High‐temperature dielectric materials for capacitive energy storage are in urgent demand for modern power electronic and electrical systems. However, the drastically degraded energy storage capabilities owing to the inevitable conduction loss severely limit the utility of dielectric polymers at elevated temperatures. Herein, a new approach based on the in situ preparation of oxides onto polyimide (PI) films to high‐temperature laminated polymer dielectrics is described. As confirmed by computational simulations, the charge injection at the electrode/dielectric interface and electrical conduction in dielectric films are substantially depressed via engineering the in situ prepared oxide layer in the laminated composites. Consequently, ultrahigh dielectric energy densities and high efficiencies are simultaneously achieved at elevated temperatures. Especially, an excellent energy density of 1.59 J cm−3 at a charge–discharge efficiency of above 90% has been achieved at 200 °C, outperforming the current dielectric polymers and composites. Together with its excellent discharging capability and cyclic reliability, the laminate‐structured film is demonstrated to be a promising class of polymer dielectrics for high‐power energy storage capacitors operating at elevated temperatures. The facile preparation method reported herein is readily adaptable to a variety of polymer thin films for energy applications under extreme environments.

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We report enhancement of the dielectric permittivity of poly(vinylidene fluoride) (PVDF) generated by depositing magnetic iron oxide (Fe3O4) nanoparticles on the surface of barium titanate (BT) to fabricate BT–Fe3O4/PVDF composites. This process introduced an external magnetic field and the influences of external magnetic field on dielectric properties of composites were investigated systematically. The composites subjected to magnetic field treatment for 30 min at 60 °C exhibited the largest dielectric permittivity (385 at 100 Hz) when the BT–Fe3O4 concentration is approximately 33 vol.%. The BT–Fe3O4 suppressed the formation of a conducting path in the composite and induced low dielectric loss (0.3) and low conductivity (4.12 × 10−9 S/cm) in the composite. Series-parallel model suggested that the enhanced dielectric permittivity of BT–Fe3O4/PVDF composites should arise from the ultrahigh permittivity of BT–Fe3O4 hybrid particles. However, the experimental results of the BT–Fe3O4/PVDF composites treated by magnetic field agree with percolation theory, which indicates that the enhanced dielectric properties of the BT–Fe3O4/PVDF composites originate from the interfacial polarization induced by the external magnetic field. This work provides a simple and effective way for preparing nanocomposites with enhanced dielectric properties for use in the electronics industry.

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Iron Oxide (Fe3O4) nanoparticles were deposited on the surface of low density polyethylene (LDPE) particles by solvothermal method. A magnetic field was introduced to the preparation of Fe3O4/LDPE composites, and the influences of the magnetic field on thermal conductivity and dielectric properties of composites were investigated systematically. The Fe3O4/LDPE composites treated by a vertical direction magnetic field exhibited a high thermal conductivity and a large dielectric constant at low filler loading. The enhancement of thermal conductivity and dielectric constant is attributed to the formation of the conductive chains of Fe3O4 in LDPE matrix under the action of the magnetic field, which can effectively enhance the heat flux and interfacial polarization of the Fe3O4/LDPE composites. Moreover, the relatively low dielectric loss and low conductivity achieved are attributed to the low volume fraction of fillers and excellent compatibility between Fe3O4 and LDPE. Of particular note is the dielectric properties of Fe3O4/LDPE composites induced by the magnetic field also retain good stability across a wide temperature range, and this contributes to the stability and lifespan of polymer capacitors. All the above-mentioned properties along with the simplicity and scalability of the preparation for the polymer nanocomposites make them promising for the electronics industry.

Polymer film capacitors have been widely used in electronics and electrical power systems due to their advantages of high power densities, fast charge–discharge speed, and great stability. However, the exponential increase of electrical conduction with temperature and applied electric field substantially degrades the capacitive performance of dielectric polymers at elevated temperatures. Here, the first example of controlling the energy level of charge traps in all‐organic crosslinked polymers by tailoring molecular structures that significantly inhibit high‐field high‐temperature conduction loss, which largely differs from current approaches based on the introduction of inorganic fillers, is reported. The polymer network with optimized crosslinking structures exhibits an ultrahigh discharged energy density of 7.02 J cm−3 with charge/discharge efficiencies of >90% at 150 °C, far outperforming current dielectric polymers and composites. The charge‐trapping effects in different crosslinked structures, as the origins of the marked improvements in the high‐temperature capacitive performance, are comprehensively investigated experimentally and confirmed computationally. Moreover, excellent cyclability and self‐healing features are demonstrated in the polymer film capacitors. This work offers a promising pathway of molecular structure design to scalable high‐energy‐density polymer dielectrics capable of operating under harsh environments.

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