Scalable co-cured polyimide/poly(p-phenylene benzobisoxazole) all-organic composites enabling improved energy storage density, low leakage current and long-term cycling stability

Abstract

The all-organic high-temperature polymer dielectrics with promising scale-up potential have witnessed much progress in the energy storage area, etc. However, the electron suppression trap mechanisms behind many all-organic dielectrics are still unclear, especially for high temperature resistant poly(p-phenylene benzobisoxazole) (PBO) polymers. To resolve this tough issue, we herein innovatively prepared PBO-based all-organic thin films containing sulfone-based polyimide (P(DSDA-ODA)) functioning as an electron trap phase using a facile and scalable co-curing method. The great linear dielectric properties of the prepared P(DSDA-ODA)/PBO films hold high dielectric thermal stability over the temperature range from 25 °C to 200 °C. The 60 wt% P(DSDA-ODA) systems yield the lowest leakage current (3.8 × 10⁻⁸ A cm⁻²). The tight structure and reduced leakage current enable an enhanced breakdown strength of 60 wt% P(DSDA-ODA)/PBO (470 kV mm⁻¹), which is 1.7 times that of pure PBO. Meanwhile, it can reach 4.16 J cm⁻³ of energy density, which is 257% higher than that for pure PBO thin films while concurrently maintaining a long stable charge–discharge cycle (at least 5000 times) and high charge–discharge efficiency at 85.10%. Moreover, P(DSDA-ODA)/PBO still exhibits excellent energy storage performance at high temperature compared to PBO. This innovative strategy is further verified by replacing P(DSDA-ODA) with P(6FDA-ODA), and therefore lays a solid foundation for more investigation on scalable all-organic dielectrics.