High-dielectric-constant polymer-based elastomeric dielectrics for soft electronic devices

Abstract

Polymer-based elastomeric dielectrics have demonstrated significant application prospects in flexible electronic skins, dielectric actuators, and energy harvesting and storage due to their light weight, tunable structures, and mechanical flexibility. A key focus in developing polymer-based dielectric elastomers is the simultaneous enhancement of dielectric constant and breakdown strength, along with the reduction of dielectric loss, without compromising mechanical flexibility. This review summarizes recent advances in the design and preparation of high-dielectric-constant (high-k) polymer-based elastomeric dielectrics, with special emphasis on strategies for balancing and improving both dielectric and mechanical properties. Finally, we summarize and provide an outlook on the application fields of polymer-based elastic dielectric materials.

Keywords

Elastomeric dielectrics, high-k / soft materials, mechanical properties

References

[1] Park S,Lee W.Self-powered ultra-flexible electronics via nano-grating-patterned organic photovoltaics.Nature2018;561:516-21

[2] Jing Z,He Z.Highly robust and conductive polymer electrodes for droplet energy harvesting and printable on-skin electronics.Adv Mater2025;37:2506511

[3] Meng S,Wang X,Zhang Y.High-dielectric PVDF/MXene composite dielectric materials for energy storage preparation and performance study.Polym Compos2023;45:3460-73

[4] Li Z,Wang J.Sensitive, robust, wide-range, and high-consistency capacitive tactile sensors with ordered porous dielectric microstructures.ACS Appl Mater Interfaces2024;16:7384-98

[5] Zhao S,Cui L.Elastomeric nanodielectrics for soft and hysteresis-free electronics.Adv Mater2021;33:2104761

[6] Li Y,Liu B.Remarkable interfacial dielectric relaxation of physically cross-linked ice-hydrogel.Soft Sci2021;1:11

[7] Xing J,Qu Y.Helical ionotropic gel-fiber sensor with omnidirectional strain perception for multidimensional motion correction in adolescent activity assessment.Soft Sci2025;5:37

[8] Crawford KE.De novo design of a new class of “hard-soft” amorphous, microphase-separated, polyolefin block copolymer thermoplastic elastomers.ACS Macro Lett2015;4:921-5

[9] Munzenrieder N,Petti L.Flexible self-aligned double-gate IGZO TFT.IEEE Electron Device Lett2014;35:69-71

[10] Zou S,de Vries J,Sakes A.A retrofit sensing strategy for soft fluidic robots.Nat Commun2024;15:539 PMCID:PMC10789869

[11] Fan Z,Huang Y.Superior energy storage capacity of polymer-based bilayer composites by introducing 2D ferroelectric micro-sheets.Nat Commun2025;16:1180 PMCID:PMC11782609

[12] Qiu Y,Plamthottam R.Dielectric elastomer artificial muscle: materials innovations and device explorations.Acc Chem Res2019;52:316-25

[13] Benouhiba A,Konstantinidi S,Perriard Y.The elastic frontier: dielectric elastomer actuators in healthcare technology.Smart Mater Struct2025;34:033001

[14] Cheng N,Gao Y.Ultra-elastic, durable, bio-degradable, and recyclable pulp foam as an air dielectric substitute for sustainable capacitive pressure sensing.Adv Funct Mater2025;35:2423122

[15] Shu L,Yu Y,Rao Z.Unique elastic, dielectric and piezoelectric properties of micro-architected metamaterials.J Mater Chem C2019;7:2758-65

[16] Zeng T,Li Q.Enhancing energetic disorder in all-organic composite dielectrics for high-temperature capacitive energy storage.Nat Commun.2025;16:5620 PMCID:PMC12216148

[17] Qian X,Zhu L.Fluoropolymer ferroelectrics: multifunctional platform for polar-structured energy conversion.Science2023;380:eadg0902

[18] Wang L,Peng J,Jiang S.A stretchable soft pump driven by a heterogeneous dielectric elastomer actuator.Adv Funct Mater2024;34:2411160

[19] Gao L,Wang L.Intrinsically elastic polymer ferroelectric by precise slight cross-linking.Science2023;381:540-4

[20] Kim J,Shi M.Fracture, fatigue, and friction of polymers in which entanglements greatly outnumber cross-links.Science2021;374:212-6

[21] Pan C,Malakooti MH.A liquid-metal-elastomer nanocomposite for stretchable dielectric materials.Adv Mater2019;31:1900663

