Chair of Inorganic Molecular Chemistry, Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01062 Dresden, Germany.
Chair of Inorganic Molecular Chemistry, Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01062 Dresden, Germany.
J Hazard Mater. 2022 Oct 15;440:129682. doi: 10.1016/j.jhazmat.2022.129682. Epub 2022 Jul 26.
Efficient removal of uranyl ions from wastewater requires excellent selectivity of the adsorbents. Herein, we report a new strategy using a high monomer/template molar ratio of 500:1 to prepare surface ion-imprinted brewer's spent grain (IIP-BSG) for selective U(VI) removal using binary functional monomers (2-hydroxyethyl methacrylate and diethyl vinylphosphonate) with high site accessibility and easy template removal. IIP-BSG exhibits a maximum U(VI) adsorption capacity of 165.7 mg/g, a high selectivity toward U(VI) in the presence of an excess amount of Eu(III) (Eu/U molar ratio = 20), a good tolerance of salinity, and a high reusability. In addition, mechanism studies have revealed electrostatic interaction and a coordination of uranyl ions by carboxyl and phosphoryl groups, the predominant contribution of high-energy (specific) sites during selective adsorption, and internal mass transfer as the rate-controlling step of U(VI) adsorption. Furthermore, IIP-BSG shows great potentials to separate U(VI) from lanthanides in simulated nuclear wastewater (pH = 3.5) and selectively concentrate U(VI) from simulated mine water (pH = 7.1). This study proves that the ion-imprinting effect can be achieved using a very low template amount with reduced production cost and secondary pollution, which benefits large-scale promotion of the ion-imprinted materials for selective uranyl ions removal.
从废水中高效去除铀酰离子需要吸附剂具有优异的选择性。在此,我们报告了一种新策略,使用单体/模板摩尔比高达 500:1 的高单体/模板摩尔比,使用具有高反应活性和易于模板去除的二元功能单体(2-羟乙基甲基丙烯酸酯和二乙烯基膦酸)制备表面离子印迹的啤酒糟(IIP-BSG),用于选择性去除 U(VI)。IIP-BSG 对 U(VI)的最大吸附容量为 165.7 mg/g,在 Eu(III)过量(Eu/U 摩尔比=20)的情况下对 U(VI)具有高选择性、良好的耐盐性和高可重复使用性。此外,机理研究表明,静电相互作用和铀酰离子与羧基和膦酸基团的配位作用、选择性吸附过程中高能(特异性)位点的主要贡献以及内部传质是 U(VI)吸附的速率控制步骤。此外,IIP-BSG 在模拟核废水中(pH = 3.5)从镧系元素中分离 U(VI)和从模拟矿山水中(pH = 7.1)选择性浓缩 U(VI)方面表现出巨大的潜力。这项研究证明,即使模板用量非常低,也可以实现离子印迹效应,从而降低生产成本和二次污染,有利于大规模推广用于选择性去除铀酰离子的离子印迹材料。