Assembly-Dissociation-Reconstruction Synthesis of Covalent Organic Framework Membranes with High Continuity for Efficient CO2 Separation

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Hao Zhang, Tianci Shao, Zeliang Cheng, Junchao Dong, Ziyang Wang, Haicheng Jiang, Xu Zhao, Dr. Terence Xiaoteng Liu, Prof. Dr. Guangshan Zhu, Prof. Dr. Xiaoqin Zou
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Abstract

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 CO2/N2 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 CO2 adsorption over N2, resulting in CO2 permeance exceeding 1060 GPU and CO2/N2 selectivity surpassing 30.6. The efficacy of this strategy offers valuable guidance for the precise fabrication of gas-separation membranes.

组装-解离-重构高连续性共价有机框架膜的合成,用于高效分离二氧化碳。
共价有机框架(COFs)是多孔材料中的佼佼者,在膜分离领域具有巨大潜力;然而,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,我们提出了一种称为 "组装-解离-重构 "的独特方法,用于制造专门用于 CO2/N2 分离的 COF 膜。母 COF 由双节醛和三节胺单体设计而成,并解离成高宽比纳米片。随后,COF 纳米片在水蒸发条件下通过表面反应有序地重构成无裂缝膜。这种膜具有高结晶度、开放式孔隙以及对二氧化碳的吸附力强于对 N2 的吸附力,因此二氧化碳渗透率超过 1060 GPU,二氧化碳/N2 选择性超过 30.6。这一策略的有效性为精确制造气体分离膜提供了宝贵的指导。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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