Ab initio study of sulfur isotope fractionation in the reaction of OCS with OH

被引：27

作者：

Danielache, Sebastian O. ^{[1
]}

Johnson, Matthew S. ^{[2
]}

Nanbu, Shinkoh ^{[3
]}

Grage, Mette M. -L. ^{[2
]}

McLinden, Chris ^{[4
]}

Yoshida, Naohiro ^{[1
,5
,6
]}

机构：

[1] Tokyo Inst Technol, Interdisciplinary Grad Sch Sci & Engn, Dept Environm Sci & Technol, Midori Ku, Yokohama, Kanagawa 2268502, Japan

[2] Univ Copenhagen, Dept Chem, DK-2100 Copenhagen, Denmark

[3] Kyushu Univ, Comp & Commun Ctr, Stn Collaborat Res 2, Higashi Ku, Fukuoka 8128512, Japan

[4] Meteorol Serv Canada, Downsview, ON, Canada

[5] Japan Sci & Technol Agcy JST, SORST Project, Kawaguchi, Saitama 3320012, Japan

[6] Tokyo Inst Technol, Interdisciplinary Grad Sch Sci & Engn, Dept Environm Chem & Engn, Yokohama, Kanagawa 2268502, Japan

来源：

CHEMICAL PHYSICS LETTERS | 2008年 / 450卷 / 4-6期

关键词：

D O I：

10.1016/j.cplett.2007.11.054

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The fractionation of sulfur isotopes in the gas-phase reaction of OCS with OH was calculated by ab initio methods. The first reaction step occurs through a carbon bonded OH-OCS transition state. The activation barrier is 18.4 kJ mol(-1) (CCSD(T)/aug-cc-pVDZ level plus zero-point energy) relative to the reactants. Fractionation constants are -1.4, -2.6 and -6.3 parts per thousand for S-33, S-34 and S-36 respectively. These results bring new insight regarding the origin of stratospheric sulfate aerosols, including the identification of characteristic isotopic fractionations in the lower and middle stratosphere. (C) 2007 Elsevier B.V. All rights reserved.

引用

页码：214 / 220

页数：7

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