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具有双反应中心和氧空位的双金属催化剂,用于通过O生成协同促进过氧乙酸活化和去污。

Bimetallic catalyst with dual-reaction-center and oxygen vacancies for synergistically boosting peracetic acid activation and decontamination via O generation.

作者信息

Li Shuo, Yang Yalun, Zheng Heshan, Niu Junfeng, Deng Ying, Ma Jun, Leong Yoong Kit, Chang Jo-Shu, Li Wen-Wei

机构信息

College of Food and Bioengineering, Qiqihar University, Qiqihar, 161006, China.

College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China.

出版信息

Water Res. 2025 Sep 15;284:124001. doi: 10.1016/j.watres.2025.124001. Epub 2025 Jun 10.

DOI:10.1016/j.watres.2025.124001
PMID:40516403
Abstract

Peracetic acid (PAA)-based advanced oxidation processes (AOPs) are appealing for water treatment due to their environmentally benignity and ease of activation. However, the predominant generation of radicals in the existing catalytic systems severely limits their practical water decontamination performance. In this study, we report an Mn-doped Cu(OH)Cl catalyst supported on hexagonal boron nitride (Mn-Cu(OH)Cl@BN), providing dual reaction centers (DRCs) and abundant oxygen vacancies (OVs) to facilitate selective generation of singlet oxygen (O) from PAA activation. The Mn introduction raised the electron density of Cu sites to enhance PAA binding and activation towards O generation. Additionally, the BN support and the induced OVs further accelerated the electron transfer, rendering the composite catalyst high activity. As a consequence, the Mn-Cu(OH)Cl@BN/PAA system exhibited excellent activity for degradation of tetracycline hydrochloride (TCH), with a reaction kinetic constant 91 times higher than that of Cu(OH)Cl. In addition, the degradation efficiency was still above 85 % after five runing cycle, indicating its good stability. Our work lays an important basis for innovation of PAA-based AOPs towards low-carbon water treatment application.

摘要

基于过氧乙酸(PAA)的高级氧化工艺(AOPs)因其环境友好性和易于活化而在水处理方面具有吸引力。然而,现有催化体系中自由基的主要生成严重限制了它们实际的水净化性能。在本研究中,我们报道了一种负载在六方氮化硼上的锰掺杂氢氧化铜氯催化剂(Mn-Cu(OH)Cl@BN),它提供双反应中心(DRCs)和丰富的氧空位(OVs),以促进从PAA活化中选择性生成单线态氧(O)。锰的引入提高了铜位点的电子密度,增强了PAA对O生成的结合和活化。此外,BN载体和诱导的OVs进一步加速了电子转移,使复合催化剂具有高活性。因此,Mn-Cu(OH)Cl@BN/PAA体系对盐酸四环素(TCH)的降解表现出优异的活性,反应动力学常数比Cu(OH)Cl高91倍。此外,经过五个运行周期后,降解效率仍高于85%,表明其具有良好的稳定性。我们的工作为基于PAA的AOPs在低碳水处理应用方面的创新奠定了重要基础。

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