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纳米-Fe@NdFeB/AC 磁催化粒子电极的合成及其在电辅助过硫酸盐工艺降解 2,4,6-三氯苯酚中的应用。

Synthesis of Nano-Fe@NdFeB/AC magnetic catalytic particle electrodes and application in the degradation of 2,4,6-trichlorophenol by electro-assisted peroxydisulfate process.

机构信息

Key Laboratory of Environmental Materials and Pollution Control, the Education Department of Jilin Province, Jilin Normal University, Siping, People's Republic of China.

College of Environmental Science and Engineering, Jilin Normal University, Siping, People's Republic of China.

出版信息

Environ Technol. 2020 Aug;41(19):2464-2477. doi: 10.1080/09593330.2019.1567826. Epub 2019 Jan 22.

Abstract

The coupling of electrolysis and the peroxydisulfate (PDS) activation was selected in this study to degrade solution-phase 2,4,6-trichlorophenol (TCP). To enhance the PDS activation efficiency and catalytic recycling ratio, a novel magnetic activator, nano iron coated on neodymium iron boron/activated carbon nanocomposite (Nano-Fe@NdFeB/AC), was synthesized and utilized as catalytic particle electrodes. To increase the mass transfer ability, a novel magnetic internal circulation electrolytic reactor (MICE) was established. The results indicated that globular Fe, with sizes ranging from 25 nm to 300 nm, is present on the surface of the catalyst. This catalyst has sufficient magnetism to be separated by the magnetic separation method and its specific saturation magnetization and residual magnetization were 1.48 and 0.26 emu/g, respectively. At the optimal condition of [pH]= 9.0, [NaSO]= 2.0 mmol/L, [Nano-Fe@NdFeB/AC]= 5.0 g/L and I = 50 mA, the TOC percentage of removal could reach 84% after 30 min of reaction. The TCP mineralization follows pseudo-first-order kinetics. The intermediate products of 2,6-dichloro-2,5-cyclohexadiene-1,4-dione, Tetrachloro-hydroquinone, and 2,3,5,6-tetrachloro-p-benzoquinone were found during the reaction. TCP mineralization was confirmed to have a hybrid mechanism involving reductive dechlorination with Fe, •OH addition oxidation and electron capture by SO• . This study provides a new method for the treatment of degradation-resistant pollutants.

摘要

本研究选择电解与过一硫酸盐(PDS)活化相结合的方法来降解溶液相中的 2,4,6-三氯苯酚(TCP)。为了提高 PDS 活化效率和催化循环比,合成了一种新型磁性活化剂,即纳米铁包裹在钕铁硼/活性炭纳米复合材料(Nano-Fe@NdFeB/AC)上,并将其用作催化颗粒电极。为了提高传质能力,建立了一种新型的磁性内循环电解反应器(MICE)。结果表明,催化剂表面存在尺寸为 25nm 至 300nm 的球形 Fe。该催化剂具有足够的磁性,可通过磁分离法进行分离,其比饱和磁化强度和剩余磁化强度分别为 1.48 和 0.26 emu/g。在最佳条件下 [pH]=9.0、[NaSO]=2.0mmol/L、[Nano-Fe@NdFeB/AC]=5.0g/L 和 I=50mA 时,反应 30min 后 TOC 的去除率可达 84%。TCP 的矿化遵循准一级动力学。反应过程中发现了 2,6-二氯-2,5-环己二烯-1,4-二酮、四氯对苯二酚、2,3,5,6-四氯-对苯醌等中间产物。TCP 的矿化被证实具有混合机制,涉及 Fe 的还原脱氯、•OH 加成氧化和 SO• 的电子捕获。本研究为降解难降解污染物提供了一种新方法。

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