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Biocompatible and biodegradable peptide hydrogels are drawing increasing attention as prospective materials for human soft tissue repair and replacement. To improve the rather unfavorable mechanical properties of our pure peptide hydrogels, in this work we examined the possibility of creating a double hydrogel network. This network was created by means of the coassembly of mutually attractive, but self-repulsive oligopeptides within an already-existing fibrous network formed by the charged, biocompatible polysaccharides chitosan, alginate, and chondroitin. Using dynamic oscillatory rheology experiments, it was found that the coassembly of the peptides within the existing polysaccharide network resulted in a less stiff material as compared to the pure peptide networks (the elastic modulus G' decreased from 90 to 10 kPa). However, these composite oligopeptide-polysaccharide hydrogels were characterized by a greater resistance to deformation (the yield strain γ grew from 4 to 100%). Small-angle neutron scattering (SANS) was used to study the 2D cross-sectional shapes of the fibers, their dimensional characteristics, and the mesh sizes of the fibrous networks. Differences in material structures found with SANS experiments confirmed rheology data, showing that incorporation of the peptides dramatically changed the morphology of the polysaccharide network. The resulting fibers were structurally very similar to those forming the pure peptide networks, but formed less stiff gels because of their markedly greater mesh sizes. Together, these findings suggest an approach for the development of highly deformation-resistant biomaterials., (Copyright © 2011 Wiley Periodicals, Inc.)

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., (2011 Wiley Periodicals, Inc.)