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Topology-Selective Manipulation of Two-Dimensional Covalent Organic Frameworks

Xinyu Wang, Minghui Liu, Youxing Liu, Youxing Liu, Shengcong Shang, Changsheng Du, Jiaxin Hong, Wenqiang Gao, Chunyu Hua, Helin Xu, Zewen You, Jianyi Chen, Yunqi Liu, Yunqi Liu

2023Journal of the American Chemical Society72 citationsDOI

Abstract

The manipulation of topological architectures in two-dimensional (2D) covalent organic framework (COF) materials for different applications is promising but remains a great challenge. Here, we first report the topology-selective synthesis of two distinct varieties of 2DCOFs, imine-based HT-COFs and benzimidazole-fused BI-HT-COFs, by simply altering acid catalysts. To HT-COFs, a superlattice of 1D channel with a persistent triangular shape is formed via Schiff base reaction, while to BI-HT-COFs, a hexagonal lattice structure with a highly conjugated structure and imidazole linkages is constructed due to an imine-based cyclization reaction. The two COFs exhibited marked differences in their bandgap, chemical stability, molecular adsorption, and catalytic activity, which make them have different fields of application. This work not only diversifies the hexaaminotriphenylene-based 2DCOF topologies but also provides vivid examples of structure-property relationships, which would facilitate fundamental research and potential applications of 2DCOFs.

Topics & Concepts

ChemistryImineCovalent bondTopology (electrical circuits)ImidazoleConjugated systemCombinatorial chemistryCatalysisBenzimidazoleNanotechnologyStereochemistryOrganic chemistryMaterials sciencePolymerCombinatoricsMathematicsCovalent Organic Framework ApplicationsMetal-Organic Frameworks: Synthesis and ApplicationsLuminescence and Fluorescent Materials