Department of Chemical and Biomolecular Engineering, Center for Catalytic Science and Technology, University of Delaware, Newark, DE 19716 (USA).
Angew Chem Int Ed Engl. 2014 Mar 10;53(11):2878-82. doi: 10.1002/anie.201310500. Epub 2014 Feb 7.
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.
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。