PVDF Composites Research Articles

Improved dielectric properties and thermal conductivity of PVDF composites filled with core–shell structured Cu@CuO particles

To suppress dielectric loss while still harvesting high dielectric constant (k) and thermal conductivity in polymer composites, core–shell structured fillers are synthesized via controlled calcination under air, where the conductive copper (Cu) particles are encapsulated by a thin insulating oxidation layer (CuO). The dielectric constant can be substantially improved in the poly(vinylidene fluoride) PVDF composites filled with Cu@CuO fillers, and the dielectric loss is strongly restrained even at high filler loadings. The improved dielectric performance can be ascribed to the insulating CuO shell, which promotes the multiple interfacial polarization and meanwhile impedes the long-range electron migration. Additionally, the Cu@CuO/PVDF composites exhibit higher thermal conductivity (TC) than the unfilled polymer and the Cu/PVDF, owing to the reduced interfacial thermal resistance between the fillers and the matrix. Composites with high TC and k but low loss are promising materials for potential applications in microelectronic, electrical and energy storage devices.

Study on the effect of PVDF and TiO2 composition on quasi-solid state DSSC

Dye sensitized solar cell (DSSC) is a third generation solar cell that has become an interesting research topic on energy area due to its properties such as low cost, green technology and simple fabrication. DSSC is mainly constructed with three components consisting of semiconductor photoelectrode, counter electrode and an electrolyte, which usually contains redox couple. Liquid electrolyte is commonly used in standard DSSC device, although it is vulnerable to leakage and susceptible to the environment. Furthermore, liquid electrolyte could react to some kind of sealing material that encapsulates the device as it affects the stability performance. Accordingly, this research attempted to develop quasi-solid-state DSSC (QS-DSSC) by replacing liquid to gel electrolyte in a sandwich structured DSSC with a size of 0.5 cm × 0.5 cm per unit cell. The gel electrolyte prepared in this work was based on liquid electrolyte that was mixed with TiO2 and polymer material in the form of PVDF with various compositions for optimizing the gel electrolyte material. The performance of QS-DSSC samples was obtained using IPCE and I – V measurement, while the viscosity characteristic of the electrolyte was also assessed. The best performance of QS-DSSC sample achieved in this work had short-circuit current density, open-circuit voltage, fill factor, and photoconversion efficiency of 3.708 mA/cm2, 0.637 V, 0.64, and 2.98%, respectively.

Integration of PDA Chemistry and Surface‐Initiated ATRP to Prepare Poly(methyl methacrylate)‐Grafted Carbon Nanotubes and Its Effect on Poly(vinylidene fluoride)–Carbon Nanotube Composite Properties

AbstractPoly(methyl methacrylate)‐grafted carbon nanotubes (PMMA@MWCNTs) are nondestructively prepared via the integration of mussel‐inspired polydopamine (PDA) chemistry and the surface‐initiated atom transfer radical polymerization (ATRP) method. The structures and properties of the poly(vinylidene fluoride)‐based (PVDF‐based) nanocomposites filled with pristine MWCNTs and PMMA@MWCNTs are investigated. The results show that the encapsulation of PMMA on the MWCNTs surface not only improves the dispersibility of MWCNTs in the PVDF matrix but also enhances the interfacial interaction between MWCNTs and PVDF. The addition of PMMA@MWCNTs nanofillers to PVDF can effectively induce the crystal structure of PVDF to transform from the α‐phase to the β/γ ‐phase, and nearly 100% β/γ ‐phase PVDF formed when the nanofiller loading is higher than 5 wt%. Compared with the MWCNTs/PVDF composites, the PMMA@MWCNTs/PVDF composites exhibit obvious improvement in the percolation threshold because the PMMA shells hinder the direct contact of the MWCNTs. Moreover, the loss tangent of the PMMA@MWCNTs/PVDF composites is effectively suppressed due to the reduced leakage current in the composites and the enhanced interfacial strength between the nanofiller and the matrix.

