Electron-rich CuO<sub>x</sub>@Al<sub>2</sub>O<sub>3</sub> Catalyst for Sustainable O<sub>2</sub> Activation in Fenton-Like Reactions
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
Abstract
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.