| Autor: |
Huang, Li’nan, Jiang, Lei, Tian, Dong, Li, Yuelun, Zuo, Huicong, Li, Zhiqiang, Li, Kongzhai |
| Zdroj: |
Journal of Rare Earths; 20240101, Issue: Preprints |
| Abstrakt: |
Energy shortages and global warming are driving the focus on the greenhouse gases CH4and CO2. The main reason why dry reforming of methane (DRM) has yet to be industrialized is its catalytic tendency to deactivate due to carbon deposition or sintering. Single-atom Ni/CeO2catalysts with suitable metal-support interactions may provide a new strategy for developing highly active and coking-resistant nickel-based catalysts. In this work, we investigated the properties of the catalytic models of single-atom Ni loaded on CeO2(111), CeO2(110) and CeO2(100), as well as their catalytic DRM performance with the density functional theory method (DFT). The interaction of CeO2with different low-index crystal planes and single-atom Ni can be explained by the anchoring effect of surface O ions on Ni. Adsorption energies, growth patterns of Ni clusters, and migration studies of Ni atoms all indicate that the CeO2(100) surface has the strongest anchoring effect on isolated Ni atoms, followed by the CeO2(110) surface, with the CeO2(111) surface being the weakest. Methane activation studies have shown that the activation ability of Ni1/CeO2(110) for methane strongly depends on the coordination environment of Ni. By contrast, methane activation by Ni on Ni1/CeO2(111) exhibits better activity and stability. Moreover, the Ni–CeO2interaction correlates well with the DRM reaction performance. Interactions that are too strong anchor Ni atoms well but are not optimal for DRM activity. Ni1/CeO2(110) has relatively moderate interactions, promotes the *CH4→*CH process, and has good resistance to carbon deposition. The metal-support interaction-DRM reactivity (or stability) relationship is vital for the design of “super” high-activity and high-stability DRM catalysts. |
| Databáze: |
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