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
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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.

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