Boosting electrochemical oxidation of As(Ⅲ)on Fe-doped RuO_(2)/PEDOT/SnO_(2) nanocomposite anode:Fabrication,performance and mechanism  

作　　者：Xinyu Miao Jiao Shen Wenlan Ji Tian CZhang Ying Liang Shaojun Yuan 

机构地区：[1]Low-carbon Technology&Chemical Reaction Engineering Lab,College of Chemical Engineering,Sichuan University,Chengdu 610065,China [2]College of Architecture and Environmental Engineering,Sichuan University,Chengdu 610065,China [3]Civil&Environmental Engineering Department,University of Nebraska-Lincoln,Omaha,NE 68182-0178,United States of America

出　　处：《Journal of Materials Science & Technology》2024年第13期243-258,共16页材料科学技术（英文版）

基　　金：National Natural Science Foundation of China(No.21978182)。

摘　　要：Design of electrode materials for stable and efficient electrocatalytic oxidation of As(Ⅲ)in arsenic-contaminated groundwater poses a great challenge due to the rapid deactivation of catalysts resulting from the high oxygen evolution potential(OEP)and considerable barrier to generating reactive oxygen species(ROS).Herein,an innovative TNAs/SnO_(2)/PEDOT/Fe(Ⅲ)-RuO_(2) multilayer electrode was synthesized by utilizing a PEDOT-coated SnO_(2) interlayer as a supportive framework to combine Fe-doped amorphous RuO_(2) catalytic layer with TiO_(2) nanotube array substrate.Such electrode exhibited high activity and sta-bility for the oxidation of As(Ⅲ)to As(V)due to the large surface area provided by the TiO_(2) nanotube arrays and the SnO_(2)/PEDOT interlayer for facilitating the growth of the catalytic layer.The electrochem-ically active surface area of the electrode reached as high as 31.7 mF/cm^(2).Impressively,the doping of Fe into RuO_(2) layer led to a remarkable increase in the OEP value to 3.12 V,which boosted the indirect oxidation process mediated by ROS at a lower potential to achieve the As(Ⅲ)oxidation ratio of 98.5%.DFT calculations revealed that the Fe-doped amorphous RuO_(2) weakened the adsorption strength of·OH and.SO4-intermediates and lowered the energy barrier for generating ROS.Combined with ESR results,the formation of·OH and·SC4-with strong oxidizing properties was fully verified,providing further evi-dence for the involvement of ROS as the main mediator of the oxidation mechanism of As(Ⅲ).This work may provide valuable perspectives into the design of catalytic layer structures and heteroatom doping modifications for composite-coated electrodes.

关 键 词：ARSENITE Electrocatalytic oxidation Iron-doped ruthenium oxide Anode Reactive oxygen species 

分 类 号：TQ131.11[化学工程—无机化工] TM912[电气工程—电力电子与电力传动]