期刊
JOURNAL OF MOLECULAR MODELING
卷 20, 期 6, 页码 -出版社
SPRINGER
DOI: 10.1007/s00894-014-2301-x
关键词
Activation of O-O bond; Apparent activation energy; Catalysis; Non-adiabatic reaction; Turnover frequency
类别
资金
- National Natural Science Foundation of China [21263023]
- Supercomputing Center of Gansu Province
Carbon monoxide (CO) and oxygen (O-2) catalyzed by small neutral iron oxide clusters (FeO1-3) was investigated at the density functional level of theory using the Becke-Perdew-Wang functional (BPW91). Three reaction pathways along with singlet, triplet and quintet states were calculated for ascertaining the presence of some spin inversion during the catalytic cycle. The catalytic cycle was found to be two state reactivity resulting from the crossing among the multistate energetic profiles. The Landau-Zener equation was used to calculate the thermally-averaged spin transition probabilities for the non-adiabatic surface crossing reaction. In order to predict the efficiency of catalyst the energetic span model developed by Kozuch was implemented, whereas this model is not suitable for handling the diabatic reaction, this feature we must take into consideration. To this end, a kinetic assessment is carried out with an expansion of the energetic span model, including the spin-crossing effects. This approximation enables one to measure the efficiency of catalytic cycle including spin-crossing effects by quantum mechanical computation.
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