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Abstract

Based on the recent interest in oxy-carbide materials in catalysis, we employ a thin film model concept to highlight that variation of key reaction parameters in the reactive magnetron sputtering of zirconium carbide films (sputtering power, template temperature or reactive plasma environment) under realistic preparation and application conditions often results in zirconium oxy-carbide films of varying stoichiometry. The composition of the films grown on silicon wafers and in vacuo - cleaved NaCl (001) single crystal facets was confirmed by depth profiling X-ray photoelectron spectroscopy and electron microscopy analysis. A correlation between methane-to-argon ratio, excess carbon and template temperature with elemental composition emphasizes the exclusive presence of oxygen-containing zirconium carbides. To generalize the approach, we also show that embedding of highly ordered Cu particles with uniform sizes in zirconium oxy-carbide matrices yields well-defined metal / oxy-carbide interfaces. As the presence of an oxy-carbide and its reactivity has been inextricably linked to enhanced activity and selectivity in a variety of processes, including hydrogenation, oxidation or reduction reactions, our model thin film approach provides the necessary well-defined catalysts to derive mechanistic details and to study the decomposition/re-carburization cycles of oxy-carbides. We have exemplified the concept for zirconium oxy-carbide, but deliberate extension to similar systems is easily possible.