Regensburg 2025 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 41: Heterogeneous Catalysis II

O 41.4: Vortrag

Dienstag, 18. März 2025, 14:45–15:00, H8

Automatic Exploration of Catalytic Reaction Networks — •Hyunwook Jung, Johannes T. Margraf, Hendrik H. Heenen, and Karsten Reuter — Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin

The reaction network is a crucial element of first-principles microkinetics simulations, representing the connection between surface species and elementary reactions. Lacking systematic exploration methods, the reaction network is presently typically set up by human intuition. Especially for complicated processes such as syngas conversion, this is error prone and the absence of important species and reaction steps can be a source of sizable discrepancy between theoretical modeling and experiment. To address this problem, we introduce an automatic reaction network exploration scheme that starts with a fully enumerated, yet redundant reaction network, in which a reaction pathway is refined iteratively. The associated computational cost for extensive sampling of structures for both adsorption and activation energy calculations along the pathway is circumvented by simultaneously fine-tuning a MACE foundation model. Each trial reaction pathway is coupled with corresponding mean-field microkinetics and a detouring operation is attempted for the identified rate-limiting step. This procedure is repeated until user-defined criteria are reached. We demonstrate this automatic scheme on methanol synthesis at a Cu(111) surface.

Keywords: reaction network; heterogeneous catalysis; density functional theory; machine-learning; microkinetics