Shang Denghui, Zheng Wenwen, Zhao Peng, Li Yi, Xie Liangbo, Zhang Jinlong, Zhan Sihui, Hu Wenping
Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
China National Offshore Oil Corporation, Tianjin Branch, Tianjin, 300452, China.
Chemosphere. 2023 Jun;325:138339. doi: 10.1016/j.chemosphere.2023.138339. Epub 2023 Mar 7.
Heterogeneous electro-Fenton (HEF) process has been regarded as a promising method in environmental remediation. However, the reaction kinetic mechanism of the HEF catalyst for simultaneous production and activation of HO remained confounded. Herein, the copper supported on polydopamine (Cu/C) was synthesized by a facile method and employed as a bifunctional HEFcatalyst, and the catalytic kinetic pathways were deeply investigated by using rotating ring-disk electrode (RRDE) voltammetry based on the Damjanovic model. Experimental results substantiated that a two-electron oxygen reduction reaction (2e ORR) and a sequential Fenton oxidation reaction were proceeded on 1.0-Cu/C, where metallic copper played a crucial role in the fabrication of 2e active sites as well as utmost HO activation to produce highly reactive oxygen species (ROS), resulting in the high HO productivity (52.2%) and the almost complete removal of contaminant ciprofloxacin (CIP) after 90 min. The work not only expanded the idea of reaction mechanism on Cu-based catalyst in HEF process but also provided a promising catalyst for pollutants degradation in wastewater treatment.
非均相电芬顿(HEF)工艺被认为是环境修复领域一种很有前景的方法。然而,HEF催化剂同时产生和活化羟基自由基(HO·)的反应动力学机制仍不清楚。在此,通过一种简便方法合成了负载在聚多巴胺上的铜(Cu/C),并将其用作双功能HEF催化剂,基于达米亚诺维奇模型,利用旋转环盘电极(RRDE)伏安法深入研究了催化动力学途径。实验结果证实,在1.0-Cu/C上发生了两电子氧还原反应(2e ORR)和连续芬顿氧化反应,其中金属铜在2e活性位点的形成以及最大程度活化HO·以产生活性氧(ROS)方面起着关键作用,从而实现了高HO·产率(52.2%),并在90分钟后几乎完全去除污染物环丙沙星(CIP)。这项工作不仅拓展了HEF工艺中基于铜的催化剂的反应机理概念,还为废水处理中的污染物降解提供了一种有前景的催化剂。