Reticulating 1D Ribbons into 2D Covalent Organic Frameworks by Imine and Imide Linkages

Reticulating 1D Ribbons into 2D Covalent Organic Frameworks by Imine and Imide Linkages
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DOI:
10.1021/jacs.9b13971
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发表时间:
2020-02-12
影响因子:
15
通讯作者:
Yaghi, Omar M.
Yaghi, Omar M.
中科院分区:
化学1区
文献类型:
--
作者:
Nguyen, Ha L.;Gropp, Cornelius;Yaghi, Omar M.

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从大分子甚至无限的结构单元设计和合成 2D 和 3D 晶体共价有机框架 (COF) 在很大程度上尚未开发。在这里,我们报告了一种将分子和一维带连接成二维晶体框架的策略。三角形的三(4-氨基苯基)胺(TAA)和方形的1,3,6,8-四(对甲酰基苯基)芘(TFPPy)有机结构单元通过亚化学计量通过亚胺键连接起来,产生一维带,称为COF-76,带有游离胺,然后用于将带连接成二维框架COF-77和COF-78。除了这种逐步方法之外,我们还演示了这些 COF 的原位合成。我们相信,我们能够将无限的构建模块(例如 COF-76 的带)连接成更高维度的 COF,为由分层化学结构组成的共价框架铺平了道路。
The design and synthesis of 2D and 3D crystalline covalent organic frameworks (COFs) from macromolecular and even infinite building units is largely undeveloped. Here, we report a strategy to link molecules and 1D ribbons into 2D cystalline frameworks. Triangular, tris(4-aminophenyl)amine (TAA), and square, 1,3,6,8-tetrakis(p-formylphenyl)pyrene (TFPPy), organic building units are joined substoichiometrically by imine linkages to produce 1D ribbons, termed COF-76, bearing free amines, which are then used to link the ribbons into 2D frameworks COF-77 and COF-78. In addition to this stepwise approach, we also demonstrate an in situ synthesis of these COFs. We believe our ability to link infinite building blocks, such as the ribbons of COF-76, into higher dimensionality COFs, paves the way to covalent frameworks composed of hierachical chemical structures.