Intensifying energy density, dielectric and mechanical properties of electroactive β-PVDF/f-BTO nanocomposites

In this paper, we report the enhancement of energy density and consequently energy harvesting efficiency of PVDF/f-BaTiO3 nanocomposite. Synthesis of semicrystalline β phase PVDF, PVDF-BTO and PVDF-BTOf composites by spin coating method and their characteristics investigations have been reported. The energy storage density of composite with modified structure was largely increased and was found to be 0.242 J/cm3 at 10 MV/m with 68% energy harvesting efficiency. Maximum dielectric constant was found to be 230 at 1 Hz for PVDF-BTOf composite. Maximum capacitance obtained for PVDF-BTOf composite was 816 μF. From CV and chronopotentiometry scan investigation, the maximum power density was found to be 59.5 W/kg with specific energy density of 0.082 Wh/kg for PVDF-BTO composite. Tensile strength and young's modulus of PVDF-BTOf composite are found to be 6.37 MPa and 48.7 MPa respectively. These results demonstrate a potential way to enhance the performance of composites for energy harvestor, capacitor etc.

Enhanced energy storage property of plate-like Na0.5Bi4.5Ti4O15/poly(vinylidene fluoride) composites through texture arrangement

The plate-like Na0.5Bi4.5Ti4O15 (P-NBT4) particles were synthesized by molten salt method and dispersed in a poly (vinylindene fluoride) (PVDF) matrix. The alignment of P-NBT4 particles in PVDF matrix perpendicular to the direction of applied electric field could bring to impressive dielectric performance and breakdown strength to the composites. On the one hand, the excellent dielectric property of the P-NBT4/PVDF composites is ascribed to the high capacitance that is consist of P-NBT4 particles micro-capacitances. On the other hand, a higher breakdown strength of the P-NBT4/PVDF composites is owing to that strong barrier layer was formed in the composites by P-NBT4 particles alignment, which bring difficulty to form a conductive pathway. Moreover, the textured P-NBT4/PVDF composites exhibit a high energy density (9.45 J/cm3) and energy efficiency (η) of 52.28% under the critical electric field of 300 kV/mm.

Development of strain sensor using conductive poly(vinylidene fluoride) (PVDF) nanocomposite membrane reinforced with ionic liquid (IL) & carbon nanofiber (CNF)

High sensitivity and good mechanical strength are required for conductive polymer nano-composites (CPNC) based flexible strain sensors. Here we have developed CPNC membranes using PVDF as a base polymer along with carbon nanofiber (CNF) and ionic liquid (IL) as conducting fillers exhibiting good thermal stability, high sensing voltage, and mechanical performance for strain sensors. The IL infiltration in PVDF and CNFs composition resulted in micro-porous morphology that exhibited stretchability (maximum elongation = 5.8 mm) and a high gauge factor (4.08) (property of a good strain sensor). Further, infiltration of IL in PVDF/CNF membrane brings microstructural changes (α to β phase) of PVDF and provides an electrolyte mixture of CNF and IL for the facile flow of ions through it. The CNFs in CPNC having IL helped in maintaining the crack initiation during strain. Hence, the deformed CNFs across the pores or within the PVDF act as an interlinking agent and provides an electrical conduction pathway in the shrink lattice of the composite.

Effects of surface modification on electrical properties of KNN nanorod-incorporated PVDF composites

The demand of self-powered electronic devices has stimulated a great interest in daily life. To fulfill this, thrust researchers are engaged to develop different piezoelectric self-powered-based devices. The piezoelectricity is broadly dependent on the electroactive phase of the polymer structure. Herein, lead-free potassium sodium niobate (KNN) nanorods-incorporated PVDF polymer-based nanocomposite films have been developed wherein KNN nanorods have been surface-modified by three diverse surface modifiers such as 3-aminopropyltrimethoxysilane (APS), polyaniline (PANI) and polyvinylpyrrolidone (PVP) for resolving the agglomeration problem of the nanorods and to look into their effect on the microstructural growth including nucleation of polar crystals. The nanocomposite films have been developed simply by solution cast method. The growth of electroactive phases (β and γ) of the PVDF polymer has been observed to be improved significantly by incorporation of surface-modified KNN nanorods. The calculated beta fraction (F(β)) and gamma fraction (F(γ)) as calculated by the FTIR spectrum (98% and 99%) are maximum for the silane- and PVP-modified KNN nanorods-incorporated PVDF polymer, because of the higher molecular weight and homogeneous distribution of the nanorods throughout the PVDF matrix. The total crystallinity evaluated by XRD patterns, specifically β crystal part for the surface-modified KNN nanorods-based film, has been improved (17% for pure PVDF, 45% for untreated KNN-based film and more than 50% for the surface-modified KNN-based films). The remnant polarization values are also remarkably higher (0.49 μC/cm2 for silane, 0.022 μC/cm2 for PVP and 0.015 μC/cm2 for PANI-modified KNN nanorods-based composites, respectively) for surface-modified KNN nanorods-based composite with contrast to pure PVDF (0.001 μC/cm2) and untreated KNN-based film (0.002 μC/cm2). The dielectric constant values for modified KNN nanorods-incorporated PVDF polymer composites have also been demonstrated as substantial enhancement which are 68, 71 and 70, respectively, for silane-, PANI- and PVP-modified samples, whereas the values are 2 and 38 for pure PVDF and untreated KNN-based films. This study clearly defines that the selection of a suitable surface modifier (interface) can play a noteworthy role in exploitation of excelling electroactive phases of PVDF to the maximum extent to enhance its dielectric, ferroelectric as well as piezoelectric response with low level of loading.

