Triple crosslinking conductive hydrogels with digitally printable and outstanding mechanical stability for high-resolution conformable bioelectronics

Abstract

Soft, conductive, and stretchable hydrogels offer a broad variety of applications, including skin-interfacing electrodes, biomonitoring patches, and electrostimulation. Despite rapid developments over the last decades, a combination of good electrical and mechanical properties, low-cost fabrication, and biocompatibility is yet to be demonstrated. Also, the current methods for deposition and patterning of these hydrogels are manual, and there is a need toward autonomous and digital fabrication techniques. In this work, we demonstrate a novel Gallium (Ga) embedded sodium–alginate–polyacrylamide–LAPONITE® (Ga–SA–PAAM–La) hydrogel, that is ultra-stretchable (Maximum strain tolerance of∼985%), tough (toughness ∼30 kJ m⁻³), bio-adhesive (adhesion energy ∼216 J m⁻²), conductive, and digitally printable. Ga nanoparticles are used as radical initiators. By adjusting the sonication parameters, we control the solution viscosity and curing time, thus allowing us to prepare pre-polymers with the desired properties for casting, or digital printing. These hydrogels benefit from a triple-network structure due to the role of Ga droplets as crosslinkers besides BIS (N,N′-methylene-bis-acrylamide) and LAPONITE®, thus resulting in tough composite hydrogels. The inclusion of LAPONITE® into the hydrogel network improved its electrical conductivity, adhesion, digital printability, and its mechanical properties, (>6× compared to the same hydrogel without LAPONITE®). As electrodes in the electrocardiogram, the signal-to-noise ratio was surprisingly higher than the medical-grade Ag/AgCl electrodes, which are applied for monitoring muscles, heart, respiration, and body joint angle through EMG, ECG, and bioimpedance measurements. The results obtained prove that such digitally printed conductive and tough hydrogels can be used as potential electrodes and sensors in practical applications in the next generation of printed wearable computing devices.