Hyaluronic acid single-network hydrogel with high stretchable and elastic properties

Stretchable materials have demonstrated great interest in wearable or implantable applications. Most of the existing hydrogels with high stretchability characteristics are based on double networks, exhibit large hysteresis loops, and cannot recover after deformation due to permanent rupture of network. Elastic, biodegradable, and biocompatible hydrogels are desirable for wound dressing of joints with frequent motions or post-surgical healing of mobile tissues. Here, we show a simple strategy for the preparation of a hyaluronic acid (HA) single-network hydrogel that can be stretchable and highly elastic without the addition of other components/partners or complicated processes of preparation. Our strategy relies on the use of high Mw HA to create a chemical hydrogel in which densely entangled HA chains are tied together by a small number of covalent bonds. While the presence of covalent cross-links can prevent disintegration of the HA network, entanglements endow the hydrogel with high stretchability through transmission of tension along the length of the long HA chains. The stretching-relaxation cycles show negligible hysteresis and perfect recovery of material after the release of force. The diminution of Mw together with increasing the concentration or cross-linker amount leads to brittle hydrogels.