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DOI10.1016/j.atmosenv.2013.12.013
Impact of sulfur dioxide oxidation by Stabilized Criegee Intermediate on sulfate
Sarwar, Golam1; Simon, Heather2; Fahey, Kathleen1; Mathur, Rohit1; Goliff, Wendy S.3; Stockwell, William R.4
发表日期2014-03-01
ISSN1352-2310
卷号85页码:204-214
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 similar to 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 similar to 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 4 mu g/m(3) over a 24-h period 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. Published by Elsevier Ltd.


英文关键词Stabilized Criegee Intermediate;Alkene;Ozone;Sulfur dioxide;Sulfate;Water;Oxidation
语种英语
WOS记录号WOS:000331417700023
来源期刊ATMOSPHERIC ENVIRONMENT
来源机构美国环保署
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/59636
作者单位1.US EPA, Natl Exposure Res Lab, Atmospher Modeling & Anal Div, Res Triangle Pk, NC 27711 USA;
2.US EPA, Off Air Qual Planning & Stand, Res Triangle Pk, NC 27711 USA;
3.Univ Calif Riverside, Ctr Environm Res & Technol, Coll Engn, Riverside, CA 92507 USA;
4.Howard Univ, Dept Chem, Washington, DC 20059 USA
推荐引用方式
GB/T 7714
Sarwar, Golam,Simon, Heather,Fahey, Kathleen,et al. Impact of sulfur dioxide oxidation by Stabilized Criegee Intermediate on sulfate[J]. 美国环保署,2014,85:204-214.
APA Sarwar, Golam,Simon, Heather,Fahey, Kathleen,Mathur, Rohit,Goliff, Wendy S.,&Stockwell, William R..(2014).Impact of sulfur dioxide oxidation by Stabilized Criegee Intermediate on sulfate.ATMOSPHERIC ENVIRONMENT,85,204-214.
MLA Sarwar, Golam,et al."Impact of sulfur dioxide oxidation by Stabilized Criegee Intermediate on sulfate".ATMOSPHERIC ENVIRONMENT 85(2014):204-214.
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