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Quantitative Grafting for Structure-Function Establishment: Thermoresponsive Poly(alkylene oxide) Graft Copolymers Based on Hyaluronic Acid and Carboxymethylcellulose

Journal article
Authors Markus Andersson Trojer
Mats Andersson
Johan Bergenholtz
Paul Gatenholm
Published in Biomacromolecules
Volume 20
Issue 3
Pages 1271-1280
ISSN 1525-7797
Publication year 2019
Published at Department of Chemistry and Molecular Biology
Pages 1271-1280
Language en
Links doi.org/10.1021/acs.biomac.8b01692
Subject categories Polymer Chemistry, Materials Chemistry, Surface and colloid chemistry

Abstract

© 2019 American Chemical Society. A series of thermoresponsive graft copolymers, gelling at physiological conditions in aqueous solution and cell growth media, have been synthesized using quantitative coupling between a small set of amino-functionalized poly(alkylene oxide) copolymers (PAO) and the carboxylate of the biologically important polysaccharides (PSa) carboxymethylcellulose and the less reactive hyaluronate. Quantitative grafting enables the establishment of structure-function relationship which is imperative for controlling the properties of in situ gelling hydrogels. The EDC/NHS-mediated reaction was monitored using SEC-MALLS, which revealed that all PAOs were grafted onto the PSa backbone. Aqueous solutions of the graft copolymers were Newtonian fluids at room temperatures and formed reversible physical gels at elevated temperatures which were noncytotoxic toward chondrocytes. The established structure-function relationship was most clearly demonstrated by inspecting the thermogelling strength and the onset of thermogelling in a phase diagram. The onset of the thermogelling function could be controlled by the global PAO concentration, independent of graft ratio.

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