Progress in the fields of wearable computing, soft robotics and bio hybrid engineering depend on new classes of soft multifunctional materials that match the mechanical properties of soft biological tissue and possess high toughness, while having metal-like electrical and thermal properties.

<p dir="ltr">Increasing power density and power consumption in electronic devices require heat dissipating components with high thermal conductivity to prevent overheating and improve performance and reliability. Polymers offer the advantages of low cost and weight over conventional metallic components, but their intrinsic thermal conductivity is low. Previous studies have shown that the thermal conductivity of polymers can be enhanced by aligning the polymer chains or by adding high thermal conductivity fillers to create percolation paths within the polymeric matrix. To further enhance the in-plane thermal conductivity, the conductive fillers can be aligned preferentially, but this leads to a lower increase in performance in the cross-plane direction. Yet, the cross-plane thermal conductivity plays a vital role in dissipating heat from active devices and transmitting it to the surrounding environment. Alternatively, when the fillers are aligned to enhance cross-plane thermal transport, the enhancement in the in-plane direction is limited. There is a need to develop polymer composites with an approximately isotropic increase in thermal performance compared to their neat counterparts.</p><p dir="ltr">To achieve this goal, in this study, I combine conductive fibers and fillers to enhance thermal conductivity of polymers without significantly inducing thermal anisotropy while preserving the mechanical performance of the matrix. I employ three approaches to enhance the thermal conductivity () of thermoset polymeric matrices. In the first approach, I fabricate thermally conductive polymer composites by creating an emulsion consisting of eutectic gallium indium alloy (EGaIn) liquid metal in the uncured polydimethylsiloxane (PDMS) matrix. In the second approach, I infiltrate mats formed from chopped fibers of Ultra High Molecular Weight Polyethylene (UHMWPE) with an uncured epoxy resin. Finally, the third approach combines the two previous methods by infiltrating the UHMWPE fiber mat with an emulsion of the liquid metal and uncured epoxy matrix.</p><p dir="ltr">To evaluate the thermal performance of the composites, I use infrared thermal microscopy with two different experimental setups, enabling independent measurement of in-plane and cross-plane thermal conductivity. The results demonstrate that incorporating thermally conductive fillers enhances the overall conductivity of the polymer composite. Moreover, I demonstrate that the network structure achieved by the fiber mat, in combination with the presence of liquid metal, promotes a more uniform increase in the thermal conductivity of the composite in all directions. Additionally, I assess the impact of filler incorporation and filler concentration on matrix performance through tension, indentation, and bending tests for mechanical characterization of my materials.</p><p dir="ltr">This work demonstrates the potential of strategic composite design to achieve polymeric materials with isotropically high thermal conductivity. These new materials offer a solution to the challenges posed by higher power density and consumption in electronics and providing improved heat dissipation capabilities for more reliable devices.</p>