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基于高分子碳水化合物的偕胺肟功能化金属有机骨架对 U(VI) 的去除的建模和光谱研究。

Modeling and spectroscopic investigation of U(VI) removal on porous amidoxime-functionalized metal organic framework derived from macromolecular carbohydrate.

机构信息

Key Laboratory of Pollution Exposure and Health Intervention of Zhejiang Province, College of Biological and Environmental Engineering, Zhejiang Shuren University, Hangzhou 310015, China.

Institute of Rural Energy and Ecology, Jilin Academy of Agricultural Sciences, Changchun 130033, China.

出版信息

Int J Biol Macromol. 2023 Jul 1;242(Pt 3):125043. doi: 10.1016/j.ijbiomac.2023.125043. Epub 2023 May 22.

Abstract

The investigation of interaction mechanism of U(VI) selective removal on amidoxime-functionalized metal organic framework (i.e., UiO-66(Zr)-AO) derived from macromolecular carbohydrate is conducive to apply metal organic frameworks in actual environmental remediation. The batch experiments showed that UiO-66(Zr)-AO displayed the fast removal rate (equilibrium time of 0.5 h), high adsorption capacity (384.6 mg/g), excellent regeneration performance (<10 % decrease after three cycles) towards U(VI) removal due to the unprecedented chemical stability, large surface area and simple fabrication. U(VI) removal at different pH can be satisfactorily fitted by diffuse layer modeling with cation exchange at low pH and an inner-sphere surface complexation at high pH. The inner-sphere surface complexation was further demonstrated by X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) analysis. These findings revealed that UiO-66(Zr)-AO can be an effective adsorbent to remove the radionuclides from aqueous solution, which is crucial for recycling of uranium resource and decreasing the uranium harm to the environment.

摘要

研究 U(VI)与偕胺肟功能化金属有机骨架(即 UiO-66(Zr)-AO)之间的相互作用机制有利于将金属有机骨架应用于实际环境修复中。批量实验表明,UiO-66(Zr)-AO 对 U(VI)的去除具有快速的去除速率(平衡时间为 0.5 h)、高吸附容量(384.6 mg/g)和优异的再生性能(经过三次循环后仅下降<10%),这归因于其前所未有的化学稳定性、大比表面积和简单的制备方法。在不同 pH 值下去除 U(VI)可以通过扩散层模型进行满意的拟合,在低 pH 值下发生阳离子交换,在高 pH 值下发生内球表面络合。X 射线吸收近边结构(XANES)和扩展 X 射线吸收精细结构(EXAFS)分析进一步证明了内球表面络合的存在。这些发现表明,UiO-66(Zr)-AO 可以作为一种有效的吸附剂从水溶液中去除放射性核素,这对于铀资源的回收和降低铀对环境的危害至关重要。

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