Saturated Linkers in Two-Dimensional Covalent Organic Frameworks Boost Their Luminescence
The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly observed photoluminescence quenching of COFs, we propose a strategy involving interrupting the intralayer conjugation and interlayer interaction...
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| Published in | Journal of the American Chemical Society Vol. 145; no. 26; pp. 14417 - 14426 |
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| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
05.07.2023
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| Abstract | The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly observed photoluminescence quenching of COFs, we propose a strategy involving interrupting the intralayer conjugation and interlayer interactions using cyclohexane as the linker unit. By variation of the building block structures, imine-bonded COFs with various topologies and porosities are obtained. Experimental and theoretical analyses of these COFs disclose high crystallinity and large interlayer distances, demonstrating enhanced emission with record-high photoluminescence quantum yields of up to 57% in the solid state. The resulting cyclohexane-linked COF also exhibits excellent sensing performance for the trace recognition of Fe3+ ions, explosive and toxic picric acid, and phenyl glyoxylic acid as metabolites. These findings inspire a facile and general strategy to develop highly emissive imine-bonded COFs for detecting various molecules. |
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| AbstractList | The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly observed photoluminescence quenching of COFs, we propose a strategy involving interrupting the intralayer conjugation and interlayer interactions using cyclohexane as the linker unit. By variation of the building block structures, imine-bonded COFs with various topologies and porosities are obtained. Experimental and theoretical analyses of these COFs disclose high crystallinity and large interlayer distances, demonstrating enhanced emission with record-high photoluminescence quantum yields of up to 57% in the solid state. The resulting cyclohexane-linked COF also exhibits excellent sensing performance for the trace recognition of Fe
ions, explosive and toxic picric acid, and phenyl glyoxylic acid as metabolites. These findings inspire a facile and general strategy to develop highly emissive imine-bonded COFs for detecting various molecules. The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly observed photoluminescence quenching of COFs, we propose a strategy involving interrupting the intralayer conjugation and interlayer interactions using cyclohexane as the linker unit. By variation of the building block structures, imine-bonded COFs with various topologies and porosities are obtained. Experimental and theoretical analyses of these COFs disclose high crystallinity and large interlayer distances, demonstrating enhanced emission with record-high photoluminescence quantum yields of up to 57% in the solid state. The resulting cyclohexane-linked COF also exhibits excellent sensing performance for the trace recognition of Fe 3+ ions, explosive and toxic picric acid, and phenyl glyoxylic acid as metabolites. These findings inspire a facile and general strategy to develop highly emissive imine-bonded COFs for detecting various molecules. The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly observed photoluminescence quenching of COFs, we propose a strategy involving interrupting the intralayer conjugation and interlayer interactions using cyclohexane as the linker unit. By variation of the building block structures, imine-bonded COFs with various topologies and porosities are obtained. Experimental and theoretical analyses of these COFs disclose high crystallinity and large interlayer distances, demonstrating enhanced emission with record-high photoluminescence quantum yields of up to 57% in the solid state. The resulting cyclohexane-linked COF also exhibits excellent sensing performance for the trace recognition of Fe3+ ions, explosive and toxic picric acid, and phenyl glyoxylic acid as metabolites. These findings inspire a facile and general strategy to develop highly emissive imine-bonded COFs for detecting various molecules. The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly observed photoluminescence quenching of COFs, we propose a strategy involving interrupting the intralayer conjugation and interlayer interactions using cyclohexane as the linker unit. By variation of the building block structures, imine-bonded COFs with various topologies and porosities are obtained. Experimental and theoretical analyses of these COFs disclose high crystallinity and large interlayer distances, demonstrating enhanced emission with record-high photoluminescence quantum yields of up to 57% in the solid state. The resulting cyclohexane-linked COF also exhibits excellent sensing performance for the trace recognition of Fe³⁺ ions, explosive and toxic picric acid, and phenyl glyoxylic acid