Citation: Chang Huang, Zhi-Qiang Wang, Xue-Qing Gong. Activity and selectivity of propane oxidative dehydrogenation over VO₃/CeO₂(111) catalysts: A density functional theory study[J]. Chinese Journal of Catalysis, ;2018, 39(9): 1520-1526. doi: 10.1016/S1872-2067(18)63072-4 shu

Activity and selectivity of propane oxidative dehydrogenation over VO₃/CeO₂(111) catalysts: A density functional theory study

Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

Received Date: 18 February 2018
Revised Date: 28 March 2018

Fund Project: This work was supported by the National Natural Science Foundation of China (21421004, 21573067, 91545103) and Program of Shanghai Academic Research Leader (17XD1401400). The authors also thank the National Super Computing Center in Jinan for computing time.

The oxidative dehydrogenation (ODH) of propane on monomeric VO₃ supported by CeO₂(111) (VO₃/CeO₂(111)) is studied by periodic density functional theory calculations. Detailed energetic, structural, and electronic properties of these reactions are determined. The calculated activation energies of the breaking of the first and second C-H bonds of propane on the VO₃/CeO₂(111) catalyst are compared, and it is found that both the unique structural and electronic effects of the VO₃/CeO₂(111) catalyst contribute to the relatively easy rupture of the first C-H bond of the propane molecule during the ODH reaction. In particular, the so-called new empty localized states that are mainly constituted of O 2p orbitals of the ceria-supported VO₃ species are determined to be crucial for assisting the cleavage of the first C-H bond of the propane molecule. Following this they become occupied and the remaining C-H bonds become increasingly difficult to break owing to the increasing repulsion between the localized 4f electrons at the Ce cations, resulting in the adsorption of more H and other moieties. This work illustrates that CeO₂-supported monomeric vanadium oxides can exhibit unique activity and selectivity for the catalytic ODH of alkanes to alkenes.
- Oxidative dehydrogenation,
- Propane to propylene,
- C-H bond cleavage,
- Ceria-supported vanadia,
- Density functional theory calculations
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]
1. [1]
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Activity and selectivity of propane oxidative dehydrogenation over VO₃/CeO₂(111) catalysts: A density functional theory study