High power density capacitors have been highly demanded
in modern
electronics and pulsed power systems. Yet the long-standing challenge
that restricts achieving high power in capacitors lies in the inverse
relationship between the breakdown strength and permittivity of dielectric
materials. Here, we introduce poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE) into the host poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) to produce PVDF-based
copolymer blends, resulting in composition-driven 0–3 type
microstructures, featuring nanospheres of P(VDF-TrFE) lamellar crystals
dispersed homogeneously in a P(VDF-HFP) matrix together with crystalline
phase evolution from the γ-phase to the α-phase. At the critical composition, the TrFE/HFP mole ratio
is equal to 1, and the blend film achieves maximum energy storage
performance with discharged energy density (U
dis) ∼ 24.3 J/cm3 at 607 MV/m. Finite element
analyses reveal the relationship between microstructures, compositions,
and the distribution of local electric field and polarization, which
provide an in-depth understanding of the microscopic mechanism of
the enhancement in energy storage capability of the blend films. More
importantly, in a practical charge/discharge circuit, the blend film
could deliver an ultrahigh energy density of 20.4 J/cm3, i.e., 88.3% of the total stored energy to 20 kΩ load in 2.8
μs (τ0.9), resulting a high power density of
7.29 MW/cm3, outperforming the reported dielectric polymer-based
composites and copolymer films in both energy and power densities.
The study thus demonstrates a promising strategy to develop high-performance
dielectrics for high power capacitors.