State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228, P. R. China.
Angew Chem Int Ed Engl. 2020 Mar 9;59(11):4262-4268. doi: 10.1002/anie.201916450. Epub 2020 Jan 29.
Biology has evolved excellent spatial structures for high-selectivity and high-affinity capture of heavy metals. Inspired by the spatial structure of the superb-uranyl binding protein SUP, we mimic the spatial structure of SUP in metal-organic frameworks (MOFs). The MOF UiO-66-3C4N fabricated by introducing 4-aminoisophthalic acid into UiO-66 shows high uranyl adsorption capacity both in simulated seawater and in natural seawater. In natural seawater, UiO-66-3C4N exhibits 17.03 times higher uranium extraction capacity than that of vanadium, indicating the high selectivity of the adsorbent. The EXAFS analysis and DFT calculation reveal that UiO-66-3C4N forms smaller nano-pocket for uranyl capture than that of SUP protein, which can both restrict the entrance of the other interfering ions with larger size and reinforce the binding by increasing the coordination interaction, and therefore qualify the nano-pocket with high affinity and high selectivity to uranyl.
生物学已经进化出了出色的空间结构，用于高选择性和高亲和力地捕获重金属。受超铀结合蛋白 SUP 的空间结构的启发，我们在金属有机骨架（MOFs）中模拟了 SUP 的空间结构。通过将 4-氨基间苯二甲酸引入 UiO-66 制备的 MOF UiO-66-3C4N 在模拟海水中和天然海水中均表现出高的铀吸附容量。在天然海水中，UiO-66-3C4N 的铀提取能力比钒高 17.03 倍，表明该吸附剂具有高选择性。EXAFS 分析和 DFT 计算表明，UiO-66-3C4N 形成的用于捕获铀酰的纳米口袋比 SUP 蛋白小，这既能限制较大尺寸的其他干扰离子的进入，又能通过增加配位相互作用来增强结合，从而使纳米口袋具有高亲和力和高选择性。
