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Heterogeneous oxidation catalysis on ruthenium: bridging the pressure and materials gaps and beyond

It is shown that both the materials and the pressure gaps can be bridged for ruthenium in heterogeneous oxidation catalysis using the oxidation of carbon monoxide as a model reaction. Polycrystalline catalysts, such as supported Ru catalysts and micrometer-sized Ru powder, were compared to single-crystalline ultrathin RuO2 films serving as model catalysts. The microscopic reaction steps on RuO2 were identified by a combined experimental and theoretical approach applying density functional theory. Steady-state CO oxidation and transient kinetic experiments such as temperature-programmed desorption were performed with polycrystalline catalysts and single-crystal surfaces and analyzed on the basis of a microkinetic model. Infrared spectroscopy turned out to be a valuable tool allowing us to identify adsorption sites and adsorbed species under reaction conditions both for practical catalysts and for the model catalyst over a wide temperature and pressure range. The close interplay of the experimental and theoretical surface science approach with the kinetic and spectroscopic research on catalysts applied in plug–flow reactors provides a synergistic strategy for improving the performance of Ru-based catalysts. The most active and stable state was identified with an ultrathin RuO2 shell coating a metallic Ru core. The microscopic processes causing the structural deactivation of Ru-based catalysts while oxidizing CO have been identified.