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低添加量臭氧电生过锰酸钾同时促进活性锰物种和羟基自由基的生成。

Simultaneously promoted reactive manganese species and hydroxyl radical generation by electro-permanganate with low additive ozone.

机构信息

Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, Chongqing University, Chongqing 400045, China; State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, China.

Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, Chongqing University, Chongqing 400045, China; State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, China.

出版信息

Water Res. 2021 Feb 1;189:116623. doi: 10.1016/j.watres.2020.116623. Epub 2020 Nov 9.

DOI:10.1016/j.watres.2020.116623
PMID:33207290
Abstract

A novel water treatment process combining electrolysis, permanganate and ozone was tested in the laboratory. The combination showed synergistic effects in degrading various organic contaminants (like diclofenac, sulfamethoxazole, carbamazepine, etc.). A small amount of O (1 mg L, 60 mL min) significantly improved the oxidation and mineralization ability of an electro-permanganate process by generating more reactive manganese species and hydroxyl radicals. The combination required less energy consumption than comparable processes. Mechanism experiments showed that the ·OH involved was mainly generated by cathode reduction, homogeneous manganese catalysis, and heterogeneous manganese catalysis of O decomposition. Reactive Mn species were generated by electro-reduction, ·OH oxidation or/and O activation. In situ generated Mn (Ⅳ) plays a vital role in generating ·OH and reactive Mn species. ·OH generated by O catalysis could transfer colloid Mn (Ⅳ) to free Mn (Ⅴ) and Mn (Ⅵ) . And both the ·OH and RMnS played the dominant role for DCF removal. Increasing permanganate dosage, O concentration, the current density, Cl, or humic acid, and decreasing the pH all enhanced the degradation of diclofenac, but the presence of PO or HCO inhibited it. Supplementing electrolysis with permanganate and O might be a practical, sustainable, and economical technology for treating refractory organics in natural waters.

摘要

一种结合电解、高锰酸盐和臭氧的新型水处理工艺在实验室中进行了测试。该组合在降解各种有机污染物(如双氯芬酸、磺胺甲恶唑、卡马西平等)方面表现出协同作用。少量的 O(1mg L,60mL min)通过生成更多的反应性锰物种和羟基自由基,显著提高了电-高锰酸盐工艺的氧化和矿化能力。该组合比可比工艺需要更少的能耗。机理实验表明,所涉及的·OH 主要由阴极还原、均相锰催化和 O 分解的多相锰催化产生。反应性 Mn 物种由电还原、·OH 氧化或/和 O 活化生成。原位生成的 Mn(Ⅳ)在生成·OH 和反应性 Mn 物种方面起着至关重要的作用。O 催化生成的·OH 可以将胶体 Mn(Ⅳ)转移为游离 Mn(Ⅴ)和 Mn(Ⅵ)。并且·OH 和 RMnS 都对 DCF 的去除起主导作用。增加高锰酸盐用量、O 浓度、电流密度、Cl 或腐殖酸,并降低 pH 值都能增强双氯芬酸的降解,但 PO 或 HCO 的存在会抑制其降解。在电解中补充高锰酸盐和 O 可能是一种实用、可持续和经济的处理天然水中难降解有机物的技术。

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