Computational modelling of the reaction-induced surface evolution of nanoporous gold

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Within this subproject we will perform quantum-chemical modelling at the atomic scale to investigate how surface morphology, chemical composition, and surface strain of nanoporous gold influence the catalytic activity and selectivity of this material toward oxidation reactions. We will study these effects in the context of CO, methanol, and propylene oxidation. The subproject will have a focus on the adsorbate- and reaction-induced surface dynamics. Hence, an idealized picture of a perfect clean and rigid surface will be replaced by a surface, which is covered by adsorbates and is dynamicallychanging during catalytic transformations. These insights will be achieved through a combination between traditional (static) DFT calculations and AIMD simulations. Our modelling studies will contribute to a more advanced understanding of the role played by (i) surface morphology and, in particular, low-coordinated sites, (ii) lattice strain (iii) concentration and distribution of an impurity metal, such as Ag or Cu, (iv) surface population of O containing species, e.g. O2, O, OH, OOH, and H2O, for the catalytic function of nanoporous gold. Theoretical prediction of the key reaction intermediates, their adsorption geometry, binding strengths, vibrational frequencies, as well as kinetic parameters will assist the analysis and interpretation of the experimental data of the participating research groups.