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Printable homocomposite hydrogels with synergistically reinforced molecular-colloidal networks.

ABSTRACT: The design of hydrogels where multiple interpenetrating networks enable enhanced mechanical properties can broaden their field of application in biomedical materials, 3D printing, and soft robotics. We report a class of self-reinforced homocomposite hydrogels (HHGs) comprised of interpenetrating networks of multiscale hierarchy. A molecular alginate gel is reinforced by a colloidal network of hierarchically branched alginate soft dendritic colloids (SDCs). The reinforcement of the molecular gel with the nanofibrillar SDC network of the same biopolymer results in a remarkable increase of the HHG's mechanical properties. The viscoelastic HHGs show >3× larger storage modulus and >4× larger Young's modulus than either constitutive network at the same concentration. Such synergistically enforced colloidal-molecular HHGs open up numerous opportunities for formulation of biocompatible gels with robust structure-property relationships. Balance of the ratio of their precursors facilitates precise control of the yield stress and rate of self-reinforcement, enabling efficient extrusion 3D printing of HHGs.

SUBMITTER: Williams AH

PROVIDER: S-EPMC8121785 | biostudies-literature | 2021 May

REPOSITORIES: biostudies-literature

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Printable homocomposite hydrogels with synergistically reinforced molecular-colloidal networks.

Williams Austin H AH Roh Sangchul S Jacob Alan R AR Stoyanov Simeon D SD Hsiao Lilian L Velev Orlin D OD

Nature communications 20210514 1

The design of hydrogels where multiple interpenetrating networks enable enhanced mechanical properties can broaden their field of application in biomedical materials, 3D printing, and soft robotics. We report a class of self-reinforced homocomposite hydrogels (HHGs) comprised of interpenetrating networks of multiscale hierarchy. A molecular alginate gel is reinforced by a colloidal network of hierarchically branched alginate soft dendritic colloids (SDCs). The reinforcement of the molecular gel ...[more]

PMID: 33990593

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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 β-cyclodextrin (β-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.

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Printable homocomposite hydrogels with synergistically reinforced molecular-colloidal networks.

Publications

Printable homocomposite hydrogels with synergistically reinforced molecular-colloidal networks.

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