Infrared-driven poly(vinylidene difluoride)/tungsten oxide pyroelectric generator for non-contact energy harvesting

Wasted heat has been regarded as one of the most important and widely available renewable energy sources worldwide, and a lot of attention has been paid to harvesting ambient wasted thermal energy. In this study, a novel infrared (IR)-driven non-contact pyroelectric generator based on electrospun poly(vinylidene fluoride) (PVDF) nanofibrous membranes is developed for converting photothermal energy into useful electrical energy. Here, we incorporate a photothermal conversion material: reduced tungsten oxide (WO2.72), into PVDF to enhance the heat transfer of PVDF/WO2.72 nanofibrous membranes, which is due to their excellent IR absorbance. Meanwhile, partially covered electrodes are used to achieve faster and larger temperature fluctuations, which further improve pyroelectric energy transformation. Under IR irradiation, the temperature of the PVDF/WO2.72 pyroelectric composites containing 7 wt% WO2.72 rapidly rises to 107.1 °C after 60 s, which is 41.5 °C higher than that of the WO2.72-free PVDF composites. The maximum output voltage of the WO2.72-free PVDF composites is 0.5 V, while that of the 7 wt% PVDF/WO2.72 composites is three times higher, and reaches 1.5 V. Moreover, the 7 wt% PVDF/WO2.72 composites also presents good pyroelectric energy output stability and durability.

Fabrication and characterization of poly(vinylidene fluoride)–polytetrafluoroethylene composite membrane for CO2 absorption in gas–liquid contacting process

ABSTRACTThe wetting resistance of poly(vinylidene fluoride) (PVDF) membrane is a critical factor which determines the carbon dioxide (CO2) absorption performance of the gas–liquid membrane contactors. In this study, the composite PVDF–polytetrafluoroethylene (PTFE) hollow fiber membranes were fabricated through dry‐jet wet phase‐inversion method by dispersing PTFE nanoparticles into PVDF solution and adopting phosphoric acid as nonsolvent additive. Compared with the PVDF membrane, the composite membranes presented higher CO2 absorption flux due to their higher effective surface porosity and surface hydrophobicity. The composite membrane with addition of 5 wt % PTFE in the dope gained the optimum CO2 absorption flux of 9.84 × 10−4 and 2.02 × 10−3 mol m−2 s−1 at an inlet gas (CO2/N2 = 19/81, v/v) flow rate of 100 mL min−1 by using distilled water and aqueous diethanolamine solution, respectively. Moreover, the 5% PTFE membrane showed better long‐term stability than the PVDF membrane regardless of different types of absorbent, indicating that polymer blending demonstrates great potential for gas separation. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47767.

Surface modification of GO by PDA for dielectric material with well-suppressed dielectric loss

To suppress the high dielectric loss of graphene oxide (GO)/poly(vinylidene fluoride) (PVDF) while maintaining high dielectric constant (high- k) near the percolation threshold, in this study, GO nanosheets coated with polydopamine (PDA) were integrated into PVDF to investigate the effects of the PDA shell and its concentrations on the dielectric properties of the nanocomposites. The results indicate that the dissipation factor and conductivity of the GO@PDA/PVDF are significantly suppressed to very low values compared with the pristine GO/PVDF composites, attributable to the PDA interlayer between the GO nanosheets which prevents them from direct contact with each other and remarkably reduces the leakage loss. Furthermore, activation energies of the GO/PVDF and GO@PDA/PVDF composites were calculated as 1.247 and 0.884 eV, respectively, indicating that the presence of PDA interlayer reduces the relaxation activation energy and makes the relaxation occur at low temperature for the GO@PDA/PVDF. The prepared GO@PDA/PVDF nanocomposites with high- k but low loss have potential applications in microelectronic engineering.

