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胺链共价有机骨架作为合成后结构转换和孔壁修饰的平台
作者:小柯机器人 发布时间:2021/2/28 16:07:34

德国慕尼黑大学Bettina V. Lotsch团队发现胺链共价有机骨架可以作为合成后结构转换和孔壁修饰的平台。相关研究成果于2021年2月24日发表在国际知名学术期刊《美国化学会杂志》。

共价有机框架已经成为一个具有以原子精度在晶体聚合物主链上安装和相互转换专用的分子功能的强大合成平台。

该文中,研究人员提出了一种新的策略,这是基于Leuckart-Wallach还原甲酸和甲酸铵直接访问作为一个支架的胺连接共价有机框架,使孔壁修饰和链接转换的新合成方法。完全通过仲胺键,混合的胺/亚胺键和部分甲酰化的胺键连接的骨架可在一个步骤中从亚胺连接的骨架中获得,或通过单罐结晶还原法直接从相应的连接体获得。

新的二维胺键共价有机骨架rPI-3-COF、rTTI-COF和rPy1P-COF具有较高的结晶度和较大的比表面积。仲胺作为反应位点安装在孔壁上,使得进一步的合成后功能化能够获得定制的共价有机框架,具有更高的水解稳定性,作为潜在的多相催化剂。

附:英文原文

Title: Amine-Linked Covalent Organic Frameworks as a Platform for Postsynthetic Structure Interconversion and Pore-Wall Modification

Author: Lars Grunenberg, Gkcen Savasci, Maxwell W. Terban, Viola Duppel, Igor Moudrakovski, Martin Etter, Robert E. Dinnebier, Christian Ochsenfeld, Bettina V. Lotsch

Issue&Volume: February 24, 2021

Abstract: Covalent organic frameworks have emerged as a powerful synthetic platform for installing and interconverting dedicated molecular functions on a crystalline polymeric backbone with atomic precision. Here, we present a novel strategy to directly access amine-linked covalent organic frameworks, which serve as a scaffold enabling pore-wall modification and linkage-interconversion by new synthetic methods based on Leuckart–Wallach reduction with formic acid and ammonium formate. Frameworks connected entirely by secondary amine linkages, mixed amine/imine bonds, and partially formylated amine linkages are obtained in a single step from imine-linked frameworks or directly from corresponding linkers in a one-pot crystallization-reduction approach. The new, 2D amine-linked covalent organic frameworks, rPI-3-COF, rTTI-COF, and rPy1P-COF, are obtained with high crystallinity and large surface areas. Secondary amines, installed as reactive sites on the pore wall, enable further postsynthetic functionalization to access tailored covalent organic frameworks, with increased hydrolytic stability, as potential heterogeneous catalysts.

DOI: 10.1021/jacs.0c12249

Source: https://pubs.acs.org/doi/10.1021/jacs.0c12249

 

期刊信息

JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000