Regensburg 2019 – wissenschaftliches Programm

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DS: Fachverband Dünne Schichten

DS 4: Frontiers of Electronic-Structure Theory: Focus on the Interface Challenge I (joint session O/CPP/DS/TT)

DS 4.1: Topical Talk

Montag, 1. April 2019, 10:30–11:00, H9

Scaling relations and beyond for kinetic Monte Carlo models in heterogeneous catalysis — •Mie Andersen — Theoretical Chemistry, Technische Universität München, Germany

Heterogeneous catalysis typically operates at the interface between a gas or liquid and a solid catalytic material. In my talk, I will discuss mean-field and kinetic Monte Carlo models for the operating catalyst. These often rely on input data calculated using either first principles or more approximate methods, e.g. scaling relations, which use only selected adsorption energies as descriptors for the catalyst function [1,2]. I will also discuss recent work [3] where we used compressed sensing methods to identify new low-cost and accurate descriptors that allow to predict adsorption energies for a wide range of adsorbates, multi-metallic transition metal surfaces and facets. The descriptors are expressed as non-linear functions of intrinsic properties of the clean catalyst surface, e.g. coordination numbers and d-band moments. From a single DFT calculation of these properties, we predict adsorption energies at all potential surface sites, and thereby also the most stable geometry. Compared to previous approaches such as scaling relations, we find our approach to be both more general and more accurate for the prediction of adsorption energies on alloys with mixed-metal surfaces, already when based on training data including only pure metals.

[1] M. Andersen et al., Ang. Chem. Int. Ed. 55, 5210 (2016)

[2] M. Andersen et al., J. Chem. Phys. 147, 152705 (2017)

[3] M. Andersen et al., submitted