Zhao Yingji, Gao Zhi, Chen Norman C-R, Asakura Yusuke, Nam Ho Ngoc, Phung Quan Manh, Kang Yunqing, Leung Mandy Hei Man, Jiang Dong, Fu Lei, Huang Lijin, Asahi Toru, Yamauchi Yusuke
Department of Materials Process Engineering, Graduate School of Engineering, Nagoya University, Nagoya, 464-8603, Japan.
Faculty of Science and Engineering, Waseda University, 3-4-1 Okubo, Shinjuku, Tokyo, 169-8555, Japan.
Adv Mater. 2025 Sep;37(36):e2508105. doi: 10.1002/adma.202508105. Epub 2025 Jun 16.
Designing 2D mesoporous metal-organic framework (MOF) nanosheets to overcome the limitations of bulk MOF counterparts, with a focus on enabling smooth mass transport, presents an attractive yet challenging endeavor. Here, a novel bottom-up interface-directed co-assembly method is presented for the synthesis of ultrathin 2D mesoporous UiO-66(Ce) nanosheets. The method utilizes an interface-directed co-assembly of amphiphilic perfluorooctanoic acid-induced lipid bilayers and spherical micelles from PS-b-PEO block copolymers to form unique 2D sandwich-like assemblies that guide the creation of 2D mesoporous UiO-66(Ce). The resultant 2D mesoporous UiO-66(Ce), with ≈23 nm pore diameters and a thickness that can be tuned from 3 to 150 nm, represents a substantial advancement in the application of MOFs for environmental remediation. As a model reaction, the U(VI) photoreduction benefits from the through-mesopores of its 2D morphology, which are absent in previously reported UiO-66(Ce), as they shorten the diffusion path, thereby improving mass transport and accessibility to active sites. This report demonstrates the significant role of existing mesopores in MOFs and the shape control of MOFs.
设计二维介孔金属有机框架(MOF)纳米片以克服块状MOF的局限性,重点是实现顺畅的质量传输,这是一项具有吸引力但具有挑战性的工作。在此,提出了一种新颖的自下而上的界面导向共组装方法来合成超薄二维介孔UiO-66(Ce)纳米片。该方法利用两亲性全氟辛酸诱导的脂质双层与PS-b-PEO嵌段共聚物形成的球形胶束的界面导向共组装,形成独特的二维三明治状组装体,从而引导二维介孔UiO-66(Ce)的形成。所得的二维介孔UiO-66(Ce),孔径约为23nm,厚度可在3至150nm之间调节,代表了MOF在环境修复应用中的重大进展。作为模型反应,U(VI)光还原受益于其二维形态的贯通介孔,而先前报道的UiO-66(Ce)中不存在这种介孔,因为它们缩短了扩散路径,从而改善了质量传输和对活性位点的可及性。本报告证明了现有介孔在MOF中的重要作用以及MOF的形状控制。