Polymers are key dielectric materials for energy storage capacitors in advanced electronics and electric power systems due to their high breakdown strengths, low loss, great reliability, lightweight, and low cost. However, their electric and dielectric performance deteriorates at elevated temperatures, making them unable to meet the rising demand for harsh-environment electronics such as electric vehicles, renewable energy, and electrified transportation. Here, we present an all-polymer nanostructured dielectric material that achieves a discharged energy density of 7.1 J/cm³ with a charge-discharge efficiency of 90% at 150°C, outperforming the existing dielectric polymers and representing more than a twofold improvement in discharged energy density compared with polyetherimide. The self-assembled nano-scale multiboundaries effectively impede the charge injection and excitation, leading to more than one order of magnitude lower leakage current density than the pristine polymer matrix PEI at high electric fields and elevated temperature. In addition, the film processing is simple, straightforward, and low cost, thus this all-polymer nanostructured dielectric material strategy is suitable for the mass production of dielectric polymer films for high-temperature capacitive energy storage.
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