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多氨基协效的偕胺肟基吸附材料制备及其铀吸附性能

Preparation of amidoxime-based adsorption materials with a multi-amino synergistic effect and their uranium adsorption performance
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摘要 海水中的有机物易于与铀酰离子络合成稳定的化合物,从而影响铀吸附材料的吸附性能。本研究使用聚丙烯/聚乙烯无纺布(PP/PESNW)为基材,通过辐射诱导接枝聚合(RIGP)在基材表面引入甲基丙烯酸缩水甘油酯(GMA)单体后,分别与三亚乙基四胺(TETA)、四亚乙基五胺(TEPA)以及五乙烯基六胺(PEHA)进行开环反应引入氨基,与丙烯腈进行加成反应后,再进行胺肟化反应制备出具有多氨基协效官能团的偕胺肟基(AO)吸附材料P-TETA-AO、P-TEPA-AO、P-PEHA-AO。对制得的材料进行了结构表征、吸附性能探究以及吸附机理分析。实验结果表明:成功在基材表面修饰了3种不同链长功能高分子链,制备出目标偕胺肟基吸附材料;3种材料P-TETA-AO、P-TEPA-AO、P-PEHA-AO的铀吸附行为均符合准二级动力学模型以及Langmuir等温吸附模型;24 h内3种材料对铀的吸附容量分别为66.1 mg/g、63.22 mg/g、65.62 mg/g,在pH为5~9范围内表现出良好的吸附性能;5次吸附-解吸实验中材料的铀吸附率仅下降6%,解吸率维持在95%以上,具有良好的可再生性;模拟海水吸附实验中3种材料的铀去除率分别为72.94%、79.97%、87.78%,并且材料吸附性能随着接枝链的增长而上升;XPS结果表明,3种吸附材料在吸附铀的过程中,氨基与偕胺肟基均参与了与铀酰离子的配位,具有协效作用。 Uranyl ions in seawater are prone to complexing with organic matter,forming stable compounds that can impact the adsorption performance of uranium adsorption materials.Herein,glycidyl methacrylate(GMA)monomers were introduced onto the surface of the polypropylene/polyethylene nonwoven(PP/PE SNW)substract using radiation-induced graft polymerization(RIGP).Thereafter,three different polyamines,namely,triethylenetetramine(TETA),tetraethylenepentamine(TEPA),and pentaethylenehexamine(PEHA),were utilized to a ring-opening reaction,introducing the amine group into the substrate.This was followed by an addition reaction with acrylonitrile and an amidoxime reaction to produce the straight-chain-structured AO-based adsorbents,termed P-TETA-AO,P-TEPA-AO,and P-PEHA-AO.Subsequently,structural characterization,adsorption performance investigation,and adsorption mechanism analysis were performed.The experimental results confirm that three different functional polymer chains with varying chain lengths were successfully modified on the substrate surface and that the target amidoxime-based adsorption material was successfully prepared.The adsorption process followed a pseudo-second-order kinetic model,and the adsorption isotherm was well described by the Langmuir model.The adsorption capacities of P-TETA-AO,P-TEPA-AO,and P-PEHA-AO for uranium were 66.1 mg/g,63.22 mg/g,and 65.62 mg/g,respectively,within 24 h and exhibited adequate adsorption performance in the pH range of 5~9.The adsorption-desorption experiments indicated good regenerability,with only a 6%decrease in the uranium adsorption rate after five cycles,and a desorption ratio that was consistently above 95%.In the simulated seawater adsorption experiment,the uranium removal rates for P-TETA-AO,P-TEPA-AO,and P-PEHA-AO were found to be 72.94%,79.97%,and 87.78%,respectively,indicating that the adsorption performance improved with the growth of the grafting chain in a highly saline,multi-competitive ion environment.The X-ray photoelectron spectroscopy results indicate that du
作者 任婉宁 冯鑫鑫 韩泓炜 胡江涛 吴国忠 REN Wanning;FENG Xinxin;HAN Hongwei;HU Jiangtao;WU Guozhong(ShanghaiTech University,Shanghai 200031,China;Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai 201800,China;University of Chinese Academy of Sciences,Beijing 100049,China;Shanghai University,Shanghai 200444,China)
出处 《辐射研究与辐射工艺学报》 CAS CSCD 2024年第2期27-41,共15页 Journal of Radiation Research and Radiation Processing
基金 国家自然科学基金(22176194)资助。
关键词 辐射接枝聚合 氨基协效 有机纤维 铀吸附 电子束辐照 Radiation grafting polymerization Amino synergistic Polymer fibers Uranium adsorption Electron beam irradiation
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