Enhanced Loading Efficiency and Sustained Release of Doxorubicin from Hyaluronic Acid/Graphene Oxide Composite Hydrogels by a Mussel-Inspired Catecholamine

Hydrogels have been widely investigated as depots and carriers for drug delivery. For example, hydrogels have been successfully used to encapsulate a variety of pharmaceuticals, such as peptides and proteins. Recently, carbon material/hydrogel hybrid systems have been of interest as new hydrogel systems because of the attractiveness of structural reinforcement for biomedical applications. In particular, graphene and graphene oxide (GO) have been recognized as novel biomaterials with unique physical, electrical, and thermal properties. Among the various applications of these materials, many research groups are intensively exploring the biomedical applications of graphene and GO. In this study, we propose a new role for GO in hybrid hydrogels, with the inclusion of GO in the gel network resulting in a nearly 90% enhancement in the loading of small, hydrophobic drugs (e.g., doxorubicin, Dox) compared to the hydrogel without encapsulated GO. The hydrogels were prepared from hyaluronic acid (HA), with a mussel-inspired crosslinking chemistry used to prepare the HA hydrogels. Dox was then loaded into the hydrogels. The HA/GO composite hydrogel not only enhanced the loading amount but also exhibited long-lasting anticancer activity over 10 days. We believe that these graphene oxide-containing composite hydrogels can solve one of the challenges in the application of hydrogels by improving the loading efficiency of small-molecule drugs.