U(VI) and Eu(III), as representative elements of the hexavalent actinide and trivalent lanthanides (always as a chemical analogue for trivalent actinide), respectively, have attracted more and more attentions due to the widespread use of nuclear energy. Much effort has been focused on developing versatile materials for their uptake from aqueous solution. For the first time, we report here UiO-66 and its mono- (UiO-66-COOH) and di-carboxyl (UiO-66-2COOH) functional derivatives as robust adsorbents for efficient U(VI) and Eu(III) removal. It is found that the introduction of carboxyl groups greatly reduces the surface charge of UiO-66, thus guaranteeing excellent adsorption capacity at low pH. At pH = 3, for example, the adsorption capacity of UiO-66-2COOH for U(VI) and Eu(III) is more than 100 and 60 mg/g, respectively, while almost no adsorption occurs for pristine UiO-66. At pH = 4, both UiO-66-COOH and UiO-66-2COOH show high performance on U(VI) and Eu(III) removal. UiO-66-COOH has adsorption capacities of 80 and 43 mg/g for U(VI) and Eu(III), respectively, while the values for UiO-66-2COOH reach 150 and 80 mg/g, respectively. Also, all these materials achieve adsorption equilibrium within 100 min. More importantly, combining the needs of practical applications and the characteristics of high stability, high porosity, and excellent adsorption performance of UiO-66-2COOH, dynamic adsorption column experiments were successfully conducted; ∼99% U(VI)/Eu(III) can be efficiently adsorbed, and >90% adsorbed U(VI)/Eu(III) can be re-collected with dilute nitric acid solution, even after four adsorption–desorption cycles. The findings of this work demonstrate the application potential of metal–organic framework materials to remove radionuclides from environmental samples or nuclear waste liquids.
Polymeric ionic liquids (PILs) not only have the unique properties of ionic liquid, but also possess diverse mechanical properties of polymers. Due to their safety and conductivity, PILs-based gel polymer electrolytes (GPEs) are the promising candidates for the design of the devices. Here, we reported a facile approach to synthesize novel star-shaped GPE (named PIL-POSS-Li GPE) based on 1-vinyl-3-butylimidazolium hexafluorophosphate ionic liquid, octavinyl polyhedral oligomeric silsesquioxane (POSS) and LiPF 6 solution in one step via gamma-ray radiation. Compared with PIL-Li GPE without POSS, the incorporation of POSS into the PIL-Li GPE can improve properties of PIL-POSS-Li GPE due to the formation of a star-shaped structure, and the as-prepared PIL-POSS-Li GPE showed excellent compressive strength of 1617 kPa, high fracture compression stain of 79% and high ionic conductivity of 3.88 mS cm -1 at 25°C. What is more, the PIL-POSS-Li supercapacitor (SC) showed better electrochemical performance than PIL-Li SC.
A novel quaternary phosphonium-grafted hierarchically macro-/ mesoporous silica, named as HPS-C-P, was synthesized by alkylating hierarchically porous silica with trimethylchlorosilane and a subsequent twostep radiation-induced grafting of quaternary phosphonium. Fourier transform infrared, X-ray photoelectron spectroscopy (XPS), Brunauer−Emmett−Teller, and scanning electron microscopy analyses testified that alkyl and quaternary phosphonium groups were grafted uniformly in HPS-C-P. The adsorption of HPS-C-P for ReO 4− was evaluated and it was found that the adsorption equilibrium could be achieved within 4 min, and the adsorption isotherm was fitted well by the modified Langmuir model. The maximum ReO 4 − uptake of this adsorbent could reach 140.5 mg•g −1 , which was higher than the quaternary phosphonium-grafted hierarchically porous silica synthesized by a chemical method. HPS-C-P has good radiation resistance and cyclic adsorption performance, and the adsorption selectivity of HPS-C-P toward ReO 4 − in the presence of competitive anions, including NO 3 − , SO 4 2− , Cl − , CO 3 2− , and PO 4 3− , is extremely high, which is higher than most of the adsorbents reported in recent literature studies. Infrared and XPS analysis revealed that ReO 4 − was adsorbed onto HPS-C-P through the ion-exchange mechanism. This work provided a new method to produce highly efficient silica-based adsorbents to selectively remove Re from an aqueous solution even exposed to a radiation environment.
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