期刊
ACS CATALYSIS
卷 6, 期 8, 页码 5508-5519出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b01080
关键词
spinel cobalt oxides; DFT; methane combustion; C-H bond activation; multiple active sites
资金
- NSFC [21333003, 21303051]
- Shanghai Natural Science Foundation [13ZR1453000]
- Fundamental Research Funds for the Central Universities
A complete catalytic cycle for methane combustion on the Co3O4(110) surface was investigated and compared with that on the Co3O4(100) surface on the basis of first-principles calculations. It is found that the 2-fold coordinated lattice oxygen (O-2c) would be of vital importance for methane combustion over Co3O4 surfaces, especially for the first two C-H bond activations and the C-O bond coupling. It could explain the reason the Co3O4(110) surface significantly outperforms the Co3O4(100) surface without exposed O-2c for methane combustion. More importantly, it is found that the cooperation of homogeneous multiple sites for multiple elementary steps would be indispensable. It not only facilitates the hydrogen transfer between different sites for the swift formation of H2O to effectively avoid the passivation of the active low-coordinated O-2c site but also stabilizes surface intermediates during the methane oxidation, optimizing the reaction channel. An understanding of this cooperation of multiple active sites not only might be beneficial in developing improved catalysts for methane combustion but also might shed light on one advantage of heterogeneous catalysts with multiple sites in comparison to single-site catalysts for catalytic activity.
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