Zhang Hao, Shao Tianci, Cheng Zeliang, Dong Junchao, Wang Ziyang, Jiang Haicheng, Zhao Xu, Xiaoteng Liu Terence, Zhu Guangshan, Zou Xiaoqin
Faculty of Chemistry, Northeast Normal University, Changchun, 130024, P. R. China.
Department of Mechanical and Construction Engineering, Northumbria University, Newcastle upon Tyne, NE1 8ST, United Kingdom.
Angew Chem Int Ed Engl. 2024 Nov 4;63(45):e202411724. doi: 10.1002/anie.202411724. Epub 2024 Aug 22.
Covalent organic frameworks (COFs), at the forefront of porous materials, hold tremendous potential in membrane separation; however, achieving high continuity in COF membranes remains crucial for efficient gas separation. Here, we present a unique approach termed assembly-dissociation-reconstruction for fabricating COF membranes tailored for CO/N separation. A parent COF is designed from two-node aldehyde and three-node amine monomers and dissociated to high-aspect-ratio nanosheets. Subsequently, COF nanosheets are orderly reconstructed into a crack-free membrane by surface reaction under water evaporation. The membrane exhibits high crystallinity, open pores and a strong affinity for CO adsorption over N, resulting in CO permeance exceeding 1060 GPU and CO/N selectivity surpassing 30.6. The efficacy of this strategy offers valuable guidance for the precise fabrication of gas-separation membranes.
共价有机框架材料（COFs）作为多孔材料的前沿领域，在膜分离方面具有巨大潜力；然而，要实现COF膜的高连续性对于高效气体分离仍然至关重要。在此，我们提出一种独特的方法，称为组装 - 解离 - 重构，用于制备针对CO/N分离量身定制的COF膜。一种母体COF由双节点醛和三节点胺单体设计而成，并解离为高纵横比的纳米片。随后，在水蒸发过程中通过表面反应将COF纳米片有序重构为无裂纹膜。该膜具有高结晶度、开放孔以及对CO的吸附亲和力强于N，导致CO渗透率超过1060 GPU且CO/N选择性超过30.6。这种策略的有效性为气体分离膜的精确制备提供了有价值的指导。
