Transport limitations and bistability for in situ CO oxidation at RuO2(110): First-principles based multiscale modeling

Sebastian Matera and Karsten Reuter
Phys. Rev. B 82, 085446 – Published 30 August 2010

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.

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  • Received 1 June 2010

DOI:https://doi.org/10.1103/PhysRevB.82.085446

©2010 American Physical Society

Authors & Affiliations

Sebastian Matera1 and Karsten Reuter1,2

  • 1Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Germany
  • 2Department Chemie, Technische Universität München, Lichtenbergstr. 4, D-85747 Garching, Germany

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Issue

Vol. 82, Iss. 8 — 15 August 2010

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