Versatile and recyclable double-network PVA/cellulose hydrogels for strain sensors and triboelectric nanogenerators under harsh conditions

Versatile and recyclable conductive hydrogels with long-term environmental adaptability and mechanical stability have attracted tremendous attention in wearable smart electronics. Here, double-network (DN) polyvinyl alcohol (PVA)/cellulose hydrogels were constructed after introducing a conductive rigid cellulose/Zn2+/Ca2+ network into a soft PVA/borax network. The resultant hydrogels possessed good mechanical and self-adhesive properties, along with transparency, recyclability, and remarkable resistance to freezing. They showed 30-day non-drying properties due to the presence of hygroscopic salts through a dynamic moisture adsorption and desorption process. Dehydrated hydrogels can return to their original states via self-regeneration under high relative humidity. Hydrogel-based strain sensors retained good sensitivity and a wide sensing range during the wide working temperature ranging from -40 °C to 50 °C and after recycling. Additionally, conductive hydrogels were integrated into triboelectric nanogenerators (TENGs) functioning as energy harvesters for powering electronics. TENGs retained stable electrical outputs even under harsh conditions and after recycling. Hydrogels were also assembled into flexible self-powered biomechanical sensors and tactile sensors. Thermally reversible interactions in composite hydrogels enabled their good recyclability, thereby reducing economic costs and environmental impacts caused by e-wastes. This work demonstrates the great potential of versatile and recyclable hydrogels with good environmental and mechanical stability in wearable smart electronics under harsh conditions.