The hydrogen abstraction reaction from H_(2)S by OH is of key importance in understanding of the causes of acid rain,air pollution,and climate change.In this work,the reaction OH+H_(2)S→H_(2)O+SH is investigated on a...The hydrogen abstraction reaction from H_(2)S by OH is of key importance in understanding of the causes of acid rain,air pollution,and climate change.In this work,the reaction OH+H_(2)S→H_(2)O+SH is investigated on a recently developed ab initio-based globally accurate potential energy surface by the time-dependent wave packet approach under a reduceddimensional model.This reaction behaves like a barrier-less reaction at low collision energies and like an activated reaction with a well-defined barrier at high collision energies.Exciting either the symmetric or antisymmetric stretching mode of the molecule H_(2)S enhances the reactivity more than exciting the bending mode,which is rationalized by the coupling strength of each normal mode with the reaction coordinate.In addition,the modespecific rate constant shows a remarkable non-Arrhenius temperature dependence.展开更多
基金supported by the National Natural Science Foundation of China(No.21973109 to Hongwei Song,No.21773297,No.21973108,and No.21921004 to Minghui Yang)the Ministry of Education,Singapore,under its Academic Research Fund Tier 1(RG83/20)to Yunpeng Lu。
文摘The hydrogen abstraction reaction from H_(2)S by OH is of key importance in understanding of the causes of acid rain,air pollution,and climate change.In this work,the reaction OH+H_(2)S→H_(2)O+SH is investigated on a recently developed ab initio-based globally accurate potential energy surface by the time-dependent wave packet approach under a reduceddimensional model.This reaction behaves like a barrier-less reaction at low collision energies and like an activated reaction with a well-defined barrier at high collision energies.Exciting either the symmetric or antisymmetric stretching mode of the molecule H_(2)S enhances the reactivity more than exciting the bending mode,which is rationalized by the coupling strength of each normal mode with the reaction coordinate.In addition,the modespecific rate constant shows a remarkable non-Arrhenius temperature dependence.
