Au–Carbon Electronic Interaction Mediated Selective Oxidation of Styrene

Abstract

The rational design of the Au–support electronic interaction is crucial for Au nanocatalysis. We herein report our observation of electronic perturbation at the Au–carbon interface and its application in controlling the reaction selectivity in styrene oxidation. Ultrasmall Au nanocatalysts were grown in situ on a nitrided carbon support where the nitrogen-doped carbon supports enriched the surface charge density and generated electron-rich Au surface sites. The Au–carbon interaction altered the binding behavior of C═C bonds to catalytic centers, leading to a solvent-polarity-dependent selectivity in C═C oxidation reactions. A high selectivity of 90% to benzaldehyde was achieved in an apolar solvent, and a selectivity of 95% to styrene epoxide was attained in a polar solvent. The Au–carbon electronic perturbation, originating from surface functional groups on the carbon support, may provide an alternative avenue to tune the selectivity and activity of more complex reactions in heterogeneous catalysis.