Accelerated degradation of bisphenol A induced by the interaction of EGCG and Cu(II) in Cu(II)/EGCG/peroxymonosulfate process
Accelerated degradation of bisphenol A induced by the interaction of EGCG and Cu(II) in Cu(II)/EGCG/peroxymonosulfate process
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Cu(II)/EGCG/过一硫酸盐工艺中 EGCG 和 Cu(II) 相互作用导致双酚 A 加速降解
DOI：
10.1016/j.cej.2020.125134
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发表时间：
2020-09-01
影响因子：
15.1
通讯作者：
Shi, Zhou
中科院分区：
文献类型：
--
作者：
Cai, Ting;Bu, Lingjun;Shi, Zhou
过渡金属活化过一硫酸盐(PMS)在去除新出现的有机污染物方面具有广阔的前景，其中铜因其在饮用水中的可控浓度较高和有机铜农药的广泛使用而成为替代方案。铜(I)表现出良好的活化PMS的性能，而据报道铜(II)对自然环境中最稳定的价态PMS没有激活能力。在本研究中，由于铜(II)转化为铜(I)并被EGCG络合，铜(II)/PMS工艺对双酚A(BPA)的降解作用随着EGCG的加入而显著增强。通过批量实验研究了铜(II)、EGCG和PMS的浓度及其共存组分(包括天然有机物、碱度和氯离子)的影响。考察了溶液pH值和溶解氧对双酚A降解的影响，揭示了铜(I)和超氧阴离子自由基在铜(II)/EGCG/PMS过程中的作用，并测定了铜(I)的生成浓度。提出了铜(III)的可能生成途径。通过猝灭实验和电子顺磁共振分析，确定了Cu(II)/EGCG/PMS过程中的羟基自由基和硫酸根是BPA降解的主要贡献者。此外，对双酚A的转化产物进行了鉴定，并计算了它们各自的生态毒性。这项工作旨在揭示EGCG与铜(II)的相互作用，并对EGCG和PMS存在下的铜转化提供更深刻的见解。
Transition metals to activate peroxymonosulfate (PMS) has promising prospect to remove emerging organic contaminants, among which copper is an alternative because of its relatively high regulated concentration in drinking water and wide use of organic copper pesticide. Cu(I) shows good performance on the activation of PMS, while Cu(II) is reported to have no ability to activate PMS, which is the most stable valent in natural environment. In this study, degradation of bisphenol A (BPA) by Cu(II)/PMS process was significantly enhanced with involvement EGCG, because Cu(II) was transformed to Cu(I) and chelated by EGCG. Batch experiments were conducted to investigate the impacts of Cu(II), EGCG and PMS concentration and co-existing components including natural organic matters, alkalinity, and chloride ion. The impacts of solution pH and dissolved oxygen on BPA degradation were also evaluated to interpret the roles of Cu(I) and superoxide radical in Cu(II)/EGCG/ PMS process, and the generated concentration of Cu(I) was determined. Possible generation pathway of Cu(III) were also proposed. By quenching experiment and electron paramagnetic resonance analysis, hydroxyl radical and sulfate radical in Cu(II)/EGCG/PMS process were confirmed to be main contributors for BPA degradation. Furthermore, transformation products of BPA were identified and their respective eco-toxicities were calculated. This work aims to unravel the interaction of EGCG and Cu(II), and provide a deep insight to the copper conversion in the presence of EGCG and PMS.