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Selective lanthanides sequestration based on a self-assembled organosilica

机译:基于自组装有机硅的选择性镧系元素螯合

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In this paper, we investigate the cation-exchange properties of a self-assembled hybrid material towards trivalent ions, lanthanides (La ~(3+), Eu~(3+), Gd~(3+), Yb~(3+)) and Fe ~(3+). The bis-zwitterionic lamellar material was prepared by sol-gel process from only 3-aminopropyltriethoxysilane (APTES), succinic anhydride, and ethylenediamine. In ethanol heated under reflux, the exchange ethylenediammonium versus Ln~(3+) proved to be complete by complexometry measurements and elemental analyses, one Clion per one Ln~(III) remaining as expected for charge balance. In aqueous solution at 20 °C, the material was found to be selective towards lanthanide in spite of the similarity of their ionic radii. The cation uptake depends on the nature of the salt, the difference between two lanthanides reaching up to 20% in some cases. Finally, ion-exchange reaction with FeCl_3 was chosen as a probe to get more information on the material after incorporation of trivalent ions. Based on M?ssbauer spectroscopic investigations on the resulting material in conjunction with the XRD analysis of materials containing trivalent ions, a structural model was proposed to describe the incorporation of trivalent ions by exchange reaction within the original zwitterionic material.
机译:本文研究了自组装杂化材料对三价离子镧系元素(La〜(3 +),Eu〜(3 +),Gd〜(3 +),Yb〜(3+)的阳离子交换性质))和Fe〜(3+)。双两性离子层状材料仅通过3-氨基丙基三乙氧基硅烷(APTES),琥珀酸酐和乙二胺通过溶胶-凝胶法制备。在回流加热的乙醇中,通过络合度测定和元素分析证明乙二铵与Ln〜(3+)的交换完成,每电荷Ln〜(III)保留一个Clion,这是电荷平衡所期望的。在20°C的水溶液中,尽管其离子半径相似,但发现该材料对镧系元素具有选择性。阳离子的摄取取决于盐的性质,在某些情况下,两种镧系元素之间的差异最高可达20%。最后,选择了与FeCl_3进行离子交换反应作为探针,以在引入三价离子后获得有关该材料的更多信息。基于对所得物质的Msssbauer光谱学研究以及对含三价离子物质的XRD分析,提出了一种结构模型来描述三价离子通过交换反应在原始两性离子物质中的结合。

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