Flowerlike Nanosheet-Based High-Entropy Oxides as Catalysts for Aerobic Oxidation of Benzyl Alcohol

Abstract

Aerobic oxidation of benzyl alcohol (BAL) under ambient reaction conditions is a charming goal for the fabrication of high-value oxygenates. However, competent catalysts are presently lacking. Herein, we present a flower-like high entropy oxide (HEO) nanosheet with rich oxygen vacancies for the BAL oxidation by utilizing the high-entropy metal organic framework (HE-MOF) as a precursor. Collective characterizations indicate that the substantial OV and massive pores of HEO facilitate substrate activation, promote mass transfer, and enhance catalytic efficiency. Both experimental results and density functional theory (DFT) simulations clearly illustrate the promoting role of OV in the process for reactant activation, thus significantly contributing to the formation of active oxygen species and driving subsequent oxidation more feasible. This work shines light on structural microenvironmental regulation induced via oxygen-vacancy defect engineering to realize superior selective oxidation catalysis.