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DOI | 10.1016/j.atmosenv.2012.11.036 |
Potential impacts of two SO2 oxidation pathways on regional sulfate concentrations: Aqueous-phase oxidation by NO2 and gas-phase oxidation by Stabilized Criegee Intermediates | |
Sarwar, Golam1; Fahey, Kathleen1; Kwok, Roger1; Gilliam, Robert C.1; Roselle, Shawn J.1; Mathur, Rohit1; Xue, Jian2; Yu, Jianzhen2; Carter, William P. L.3 | |
发表日期 | 2013-04-01 |
ISSN | 1352-2310 |
卷号 | 68页码:186-197 |
英文摘要 | We examine the potential impacts of two additional sulfate production pathways using the Community Multiscale Air Quality modeling system. First we evaluate the impact of the aqueous-phase oxidation of S(IV) by nitrogen dioxide using two published rate constants, differing by 1-2 orders of magnitude. The reaction with alternate high and low rate constants enhances monthly mean wintertime sulfate by 4-20% and 0.4-1.2% respectively. The reaction does not significantly impact summertime sulfate. The higher sulfate predictions in winter compare better with the observed data as the model tends to underpredict sulfate concentrations both in winter and summer. We also investigate the potential impact of the gas-phase oxidation of sulfur dioxide by the Stabilized Criegee Intermediate (SCI) using a recently measured rate constant for its reaction with sulfur dioxide. Model results indicate that the gas-phase oxidation of sulfur dioxide by the SCI does not significantly affect sulfate concentrations due to the competing reaction of the SCI with water vapor. The current estimate of the rate constant for the SCI reaction with water vapor is too high for the SCI reaction with sulfur dioxide to significantly affect sulfate production. However, a sensitivity analysis using a lower rate constant for the water vapor reaction suggests that the SCI reaction with sulfur dioxide could potentially enhance sulfate production in the model. Further study is needed to accurately measure the rate constants of the aqueous-phase oxidation of S(IV) by nitrogen dioxide and the gas-phase reaction of the SCI with water vapor. Published by Elsevier Ltd. |
英文关键词 | Sulfate;Aqueous chemistry;Criegee intermediate;SO2;NO2;Alkene;O-3 |
语种 | 英语 |
WOS记录号 | WOS:000315241100022 |
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/59584 |
作者单位 | 1.US EPA, Atmospher Modeling & Anal Div, Natl Exposure Res Lab, Res Triangle Pk, NC 27711 USA; 2.Hong Kong Univ Sci & Technol, Kowloon, Hong Kong, Peoples R China; 3.Univ Calif Riverside, CE CERT, Riverside, CA 92521 USA |
推荐引用方式 GB/T 7714 | Sarwar, Golam,Fahey, Kathleen,Kwok, Roger,et al. Potential impacts of two SO2 oxidation pathways on regional sulfate concentrations: Aqueous-phase oxidation by NO2 and gas-phase oxidation by Stabilized Criegee Intermediates[J]. 美国环保署,2013,68:186-197. |
APA | Sarwar, Golam.,Fahey, Kathleen.,Kwok, Roger.,Gilliam, Robert C..,Roselle, Shawn J..,...&Carter, William P. L..(2013).Potential impacts of two SO2 oxidation pathways on regional sulfate concentrations: Aqueous-phase oxidation by NO2 and gas-phase oxidation by Stabilized Criegee Intermediates.ATMOSPHERIC ENVIRONMENT,68,186-197. |
MLA | Sarwar, Golam,et al."Potential impacts of two SO2 oxidation pathways on regional sulfate concentrations: Aqueous-phase oxidation by NO2 and gas-phase oxidation by Stabilized Criegee Intermediates".ATMOSPHERIC ENVIRONMENT 68(2013):186-197. |
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