流体电化学靶向诱生硫酸根自由基降解水中微污染物

郑文天, 尤世界, 姚远, 任南琪, 丁彬, 李方, 刘艳彪

工程（英文） ›› 2023, Vol. 30 ›› Issue (11) : 144-152.

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工程（英文） ›› 2023, Vol. 30 ›› Issue (11) : 144-152. DOI: 10.1016/j.eng.2022.12.005
研究论文
Article

流体电化学靶向诱生硫酸根自由基降解水中微污染物

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Sustainable Generation of Sulfate Radicals and Decontamination of Micropollutants via Sequential Electrochemistry

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Highlight

• A system that runs solely on sulfate by sequential electrochemistry was proposed.

• The circular transformation of SO42-→ S2O82-→ SO4•-→ SO42- can be achieved.

• Ultra-fast degradation of selected contaminants can be achieved within 2 sec.

• The system implemented green chemistry principle to decontaminate diverse micropollutants.

摘要

水中微污染物的深度去除是环境工程领域的重大挑战。受限于低浓度和高毒性等污染特征，传统水处理策略难以实现这类污染物的有效去除。基于此，本文提出了流体电化学靶向诱生硫酸根自由基（SO4•-）的研究设想，通过构筑穿透式电化学反应系统，实现了阳极将硫酸根离子（SO42−）氧化生成过硫酸根（S2O82−），再通过阴极还原反应将S2O82−转化为SO4•-。开展了流体电化学系统构造原理、硫酸根自由基靶向生成机制和微污染物降解机理等相关研究。结果表明，在最优实验条件下，该系统可在单次流模式下实现苯胺的高效降解（100%）和总有机碳的有效去除（65.0%）。该系统在宽pH范围内和复杂水基质条件下均能实现多种微污染物的有效去除。本工作基于“以废治废”理念，结合了膜分离和电化学的技术优势，有望为水中微污染物的深度去除提供一种潜在可行的技术选择。

Abstract

The removal of emerging micropollutants in the aquatic environment remains a global challenge. Conventional routes are often chemically, energetically, and operationally intensive, which decreases their sustainability during applications. Herein, we develop an advanced chemical-free strategy for micropollutants decontamination that is solely based on sequential electrochemistry involving ubiquitous sulfate anions in natural and engineered waters. This can be achieved via a chain reaction initiated by electrocatalytic anodic sulfate (SO42−) oxidation to produce persulfate (S2O82−) and followed by a cathodic persulfate reduction to produce sulfate radicals (SO4̇−). These SO4̇− are powerful reactive species that enable the unselective degradation of micropollutants and yield SO42− again in the treated water. The proposed flow-through electrochemical system achieves the efficient degradation (100.0%) and total organic carbon removal (65.0%) of aniline under optimized conditions with a single-pass mode. We also reveal the effectiveness of the proposed system for the degradation of a wide array of emerging micropollutants over a broad pH range and in complex matrices. This work provides the first proof-of-concept demonstration using ubiquitous sulfate for micropollutants decontamination, making water purification more sustainable and more economical.

关键词

高级氧化 / 链式反应 / 硫酸根离子 / 微污染物 / 顺序电化学体系

Keywords

Advanced oxidation / Chain reaction / Sulfate radical / Micropollutants / Sequential electrochemistry

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郑文天, 尤世界, 姚远. 流体电化学靶向诱生硫酸根自由基降解水中微污染物. Engineering. 2023, 30(11): 144-152 https://doi.org/10.1016/j.eng.2022.12.005

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