We present an ab initio investigation of the interaction between methane, its dehydrogenated forms and the cerium oxide surface. In particular, the stoichiometric CeO2(111) surface and the one with oxygen vacancies are considered. We study the geometries, energetics and electronic structures of various configurations of these molecules adsorbed on the surface in vacuum, and we extend the analysis to realistic environmental conditions. A phase diagram of the adsorbate-surface system is constructed and relevant transition phases are analyzed in detail, showing the conditions where partial oxidation of methane can occur. © 2014 The Royal Society of Chemistry.
Bibliographical noteKAUST Repository Item: Exported on 2020-10-01
Acknowledgements: The authors gratefully acknowledge support from the Australian Research Council (ARC), the Australian National Computational Infrastructure (NCI) and the Australian Center for Advanced Computing and Communication (AC3). MF expresses his gratitude to Jason Gao and Irina Holca for proofreading the manuscript.
ASJC Scopus subject areas
- Chemical Engineering(all)