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Abstract

We present a first-principles based multiscale modeling approach to heterogeneous catalysis that integrates
first-principles kinetic Monte Carlo simulations of the surface reaction chemistry into a fluid dynamical treatment
of the macroscale flow structures in the reactor. The approach is applied to a stagnation flow field in front
of a single-crystal model catalyst using the CO oxidation at RuO2(110) as representative example. Our simulations
show how heat and mass transfer effects can readily mask the intrinsic reactivity at gas-phase conditions
typical for modern in situ experiments. For a range of gas-phase conditions we furthermore obtain
multiple steady states that arise solely from the coupling of gas-phase transport and surface kinetics. This
additional complexity needs to be accounted for when aiming to use dedicated in situ experiments to establish
an atomic-scale understanding of the function of heterogeneous catalysts at technologically relevant gas-phase conditions.