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    赵 钰, 林海波, 毕秋艳, 王 晓, 张国亮, 刘 富. 钴铁双金属基碳纳米管催化膜的制备及高效去除四环素[J]. 功能高分子学报,2023,36(4):381-391. doi: 10.14133/j.cnki.1008-9357.20230309001
    引用本文: 赵 钰, 林海波, 毕秋艳, 王 晓, 张国亮, 刘 富. 钴铁双金属基碳纳米管催化膜的制备及高效去除四环素[J]. 功能高分子学报,2023,36(4):381-391. doi: 10.14133/j.cnki.1008-9357.20230309001
    ZHAO Yu, LIN Haibo, BI Qiuyan, WANG Xiao, ZHANG Guoliang, LIU Fu. Preparation and Efficient Tetracycline Removal of Co-Fe Bimetallic Carbon Nanotubes Catalytic Membranes[J]. Journal of Functional Polymers, 2023, 36(4): 381-391. doi: 10.14133/j.cnki.1008-9357.20230309001
    Citation: ZHAO Yu, LIN Haibo, BI Qiuyan, WANG Xiao, ZHANG Guoliang, LIU Fu. Preparation and Efficient Tetracycline Removal of Co-Fe Bimetallic Carbon Nanotubes Catalytic Membranes[J]. Journal of Functional Polymers, 2023, 36(4): 381-391. doi: 10.14133/j.cnki.1008-9357.20230309001

    钴铁双金属基碳纳米管催化膜的制备及高效去除四环素

    Preparation and Efficient Tetracycline Removal of Co-Fe Bimetallic Carbon Nanotubes Catalytic Membranes

    • 摘要: 采用煅烧钴铁双金属的普鲁士蓝类似物(CoFe PBA)的方法获得了包裹钴铁合金的碳纳米管催化剂(CoFe@Cs),然后使用真空抽滤制备复合催化膜。通过扫描电子显微镜(SEM)、X射线衍射图谱(XRD)、X射线光电子能谱(XPS)等对样品的形貌及组成进行表征;以四环素(TC)为目标污染物对所制备的催化剂及催化膜的催化机理及性能进行测试。结果表明,改变煅烧温度可以有效调控碳纳米管催化剂的形貌及组成。在900 ℃煅烧温度下制备的碳纳米管催化剂(CoFe@Cs-900)主要产生以硫酸根自由基及单线态氧为主的活性氧物质,并可对TC进行快速的降解去除。由其组装的碳纳米管催化膜在24 h错流过滤中对TC的降解去除率大于99%,水通量保持在172 L/(m2·h),表现出优异的膜催化降解性能。

       

      Abstract: Carbon nanotube catalysts encapsulating cobalt-iron (CoFe) alloy nanoparticles (CoFe@Cs) were synthesized by calcination of cobalt-iron bimetallic Prussian Blue analogs (CoFe PBA), and further assembled on polyethersulfone (PES) membrane support by vacuum filtration to prepare composite catalytic membranes for catalytic activation of peroxymonosulfate and efficient degradation of tetracycline (TC). The morphology and structure of the samples were analyzed by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The composition was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. Based on the morphology, composition and performance, carbon nanotube catalysts (CoFe@Cs-900) were selected from the prepared series of CoFe@Cs, and further the reactive oxygen species (ROS) in the catalytic process was analyzed by reactive oxygen quenching experiments and electron paramagnetic resonance (EPR). The stability of the carbon nanotube catalytic membrane under long-term operation was tested under optimized conditions. The results showed that the calcination temperature played an important role in regulating the morphology and composition of the catalysts. Among them, the carbon nanotube catalyst prepared by calcination at 900 ℃ can produce the reactive oxygen species, including sulfate radicals (·SO4) and singlet oxygen (1O2), for the rapid removal of tetracycline. The carbon nanotube catalytic membrane achieved more than 99% removal of TC in continuous 24 h cross-flow filtration, and the water flux was maintained at 172 L/(m2·h). Overall, the catalytic membrane showed excellent degradation performances and potential application.

       

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