Symmetry-breaking dynamics in a tautomeric 3D covalent organic framework

Yangyang Xu, Tu Sun, Tengwu Zeng, Xiangyu Zhang, Xuan Yao, Shan Liu, Zhaolin Shi, Wen Wen, Yingbo Zhao, Shan Jiang, Yanhang Ma and Yue-Biao Zhang ()
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Yangyang Xu: ShanghaiTech University
Tu Sun: ShanghaiTech University
Tengwu Zeng: ShanghaiTech University
Xiangyu Zhang: ShanghaiTech University
Xuan Yao: ShanghaiTech University
Shan Liu: ShanghaiTech University
Zhaolin Shi: ShanghaiTech University
Wen Wen: Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academic of Sciences
Yingbo Zhao: ShanghaiTech University
Shan Jiang: ShanghaiTech University
Yanhang Ma: ShanghaiTech University
Yue-Biao Zhang: ShanghaiTech University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract The enolimine-ketoenamine tautomerism has been utilised to construct 2D covalent organic frameworks (COFs) with a higher level of chemical robustness and superior photoelectronic activity. However, it remains challenging to fully control the tautomeric states and correlate their tautomeric structure-photoelectronic properties due to the mobile equilibrium of proton transfer between two other atoms. We show that symmetry-asymmetry tautomerisation from diiminol to iminol/cis-ketoenamine can be stabilised and switched in a crystalline, porous, and dynamic 3D COF (dynaCOF-301) through concerted structural transformation and host-guest interactions upon removal and adaptive inclusion of various guest molecules. Specifically, the tautomeric dynaCOF-301 is constructed by linking the hydroquinone with a tetrahedral building block through imine linkages to form 7-fold interwoven diamondoid networks with 1D channels. Reversible framework deformation and ordering-disordering transition are determined from solvated to activated and hydrated phases, accompanied by solvatochromic and hydrochromic effects useful for rapid, steady, and visual naked-eye chemosensing.

Date: 2023
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DOI: 10.1038/s41467-023-39998-x

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