Achieving high thermal conductivity in polymer composites with micro or nanoparticle fillers are challenging. Typically, over 50 vol% filler loading is necessary to form a thermal conductive network. However, even with such a network in place, the increase in thermal conductivity may not be significant compared to that in electrically conductive composites. To clarify the ideal filler network structure, we endeavored to selectively disperse nano-sized Al₂O₃ nanoparticles at the interface of co-continuous SEBS/PA6 blends, with and without various filler surface modification methods. A thermal conductive network forms when all interface areas are fully covered by 2.56 vol% of Al2O3 nanoparticles (very close to theoretical loading content 2.29 vol%). In this case, the Al2O3 nanoparticle has the highest thermal conductive contribution (TCC). However, the absolute TCC values are extremely low because of the interfacial thermal resistance and it will decrease when the filler content exceeds 2.56 vol%, indicating that some nanoparticles are dispersed separately out of the existed thermal conductive network. These findings suggest that the construction of a connected thermal conductive network, relatively lower interfacial thermal resistance and the precise positioning of fillers within this network are essential for achieving high thermal conductivity composites.
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