Theoretical Investigation for Two-state Reactivity of CO2 Hydrogenation Catalyzed by Ru in Gas Phase

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Gas-phase CO2 catalyzed activation hydrogenation by Ru atoms was studied with density functional theory. Based on the structure optimization of different potential energy surfaces, there are two crossing points between singlet and triplet potential energy surfaces and there is a crossing point between quintet and triplet potential energy surfaces in the whole catalytic cycle. Spin transition probabilities in the vicinity of the intersections have been calculated by the Landau-Zener model theory. There are three minimum energy crossing points (MECPs) with strong spin-orbital coupling effect and higher spin transition probability, and all spin inversion occurred in s orbital and different d orbitals of ruthenium, indicating this is a typical two-state reactivity (TSR) reaction. Finally, the lowest energy reaction path is ensured.

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	王永成
	贾义明
	王文雪
	马盼盼

关键词 ： two-state reactivity(TSR), carbon dioxide hydrogenation, minimum energy crossing point (MECP), transition metal catalyzed, intersystem crossing (ISC)

Abstract：

Key words： two–state reactivity(TSR) Carbon dioxide hydrogenation minimum energy crossing point (MECP) transition metal catalyzed intersystem crossing(ISC)

收稿日期: 2016-01-08 出版日期: 2016-12-12

基金资助:

This project was supported by the National Natural Science Foundation of China (21263023)

通讯作者: ycwang@163.com E-mail: ycwang@163.com

引用本文:

王永成;贾义明;王文雪;马盼盼. Theoretical Investigation for Two-state Reactivity of CO2 Hydrogenation Catalyzed by Ru in Gas Phase[J]. 结构化学, 2016, 35(12): 1819-1828.
WANG Yong-Cheng;JIA Yi-Ming;WANG Wen-Xue;MA Pan-Pan . two-state reactivity(TSR)|carbon dioxide hydrogenation|minimum energy crossing point (MECP)|transition metal catalyzed|intersystem crossing (ISC). CHINESE JOURNAL OF STRUCTURAL CHEMISTRY, 2016, 35(12): 1819-1828.

链接本文:

http://manu30.magtech.com.cn/jghx/CN/ 或 http://manu30.magtech.com.cn/jghx/CN/Y2016/V35/I12/1819

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