College of Environmental Engineering, Henan University of Technology, Zhengzhou, Henan 450001, China; Henan Academician Workstation of Combined Pollution Control and Research, Zhengzhou, Henan 450001, China.
College of Environmental Engineering, Henan University of Technology, Zhengzhou, Henan 450001, China.
Sci Total Environ. 2021 Mar 20;761:143956. doi: 10.1016/j.scitotenv.2020.143956. Epub 2020 Dec 4.
In this study, the synergetic adsorption and Fenton-like degradation of tetracycline hydrochloride (TCH) by magnetic spent bleaching earth carbon (Mag-SBE@C) with HO were developed and performed, with 91.5% of TCH degradation efficiency and 42.1% of TOC removal efficiency. The effects of the reaction parameters (temperature, initial pH, catalyst dosage, molar ratio of TCH to HO) on TCH degradation in Mag-SBE@C/HO system were studied. Under the optimal conditions (temperature 41.1 °C, initial pH 4.89 and molar ratio of HO to TCH 114.435) forecasted by response surface methodology (RSM), high TCH degradation efficiency (99%) was achieved. Also, four cycling tests were performed to confirm the excellent stability and regeneration ability of Mag-SBE@C in presence of HO. In addition, the characteristics of Mag-SBE@C after reaction are analyzed in details via scanning electron microscope (SEM), energy dispersive spectrometer (EDS), Brunner-Emmet-Teller (BET), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectrum (FTIR) and X-ray diffraction (XRD), and it was found that FeO nanoparticles on Mag-SBE@C surface acted as co-catalyst and participated in degradation and improved reaction efficiency, while its properties were not greatly changed. The quenching experiments showed that hydroxyl radicals on Mag-SBE@C surface (OH) were dominant in Mag-SBE@C/HO system. Meanwhile, three possible TCH degradation pathways were given based on the possible intermediates determined by liquid chromatography quadrupole-time-of-flight mass spectrometry (LC-Q-TOF-MS/MS). Mag-SBE@C is an excellent heterogeneous Fenton-like catalyst, exhibiting greatly potential to antibiotics elimination.
在这项研究中,开发并实施了磁性废漂白土碳(Mag-SBE@C)与 HO 的协同吸附和类 Fenton 降解盐酸四环素(TCH),TCH 的降解效率为 91.5%,TOC 的去除效率为 42.1%。研究了反应参数(温度、初始 pH 值、催化剂用量、TCH 与 HO 的摩尔比)对 Mag-SBE@C/HO 体系中 TCH 降解的影响。在响应面法(RSM)预测的最佳条件(温度 41.1°C、初始 pH 4.89 和 HO 与 TCH 的摩尔比 114.435)下,TCH 的降解效率达到 99%。此外,还进行了四次循环测试,以确认 HO 存在下 Mag-SBE@C 的优异稳定性和再生能力。此外,通过扫描电子显微镜(SEM)、能谱(EDS)、Brunauer-Emmett-Teller(BET)、X 射线光电子能谱(XPS)、傅里叶变换红外光谱(FTIR)和 X 射线衍射(XRD)详细分析了反应后 Mag-SBE@C 的特性,发现 Mag-SBE@C 表面的 FeO 纳米颗粒作为共催化剂参与降解并提高了反应效率,但其性质没有发生很大变化。猝灭实验表明,Mag-SBE@C 表面的羟基自由基(OH)是 Mag-SBE@C/HO 体系中的主要自由基。同时,根据液相色谱四极杆飞行时间质谱(LC-Q-TOF-MS/MS)确定的可能中间体,给出了三种可能的 TCH 降解途径。Mag-SBE@C 是一种优异的非均相类 Fenton 催化剂,在抗生素消除方面具有很大的潜力。