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

Chengjun Kang, Kuiwei Yang, Zhaoqiang Zhang, Adam K. Usadi, David C. Calabro, Lisa Saunders Baugh, Yuxiang Wang, Jianwen Jiang, Xiaodong Zou, Zhehao Huang () and Dan Zhao ()
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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

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-29086-x

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