Microenvironment tailoring mediated oxygen-vacancy defect engineering strategy facilitating O2 and alcohols activation on HEOs with superior catalytic efficiency

Achieving selective oxidation of biomass-derived benzyl alcohol under mild environment for the preparation of high value-added oxygenates is an attractive goal, but remains significant challenges in the absence of qualifying catalysts. Herein, we propose a microenvironment modulation mediated oxygen-vacancy defect engineering for piloting the benzyl alcohol oxidation on catalyst MW-HEO. Collective characterizations indicate that the contemporary tactic can modulate the pore structure and surface electronic states of the catalyst and form massive oxygen vacancies. Both density functional theory (DFT) simulations and experimental results conclusively reveal that the oxygen vacancies contribute to the O₂ activation and the formation for active radicals, thus facilitating the deeper reactants activation and enabling the subsequent oxidation reactions to proceed feasibly. This work lays a solid foundation for microenvironment regulation mediated oxygen vacancy defect engineering for the high efficiency oxidation catalysis of benzyl alcohol and a series of alcohol derivatives.