Self‐Catalyzed Chemically Coalescing Liquid Metal Emulsions

Abstract Gallium‐based liquid metal alloys (GaLMAs) have widespread applications ranging from soft electronics, energy devices, and catalysis. GaLMAs can be transformed into liquid metal emulsions (LMEs) to modify their rheology for facile patterning, processing, and material integration for GaLMA‐based device fabrication. One drawback of using LMEs is reduced electrical conductivity owing to the oxides that form on the surface of dispersed liquid metal droplets. LMEs thus need to be activated by coalescing liquid metal droplets into an electrically conductive network, which usually involves techniques that subject the LME to harsh conditions. This study presents a way to coalesce these droplets through a chemical reaction at mild temperatures ( T ∼ 80 °C). Chemical activation is enabled by adding halide compounds into the emulsion that chemically etch the oxide skin on the surface of dispersed droplets of eutectic gallium indium (eGaIn). LMEs synthesized with halide activators can achieve electrical conductivities close to bulk liquid metal (2.4 × 10 4 S cm −1 ) after being heated. 3D printable chemically coalescing LME ink formulations are optimized by systematically exploring halide activator type and concentration, along with mixing conditions, while maximizing for electrical conductivity, shape retention, and compatibility with direct ink writing (DIW). The utility of this ink is demonstrated in a hybrid 3D printing process to create a battery‐integrated light emitting diode array, followed by a nondestructive low temperature heat activation that produces a functional device.