Tough and Elastic Cellulose Composite Hydrogels/Films for Flexible Wearable Sensors

Cellulose and its composites, despite being abundant and sustainable, are typically brittle with very low flexibility/stretchability. This study reports a solution processing method to prepare porous, amorphous, and elastic cellulose hydrogels and films. Native cellulose dissolved in a water-ZnCl₂ mixture can form ionic gels through in situ polymerization of acrylic acid (AA) to poly(acrylic acid) (PAA). The addition of up to 30 vol % AA does not change the solubility of cellulose in the water-ZnCl₂ mixture. After polymerization, the formation of interpenetrated networks, resulting from the chemical cross-linking of PAA and the ionic/coordination binding among cellulose/PAA and ZnCl₂, gives rise to strong, transparent, and ionically conductive hydrogels. These hydrogels can be used for wearable sensors to detect mechanical deformation under stretching, compression, and bending. Upon removal of ZnCl₂ and drying the gels, semitransparent amorphous cellulose composite films can be obtained with a Young's modulus of up to 4 GPa. The rehydration of these films leads to the formation of tough, highly elastic composites. With a water content of 3-10.5%, cellulose-containing films as strong as paper also show typical characteristics of elastomers with an elongation of up to 1300%. Such composite films provide an alternative solution to resolving the material sustainability of natural polymers without compromising their mechanical properties.