Enhanced high-temperature energy storage performance in all-organic dielectric films through synergistic crosslinking of chemical and physical interaction

Advanced electronic devices and energy systems urgently require high-temperature polymer dielectrics that can offer both high discharge energy density and energy storage efficiency. However, the capacitive properties of most polymers sharply deteriorate at elevated temperatures, due to the significant rise in leakage current density and energy loss. Herein, a new design approach is adopted to fabricate high-temperature polyetherimide (PEI) dielectrics with chemical and physical cooperative crosslinking networks, the dual-crosslinked PEI dielectrics are prepared through amine crosslinking agent and the electrostatic interaction of oppositely charged phenyl groups between triptycene (TE) and PEI chain segments. Benefiting from the increased crosslinking sites, the dual-crosslinked PEI films achieve the simultaneously enhancement in Tg, modulus and bandgap compared to un-crosslinked and single-crosslinked polymers. Meanwhile, the PEI with dual-crosslinked network displays higher chain packing density, effectively reducing the mean motion pathways of charge carriers and the conduction loss inside polymer dielectric. Consequently, the dual-crosslinked PEI containing 0.25 wt% TE delivers an outstanding discharge energy density of 2.69 J/cm3 and retains excellent cyclability after 100,000 charge–discharge cycles at 200 ℃. Additionally, finite element analysis and molecular dynamics simulation further confirm that less Joule heat and tighter chain structure are formed in the dual-crosslinked polymer dielectric. This research offers a novel methodology to prepare high-performance polymer dielectrics for high-temperature applications. © 2024 Elsevier B.V.