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Material extrusion (MEX) of soft, multifunctional composites consisting of liquid metal (LM) droplets can enable highly tailored properties for a range of applications from soft robotics to stretchable electronics. However, an understanding of how LM ink rheology and print process parameters can reconfigure LM droplet shape during MEX processing for in-situ control of properties and function is currently limited. Herein, the material (ink viscosity, and LM droplet size) and process (nozzle velocity, height from print bed, and extrusion rate) parameters are determined which control LM microstructure during MEX of these composites. The interplay and interdependence of these parameters is evaluated and nearly spherical LM droplets are transformed into highly elongated ellipsoidal shapes with an average aspect ratio of 12.4 by systematically tuning each individual parameter. Material and process relationships are established for the LM ink which show that an ink viscosity threshold should be fulfilled to program the LM microstructure from spherical to an ellipsoidal shape during MEX. Additionally, the thin oxide layer on the LM droplets is found to play a unique and critical role in the reconfiguration and retention of droplet shape. Finally, two quantitative design maps based on material and process parameters are presented to guide MEX additive manufacturing strategies for tuning liquid droplet architecture in LM-polymer inks. The insights gained from this study enable informed design of materials and manufacturing to control microstructure of emerging multifunctional soft composites. 

Abstract Thermal management in electric vehicles, electronics, and robotics requires the systematic ability to dissipate and direct the flow of heat. Thermally conductive soft composites are promising for thermal management due to their high thermal conductivity and mechanical flexibility. However, composites typically have the same microstructure throughout a film, which limits directional and spatial control of thermal management in emerging systems that have distributed heat loads. Herein, directional and spatially tunable thermal properties are programmed into liquid metal (LM) soft composites through a direct ink writing (DIW) process. Through the local control of LM droplet aspect ratio and orientation this programmable LM microstructure has a thermal conductivity in the direction of LM elongation of 9.9 W m⁻¹·K⁻¹, which is ∼40 times higher than the unfilled elastomer (0.24 W m⁻¹·K⁻¹). The DIW process enables LM droplets to be oriented in specific directions with tunable aspect ratios at different locations throughout a continuous film. This introduces anisotropic and heterogeneous thermal conductivity in compliant films to control the direction and magnitude of heat transfer. This methodology and resulting materials can provide designed thermal management solutions for rigid and soft devices.