Ultra-high thermally conductive graphite microplatelet/aramid nanofiber composites with reduced interfacial thermal resistances by engineered interface π-π interactions.

Polymer-based thermally conductive composites with ultrahigh in-plane thermal conductivity are ideal candidates for heat dissipation applications in electronics. However, the complex interfaces between the functional filler and polymer matrix limit the significant increase in thermal conductivity of the polymer composites. In this study, we developed a one-pot strategy to prepare highly thermally conductive composite films of freeze-expansion large-size graphite microplatelets (F-GMPs) and aramid nanofibers (ANFs) with π-π interactions. The obtained F-GMP/ANF nanocomposite films present salient in-plane thermal conductivity, considerable flexibility, and outstanding long-term stability. The π-π interactions between the F-GMPs and ANFs promote the freeze-expansion exfoliation of graphite, yielding stable F-GMP/ANF precursor pastes with high-quality graphite platelets. Moreover, the π-π interactions improve the filler-matrix interfacial compatibility and reduce the interfacial thermal resistance, while the large-size F-GMP particles are directly lapped to construct a thermal transfer pathway with a reduction in the filler-filler interfacial thermal resistance. Consequently, the F-GMP/ANF composite films with 30 wt% F-GMPs exhibit unprecedentedly high in-plane thermal conductivity (56.89 W m^-1 K^-1) and corresponding thermal conductivity enhancement efficiency, presenting great application potential for the effective thermal management of highly integrated electronics.