as metabolites. These findings inspire a facile and general strategy to develop highly emissive imine-bonded COFs for detecting various molecules. The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly observed photoluminescence quenching of COFs, we propose a strategy involving interrupting the intralayer conjugation and interlayer interactions using cyclohexane as the linker unit. By variation of the building block structures, imine-bonded COFs with various topologies and porosities are obtained. Experimental and theoretical analyses of these COFs disclose high crystallinity and large interlayer distances, demonstrating enhanced emission with record-high photoluminescence quantum yields of up to 57% in the solid state. The resulting cyclohexane-linked COF also exhibits excellent sensing performance for the trace recognition of Fe3+ ions, explosive and toxic picric acid, and phenyl glyoxylic acid as metabolites. These findings inspire a facile and general strategy to develop highly emissive imine-bonded COFs for detecting various molecules.The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly observed photoluminescence quenching of COFs, we propose a strategy involving interrupting the intralayer conjugation and interlayer interactions using cyclohexane as the linker unit. By variation of the building block structures, imine-bonded COFs with various topologies and porosities are obtained. Experimental and theoretical analyses of these COFs disclose high crystallinity and large interlayer distances, demonstrating enhanced emission with record-high photoluminescence quantum yields of up to 57% in the solid state. The resulting cyclohexane-linked COF also exhibits excellent sensing performance for the trace recognition of Fe3+ ions, explosive and toxic picric acid, and phenyl glyoxylic acid as metabolites. These findings inspire a facile and general strategy to develop highly emissive imine-bonded COFs for detecting various molecules. |
| Author | Graf, Robert Harano, Koji Jin, Enquan Yang, Meijia Fang, Long Guo, Yunyu Narita, Akimitsu Hanayama, Hiroki Kikkawa, Jun Müllen, Klaus Addicoat, Matthew A. |
| AuthorAffiliation | School of Science and Technology State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry and International Center of Future Science National Institute for Materials Science Center for Basic Research on Materials Organic and Carbon Nanomaterials Unit Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Chemistry |
| AuthorAffiliation_xml | – name: National Institute for Materials Science – name: Organic and Carbon Nanomaterials Unit – name: Center for Basic Research on Materials – name: School of Science and Technology – name: Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Chemistry – name: State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry and International Center of Future Science |
| Author_xml | – sequence: 1 givenname: Meijia surname: Yang fullname: Yang, Meijia organization: Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Chemistry – sequence: 2 givenname: Hiroki surname: Hanayama fullname: Hanayama, Hiroki organization: Organic and Carbon Nanomaterials Unit – sequence: 3 givenname: Long surname: Fang fullname: Fang, Long organization: Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Chemistry – sequence: 4 givenname: Matthew A. orcidid: 0000-0002-5406-7927 surname: Addicoat fullname: Addicoat, Matthew A. organization: School of Science and Technology – sequence: 5 givenname: Yunyu surname: Guo fullname: Guo, Yunyu organization: State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry and International Center of Future Science – sequence: 6 givenname: Robert orcidid: 0000-0003-2302-0760 surname: Graf fullname: Graf, Robert – sequence: 7 givenname: Koji orcidid: 0000-0001-6800-8023 surname: Harano fullname: Harano, Koji organization: National Institute for Materials Science – sequence: 8 givenname: Jun orcidid: 0000-0003-0659-1844 surname: Kikkawa fullname: Kikkawa, Jun organization: National Institute for Materials Science – sequence: 9 givenname: Enquan orcidid: 0009-0008-5043-5543 surname: Jin fullname: Jin, Enquan email: enquanjin@jlu.edu.cn organization: Organic and Carbon Nanomaterials Unit – sequence: 10 givenname: Akimitsu orcidid: 0000-0002-3625-522X surname: Narita fullname: Narita, Akimitsu email: akimitsu.narita@oist.jp organization: Organic and Carbon Nanomaterials Unit – sequence: 11 givenname: Klaus surname: Müllen fullname: Müllen, Klaus email: muellen@mpip-mainz.mpg.de |
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| Snippet | The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly... The development of highly luminescent two-dimensional covalent organic frameworks (COFs) for sensing applications remains challenging. To suppress commonly... |
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| SubjectTerms | crystal structure cyclohexanes glyoxylic acid metabolites photoluminescence toxicity |
| Title | Saturated Linkers in Two-Dimensional Covalent Organic Frameworks Boost Their Luminescence |
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