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Improved Energy Density Obtained in Trilayered Poly(vinylidene fluoride)-Based Composites by Introducing Two-Dimensional BN and TiO<sub>2</sub> Nanosheets

Dielectric capacitors with an ultrahigh power density have received extensive attention due to their potential applications in advanced electronic devices. However, their inherent low energy density restricts their application for miniaturization and integration of advanced dielectric capacitors. Herein, a novel composite entirely incorporated with two-dimensional (2D) nanosheets with a topological trilayered construction is prepared by a solution casting and hot-pressing method. The 2D boron nitride nanosheets (BNNS) with a wide band gap that are oriented in a poly(vinylidene fluoride) (PVDF) matrix to form the upper and bottom outer layers would efficiently suppress the leakage current in composites, thus significantly improving the overall breakdown strength. Meanwhile, the 2D anatase-type TiO2 nanosheets (TONS) uniformly distributed in the middle layer can enhance their interfacial compatibility and polarization with the PVDF matrix, leading to a synergistic improvement in both the breakdown strength and dielectric constant of the composite. In particular, a significantly improved dielectric constant of ∼11.42, a reduced dielectric loss of 0.03 at 100 Hz, and a maximum discharge energy density (Udis) of 10.17 J cm-3 at an electric field of 370.1 MV m-1 can be obtained from the trilayered composite containing 3 wt % 2D TONS in the middle layer and 2 wt % 2D BNNS on the outer layer. The finding of this research offers an effective strategy for the preparation of advanced polymer-based composites with an outstanding discharge energy density performance.

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Enhanced electro-actuation property of heterogeneous multi-layered polydimethylsiloxane-based dielectric elastomer composites

Due to their feature of the conversion from electrical to mechanical energy under an applied electric field, dielectric elastomers (DEs) have been widely adopted in smart devices. However, the significant electro-actuated property of DEs is always obtained under a giant driving electric field, which raises a potential safety hazard and limits their practical application range. Moreover, the traditional strategy of regulating the flexibility of DEs via physical swelling effect would result in an undesired plasticizer leakage and an irreversible reduction in both electromechanical stability and lifetime. Herein, a typical heterogeneous multi-layered polydimethylsiloxane (PDMS)-based DE composite was prepared by solution blending and the layer-by-layer casting method. Through synchronously introducing the high-permittivity BaTiO3 and the plasticizer dimethyl silicone oil in the middle layer, both the dielectric and mechanical property of the composite are effectively regulated. Not only the interlayered mechanical mismatch is eliminated but also the problem of plasticizer leakage is optimized through this reasonable structural design. The maximum electro-actuated strain obtained in the sandwiched DE composite was as large as 24.25% under 60 V/μm, which is 338.52% higher than that of pristine PDMS. Furthermore, the composite exhibits the largest driving strain (58.31%) near its breakdown electric field of 77.82 V/μm. Therefore, this study provides a promising route for the preparation of advanced DE composite with an improved low-field electro-actuated property.

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