Massively Parallel Aligned Poly(vinylidene fluoride) Nanofibrils in All-Organic Dielectric Polymer Composite Films for Electric Energy Storage

It is a formidable challenge to combine the performance advantages of linear and nonlinear polymer dielectrics for developing all-organic film capacitors with high energy density and low loss. In this work, massively parallel aligned poly(vinylidene fluoride) (PVDF) nanofibrils were in situ fabricated for the first time in the polyethylene (PE) matrix via a multistage stretching technology involving hot stretching and solid-state stretching at an elevated temperature. The largely enhanced interfacial area of PVDF nanofibrils could effectively induce interfacial polarization, imparting PE composite films with a high dielectric constant of 4.50. More interestingly, the nanoconfinement effect of PVDF nanofibrils greatly restricted the migration of free electrons and impurity ions, and an impressive breakdown strength of 624 MV m–1 was obtained. As a result, the as-prepared PE/PVDF composite films exhibited an attractive discharged energy density of as high as 6.4 J cm–3, which was more than 10 times of the conventional counterparts, and outperformed the current linear dielectric polymers. The ingenious structure design of in situ nonlinear dielectric nanofibrils provides a promising approach to maximize the advantageous polarizations and minimize the disadvantageous polarizations in the linear and nonlinear polymer dielectric blends, achieving all-organic polymer dielectric composite films with high energy density and low loss.