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Growing single crystals of two-dimensional covalent organic frameworks enabled by intermediate tracing study

Author

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  • Chengjun Kang

    (National University of Singapore)

  • Kuiwei Yang

    (National University of Singapore)

  • Zhaoqiang Zhang

    (National University of Singapore)

  • Adam K. Usadi

    (ExxonMobil Asia Pacific Pte. Ltd., 1 HarbourFront Place HarbourFront Tower 1)

  • David C. Calabro

    (Corporate Strategic Research Laboratory, ExxonMobil Research and Engineering Company)

  • Lisa Saunders Baugh

    (Corporate Strategic Research Laboratory, ExxonMobil Research and Engineering Company)

  • Yuxiang Wang

    (National University of Singapore)

  • Jianwen Jiang

    (National University of Singapore)

  • Xiaodong Zou

    (Stockholm University)

  • Zhehao Huang

    (Stockholm University)

  • Dan Zhao

    (National University of Singapore)

Abstract

Resolving single-crystal structures of two-dimensional covalent organic frameworks (2D COFs) is a great challenge, hindered in part by limited strategies for growing high-quality crystals. A better understanding of the growth mechanism facilitates development of methods to grow high-quality 2D COF single crystals. Here, we take a different perspective to explore the 2D COF growth process by tracing growth intermediates. We discover two different growth mechanisms, nucleation and self-healing, in which self-assembly and pre-arrangement of monomers and oligomers are important factors for obtaining highly crystalline 2D COFs. These findings enable us to grow micron-sized 2D single crystalline COF Py-1P. The crystal structure of Py-1P is successfully characterized by three-dimensional electron diffraction (3DED), which confirms that Py-1P does, in part, adopt the widely predicted AA stacking structure. In addition, we find the majority of Py-1P crystals (>90%) have a previously unknown structure, containing 6 stacking layers within one unit cell.

Suggested Citation

  • Chengjun Kang & Kuiwei Yang & Zhaoqiang Zhang & Adam K. Usadi & David C. Calabro & Lisa Saunders Baugh & Yuxiang Wang & Jianwen Jiang & Xiaodong Zou & Zhehao Huang & Dan Zhao, 2022. "Growing single crystals of two-dimensional covalent organic frameworks enabled by intermediate tracing study," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-29086-x
    DOI: 10.1038/s41467-022-29086-x
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    References listed on IDEAS

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