Combined multi-level quantum mechanics theories and molecular mechanics study of water-induced transition state of OH-+CO2 reaction in aqueous solution

doi:10.1088/1674-1056/26/10/103401

中国物理B ›› 2017, Vol. 26 ›› Issue (10): 103401-103401.doi: 10.1088/1674-1056/26/10/103401

• ATOMIC AND MOLECULAR PHYSICS • 上一篇下一篇

Combined multi-level quantum mechanics theories and molecular mechanics study of water-induced transition state of OH^-+CO₂ reaction in aqueous solution

Chen Li(李琛), Meixing Niu(牛美兴), Peng Liu(刘鹏), Yongfang Li(李永方), Dunyou Wang(王敦友)

College of Physics and Electronics, Shandong Normal University, Ji'nan 250014, China

收稿日期:2017-05-22 修回日期:2017-07-06 出版日期:2017-10-05 发布日期:2017-10-05
通讯作者: Dunyou Wang E-mail:dywang@sdnu.edu.cn
基金资助:
Project supported by the National Natural Science Foundation of China (Grant No. 11374194) and Taishan Scholarship Fund from Shandong Province, China.

Combined multi-level quantum mechanics theories and molecular mechanics study of water-induced transition state of OH^-+CO₂ reaction in aqueous solution

Chen Li(李琛), Meixing Niu(牛美兴), Peng Liu(刘鹏), Yongfang Li(李永方), Dunyou Wang(王敦友)

College of Physics and Electronics, Shandong Normal University, Ji'nan 250014, China

Received:2017-05-22 Revised:2017-07-06 Online:2017-10-05 Published:2017-10-05
Contact: Dunyou Wang E-mail:dywang@sdnu.edu.cn
Supported by:
Project supported by the National Natural Science Foundation of China (Grant No. 11374194) and Taishan Scholarship Fund from Shandong Province, China.

摘要/Abstract

摘要：

The presence of a solvent interacting with a system brings about qualitative changes from the corresponding gas-phase reactions. A solvent can not only change the energetics along the reaction pathway, but also radically alter the reaction mechanism. Here, we investigated the water-induced transition state of the OH^-+CO₂→HCO₃^- reaction using a multi-level quantum mechanics and molecular mechanics method with an explicit water model. The solvent energy contribution along the reaction pathway has a maximum value which induces the highest energy point on the potential of mean force. The charge transfer from OH^- to CO₂ results in the breaking of the OH^- solvation shell and the forming of the CO₂ solvation shell. The loss of hydrogen bonds in the OH^- solvation shell without being compensated by the formation of hydrogen bonds in the CO₂ solvation shell induces the transition state in the aqueous solution. The calculated free energy reaction barrier at the CCSD(T)/MM level of theory, 11.8 kcal/mol, agrees very well with the experimental value, 12.1 kcal/mol.

关键词: transition state, reaction pathway, free energy barrier, solvent effect

Abstract:

Key words: transition state, reaction pathway, free energy barrier, solvent effect

中图分类号: (Interatomic and intermolecular potentials and forces, potential energy surfaces for collisions)

34.20.-b

34.20.Cf (Interatomic potentials and forces) 34.20.Gj (Intermolecular and atom-molecule potentials and forces) 34.50.Lf (Chemical reactions)

李琛, 牛美兴, 刘鹏, 李永方, 王敦友. Combined multi-level quantum mechanics theories and molecular mechanics study of water-induced transition state of OH^-+CO₂ reaction in aqueous solution[J]. 中国物理B, 2017, 26(10): 103401-103401.

Chen Li(李琛), Meixing Niu(牛美兴), Peng Liu(刘鹏), Yongfang Li(李永方), Dunyou Wang(王敦友). Combined multi-level quantum mechanics theories and molecular mechanics study of water-induced transition state of OH^-+CO₂ reaction in aqueous solution[J]. Chin. Phys. B, 2017, 26(10): 103401-103401.

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Combined multi-level quantum mechanics theories and molecular mechanics study of water-induced transition state of OH^-+CO₂ reaction in aqueous solution

Combined multi-level quantum mechanics theories and molecular mechanics study of water-induced transition state of OH^-+CO₂ reaction in aqueous solution

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