Highly Efficient Interfacial Heat Conduction Enhanced by the Synergistic Effect of Irregularly Shaped Thermally Conductive Particle Assembly and Polar Network Adhesion

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Thermal interface materials have broad application prospects in the fields of thermal management and energy-efficient utilization of high-power chips. Developing thermal interface materials with both high thermal conductivity and high adhesion is of great significance for realizing their reliable heat transfer function. However, the unclear synergistic mechanism between thermally conductive materials and polymer networks in thermal interface materials makes it difficult to simultaneously regulate their thermal conductivity and adhesion. Here, we report a synergistic enhancement of interfacial thermal conduction through the assembly of irregularly shaped thermally conductive particles and the adhesion of polar networks. A thermally conductive network coassembled from spherical boron nitride and boron nitride sheets was designed, and an efficient thermally conductive network was constructed by optimizing the ratio and concentration. Dispersing a polymer network containing multiple polar sites within the thermal interface material promotes molecular-scale connections between the thermally conductive network, the polymer network, and the interface. The resulting TIM exhibits an effective thermal conductivity of 1.52 W·m–1·K–1 together with thermoresponsive mechanical and adhesive properties, enabling adaptive interfacial contact during thermal management. Integrated assembly in a photothermal conversion-thermal utilization device was successfully completed, enabling its application in the cold start of energy batteries. This work provides a feasible strategy for designing multifunctional thermoresponsive thermal interface materials for battery cold-start thermal management.