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

Author

Listed:
  • Yangyang Xu

    (ShanghaiTech University)

  • Tu Sun

    (ShanghaiTech University
    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
    ShanghaiTech University)

  • Shan Jiang

    (ShanghaiTech University
    ShanghaiTech University)

  • Yanhang Ma

    (ShanghaiTech University
    ShanghaiTech University)

  • Yue-Biao Zhang

    (ShanghaiTech University
    ShanghaiTech University)

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.

Suggested Citation

  • Yangyang Xu & Tu Sun & Tengwu Zeng & Xiangyu Zhang & Xuan Yao & Shan Liu & Zhaolin Shi & Wen Wen & Yingbo Zhao & Shan Jiang & Yanhang Ma & Yue-Biao Zhang, 2023. "Symmetry-breaking dynamics in a tautomeric 3D covalent organic framework," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39998-x
    DOI: 10.1038/s41467-023-39998-x
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