The steady-state of heterogeneous catalysis, studied by first-principles statistical mechanics

Abstract

The turn-over frequency of the catalytic oxidation of CO at RuO2(110) was calculated as function of temperature and partial pressures using ab initio statistical mechanics. The underlying energetics of the gas-phase molecules, dissociation, adsorption, surface diffusion, surface chemical reactions, and desorption were obtained by all-electron density-functional theory. The resulting CO2 formation rate [in the full (T, p_CO, p_O2)-space], the movies displaying the atomic motion and reactions over times scales from picoseconds to seconds, and the statistical analyses provide insights into the concerted actions ruling heterogeneous catalysis and open thermodynamic systems in general.

4 pages including 3 figures, Related publications can be found at http://www.fhi-berlin.mpg.de/th/paper.html

References in corpus (3)

• Composition, structure and stability of RuO_2(110) as a function of oxygen pressure
• Composition and structure of the RuO2(110) surface in an O2 and CO environment: implications for the catalytic formation of CO2
• First-principles, atomistic thermodynamics for oxidation catalysis

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