Co-modulated interface binding energy and electric field distribution of layer-structured PVDF–LDPE dielectric composites with BaTiO₃: experiment and multiscale simulations

Abstract

The layer-structured composites were built by the dielectric and insulating layers composed of polyvinylidene fluoride (PVDF) and low-density polyethylene (LDPE) composites containing barium titanate (BT) to modulate the dielectric and energy storage properties of the composites. The simulations on the interface models for molecular dynamics and the geometric models for finite element analysis were performed together with the experimental characterization of the morphology, dielectric, and energy storage properties of the composites. The results revealed that polyethylene as an insulating layer played a successful role in modulating dielectric permittivity and breakdown strength while BT particles exerted positive effects in improving the miscibility between the composed layers and redistributing the electric field. The strong interface binding energy and the similar dielectric permittivity between the PVDF layer and the BT20/LDPE layer made for the layer-structured composites with a characteristic breakdown strength (E_b) of 188.9 kV·mm⁻¹, a discharge energy density (U_d) of 1.42 J·cm⁻³, and a dielectric loss factor (tanδ) of 0.017, which were increased by 94%, 141%, and decreased by 54% in comparison with those of the BT20/PVDF composite, respectively.

Graphical abstract

Keywords

dielectric composite / layer structure / low-density polyethylene / polyvinylidene fluoride / molecular dynamics simulation / finite element analysis

References

[1] Wang L, Luo H, Zhou X, . Enhanced permittivity and energy density of P (VDF–HFP)-based capacitor using core‒shell structured BaTiO₃@TiO₂ fillers.Ionics, 2018, 24(12): 3975–3982

[2] Zheng M S, Zheng Y T, Zha J W, . Improved dielectric, tensile and energy storage properties of surface rubberized BaTiO₃/polypropylene nanocomposites.Nano Energy, 2018, 48: 144–151

[3] Prateek , Thakur V K, Gupta R K . Recent progress on ferroelectric polymer-based nanocomposites for high energy density capacitors: synthesis, dielectric properties, and future aspects.Chemical Reviews, 2016, 116(7): 4260–4317

[4] Dong Y, Wang Z, Huo S, . Improved dielectric breakdown strength of polyimide by incorporating polydopamine-coated graphitic carbon nitride.Polymers, 2022, 14(3): 385

[5] Dang Z M, Xu H P, Wang H Y . Significantly enhanced low-frequency dielectric permittivity in the BaTiO₃/poly (vinylidene fluoride) nanocomposite.Applied Physics Letters, 2007, 90(1): 012901

[6] Muralidhar C, Pillai P K C . Pyroelectric, dielectric, resistivity and hysteresis behaviour of barium titanate (BaTiO₃)/polyvinylidene fluoride (PVDF) composites and correlation by SEM.Journal of Materials Science Letters, 1987, 6(11): 1243–1245

[7] Silakaew K, Thongbai P . Continually enhanced dielectric constant of poly (vinylidene fluoride) with BaTiO₃@poly (vinylidene fluoride) core–shell nanostructure filling.Ceramics International, 2022, 48(5): 7005–7012

[8] Ma J, Azhar U, Zong C, . Core–shell structured PVDF@BT nanoparticles for dielectric materials: a novel composite to prove the dependence of dielectric properties on ferroelectric shell.Materials & Design, 2019, 164: 107556

[9] Sang X, Li X, Zhang D, . Improved dielectric properties and energy-storage densities of BaTiO₃-doped PVDF composites by heat treatment and surface modification of BaTiO₃.Journal of Physics D: Applied Physics, 2022, 55(21): 215501

[10] Tuncer E, Sauers I, James D R, . Enhancement of dielectric strength in nanocomposites.Nanotechnology, 2007, 18(32): 325704

[11] Wang G, Huang Y, Wang Y, . Substantial enhancement of energy storage capability in polymer nanocomposites by encapsulation of BaTiO₃ NWs with variable shell thickness.Physical Chemistry Chemical Physics, 2017, 19(31): 21058–21068

[12] Fan Y, Huang X, Wang G, . Core–shell structured biopolymer@BaTiO₃ nanoparticles for biopolymer nanocomposites with significantly enhanced dielectric properties and energy storage capability.The Journal of Physical Chemistry C, 2015, 119(49): 27330–27339

