Microenvironment tailoring mediated oxygen-vacancy defect engineering strategy facilitating O2 and alcohol activation on HEOs with superior catalytic efficiency
APPLIED SURFACE SCIENCE(2024)
摘要
Achieving selective oxidation of biomass-derived benzyl alcohol under a mild environment to prepare high-value-added oxygenates is an attractive goal but remains a significant challenge 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 catalyst's pore structure and surface electronic states 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 forming active radicals, thus facilitating the deeper reactant 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.
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关键词
Microenvironment modulation,High entropy oxides,Oxygen vacancy engineering,Benzyl alcohol oxidation
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