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
1. [1]
2. [2]
3. [3]
4. [4]
5. [5]
6. [6]
7. [7]
8. [8]
9. [9]
10. [10]
11. [11]
12. [12]
13. [13]
14. [14]
15. [15]
16. [16]
17. [17]
18. [18]
19. [19]
20. [20]
21. [21]
22. [22]
23. [23]
24. [24]
25. [25]
26. [26]
27. [27]
28. [28]
29. [29]
30. [30]
31. [31]
32. [32]
33. [33]
34. [34]
35. [35]
36. [36]
37. [37]
38. [38]
39. [39]
40. [40]
41. [41]
42. [42]
43. [43]
44. [44]
45. [45]
46. [46]
47. [47]
48. [48]
49. [49]
50. [50]
51. [51]
52. [52]
53. [53]
54. [54]
55. [55]
56. [56]
57. [57]
58. [58]
59. [59]
60. [60]
61. [61]
62. [62]
63. [63]
64. [64]
65. [65]
66. [66]
67. [67]
68. [68]
69. [69]
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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