SurfaceScience21 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 7: Poster Session I: Heterogeneous catalysis I
O 7.3: Poster
Montag, 1. März 2021, 10:30–12:30, P
Active Site Representation in First-Principles Microkinetic Models: Data-Enhanced Computational Screening for Improved Methanation Catalysts — •Martin Deimel1, Karsten Reuter1,2, and Mie Andersen1 — 1Chair for Theoretical Chemistry, Technical University of Munich, Garching, Germany — 2Fritz Haber Institute of the Max Planck Society, Berlin, Germany
In heterogeneous catalysis first-principles microkinetic models have largely contributed to our trend understanding of transition metal (TM) and TM alloy catalysts. Within prevalent screening approaches, the computational costs are kept tractable through the use of reductionist models that only resolve a minimal amount of active site motifs at the surface. This reduces the required input to only a few adsorption energies of key reaction intermediates, while the predictive power might be jeopardized. Here, we scrutinize this common practice by systematically comparing the screening predictions for the CO methanation reaction when using microkinetic models that resolve an increasing number of sites at stepped TM and binary TM alloy catalysts. The excessive amount of predictive-quality adsorption energetics required is obtained from a compressed sensing descriptor that once trained provides these data for a new material from a single DFT calculation of the clean surface.[1] We show that the explicit consideration of hitherto neglected step and terrace sites yields new mechanistic insights and highly active materials.[2]
[1] M. Andersen et al., ACS Catal. 9, 2752 (2019)
[2] M. Deimel et al., ACS Catal. 10, 13729 (2020)