Structurally diverse and readily tunable photocrosslinked chondroitin sulfate based copolymers

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Abstract

ABSTRACT Our group has previously reported on successful biofunctionalization of poly(ethylene glycol diacrylate) (PEGDA) gels using chondroitin sulfate (CS) and improving moduli of methacrylated‐CS (MCS) gels using short PEGDA comonomers. Here, we focused on understanding the composition‐property relationship of MCS‐PEGDA copolymers. By changing concentration, composition, and medium's ionic strength the gels were modified to show a diverse range of properties. Photopolymerized copolymers with >4:1 ratio of one component had compressive moduli of up to 24 times higher and up to 17 times lower swelling degree ( q ) than those of MCS alone. The increased moduli and lowered q were consistent with the hypothesis that PEGDA improves kinetic chain growth by overcoming the steric hindrances of the macromer. The swelling and moduli of the gels were tuned by changing the ratio of the comonomers. The swelling and moduli of the gels were lowered with presence of salt in solution while the fracture strain increased. These changes were hypothesized to be the result of transition of CS chain conformation from highly extended and non‐Gaussian to less extended and Gaussian distribution. The complete understanding of MCS‐PEGDA composition–property relationship provides a general strategy to tune the moduli or q of polysaccharide‐based hydrogels while avoiding undesirable phase separation. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2015 , 53 , 1070–1079

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