Boosting electrochemical oxidation of As(III) on Fe-doped RuO2 /PEDOT/SnO2 nanocomposite anode: Fabrication, performance and mechanism

被引:14
|
作者
Miao, Xinyu [1 ]
Shen, Jiao [2 ]
Ji, Wenlan [1 ]
Zhang, Tian C. [3 ]
Liang, Ying [2 ]
Yuan, Shaojun [1 ]
机构
[1] Sichuan Univ, Coll Chem Engn, Low Carbon Technol & Chem React Engn Lab, Chengdu 610065, Peoples R China
[2] Sichuan Univ, Coll Architecture & Environm Engn, Chengdu 610065, Peoples R China
[3] Univ Nebraska Lincoln, Civil & Environm Engn Dept, Omaha, NE 68182 USA
来源
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY | 2024年 / 180卷
基金
中国国家自然科学基金;
关键词
Arsenite; Electrocatalytic oxidation; Iron-doped ruthenium oxide; Anode; Reactive oxygen species; EVOLUTION REACTION; DEGRADATION; REMEDIATION; POLLUTANTS; KINETICS; SURFACE; SINGLE;
D O I
10.1016/j.jmst.2023.09.013
中图分类号
T [工业技术];
学科分类号
08 ;
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/SnO2/PEDOT/Fe(III)-RuO2 multilayer electrode was synthesized by utilizing a PEDOT-coated SnO2 interlayer as a supportive framework to combine Fe-doped amorphous RuO2 catalytic layer with TiO2 nanotube array substrate. Such electrode exhibited high activity and stability for the oxidation of As(III) to As(V) due to the large surface area provided by the TiO2 nanotube arrays and the SnO2/PEDOT interlayer for facilitating the growth of the catalytic layer. The electrochemically active surface area of the electrode reached as high as 31.7 mF/cm2. Impressively, the doping of Fe into RuO2 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 RuO2 weakened the adsorption strength of center dot OH and center dot SO4- intermediates and lowered the energy barrier for generating ROS. Combined with ESR results, the formation of center dot OH and center dot SO4- with strong oxidizing properties was fully verified, providing further evidence 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. (c) 2023 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
引用
收藏
页码:243 / 258
页数:16
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