Reconstructed covalent organic frameworks
Weiwei Zhang,
Linjiang Chen,
Sheng Dai,
Chengxi Zhao,
Cheng Ma,
Lei Wei,
Minghui Zhu,
Samantha Y. Chong,
Haofan Yang,
Lunjie Liu,
Yang Bai,
Miaojie Yu,
Yongjie Xu,
Xiao-Wei Zhu,
Qiang Zhu,
Shuhao An,
Reiner Sebastian Sprick,
Marc A. Little,
Xiaofeng Wu,
Shan Jiang,
Yongzhen Wu,
Yue-Biao Zhang,
He Tian,
Wei-Hong Zhu () and
Andrew I. Cooper ()
Additional contact information
Weiwei Zhang: East China University of Science and Technology
Linjiang Chen: East China University of Science and Technology
Sheng Dai: East China University of Science and Technology
Chengxi Zhao: East China University of Science and Technology
Cheng Ma: East China University of Science and Technology
Lei Wei: ShanghaiTech University
Minghui Zhu: East China University of Science and Technology
Samantha Y. Chong: University of Liverpool
Haofan Yang: University of Liverpool
Lunjie Liu: University of Liverpool
Yang Bai: University of Liverpool
Miaojie Yu: East China University of Science and Technology
Yongjie Xu: University of Liverpool
Xiao-Wei Zhu: University of Liverpool
Qiang Zhu: University of Liverpool
Shuhao An: East China University of Science and Technology
Reiner Sebastian Sprick: University of Liverpool
Marc A. Little: University of Liverpool
Xiaofeng Wu: East China University of Science and Technology
Shan Jiang: ShanghaiTech University
Yongzhen Wu: East China University of Science and Technology
Yue-Biao Zhang: ShanghaiTech University
He Tian: East China University of Science and Technology
Wei-Hong Zhu: East China University of Science and Technology
Andrew I. Cooper: East China University of Science and Technology
Nature, 2022, vol. 604, issue 7904, 72-79
Abstract:
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.
Date: 2022
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Persistent link: https://EconPapers.repec.org/RePEc:nat:nature:v:604:y:2022:i:7904:d:10.1038_s41586-022-04443-4
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DOI: 10.1038/s41586-022-04443-4
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