Abstract
Many mainstream dielectric energy storage technologies in the emergent applications, such as renewable energy, electrified transportations and advanced propulsion systems, are usually required to operate under harsh-temperature conditions. However, excellent capacitive performance and thermal stability tend to be mutually exclusive in the current polymer dielectric materials and applications. Here, we report a strategy to tailor structural units for the design of high-temperature polymer dielectrics. A library of polyimide-derived polymers from diverse combinations of structural units are predicted, and 12 representative polymers are synthesized for direct experimental investigation. This study provides important insights into decisive structural factors necessary to achieve robust and stable dielectrics with high energy storage capabilities at elevated temperature. We also find that the high-temperature insulation performance would experience diminishing marginal utility as the bandgap increases beyond a critical point, which is strongly correlated to the dihedral angle between neighboring planes of conjugation in these polymers. By experimentally testing the optimized and predicted structures, an increased energy storage at temperatures up to 250 °C is observed. We discuss the possibility for this strategy to be generally applied to other polymer dielectrics to achieve further performance enhancement.