氯离子对 Cr(III)-EDTA 电化学解络合和降解的影响:HO- 和 RCS 的反应机制。

Journal of hazardous materials Pub Date : 2024-10-05 Epub Date: 2024-08-25 DOI:10.1016/j.jhazmat.2024.135636
Shujie Zheng, Jiani Yao, Ying Huang, Jiaqi Ren, Yang Hou, Bin Yang, Lecheng Lei, Jianjie Fu, Abdulaziz Al-Anazi, Guibin Jiang, Zhongjian Li
{"title":"氯离子对 Cr(III)-EDTA 电化学解络合和降解的影响:HO- 和 RCS 的反应机制。","authors":"Shujie Zheng, Jiani Yao, Ying Huang, Jiaqi Ren, Yang Hou, Bin Yang, Lecheng Lei, Jianjie Fu, Abdulaziz Al-Anazi, Guibin Jiang, Zhongjian Li","doi":"10.1016/j.jhazmat.2024.135636","DOIUrl":null,"url":null,"abstract":"<p><p>The removal of Cr(III)-organic complexes, encompassing both decomplexation and ligand degradation, presents significant challenges in industrial wastewater treatment. As one of the most common anions in wastewater, Cl<sup>-</sup> significantly improves the efficiency of electrochemically removing Cr(III)-organic complexes through generated reactive chlorine species (RCS). In the electrochemical chlorine (EC/Cl<sub>2</sub>) process, extensive experimentation revealed that ClO<sup>•</sup> plays a dominant role in the degradation of Cr(III)-EDTA, surpassing the effects of free chlorine, direct electrooxidation, HO<sup>•</sup>, and other RCS. Density functional theory calculations indicated that RCS, primarily Cl<sup>•</sup> and ClO<sup>•</sup>, preferentially oxidize the ligand in Cr(III)-EDTA via H-abstraction, whereas HO<sup>•</sup> trends to attack the Cr atom through electron transfer. The influential factors on the degradation efficiency of Cr(III)-EDTA, Cr(VI) yield, and total organic carbon removal in EC/Cl<sub>2</sub> were also assessed, including Cl<sup>-</sup> concentration, current density, and pH. Real industrial wastewater was employed as a reaction matrix to evaluate the application of the EC/Cl<sub>2</sub> process for treating Cr(III)-EDTA, accompanied by energy efficiency calculations. Additionally, a two-chamber reactor was established to simultaneously oxidize Cr(III)-EDTA at the anode and reduce Cr(VI) at the cathode. This study provided insight into developing RCS-dominated AOPs to effectively decomplex and decompose organic Cr(III)-complexes in Cl<sup>-</sup>-containing industrial wastewater.</p>","PeriodicalId":94082,"journal":{"name":"Journal of hazardous materials","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2024-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Impacts of chloride ions on the electrochemical decomplexation and degradation of Cr(III)-EDTA: Reaction mechanisms of HO<sup>•</sup> and RCS.\",\"authors\":\"Shujie Zheng, Jiani Yao, Ying Huang, Jiaqi Ren, Yang Hou, Bin Yang, Lecheng Lei, Jianjie Fu, Abdulaziz Al-Anazi, Guibin Jiang, Zhongjian Li\",\"doi\":\"10.1016/j.jhazmat.2024.135636\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>The removal of Cr(III)-organic complexes, encompassing both decomplexation and ligand degradation, presents significant challenges in industrial wastewater treatment. As one of the most common anions in wastewater, Cl<sup>-</sup> significantly improves the efficiency of electrochemically removing Cr(III)-organic complexes through generated reactive chlorine species (RCS). In the electrochemical chlorine (EC/Cl<sub>2</sub>) process, extensive experimentation revealed that ClO<sup>•</sup> plays a dominant role in the degradation of Cr(III)-EDTA, surpassing the effects of free chlorine, direct electrooxidation, HO<sup>•</sup>, and other RCS. Density functional theory calculations indicated that RCS, primarily Cl<sup>•</sup> and ClO<sup>•</sup>, preferentially oxidize the ligand in Cr(III)-EDTA via H-abstraction, whereas HO<sup>•</sup> trends to attack the Cr atom through electron transfer. The influential factors on the degradation efficiency of Cr(III)-EDTA, Cr(VI) yield, and total organic carbon removal in EC/Cl<sub>2</sub> were also assessed, including Cl<sup>-</sup> concentration, current density, and pH. Real industrial wastewater was employed as a reaction matrix to evaluate the application of the EC/Cl<sub>2</sub> process for treating Cr(III)-EDTA, accompanied by energy efficiency calculations. Additionally, a two-chamber reactor was established to simultaneously oxidize Cr(III)-EDTA at the anode and reduce Cr(VI) at the cathode. This study provided insight into developing RCS-dominated AOPs to effectively decomplex and decompose organic Cr(III)-complexes in Cl<sup>-</sup>-containing industrial wastewater.</p>\",\"PeriodicalId\":94082,\"journal\":{\"name\":\"Journal of hazardous materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-10-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of hazardous materials\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1016/j.jhazmat.2024.135636\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/8/25 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of hazardous materials","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1016/j.jhazmat.2024.135636","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/8/25 0:00:00","PubModel":"Epub","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0

