Imaging of coexisting classical and non-classical oriented attachment growth pathways in covalent organic framework microcrystals

Jinxiang Wu, Qianxi Wang, Yanhao Li and Yi He ()
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Jinxiang Wu: Southwest University of Science and Technology
Qianxi Wang: Southwest University of Science and Technology
Yanhao Li: Southwest University of Science and Technology
Yi He: Southwest University of Science and Technology

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract Three-dimensional covalent organic frameworks are promising multifunctional materials for applications in adsorption, separation, and catalysis. However, despite the continuous synthesis of an increasing number of three-dimensional covalent organic frameworks, little is known about the crystal growth pathways. Here, we report the real-time visual observation of the crystal growth process of COF-300 and LZU-79, two typical three-dimensional covalent organic frameworks, using in situ dark-field optical microscopy. Our dark-field optical microscopy imaging results reveal that two crystal-growth pathways are simultaneously operative during the liquid growth of COF-300 and LZU-79 microcrystals, including classical crystal growth modes and non-classical oriented attachment mechanisms. Specifically, detailed tracking of the trajectories between two rod-shaped single-crystal COF-300 pairs suggests that the oriented attachment process undergoes several distinct stages such as approach, alignment at (021) facets, tip-to-tip attachment, fusion, and shaping. Theoretical simulation results show that (021) facets of COF-300 microcrystals, which have a lower repulsive energy barrier due to steric solvation forces from intervening solvents, are energetically more favorable than (010) facets, inducing the oriented attachment between adjacent facets. This work enables a fundamental understanding of how three-dimensional covalent organic framework microcrystals grow dynamically, which can aid the further design of three-dimensional covalent organic frameworks with enhanced performances.

Date: 2025
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DOI: 10.1038/s41467-025-58130-9

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