High-water-content mouldable polyvinyl alcohol-borax hydrogels reinforced by well-dispersed cellulose nanoparticles: Dynamic rheological properties and hydrogel formation mechanism

Cellulose nanoparticle (CNP) reinforced polyvinyl alcohol-borax (PB) hydrogels were produced via a facile approach in an aqueous system. The effects of particle size, aspect ratio, crystal structure, and surface charge of CNPs on the rheological properties of the composite hydrogels were investigated. The rheological measurements confirmed the incorporation of well-dispersed CNPs to PB system significantly enhanced the viscoelasticity and stiffness of hydrogels. The obtained free-standing, high elasticity and mouldable hydrogels exhibited self-recovery under continuous step strain and thermo-reversibility under temperature sweep. With the addition of cellulose I nanofibers, a 19-fold increase in the high-frequency plateau of storage modulus was obtained compared with that of the pure PB. CNPs acted as multifunctional crosslinking agents and nanofillers to physically and chemically bridge the 3D network hydrogel. The plausible mechanism for the multi-complexation between CNPs, polyvinyl alcohol and borax was proposed to understand the relationship between the 3D network and hydrogel properties.