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<p>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&#xa0;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 <i>block-stacking</i> model. A statistical analysis of the concentration-dependent lag time on macroscopic observation of the gelation suggests the presence of a&#xa0;tetrameric or octameric nucleus of the urea molecules.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月22日

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  • Shinya Kimura,
  • Kurea Adachi,
  • Yoshiki Ishii,
  • Tomoki Komiyama,
  • Takuho Saito,
  • Naofumi Nakayama,
  • Masashi Yokoya,
  • Hikaru Takaya,
  • Shiki Yagai,
  • Shinnosuke Kawai,
  • Takayuki Uchihashi,
  • Masamichi Yamanaka

摘要

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.