Integrated Molecular Engineering Strategy in All-Organic Dielectrics for Ultrahigh-Temperature Capacitive Energy Storage
Polymer composite dielectrics are key materials for high-temperature film capacitors, yet their energy storage capability is severely constrained at elevated temperatures. Molecular fillers that simultaneously integrate deep-level trapping (high electron affinity, Ea), strong insulation (large bandgap, Eg), and high thermal stability are rarely available, posing a major challenge for improving high-temperature energy storage performance. To address this challenge, we screen and identify hexaazatriphenylene hexacarbonitrile (HAT-CN) as a promising candidate that fulfills the above critical requirements from numerous commercial organic molecules. When incorporated into a high glass transition temperature (Tg) polymer fluorene polyester (FPE), the resulting all-organic composite exhibits simultaneously suppressed high-temperature conduction loss and preserved mechanical robustness. Consequently, the optimized composite achieves record-high discharged energy densities of 7.31 J cm−3 at 150 °C and 6.14 J cm−3 at 200 °C (η≥90%) with a low cost and scalable process. This work demonstrates that the filler design based on synergistic key properties provides a potent pathway to break the longstanding high-temperature performance bottleneck in polymer dielectrics.