Wang Pengyuan, Peng Yuan, Zhu Chenyu, Yao Rui, Song Hongling, Kun Lun, Yang Weishen
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China.
Dalian National Laboratory for Clean Energy, Dalian, 116023, China.
Angew Chem Int Ed Engl. 2021 Aug 23;60(35):19047-19052. doi: 10.1002/anie.202106346. Epub 2021 Jul 20.
Two-dimensional covalent organic frameworks (2D COFs) are considered as potential candidates for gas separation membranes, benefiting from permanent porosity, light-weight skeletons, excellent stability and facilely-tailored functionalities. However, their pore sizes are generally larger than the kinetic diameters of common gas molecules. One great challenge is the fabrication of single-phase COF membranes to realize precise gas separations. Herein, three kinds of high-quality β-ketoenamine-type COF nanosheets with different pore sizes were developed and aggregated to ultrathin nanosheet membranes with distinctive staggered stacking patterns. The narrowed pore sizes derived from the micro-structures and selective adsorption capacities synergistically endowed the COF membranes with intriguing CO -philic separation performances, among which TpPa-2 with medium pore size exhibited an optimal CO /H separation factor of 22 and a CO permeance of 328 gas permeation units at 298 K. This membrane performance reached the target with commercial feasibility for syngas separations.
二维共价有机框架(2D COF)因其具有永久孔隙率、轻质骨架、出色的稳定性和易于定制的功能,被视为气体分离膜的潜在候选材料。然而,它们的孔径通常大于常见气体分子的动力学直径。一个巨大的挑战是制备单相COF膜以实现精确的气体分离。在此,开发了三种具有不同孔径的高质量β-酮胺型COF纳米片,并将其聚集成具有独特交错堆叠模式的超薄纳米片膜。微观结构导致的孔径缩小和选择性吸附能力协同赋予了COF膜有趣的亲CO分离性能,其中中等孔径的TpPa-2在298 K时表现出最佳的CO/H分离因子22和328气体渗透单位的CO渗透率。这种膜性能达到了合成气分离商业可行性的目标。