It remains a challenge to develop highly polymer-based nanocomposite thermal interface materials, which can effectively remove heat developed during the miniaturization of electronic instruments. It has been reported that a large number of graphene-based nanocomposites exhibit excellent performance. However, it is still an issue to construct thermal conductive pathways by orientation arrangements with a low filler volume fraction. Herein, a high-thermal conductivity filler of magnetic carbon nanotube-grafted graphene polyhedra (Co@Co3O4-G) was exploited via the annealing of metal-organic frameworks (ZIF-67). Co@Co3O4-G can improve the thermal conductivity of nanocomposites obviously by forming oriented pathways for phonon transport in an external magnetic field. Therefore, the resulting nanocomposite displayed a high thermal conductivity of 2.11 W m-1 K-1 for only 8.7 vol%, which is 10 times higher than that of the pure epoxy resin. Core-shell magnetic cobalt oxide (Co@Co3O4) was encapsulated in situ in the nanoarchitecture to avoid falling off. Moreover, the equilibrium molecular dynamics (EMD) simulation verifies that Co@Co3O4-G had high thermal conductivity to effectively improve the heat dissipation of nanocomposites. This strategy provides an approach for developing high-performance thermal management materials and opens up the possibility for the pioneering applications of encapsulated magnetic-oriented thermal conductive fillers.
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