Charged glycopolymers are natural components of biological tissue, abundant in the mammalian extracellular matrix and provide the mechanical support and biological interaction for cell migration and morphogenetic activities. Chondroitin sulfate (CS) and hyaluronic acid (HA) are the two major anionic glycosaminoglycans (GAG) present in connective tissue which have been used as biocompatible precursors to synthesize 3D matrices for cartilage regeneration purposes. Due to polyelectrolyte nature of these scaffolds, however, retaining the mechanical integrity of GAG based hydrogels has been a challenge. Copolymerization of functionalized GAGs with oligo(ethylene glycol) acrylate was the approach used in this study to improve the moduli of the crosslinked gels. The moduli of copolymers were 2 to 25 times higher than the parent homopolymer (depending on the GAG and comonomer type). Longer oligomers of ethylene glycol (up to 700Da) as well as higher ratios of functionalized groups on the host glycopolymer, and differences in reactivity ratios of the macromer and comonomer effectively increased the moduli and crosslink density of the gels. Improved structures were observed in copolymerization of both CS and HA functionalized GAGs which suggested independence of the reaction mechanism from the host glycopolymer. Figure1 � Suggested reaction mechanism for copolymerization of acrylate and methacrylate comonomers with methcrylated GAG. Homogeneity (b) or heterogeneity (c) of the copolymers was attributed to differences or similarities in reactivity ratios of the functional groups. Right picture compares the transparent MCS-acrylate copolymer (b) versus the translucent MCS-methacrylate (c) copolymer.

Copolymerization: A humble approach to synthesize high strength glycosaminoglycan hydrogel scaffolds

247th National Meeting (2014)

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