Quantum chemical modelling of metal-support interactions in metal-based catalysts

Production of synthesis gas (carbon monoxide and hydrogen) is a process of major importance for chemical upgrading of natural gas. In this process, a catalyst consisting of metal clusters supported on an oxide surface is used. The project's main challenge will be to elucidate the role of strong metal/support interactions (SMSI) in the reforming of light alkanes on oxide-supported nickel catalysts. This is a demanding task, requiring the use of new methods. Specifically, we will use computational methods b ased on quantum chemical and band structure calculations. Of particular interest are the following questions: A. Does CO2 preferentially chemisorb on the metal or the support? B. What is the fate of CO2 immediately after chemisorption? Surface diffusion or dissociation or both? C. Spillover: How may CO2 diffuse between metal and support? D. Reactions at the metal-support interface: Will CO2 simply spill over to the metal and then dissociate, or is CO2 dissociation facilitated at the metal-support interf ace? Strong emphasis will be placed on the interface between metal and oxide; the diffusion of CO2 past the interface, and reactions taking place at the interface. Elucidation will be achieved by considering and comparing the reaction and activation ener gies for a number of different elementary steps. The results from the project will put us in a position to design better catalysts on a more rational basis.