一种用于高效氯酚废水处理的环保型光催化耦合电容去离子系统

doi:10.1016/S1872-2067(25)64839-X

催化学报 ›› 2025, Vol. 79: 148-161.DOI: 10.1016/S1872-2067(25)64839-X

一种用于高效氯酚废水处理的环保型光催化耦合电容去离子系统

郑子叶^a, 任怡^a, 代孟^a^,^b, 李红盛^a^,^b, 崔会珍^a, 王森^c, 王曙光^a^,^b^,^d, 何作利^a^,^b^,^*()

^a山东大学环境科学与工程学院, 山东省多介质复合污染协同治理重点实验室, 山东省环境过程与健康危害重点实验室, 山东青岛266237
^b山东大学威海工业技术研究院, 山东威海264209
^c山东大学微生物技术研究院, 微生物改造技术全国重点实验室, 山东青岛266237
^d山东大学环境科学与工程学院, 中法生态环保产业技术研究院, 山东青岛266237

收稿日期:2025-07-02 接受日期:2025-08-25 出版日期:2025-12-05 发布日期:2025-10-27
通讯作者: 何作利
基金资助:
国家自然科学基金(22278245);山东省泰山学者特聘专家(tstp20230604);山东大学青年学者未来计划(61440089964189);有机化合物污染控制工程教育部重点实验室基金(20190202)

An eco-friendly photocatalytic coupling capacitive deionization system for efficient chlorophenol wastewater treatment

Ziye Zheng^a, Yi Ren^a, Meng Dai^a^,^b, Hongsheng Li^a^,^b, Huizhen Cui^a, Sen Wang^c, Shuguang Wang^a^,^b^,^d, Zuoli He^a^,^b^,^*()

^aShandong Key Laboratory of Synergistic Control of Complex Multi-Media Pollution, Shandong Key Laboratory of Environmental Processes and Health, School of Environmental Science and Engineering, Shandong University, Qingdao 266237, Shandong, China
^bWeihai Research Institute of Industrial Technology of Shandong University, Weihai 264209, Shandong, China
^cState Key Laboratory of Microbial Technology, Microbial Technology Institute, Shandong University, Qingdao 266237, Shandong, China
^dSino-French Research Institute for Ecology and Environment (ISFREE), School of Environmental Science and Engineering, Shandong University, Qingdao 266237, Shandong, China

Received:2025-07-02 Accepted:2025-08-25 Online:2025-12-05 Published:2025-10-27
Contact: Zuoli He
Supported by:
National Natural Science Foundation of China(22278245);Taishan Scholars Project of Shandong Province(tstp20230604);Shandong University Future Youth Grant Program(61440089964189);Key Laboratory of Organic Compound Pollution Control Engineering (MOE) Foundation, China(20190202)