[22] Yin LJ,Zhu J.Soft, tough, and fast polyacrylate dielectric elastomer for non-magnetic motor.Nat Commun2021;12:4517 PMCID:PMC8313586

[23] Liu Y,Tian Z.Self-powered and self-healable extraocular-muscle-like actuator based on dielectric elastomer actuator and triboelectric nanogenerator.Adv Mater2024;36:2309893

[24] Wang Y,Yuan Q,Bai Y.Significantly enhanced breakdown strength and energy density in sandwich-structured barium titanate/poly(vinylidene fluoride) nanocomposites.Adv Mater2015;27:6658-63

[25] Lang C,Matuszewski KE.Nanostructured block copolymer muscles.Nat Nanotechnol2022;17:752-8

[26] Wang S,Li X.Polymer-based dielectrics with high permittivity and low dielectric loss for flexible electronics.J Mater Chem C2022;10:6196-221

[27] Yue D,Zhang WC.Computational simulation for breakdown and energy storage performances with optimization in polymer dielectrics.Adv Funct Mater2023;33:2300658

[28] Yin G,Song F.Dielectric elastomer generator with improved energy density and conversion efficiency based on polyurethane composites.ACS Appl Mater Interfaces2017;9:5237-43

[29] Bonardd S,Kortaberria G,Leiva A.Dipolar glass polymers containing polarizable groups as dielectric materials for energy storage applications. A minireview.Polymers2019;11:317 PMCID:PMC6419174

[30] Li F,Wang L.Unlocking the elasticity in ferroelectrics by slight crosslinking.Chin J Struct Chem2025;44:100443

[31] Feng QK,Pei JY.Recent progress and future prospects on all-organic polymer dielectrics for energy storage capacitors.Chem Rev2022;122:3820-78

[32] Hu Q,Pan L.Slight-crosslinking: opening a new journey for the intrinsic elastification of ferroelectric polymers.Chemistry2025;31:e202500247

[33] Alhasadi MF,Federico S.Theory of uniformity applied to elastic dielectric materials and piezoelectricity.Eur J Mech A Solids2022;91:104391

[34] Liu L,Gu A.Percolative polymer composites for dielectric capacitors: a brief history, materials, and multilayer interface design.J Mater Chem A2020;8:18515-37

[35] Dakin T.Conduction and polarization mechanisms and trends in dielectric.IEEE Electr Insul Mag2006;22:11-28

[36] 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.Chem Rev2016;116:4260-317

[37] Yadegari A.Exploring modification strategies to enhance energy storage performance of BOPP dielectric films.J Mater Chem A2025;13:30768-95

[38] Wang B,Jiao Y.Two-layer materials of polyethylene and a carbon nanotube/cyanate ester composite with high dielectric constant and extremely low dielectric loss.Carbon2013;54:224-33

[39] Yang M,Guo M.High-energy-density and high efficiency polymer dielectrics for high temperature electrostatic energy storage: a review.Small2022;18:2205247

[40] Qin M,Wu H.Dielectric loss mechanism in electromagnetic wave absorbing materials.Adv Sci2022;9:2105553 PMCID:PMC8981909

[41] Tian G,Yang T.Insight into interfacial polarization for enhancing piezoelectricity in ferroelectric nanocomposites.Small2023;19:2207947

[42] Wei J.Intrinsic polymer dielectrics for high energy density and low loss electric energy storage.Prog Polym Sci2020;106:101254

[43] Rui G,Zhang S.Dilute nanocomposites: tuning polymer chain local nanostructures to enhance dielectric responses.Adv Mater2024;36:2311739

[44] Deng Y,Qu D.Emerging hydrogen-bond design for high-performance dynamic polymeric materials.ACS Mater Lett2023;5:480-90

[45] Chen L,You W.Construction of slide-ring polymers based on pillar[5]arene/alkyl chain host-guest interactions.Angew Chem Int Ed2025;64:e202417713

[46] Kim M,Kim E,Oh JH.Photo-crosslinkable organic materials for flexible and stretchable electronics.Mater Horiz2025;12:4573-607

[47] Kong VA,Laaser JE.Effect of cross-link homogeneity on the high-strain behavior of elastic polymer networks.Macromolecules2024;57:4670-9 PMCID:PMC11140753

[48] Deng J,Zhao J.Insights into the correlation of cross-linking modes with mechanical properties for dynamic polymeric networks.Angew Chem Int Ed2023;62:e202309058

