Riboflavin mediated UV crosslinking of chitosan-gelatin cryogels for loading of hydrophobic bioactive compounds

Abstract

Chitosan-gelatin cryogels with good loading capacity of hydrophobic compounds were successfully obtained by UV-induced crosslinking. Using riboflavin as photoinitiator was a suitable alternative to classical carbodiimide crosslinking in obtaining carrier matrices for bioactive hydrophobic compounds. Chitosan had a double role, acting both as a base polymer for the hydrogel network and as co-initiator in riboflavin photo-crosslinking. This co-initiator role of chitosan is due to its electron donor capacity, being well known as a Lewis base type macromolecule. The rheological behaviour of the chitosan-gelatin hydrogel precursor solutions was greatly influenced by riboflavin addition as well as by UV irradiation. As a consequence, the temperature of the sol-gel transition during cooling decreased to 25.5 °C. Compared with classical carbodiimide crosslinking, UV irradiation lead to gels with increased network stability, enhanced elastic behaviour, higher structural strength and almost total stress recovery yield (99 %), the latter indicating self-healing capacity. The cryogels manifested pH responsive swelling, this being highest at close to neutral pH of 7.4. Although hydrophilic in nature, the chitosan-gelatin cryogels crosslinked under the combined effect of riboflavin and UV exposure possess the necessary chemical functionality and morphology that allowed successful embedding of hydrophobic clove essential oil. This was loaded by immersion or fumigation and imparted antioxidant activity to the polymeric matrix.