Molecular-level insights into the supramolecular gelation mechanism of urea derivative

Shinya Kimura (), Kurea Adachi, Yoshiki Ishii, Tomoki Komiyama, Takuho Saito, Naofumi Nakayama, Masashi Yokoya, Hikaru Takaya, Shiki Yagai (), Shinnosuke Kawai (), Takayuki Uchihashi () and Masamichi Yamanaka
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Shinya Kimura: Meiji Pharmaceutical University
Kurea Adachi: Meiji Pharmaceutical University
Yoshiki Ishii: Nagoya University
Tomoki Komiyama: Meiji Pharmaceutical University
Takuho Saito: Chiba University
Naofumi Nakayama: CONFLEX Corporation
Masashi Yokoya: Meiji Pharmaceutical University
Hikaru Takaya: Teikyo University of Science
Shiki Yagai: Chiba University
Shinnosuke Kawai: Shizuoka University
Takayuki Uchihashi: Nagoya University
Masamichi Yamanaka: Meiji Pharmaceutical University

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Despite being a promising soft material embodied by molecular self-assembly, the formation mechanism of supramolecular gels remains challenging to fully understand. Here we provide molecular to nanoscopic insights into the formation mechanism of gel-forming fibers from a urea derivative. High-speed atomic force microscopy of the urea derivative revealed the presence of a lag phase prior to the formation of supramolecular fibers, suggesting a nucleation process. The fiber growth kinetics differ at both termini of the fiber, indicating a directional hydrogen-bonding motif by the urea units, which is supported by single-crystal X-ray crystallography of a reference compound. Moreover, we observed an intermittent growth pattern of the fibers with repeated elongation and pause phases. This unique behavior can be simulated by a theoretical block-stacking model. A statistical analysis of the concentration-dependent lag time on macroscopic observation of the gelation suggests the presence of a tetrameric or octameric nucleus of the urea molecules.

Date: 2025
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DOI: 10.1038/s41467-025-59032-6

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