{"title":"通过简便的 Ti/Pd@MXene 滤波电极实现原子 H⁎ 介导的溴酸盐电化学还原","authors":"Xu Yin , Jiatian Yu , Zhifeng Gao , Wei Li , Kajia Wei , Yun Jiang , Yonghao Zhang , Haoming Chen , Weiqing Han","doi":"10.1016/j.jhazmat.2024.136598","DOIUrl":null,"url":null,"abstract":"<div><div>Bromate (BrO<sub>3</sub><sup>–</sup>) is a common by-product of advanced oxidation water treatment processes. In this study, a catalyst combining MXene and Pd was synthesized to eliminate BrO<sub>3</sub><sup>–</sup> by electrochemical reduction in flow-through mode. The fabricated Ti/Pd@MXene filter showed superior activity for BrO<sub>3</sub><sup>–</sup> reduction compared with Ti/MXene filter. A satisfactory BrO<sub>3</sub><sup>−</sup> removal performance by Ti/Pd@MXene filter was obtained at pH values of 5–7 with a current density of 1.0–2.5 mA·cm<sup>–2</sup>. The mechanism explored by quenching experiments and EPR analysis demonstrated that atomic hydrogen (H*)-mediated reduction was dominant in the Ti/Pd@MXene filter system and contributed to 84.2 % of the BrO<sub>3</sub><sup>−</sup> removal, which was greater than that of Ti (7.1 %) and Ti/MXene (43.9 %). DFT calculations revealed the introduction of Pd nanoparticles on MXene lowered the energy barrier for generating H* from OH* -H* , thus boosting H* formation. Furthermore, the Ti/Pd@MXene filter had favorable stability and applicability, and nearly 90 % of BrO<sub>3</sub><sup>−</sup> could be eliminated in different water matrices. Moreover, energy consumption of the Ti/Pd@MXene filter was more competitive than that previously reported (0.348 kWh·mmol<sup>−1</sup>), especially for high BrO<sub>3</sub><sup>−</sup> removal (≥75 %). This work highlighted an effective flow-through electrocatalytic filter to induce H* -mediated electrochemical reduction of BrO<sub>3</sub><sup>−</sup>.</div></div>","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"482 ","pages":"Article 136598"},"PeriodicalIF":12.2000,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Atomic H*-mediated electrochemical reduction of bromate by a facile Ti/Pd@MXene filter electrode\",\"authors\":\"Xu Yin , Jiatian Yu , Zhifeng Gao , Wei Li , Kajia Wei , Yun Jiang , Yonghao Zhang , Haoming Chen , Weiqing Han\",\"doi\":\"10.1016/j.jhazmat.2024.136598\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Bromate (BrO<sub>3</sub><sup>–</sup>) is a common by-product of advanced oxidation water treatment processes. In this study, a catalyst combining MXene and Pd was synthesized to eliminate BrO<sub>3</sub><sup>–</sup> by electrochemical reduction in flow-through mode. The fabricated Ti/Pd@MXene filter showed superior activity for BrO<sub>3</sub><sup>–</sup> reduction compared with Ti/MXene filter. A satisfactory BrO<sub>3</sub><sup>−</sup> removal performance by Ti/Pd@MXene filter was obtained at pH values of 5–7 with a current density of 1.0–2.5 mA·cm<sup>–2</sup>. The mechanism explored by quenching experiments and EPR analysis demonstrated that atomic hydrogen (H*)-mediated reduction was dominant in the Ti/Pd@MXene filter system and contributed to 84.2 % of the BrO<sub>3</sub><sup>−</sup> removal, which was greater than that of Ti (7.1 %) and Ti/MXene (43.9 %). DFT calculations revealed the introduction of Pd nanoparticles on MXene lowered the energy barrier for generating H* from OH* -H* , thus boosting H* formation. Furthermore, the Ti/Pd@MXene filter had favorable stability and applicability, and nearly 90 % of BrO<sub>3</sub><sup>−</sup> could be eliminated in different water matrices. Moreover, energy consumption of the Ti/Pd@MXene filter was more competitive than that previously reported (0.348 kWh·mmol<sup>−1</sup>), especially for high BrO<sub>3</sub><sup>−</sup> removal (≥75 %). This work highlighted an effective flow-through electrocatalytic filter to induce H* -mediated electrochemical reduction of BrO<sub>3</sub><sup>−</sup>.</div></div>\",\"PeriodicalId\":361,\"journal\":{\"name\":\"Journal of Hazardous Materials\",\"volume\":\"482 \",\"pages\":\"Article 136598\"},\"PeriodicalIF\":12.2000,\"publicationDate\":\"2024-11-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Hazardous Materials\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0304389424031790\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Hazardous Materials","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0304389424031790","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Atomic H*-mediated electrochemical reduction of bromate by a facile Ti/Pd@MXene filter electrode
Bromate (BrO3–) is a common by-product of advanced oxidation water treatment processes. In this study, a catalyst combining MXene and Pd was synthesized to eliminate BrO3– by electrochemical reduction in flow-through mode. The fabricated Ti/Pd@MXene filter showed superior activity for BrO3– reduction compared with Ti/MXene filter. A satisfactory BrO3− removal performance by Ti/Pd@MXene filter was obtained at pH values of 5–7 with a current density of 1.0–2.5 mA·cm–2. The mechanism explored by quenching experiments and EPR analysis demonstrated that atomic hydrogen (H*)-mediated reduction was dominant in the Ti/Pd@MXene filter system and contributed to 84.2 % of the BrO3− removal, which was greater than that of Ti (7.1 %) and Ti/MXene (43.9 %). DFT calculations revealed the introduction of Pd nanoparticles on MXene lowered the energy barrier for generating H* from OH* -H* , thus boosting H* formation. Furthermore, the Ti/Pd@MXene filter had favorable stability and applicability, and nearly 90 % of BrO3− could be eliminated in different water matrices. Moreover, energy consumption of the Ti/Pd@MXene filter was more competitive than that previously reported (0.348 kWh·mmol−1), especially for high BrO3− removal (≥75 %). This work highlighted an effective flow-through electrocatalytic filter to induce H* -mediated electrochemical reduction of BrO3−.
期刊介绍:
The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.