4.8 Article

Holey Lamellar High-Entropy Oxide as an Ultra-High-Activity Heterogeneous Catalyst for Solvent-free Aerobic Oxidation of Benzyl Alcohol

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 44, Pages 19503-19509

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202004892

Keywords

anchoring and merging process; high-entropy oxide; mesoporous structures; benzyl alcohol oxidation; porous materials

Funding

  1. Young Thousand Talented Program
  2. National Natural Science Foundation of China [21671073, 21621001]
  3. 111 Project of the Ministry of Education of China [B17020]
  4. Program for JLU Science and Technology Innovative Research Team
  5. U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geoscience, and Bioscience Division

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The development of noble-metal-free heterogeneous catalysts is promising for selective oxidation of aromatic alcohols; however, the relatively low conversion of non-noble metal catalysts under solvent-free atmospheric conditions hinders their industrial application. Now, a holey lamellar high entropy oxide (HEO) Co0.2Ni0.2Cu0.2Mg0.2Zn0.2O material with mesoporous structure is prepared by an anchoring and merging process. The HEO has ultra-high catalytic activity for the solvent-free aerobic oxidation of benzyl alcohol. Up to 98 % conversion can be achieved in only 2 h, to our knowledge, the highest conversion of benzyl alcohol by oxidation to date. By regulating the catalytic reaction parameters, benzoic acid or benzaldehyde can be selectively optimized as the main product. Analytical characterizations and calculations provide a deeper insight into the catalysis mechanism, revealing abundant oxygen vacancies and holey lamellar framework contribute to the ultra-high catalytic activity.

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