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O: Fachverband Oberflächenphysik

O 102: Heterogeneous Catalysis on Metals

O 102.3: Vortrag

Donnerstag, 19. März 2020, 11:15–11:30, TRE Phy

Active site representation in first-principles microkinetic models: Data-enhanced computational screening for improved methanation catalysts — •Martin Deimel, Mie Andersen, and Karsten Reuter — Chair for Theoretical Chemistry and Catalysis Research Center, Technical University of Munich, Germany

Reductionist first-principles microkinetic models have largely contributed to our trend understanding and computational screening of transition metal (TM) and TM alloy catalysts. As a key enabling step, these models draw much of their computational efficiency from scaling relations that reduce the required first-principles input to only a few adsorption energies of key reaction intermediates. Not withstanding, as these relations need to be established separately for every surface site considered, the predictive power of existing such models might be jeopardized by an overly simplistic representation of the active catalyst surface. Here we employ a recently established compressed-sensing approach [1] that (once trained) provides the required adsorption energies of ALL involved reaction intermediates at ALL high-symmetry sites from a single density-functional theory calculation of the clean TM or binary TM alloy surface. This enables refined microkinetic models considering multiple active sites. We revisit existing work investigating methanation catalysts on the basis of a less detailed microkinetic model [2] and show that the explicit consideration of hitherto neglected step and terrace sites indeed yields new mechanistic insights and highly active materials. [1] M. Andersen et al., ACS Catal. 9, 2752 (2019); [2] A. C. Lausche et al., J. Catal. 307, 275 (2013).