Liu Tianqi, Li Zhan, Zhang Xin, Tan Hongxin, Chen Ziying, Wu Jinsheng, Chen Jia, Qiu Hongdeng
CAS Key Laboratory of Chemistry of Northwestern Plant Resources and Key Laboratory for Natural Medicine of Gansu Province, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China.
School of Nuclear Science and Technology, Lanzhou University, Lanzhou 730000, China.
Anal Chem. 2021 Dec 7;93(48):16175-16183. doi: 10.1021/acs.analchem.1c03982. Epub 2021 Nov 22.
Design and construction of a membrane that can achieve selective separation of uranium from spent fuel or seawater is a big challenge in the field of separation science. In this work, 1,3,5-benzenetricarboxylic acid (BTC) and three different nitrates (Zn/Ni/Cu) were used to prepare metal-organic frameworks (BTC-MOFs) with different pore sizes, and then, BTC-MOFs were intercalated into the interlayers of graphene oxide (GO) for preparing the composite membranes which presented selective separation of uranium with strong acid resistance. Composite membranes prepared by Zn/Ni/Cu-BTC-MOFs and GO can achieve the separation between ions of different valence states, and their permeability and selectivity depend on the membrane thickness, the acidity of driving solution, and the pore sizes of MOFs. Importantly, Cu-BTC-MOF-intercalated GO membranes can not only achieve the selective separation of Th and UO with a selectivity of ≈6 but also induce the ultra-high selectively separation of UO and Ce because the rejection rate of Ce is about 100%. Moreover, the Zn-BTC-MOF-intercalated GO membrane shows an excellent selectivity of Th and UO with a selectivity of ≈25, and it may also achieve selective separation of uranium from seawater.
设计并构建一种能够从乏燃料或海水中实现铀选择性分离的膜,是分离科学领域的一项重大挑战。在本工作中,采用1,3,5-苯三甲酸(BTC)和三种不同的硝酸盐(锌/镍/铜)制备了具有不同孔径的金属有机框架材料(BTC-MOFs),然后将BTC-MOFs插层到氧化石墨烯(GO)的层间,以制备出具有强酸抗性且能实现铀选择性分离的复合膜。由锌/镍/铜-BTC-MOFs和GO制备的复合膜能够实现不同价态离子之间的分离,其渗透性和选择性取决于膜的厚度、驱动溶液的酸度以及MOFs的孔径。重要的是,插层有Cu-BTC-MOF的GO膜不仅能够以约6的选择性实现钍和铀酰的选择性分离,还能诱导铀酰和铈的超高选择性分离,因为铈的截留率约为100%。此外,插层有Zn-BTC-MOF的GO膜对钍和铀酰表现出约25的优异选择性,并且它也可能实现从海水中选择性分离铀。