Achieving Significantly Boosted Dielectric Energy Density of Polymer Film via Introducing a Bumpy Gold/Polymethylsilsesquioxane Granular Blocking Layer

Abstract Polymer dielectrics are the key materials for pulsed energy storage systems, but their low energy densities greatly restrict the applications in integrated electronic devices. Herein, a unique bumpy granular interlayer consisting of gold nanoparticles (Au NPs) and polymethyksesquioxane (PMSQ) microspheres is introduced into a poly(vinylidene fluoride) (PVDF) film, forming trilayered PVDF‐Au/PMSQ‐PVDF films. Interestingly, the Au/PMSQ interlayer arouses a dielectric enhancement of 47% and an ultrahigh breakdown strength of 704 MV m ⁻¹ , which reaches 153% of pure PVDF. It is revealed that the greatly enhanced breakdown strength originated from the Coulomb‐blockade effect of Au NPs and the excellent insulating properties of PMSQ microspheres with a special molecular‐scale organic–inorganic hybrid structure. Benefiting from the concurrently enhanced dielectric and breakdown performances, an outstanding energy density of 22.42 J cm ⁻³ with an efficiency of 67.1%, which reaches 249% of that of the pure PVDF, is achieved. It is further confirmed that this design strategy is also applicable to linear dielectric polymer polyethyleneimine. The composites exhibit an energy density of 8.91 J cm ⁻³ with a high efficiency of ≈95%. This work offers a novel and efficient strategy for concurrently enhancing the dielectric and breakdown performances of polymers toward pulsed power applications.