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High temperature polymer-based dielectric capacitors are crucial forapplication in electronic power systems. However, the storage performance ofconventional dielectrics polymer dramatically deteriorates due to the thermalbreakdown under concurrent high temperatures and electric fields, and there arehardly reports on the causes of thermal breakdown from the aspects of the hightemperature conduction loss and Joule heat dissipation. Herein, a combinedstrategy of crosslinking and compositing for polyimide-based nanocomposites isproposed, which minimizes the thermal breakdown by significantly inhibiting thehigh-temperature conduction loss and enhancing the high thermal conductivity.Furthermore, the rationale of the strategy was theoretically and experimentallyverified from multiple perspectives. The charge-trapping effect is directlyobserved and quantitatively probed by Kelvin probe force microscopy with nanolevel resolution, indicating that the crosslinking network introduces localdeep traps and effectively suppresses the charge transport. The thermalconductivity of the nanocomposites inhibits the high temperature thermalbreakdown, which is confirmed by phase field simulations. Consequently, theoptimized nanocomposites possess an ultra high discharge energy density(Ud) of5.45 J/cm3 and 3.54 J/cm3 with a charge discharge efficiency, respectively,which outperforms the reported polyimide based dielectric nanocomposites. Thiswork provides a scalable direction for high temperature polymer basedcapacitors with excellent performance.

Polyimides Crosslinked by Aromatic Molecules and Nanocomposites for High Temperature Capacitive Energy Storage