Authors
Fan Qiu, Lei Gao, Yubin Fu, Sankalpa N Panda, Xing Su, Ya Lu, Mei-Mei Zhang, Mischa Bonn, Paolo Samorì, Yuqiao Wang, Xin Zhao, Shun-Qi Xu
Published in
Angewandte Chemie (International ed. in English). Pages e5409854. Sep 18, 2026. Epub Sep 18, 2026.
Abstract
Covalent organic frameworks derived from triformylphloroglucinol (Tp-COFs) represent a prominent branch of COFs due to their high potential in separation, energy storage, and optoelectronics. However, the development of Tp-COFs is often hindered by limited crystallinity, resulting from the low reversibility of β-ketoenamine bond formation. In this study, we report an unprecedented dynamic self-healing mechanism during Tp-COF formation, arising from a reversible Michael-addition-elimination (MAE) process. Building on this insight, a modulator-mediated MAE pathway is further established for crystallinity control. As a representative example, Tp-COF-1 synthesized via this strategy (Tp-COF-1(H)) forms well-defined columnar crystals with domain sizes up to 20 µm × 2 µm, and exhibits significantly improved structural order, as evidenced by a sharper powder x-ray diffraction (PXRD) peak (full width at half maximum: 0.44° vs. 0.74°) and a higher specific surface area (1314 vs. 647 m2 g-1), compared to Tp-COF-1 synthesized by the conventional method (Tp-COF-1(O)). Moreover, optical pump-terahertz probe spectroscopy reveals a photoexcited charge-carrier mobility of 10.84 cm2 V-1 s-1 for Tp-COF-1(H), which is 1.77 times higher than that of Tp-COF-1(O). These findings identify dynamic self-healing process via MAE as a key mechanism for governing Tp-COF crystallization toward highly ordered Tp-COFs for optoelectronic applications.
PMID:
42757985
Bibliographic data and abstract were imported from PubMed on 18 Sep 2026.
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