摘要

铬(III)有机络合物的去除包括解络合和配体降解,这给工业废水处理带来了巨大挑战。作为废水中最常见的阴离子之一,Cl- 可通过生成活性氯(RCS)显著提高电化学去除铬(III)有机络合物的效率。在电化学氯(EC/Cl2)过程中,大量实验表明,ClO- 在降解 Cr(III)-EDTA 的过程中起着主导作用,超过了游离氯、直接电氧化、HO- 和其他 RCS 的作用。密度泛函理论计算表明,RCS(主要是 Cl- 和 ClO-)优先通过 H-萃取氧化 Cr(III)-EDTA 中的配体,而 HO- 则倾向于通过电子转移攻击 Cr 原子。此外,还评估了 EC/Cl2 中对 Cr(III)-EDTA 降解效率、Cr(VI)产量和总有机碳去除率的影响因素,包括 Cl- 浓度、电流密度和 pH 值。实际工业废水被用作反应矩阵,以评估 EC/Cl2 工艺在处理 Cr(III)-EDTA 方面的应用,同时进行能效计算。此外,还建立了一个双室反应器,以同时在阳极氧化 Cr(III)-EDTA 和在阴极还原 Cr(VI)。这项研究为开发以 RCS 为主导的 AOPs 提供了深入的见解,从而有效地解聚和分解含氯工业废水中的有机铬(III)络合物。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Impacts of chloride ions on the electrochemical decomplexation and degradation of Cr(III)-EDTA: Reaction mechanisms of HO and RCS.

The removal of Cr(III)-organic complexes, encompassing both decomplexation and ligand degradation, presents significant challenges in industrial wastewater treatment. As one of the most common anions in wastewater, Cl- significantly improves the efficiency of electrochemically removing Cr(III)-organic complexes through generated reactive chlorine species (RCS). In the electrochemical chlorine (EC/Cl2) process, extensive experimentation revealed that ClO plays a dominant role in the degradation of Cr(III)-EDTA, surpassing the effects of free chlorine, direct electrooxidation, HO, and other RCS. Density functional theory calculations indicated that RCS, primarily Cl and ClO, preferentially oxidize the ligand in Cr(III)-EDTA via H-abstraction, whereas HO trends to attack the Cr atom through electron transfer. The influential factors on the degradation efficiency of Cr(III)-EDTA, Cr(VI) yield, and total organic carbon removal in EC/Cl2 were also assessed, including Cl- concentration, current density, and pH. Real industrial wastewater was employed as a reaction matrix to evaluate the application of the EC/Cl2 process for treating Cr(III)-EDTA, accompanied by energy efficiency calculations. Additionally, a two-chamber reactor was established to simultaneously oxidize Cr(III)-EDTA at the anode and reduce Cr(VI) at the cathode. This study provided insight into developing RCS-dominated AOPs to effectively decomplex and decompose organic Cr(III)-complexes in Cl--containing industrial wastewater.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
自引率
0.00%
发文量
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信