Construction of Covalent Organic Frameworks via Three-Component One-Pot Strecker and Povarov Reactions

Construction of Covalent Organic Frameworks via Three-Component One-Pot Strecker and Povarov Reactions
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通过三组分一锅 Strecker 和 Povarov 反应构建共价有机框架

DOI:
10.1021/jacs.0c00969
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发表时间:
2020-04-08
影响因子:
15
通讯作者:
Dong, Yu-Bin
Dong, Yu-Bin
中科院分区:
化学1区
文献类型:
--
作者:
Li, Xue-Tian;Zou, Jie;Dong, Yu-Bin

文献摘要

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合成后修饰(PSM)已被证明是通过在已建立的COF框架上进行单步或多步有机官能团转化来获得新的共价有机框架(COF)的有力方法。然而,PSM,有时可能会导致崩溃的COF框架,结晶度下降,或低合成后的产量由于固态合成的固有限制。在这里,我们报告,第一次,一种新的合成策略,可以通过多组分一锅原位反应生成新的COFs。在溶剂热条件下,通过三组分一锅法原位Strecker和Povarov反应,以高产率成功地获得了12个具有高结晶度和永久孔隙率的α-氨基腈和喹啉连接的COF。所获得的COF具有与在已建立的亚胺连接的COF上从逐步PSM方法获得的那些相同的结构。这种原位多组分组装策略,作为一种与PSM平行的合成方法,可能为构建COFs开辟一条新的途径,这在PSM条件下是不可能的。
Postsynthetic modification (PSM) has been demonstrated to be a powerful method for achieving new covalent organic frameworks (COFs) via single-step or multistep organic functional group transformations on established COF frameworks. PSM, however, might sometimes lead to collapse of the COF framework, decreases in crystallinity, or low postsynthetic yield due to the inherent limit of solid-state synthesis. Herein we report, for the first time, a new synthetic strategy that can generate new COFs via multicomponent one-pot in situ reactions. In total, 12 alpha-aminonitrile- and quinoline-linked COFs with high crystallinity and permanent porosity are successfully achieved by three-component one-pot in situ Strecker and Povarov reactions under solvothermal conditions in high yields. The obtained COFs feature the same structures as those obtained from the stepwise PSM approach on an established imine-linked COF. This in situ multicomponent assembly strategy, as a synthetic methodology parallel to PSM, might open a new route for constructing COFs that is not possible under PSM conditions.