Abstract
Ionogels have garnered great attention as promising soft conducting materials for the fabrication of flexible energy storage devices, soft actuators, and ionotronics. However, the leakage of the ionic liquids, weak mechanical strength, and poor manufacturability have greatly limited their reliability and applications. Here, we propose a new ionogel synthesis strategy by utilizing granular zwitterionic microparticles to stabilize ionic liquids. The ionic liquids swell the microparticles and physically crosslink microparticles via either electronic interaction or hydrogen bonding. Further introducing a photocurable acrylic monomer enables the fabrication of double-network (DN) ionogels with high stretchability (>600%) and ultrahigh toughness (fracture energy > 10 kJ/m2). The synthesized ionogels exhibit a wide working temperature of -60 to 90 °C. By tuning the crosslinking density of microparticles and physical crosslinking strength of ionogels, we synthesize DN ionogel inks and print them into three-dimensional (3D) motifs. Several ionogel-based ionotronics are 3D printed as demonstrations, including strain gauges, humidity sensors, and ionic skins made of capacitive touch sensor arrays. Via covalently linking ionogels with silicone elastomers, we integrate the ionogel sensors onto pneumatic soft actuators and demonstrate their capacities in sensing large deformation. As our last demonstration, multimaterial direct ink writing is harnessed to fabricate highly stretchable and durable alternating-current electroluminescent devices with arbitrary structures. Our printable granular ionogel ink represents a versatile platform for the future manufacturing of ionotronics.