Converging Cooperative Functions into the Nanospace of Covalent Organic Frameworks for Efficient Uranium Extraction from Seawater
Converging Cooperative Functions into the Nanospace of Covalent Organic Frameworks for Efficient Uranium Extraction from Seawater
复制标题
将协同功能融合到共价有机框架的纳米空间中，以从海水中高效提取铀
DOI：
10.31635/ccschem.022.202201897
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发表时间：
2022-07-01
期刊：
影响因子：
11.2
通讯作者：
Ma, Shengqian
中科院分区：
文献类型：
--
作者：
Hao, Mengjie;Chen, Zhongshan;Ma, Shengqian
从海水中提取铀具有挑战性，尽管它为能源部门可持续生产核燃料提供了巨大的潜力。在此，我们报道了一种新的策略，通过将吸附-光催化的协同功能聚合到共价有机框架（COFs）的纳米空间中，从海水中高效提取铀。多组分COFs中有机连接体的功能化可以探索材料组成与铀萃取吸附光催化活性之间的关系。COFs中偕胺肟基的存在为铀酰提供了选择性的结合位点，而三嗪基和联吡啶- pd基协同作用，光催化将吸附的U（VI）还原为U（IV）固体产物（UO2），便于收集。我们开发的COFs之一，4-Pd-AO，在天然海水中表现出优异的隔离和还原铀酰的性能，在可见光照射下，其提取能力高达4.62 mg U/g /天（平均数据）。机理研究表明，4-Pd-AO不仅能将吸附的铀酰（VI）还原为U(IV)O-2，还能在可见光激发下生成O-1(2)和超氧自由基，从而具有良好的抗菌和抗藻活性（即抗生物污染性能），从而保持高效的铀萃取性能。这项概念验证研究确立了多组分COFs作为从海水中高效提取铀的有希望的候选物。
The extraction of uranium from seawater is challenging though it offers tremendous potential for the sustainable production of nuclear fuel for the energy sector. Herein, we report a new strategy for efficient extraction of uranium from seawater via converging the cooperative functions of adsorption- photocatalysis into the nanospace of covalent organic frameworks (COFs). Functionalization of the organic linkers in the multicomponent COFs allowed exploration of the relationship between material composition and adsorption-photocatalytic activity for uranium extraction. The presence of amidoxime groups in the COFs offered selective binding sites for uranyl, whilst triazine units and bipyridine-Pd groups acted cooperatively to photo-catalytically reduce adsorbed U(VI) to a U(IV) solid product (UO2) for facile collection. One of our developed COFs, 4-Pd-AO, displayed exceptional performance in sequestering and reducing uranyl from natural seawater, with a high extraction capacity of 4.62 mg U/g per day (average data) under visible light irradiation. Mechanistic studies revealed that 4-Pd-AO not only reduced adsorbed uranyl(VI) to U(IV)O-2, but also generated O-1(2) and superoxide radicals under visible light excitation, thus affording excellent antibacterial and antialgal activities (i.e., anti-biofouling properties) for sustained efficient uranium extraction performance. This pro-of-ofconcept study establishes multicomponent COFs as promising candidates for efficient uranium extraction from seawater.[GRAPHICS].