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    Relation between the Water Content and Mechanical Properties of Hydrogels with Movable Cross-Links
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    • Koki Nishida
      Koki Nishida
      Department of Macromolecular Science, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
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    • Ryohei Ikura
      Ryohei Ikura
      Department of Macromolecular Science, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
      Forefront Research Center for Fundamental Sciences, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
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    • Kenji Yamaoka
      Kenji Yamaoka
      Department of Macromolecular Science, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
      Forefront Research Center for Fundamental Sciences, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
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      Orcidhttps://orcid.org/0000-0001-5655-1643
    • Osamu Urakawa
      Osamu Urakawa
      Department of Macromolecular Science, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
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      Orcidhttps://orcid.org/0000-0001-5071-208X
    • Takashi Konishi*
      Takashi Konishi
      Graduate School of Human and Environmental Studies, Kyoto University, Kyoto 606-8501, Japan
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0003-1134-5445
    • Tadashi Inoue
      Tadashi Inoue
      Department of Macromolecular Science, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
      Forefront Research Center for Fundamental Sciences, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
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      Orcidhttps://orcid.org/0000-0002-9934-1299
    • Go Matsuba*
      Go Matsuba
      Graduate School of Organic Materials Engineering, Yamagata University, 4-3-16 Jonan, Yonezawa, Yamagata 992-8510, Japan
      *Email: [email protected]
      More by Go Matsuba
      Orcidhttps://orcid.org/0000-0002-6863-5796
    • Masaru Tanaka*
      Masaru Tanaka
      Institute for Materials Chemistry and Engineering, Kyushu University, CE41 744 Motooka, Nishi, Fukuoka 819-0395, Japan
      *Email: [email protected]
      More by Masaru Tanaka
      Orcidhttps://orcid.org/0000-0002-1115-2080
    • Yoshinori Takashima*
      Yoshinori Takashima
      Department of Macromolecular Science, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
      Forefront Research Center for Fundamental Sciences, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-0043, Japan
      Innovative Catalysis Science Division, Institute for Open and Transdisciplinary Research Initiatives (ICS-OTRI), Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan
      *Email: [email protected]
      More by Yoshinori Takashima
      Orcidhttps://orcid.org/0000-0002-2620-3266
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    Macromolecules

    Cite this: Macromolecules 2024, 57, 16, 7745–7754
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    https://doi.org/10.1021/acs.macromol.4c00732
    Published August 13, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    To reveal the synergic effects of movable and reversible cross-links, we fabricated movable cross-linked hydrogels with hydrophobic acetylated cyclodextrins (CDs). The obtained hydrogels showed high toughness based on the broad range of relaxation times achieved by the high mobility of movable cross-links and reversible hydrophobic interaction. The high mobility of movable cross-links resulted from the lack of hydrogen bonds between the triacetylated γCD (TAcγCD) units and main chains. High mobility also occurred because TAcγCD units were not hydrated. The localization of hydration forms hydrophobic domains with the distribution of TAcγCD units. The hydrophobic domains also disperse the stress upon tensile deformation. The low water content (Wc = 15 wt %) achieved further high toughness (36.8 MJ·m–3) by the triple-synergic effects of movable cross-links, reversible hydrophobic interaction, and craze/fibril-like structures upon deformation. The mobility of movable cross-links and the reformation of reversible hydrophobic interaction achieved high self-restoring properties.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.macromol.4c00732.

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    • Movie of the hydrogel pTAcγCD(0.5):43 being stretched over 6000% strain (MP4)

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    1. Arbind Chaurasiya, Poorn Prakash Pande, Ravi Shankar, Prateek Khare, Praveen Kumar, Navneet Kumar Yadav, Kajal Kumar Dey. Synthesis and characterization of chemically functionalized novel smart guar gum xanthate based hydrogel: Swelling, isotherm, kinetics, thermodynamic and reusability studies. Journal of Physics and Chemistry of Solids 2025, 200 , 112584. https://doi.org/10.1016/j.jpcs.2025.112584
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    Macromolecules

    Cite this: Macromolecules 2024, 57, 16, 7745–7754
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.macromol.4c00732
    Published August 13, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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