2D SnO2 nanosheet/PVDF composite based flexible, self-cleaning piezoelectric energy harvester

Flexible piezoelectric nanogenerators have been considered as the most promising candidates in recent years for powering the portable, bendable, and wearable electronics devices by scavenging low frequency biomechanical energy. This work reports an analysis of remarkable output power enhancement of a human-body motion based piezoelectric nanogenerator comprising of self-polarized 2D SnO2 nanosheet/poly(vinylidene fluoride) (PVDF) nanocomposite. Structural, mechanical, thermal as well as piezoelectric properties of the composites were studied rigorously, which proved that 5 wt% SnO2 nanosheet/PVDF composite is the most promising one for nanogenerator applications. The inorganic-organic 2D SnO2 nanosheet/PVDF composite based piezoelectric nanogenerators (PSNG) were found to produce outstanding power output due to the gentle human finger imparting with a maximum voltage of 42 V and current density of 6.25 μA·cm−2. The output power density of the PSNG reached 4900 W·m−3 with an efficiency c.a. 16.3%. The obtained output of the reported nanogenerator is in well agreement with the fundamental piezoelectric theory. The improved performance of the self-polarized composite can be attributed to the incorporation of homogeneously distributed 2D SnO2 nanosheets (2D SnO2 NS) having high surface area, which enhances the electroactive β phase contain in PVDF composites as well as piezoelectric properties. The electrical energy (a.c.) generated from the nanogenerator due to gentle human finger imparting was directly utilized to illuminate 85 numbers commercial LEDs and to charge capacitors rapidly through a bridge rectifier. A hydrophobic 2D SnO2 nanosheet/PVDF composite film (static contact angle of water drop ∼82.6°) was wrapped on the fabricated nanogenerator to attain self-cleaning feature of the PSNG, making the device water and dirt resistive. This work explores a new prospect for self-cleaning Gr-IV oxide/PVDF based high-efficiency, high power density energy harvester scavenging biomechanical energy for realizing next generation flexible self-powered electronics systems.

Influence of nanoparticle size on nucleation of electroactive phase and energy storage behaviour of zinc ferrite/ poly(vinylidene fluoride) nanocomposite

The incorporation of different size of nanoparticles in polymer matrix plays a dominating role in determining the overall structural, microstructural and electrical properties of the fabricated composites. In this paper, an investigation was done in order to establish the effect of incorporating different size of zinc ferrite (ZF) nanoparticles in poly(vinylidene fluoride) (PVDF) matrix. The incorporated spherical ZF nanoparticle induced nucleation of electroactive phases in PVDF matrix by means of electrostatic interaction between the surface charge of the filler and the dipoles of PVDF. The fraction of nucleated electroactive phases is strongly dependent on the size of the nanoparticles. There is a critical size of the nanoparticle, below which the nucleation efficiency of the filler diminishes as it may be swelled by the polymer macromolecules. On the other hand, if the filler size is too large, there is a possibility of formation of mixed conformation of polar and nonpolar phase. Further, this behaviour was correlated with the electrical response of composite where nanoparticle with the critical radius incorporated PVDF composite, exhibited maximum dielectric and ferroelectric property. Finally, a number of participating dipoles of polymer chain interact with ZF nanoparticle of different size were calculated by a model analysis and were represented schematically.

Continuous network of CNTs in poly(vinylidene fluoride) composites with high thermal and mechanical performance for heat exchangers

Polymeric materials with high thermal conductivity have drawn much attention in academic and industrial field recently. Due to poor dispersion and insufficient interconnection of fillers, traditional polymer composites present not only undesirable thermal conductivity but other declined properties even with high loaded thermal conductive nanofillers. In this work, the uniform and continuous network of (3-Aminopropyl)trimethoxysilane (APTMS) modified carbon nanotubes (A-CNTs) in poly(vinylidene fluoride) (PVDF) was built up by using the simple casting method. Thermal conductivity of 2.15 Wm−1K−1 and tensile strength enhancement of 70% are achieved at 40 vol% A-CNTs loading compared with that of pure PVDF. The A-CNTs/PVDF composites exhibit an intensified thermal stability and sharply increased crystallinity (45.7%) compared with pure PVDF (28.5%). Moreover, for practical heat exchange experiment, the PVDF composites possess high heat transfer efficiency and long-last stability in corrosive water, which leads to the use of PVDF materials to supersede metal materials in heat transfers.

