Theoretical study of the crystal plane effect and ion-pair active center for C-H bond activation by Co3O4 nanocrystals

doi:10.1016/S1872-2067(14)60043-7

Chinese Journal of Catalysis ›› 2014, Vol. 35 ›› Issue (4): 462-467.DOI: 10.1016/S1872-2067(14)60043-7

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Theoretical study of the crystal plane effect and ion-pair active center for C-H bond activation by Co₃O₄ nanocrystals

Yanggang Wang^a, Xiaofeng Yang^a,b, Linhua Hu^a, Yadong Li^a, Jun Li^a

a Department of Chemistry, Tsinghua University, Beijing 100084, China;
b State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2013-12-29 Revised:2014-01-20 Online:2014-03-20 Published:2014-03-21
Supported by:
This work was supported by the State Key Project of Fundamental Research for Nanoscience and Nanotechnology (2011CB932401) and the National Natural Science Foundation of China (21221062, 10979031).

Abstract

Abstract:

Methane has attracted extensive interest in recent years due to its potential application as a replacement of oil and a feedstock for valuable chemicals. Due to the large C-H bond energy, the conversion of methane into useful products has been a challenge. In the present study, density functional theory (DFT) calculations were performed to study the activation of the C-H bond of methane on the (001) and (011) planes of Co₃O₄, which showed that CH₄ activation on Co₃O₄ nanocrystals was fairly easy with only small energy barriers (less than 1.1 eV). Surface Co-O ion pairs are the active site for C-H bond activation, where the two ions provide a synergistic effect for the activation of the strong C-H bond and yield surface Co-CH₃ and O-H species. The Co₃O₄(011) surface is shown to be more reactive for C-H bond activation than the Co₃O₄(001) surface, which is consistent with previous experimental results. Our results suggest that methane oxidation on Co₃O₄ nanocrystals has strong crystal plane effect and structure sensitivity and the ion-pair active center plays a significant role in activating the strong C-H bond.

Key words: C-H bond activation, Methane conversion, Crystal plane effect, Microkinetic analysis, Ion-pair active center

Yanggang Wang, Xiaofeng Yang, Linhua Hu, Yadong Li, Jun Li. Theoretical study of the crystal plane effect and ion-pair active center for C-H bond activation by Co₃O₄ nanocrystals[J]. Chinese Journal of Catalysis, 2014, 35(4): 462-467.

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Theoretical study of the crystal plane effect and ion-pair active center for C-H bond activation by Co₃O₄ nanocrystals

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