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O: Fachverband Oberflächenphysik
O 81: Catalysis and surface reactions II
O 81.3: Vortrag
Donnerstag, 12. März 2026, 11:00–11:15, TRE/MATH
Automated Workflow for Kinetic Modeling in Heterogeneous Catalysis: A Case Study of the Ammonia Oxidation Reaction — •Emanuel Colombi Manzi, Hyunwook Jung, Hendrik H. Heenen, Vanessa J. Bukas, and Karsten Reuter — Fritz-Haber-Institut der MPG, Berlin
Developing reliable kinetic models in computational catalysis is a big challenge, especially when involving large reaction networks with complex intermediates. Atomistic models built upon first-principles energetics, typically density-functional theory (DFT), are widely used today for elucidating catalytic mechanisms and trends. The cost of DFT calculations, however, makes these models far too expensive to thoroughly sample the many structural configurations that are possible for all relevant surface-bound intermediates. As a result, assumptions on the preferred geometry or surface binding site are commonly adopted based on chemical intuition. Here, we present a fully automated workflow that derives an entire microkinetic model without any a priori knowledge or heuristics about the preferred binding configurations. The approach is demonstrated on the kinetics of NH3 oxidation over selected metal surfaces and alloys. Enabled by an efficient DFT-trained machine learned interatomic potential, an ensemble of low-energy adsorbate structures is identified through global optimization and all process barriers between them are systematically computed. Our simulations provide chemical insight beyond the limitations of standard DFT models and open the road for large-scale screening studies without the need of simplifying assumptions like scaling relations.
Keywords: microkinetic model; barrier; automated workflow; machine learned potential; global optimization