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Construction of Flexible Amine‐linked Covalent Organic Frameworks by Catalysis and Reduction of Formic Acid via the Eschweiler–Clarke Reaction
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-03-07 , DOI: 10.1002/anie.202102373 Meicheng Zhang 1 , Yang Li 2 , Wenli Yuan 1 , Xinghua Guo 1 , Chiyao Bai 1 , Yingdi Zuo 1 , Honghan Long 1 , Yue Qi 1 , Shoujian Li 1 , Guohong Tao 1 , Chuanqin Xia 1 , Lijian Ma 3
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-03-07 , DOI: 10.1002/anie.202102373 Meicheng Zhang 1 , Yang Li 2 , Wenli Yuan 1 , Xinghua Guo 1 , Chiyao Bai 1 , Yingdi Zuo 1 , Honghan Long 1 , Yue Qi 1 , Shoujian Li 1 , Guohong Tao 1 , Chuanqin Xia 1 , Lijian Ma 3
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Compared to the current mainstream rigid covalent organic frameworks (COFs) linked by imine bonds, flexible COFs have certain advantages of elasticity and self‐adaptability, but their construction and application are greatly limited by the complexity in synthesis and difficulty in obtaining regular structure. Herein, we reported for the first time a series of flexible amine‐linked COFs with high crystallinity synthesized by formic acid with unique catalytic and reductive bifunctional properties, rather than acetic acid, the most common catalyst for COF synthesis. The reaction mechanism was demonstrated to be a synchronous in situ reduction during the formation of imine bond. The flexibilities of the products endow them with accommodative adaptability to guest molecules, thus increasing the adsorption capacities for nitrogen and iodine by 27 % and 22 %, respectively. Impressively, a novel concept of flexibilization degree was proposed firstly, which provides an effective approach to rationally measure the flexibility of COFs.
中文翻译：
通过Eschweiler-Clarke反应催化和还原甲酸，构建柔性胺连接的共价有机骨架
与目前主流的亚胺键连接的刚性共价有机骨架相比，柔性COF具有一定的弹性和自适应性，但其合成和应用受到合成的复杂性和难以获得规则结构的限制。在本文中，我们首次报道了一系列具有高结晶度的柔性胺连接的COF，它们是由具有独特的催化和还原双功能性质的甲酸而不是乙酸（COF合成中最常用的催化剂）合成的。反应机理被证明是亚胺键形成过程中的同步原位还原。产品的灵活性赋予了它们对客体分子的适应性适应能力，因此，氮和碘的吸附量分别增加了27％和22％。令人印象深刻的是，首先提出了一种新的柔性度概念，它为合理地测量COF的柔性提供了一种有效的方法。
更新日期：2021-03-07
中文翻译：
通过Eschweiler-Clarke反应催化和还原甲酸，构建柔性胺连接的共价有机骨架
与目前主流的亚胺键连接的刚性共价有机骨架相比，柔性COF具有一定的弹性和自适应性，但其合成和应用受到合成的复杂性和难以获得规则结构的限制。在本文中，我们首次报道了一系列具有高结晶度的柔性胺连接的COF，它们是由具有独特的催化和还原双功能性质的甲酸而不是乙酸（COF合成中最常用的催化剂）合成的。反应机理被证明是亚胺键形成过程中的同步原位还原。产品的灵活性赋予了它们对客体分子的适应性适应能力，因此，氮和碘的吸附量分别增加了27％和22％。令人印象深刻的是，首先提出了一种新的柔性度概念，它为合理地测量COF的柔性提供了一种有效的方法。
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