[13] Nian W, Wang Z, Wang T, . Significantly enhanced breakdown strength and energy density in sandwich-structured NBT/PVDF composites with strong interface barrier effect.Ceramics International, 2018, 44: S50–S53

[14] Joyce D M, Ouchen F, Grote J G . Re-engineering the polymer capacitor, layer by layer.Advanced Energy Materials, 2016, 6(15): 1600676

[15] Pan Z, Liu B, Zhai J, . NaNbO₃ two-dimensional platelets induced highly energy storage density in trilayered architecture composites.Nano Energy, 2017, 40: 587–595

[16] Wu Y, Wang Z, Shen X, . Graphene/boron nitride–polyurethane microlaminates for exceptional dielectric properties and high energy densities.ACS Applied Materials & Interfaces, 2018, 10(31): 26641–26652

[17] Wang Y F, Wang L X, Yuan Q B, . Ultrahigh electric displacement and energy density in gradient layer-structured BaTiO₃/PVDF nanocomposites with an interfacial barrier effect.Journal of Materials Chemistry A: Materials for Energy and Sustainability, 2017, 5(22): 10849–10855

[18] Hu P H, Shen Y, Guan Y H, . Topological-structure modulated polymer nanocomposites exhibiting highly enhanced dielectric strength and energy density.Advanced Functional Materials, 2014, 24(21): 3172–3178

[19] Wang Y F, Wang L X, Yuan Q B, . Ultrahigh energy density and greatly enhanced discharged efficiency of sandwich-structured polymer nanocomposites with optimized spatial organization.Nano Energy, 2018, 44: 364–370

[20] Sun Q Z, Mao P, Zhang L X, . Significantly enhanced dielectric and energy storage performance of AlN/KNbO₃/PVDF sandwich-structured composites via introducing the AlN/PVDF insulating layers.Ceramics International, 2020, 46(8): 9990–9996

[21] Sun Q Z, Wang J P, Sun H N, . Simultaneously enhanced energy density and discharge efficiency of layer-structured nanocomposites by reasonably designing dielectric differences between BaTiO₃@SiO₂/PVDF layers and BNNSs/PVDF–PMMA layers.Composites Part A: Applied Science and Manufacturing, 2021, 149: 106546

[22] Zhou Y J, Liu Q X, Chen F J, . Improving breakdown strength and energy storage efficiency of poly(vinylidene fluoride-co-chlorotrifluoroethylene) and polyurea blend films by double layer structure design.Polymer Testing, 2020, 81: 106261

[23] Li Z Y, Shen Z H, Yang X, . Ultrahigh charge‒discharge efficiency and enhanced energy density of the sandwiched polymer nanocomposites with poly(methyl methacrylate) layer.Composites Science and Technology, 2021, 202: 108591

[24] Mansour D A, Abdel-Gawad N M K, El Dein A Z, . Recent advances in polymer nanocomposites based on polyethylene and polyvinylchloride for power cables.Materials, 2020, 14(1): 66

[25] Wang B H, Liang G Z, Jiao Y C, . Two-layer materials of polyethylene and a carbon nanotube/cyanate ester composite with high dielectric constant and extremely low dielectric loss.Carbon, 2013, 54: 224–233

[26] Li D W, Zhou L W, Wang X, . Space charge property at the interface in low-density polyethylene/MgO three-layered nanocomposites.Modern Physics Letters B, 2019, 33(3): 1950210

[27] Bo R T, Wang J H, Wang C F, . Selective distribution of BaTiO₃ and graphene in PS/PVDF blends: molecular dynamics simulations.Materials Today: Communications, 2023, 34: 105247

[28] Bo R T, Liu J W, Wang C F, . Molecular dynamics simulation on structure and dielectric permittivity of BaTiO₃/PVDF.Advances in Polymer Technology, 2021, 2021: 1–14

[29] Guo R, Luo H, Zhai D, . Bilayer structured PVDF-based composites via integrating BaTiO₃ nanowire arrays and BN nanosheets for high energy density capacitors.Chemical Engineering Journal, 2022, 437: 135497

