Defect Engineering of High-Entropy Oxides for Superior Catalytic Oxidation Performance

Bingzhen Zhang; Dan Deng; Jian Chen; Ying Li; Mingwei Yuan; Weiming Xiao; Shuhua Wang; Xiaolei Wang; Pengfei Zhang; Yuan Shu; Shunli Shi; Chao Chen

doi:10.1021/acsami.3c15235

Defect Engineering of High-Entropy Oxides for Superior Catalytic Oxidation Performance

ACS Appl Mater Interfaces. 2023 Nov 3. doi: 10.1021/acsami.3c15235. Online ahead of print.

Authors

Bingzhen Zhang^{1

2}, Dan Deng³, Jian Chen¹, Ying Li¹, Mingwei Yuan¹, Weiming Xiao¹, Shuhua Wang¹, Xiaolei Wang³, Pengfei Zhang^{4

5}, Yuan Shu⁴, Shunli Shi¹, Chao Chen¹

Affiliations

¹ Key Laboratory of Jiangxi Province for Environment and Energy Catalysis, College of Chemical Engineering and Chemistry, Nanchang University, Nanchang, Jiangxi 330031, P. R. China.
² School of Power and Mechanical Engineering, The Institute of Technological Sciences, Wuhan University, Wuhan, Hubei 430072, P. R. China.
³ College of Chemical Engineering and Chemistry, Nanchang University, Nanchang, Jiangxi 330031, P. R. China.
⁴ State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China.
⁵ School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China.

PMID: 37922463
DOI: 10.1021/acsami.3c15235

Abstract

High-entropy oxides (HEOs) are crucial in various fields (power storage/conversion, electronic devices, and catalysis) owing to their adjustable structural characteristics, fabulous stability, and massive components. However, the current strategies for synthesizing HEOs suffer from low surface area and limited active sites. Herein, we present a salt-assisted strategy with remarkable universality for the preparation of HEOs with high surface area [e.g., HP-(FeCrCoNiCu)_xO_y: 59 m²/g, HP-(ZnMgNiCuCo)_xO_y: 49 m²/g, and HP-(CrMnFeNiZn)_xO_y: 11 m²/g], where HP means high porosity. Especially, HP-(FeCrCoNiCu)_xO_y with rich-oxygen vacancies promotes catalytic efficiency for hydrocarbon and alcohol oxidation owing to its hierarchical texture and massive oxygen vacancies. Furthermore, density functional theory is utilized to well illustrate the relationship of the structure and catalytic efficiency within the catalysts. This work offers realistic pathway for the large-scale application of HEOs in catalytic areas.

Keywords: defect engineering; high-entropy oxide; hydrocarbon oxidation; rich-oxygen vacancies; selective aerobic catalysis.