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Redox-responsive self-healing materials formed from host-guest polymers.

ABSTRACT: Expanding the useful lifespan of materials is becoming highly desirable, and self-healing and self-repairing materials may become valuable commodities. The formation of supramolecular materials through host-guest interactions is a powerful method to create non-conventional materials. Here we report the formation of supramolecular hydrogels and their redox-responsive and self-healing properties due to host-guest interactions. We employ cyclodextrin (CD) as a host molecule because it is environmentally benign and has diverse applications. A transparent supramolecular hydrogel quickly forms upon mixing poly(acrylic acid) (pAA) possessing ?-CD as a host polymer with pAA possessing ferrocene as a guest polymer. Redox stimuli induce a sol-gel phase transition in the supramolecular hydrogel and can control self-healing properties such as re-adhesion between cut surfaces.

SUBMITTER: Nakahata M

PROVIDER: S-EPMC3207205 | biostudies-literature | 2011 Oct

REPOSITORIES: biostudies-literature

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Redox-responsive self-healing materials formed from host-guest polymers.

Nakahata Masaki M Takashima Yoshinori Y Yamaguchi Hiroyasu H Harada Akira A

Nature communications 20111025

Expanding the useful lifespan of materials is becoming highly desirable, and self-healing and self-repairing materials may become valuable commodities. The formation of supramolecular materials through host-guest interactions is a powerful method to create non-conventional materials. Here we report the formation of supramolecular hydrogels and their redox-responsive and self-healing properties due to host-guest interactions. We employ cyclodextrin (CD) as a host molecule because it is environmen ...[more]

PMID: 22027591

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Project description:Natural polymer hydrogels are one of the best biomaterials for soft tissue repair because of their excellent biocompatibility, biodegradability and low immune rejection. However, they lack mechanical strength matching that of natural tissue and desired functionality (e.g. self-healing and 3D-printability). To solve this problem, we developed a host-guest supramolecule (HGSM) with three arms covalently crosslinked with a natural polymer to construct a novel hydrogel with non-covalent bonds integrated in a covalently crosslinked network. The unique structure enabled the hydrogel to bear improved mechanical properties and show both self-healing and 3D printing capabilities. The three-armed HGSM was first prepared via the efficient non-covalent host-guest inclusion interactions between isocyanatoethyl acrylate-modified ?-cyclodextrin (?-CD-AOI2) and acryloylated tetra-ethylene glycol-modified adamantane (A-TEG-Ad). Subsequently, a host-guest supramolecular hydrogel (HGGelMA) was obtained through copolymerization between the arms of HGSM and gelatin methacryloyl (GelMA) to form a covalently crosslinked network. The HGGelMA was robust, fatigue resistant, reproducible and rapidly self-healing. In HGGelMA, the covalent crosslinking maintained its overall shape whereas the weak reversible non-covalent host-guest interactions reinforced its mechanical properties and enabled it to rapidly self-heal upon fracturing. The reversible non-covalent interactions could be re-established upon breaking, so as to heal the hydrogel and dissipate energy to prevent catastrophic fracture propagation. Furthermore, the precursors of the HGGelMA were sufficiently viscous and could be rapidly photocrosslinked to produce a robust scaffold with an exquisite internal structure through 3D printing. The 3D-printed HGGelMA hydrogel scaffold was biocompatible, promoted cell adhesion and proliferation, and supported tissue in-growth. Our strategy of integrating non-covalently linked HGSM in a covalently linked hydrogel network represents a new approach to the development of natural polymers into biocompatible hydrogels with improved strength as well as desired self-healing and 3D-printability.

Dataset Information

Redox-responsive self-healing materials formed from host-guest polymers.

Publications

Redox-responsive self-healing materials formed from host-guest polymers.

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