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用于高效铀萃取的分级多孔偕胺肟化金属有机框架

Hierarchical Porous Amidoximated Metal-Organic Framework for Highly Efficient Uranium Extraction.

作者信息

Li Jin, Tuo Kai, Fan Congbin, Liu Gang, Pu Shouzhi, Li Zhijian

机构信息

Jiangxi Key Laboratory of Organic Chemistry, Jiangxi Science and Technology Normal University, Nanchang, 330013, P. R. China.

YuZhang Normal University, Nanchang, 330013, P. R. China.

出版信息

Small. 2024 Mar;20(13):e2306545. doi: 10.1002/smll.202306545. Epub 2023 Nov 16.

Abstract

With the rapid development of industry and technology, high-efficiency extraction of uranium from seawater is a research hotspot from the aspect of nuclear energy development. Herein, a new amidoximated metal-organic framework (UiO-66-DAMN-AO) constructed through a novel organic ligand of 2-diaminomaleonitrile-terephthalic acid (BDC-DAMN) is designed via one-step post-synthetic methods (PSM), which possess the merit of abundant multiaffinity sites, large specific surface area, and unique porous structure for efficient uranium extraction. Adopting one-step PSM can alleviate the destruction of structural stability and the reduction of the conversion rate of amidoxime groups. Meanwhile, introducing the BDC-DAMN ligand with abundant multiaffinity sites endow UiO-66-DAMN-AO with excellent adsorption ability (Q = 426.3 mg g) and selectivity. Interestingly, the UiO-66-DAMN-AO has both micropores and mesopores, which may be attributed to the partial etching of UiO-66-DAMN-AO during the amidoximation. The presence of mesopores improves the mass transfer rate of UiO-66-DAMN-AO and provides more exposed active sites, favoring the adsorption of uranium on UiO-66-DAMN-AO. Thus, this study provides a feasible strategy for modifying metal-organic framework (MOFs) with plentiful amidoxime groups and the promising prospect for MOF-based materials to adsorb uranium from ocean.

摘要

随着工业和技术的快速发展,从核能开发的角度来看,从海水中高效提取铀是一个研究热点。在此,通过一步后合成方法(PSM)设计了一种新型的偕胺肟化金属有机框架(UiO-66-DAMN-AO),它由2-二氨基马来腈-对苯二甲酸(BDC-DAMN)这种新型有机配体构建而成,具有丰富的多亲和位点、大比表面积和独特的多孔结构,有利于高效提取铀。采用一步后合成方法可以减轻结构稳定性的破坏以及偕胺肟基团转化率的降低。同时,引入具有丰富多亲和位点的BDC-DAMN配体赋予了UiO-66-DAMN-AO优异的吸附能力(Q = 426.3 mg g)和选择性。有趣的是,UiO-66-DAMN-AO同时具有微孔和介孔,这可能归因于在偕胺肟化过程中UiO-66-DAMN-AO的部分蚀刻。介孔的存在提高了UiO-66-DAMN-AO的传质速率,并提供了更多暴露的活性位点,有利于铀在UiO-66-DAMN-AO上的吸附。因此,本研究为用大量偕胺肟基团修饰金属有机框架(MOF)提供了一种可行的策略,以及基于MOF的材料从海洋中吸附铀的广阔前景。

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