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Fabrication of Epigallocatechin-3-gallate (EGCG) functionalized Mn3O4 for enhanced degradation of carbamazepine with peroxymonosulfate activation
Process Safety and Environmental Protection ( IF 6.9 ) Pub Date : 2021-11-28 , DOI: 10.1016/j.psep.2021.11.033
Lei Zhu 1 , Zhou Shi 1 , Lin Deng 1 , Jing Chen 2 , Haojie Zhang 1
Affiliation  

Peroxymonosulfate activation via heterogeneous catalyst was broadly applied for the treatment of PPCPs. In this work, a novel material of Epigallocatechin-3-gallate (EGCG) fuctionalized Mn3O4 nano-octahedra (E@MO) was synthesized and utilized for the degradation of carbamazepine. Various technologies such as X-ray diffraction, Fourier transform-infrared spectroscopy, Scanning electron microscope, Transmission electron microscope, Brunauer-Emmett-Teller and X-ray photoelectron spectroscopy were employed for the characterization of the as-synthesized catalyst. The results depicted that under the conditions of CBZ concentration 5 mg/L, PMS concentration 1 mM, catalyst dosage 0.2 g/L, initial pH 5.8 and 25 °C, the targeted pollutant could be totally degraded in 60 min with a rate constant of 0.0622 min−1. When temperature raised to 45 °C, CBZ was removed completely in 20 min and the rate constant (0.1668 min−1) was 2.59 times than that of 25 °C, implying the degradation process was an endothermic reaction. Scavenging experiments and EPR analysis confirmed the main reactive oxygen species generated in the reaction were sulfate radical (SO4single bond) and hydroxyl radical (OH), while SO4single bond serviced as the leading role. Due to the reduction property of EGCG, compared with bare Mn3O4, the CBZ degradation was markably enhanced and the degradation reaction were accurately matched with the pseudo first-order kinetics equation. The possible twelve intermediates produced in the decomposition of CBZ were identified by HPLC-MS/MS, their ecotoxicity were evaluated and compared by ECOSAR model. Together with the consequences, the degradation mechanism of CBZ in the E@MO/PMS system was propounded.



中文翻译:

表没食子儿茶素-3-没食子酸酯 (EGCG) 功能化 Mn3O4 的制备,用于通过过硫酸盐活化增强卡马西平的降解

通过多相催化剂活化过硫酸盐被广泛应用于 PPCPs 的处理。在这项工作中,表没食子儿茶素-3-没食子酸酯 (EGCG) 功能化 Mn 3 O 4的新型材料纳米八面体(E@MO)被合成并用于降解卡马西平。X射线衍射、傅里叶变换红外光谱、扫描电子显微镜、透射电子显微镜、Brunauer-Emmett-Teller和X射线光电子能谱等各种技术用于表征合成的催化剂。结果表明,在CBZ浓度5 mg/L、PMS浓度1 mM、催化剂用量0.2 g/L、初始pH 5.8和25℃条件下,目标污染物可在60 min内完全降解,速率常数为0.0622 分钟-1。当温度升至 45 °C 时,CBZ 在 20 min 内完全去除,速率常数 (0.1668 min -1) 是 25 °C 的 2.59 倍,表明降解过程是吸热反应。清除实验和EPR分析证实反应中产生的主要活性氧物质是硫酸根(SO 4 单键 )和羟基自由基( OH),而SO 4 单键起主导作用。由于 EGCG 的还原性,与裸 Mn 3 O 4 相比,CBZ降解显着增强,降解反应与伪一级动力学方程准确匹配。通过HPLC-MS/MS鉴定了CBZ分解过程中可能产生的12种中间体,并通过ECOSAR模型对它们的生态毒性进行了评价和比较。连同结果,提出了CBZ在E@MO/PMS系统中的降解机制。

更新日期:2021-12-03
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