Viscoelastic Metal-in-Water Emulsion Gel via Host–Guest Bridging for Printed and Strain-Activated Stretchable Electrodes

Stretchable conductive electrodes that can be made by printing technology with high resolution is desired for preparing wearable electronics. Printable inks composed of liquid metals are ideal candidates for these applications, but their practical applications are limited by their low stability, poor printability, and low conductivity. Here, thixotropic metal-in-water (M/W) emulsion gels (MWEGs) were designed and developed by stabilizing and bridging liquid metal droplets (LMDs) via a host-guest polymer. In the MWEGs, the hydrophilic main chain of the host-guest polymers emulsified and stabilized LMDs via coordination bonds. The grafted cyclodextrin and adamantane groups formed dynamic inclusion complexes to bridge two neighboring LMDs, leading to the formation of a dynamically cross-linked network of LMDs in the aqueous phase. The MWEGs exhibited viscoelastic and shear-thinning behavior, making them ideal for direct three-dimensional (3D) and screen printing with a high resolution (∼65 μm) to assemble complex patterns consisting of ∼95 wt % liquid metal. When stretching the printed patterns, strong host-guest interactions guaranteed that the entire droplet network was cross-linked, while the brittle oxide shell of the droplets ruptured, releasing the liquid metal core and allowing it to fuse into continuous conductive pathways under an ultralow critical strain (<1.5%). This strain-activated conductivity exceeded 15800 S/cm under a large strain of 800% and exhibited long-term cyclic stability and robustness.