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

doi:10.1016/S1872-2067(14)60037-1

Abstract

Abstract:

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.

Key words: Nitrogen monoxide, Ethane, Cycle reaction, Density functional theory, Two-state reaction, Intersystem cross, Energetic span, Turnover frequency

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.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(14)60037-1

https://www.cjcatal.com/EN/Y2014/V35/I4/579

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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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