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Reconstructed covalent organic frameworks.
Zhang, Weiwei; Chen, Linjiang; Dai, Sheng; Zhao, Chengxi; Ma, Cheng; Wei, Lei; Zhu, Minghui; Chong, Samantha Y; Yang, Haofan; Liu, Lunjie; Bai, Yang; Yu, Miaojie; Xu, Yongjie; Zhu, Xiao-Wei; Zhu, Qiang; An, Shuhao; Sprick, Reiner Sebastian; Little, Marc A; Wu, Xiaofeng; Jiang, Shan; Wu, Yongzhen; Zhang, Yue-Biao; Tian, He; Zhu, Wei-Hong; Cooper, Andrew I.
Afiliação
  • Zhang W; Key Laboratory for Advanced Materials and Institute of Fine Chemicals, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry
  • Chen L; Key Laboratory for Advanced Materials and Institute of Fine Chemicals, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry
  • Dai S; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Zhao C; Key Laboratory for Advanced Materials and Institute of Fine Chemicals, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry
  • Ma C; Key Laboratory for Advanced Materials and Institute of Fine Chemicals, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry
  • Wei L; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Zhu M; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, China.
  • Chong SY; School of Physical Science and Technology, ShanghaiTech University, Shanghai, China.
  • Yang H; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, China.
  • Liu L; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Bai Y; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Yu M; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Xu Y; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Zhu XW; Key Laboratory for Advanced Materials and Institute of Fine Chemicals, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry
  • Zhu Q; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • An S; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Sprick RS; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Little MA; Key Laboratory for Advanced Materials and Institute of Fine Chemicals, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry
  • Wu X; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Jiang S; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Wu Y; Key Laboratory for Advanced Materials and Institute of Fine Chemicals, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry
  • Zhang YB; Leverhulme Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool, UK.
  • Tian H; School of Physical Science and Technology, ShanghaiTech University, Shanghai, China.
  • Zhu WH; Key Laboratory for Advanced Materials and Institute of Fine Chemicals, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry
  • Cooper AI; School of Physical Science and Technology, ShanghaiTech University, Shanghai, China.
Nature ; 604(7904): 72-79, 2022 04.
Article em En | MEDLINE | ID: mdl-35388196
ABSTRACT
Covalent organic frameworks (COFs) are distinguished from other organic polymers by their crystallinity1-3, but it remains challenging to obtain robust, highly crystalline COFs because the framework-forming reactions are poorly reversible4,5. More reversible chemistry can improve crystallinity6-9, but this typically yields COFs with poor physicochemical stability and limited application scope5. Here we report a general and scalable protocol to prepare robust, highly crystalline imine COFs, based on an unexpected framework reconstruction. In contrast to standard approaches in which monomers are initially randomly aligned, our method involves the pre-organization of monomers using a reversible and removable covalent tether, followed by confined polymerization. This reconstruction route produces reconstructed COFs with greatly enhanced crystallinity and much higher porosity by means of a simple vacuum-free synthetic procedure. The increased crystallinity in the reconstructed COFs improves charge carrier transport, leading to sacrificial photocatalytic hydrogen evolution rates of up to 27.98 mmol h-1 g-1. This nanoconfinement-assisted reconstruction strategy is a step towards programming function in organic materials through atomistic structural control.
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2022 Tipo de documento: Article
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2022 Tipo de documento: Article