Thermal Conductivity Enhancement of Soft Polymer Composites through Magnetically Induced Percolation and Particle–Particle Contact Engineering

Abstract Despite major advancements in the performance of thermal interface materials (TIMs), contact resistance between components persists as a major thermal bottleneck in electronics packaging. In this work, the thermal performance of composite TIMs is enhanced through a synergistic coupling of magnetic alignment and engineered particle coatings that reduce the thermal resistance between particles. By itself, magnetically induced percolation of nickel particles within a cross‐linked silicone matrix doubles the thermal conductivity of the composite. This process significantly increases contact between particles, making the interfacial particle–particle resistance a major contributor to the composites thermal performance. The resistance at these interfaces can be reduced by introducing soft metal (silver) or liquid metal coatings onto the nickel particles. Compressing powder beds of these hybrid particles reveals that, dependent on coating thickness, the contact engineering approach provides multifold increases in thermal conductivity at mild pressures. When dispersed in a polymer matrix and magnetically aligned, the coated particles provide a threefold increase in composite thermal conductivity, as compared to unaligned samples (up to nearly 6 W m−1 K−1 with volumetric fill fraction of 0.5). For equivalent coating thicknesses, silver coatings achieve better performance than liquid metal coatings.