Pulsed versus direct current electrochemical co-catalytic peroxymonosulfate-based system: Elevated degradation and energy efficiency with enhanced oxidation mechanisms.
Pulsed versus direct current electrochemical co-catalytic peroxymonosulfate-based system: Elevated degradation and energy efficiency with enhanced oxidation mechanisms.
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DOI：
10.1016/j.jhazmat.2023.132004
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发表时间：
2023-07
影响因子：
13.6
通讯作者：
Jiahao Wang;Xianhu Long;Igor Ying Zhang;Rongfu Huang
中科院分区：
文献类型：
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作者：
Jiahao Wang;Xianhu Long;Igor Ying Zhang;Rongfu Huang
本文研究了脉冲电化学(PE)体系活化过一硫酸盐(PMS)和添加Fe(III)以实现对磺胺甲恶唑(SMX)的高效降解，并与直流(DC)电化学体系进行了比较。优化了PE/PMS/Fe(III)体系的运行条件：脉冲频率为4 kHz，占空比为50%，pH为3，与DC/PMS/Fe(III)体系相比，能耗降低67.6%，降解性能增强。电子顺磁共振分析、猝灭和化学探针实验结果表明，体系中存在·OH、SO4·−和1O2，其中·OH起主导作用。在PE/PMS/Fe(III)体系中，这些活性物种的浓度比DC/PMS/Fe(III)体系中活性物种的浓度平均高出15%±21%。基于高分辨质谱学分析预测降解途径，实现了对SMX副产物的鉴定。随着处理时间的延长，PE/PMS/Fe(III)体系最终可以消除SMX的副产物。总体而言，PE/PMS/Fe(III)体系具有较高的能量和降解性能，是一种实用的废水处理策略。
In this work, the pulsed electrochemical (PE) system was investigated to activate peroxymonosulfate (PMS) with the addition of Fe(III) to achieve efficient degradation of sulfamethoxazole (SMX) with reduced energy consumption, in comparison with the direct current (DC) electrochemical system. The operational conditions of PE/PMS/Fe(III) system were optimized as 4 kHz pulse frequency, 50% duty cycle, and pH 3, at which 67.6% reduction of energy consumption and enhanced degradation performance were achieved compared to the DC/PMS/Fe(III) system. Results of electron paramagnetic resonance spectroscopy analysis and quenching and chemical probe experiment revealed the presence of•OH, SO4•−, and1O2in the system, with•OH being the dominant role. The concentrations of these active species were averagely 15 ± 1% higher in the PE/PMS/Fe(III) system than those of the DC/PMS/Fe(III) system. Identification of SMX byproducts was achieved based on high resolution mass spectrometry analysis to predict the degradation pathways. The SMX byproducts could eventually be eliminated by the PE/PMS/Fe(III) system with extended treatment time. Overall, the PE/PMS/Fe(III) system was demonstrated with high energy and degradation performance, and is appear to be an robust strategy for practical treatment of wastewater.