Electrochemical activation of periodate with graphite electrodes for water decontamination: Excellent applicability and selective oxidation mechanism

化学 单线态氧 高碘酸盐 电化学 氧化剂 水溶液 人体净化 氧气 光化学 组合化学 电极 有机化学 物理 物理化学 核物理学
作者
Meng-Fan Luo,Heng Zhang,Yang Shi,Jia Zhao,Can Feng,Jialong Yin,Yang Liu,Peng Zhou,Zhaokun Xiong,Bo Lai
出处
期刊:Water Research [Elsevier BV]
卷期号:240: 120128-120128 被引量:49
标识
DOI:10.1016/j.watres.2023.120128
摘要

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.
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