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Viscoelastic properties and nanoscale structures of composite oligopeptide-polysaccharide hydrogels.

ABSTRACT: 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 ? 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.

SUBMITTER: Hyland LL

PROVIDER: S-EPMC3506395 | biostudies-literature | 2012 Mar

REPOSITORIES: biostudies-literature

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Viscoelastic properties and nanoscale structures of composite oligopeptide-polysaccharide hydrogels.

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

Biopolymers 20111012 3

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, bioc ...[more]

PMID: 21994046

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Project description:BackgroundTissue engineering, which involves the selection of scaffold materials, presents a new therapeutic strategy for damaged tissues or organs. Scaffold design based on blends of proteins and polysaccharides, as mimicry of the native extracellular matrix, has recently become a valuable strategy for tissue engineering.ObjectiveThis study aimed to construct composite hydrogels based on natural polymers for tissue engineering.MethodsComposite hydrogels based on blends of gelatin with a polysaccharide component (chitosan or alginate) were produced and subsequently enzyme crosslinked. The other three hydrogels, chitosan hydrogel, sodium alginate hydrogel, and microbial transglutaminase-crosslinked gelatin (mTG/GA) hydrogel were also prepared. All hydrogels were evaluated for in vitro degradation property, swelling capacity, and mechanical property. Rat adipose-derived stromal stem cells (ADSCs) were isolated and seeded on (or embedded into) the above-mentioned hydrogels. The morphological features of ADSCs were observed and recorded. The effects of the hydrogels on ADSC survival and adhesion were investigated by immunofluorescence staining. Cell proliferation was tested by thiazolyl blue tetrazolium bromide (MTT) assay.ResultsCell viability assay results showed that the five hydrogels are not cytotoxic. The mTG/GA and its composite hydrogels showed higher compressive moduli than the single-component chitosan and alginate hydrogels. MTT assay results showed that ADSCs proliferated better on the composite hydrogels than on the chitosan and alginate hydrogels. Light microscope observation and cell cytoskeleton staining showed that hydrogel strength had obvious effects on cell growth and adhesion. The ADSCs seeded on chitosan and alginate hydrogels plunged into the hydrogels and could not stretch out due to the low strength of the hydrogel, whereas cells seeded on composite hydrogels with higher elastic modulus, could spread out, and grew in size.ConclusionThe gelatin-polysaccharide composite hydrogels could serve as attractive biomaterials for tissue engineering due to their easy preparation and favorable biophysical properties.

Project description:Biological materials combine stress relaxation and self-healing with non-linear stress-strain responses. These characteristic features are a direct result of hierarchical self-assembly, which often results in fiber-like architectures. Even though structural knowledge is rapidly increasing, it has remained a challenge to establish relationships between microscopic and macroscopic structure and function. Here, we focus on understanding how network topology determines the viscoelastic properties, i.e., stress relaxation, of biomimetic hydrogels. We have dynamically crosslinked two different synthetic polymers with one and the same crosslink. The first polymer, a polyisocyanopeptide (PIC), self-assembles into semi-flexible, fiber-like bundles, and thus displays stress-stiffening, similar to many biopolymer networks. The second polymer, 4-arm poly(ethylene glycol) (starPEG), serves as a reference network with well-characterized structural and viscoelastic properties. Using one and the same coiled coil crosslink allows us to decouple the effects of crosslink kinetics and network topology on the stress relaxation behavior of the resulting hydrogel networks. We show that the fiber-containing PIC network displays a relaxation time approximately two orders of magnitude slower than the starPEG network. This reveals that crosslink kinetics is not the only determinant for stress relaxation. Instead, we propose that the different network topologies determine the ability of elastically active network chains to relax stress. In the starPEG network, each elastically active chain contains exactly one crosslink. In the absence of entanglements, crosslink dissociation thus relaxes the entire chain. In contrast, each polymer is crosslinked to the fiber bundle in multiple positions in the PIC hydrogel. The dissociation of a single crosslink is thus not sufficient for chain relaxation. This suggests that tuning the number of crosslinks per elastically active chain in combination with crosslink kinetics is a powerful design principle for tuning stress relaxation in polymeric materials. The presence of a higher number of crosslinks per elastically active chain thus yields materials with a slow macroscopic relaxation time but fast dynamics at the microscopic level. Using this principle for the design of synthetic cell culture matrices will yield materials with excellent long-term stability combined with the ability to locally reorganize, thus facilitating cell motility, spreading, and growth.

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Viscoelastic properties and nanoscale structures of composite oligopeptide-polysaccharide hydrogels.

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Viscoelastic properties and nanoscale structures of composite oligopeptide-polysaccharide hydrogels.

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