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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 × 10⁴S 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. 

Abstract 4D printing is an emerging field where 3D printing techniques are used to pattern stimuli‐responsive materials to create morphing structures, with time serving as the fourth dimension. However, current materials utilized for 4D printing are typically soft, exhibiting an elastic modulus (E) range of 10⁻⁴to 10 MPa during shape change. This restricts the scalability, actuation stress, and load‐bearing capabilities of the resulting structures. To overcome these limitations, multiscale heterogeneous polymer composites are introduced as a novel category of stiff, thermally responsive 4D printed materials. These inks exhibit anEthat is four orders of magnitude greater than that of existing 4D printed materials and offer tunable electrical conductivities for simultaneous Joule heating actuation and self‐sensing capabilities. Utilizing electrically controllable bilayers as building blocks, a flat geometry is designed and printed that morphs into a 3D self‐standing lifting robot, setting new records for weight‐normalized load lifted and actuation stress when compared to other 3D printed actuators. Furthermore, the ink palette is employed to create and print planar lattice structures that transform into various self‐supporting complex 3D shapes. These contributions are integrated into a 4D printed electrically controlled multigait crawling robotic lattice structure that can carry 144 times its own weight. 

A strain-induced electrically conductive liquid metal emulsion for the programmable assembly of soft conductive composites is reported. This emulsion exhibits the shear yielding and shear thinning rheology required for direct ink writing. Examples of complex self-supported 3D printed structures with spanning features are presented to demonstrate the 3D printability of this emulsion. Stretchable liquid metal composites are fabricated by integrating this emulsion into a multi-material printing process with a 3D printable elastomer. The as-printed composites exhibit a low electrical conductivity but can be transformed into highly conductive composites by a single axial strain at low stresses ([Formula: see text] 0.3 MPa), an order of magnitude lower than other mechanical sintering approaches. The effects of axial strain and cyclic loading on the electrical conductivities of these composites are characterized. The electrical conductivity increases with activation strain, with a maximum observed relaxed conductivity of 8.61 × 10⁵S⋅m⁻¹, more than 300% higher than other mechanical sintering approaches. The electrical conductivity of these composites reaches a steady state for each strain after one cycle, remaining stable with low variation ([Formula: see text] standard deviation) over 1000 cycles. The strain sensitivities of these composites are quantitatively analyzed. All samples exhibit strain sensitivities that are lower than a bulk conductor throughout all strains. The printed composites showed low hysteresis at high strains, and high hysteresis at low strains, which may be influenced by the emulsion internal structure. The utility of these composites is shown by employing them as wiring into a single fabrication process for a stretchable array of LEDs.