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Exploiting the nodes of metal-organic framework by grafting functional organic molecules for synergistic uranium extraction
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2024-11-19 , DOI: 10.1016/j.seppur.2024.130607
Zixuan Ma, Chang Sun, Danyan Lin, Wen Yao, Hairui Hou, Dedong Wu, Xinrong Guo, Xin Yu, Xiangxue Wang

High-efficiency elimination of uranium was a research hotspot from the aspect of nuclear energy development. Metal chelators and porous materials were two cutting-edge technologies for the recovery and separation of uranium from wastewater. However, there was only limited success in transferring the metal coordination function of metal chelators to chemically stable host materials. Herein, oxamic acid (OxA) and glycine (Gly) functionalized MOF-808 were prepared by a simple solvent-assisted ligand incorporation method and used for uranium removal. The ordered porous structure of MOFs provided rapid diffusion channels, and the introduction of amino acids on Zr6 nodes endowed MOF-808 channels more functional groups with strong binding ability and high hydrophily. The MOF-808@OxA exhibited higher elimination ability (qmax = 370.76 mg·g−1), rapider elimination rate (∼40 min), and higher selectivity than those of MOF-808@Gly and original MOF-808 at pH = 5. Particularly, density functional theory calculations revealed that MOF-808@OxA had a stronger affinity for uranium compared to MOF-808@Gly due to the synergistic effect of C = O and –NH2 groups. Thus, this study provided a feasible strategy for modifying MOFs and a promising prospect for MOF-based materials to eliminate uranium from wastewater.

中文翻译:


通过接枝功能性有机分子开发金属有机框架的节点以进行协同铀提取



高效消解铀是核能发展方面的研究热点。金属螯合剂和多孔材料是从废水中回收和分离铀的两项尖端技术。然而,将金属螯合剂的金属配位功能转移到化学稳定的宿主材料方面取得了有限的成功。在此,通过简单的溶剂辅助配体掺入方法制备了草酸 (OxA) 和甘氨酸 (Gly) 官能化的 MOF-808,并用于铀的去除。MOF 的有序多孔结构提供了快速扩散通道,在 Zr6 节点上引入氨基酸赋予了 MOF-808 通道更多的官能团,具有很强的结合能力和高亲水性。在 pH = 5 时,MOF-808@OxA 表现出比 MOF-808@Gly 和原始 MOF-808 更高的消除能力 (qmax = 370.76 mg·g-1)、更快的消除速率 (∼40 min) 和更高的选择性。特别是,密度泛函理论计算表明,由于 C = O 和 –NH2 基团的协同作用,与 MOF-808@Gly 相比,MOF-808@OxA 对铀具有更强的亲和力。因此,本研究为改性 MOF 提供了一种可行的策略,并为基于 MOF 的材料从废水中去除铀提供了广阔的前景。
更新日期:2024-11-19
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