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Mutually reinforced multicomponent polysaccharide networks.

ABSTRACT: Networks made from chitosan and alginate have been utilized as prospective tissue engineering scaffolds due to material biocompatibility and degradability. Calcium (Ca(2+) ) is often added to these networks as a modifier for mechanical strength enhancement. In this work, we examined changes in the bulk material properties of different concentrations of chitosan/alginate mixtures (2, 3, or 5% w/w) upon adding another modifier, chondroitin. We further examined how material properties depend on the order the modifiers, Ca(2+) and chondroitin, were added. It was found that the addition of chondroitin significantly increased the mechanical strength of chitosan/alginate networks. Highest elastic moduli were obtained from samples made with mass fractions of 5% chitosan and alginate, modified by chondroitin first and then Ca(2+) . The elastic moduli in dry and hydrated states were (4.41 ± 0.52) MPa and (0.11 ± 0.01) MPa, respectively. Network porosity and density were slightly dependent on total polysaccharide concentration. Average pore size was slightly larger in samples modified by Ca(2+) first and then chondroitin and in samples made with 3% starting mass fractions. Here, small-angle neutron scattering (SANS) was utilized to examine mesh size of the fibrous networks, mass-fractal parameters and average dimensions of the fiber cross-sections prior to freeze-drying. These studies revealed that addition of Ca(2+) and chondroitin modifiers increased fiber compactness and thickness, respectively. Together these findings are consistent with improved network mechanical properties of the freeze-dried materials.

SUBMITTER: Hyland LL

PROVIDER: S-EPMC3183399 | biostudies-literature | 2011 Dec

REPOSITORIES: biostudies-literature

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Mutually reinforced multicomponent polysaccharide networks.

Hyland Laura L LL Taraban Marc B MB Hammouda Boualem B Bruce Yu Y Y

Biopolymers 20110622 12

Networks made from chitosan and alginate have been utilized as prospective tissue engineering scaffolds due to material biocompatibility and degradability. Calcium (Ca(2+) ) is often added to these networks as a modifier for mechanical strength enhancement. In this work, we examined changes in the bulk material properties of different concentrations of chitosan/alginate mixtures (2, 3, or 5% w/w) upon adding another modifier, chondroitin. We further examined how material properties depend on the ...[more]

PMID: 21698596

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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.

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Mutually reinforced multicomponent polysaccharide networks.

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Mutually reinforced multicomponent polysaccharide networks.

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