Dynamic Double-Networked Hydrogels by Hybridizing PVA and Herbal Polysaccharides: Improved Mechanical Properties and Selective Antibacterial Activity

Chinese herbal medicine has offered an enormous source for developing novel bio-soft materials. In this research, the natural polysaccharide isolated from the Chinese herbal medicine <i>Dendrobium</i> was employed as the secondary building block to fabricate a "hybrid" hydrogel with synthetic poly (vinyl alcohol) (PVA) polymers. Thanks to the presence of mannose units that contain cis-diol motifs on the chain of the <i>Dendrobium</i> polysaccharides, efficient crosslinking with the borax is allowed and reversible covalent borate ester bonds are formed. Eventually, highly dynamic and double-networked hydrogels were successfully prepared by the integration of <i>Dendrobium</i> polysaccharides and PVA. Interestingly, the introduction of polysaccharides has given rise to more robust and dynamic hydrogel networks, leading to enhanced thermal stability, mechanical strength, and tensile capacity (>1000%) as well as the rapid self-healing ability (<5 s) of the "hybrid" hydrogels compared with the PVA/borax single networked hydrogel. Moreover, the polysaccharides/PVA double network hydrogel showed selective antibacterial activity towards <i>S. aureus</i>. The reported polysaccharides/PVA double networked hydrogel would provide a scaffold to hybridize bioactive natural polysaccharides and synthetic polymers for developing robust but dynamic multiple networked hydrogels that are tailorable for biomedical applications.