Multiply cross-linked poly(vinyl alcohol)/cellulose nanofiber composite ionic conductive hydrogels for strain sensors

Building multiple chemical crosslinks is an effective strategy to improve mechanical properties and to diversify final application of polysaccharide nanoparticles reinforced poly(vinyl alcohol) (PVA) physical hydrogels. In this work, PVA/cellulose nanofibers (CNFs) were used as composite substrate to fabricate ionic conductive hydrogels for strain sensor. Three types of characteristic crosslinks, including chemical crosslinking via boronic ester covalent bonds only, and with additional metal coordination bonding, as well as coexistence of physical crosslinks via PVA crystallites and aforementioned two kinds of chemical crosslinks, were constructed. The sample with triple crosslinks has superior mechanical strength and resistance to fatigue, and the polydopamine/Fe³⁺ ratio act as key to tune final performance because double-network structure prefers to form as Fe³⁺ is superfluous, while dual-crosslink one forms in the case of insufficient Fe³⁺. As-optimized ionic conductive hydrogel is suitable as strain sensor for probing human motions. This work provides an interesting insight into the network structure and property regulation for PVA/CNF composite hydrogels with multiple crosslinks.