Molecular-level insights into the supramolecular gelation mechanism of urea derivative
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.
Authors
- Yoshiki Ishii (ORCID: https://orcid.org/0000-0003-0102-9326)
- Shinya Kimura (ORCID: https://orcid.org/0000-0003-3451-1389)
- Tomoki Komiyama
- Masamichi Yamanaka (ORCID: https://orcid.org/0000-0002-6591-9005)
- Kiyo Adachi
- Takayuki Uchihashi (ORCID: https://orcid.org/0000-0002-0263-5312)
- Takuho Saito (ORCID: https://orcid.org/0000-0002-5941-6006)
- Shinnosuke Kawai (ORCID: https://orcid.org/0000-0001-8813-0253)
- Masashi Yokoya (ORCID: https://orcid.org/0000-0003-0187-7595)
- Naofumi Nakayama (ORCID: https://orcid.org/0000-0002-1316-1861)
- Shiki Yagai (ORCID: https://orcid.org/0000-0002-4786-8603)
- Hikaru Takaya (ORCID: https://orcid.org/0000-0003-4688-7842)
Institutions
- Shizuoka University (JP)
- Teikyo University of Science (JP)
- University of Shizuoka (JP)
- Chiba University (JP)
- National Institutes of Natural Sciences (JP)
- Meiji Pharmaceutical University (JP)
- Inpex (Japan) (JP)
- Institute for Molecular Science (JP)
- Shizuoka Eiwa Gakuin University (JP)
- Nagoya University (JP)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-04-22
- DOI
- https://doi.org/10.1038/s41467-025-59032-6
- Citations
- 10
- Primary Topic
- Supramolecular Self-Assembly in Materials
- Type
- article
- Field-Weighted Citation Impact
- 5.97
Funders
- Ministry of Education, Culture, Sports, Science and Technology
- Shizuoka University
- Japan Society for the Promotion of Science
- Japan Science and Technology Agency
- Core Research for Evolutional Science and Technology