Topology-Templated Synthesis of Crystalline Porous Covalent Organic Frameworks

Enquan Jin; Keyu Geng; Ka Hung Lee; Weiming Jiang; Juan Li; Qiuhong Jiang; Stephan Irle; Donglin Jiang

doi:10.1002/anie.202004728

Topology-Templated Synthesis of Crystalline Porous Covalent Organic Frameworks

Enquan Jin, Keyu Geng, Ka Hung Lee, Weiming Jiang, Juan Li, Qiuhong Jiang, Stephan Irle, Donglin Jiang

Computational Chemistry and Nanomaterial

Research output: Contribution to journal › Article › peer-review

81 Scopus citations

Abstract

A strategy is presented for the synthesis of crystalline porous covalent organic frameworks via topology-templated polymerization. The template is based on imine-linked frameworks and their (001) facets seed the C=C bond formation reaction to constitute 2D sp² carbon-conjugated frameworks. This strategy is applicable to templates with different topologies, enables designed synthesis of frameworks that cannot be prepared via direct polymerization, and creates a series of sp² carbon frameworks with tetragonal, hexagonal, and kagome topologies. The sp² carbon frameworks are highly luminescent even in the solid state and exhibit topology-dependent π transmission and exciton migration; these key fundamental π functions are unique to sp² carbon-conjugated frameworks and cannot be accessible by imine-linked frameworks, amorphous analogues, and 1D conjugated polymers. These results demonstrate an unprecedented strategy for structural and functional designs of covalent organic frameworks.

Original language	English
Pages (from-to)	12162-12169
Number of pages	8
Journal	Angewandte Chemie - International Edition
Volume	59
Issue number	29
DOIs	https://doi.org/10.1002/anie.202004728
State	Published - Jul 13 2020

Funding

K.H.L. was supported by an Energy Science and Engineering Fellowship by the Bredesen Centre for Interdisciplinary Research and Graduate Education at the University of Tennessee, Knoxville. S.I. acknowledges support by the Laboratory Directed Research and Development (LDRD) Program of Oak Ridge National Laboratory. ORNL is managed by UT‐Battelle, LLC, for DOE under contract DE‐AC05‐00OR22725. D.J. acknowledges supports by MOE tier 1 grant (R‐143‐000‐A71‐114) and NUS start‐up grant (R‐143‐000‐A28‐133).

Funders	Funder number
Bredesen Centre for Interdisciplinary Research and Graduate Education at the University of Tennessee
U.S. Department of Energy	DE‐AC05‐00OR22725
Oak Ridge National Laboratory
Laboratory Directed Research and Development
National University of Singapore	R‐143‐000‐A28‐133
Ministry of Education - Singapore	R‐143‐000‐A71‐114

Keywords

covalent organic frameworks
exciton migration
luminescence
topology template
π transmission

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10.1002/anie.202004728

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title = "Topology-Templated Synthesis of Crystalline Porous Covalent Organic Frameworks",

abstract = "A strategy is presented for the synthesis of crystalline porous covalent organic frameworks via topology-templated polymerization. The template is based on imine-linked frameworks and their (001) facets seed the C=C bond formation reaction to constitute 2D sp2 carbon-conjugated frameworks. This strategy is applicable to templates with different topologies, enables designed synthesis of frameworks that cannot be prepared via direct polymerization, and creates a series of sp2 carbon frameworks with tetragonal, hexagonal, and kagome topologies. The sp2 carbon frameworks are highly luminescent even in the solid state and exhibit topology-dependent π transmission and exciton migration; these key fundamental π functions are unique to sp2 carbon-conjugated frameworks and cannot be accessible by imine-linked frameworks, amorphous analogues, and 1D conjugated polymers. These results demonstrate an unprecedented strategy for structural and functional designs of covalent organic frameworks.",

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AU - Lee, Ka Hung

AU - Jiang, Weiming

AU - Li, Juan

AU - Jiang, Qiuhong

AU - Irle, Stephan

AU - Jiang, Donglin

PY - 2020/7/13

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N2 - A strategy is presented for the synthesis of crystalline porous covalent organic frameworks via topology-templated polymerization. The template is based on imine-linked frameworks and their (001) facets seed the C=C bond formation reaction to constitute 2D sp2 carbon-conjugated frameworks. This strategy is applicable to templates with different topologies, enables designed synthesis of frameworks that cannot be prepared via direct polymerization, and creates a series of sp2 carbon frameworks with tetragonal, hexagonal, and kagome topologies. The sp2 carbon frameworks are highly luminescent even in the solid state and exhibit topology-dependent π transmission and exciton migration; these key fundamental π functions are unique to sp2 carbon-conjugated frameworks and cannot be accessible by imine-linked frameworks, amorphous analogues, and 1D conjugated polymers. These results demonstrate an unprecedented strategy for structural and functional designs of covalent organic frameworks.

AB - A strategy is presented for the synthesis of crystalline porous covalent organic frameworks via topology-templated polymerization. The template is based on imine-linked frameworks and their (001) facets seed the C=C bond formation reaction to constitute 2D sp2 carbon-conjugated frameworks. This strategy is applicable to templates with different topologies, enables designed synthesis of frameworks that cannot be prepared via direct polymerization, and creates a series of sp2 carbon frameworks with tetragonal, hexagonal, and kagome topologies. The sp2 carbon frameworks are highly luminescent even in the solid state and exhibit topology-dependent π transmission and exciton migration; these key fundamental π functions are unique to sp2 carbon-conjugated frameworks and cannot be accessible by imine-linked frameworks, amorphous analogues, and 1D conjugated polymers. These results demonstrate an unprecedented strategy for structural and functional designs of covalent organic frameworks.

KW - covalent organic frameworks

KW - exciton migration

KW - luminescence

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Topology-Templated Synthesis of Crystalline Porous Covalent Organic Frameworks

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