Control of seed formation allows two distinct self-sorting patterns of supramolecular nanofibers

Ryou Kubota, Kazutoshi Nagao, Wataru Tanaka, Ryotaro Matsumura, Takuma Aoyama, Kenji Urayama and Itaru Hamachi ()
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Ryou Kubota: Kyoto University, Katsura, Nishikyo-ku
Kazutoshi Nagao: Kyoto University, Katsura, Nishikyo-ku
Wataru Tanaka: Kyoto University, Katsura, Nishikyo-ku
Ryotaro Matsumura: Kyoto University, Katsura, Nishikyo-ku
Takuma Aoyama: Kyoto Institute of Technology, Matsugasaki
Kenji Urayama: Kyoto Institute of Technology, Matsugasaki
Itaru Hamachi: Kyoto University, Katsura, Nishikyo-ku

Nature Communications, 2020, vol. 11, issue 1, 1-13

Abstract: Abstract Self-sorting double network hydrogels comprising orthogonal supramolecular nanofibers have attracted attention as artificially-regulated multi-component systems. Regulation of network patterns of self-sorted nanofibers is considered as a key for potential applications such as optoelectronics, but still challenging owing to a lack of useful methods to prepare and analyze the network patterns. Herein, we describe the selective construction of two distinct self-sorting network patterns, interpenetrated and parallel, by controlling the kinetics of seed formation with dynamic covalent oxime chemistry. Confocal imaging reveals the interpenetrated self-sorting network was formed upon addition of O-benzylhydroxylamine to a benzaldehyde-tethered peptide-type hydrogelator in the presence of lipid-type nanofibers. We also succeed in construction of a parallel self-sorting network through deceleration of seed formation using a slow oxime exchange reaction. Through careful observation, the formation of peptide-type seeds and nanofibers is shown to predominantly occur on the surface of the lipid-type nanofibers via highly dynamic and thermally-fluctuated processes.

Date: 2020
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DOI: 10.1038/s41467-020-17984-x

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