摘要/Abstract

摘要：

氯酚类污染物广泛存在于焦化、石化及造纸废水中, 其因具有高毒性、持久性和生物累积性, 对生态系统与人类健康构成严重威胁. 现有处理技术(物理吸附、高级氧化、生物降解)普遍存在矿化不彻底、二次污染风险高及规模化成本高等瓶颈. 其中, 传统光催化(PC)技术虽可用于降解氯酚, 但仍面临催化剂回收困难、矿化不彻底、复杂基质下的效率衰减及氯离子(Cl⁻)干扰引发氯化副产物生成等挑战. 电容去离子(CDI)技术通过电极的电吸附作用选择性去除离子, 具有能耗低、电极可再生、同步去除无机盐与带电有机物等优势, 但其单一技术对有机污染物的降解能力有限. 针对上述挑战, 本文提出了光催化-电容去离子(PC-CDI)协同策略, 通过氮化硼/氮化碳(BN/CN) Z型异质结电极构建PC-CDI耦合系统, 旨在实现氯酚的高效降解与深度矿化, 同时阐明Cl⁻去除-污染物富集-自由基降解的协同机制.
本文通过原位煅烧法成功制备了BN/CN异质结电极材料, 并进一步构建了PC-CDI协同反应体系. 高比表面积的多孔BN/CN复合材料促进了电吸附和电荷载流子分离, 从而协同优化了PC和CDI功能. 光电流测试结果表明, BN/CN异质结的构建大幅提高了光催化活性. 这主要归因于Z型异质结的形成有利于电荷的空间分离, 并保持体系中光生载流子的强氧化还原能力. PC-CDI耦合系统在2 h内实现了97.15%的2,4-二氯苯酚降解效率和72.35%的总有机碳(TOC)去除率, 均显著优于单一的PC和CDI体系. 并且, 该耦合系统表现出良好的稳定性(五个循环后效率仍高于95%)以及对多种氯酚衍生物的广泛适用性. 通过自由基捕获实验发现, •OH、¹O₂、h⁺和•O₂^-共同参与PC-CDI降解过程. 此外, 通过密度泛函理论计算, 系统地研究了BN与CN之间界面内建电场诱导的Z型电荷转移机制. 二者的复合使BN/CN中N 2p轨道的能级聚集得更加紧密, 显著优化了光催化过程中的电荷传输特性, 同时改善了CDI过程中的电荷转移动力学. 最后, 本文总结了PC-CDI协同降解机制. 基于BN/CN电极在正负偏压作用下的特性, 耦合体系中的CDI单元通过电吸附将Cl⁻富集于阳极, 实现其空间分离, 有效减轻了其干扰并抑制了氯化副产物的形成. 同时, 通过规避光催化过程中Cl^‒诱导的副反应抑制了氯自由基的产生. 带正电的氯酚污染物的电吸附加速了其向催化位点的扩散, 促进了活性氧驱动的氯酚污染物降解反应.
综上, 本文通过构建PC-CDI耦合系统实现了氯酚污染物的高效降解, 最大限度地降低了氯酚废水处理过程中氯化副产物相关的环境风险, 并阐明了PC-CDI协同反应机制. 本研究将有助于推动利用PC-CDI技术处理氯酚废水, 同时也为实际高盐度废水的处理提供了重要启示.

关键词: 光催化, 氯酚, 电容去离子, 氮化硼, 氮化碳

Abstract:

Since conventional photocatalytic technology fails to achieve complete elimination of chlorophenol contaminants from aqueous environments, this study presents a synergistic photocatalysis-capacitive deionization (PC-CDI) system as an advanced solution for industrial chlorophenol wastewater remediation. The PC-CDI system, employing boron nitride/carbon nitride (BN/CN) heterojunction electrodes, demonstrates exceptional degradation performance toward chlorophenols. The high-surface-area porous BN/CN heterojunction facilitates electro-adsorption and charge carrier separation, thereby synergistically optimizing both photocatalytic (PC) and capacitive deionization (CDI) functionalities. Remarkably, the integrated system achieves a 2,4-DCP degradation efficiency of 97.15% and a 2,4,6-TCP degradation efficiency of 100% in 2 h. The CDI component enables spatial separation through the electro-adsorption of Cl^- ions at the anode, effectively mitigating their interference and suppressing chlorinated byproduct formation. Concurrently, the electro-adsorption of positively charged chlorophenol pollutants accelerates their diffusion to catalytic sites, promoting the reactive oxygen species (ROS)-driven degradation of chlorophenol pollutants. The PC-CDI system exhibits robust stability (> 95% efficiency retention over five cycles) and broad applicability across various chlorophenol derivatives. By circumventing Cl^--induced side reactions and inhibiting chlorine radical generation during photocatalysis, this strategy minimizes the environmental risks associated with chlorinated byproducts during chlorophenol wastewater treatment. These findings establish the PC-CDI system as a sustainable and eco-friendly technology for industrial wastewater treatment.

Key words: Photocatalysis, Chlorophenols, Capacitive deionization, Boron nitride, C₃N₄

郑子叶, 任怡, 代孟, 李红盛, 崔会珍, 王森, 王曙光, 何作利. 一种用于高效氯酚废水处理的环保型光催化耦合电容去离子系统[J]. 催化学报, 2025, 79: 148-161.

Ziye Zheng, Yi Ren, Meng Dai, Hongsheng Li, Huizhen Cui, Sen Wang, Shuguang Wang, Zuoli He. An eco-friendly photocatalytic coupling capacitive deionization system for efficient chlorophenol wastewater treatment[J]. Chinese Journal of Catalysis, 2025, 79: 148-161.

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一种用于高效氯酚废水处理的环保型光催化耦合电容去离子系统

An eco-friendly photocatalytic coupling capacitive deionization system for efficient chlorophenol wastewater treatment

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