Xie Zhi-Hui, He Chuan-Shu, He Yong-Li, Yang Shu-Run, Yu Si-Ying, Xiong Zhaokun, Du Ye, Liu Yang, Pan Zhi-Cheng, Yao Gang, Lai Bo
State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.
State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.
Water Res. 2023 Apr 1;232:119666. doi: 10.1016/j.watres.2023.119666. Epub 2023 Jan 26.
As an oxidant, peracetic acid (PAA) is gradually applied in advanced oxidation processes (AOPs) for pollutants degradation due to its high oxidation and low toxicity. In this study, the prepared CoFe-LDH showed excellent PAA activation ability for efficient degradation of various pharmaceuticals with a removal efficiency ranging from 82.3% to 100%. Taking sulfamethoxazole (SMX) as a model pharmaceutical, it's found that organic radical (R-O) with high concentration of 5.27 × 10 M is the dominant ROS responsible for contaminants degradation. Further analysis demonstrated that bimetallic synergistic effect between Co and Fe can improve electron transfer ability of CoFe-LDH, resulting in the accelerated conversion of Co from +3 to +2 valence state with a high reaction rate (4.3 × 10-1.483 × 10 M s) in this system. Density functional theory (DFT) reveals that C1, C3, C5 and N11 with higher ƒ and ƒvalues concentrated on aniline group of SMX are the main attack sites, which is consistent with the results of degradation products. Besides, CoFe-LDH/PAA system can effectively reduce biological toxicity after reaction, due to lower biotoxicity of degradation products and the carbon sources provided by PAA. In application, CoFe-LDH/PAA system was capable of resisting the influence of water matrix and effectively removing pollutants in actual hospital wastewater. Importantly, this study comprehensively evaluated the ability of CoFe-LDH/PAA system to remove organics and improve the biodegradability of actual hospital wastewater, providing guidance for application of PAA activation system.
作为一种氧化剂,过氧乙酸(PAA)因其高氧化性和低毒性,正逐渐应用于高级氧化过程(AOPs)中以降解污染物。在本研究中,制备的CoFe-LDH对多种药物具有优异的PAA活化能力,降解效率在82.3%至100%之间。以磺胺甲恶唑(SMX)为模型药物,发现浓度高达5.27×10 M的有机自由基(R-O)是负责污染物降解的主要活性氧。进一步分析表明,Co和Fe之间的双金属协同效应可以提高CoFe-LDH的电子转移能力,导致该体系中Co从+3价态加速转化为+2价态,反应速率较高(4.3×10 - 1.483×10 M s)。密度泛函理论(DFT)表明,SMX苯胺基团上具有较高ƒ和ƒ值的C1、C3、C5和N11是主要攻击位点,这与降解产物的结果一致。此外,CoFe-LDH/PAA体系反应后能有效降低生物毒性,这是由于降解产物的生物毒性较低以及PAA提供的碳源。在实际应用中,CoFe-LDH/PAA体系能够抵抗水基质的影响并有效去除实际医院废水中的污染物。重要的是,本研究全面评估了CoFe-LDH/PAA体系去除有机物和提高实际医院废水可生物降解性的能力,为PAA活化体系的应用提供了指导。