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由电解锰渣与油茶壳生物炭耦合制备的高效过一硫酸盐催化剂用于对羟基苯甲酸乙酯降解

Highly efficient peroxymonosulfate catalyst prepared from electrolytic manganese residues coupled with Camellia oleifera shell biochar for ethylparaben degradation.

作者信息

Qin Hangdao, Hao Junnan, Wang Yong, Yang Guo, Xing Bo, Guo Lei, Huang Jiming, Chang Jun, Chen Jing

机构信息

School of Material and Chemical Engineering, Tongren University, Tongren, 554300, China.

School of Material and Chemical Engineering, Tongren University, Tongren, 554300, China.

出版信息

J Environ Manage. 2025 Sep;391:126554. doi: 10.1016/j.jenvman.2025.126554. Epub 2025 Jul 12.

Abstract

Pharmaceuticals and personal care products (PPCPs) contamination can be effectively remediated using sulfate radical-based advanced oxidation processes (SR-AOPs). In this work, a novel composite catalyst (EMR-BC) was successfully prepared using Camellia oleifera shell (COS) biochar (BC) coupled with electrolytic manganese residue (EMR), and the as-obtained catalyst was used to activate peroxymonosulfate (PMS) for the degradation of ethylparaben (EtP). EMR-BC showed superior catalytic performance comparing to EMR and BC, with an EtP remove rate of 97.5 % within 120 min. The •OH, SO•, O and O• were the dominant reactive oxygen species (ROS) during EtP degradation. Reactions between the Fe/Fe and Mn/Mn/Mn redox pairs in EMR and the existence of functional groups in BC improved the efficiency of electron transfer, and thus promoted the production of ROS in EMR-BC/PMS system. Electrochemical tests indicated that the direct-electron pathway was also involved in EtP degradation. After three recycling tests, an 87.9 % EtP removal efficiency was still achieved. Moreover, EMR-BC catalyst showed a good adaptability to actual water environment and a broad application to the removal of other pollutants. Finally, the intermediates generated during the degradation process were determined, and the plausible decomposition pathway of EtP was proposed. The developed system expanded the horizon for the high-value utilization of EMR and COS and the treatment of PPCPs in wastewater.

摘要

基于硫酸根的高级氧化工艺(SR-AOPs)能够有效修复药品及个人护理产品(PPCPs)污染问题。在本研究中,通过将油茶壳(COS)生物炭(BC)与电解锰渣(EMR)耦合,成功制备了一种新型复合催化剂(EMR-BC),并将所得催化剂用于活化过一硫酸盐(PMS)以降解对羟基苯甲酸乙酯(EtP)。与EMR和BC相比,EMR-BC表现出优异的催化性能,在120分钟内EtP去除率达到97.5%。•OH、SO•、O和O•是EtP降解过程中的主要活性氧物种(ROS)。EMR中Fe/Fe和Mn/Mn/Mn氧化还原对之间的反应以及BC中官能团的存在提高了电子转移效率,从而促进了EMR-BC/PMS体系中ROS的产生。电化学测试表明,直接电子途径也参与了EtP的降解。经过三次循环测试后,仍实现了87.9%的EtP去除效率。此外,EMR-BC催化剂对实际水环境表现出良好的适应性,并在去除其他污染物方面具有广泛的应用前景。最后,确定了降解过程中产生的中间体,并提出了EtP可能且合理的分解途径。所开发的体系拓展了EMR和COS高值利用以及废水PPCPs处理的视野。

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