One-step synthesis of Mn-doped MIL-53(Fe) for synergistically enhanced generation of sulfate radicals towards tetracycline degradation
One-step synthesis of Mn-doped MIL-53(Fe) for synergistically enhanced generation of sulfate radicals towards tetracycline degradation
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一步合成锰掺杂的 MIL-53(Fe)，协同增强硫酸根的产生，促进四环素降解
DOI：
10.1016/j.jcis.2020.07.045
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发表时间：
2020
影响因子：
9.9
通讯作者：
Zhu Juan
中科院分区：
文献类型：
--
作者：
Yu Jun;Cao Jiao;Yang Zhaohui;Xiong Weiping;Xu Zhengyong;Song Peipei;Jia Meiying;Sun Saiwu;Zhang Yanru;Zhu Juan
摘要本文采用溶剂热一锅法制备了Mn掺杂的MIL-53（Fe）催化剂，并将其用于过一硫酸盐（PMS）活化降解水溶液中的四环素（TC）。利用SEM、FTIR、XRD等手段对材料的形貌和结构进行了表征。结果表明，Mn-MIL-53（Fe）-0.3对TC的去除效果最好，去除率可达93.2%。考察了Mn MIL 53（Fe）在不同初始pH值、共存阴离子Cl-、CO32-、SO42-和腐殖酸（HA）条件下对TC的催化活性。热力学实验结果表明，该催化过程为吸热过程。此外，结合捕获实验结果和电子顺磁共振（EPR）表征结果表明，SO4·-和H O-是参与反应的活性自由基。更重要的是，根据X射线光电子能谱的结果，详细讨论了可能的活化机制。活性物种是由Mn-MIL-53（Fe）有效活化的PMS上的Fe（II）和Mn（II）活性中心产生的。最后，该催化剂在实际废水中也表现出了良好的性能，并表现出良好的可循环性。Mn-MIL-53（Fe）/PMS体系在含磷废水处理中具有良好的应用前景。
Abstract Herein, Mn-doped MIL-53 (Fe) were fabricated via one-pot solvothermal method and used for peroxymonosulfate (PMS) activation towards tetracycline (TC) degradation from aqueous solution. The characterizations of SEM, FTIR and XRD were utilized to reveal the morphology and structure of the materials. The results showed that Mn-MIL-53 (Fe)-0.3 displayed the optimal catalytic performance, the removal efficiency of TC could reach 93.2%. Moreover, the catalytic activity of Mn-MIL-53 (Fe) towards TC under different initial pH values, co-existing anions (C l-, CO 3 2-and SO 4 2-) and humic acid (HA) were investigated. The results of thermodynamic experiment suggested that the catalytic process was endothermic. In addition, integrated with capture experiments results and the characterization results of electron paramagnetic resonance (EPR), which revealed that SO 4·-and H O-were the reactive radicals involving in the reaction. More importantly, the possible activation mechanism was discussed in detail based on the X-ray photoelectron spectroscopy results. The active species were generated by the active sites of Fe (II) and Mn (II) on Mn-MIL-53 (Fe) effectively activated PMS. Furthermore, the degradation intermediates and possible degradation pathway were investigated by LC-MS. Finally, the catalyst also showed good performance in actual wastewater and demonstrated good recyclability. The Mn-MIL-53 (Fe)/PMS system exhibited a promising application prospect for antibiotic-containing waste water treatment.