Voltage-assisted 3D printing of polymer composite dielectric films with low energy loss and high energy storage density

PVDF-based polymers have garnered significant attention in the field of high-power density electrostatic capacitors due to their exceptional dielectric strength. However, their practical applications are constrained by low charge-discharge efficiency (η) and energy storage density (Ue), which stem from high ferroelectric relaxation and low breakdown strength (Eb). Here, a hydrogenated glassy polymer poly(styrene-methyl methacrylate-methylallyl alcohol) (PSMA) is designed and synthesized to be homogeneously distributed in PVDF through voltage-assisted 3D printing-hot pressing, resulting in a flexible composite film. The findings demonstrate that PSMA, rich in hydrogen bonds and high modulus strength, effectively mitigates the ferroelectric phase transition of PVDF to enhance η. Additionally, the voltage-assisted 3D printing process induces an entropy gain mechanism, facilitating the uniform distribution of the two phases and enhancing the interfacial properties for enhancing Eb. Remarkably, the study achieves prominent growth in energy storage performance, with Ue and η reaching 18.1 J/cm3 and 80 % at 525 MV/m, respectively. These remarkable results highlight the potential of 3D printing technology in enhancing the energy storage performance of PVDF-based dielectrics.