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Engineering >> 2023, Volume 30, Issue 11 doi: 10.1016/j.eng.2022.12.005

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

a Textile Pollution Controlling Engineering Center of Ministry of Environmental Protection, College of Environmental Science and Engineering, Donghua University, Shanghai 201620, China
b State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
c MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150080, China
d Innovation Center for Textile Science and Technology, College of Textiles, Donghua University, Shanghai 200051, China
e Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China

Received: 2022-08-06 Revised: 2022-10-22 Accepted: 2022-12-05 Available online: 2023-01-10

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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 (SO4·). These SO4· 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%) 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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