CuFeKao粒子电极三维非均相电Fenton体系降解亚甲基蓝

doi:10.19965/j.cnki.iwt.2024-0250

摘要/Abstract

摘要：

采用溶胶-凝胶法合成CuFe₂O₄/Fe₂O₃/Kaolin（CuFeKao）催化粒子电极，并将其应用于三维非均相电Fenton（3D/EF）体系降解亚甲基蓝（MB）。XRD结果表明，CuFeKao是由CuFe₂O₄、Fe₂O₃和高岭土（Kaolin）构成的复合材料。通过对比实验发现三维电化学作用可以提高H₂O₂的产量，非均相电Fenton体系可以催化H₂O₂原位转化为·OH。与以CuFe₂O₄/Fe₂O₃或Kaolin为粒子电极的3D体系和2D体系相比，3D/EF/CuFeKao体系表现出最大的·OH产率和最佳的MB降解率。通过单因素实验对3D/EF/CuFeKao体系的降解条件进行优化，在优化条件下反应60 min，MB和TOC的去除率分别可达99.81%和58.13%。自由基猝灭实验证实体系含·OH和O₂ ^·-两种活性氧物种（ROS），其相对占比可通过溶液pH进行调控。机理分析表明，3D/EF/CuFeKao体系降解MB的主要机理是发生在CuFeKao粒子电极表面的非均相电Fenton作用。

关键词: 铜铁双金属, 高岭土, 三维非均相电Fenton, 亚甲基蓝

Abstract:

CuFe₂O₄/Fe₂O₃/Kaolin(CuFeKao) catalytic particle electrode was synthesized by sol-gel method and used in three-dimensional heterogeneous electro-Fenton system to degrade Methylene blue(MB). XRD results showed that CuFeKao was a composite material composed of CuFe₂O₄, Fe₂O₃ and Kaolin. Through comparative experiments, it was found that three-dimensional electrochemical interactions could increase the yield of H₂O₂, and heterogeneous electro-Fenton systems could catalyze the in-situ conversion of H₂O₂ to ·OH. Compared with 3D systems using CuFe₂O₄/Fe₂O₃ or Kaolin as particle electrode and 2D systems, the 3D/EF/CuFeKao system exhibited the highest ·OH yield and the best MB degradation effect. The degradation conditions of the 3D/EF/CuFeKao system were optimized by single factor experiments. Under the optimized conditions, the removal rates of MB and TOC could reach 99.81% and 58.13% respectively after 60 minutes of reaction. The quenching of free radicals confirmed that the system contained two reactive oxygen species, ·OH and O₂ ^·-, whose relative proportions could be regulated by solution pH. Mechanism analysis showed that the main mechanism of MB degradation in the 3D/EF/CuFeKao system is the heterogeneous electro-Fenton reaction occurring on the surface of the CuFeKao particle electrode.

Key words: Cu-Fe bimetal, Kaolin, three-dimensional heterogeneous electro-Fenton, Methylene blue

中图分类号:

X703

陈越, 彭雪儿, 周琛阳, 李婧, 孟欣怡, 高丽丽. CuFeKao粒子电极三维非均相电Fenton体系降解亚甲基蓝[J]. 工业水处理, 2025, 45(2): 54-62.

Yue CHEN, Xueer PENG, Chenyang ZHOU, Jing LI, Xinyi MENG, Lili GAO. Degradation of methylene blue by three-dimensional heterogeneous electro-Fenton system with CuFeKao particle electrode[J]. Industrial Water Treatment, 2025, 45(2): 54-62.

https://www.iwt.cn/CN/Y2025/V45/I2/54

图/表 7

图1 催化粒子电极材料的XRD

Fig.1 XRD of catalytic particle electrode materials

图2 不同电极体系下MB的去除率（a）、H₂O₂产量（b）以及·OH荧光强度（c）

Fig.2 Removal rates of MB（a），H₂O₂ production（b），and fluorescence intensities of ·OH（c） under different systems

图3 pH（a）、曝气强度（b）、催化粒子投加量（c）和MB初始质量浓度（d）对MB去除的影响

Fig.3 Effects of pH（a），aeration intensity（b），dosage of catalytic particle electrode（c） and initial concentration of MB（d） on removal of MB

图4 电流密度对MB降解效果（a）的影响，以及混合电解质对TOC去除（b）、电流效率和能耗（c）的影响

Fig.4 Effects of current densities on MB degradation（a），and effects of mixed electrolyte on the removal of TOC（b），current efficiency and energy consumption（c）

图5 pH=3（a）和原pH（b）条件下自由基清除剂对MB去除率的影响

Fig.5 Effects of free radical scavengers on MB removal rate under pH=3 （a） and original pH （b） conditions

图6 3D/EF/CuFeKao体系中MB的主要降解机理

Fig.6 Main degradation mechanism of MB in 3D/EF/CuFeKao system

图7 CuFeKao的重复利用实验（a），使用前后XRD对比（b）和3D/EF/CuFeKao体系对实际地表水配制溶液中MB的去除率（c）

Fig.7 Reuse experiment of CuFeKao（a），XRD comparison before and after use（b），and removal rate in real surface water of MB by 3D/EF/CuFeKao system（c）

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