引用本文:
【打印本页】   【HTML】   【下载PDF全文】   View/Add Comment  【EndNote】   【RefMan】   【BibTex】
←前一篇|后一篇→ 过刊浏览    高级检索
本文已被:浏览 274次   下载 261 本文二维码信息
码上扫一扫!
分享到: 微信 更多
Quantum Chemical Study of Potential Energy Surface in the Formation of Atmospheric Sulfuric Acid
Emily L. Tao,Jessica Y. Li,Samantha Soriano,Fu-Ming Tao*
Author NameAffiliationE-mail
Emily L. Tao Department of Chemistry and Biochemistry, California State University, Fullerton, 800 N. State College Blvd. Fullerton, CA 92834, USA  
Jessica Y. Li Department of Chemistry and Biochemistry, California State University, Fullerton, 800 N. State College Blvd. Fullerton, CA 92834, USA  
Samantha Soriano Department of Chemistry and Biochemistry, California State University, Fullerton, 800 N. State College Blvd. Fullerton, CA 92834, USA  
Fu-Ming Tao* Department of Chemistry and Biochemistry, California State University, Fullerton, 800 N. State College Blvd. Fullerton, CA 92834, USA ftao@fullerton.edu 
Abstract:
A new potential energy surface (PES) for the atmospheric formation of sulfuric acid from OH+SO2 is investigated using density functional theory and high-level ab initio molecular orbital theory. A pathway focused on the new PES assumes the reaction to take place between the radical complex SO3·HO2 and H2O. The unusual stability of SO3·HO2 is the principal basis of the new pathway, which has the same final outcome as the current reaction mechanism in the literature but it avoids the production and complete release of SO3. The entire reaction pathway is composed of three consecutive elementary steps:(1) HOSO2+O2→SO3·HO2, (2) SO3·HO2+H2O→SO3·H2O·HO2, (3) SO3·H2O·HO2→H2SO4+HO2. All three steps have small energy barriers, under 10 kcal/mol, and are exothermic, and the new pathway is therefore favorable both kinetically and thermodynamically. As a key step of the reactions, step (3), HO2 serves as a bridge molecule for low-barrier hydrogen transfer in the hydrolysis of SO3. Two significant atmospheric implications are expected from the present study. First, SO3 is not released from the oxidation of SO2 by OH radical in the atmosphere. Second, the conversion of SO2 into sulfuric acid is weakly dependent on the humidity of air.
Key words:  Quantum chemistry  Atmospheric chemistry  Sulfur dioxide  Sulfuric acid  Computational chemistry  Density functional theory  Ab initio methods
FundProject:This work was partially funded by National Science Foundation of the United States (No.1012994) and by California State University, Fullerton.
大气中硫酸生成反应势能面的量子化学研究
陶琳,李宇杰,萨曼莎-索里亚诺,陶福明*
摘要:
关键词:  
DOI:10.1063/1674-0068/31/cjcp1805126
分类号: