2D Covalent Organic Frameworks with cem Topology

2D Covalent Organic Frameworks with cem Topology
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具有 cem 拓扑的二维共价有机框架

DOI:
10.1021/jacs.2c01082
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发表时间:
2022
影响因子:
15
通讯作者:
Yong Cui
Yong Cui
中科院分区:
化学1区
文献类型:
--
作者:
Xuan Wang;Xing Han;Cheng Cheng;Xing Kang;Yan Liu;Yong Cui

文献摘要

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大量具有二维层状结构的共价有机骨架(COF)已被报道,但由于构建单元的选择有限,它们的网络结构仅限于七种拓扑结构(即hcb,hxl,kgm,sql,tth,bex,andkgd)。在这项工作中,我们说明了如何连接伪五重对称的1,2,3,4,5-五(4-甲酰基苯基)吡咯与线性芳香族二胺通过动态亚胺键产生三个二维多孔COFs与一个前所未有的cem拓扑结构,这是第一个五顶点半正则阿基米德镶嵌在COFs的例子。3种二维COF均为同构结构,均采用重叠堆叠结构,单向分层孔道,其中吡咯单元作为网络的五个顶点,形成33.42排列的正方形和三角形孔道. COF填充的高效液相色谱柱具有很高的耐热性和耐化学性,表现出优异的性能,可分离10种不同的多环芳烃,这是一组最广泛的有机环境污染物。因此,五顶点阿基米德镶嵌的实施快递的策略,以设计具有新的拓扑结构的COF和铺平了一条新的途径,以扩大COF材料的独特性能。
A large number of covalent organic frameworks (COFs) with two-dimensional (2D) layered structures have been reported, but their network structures are restricted to only seven topologies (namely,hcb,hxl,kgm,sql,tth,bex, andkgd) because of the limited choice of building blocks. In this work, we illustrate how linking pseudo-fivefold symmetric 1,2,3,4,5-penta(4-formylphenyl)pyrrole with linear aromatic diamines through dynamic imine bonds produces three 2D porous COFs with an unprecedentedcemtopology, which represent the first examples of five-vertex semiregular Archimedean tessellations in COFs. The three 2D COFs are isostructural, and each adopts an eclipsed stacking structure with unidirectional hierarchical pores, in which the pyrrole unit is utilized as the five-vertex of network to form both square and triangular pores in a 33.42sequence. With high thermal and chemical resistances, the COF-packed HPLC columns show excellent performance to provide separation of 10 different polycyclic aromatic hydrocarbons, a group of the most widespread organic environmental pollutants. The implementation of five-vertex Archimedean tessellations thus couriers a strategy to design COFs with new topologies and paves a new way to expand the inimitable properties of COF materials.