3-[[3-(Triethoxysilyl)-propyl] amino] propane-1-sulfonic acid zwitterion grafted polyvinylidene fluoride antifouling membranes for concentrating greywater in direct contact membrane distillation

Direct contact membrane distillation (DCMD) is attractive for wastewater reuse where low-grade heat is highly abundant, but membrane fouling is of critical concerns. In this work, a zwitterion surface-grafted composite polyvinylidene fluoride membrane (PVDF-T) was introduced for DCMD treatment of greywater, a lightly polluted wastewater. Surface grafting was achieved by hydroxylation of a pristine PVDF membrane followed by silanization with the zwitterionomer 3-[[3-(triethoxysilyl)-propyl] amino] propane-1-sulfonic acid (TPAPS). The resulting composite PVDF-T membrane showed a significantly reduced water contact angle but nearly the same liquid entry pressure (LEP) indicating that silanization took place mostly at the surface, and the porous matrix remained hydrophobic. Elemental analysis confirmed that the TPAPS surface grafting was successful. Gas permeability tests indicated increased transport resistance, indicating the extra resistance imposed the zwitterionic modification. In concentrating the synthetic greywater, the PVDF-T membrane exhibited much more stable DCMD flux and constant permeate conductivity than the virgin PVDF membrane. Visual and scanning electron microscopy analysis after MD experiments showed that the PVDF-T membrane was fouled less than the pristine membrane. Improvement in surface hydrophilicity, electronegative charge and steric hindrance were ascribed as the main factors for the fouling resistance of a surface grafted zwitterionic composite PVDF membrane.

Enhanced dielectric permittivity in surface-modified graphene/PVDF composites prepared by an electrospinning-hot pressing method

In the present work, the surface-modified graphene (SMG)/poly(vinylidene fluoride) (PVDF) fibrous membranes obtained from the electrospinning were treated by the hot pressing in the laminating mode to form the SMG/PVDF composites. The SMG was prepared by subjecting the graphene oxide to silane modification, NaBH4 reduction, and PVDF grafting in sequence. The successful surface modification of graphene was confirmed by TEM, XPS, Raman spectroscopy, FTIR, WAXD, and TGA. Furthermore, the structures of SMG/PVDF composites fabricated by the electrospinning-hot pressing method were studied by SEM, FTIR, and WAXD, which exhibited the well dispersion of SMG in the PVDF matrix. Finally, the investigation showed that the dielectric permittivities of SMG/PVDF composites increased with the SMG content, which were significantly higher than that of pristine PVDF. The dielectric permittivity of SMG (16 wt%)/PVDF composite (83.8) at 1000 Hz was found to be ten-fold that of the corresponding value of pristine PVDF (8.3) with a relatively low dielectric loss factor (0.34) and a relatively high thermal conductivity (0.679 W/mK).

Achieving high performance poly(vinylidene fluoride) dielectric composites via in situ polymerization of polypyrrole nanoparticles on hydroxylated BaTiO3 particles.

