Using bacterial cellulose to bridge covalent and physical crosslinks in hydrogels for fabricating multimodal sensors

Network optimization is vital for the polysaccharide based hydrogels with multiple crosslinks. In this study, we developed a 'two-step' strategy to activate synergistic effect of chemical and physical crosslinks using a poly (vinyl alcohol) (PVA)/bacterial cellulose (BC) hydrogel as a template. The BC nanofibers, on the one hand, acted as nucleating agents, participating in the crystallization of PVA, and on the other hand, were also involved in the formation of boronic ester bond, anchored with the PVA chains via chemical bonding. Therefore, the existence of BC nanofibers, as 'bridge', linked the crystalline regions and amorphous parts of PVA together, associating the two characteristic crosslinks, which was conducive to load transfer. The mechanical properties of resultant hydrogels, including the tensile elongation and strength, as well as fracture toughness, were significantly improved. Moreover, the dually cross-linked hydrogels possessed ionic conductivity, which was sensitive to the tensile deformation and environmental temperature. This study clarifies a unique role of BC nanofibers in hydrogels, and proposes an effective approach to construct multiple networks in the nanocellulose reinforced PVA hydrogels.