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

Wentian Zheng , Shijie You , Yuan Yao , Nanqi Ren , Bin Ding , Fang Li , Yanbiao Liu

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

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Engineering ›› 2023, Vol. 30 ›› Issue (11) : 144 -152. DOI: 10.1016/j.eng.2022.12.005
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Sustainable Generation of Sulfate Radicals and Decontamination of Micropollutants via Sequential Electrochemistry

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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.

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Keywords

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

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.

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Wentian Zheng, Shijie You, Yuan Yao, Nanqi Ren, Bin Ding, Fang Li, Yanbiao Liu. Sustainable Generation of Sulfate Radicals and Decontamination of Micropollutants via Sequential Electrochemistry. Engineering, 2023, 30(11): 144-152 DOI:10.1016/j.eng.2022.12.005

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Funding

the National Natural Science Foundation of China(52170068, U21A20161)

the Open Project of State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology(QAK202108)

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