School of Hydraulic and Environmental Engineering, Changsha University of Science & Technology, Changsha, 410114, PR China; Key Laboratory of Dongting Lake Aquatic Eco-Environmental Control and Restoration of Hunan Province, Changsha, 410114, PR China; Engineering and Technical Center of Hunan Provincial Environmental Protection for River-Lake Dredging Pollution Control, Changsha, 410114, PR China.
School of Hydraulic and Environmental Engineering, Changsha University of Science & Technology, Changsha, 410114, PR China.
Environ Res. 2023 Dec 15;239(Pt 1):116842. doi: 10.1016/j.envres.2023.116842. Epub 2023 Aug 6.
In this study, a novel catalyst based on MIL-53(Fe) was synthesized and modified through sublimed sulfur (S-MIL-53(Fe)) to induce a synergistic effect of surface adsorption and persulfate activation. The S-doped modification not only increased the surface area but also accelerated the electron transfer process of the iron cycle. The performance of the newly synthesized S-MIL-53(Fe) adsorptive catalyst was evaluated by chemical adsorption and peroxydisulfate (PDS) activated removal of an emerging pollutants, oxytetracycline (OTC). The S-MIL-53(Fe) adsorptive catalyst was able to adsorb 61.7% of OTC after 120 min, and the removal efficiency reached 84.8% within 5 min after PDS dosing. The boosting effect of sulfur on the system was confirmed by characterization analysis and experimental testing. Even after 7 cycles, the removal efficiency of S-MIL-53(Fe) (69.0%) for OTC remained superior to that of pure MIL-53(Fe) (25.1%). Additionally, the adsorption kinetics and adsorption isotherm model of the material were investigated. The possible OTC degrading process was proposed based on radical quenching and electron paramagnetic resonance (EPR). This study provides a feasible way to fabricate an S-doped MIL-53(Fe) adsorptive catalyst for the remediation of antibiotics-containing wastewater.
在这项研究中，合成了一种基于 MIL-53(Fe) 的新型催化剂，并通过升华硫（S-MIL-53(Fe)）进行了修饰，以诱导表面吸附和过硫酸盐活化的协同效应。S 掺杂的修饰不仅增加了表面积，而且加速了铁循环的电子转移过程。通过化学吸附和过氧二硫酸盐（PDS）的激活去除新兴污染物土霉素（OTC）来评估新合成的 S-MIL-53(Fe) 吸附催化剂的性能。S-MIL-53(Fe) 吸附催化剂在 120 分钟内能够吸附 61.7%的 OTC，在投加 PDS 后 5 分钟内去除效率达到 84.8%。通过特征分析和实验测试证实了硫对系统的促进作用。即使经过 7 个循环，S-MIL-53(Fe)（69.0%）对 OTC 的去除效率仍优于纯 MIL-53(Fe)（25.1%）。此外，还研究了该材料的吸附动力学和吸附等温线模型。根据自由基猝灭和电子顺磁共振（EPR）提出了可能的 OTC 降解过程。这项研究为制造用于修复含抗生素废水的 S 掺杂 MIL-53(Fe) 吸附催化剂提供了一种可行的方法。
