(525c) From Electrons to Reactive Flow: Coupling First-Principles Statistical Mechanics with Continuum Level Simulations

For the simulation of in-situ experiments in heterogeneous catalysis different coupled aspects have to be encountered. On the hand the surface reactivity depends on the partial pressures and the temperature at surface. On the other hand gas flow and the heat transport in the sample is effected by the consumption and production of species at the surface, and the partial pressures and the temperature at the surface will differ from the applied ones. In order to describe the coupling of both effects we combine first-principles kinetic Monte Carlo simulations [1] to model the surface reactivity with continuum level simulation for the gas and solid phase transport. We apply our method to stagnation flow experiments for the CO oxidation at a RuO2(110) single crystal surface. We show how the gas/solid phase transport affects the outcome of the experiment for different reactor setups (e.g. different flow rates). Especially we investigate the influence of the gas and solid phase transport on the observed turn-over frequency and surface population.

[1] K. Reuter and M. Scheffler, Phys. Rev. B 73, 045433 (2006)