Fabricating iron-cobalt layered double hydroxide derived from metal-organic framework for the activation of peroxymonosulfate towards tetracycline degradation

Fabricating iron-cobalt layered double hydroxide derived from metal-organic framework for the activation of peroxymonosulfate towards tetracycline degradation
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制备源自金属有机骨架的铁钴层状双氢氧化物,用于活化过一硫酸盐以降解四环素

DOI:
10.1016/j.jssc.2020.121857
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发表时间:
2021-02
影响因子:
3.3
通讯作者:
Wei Li
Wei Li
中科院分区:
化学3区
文献类型:
--
作者:
Yue Wang;Jiao Cao;Zhaohui Yang;Weiping Xiong;Zhengyong Xu;Peipei Song;Meiying Jia;Saiwu Sun;Yanru Zhang;Wei Li

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本文以含钴咪唑类分子筛骨架材料ZIF-67为原料,在铁乙醇溶液中,室温下合成了铁钴层状双氢氧化物(FeCo-LDH)。以四环素(TC)为目标降解物,考察了催化剂对过一硫酸盐(PMS)的催化活性。实验结果表明,Fe/Co摩尔比为1.5的FeCo-LDH(FeCo-LDH-1.5)催化活性最高,在5 min内TC降解率可达92%。FeCo-LDH-1.5/PMS体系在TC浓度、初始pH、共存阴离子(Na+、Cl-、SO 42-)和腐殖酸(HA)等影响因素实验中表现出较高的稳定性和高效性。猝灭实验和电子顺磁共振(EPR)表征结果表明,O2·-和SO 4·-自由基是TC降解的主要反应物种。采用液相色谱-质谱联用仪(LC-MS)和三维荧光光谱仪(3D EEMs)对降解中间体和可能的降解途径进行了研究。此外,FeCo-LDH-1.5/PMS体系对实际废水具有较高的降解效率。与Fe 3 +/PMS和Co2+/PMS均相体系相比,FeCo-LDH-1. 5/PMS体系具有催化活性高、重复使用性好等优点。该研究为新型水滑石催化剂的合成提供了一种简便的方法,并在实际废水处理中表现出了良好的性能。
Herein, iron-cobalt layered double hydroxide (FeCo-LDH) was synthesized by sacrificing Co-containing zeolite imidazolate framework materials (ZIF-67) in iron ethanolic solution at room temperature. The catalytic performances of catalysts were investigated by activating peroxymonosulfate (PMS) for tetracycline (TC) degradation. Experimental results were demonstrated that FeCo-LDH with molar ratios of Fe and Co was 1.5 (FeCo-LDH-1.5) exhibited the highest catalytic activity, in which the TC degradation efficiency was reached to 92% within 5 ​min. The system of FeCo-LDH-1.5/PMS exhibited high stability and high efficiency in the influencing factor experiments including TC concentrations, initial pH, coexisting anions (Na+, Cl-, SO42−) and humic acid (HA). Results of quenching experiments and electron paramagnetic resonance (EPR) characterization showed that O2•-and SO4•-radicals were the foremost reactive species for TC degradation. Liquid chromatograph - mass spectrometer (LC-MS) and three-dimensional excitation emission matrix fluorescence spectro photometer (3D EEMs) were conducted to investigate the degradation intermediate and possible degradation pathway. Moreover, high degradation efficiency was implemented in actual wastewater by the FeCo-LDH-1.5/PMS system. Compared to Fe3+/PMS and Co2+/PMS homogeneous system, the FeCo-LDH-1.5/PMS system was exhibited advantages in catalytic activity and high reusability. This study provided a convenient method to synthesis advanced hydrotalcite-like catalysts, which showed remarkable performance in actual wastewater treatment.
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