通过活性氧主导的自由基过程揭示磺胺甲噁唑的降解机理和反应功效

Hongguo Zhang, Peitong Cen, Jiashuo Li, Chenxi Li, Jiayu Song, Qiong Wu, Wei Han, Lei Huang, Jia Yan, Shaoqi Zhou, Ce-Hui Mo, Meng Li
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摘要

本文首次将氧化钛电极与各种氧化剂结合,在电化学氧化(EO)系统中产生活性氧,用于去除不同的有机污染物。通过电化学测试、反应动力学、电子顺磁共振、量子化学和密度泛函理论计算,对有机污染物的去除率、反应机理和降解途径进行了评估。结果表明,12 分钟内磺胺甲噁唑(SMX)的去除率接近 100%,动力学速率常数高达 0.259 分钟,且动力学速率常数与静电电势密切相关。在通过自由基和非自由基过程去除 SMX 的过程中,过氧单硫酸盐(PMS)分子上的 O2 位点主导了自由基的生成。本研究为电化学激活 PMS 消除和降解废水中的各种有机污染物提供了一种新方法。
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Unraveling degradation mechanism and reaction efficacy of sulfamethoxazole via reactive oxygen species dominated radical process
Herein, the TiO electrode was combined for the first time with various oxidants to generate reactive oxygen species for the removal of different organic pollutants in an electrochemical oxidation (EO) system. The removal efficiency of organic pollutants, reaction mechanism, and degradation pathway were evaluated by electrochemical tests, reaction kinetics, electron paramagnetic resonance, quantum chemical, and density functional theory calculations. As a result, nearly 100 % removal efficiency of sulfamethoxazole (SMX) was achieved within 12 min with a high kinetic rate constant of 0.259 min, and the kinetic rate constant was strongly dependent on the electrostatic potential. The O2 site on the peroxymonosulfate (PMS) molecule dominated the radical generation for the removal of SMX via the radical and non−radical process. This current study offers a novel approach toward the electrochemical activation of PMS in the elimination and degradation of various organic pollutant from wastewater.
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