Tough Adhesion of Freezing- and Drying-Tolerant Transparent Nanocomposite Organohydrogels

Tough hydrogels with strong wet adhesion have drawn extensive attention for various applications. However, it is still challenging to achieve both excellent wet adhesion and freezing- and drying-tolerance in hydrogels. In this study, we present tough transparent nanocomposite organohydrogels based on the glycerol–water binary solvent system in the presence of Al(OH)3 nanoparticles as a cross-linker. The resultant organohydrogels exhibited excellent tensile strength (∼0.9 MPa), high transparency (97%), superior anti-drying and anti-freezing properties, and good ionic conductivity. In particular, polyacrylic acid (PAA) was chosen as the bridging polymer to endow the organohydrogels with strong wet adhesion. The interfacial adhesion energy exceeded 2200 J m–2, which was ascribed to the synergy of ionic coordination and hydrogen bonds between the nanoparticles and carboxyl groups in PAA chains. Interestingly, based on the strong wet adhesion, the transparent organohydrogels can be assembled into hydraulically driven soft variable-focus lenses with long-term ambient stability. This work will provide a new insight into controlled wet adhesion ̵of hydrogel and have great potential for hydrogel-based functional devices with long-term ambient stability.