Citation: WANG Yong-Cheng, JIA Yi-Ming, WANG Wen-Xue, MA Pan-Pan. Theoretical Investigation for Two-state Reactivity of CO₂ Hydrogenation Catalyzed by Ru in Gas Phase[J]. Chinese Journal of Structural Chemistry, ;2016, 35(12): 1819-1828. doi: 10.14102/j.cnki.0254-5861.2011-1119 shu

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

College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070, China

Corresponding author: WANG Yong-Cheng, ycwang@163.com
Received Date: 8 January 2016

Fund Project: National Natural Science Foundation of China 21263023

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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.
- two-state reactivity(TSR),
- carbon dioxide hydrogenation,
- minimum energy crossing point (MECP),
- transition metal catalyzed,
- intersystem crossing (ISC)
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Theoretical Investigation for Two-state Reactivity of CO2 Hydrogenation Catalyzed by Ru in Gas Phase

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通讯作者: 陈斌, bchen63@163.com

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