Periodic Density Functional Theory Study of Propane Oxidative Dehydrogenation over VO(001) Surface.
The oxidative dehydrogenation (ODH) of propane on single-crystal VO(001) is studied by periodic density functional theory (DFT) calculations. The energetics and pathways for the propane to propene conversion are determined. We show that (i) the C-H bond of propane can be activated by both the termin...
| Publicado en: | Journal of the American Chemical Society Vol. 128; no. 34; pp. 11114 - 11124 |
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| Autores principales: | , , , , |
| Formato: | Artículo |
| Publicado: |
American Chemical Society
8/30/2006
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| Materias: | |
| Acceso en línea: | Ver este registro en EBSCOhost |
| Sumario: | The oxidative dehydrogenation (ODH) of propane on single-crystal VO(001) is studied by periodic density functional theory (DFT) calculations. The energetics and pathways for the propane to propene conversion are determined. We show that (i) the C-H bond of propane can be activated by both the terminal and the bridging lattice O atoms on the surface with similar activation energies. At the terminal O site both the radical and the oxo-insertion pathways are likely for the C-H bond activation, while only the oxo-insertion mechanism is feasible at the bridging O site. (ii) Compared to that at the terminal O site, the propene production from the propoxide at the bridging O site is much easier due to the weaker binding of propoxide at the bridging O. It is concluded that single-crystal VO(001) is not a good catalyst due to the terminal O being too active to release propene. It is expected that an efficient catalyst for the ODH reaction has to make a compromise between the ability to activate the C-H bond and the ability to release propene. |
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