Synthesis and Visualization of Entangled 3D Covalent Organic Frameworks with High-Valency Stereoscopic Molecular Nodes for Gas Separation

被引:71
|
作者
Gong, Chengtao [1 ,2 ]
Wang, Hao [1 ,2 ]
Sheng, Guan [1 ,2 ]
Wang, Xiaokang [3 ]
Xu, Xiaoqiu [1 ,2 ]
Wang, Jian [1 ,2 ]
Miao, Xiaohe [4 ]
Liu, Yikuan [1 ,2 ]
Zhang, Yinling [1 ,2 ]
Dai, Fangna [3 ]
Chen, Liangjun [1 ,2 ]
Li, Nanjun [1 ,2 ]
Xu, Guodong [5 ]
Jia, Jianhong [1 ,2 ]
Zhu, Yihan [1 ,2 ]
Peng, Yongwu [1 ,2 ]
机构
[1] Zhejiang Univ Technol, Coll Mat Sci & Engn, Ctr Electron Microscopy, Inst Frontier & Interdisciplinary Sci,State Key L, Hangzhou 310014, Zhejiang, Peoples R China
[2] Zhejiang Univ Technol, Coll Chem Engn, Hangzhou 310014, Zhejiang, Peoples R China
[3] China Univ Petr East China, Sch Mat Sci & Engn, Qingdao 266580, Peoples R China
[4] Westlake Univ, Instrumentat & Serv Ctr Phys Sci, Hangzhou 310024, Zhejiang, Peoples R China
[5] Yancheng Teachers Univ, Jiangsu Prov Engn Res Ctr Agr Breeding Pollut Con, Yancheng 224007, Peoples R China
基金
中国国家自然科学基金;
关键词
covalent organic frameworks; entanglement; high-valency; stereoscopic; gas separation; C2H2/CO2; SEPARATION; CRYSTALLINE; DESIGN; STORAGE; ENERGY; CONSTRUCTION; NANOSHEETS; PLATFORM;
D O I
10.1002/anie.202204899
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The structural diversity of three-dimensional (3D) covalent organic frameworks (COFs) are limited as there are only a few choices of building units with multiple symmetrically distributed connection sites. To date, 4 and 6-connected stereoscopic nodes with T-d, D-3h, D-3d and C-3 symmetries have been mostly reported, delivering limited 3D topologies. We propose an efficient approach to expand the 3D COF repertoire by introducing a high-valency quadrangular prism (D-4h) stereoscopic node with a connectivity of eight, based on which two isoreticular 3D imine-linked COFs can be created. Low-dose electron microscopy allows the direct visualization of their 2-fold interpenetrated bcu networks. These 3D COFs are endowed with unique pore architectures and strong molecular binding sites, and exhibit excellent performance in separating C2H2/CO2 and C2H2/CH4 gas pairs. The introduction of high-valency stereoscopic nodes would lead to an outburst of new topologies for 3D COFs.
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页数:8
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