SKM 2023 – scientific programme
Parts | Days | Selection | Search | Updates | Downloads | Help
O: Fachverband Oberflächenphysik
O 52: Heterogeneous Catalysis and Surface Dynamics I
O 52.7: Talk
Wednesday, March 29, 2023, 12:15–12:30, TRE Phy
Selectivity Trends and Role of Adsorbate–Adsorbate Interactions in CO Hydrogenation on Rhodium Catalysts — •Martin Deimel1,2, Hector Prats3, Michael Seibt2, Karsten Reuter1, and Mie Andersen4 — 1Fritz-Haber-Institut der MPG, Berlin, Germany — 2Chair for Theoretical Chemistry, Technical University of Munich, Germany — 3Department of Chemical Engineering, University College London, UK — 4Aarhus Institute of Advanced Studies and Department of Physics and Astronomy, Aarhus University, Denmark
Rh is one of the most promising elemental catalysts for the conversion of syngas (CO and H2) into hydrocarbons and oxygenates, especially toward valuable higher oxygenates. Experimentally, an inverse relationship between activity and selectivity of the main products methane and acetaldehyde was identified with conflicting explanations for this trend.[1,2] Here, we revisit the question of the role played by step and terrace sites, represented by the Rh(211) and Rh(111) facets, on activity and selectivity trends.[3] We use an accelerated kinetic Monte Carlo (KMC) approach including a cluster expansion to treat lateral interactions. By comparing our results to corresponding mean-field models and experiment,[1,2] we find that only the KMC models can correctly capture the experimental selectivity trends and that quantitatively correct activity predictions require correction for well-known errors in the density functional theory parametrization of our models.
[1] N. Yang et al., J. Am. Chem. Soc. 138, 3705 (2016)
[2] M. Schumann et al., ACS Catal. 11, 5189 (2021)
[3] M. Deimel et al., ACS Catal. 12, 7907 (2022)