Polymer dielectric composites have widespread applications in many fields ranging from energy storage, microelectronic devices, and sensors to power driven systems, etc. and attract much attention of researchers. However, it is still challenging to prepare advanced polymer dielectric composites with a high dielectric constant (ε'), low dielectric loss (tan δ) and simultaneously high breakdown strength (E bd). In this work, conductive polypyrrole (PPy) nanoparticles were in situ synthesized in a reaction system containing the common barium titanate (BaTiO3, BT) or hydroxylated BaTiO3 (BTOH) particles, and then the PPy@BT and PPy@BTOH composite particles were incorporated into poly(vinylidene fluoride) (PVDF) to prepare the composites. The morphologies and microstructures of the PPy@BT and PPy@BTOH composite particles and the corresponding PVDF composites were comparatively investigated. The results showed that the PPy@BTOH composite particles had a 'mulberry'-like morphology with a rough surface and the self-assembled structure could be maintained in the PVDF composites, which was apparently different from the PVDF/PPy@BT composites, in which most of the PPy nanoparticles dissociatively dispersed in the PVDF matrix. Electrical conductivity measurements showed that at high particle content (≥20 wt%), the PPy@BTOH composite particles endowed the composites with lower electrical conductivity compared with the PPy@BT composite particles. Dielectric property measurements showed that the 'mulberry'-like PPy@BTOH composite particles endowed the PVDF composites with extremely high ε', ultralow tan δ and high E bd compared with the PVDF/PPy@BT composites with dissociatively dispersed PPy nanoparticles and BaTiO3 particles. The polarization and loss mechanisms of the composites were then proposed based on the morphologies and the microstructures of the composites. This work provides an alternative way to fabricate functional dielectric particles through trace functional groups inducing in situ polymerization of conductive polymers, and these particles can be used to fabricate advanced dielectric composites.

Microwave absorption enhancement by adjusting reactant ratios and filler contents based on 1D K-MnO2@PDA and poly(vinylidene fluoride) matrix.

One-dimensional K–MnO2 nanorods were prepared by a wet chemical process. Dopamine hydrochloride (PDA) layers with various thicknesses were coated and finally, the composites were filled in a poly(vinylidene fluoride) (PVDF) matrix using the hot-molding procedure. The complex permittivity and permeability of the K–MnO2@PDA/PVDF composites could be adjusted by reactant amount ratios and filler contents. The minimum reflection loss could reach −49.4 dB and an effective absorption bandwidth (<−10 dB) covering 11.12 GHz was achieved with 20% filler content when the reactant amount ratio between K–MnO2 and PDA was 4 : 0.375, which was derived from effective internal polarization processes. It is expected that these novel composites can be used as high-performance microwave absorbers.

A rational design for reconciling high permittivity and breakdown strength in layered PVDF composites from TaB2@Ta2O5 nanofiller induced Schottky barrier effect

A contradiction between high permittivity and breakdown strength has long been problematic for obtaining high energy density in conductor/polymer composites.

Sandwich-structured all-organic composites with high breakdown strength and high dielectric constant for film capacitor

Currently, energy storage capacitors with high breakdown strength and dielectric constant are highly desired in microelectronics and electric power systems. All-organic film capacitors have been studied owing to their high breakdown strength and low dielectric loss. In this study, poly(vinylidene fluoride) (PVDF) with high breakdown strength was used as outer layers and poly(vinylidenefluoride-ter-trifluoroethylene-ter-chlorotrifluoroethylene) (P(VDF-TrFE-CTFE)) with high dielectric constant was used as the interlayer to prepare sandwich-structured composites. These PVDF/P(VDF-TrFE-CTFE)/PVDF composites with various contents of terpolymer were manufactured through a layer-by-layer solution-casting method. At 1 kHz, the maximum dielectric constant of the sandwich-structured composites reaches up to 18.61 when the content of terpolymer is 45 vol%. The discharged energy density increases with the increasing content of terpolymer at the same electric filed. At 660 kV/mm, the composite with 25 vol% terpolymer delivers the maximum discharged energy density, which is 20.86 J/cm3.

Significantly Enhanced Electrostatic Energy Storage Performance of Flexible Polymer Composites by Introducing Highly Insulating‐Ferroelectric Microhybrids as Fillers

AbstractA hybrid nanoparticle, consisting of BaTiO3 nanoparticles tightly embedded in bronnitride (BN) nanosheets, has been fabricated based on a daring supposition that BN may act as a host to incorporate ferroelectric nanoparticles to improve insulation and polarization under a high electric field. Using the hybrids as fillers in poly(vinylidene fluoride) (PVDF) composites, a high electric breakdown strength (Eb ≈580 kV/mm), which is 1.76 times of the PVDF film, is obtained when the filler content is 5 wt%. A large displacement (9.3 µC/cm2 under 580 kV/mm) is observed so as to obtain a high discharged energy density (Ud ≈17.6 J/cm3) of the BT@BN/PVDF composites, which is 2.8 times of the PVDF film. The enhancement ratio of Eb achieved in this study demonstrates the highest among the reported results. This hybrid structure of fillers provides an effective way to adjust and improve the energy storage properties of the polymer‐based dielectrics.