Enhanced High-Temperature performance of PEI dielectrics via deep trap energy levels and physically crosslinked effects

Dielectric capacitors are indispensable energy storage components in both civilian applications and industrial processes. Under elevated temperatures and intense electric fields, polymer dielectrics usually suffer from an inevitably increase in conductivity, leading to a significant reduction in breakdown strength, energy density and efficiency. This investigation aims to design an all-organic dielectric with enhanced high-temperature capacitive performance by introducing a small molecule P-xylene F (PF) into polyetherimide (PEI). Two mechanisms including the incorporation of deep trap energy levels via wide bandgap fillers and the electrostatic interactions by hydrogen bonding between the fillers and the polymer matrix are proposed to support the enhancement. The hydrogen bonding between PF and polyamic acid (PAA)chains induces the formation of physical cross-linking between PF and the negatively charged benzene rings in PEI after imidization. This influences benzene ring stacking within the polymer chains and enhances the film’s mechanical strength. Additionally, PF’s wider bandgap compared to PEI introduces deep trap energy levels, hindering carrier transport and reducing conductive losses at high temperatures. As results, the dielectric achieves an energy density (U d ) of 4.47 J/cm 3 with an efficiency (η) above 90 % at 200 °C. Its excellent stability is also demonstrated with over 210,000 charge–discharge cycles at 200 °C. This study promotes the development of high-performance dielectrics at high temperature.