Preparation of highly thermally conductive and electrically insulating PI/BNNSs nanocomposites by hot-pressing self-assembled PI/BNNSs microspheres

Traditional polymer-based thermally conductive composites with randomly distributed fillers always yield an undesired heat removal due to the lack of efficient heat transfer pathways. Thus, realization of rational and ordered distribution of thermally conductive nanofillers in polymer matrix is believed to be significant for obtaining a desirable thermal conductivity. Herein, a series of thermally conductive polyimide/boron nitride nanosheets (PI/BNNSs) composites with a highly ordered BNNSs network have been successfully prepared. For achieving an uniform dispersion and high orientation of BN nanosheets in PI matrix, self-assembled PI/BNNSs complex microspheres were firstly prepared via the van der Waals interaction, and then these complex microspheres were further hot-pressed at the Tg of PI matrix, which rendered the alignment of BNNSs during the deformation of complex microspheres and built an efficient heat transfer pathway. As a consequence, the resultant composites possess a much higher in-plane thermal conductivity up to 4.25 W/mK with 12.4 vol% oriented BNNSs than those of pure PI and random distribution composite (0.85 W/mK for pure PI and 1.3 W/mK for the PI/random BNNSs-12.4). Meanwhile, these nanocomposites present excellent electrically insulating properties, improved dimensional stabilities and good thermal stabilities. This facile method provides a new way to design and fabricate highly thermally conductive PI-based composites for applying in heat dissipation of modern portable and collapsible electronic devices.