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Dielectric Study on Supramolecular Gels by Fiber Structure Formation from Low-Molecular-Weight Gelator/Water Mixtures

There are various types of gel materials used in a wide range of fields, and their gelation mechanisms are extremely diverse. Furthermore, in the case of hydrogels, there exist some difficulties in understanding complicated molecular mechanisms especially with water molecules interacting through hyd...

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Autores principales: Shimizu, Kenta, Abe, Fumiya, Kishi, Yasuhiro, Kita, Rio, Shinyashiki, Naoki, Yagihara, Shin
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10218103/
https://www.ncbi.nlm.nih.gov/pubmed/37233000
http://dx.doi.org/10.3390/gels9050408
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author Shimizu, Kenta
Abe, Fumiya
Kishi, Yasuhiro
Kita, Rio
Shinyashiki, Naoki
Yagihara, Shin
author_facet Shimizu, Kenta
Abe, Fumiya
Kishi, Yasuhiro
Kita, Rio
Shinyashiki, Naoki
Yagihara, Shin
author_sort Shimizu, Kenta
collection PubMed
description There are various types of gel materials used in a wide range of fields, and their gelation mechanisms are extremely diverse. Furthermore, in the case of hydrogels, there exist some difficulties in understanding complicated molecular mechanisms especially with water molecules interacting through hydrogen bonding as solvents. In the present work, the molecular mechanism of the structural formation of fibrous super-molecular gel by the low molecular weight gelator, N-oleyl lactobionamide/water mixture was elucidated using the broadband dielectric spectroscopy (BDS) method. The dynamic behaviors observed for the solute and water molecules indicated hierarchical structure formation processes in various time scales. The relaxation curves obtained at various temperatures in the cooling and heating processes showed relaxation processes respectively reflecting the dynamic behaviors of water molecules in the 10 GHz frequency region, solute molecules interacting with water in MHz region, and ion-reflecting structures of the sample and electrode in kHz region. These relaxation processes, characterized by the relaxation parameters, showed remarkable changes around the sol–gel transition temperature, 37.8 °C, determined by the falling ball method and over the temperature range, around 53 °C. The latter change suggested a structure formation of rod micelles appearing as precursors before cross-linking into the three-dimensional network of the supramolecular gels. These results clearly demonstrate how effective relaxation parameter analysis is for understanding the gelation mechanism in detail.
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spelling pubmed-102181032023-05-27 Dielectric Study on Supramolecular Gels by Fiber Structure Formation from Low-Molecular-Weight Gelator/Water Mixtures Shimizu, Kenta Abe, Fumiya Kishi, Yasuhiro Kita, Rio Shinyashiki, Naoki Yagihara, Shin Gels Article There are various types of gel materials used in a wide range of fields, and their gelation mechanisms are extremely diverse. Furthermore, in the case of hydrogels, there exist some difficulties in understanding complicated molecular mechanisms especially with water molecules interacting through hydrogen bonding as solvents. In the present work, the molecular mechanism of the structural formation of fibrous super-molecular gel by the low molecular weight gelator, N-oleyl lactobionamide/water mixture was elucidated using the broadband dielectric spectroscopy (BDS) method. The dynamic behaviors observed for the solute and water molecules indicated hierarchical structure formation processes in various time scales. The relaxation curves obtained at various temperatures in the cooling and heating processes showed relaxation processes respectively reflecting the dynamic behaviors of water molecules in the 10 GHz frequency region, solute molecules interacting with water in MHz region, and ion-reflecting structures of the sample and electrode in kHz region. These relaxation processes, characterized by the relaxation parameters, showed remarkable changes around the sol–gel transition temperature, 37.8 °C, determined by the falling ball method and over the temperature range, around 53 °C. The latter change suggested a structure formation of rod micelles appearing as precursors before cross-linking into the three-dimensional network of the supramolecular gels. These results clearly demonstrate how effective relaxation parameter analysis is for understanding the gelation mechanism in detail. MDPI 2023-05-12 /pmc/articles/PMC10218103/ /pubmed/37233000 http://dx.doi.org/10.3390/gels9050408 Text en © 2023 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Shimizu, Kenta
Abe, Fumiya
Kishi, Yasuhiro
Kita, Rio
Shinyashiki, Naoki
Yagihara, Shin
Dielectric Study on Supramolecular Gels by Fiber Structure Formation from Low-Molecular-Weight Gelator/Water Mixtures
title Dielectric Study on Supramolecular Gels by Fiber Structure Formation from Low-Molecular-Weight Gelator/Water Mixtures
title_full Dielectric Study on Supramolecular Gels by Fiber Structure Formation from Low-Molecular-Weight Gelator/Water Mixtures
title_fullStr Dielectric Study on Supramolecular Gels by Fiber Structure Formation from Low-Molecular-Weight Gelator/Water Mixtures
title_full_unstemmed Dielectric Study on Supramolecular Gels by Fiber Structure Formation from Low-Molecular-Weight Gelator/Water Mixtures
title_short Dielectric Study on Supramolecular Gels by Fiber Structure Formation from Low-Molecular-Weight Gelator/Water Mixtures
title_sort dielectric study on supramolecular gels by fiber structure formation from low-molecular-weight gelator/water mixtures
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10218103/
https://www.ncbi.nlm.nih.gov/pubmed/37233000
http://dx.doi.org/10.3390/gels9050408
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