[30] Cai Z M, Wang X H, Luo B C, . Laminated structure-induced high dielectric strength and energy storage density in dielectric composites.Composites Science and Technology, 2019, 173: 61–65

[31] Lencar C, Ramakrishnan S, Erfanian E, . The role of phase migration of carbon nanotubes in melt-mixed PVDF/PE polymer blends for high conductivity and EMI shielding.Molecules, 2022, 27(3): 933

[32] Jawalkar S S, Adoor S G, Sairam M, . Molecular modeling on the binary blend compatibility of poly(vinyl alcohol) and poly(methyl methacrylate): an atomistic simulation and thermodynamic approach.The Journal of Physical Chemistry B, 2005, 109(32): 15611–15620

[33] Yoo C S . Physical and chemical transformations of highly compressed carbon dioxide at bond energies.Physical Chemistry Chemical Physics, 2013, 15(21): 7949–7966

[34] Waqas M, Ali S, Lv W, . High-performance PE–BN/PVDF–HFP bilayer separator for lithium-ion batteries.Advanced Materials Interfaces, 2019, 6(1): 1801330

[35] Zeng J P, Zhang J Y, Gong X D . Molecular dynamics simulation of interaction between benzotriazoles and cuprous oxide crystal.Computational & Theoretical Chemistry, 2011, 963(1): 110–114

[36] Zeng J P, Wang F H, Zhou C, . Molecular dynamics simulation on scale inhibition mechanism of polyepoxysuccinic acid to calcium sulphate.Chinese Journal of Chemical Physics, 2012, 25(2): 219–225

[37] Sun D D, Huang S J, Gao Y, . PVDF, composites with spherical polymer-derived SiCN ceramic particles have significantly enhanced low-frequency dielectric constants.Journal of Alloys and Compounds, 2019, 783: 256–262

[38] Upadhyay R H, Deshmukh R R . Investigation of dielectric properties of newly prepared β-phase polyvinylidene fluorideebarium titanate nanocomposite films.Journal of Electrostatics, 2013, 71(5): 945–950

[39] Durga Prasad P, Hemalatha J . Dielectric and energy storage density studies in electrospun fiber mats of polyvinylidene fluoride (PVDF)/zinc ferrite (ZnFe₂O₄) multiferroic composite.Physica B: Condensed Matter, 2019, 573: 1–6

[40] Xie B, Zhang H B, Zhang Q, . Enhanced energy density of polymer nanocomposites at a low electric field through aligned BaTiO₃ nanowires.Journal of Materials Chemistry A: Materials for Energy and Sustainability, 2017, 5(13): 6070–6078

[41] Sun L, Shi Z C, Liang L, . Layer-structured BaTiO₃/P(VDF–HFP) composites with concurrently improved dielectric permittivity and breakdown strength toward capacitive energy-storage applications.Journal of Materials Chemistry C: Materials for Optical and Electronic Devices, 2020, 8(30): 10257–10265

[42] Wang Y, Cui J, Yuan Q, . Significantly enhanced breakdown strength and energy density in sandwich-structured barium titanate/poly(vinylidene fluoride) nanocomposites.Advanced Materials, 2015, 27(42): 6658–6663

[43] Agoris D P, Vitellas I, Gefle O S, . The barrier effect in three-layer solid dielectrics in quasi-uniform electric field.Journal of Physics D: Applied Physics, 2001, 34(24): 3485–3491

[44] Feng Y, Li J L, Li W L, . Effect of BaTiO₃ nanowire distribution on the dielectric and energy storage performance of double-layer PVDF-based composites.Composites Part A: Applied Science and Manufacturing, 2019, 125: 105524

Disclosure of potential conflicts of interests

The authors declare no competing interests.

Acknowledgements

The authors acknowledge supports from the Key projects of Natural Science Foundation of Heilongjiang Province (ZD2020E007).

Electronic supplementary information

Supplementary materials can be found in the online version at https://doi.org/10.1007/s11706-023-0657-5 and https://journal.hep.com.cn/foms/EN/10.1007/s11706-023-0657-5, which include Tables S1–S9 and Figs. S1‒S6.

RIGHTS & PERMISSIONS

2023 Higher Education Press