Electron-rich CuOx@Al2O3 Catalyst for Sustainable O2 Activation in Fenton-Like Reactions

催化作用 材料科学 化学 无机化学 化学工程 生物化学 工程类
作者
Fei Xiao,Xiaowen Xie,Zhenxu Yang,Tao Dong,Ruijie Xie,Tao Ban,Biyuan Liu,Huanran Zhong,Dennis Y.C. Leung,Michael K.H. Leung,Haibao Huang
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:59 (20): 10044-10055 被引量:14
标识
DOI:10.1021/acs.est.5c02193
摘要

Molecular oxygen (O 2 ) activation is pivotal in advancing green chemistry and catalysis, addressing processes such as energy conversion and environmental remediation. However, the inherent inertness of the O 2 necessitates highly efficient catalysts. In this study, an electron-rich CuO x @Al 2 O 3 catalyst with high metal loading and dispersion was synthesized via the ion-exchange inverse-loading method. The novel CuO x @Al 2 O 3 significantly enhanced O 2 activation due to the accelerated Cu 0 → Cu + → Cu 2+ redox cycle, achieving the 85% chlorobenzene removal in Fenton-like reaction. This is substantially higher than the chlorobenzene removal observed with conventional CuO x /Al 2 O 3 (45%). Experiments and density functional theory (DFT) calculations revealed that Cu–Cu sites over CuO x @Al 2 O 3 greatly facilitated charge transfer, weakened O–O bonds, and promoted synergistic O 2 and H 2 O 2 activation to produce • OH and O 2 •–, thereby enhancing oxidants utilization efficiency. This study provides a sustainable pathway for pollutant degradation by achieving O 2 activation and offers valuable insights for designing advanced Cu-based catalysts in green oxidation processes and environmental remediation.
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