Highly compressible and environmentally adaptive conductors with high-tortuosity interconnected cellular architecture

Abstract Conductive hydrogels that are highly elastic, fatigue resistant and environmentally adaptive are promising materials in the fields of wearable electronics, bioelectronics and soft robotics. However, these materials are challenging to develop, especially for use in harsh environments including organic solvents and extreme temperatures. Here we report a simple method for the fabrication of highly compressible and fatigue-resistant conductive hydrogels with reinforced-concrete-type constituents and high-tortuosity interconnected cellular architecture through a self-assembly and two-stage in situ polymerization process. The obtained composites exhibit excellent mechanical compressibility with negligible residual strain at 50% strain for >10 4 cyclic loadings both in air and water. Due to the structure-favoured anisotropic response to tensile deformations coupled with elastic recovery, the hydrogel is endowed with sensing dimensions which allow the direction and velocity of movement on the sensor surface to be distinguished. In addition, by interpenetrating with an oleophilic polymer network, highly elastic and adaptive organohydrogels are developed with outstanding sensing performance in a wide variety of organic solvents and cryogenic temperatures. These materials may therefore be suitable for use in flexible and wearable devices in harsh environments.