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新型非均相电 permanganate 过程中 Mn(II)作为促进剂和稳定剂生成活性 Mn(III)。

Generation of Active Mn(III) by a Novel Heterogeneous Electro-permanganate Process with Manganese(II) as Promoter and Stabilizer.

机构信息

State Key Laboratory of Coal Mine Disaster Dynamics and Control , Chongqing University , Chongqing 400044 , People's Republic of China.

Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education , Chongqing University , Chongqing 400045 , People's Republic of China.

出版信息

Environ Sci Technol. 2019 Aug 6;53(15):9063-9072. doi: 10.1021/acs.est.9b01510. Epub 2019 Jul 9.

Abstract

Our study on the synergetic effect of electrolysis and permanganate (E-PM) revealed a novel alternative method for generating active Mn(III) heterogeneously by electrochemically activating PM with Mn as promoter and stabilizer. We systematically explored the generation mechanism of Mn(III). It indicated that all three components (electrolysis + PM + Mn) were necessary to facilitate the generation of active Mn(III) in the E-PM-Mn process. It was worth noting that Mn, as essential promoter and Mn(III) stabilizer, could considerably enhance the concentration of Mn(III) in the E-PM-Mn process. Further study revealed that the active Mn(III) was mainly produced on cathode rather than in aqueous solution or on anode. In addition, the soluble Mn(III) generated in the E-PM-Mn process was demonstrated to be very efficient for the degradation and mineralization of diclofenac (DCF) as well as methyl blue, carbamazepine, phenol, sulfamethoxazole, and nitrobenzene. Moreover, the effects of the main operating parameters (Mn dosage, PM dosage, applied current density, pH of solution, and contaminant concentration) and different water matrices on the E-PM-Mn process were investigated systematically. Possible degradation pathways of DCF in the E-PM-Mn process were also proposed. The results demonstrated that the E-PM-Mn system based on active Mn(III) could create a more efficient, sustainable, and less energy costing technology for water treatment.

摘要

我们的电解与高锰酸盐(E-PM)协同作用研究揭示了一种通过电化学激活高锰酸盐并用锰作为促进剂和稳定剂来生成异相活性 Mn(III)的新方法。我们系统地研究了 Mn(III)的生成机制。结果表明,E-PM-Mn 过程中生成活性 Mn(III)需要三个组件(电解+高锰酸盐+锰)同时存在。值得注意的是,锰作为必不可少的促进剂和 Mn(III)稳定剂,可以显著提高 E-PM-Mn 过程中 Mn(III)的浓度。进一步的研究表明,活性 Mn(III)主要在阴极上生成,而不是在水溶液中或阳极上生成。此外,E-PM-Mn 过程中生成的可溶性 Mn(III)对降解和矿化二氯芬酸(DCF)以及亚甲蓝、卡马西平、苯酚、磺胺甲噁唑和硝基苯等污染物非常有效。此外,还系统地研究了主要操作参数(锰用量、高锰酸盐用量、施加电流密度、溶液 pH 值和污染物浓度)以及不同水基质对 E-PM-Mn 过程的影响。还提出了 E-PM-Mn 过程中 DCF 的可能降解途径。结果表明,基于活性 Mn(III)的 E-PM-Mn 系统可以为水处理创造一种更高效、可持续和能耗更低的技术。

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