4.7 Article

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

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ACS APPLIED NANO MATERIALS
卷 6, 期 21, 页码 20310-20319

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AMER CHEMICAL SOC
DOI: 10.1021/acsanm.3c04254

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defect engineering; oxygen vacancy; high-entropyoxides; oxidation; benzyl alcohol

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This study presents a high-entropy oxide nanosheet with rich oxygen vacancies, which is fabricated by using a high-entropy metal organic framework as a precursor. The nanosheet exhibits excellent catalytic performance in the oxidation of benzyl alcohol, due to its substantial oxygen vacancies and large pores, which promote substrate activation and mass transfer.
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 O-V 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 O-V 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.

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