Citation: Jingjing Wu, Yongcheng Wang, Jun Cai, Yanzi Jin, Huanjiang Wang, Yanzhen Gan. Theoretical investigation into the Co⁺ catalytic activity in the cycle reaction of N₂O with C₂H₆ in the gas phase[J]. Chinese Journal of Catalysis, ;2014, 35(4): 579-589. doi: 10.1016/S1872-2067(14)60037-1 shu

Theoretical investigation into the Co⁺ catalytic activity in the cycle reaction of N₂O with C₂H₆ in the gas phase

1.
Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070, Gansu, China

Corresponding author: Yongcheng Wang,
Received Date: 18 November 2013
Available Online: 15 January 2014
Fund Project: 国家自然科学基金(21263023). (21263023)

The spin-forbidden mechanism of the reaction between N₂O and C₂H₆ catalyzed by Co⁺ has been investigated using UB3LYP density functional theory. The Harvey method has been applied to optimize five minimum energy crossing points (MECP) on both triplet and quintet potential energy surfaces. Possible spin inversion processes are discussed by means of spin-orbit coupling calculations. According to the calculation of probability of electron hopping using the Landau-Zener formula, effective intersystem crossing may occur at each MECP. The energetic span model proposed by Kozuch has been applied to the catalytic cycles, and shows the turnover frequency reaches 3.35×10^-21 s^-1 when Co⁺ catalyzes the reaction to produce CH₃CHO at 298K.
- Nitrogen monoxide,
- Ethane,
- Cycle reaction,
- Density functional theory,
- Two-state reaction,
- Intersystem cross,
- Energetic span,
- Turnover frequency
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Theoretical investigation into the Co+ catalytic activity in the cycle reaction of N2O with C2H6 in the gas phase

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Theoretical investigation into the Co⁺ catalytic activity in the cycle reaction of N₂O with C₂H₆ in the gas phase