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最小化电化学氧化 Ni-EDTA 过程中产生的有毒氯化副产物:活性氯引发的 Fe(II)向 Fe(IV)的转化的重要性。

Minimizing toxic chlorinated byproducts during electrochemical oxidation of Ni-EDTA: Importance of active chlorine-triggered Fe(II) transition to Fe(IV).

机构信息

The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, School of Environment and Energy, South China University of Technology, Guangzhou 510006, PR China.

The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, School of Environment and Energy, South China University of Technology, Guangzhou 510006, PR China.

出版信息

Water Res. 2022 Jul 1;219:118548. doi: 10.1016/j.watres.2022.118548. Epub 2022 May 4.

Abstract

The formation of chlorinated byproducts represents a significant threat to the quality of the effluent treated using electrochemical advanced oxidation processes (EAOPs), thus spurring investigation into alleviating their production. This study presents a new strategy to minimize the release of chlorinated intermediates during the electrochemical oxidation of Ni-EDTA by establishing a dual mixed metal oxide (MMO)/Fe anode system. The results indicate that the dual-anode system achieved a substantially higher rate (0.141 min) of Ni-EDTA destruction and accordingly allowed a more pronounced removal of aqueous Ni (from 39.85 to 0.63 mg L) after alkaline precipitation, compared with its single MMO anode (0.017 min of Ni-EDTA removal, with 14.38 mg L Ni remaining) and single Fe anode (insignificant Ni-EDTA removal, with 38.37 mg L Ni remaining) counterparts. Compared to reactive chlorine species (RCS) produced from the single MMO anode system, Fe(IV) was in situ generated from the dual-anode system and was predominantly responsible for the attenuation of chlorinated byproducts and thus the decrease in the acute toxicity of the treated solution (evaluated using luminescent bacteria). The Fe(IV)-dominated dual-anode system also exhibited superior performance in removing multiple pollutants (including organic ligands, Ni, and phosphite) in the real electroless plating effluent. The findings suggest that the strategy for Fe(II) transition to Fe(IV) by active chlorine paves a new avenue for yielding less chlorinated products with lower toxicity when EAOPs are used to treat chloride-containing organic wastewater.

摘要

电化学高级氧化工艺(EAOPs)处理后的废水中氯化副产物的形成对出水水质构成了重大威胁,因此激发了人们研究如何减轻其生成的兴趣。本研究提出了一种新策略,通过建立双混合金属氧化物(MMO)/Fe 阳极系统,来最小化电化学氧化 Ni-EDTA 过程中氯化中间体的释放。结果表明,双阳极系统实现了 Ni-EDTA 破坏的更高速率(0.141 min),因此在碱性沉淀后,更显著地去除了水中的 Ni(从 39.85 降至 0.63 mg/L),而其单 MMO 阳极(Ni-EDTA 去除率为 0.017 min,仍有 14.38 mg/L 的 Ni 残留)和单 Fe 阳极(Ni-EDTA 去除不明显,仍有 38.37 mg/L 的 Ni 残留)则无法达到。与单 MMO 阳极系统产生的活性氯物种(RCS)相比,Fe(IV)是由双阳极系统原位生成的,主要负责衰减氯化副产物,从而降低处理溶液的急性毒性(使用发光细菌进行评估)。Fe(IV)主导的双阳极系统在去除实际化学镀废水中的多种污染物(包括有机配体、Ni 和亚磷酸盐)方面也表现出卓越的性能。研究结果表明,通过活性氯将 Fe(II)转化为 Fe(IV)的策略为 EAOPs 处理含氯有机废水时生成毒性更低的氯化产物开辟了新途径。

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