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3D 微孔基底功能化共价有机框架用于尺寸选择性催化。

3D microporous base-functionalized covalent organic frameworks for size-selective catalysis.

机构信息

Department of Chemical and Biomolecular Engineering, Center for Catalytic Science and Technology, University of Delaware, Newark, DE 19716 (USA).

出版信息

Angew Chem Int Ed Engl. 2014 Mar 10;53(11):2878-82. doi: 10.1002/anie.201310500. Epub 2014 Feb 7.

Abstract

The design and synthesis of 3D covalent organic frameworks (COFs) have been considered a challenge, and the demonstrated applications of 3D COFs have so far been limited to gas adsorption. Herein we describe the design and synthesis of two new 3D microporous base-functionalized COFs, termed BF-COF-1 and BF-COF-2, by the use of a tetrahedral alkyl amine, 1,3,5,7-tetraaminoadamantane (TAA), combined with 1,3,5-triformylbenzene (TFB) or triformylphloroglucinol (TFP). As catalysts, both BF-COFs showed remarkable conversion (96% for BF-COF-1 and 98% for BF-COF-2), high size selectivity, and good recyclability in base-catalyzed Knoevenagel condensation reactions. This study suggests that porous functionalized 3D COFs could be a promising new class of shape-selective catalysts.

摘要

三维共价有机框架(COFs)的设计和合成一直被认为是一个挑战,到目前为止,三维 COFs 的应用仅限于气体吸附。在此,我们通过使用四面体烷基胺 1,3,5,7-四氨基金刚烷(TAA)与 1,3,5-三醛基苯(TFB)或三醛基间苯三酚(TFP),设计并合成了两种新的三维微孔基底功能化 COFs,分别称为 BF-COF-1 和 BF-COF-2。作为催化剂,BF-COFs 均表现出优异的转化率(BF-COF-1 为 96%,BF-COF-2 为 98%)、高尺寸选择性和良好的在碱性条件下的 Knoevenagel 缩合反应中的可回收性。本研究表明,多孔功能化的三维 COFs 可能是一类很有前途的新型形状选择性催化剂。

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