Citation: Wende Hu, Zheng-Jiang Shao, Xiao-Ming Cao, P. Hu. Multi sites vs single site for catalytic combustion of methane over Co₃O₄(110): A first-principles kinetic Monte Carlo study[J]. Chinese Journal of Catalysis, ;2020, 41(9): 1369-1377. doi: 10.1016/S1872-2067(20)63563-X shu

Multi sites vs single site for catalytic combustion of methane over Co₃O₄(110): A first-principles kinetic Monte Carlo study

a Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, China;
b School of Chemistry and Chemical Engineering, The Queen's University of Belfast, Belfast, BT9 5AG, U. K

Received Date: 17 January 2020
Revised Date: 20 February 2020

Fund Project: This work was supported by the National Natural Science Foundation of China (21673072, 91845111), and the Program of Shanghai Subject Chief Scientist (17XD1401400).

Single-atom catalysts have been applied in many processes recently. The difference of their kinetic behavior compared to the traditional heterogeneous catalysts has not been extensively discussed yet. Herein a complete catalytic cycle of CH₄ combustion assuming to be confined at isolated single sites of the Co₃O₄(110) surface is computationally compared with that on multi sites. The macroscopic kinetic behaviors of CH₄ combustion on Co₃O₄(110) is systematically and quantitatively compared between those on the single site and multi sites utilizing kinetic Monte Carlo simulations upon the energetic information from the PBE + U calculation and statistic mechanics. The key factors governing the kinetics of CH₄ combustion are disclosed for both the catalytic cycles respectively following the single-site and multi-site mechanisms. It is found that cooperation of multi active sites can promote the activity of complete CH₄ combustions substantially in comparison to separated single-site catalyst whereas the confinement of active sites could regulate the selectivity of CH₄ oxidation. The quantitative understanding of catalytic mechanism paves the way to improve the activity and selectivity for CH₄ oxidation.
- Methane combustion,
- DFT,
- Single atom catalyst,
- Multi site,
- Single site,
- Spinel cobalt oxides,
- Kinetic Monte Carlo
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通讯作者: 陈斌, bchen63@163.com

Multi sites vs single site for catalytic combustion of methane over Co₃O₄(110): A first-principles kinetic Monte Carlo study