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Electrochemical activation of periodate with graphite electrodes for water decontamination: Excellent applicability and selective oxidation mechanism
Water Research ( IF 12.8 ) Pub Date : 2023-05-25 , DOI: 10.1016/j.watres.2023.120128
Mengfan Luo 1 , Heng Zhang 1 , Yang Shi 2 , Jia Zhao 1 , Can Feng 1 , Jialong Yin 1 , Yang Liu 1 , Peng Zhou 1 , Zhaokun Xiong 1 , Bo Lai 1
Affiliation  

Advanced oxidation technologies based on periodate (PI, IO4) have garnered significant attention in water decontamination. In this work, we found that electrochemical activation using graphite electrodes (E-GP) can significantly accelerate the degradation of micropollutants by PI. The E-GP/PI system achieved almost complete removal of bisphenol A (BPA) within 15 min, exhibited unprecedented pH tolerance ranging from pH 3.0 to 9.0, and showed more than 90% BPA depletion after 20 h of continuous operation. Additionally, the E-GP/PI system can realize the stoichiometric transformation of PI into iodate, dramatically decreasing the formation of iodinated disinfection by-products. Mechanistic studies confirmed that singlet oxygen (1O2) is the primary reactive oxygen species in the E-GP/PI system. A comprehensive evaluation of the oxidation kinetics of 1O2 with 15 phenolic compounds revealed a dual descriptor model based on quantitative structure−activity relationship (QSAR) analysis. The model corroborates that pollutants exhibiting strong electron-donating capabilities and high pKa values are more susceptible to attack by 1O2 through a proton transfer mechanism. The unique selectivity induced by 1O2 in the E-GP/PI system allows it to exhibit strong resistance to aqueous matrices. Thus, this study demonstrates a green system for the sustainable and effective elimination of pollutants, while providing mechanistic insights into the selective oxidation behaviour of 1O2.



中文翻译:

用石墨电极电化学活化高碘酸盐用于水净化:优异的适用性和选择性氧化机制

基于高碘酸盐 (PI, IO 4 - ) 的高级氧化技术在水净化领域引起了广泛关注。在这项工作中,我们发现使用石墨电极 (E-GP) 进行电化学活化可以显着加速 PI 对微污染物的降解。E-GP/PI 系统在 15 分钟内几乎完全去除了双酚 A (BPA),表现出前所未有的 pH 耐受性,范围从 pH 3.0 到 9.0,并且在连续运行 20 小时后显示超过 90% 的 BPA 消耗。此外,E-GP/PI系统可以实现PI向碘酸盐的化学计量转化,显着减少碘化消毒副产物的形成。机理研究证实单线态氧 ( 1 O 2) 是 E-GP/PI 系统中的主要活性氧。对1 O 2与 15 种酚类化合物的氧化动力学的综合评估揭示了基于定量构效关系 (QSAR) 分析的双描述符模型。该模型证实,具有强供电子能力和高 p K a值的污染物更容易通过质子转移机制受到1 O 2的攻击。1 O 2诱导的独特选择性在 E-GP/PI 系统中,它对水性基质表现出很强的抵抗力。因此,本研究展示了一个可持续且有效消除污染物的绿色系统,同时提供了对1 O 2的选择性氧化行为的机理见解。

更新日期:2023-05-28
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