisms but exhibited different precursor distributions. Alkenes (mainly isoprene and ethene) were the dominant precursors of formaldehyde, while both alkenes (e.g., propene, i-butene, and cis-2-pentene) and alkanes (mainly i-pentane) were major precursors of acetaldehyde. For dicarbonyls, both isoprene and aromatic VOCs were the dominant parent hydrocarbons of glyoxal and MGLY. Photolysis of oxygenated VOCs was the dominant source of ROx radicals (approximately >80% for HO2 and approximately >70% for RO2) in Beijing. Ozone production occurred under a mixed-control regime with carbonyls being the key VOC species. Overall, this study provides some new insights into the formation mechanisms of carbonyls, especially their parent hydrocarbon species, and underlines the important role of carbonyls in radical chemistry and ozone pollution in Beijing. Reducing the emissions of alkenes and aromatics would be an effective way to mitigate photochemical pollution in Beijing. ©2018. American Geophysical Union. All Rights Reserved. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/114643
Appears in Collections: 气候减缓与适应
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作者单位: Environment Research Institute, Shandong University, Ji'nan, China; Department of Civil and Environmental Engineering, Hong Kong Polytechnic University, Hong Kong; Chinese Research Academy of Environmental Sciences, Beijing, China; Department of Chemistry, University of California, Irvine, CA, United States
Recommended Citation:
Yang X.,Xue L.,Wang T.,et al. Observations and Explicit Modeling of Summertime Carbonyl Formation in Beijing: Identification of Key Precursor Species and Their Impact on Atmospheric Oxidation Chemistry[J]. Journal of Geophysical Research: Atmospheres,2018-01-01,123(2)