Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China; Université Clermont Auvergne, CNRS, SIGMA Clermont, Institut de Chimie de Clermont-Ferrand, F-63000 Clermont-Ferrand, France; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China.
Université Clermont Auvergne, CNRS, SIGMA Clermont, Institut de Chimie de Clermont-Ferrand, F-63000 Clermont-Ferrand, France.
Sci Total Environ. 2019 Dec 20;697:134188. doi: 10.1016/j.scitotenv.2019.134188. Epub 2019 Aug 30.
Persulfate (PS) activation reaction, which forms sulfate radical (SO), can be used to degrade organic pollutants in water. However, a drawback of this reaction is that the regeneration of ferrous ions requires a high concentration of hydrogen peroxide (Fenton-like reaction) or use of UV radiation. Catechin (CAT), a non-toxic antioxidant of natural origin from tea, is used in this work to improve the sulfate radical-mediated degradation of atenolol (ATL, a model pollutant) in water using relatively low concentrations of reactive chemical species (less than 100 μM). To the best of the author's knowledge, the direct effect of CAT on the oxidation state of iron, which is promoted by the reduction of ferric into ferrous ions with the enhancement of SO formation in the presence of PS, is demonstrated for the first time. The enhancement versus inhibition effect of CAT and the chemical mechanism of the iron-based activation process are explained. Results show that UVA radiation, which is representative of solar light, accelerates the initial degradation of ATL by more than 30% through ferric iron photolysis. Finally, a reaction mechanism leading to the formation of hydroxyl radicals (HO) and SO is proposed considering the implication of different activation/reaction chemical steps.
过硫酸盐(PS)活化反应会生成硫酸根自由基(SO),可用于降解水中的有机污染物。然而,该反应的一个缺点是亚铁离子的再生需要高浓度的过氧化氢(类芬顿反应)或使用紫外线辐射。儿茶素(CAT)是一种天然来源的无毒抗氧化剂,来自茶叶,用于提高水中的硫酸根自由基介导的阿替洛尔(ATL,一种模型污染物)的降解,使用的反应性化学物质浓度相对较低(小于 100μM)。据作者所知,儿茶素对铁的氧化态的直接影响首次得到证明,这种影响是通过还原三价铁离子形成二价铁离子,同时在 PS 存在下增强 SO 的形成来促进的。解释了 CAT 的增强与抑制效应以及基于铁的活化过程的化学机制。结果表明,代表太阳光的 UVA 辐射通过铁离子光解加速了 ATL 的初始降解,超过 30%。最后,考虑到不同的活化/反应化学步骤的影响,提出了一种导致形成羟基自由基(HO)和 SO 的反应机制。