Holey Lamellar High-Entropy Oxide as an Ultra-High-Activity Heterogeneous Catalyst for Solvent-free Aerobic Oxidation of Benzyl Alcohol
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. Furthermore, 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.
- Authors:
-
[2];
[1]
- Jilin Univ., Changchun (China). Qiao State Key Lab. of Inorganic Synthesis and Preparative Chemistry; Jilin Univ., Changchun (China). Electron Microscopy Center
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1810001
- Grant/Contract Number:
- AC05-00OR22725; 21671073; 21621001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 44; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; anchoring and merging process; high-entropy oxide; mesoporous structures; benzyl alcohol oxidation; porous materials
Citation Formats
Feng, Danyang, Dong, Yangbo, Zhang, Liangliang, Ge, Xin, Zhang, Wei, Dai, Sheng, and Qiao, Zhen‐An. Holey Lamellar High-Entropy Oxide as an Ultra-High-Activity Heterogeneous Catalyst for Solvent-free Aerobic Oxidation of Benzyl Alcohol. United States: N. p., 2020.
Web. doi:10.1002/anie.202004892.
Feng, Danyang, Dong, Yangbo, Zhang, Liangliang, Ge, Xin, Zhang, Wei, Dai, Sheng, & Qiao, Zhen‐An. Holey Lamellar High-Entropy Oxide as an Ultra-High-Activity Heterogeneous Catalyst for Solvent-free Aerobic Oxidation of Benzyl Alcohol. United States. https://doi.org/10.1002/anie.202004892
Feng, Danyang, Dong, Yangbo, Zhang, Liangliang, Ge, Xin, Zhang, Wei, Dai, Sheng, and Qiao, Zhen‐An. Tue .
"Holey Lamellar High-Entropy Oxide as an Ultra-High-Activity Heterogeneous Catalyst for Solvent-free Aerobic Oxidation of Benzyl Alcohol". United States. https://doi.org/10.1002/anie.202004892. https://www.osti.gov/servlets/purl/1810001.
@article{osti_1810001,
title = {Holey Lamellar High-Entropy Oxide as an Ultra-High-Activity Heterogeneous Catalyst for Solvent-free Aerobic Oxidation of Benzyl Alcohol},
author = {Feng, Danyang and Dong, Yangbo and Zhang, Liangliang and Ge, Xin and Zhang, Wei and Dai, Sheng and Qiao, Zhen‐An},
abstractNote = {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. Furthermore, 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.},
doi = {10.1002/anie.202004892},
journal = {Angewandte Chemie (International Edition)},
number = 44,
volume = 59,
place = {United States},
year = {Tue Jun 30 00:00:00 EDT 2020},
month = {Tue Jun 30 00:00:00 EDT 2020}
}
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