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Dielectric polymer nanocomposites are considered as one of the most promising candidates for high-power-density electrical energy storage applications. Inorganic nanofillers with high insulation property are frequently introduced into fluoropolymer to improve its breakdown strength and energy storage capability. Normally, inorganic nanofillers are thought to introducing traps into polymer matrix to suppress leakage current. However, how these nanofillers effect the leakage current is still unclear. Meanwhile, high dopant (> 5 vol%) is prerequisite for distinctly improved energy storage performance, which severely deteriorates the processing and mechanical property of polymer nanocomposites, hence brings high technical complication and cost. Herein, boron nitride nanosheet (BNNS) layers are utilized for substantially improving the electrical energy storage capability of polyvinylidene fluoride (PVDF) nanocomposite. Results reveal that the high conduction band minimum of BNNS produces energy barrier at the interface of adjacent layers, preventing the electron in PVDF from passing through inorganic layers, leading to suppressed leakage current and superior breakdown strength. Accompanied by improved Young’s modulus (from 1.2 GPa of PVDF to 1.6 GPa of nanocomposite), significantly boosted discharged energy density (14.3 J cm−3) and charge–discharge efficiency (75%) are realized in multilayered nanocomposites, which are 340 and 300% of PVDF (4.2 J cm−3, 25%). More importantly, thus remarkably boosted energy storage performance is accomplished by marginal BNNS. This work offers a new paradigm for developing dielectric nanocomposites with advanced energy storage performance.

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Surface charge density has been demonstrated to be significantly impacted by the dielectric properties of tribomaterials. However, the ambiguous physical mechanism of dielectric manipulated charge behavior still restricts the construction of high-performance tribomaterials. Here, using the atomic force microscopy and Kelvin probe force microscopy, an in situ method was conducted to investigate the contact electrification and charge dynamics on a typical tribomaterial (i.e., BaTiO3/PVDF-TrFE nanocomposite) at nanoscale. Combined with the characterization of triboelectric device at macroscale, it is found that the number of transferred electrons increases with contact force/area and tends to reach saturation under increased friction cycles. The incorporated high permittivity BaTiO3 nanoparticles enhance the capacitance and electron trapping capability of the nanocomposites, efficiently inhibiting the lateral diffusion of electrons and improving the output performance of the triboelectric devices. Exponential decay of the surface potential is observed over monitoring time for all dielectric samples. At high BaTiO3 loadings, more electrons can drift into the bulk and combine with the induced charges on the back electrode, forming a large leakage current and accordingly accelerating the electron dissipation. Hence, the charge trapping/storing and dissipating, as well as the charge attracting properties, should be comprehensively considered in the design of high-performance tribomaterials.