Alcohol

Catalysis

Engineering

Oxide

Mesoporous material

Materials science

Benzaldehyde

Lamellar structure

Solvent

Inorganic chemistry

Benzoic acid

Chemical engineering

Benzyl alcohol

Alcohol oxidation

Organic chemistry

Noble metal

Crystallography

Chemistry

Heterogeneous catalysis

Angewandte Chemie International Edition

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) Co0.2 Ni0.2 Cu0.2 Mg0.2 Zn0.2 O 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.

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