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

Danyang Feng, Yangbo Dong, Liangliang Zhang, Xin Ge, Wei Zhang, Sheng Dai, Zhen An Qiao

Research output: Contribution to journalArticlepeer-review

220 Scopus citations

Abstract

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.

Original languageEnglish
Pages (from-to)19503-19509
Number of pages7
JournalAngewandte Chemie - International Edition
Volume59
Issue number44
DOIs
StatePublished - Oct 26 2020

Funding

This work was supported by the Young Thousand Talented Program and the National Natural Science Foundation of China (21671073 and 21621001), the “111” Project of the Ministry of Education of China (B17020), Program for JLU Science and Technology Innovative Research Team. SD was supported by U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geoscience, and Bioscience Division.

Keywords

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

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