Higher loadings of Pt single atoms and clusters over reducible metal oxides: application to C–O bond activation

Abstract

We develop higher loadings of isolated noble metal atoms and clusters on a mildly reducible metal oxide. We demonstrate the approach for Pt supported on TiO₂ and confirmed it by XRD, AC-HAADF-STEM, CO-FTIR, XAS, and XPS. Density functional theory calculations rationalize the experimental stability and the IR shifts using mixtures of CH₃I and CO. The redispersed catalysts are thermally stable in inert gas or H₂ and afford enhanced selectivity and activity in hydrodeoxygenation reactions compared to metal nanoparticles by creating surface oxygen vacancies that promote C–O cleavage without side reactions. Higher metal loadings, e.g., 1%Pt/TiO₂, on the oxide surface profoundly increase the activity of the bare oxide catalyst tenfold compared to ultra-low loadings typically used for single atom catalysis.