Due to its high thermal conductivity (TC) and low electrical conductivity, boron nitride (BN) has emerged as an ideal filler for thermal interface materials (TIMs) that prevent thermal accumulation in nanostructures without causing shutdown via elect...
Due to its high thermal conductivity (TC) and low electrical conductivity, boron nitride (BN) has emerged as an ideal filler for thermal interface materials (TIMs) that prevent thermal accumulation in nanostructures without causing shutdown via electron tunneling. The polymer composite based on the BN hybrid strategy can be considered an optimal option for electrically insulating and heat-dissipating TIM. However, there is a paucity of systematic experiments and theoretical approaches investigating the optimal content and ratio of BN hybrid fillers, which are key factors in synergistically enhancing TC. In this study, we develop a hybrid thermal percolation model by modifying the Foygel model to investigate the synergistic improvement of systematically measured TC. The model effectively determines the optimal hybrid filler composition and the resultant performance enhancement. Furthermore, the effects of BN surface and interfacial chemistry are comprehensively analyzed in relation to the filler network structure. The highest isotropic TC (10.93 W/m·K) is achieved by optimizing the formation of nano-interconnections between one-dimensional BN nanotube (BNNT) and two-dimensional hexagonal BN (h-BN), corresponding to increases of 1582% and 118% compared with pure epoxy and the composite containing the optimized h-BN network, respectively.