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 dur...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(SO_(4)^(2-))oxidation to produce persulfate(S_(2)O_(8)^(2-))and followed by a cathodic persulfate reduction to produce sulfate radicals(SO_(4)^(·-)).These SO_(4)^(·-)are powerful reactive species that enable the unselective degradation of micropollutants and yield SO_(4)^(2-)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-ofconcept demonstration using ubiquitous sulfate for micropollutants decontamination,making water purification more sustainable and more economical.展开更多
基金supported by the National Natural Science Foundation of China(52170068 and U21A20161)the Open Project of State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(QAK202108)。
文摘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(SO_(4)^(2-))oxidation to produce persulfate(S_(2)O_(8)^(2-))and followed by a cathodic persulfate reduction to produce sulfate radicals(SO_(4)^(·-)).These SO_(4)^(·-)are powerful reactive species that enable the unselective degradation of micropollutants and yield SO_(4)^(2-)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-ofconcept demonstration using ubiquitous sulfate for micropollutants decontamination,making water purification more sustainable and more economical.
