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ZIF-67/VTM 核壳结构的合成及其在水溶液中高效活化过一硫酸盐处理左氧氟沙星的研究。

Synthesis of core-heteroshell structure for ZIF-67/VTM and its efficient activation of peroxymonosulfate in treatment of levofloxacin from an aqueous solution.

机构信息

School of Ecology and Environment, Zhengzhou University, 100 Kexue Avenue, Zhengzhou, Henan, 450001, PR China.

School of Ecology and Environment, Zhengzhou University, 100 Kexue Avenue, Zhengzhou, Henan, 450001, PR China; Henan International Joint Laboratory of Water Cycle Simulation and Environmental Protection, Zhengzhou, 450001, PR China; Zhengzhou Key Laboratory of Water Resource and Environment, Zhengzhou, 450001, China; Yellow River Institute for Ecological Protection and Regional Coordination Development, Zhengzhou University, 100 Kexue Avenue, Zhengzhou, Henan, 450001, PR China; Henan Key Laboratory of Water Pollution Control and Rehabilitation Technology, Pingdingshan, Henan, 467036, China.

出版信息

Environ Res. 2022 Mar;204(Pt A):111986. doi: 10.1016/j.envres.2021.111986. Epub 2021 Sep 2.

Abstract

A core-heteroshell structural magnetic composite of ZIF-67/Vanadium-titanium magnetite (VTM) was successfully synthesized through a feasible solvothermal method and efficiently used in activation of peroxymonosulfate (PMS) for the treatment of levofloxacin (LVF) in an aqueous solution. The catalytic activity of the ZIF-67/VTM composite in LVF degradation was thoroughly evaluated, demonstrating the LVF removal rate could reach up to 93.3% within 60 min at ZIF-67/VTM composite dosage of 100 mg/L, PMS concertation of 75 mg/L, and the natural pH of 6.4. It is quite interesting that the carbon organic skeleton (in the ZIF-67 shell) have accelerated the internal electron transformation rate of the ZIF-67/VTM composite, thus efficiently promoting the O-O band (in PMS) breakage and the redox cycle of cobalt, further favoring the free radicals generation. The quenching experiments and EPR analysis results demonstrated that ·SO would play a crucial role in the LVF degradation process. Surprisingly, we have found that the introduction of Cl (at some certain dosage) would not always decrease the LVF degradation ratio, for a new reactive oxygen species (singlet oxygen) was emerged in this system. What's more, the ZIF-67 (as the wrapping structure) could stabilize the VTM (the inner structure) in changing reaction conditions, prompting a good adaptability at a wider pH range (3-10) for inhibiting the leaching of various metal ions into the aqueous solution. This novel ZIF-67/VTM composite could provide new ideas and routes for the removal of emerging pollutants from an aqueous solution.

摘要

一种 ZIF-67/钒钛磁铁矿(VTM)的核-杂核壳结构磁性复合材料通过一种可行的溶剂热法成功合成,并有效地用于活化过一硫酸盐(PMS)以处理水溶液中的左氧氟沙星(LVF)。彻底评估了 ZIF-67/VTM 复合材料在 LVF 降解中的催化活性,结果表明,在 ZIF-67/VTM 复合材料用量为 100mg/L、PMS 浓度为 75mg/L、自然 pH 值为 6.4 的条件下,LVF 的去除率在 60min 内可达到 93.3%。有趣的是,碳有机骨架(在 ZIF-67 壳内)加速了 ZIF-67/VTM 复合材料的内部电子转化速率,从而有效地促进了 PMS 中的 O-O 键断裂和钴的氧化还原循环,进一步有利于自由基的生成。猝灭实验和 EPR 分析结果表明,·SO 在 LVF 降解过程中起着关键作用。令人惊讶的是,我们发现引入 Cl(在一定剂量下)并不总是会降低 LVF 的降解率,因为在这个体系中出现了一种新的活性氧物种(单线态氧)。更重要的是,ZIF-67(作为包裹结构)可以在改变的反应条件下稳定 VTM(内部结构),在更宽的 pH 范围(3-10)下具有良好的适应性,可抑制各种金属离子浸出到水溶液中。这种新型 ZIF-67/VTM 复合材料为从水溶液中去除新兴污染物提供了新的思路和途径。

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