DOI: 10.1016/j.atmosenv.2013.12.013
Scopus记录号: 2-s2.0-84891912692
论文题名: Impact of sulfur dioxide oxidation by Stabilized Criegee Intermediate on sulfate
作者: Sarwar G ; , Simon H ; , Fahey K ; , Mathur R ; , Goliff W ; S ; , Stockwell W ; R
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2014
卷: 85 起始页码: 204
结束页码: 214
语种: 英语
英文关键词: Alkene
; Oxidation
; Ozone
; Stabilized Criegee Intermediate
; Sulfate
; Sulfur dioxide
; Water
Scopus关键词: Biogenic emission
; Carbon bond
; Chemical mechanism
; Community multi-scale air quality models
; Criegee intermediates
; Sulfate
; Sulfur dioxide oxidation
; Water dimers
; Air quality
; Dimers
; Forecasting
; Hydrocarbons
; Olefins
; Oxidation
; Ozone
; Rate constants
; Sulfur
; Sulfur dioxide
; Water
; Reaction intermediates
; alkene
; dimer
; ozone
; sulfate
; sulfur dioxide
; sulfuric acid
; water
; aerosol
; air quality
; alkene
; atmospheric chemistry
; biogenic emission
; emission inventory
; oxidation
; ozone
; sensitivity analysis
; sulfate
; sulfur dioxide
; sulfuric acid
; aerosol
; air quality
; article
; chemical bond
; chemistry
; gas
; oxidation
; priority journal
; simulation
; United States
Scopus学科分类: Environmental Science: Water Science and Technology
; Earth and Planetary Sciences: Earth-Surface Processes
; Environmental Science: Environmental Chemistry
英文摘要: We revise the Carbon Bond chemical mechanism to explicitly represent three Stabilized Criegee Intermediates (SCIs) and their subsequent reactions with sulfur dioxide, water monomer, and water dimer, and incorporate the reactions into the Community Multiscale Air Quality model. The reaction of sulfur dioxide with SCI produces sulfuric acid which partitions into sulfate. We examine the impact of sulfur dioxide oxidation by SCI on sulfate using two different measured rate constants for the reaction of sulfur dioxide and SCI. When we use the higher rate constant and emissions estimates from the Biogenic Emissions Inventory System, it enhances monthly mean sulfate in summer by ~20% in biogenically active areas. Enhancements are driven primarily by SCI produced from the reactions of biogenically derived alkenes and ozone. The use of the lower rate constant only marginally enhances sulfate since it is 65 times lower than the higher rate constant. We performed several sensitivity analyses to investigate the impacts of uncertain biogenic emissions and SCI loss rates. When we use the higher rate constant and emissions estimates from the Model of Emissions of Gases and Aerosols from Nature, it enhances monthly mean sulfate by ~75%. A simulation using the lowest reported rate constant for the reaction of SCI and water indicated the maximum enhancement of sulfate from this chemistry was up to 4μg/m3 over a 24-hperiod in some locations in the Southeastern U.S. Predictions without the SCI reaction are lower than observed sulfate while predictions with the SCI reaction improve the agreements with observations. © 2013. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/80770
Appears in Collections: 气候变化事实与影响
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作者单位: Atmospheric Modeling and Analysis Division, National Exposure Research Laboratory, U.S. Environmental Protection Agency, 109 T.W. Alexander Drive, RTP, NC 27711, United States; Office of Air Quality Planning and Standards, U.S. Environmental Protection Agency, Research Triangle Park, NC, United States; College of Engineering Center for Environmental Research and Technology, University of California at Riverside, Riverside, CA 92507, United States; Department of Chemistry, Howard University, Washington, DC 20059, United States
Recommended Citation:
Sarwar G,, Simon H,, Fahey K,et al. Impact of sulfur dioxide oxidation by Stabilized Criegee Intermediate on sulfate[J]. Atmospheric Environment,2014-01-01,85