Highly Interconnected Thermal Conduction Highway for Highly Thermally Conductive and Mechanically Strong Polymeric Composites

Industrial implementation of highly thermally conductive polymeric composites has been hindered by several hurdles, such as the low intrinsic thermal conductivity (TC) of polymers, the use of expensive thermally conductive fillers, and difficulty in processing composites with high filler loading. In this study, we introduce a straightforward fabrication method for a high TC polymeric composite with a programmed internal structure of a highly interconnected thermal conduction highway (HITCH) by the simple addition of partially cured resin fragments into the conventional filler/resin combination. Critical variables, such as the concentration of the added resin fragments and the local concentration of hexagonal boron nitride (hBN) in the HITCH, as well as the packing density of the fragments, were systematically tuned to maximize the TC with the use of the least amount of the filler. Careful choice of the compositions enabled a significant TC enhancement of the composite by 2.6 times (6.5 W/mK) compared to the value of the conventional composite at the same overall concentration of hBN (∼2.5 W/mK). Finally, a composite with high TC (∼12 W/mK) and strong tensile strength (∼22.6 MPa), which is good enough for most practical thermal management applications, could be successfully fabricated with the use of the least amount of the filler (∼34 wt %). The comprehensive study of the HITCH composite here can be easily extended to other combinations with various fillers and matrices and may provide a library to researchers looking for advanced materials for future thermal management systems.