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This project was finished with a set of publications, and a successful Ph.D. thesis defence.

Quantum calculation are applied to study the C-H activation and C-C coupling on several metallic surface (Ru, Rh, Pt,) in presence and in absence of atomic oxygen on surface. The model of surface is based on coupling on several metallic surface (Ru, Rh, Pt,) in presence and in absence of atomic oxygen on surface. The model of surface is based on extended slabs.

Since methane is used in many industrial processes, such as partial oxidation, in order to produce hydrogen and carbon monoxide used as basic in Fisher Trops process, fundamental understating of methane surface reactions is of great interest in surface science. Intermediates like CH x (x=0-3), O, and OH are studied, and also the interactions between this species on the surface. Transition states are predicted for the elementary reactions, in order to understand which path the reaction occurs. Different sites of adsorption are considered for all the intermediates. The first surfaces considered are the most compacts ones (0001) for hexagonal package (hcp): example Ru, (111) and (001) for cubic package (fcc): example Rh, Pt. Also step surfaces are interesting to study, because they are more close to real catalyst. In order to be able to compute such complex surfaces, defected surfaces are considered first (added or missing atoms).

This quantum chemical study is performed in the Density Functional Theory with VASP software code (mainly) which allow the description of infinite periodic system such as chains, slabs, or bulks by employing translational symmetries. VASP uses pseudo-potentials and plane-waves basis sets. Its approach is based on a finite-temperature local-density approximation. The calculation of the forces allows a complete or a partial geometry optimization. Using this program it is possible to obtain accurate results for the relative energies, the geometries and the electronic properties. With all this information, we can understand the behavior of the surface intermediates implied in methane activation, or we can predict the behavior for the same intermediates on the not studied metallic surfaces.

These pages are maintained by Bouke Bunnik (B.S.Bunnik@tue.nl). Comments and suggestions are welcome.