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用于构建金属有机框架(MOF)的“正交扭曲臂”配体:新拓扑结构与催化活性

"Orthogonal-Twisted-Arm" Ligands for The Construction of Metal-Organic Frameworks (MOFs): New Topology and Catalytic Reactivity.

作者信息

Zhao Kai, He Ying, Shan Chuan, Ren Junyu, Wojtas Lukasz, Wang Li, Li Guanghua, Song Zhiguang, Shi Xiaodong

机构信息

State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, Jilin, 130012, P.R. China.

Department of Chemistry, University of South Florida, Tampa, FL, 33620, USA.

出版信息

Chemistry. 2020 Dec 9;26(69):16272-16276. doi: 10.1002/chem.202003878. Epub 2020 Nov 3.

DOI:10.1002/chem.202003878
PMID:33015904
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10285612/
Abstract

Extended tetratopic benzoic acid ligands with "orthogonal-twisted-arms" conformations were designed and synthesized for the construction of new MOF structures (OTA-MOF). Upon coordination with Cd and Cu cations, two well-defined new MOFs were prepared. X-ray single crystal structures were successfully obtained, demonstrating the formation of a new topology (4,4,4-c). The OTA2-MOF-Cu gave moderate stability in organic solvents and good gas sorption ability toward CO . This new MOF showed superior catalytic reactivity toward the epoxide-CO cycloaddition, giving >50 folds yield enhancement over the controlled reaction without MOF. It is expected that this new ligand design, porous structure, and excellent CO catalytic reactivity will make OTA-MOF promising new materials for applications in catalysis and separation.

摘要

设计并合成了具有“正交扭曲臂”构象的扩展四齿苯甲酸配体,用于构建新型金属有机框架结构(OTA-MOF)。与镉和铜阳离子配位后,制备了两种结构明确的新型MOF。成功获得了X射线单晶结构,证明形成了一种新的拓扑结构(4,4,4-c)。OTA2-MOF-Cu在有机溶剂中具有中等稳定性,对CO具有良好的气体吸附能力。这种新型MOF对环氧化物-CO环加成反应表现出优异的催化活性,与无MOF的对照反应相比,产率提高了50倍以上。预计这种新的配体设计、多孔结构和优异的CO催化活性将使OTA-MOF成为催化和分离应用中有前景的新材料。