Core-shell engineering of graphite nanosheets reinforced PVDF toward synchronously enhanced dielectric properties and thermal conductivity

Polymer composites integrating high dielectric permittivity (ε′) but low loss, large breakdown strength (Eb) and thermal conductivity (TC), have attracted widespread attention in electronic devices and power systems. To simultaneously achieve these properties in graphite nanosheet (GNS)/poly(vinylidene fluoride, PVDF), the GNS were first encapsulated by a layer of aluminum oxide (Al2O3), and then incorporated into PVDF, and the resulting PVDF nanocomposites' dielectric properties and TC were explored in terms of the Al2O3 shell thickness and filler loading. The insulating Al2O3 shell serves as a barrier layer for the formation of leakage current and long-distance electron migration thus resulting in much lower dielectric loss and conductivity of the GNS@Al2O3/PVDF. It effectively mitigates the dielectric mismatch between the filler and host matrix, further introduces more traps that can capture charge carriers, and increases the barrier height for electron detrapping subsequently preventing the growth of electric trees and elevating the Eb. Moreover, the Al2O3 interlayer alleviates both the phonon density state and phonon impedance mismatches between the filler and matrix and facilitates the interfacial phonon transport thus leading to improved TC. The dielectric parameters and TC of the GNS@Al2O3/PVDF can be simultaneously modulated by optimizing the Al2O3′s thickness. This work offers an effective approach for designing and fabricating the polymeric nanodielectrics concurrently integrating high ε′ but low loss, enhanced Eb, and TC for prospective applications in power equipment and microelectronic devices.