Kinetics investigation of the hydrogen abstraction reaction between CH3SS and CN radicals
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- 作者：Liu Yan ; Wang Wenliang ; Liu Zhongwen ; Ren Hongjiang
- 关键词：CH3SS ; CN ; Hydrogen abstraction reaction ; DFT
- 刊名：Journal of Molecular Modeling
- 出版年：2016
- 出版时间：January 2016
- 年：2016
- 卷：22
- 期：1
- 全文大小：1,350 KB
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Wang Wenliang (1)
Liu Zhongwen (1)
Ren Hongjiang (3)
1. School of Chemistry and Chemical Engineering, Key Laboratory for Macromolecular Science of Shaanxi Province, Shaanxi Normal University, Xi’an, Shaanxi, 710062, People’s Republic of China
2. College of Chemistry and Environment, Shaanxi Engineering Research Center of Coal Conversion Alcohol, Weinan Normal University, Weinan, Shaanxi, 714099, People’s Republic of China
3. School of Chemistry and Chemical Engineering, Xi’an University, Xi’an, Shaanxi, 710065, People’s Republic of China - 刊物类别：Chemistry and Materials Science
- 刊物主题：Chemistry
Computer Applications in Chemistry
Biomedicine
Molecular Medicine
Health Informatics and Administration
Life Sciences
Computer Application in Life Sciences - 出版者：Springer Berlin / Heidelberg
- ISSN：0948-5023
文摘
The reaction mechanisms and rates for the H abstraction reactions between CH3SS and CN radicals in the gas phase were investigated with density functional theory (DFT) methods. The geometries, harmonic vibrational frequencies, and energies of all stationary points were obtained at B3PW91/6-311G(d,p) level of theory. Relationships between the reactants, intermediates, transition states and products were confirmed, with the frequency and the intrinsic reaction coordinate (IRC) analysis at the same theoretical level. High accurate energy information was provided by the G3(MP2) method combined with the standard statistical thermodynamics. Gibbs free energies at 298.15 K for all of the reaction steps were reported, and were used to describe the profile diagrams of the potential energy surface. The rate constants were evaluated with both the classical transition state theory and the canonical variational transition state theory, in which the small-curvature tunneling correction was included. A total number of 9 intermediates (IMs) and 17 transition states (TSs) were obtained. It is shown that IM1 is the most stable intermediate by the largest energy release, and the channel of CH3SS + CN → IM3 → TS10 → P1(CH2SS + HCN) is the dominant reaction with the lowest energy barrier of 144.7 kJ mol−1. The fitted Arrhenius expressions of the calculated CVT/SCT rate constants for the rate-determining step of the favorable channel is k =7.73 × 106 T 1.40exp(−14,423.8/T) s−1 in the temperature range of 200–2000 K. The apparent activation energy E a(app.) for the main channel is −102.5 kJ mol−1, which is comparable with the G3(MP2) energy barrier of −91.8 kJ mol−1 of TS10 (relative to the reactants).