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In this study, thermally conductive composite films were fabricated using an anisotropic boron nitride (BN) and hybrid filler system mixed with spherical aluminum nitride (AlN) or aluminum oxide (Al₂O₃) particles in a polyimide matrix. The hybrid system yielded a decrease in the through-plane thermal conductivity, however an increase in the in-plane thermal conductivity of the BN composite, resulting from the horizontal alignment and anisotropy of BN. The behavior of the in-plane thermal conductivity was theoretically treated using the Lewis⁻Nielsen and modified Lewis⁻Nielsen theoretical prediction models. A single-filler system using BN exhibited a relatively good fit with the theoretical model. Moreover, a hybrid system was developed based on two-population approaches, the additive and multiplicative. This development represented the first ever implementation of two different ceramic conducting fillers. The multiplicative-approach model yielded overestimated thermal conductivity values, whereas the additive approach exhibited better agreement for the prediction of the thermal conductivity of a binary-filler system.

Synergistic Effects of Various Ceramic Fillers on Thermally Conductive Polyimide Composite Films and Their Model Predictions