[49] Zhao S,Yin L.CPBA/PVDF dielectric elastomer composites with high actuation performance under low electric field by optimizing the internal structure.Polymer2025;336:128867

[50] Park C,Koo M.Soft ferroelectrics enabling high-performance intelligent photo electronics.Adv Mater2021;33:e2004999

[51] Raji IO,Saha NK.Network polymer properties engineered through polymer backbone dispersity and structure.Angew Chem Int Ed2024;63:e202315200

[52] Zhang W,Bai Z,Qiu X.Solid-state electrolytes based on polyimides for lithium batteries: structures, key properties, synthesis methods and applications.Electrochem Energy Rev2025;8:33

[53] Chen P,Su J.Recent advances on high-performance polyaryletherketone materials for additive manufacturing.Adv Mater2022;34:2270360

[54] Wu C,Li Z.Molecular engineering: flexible temperature-invariant polymer dielectrics with large bandgap.Adv Mater2020;32:2070165

[55] Xiao Y,Mao J.Self-strengthening dielectric elastomer of triblock copolymer with significantly improved electromechanical performance under low voltage.Macromol Mater Eng2021;306:2000732

[56] He G,Wang C,Luo H.Achieving superior energy storage properties of all-organic dielectric polystyrene-based composites by blending rod-coil block copolymers.ACS Sustainable Chem Eng2021;9:8156-69

[57] de Sousa Jr RR,Da Silva LCE,Vidotti SE.High-performance block-copolymer-based dielectric elastomers with enhanced mechanical properties.ACS Appl Polym Mater2023;5:9505-14

[58] Liu Y,Jiang X,Huang X.All-organic cross-linked polysiloxane-aromatic thiourea dielectric films for electrical energy storage application.ACS Appl Energy Mater2020;3:5198-207

[59] Yang D,Kang H.New polyester dielectric elastomer with large actuated strain at low electric field.Mater Lett2012;76:229-32

[60] Luo H,Liu X,Chen S.Constructing novel high-performance dipolar glass polymer dielectrics by polar rigid/flexible side chains.ACS Appl Mater Interfaces2023;15:24470-82

[61] Gao L,Wang L.Highly elastic relaxor ferroelectrics for wearable energy storage.Mater Horiz2024;11:6150-7

[62] Xu T,Gao L.Intrinsic elastomer with remarkable dielectric constant via elastification of relaxor ferroelectric polymer.Adv Mater2024;36:2404001

[63] Panyukov S.Theory of flexible polymer networks: elasticity and heterogeneities.Polymers2020;12:767 PMCID:PMC7240557

[64] Rubinstein M.Elasticity of polymer networks.Macromolecules2002;35:6670-86

[65] Fan Y,Zhou X.Highly sensitive strain sensor from topological-structure modulated dielectric elastic nanocomposites.Adv Mater Technol2021;7:2101190

[66] Sun H,Sims MB.Architecture-transformable polymers: reshaping the future of stimuli-responsive polymers.Prog Polym Sci2019;89:61-75

[67] Li L,Rui G,Zhang QM.Dilute nanocomposites for capacitive energy storage: progress, challenges and prospects.Chem Sci2024;15:19651-68 PMCID:PMC11575606

[68] Xie Z,Xiao Y.The effect of filler permittivity on the dielectric properties of polymer-based composites.Compos Sci Technol2022;222:109342

[69] Huang X,Zhu Y,Jiang P.High-k polymer nanocomposites with 1D filler for dielectric and energy storage applications.Prog Mater Sci2019;100:187-225

[70] Han Y,Huang P.A dielectric elastomer containing bicomponent core-shell nanoparticles with enhanced electromechanical properties for flexible crawling Robots.ACS Appl Polym Mater2024;6:6667-78

[71] Zhang J,Zuo Y.Improving actuation strain and breakdown strength of dielectric elastomers using core-shell structured CNT-Al₂O₃.Compos Sci Technol2020;200:108393

[72] Huang B,Zhao Y.Al@SiO₂ core-shell fillers enhance dielectric properties of silicone composites.ACS Omega2023;8:35275-82 PMCID:PMC10536023

[73] Sun H,Sun H.Improved the high-temperature energy storage performance of PEI films via loading core-shell structured Al₂O₃@BaSrTiO₃ nanofillers.Ceram Int2024;50:43811-8

[74] Zhou W,Yuan M.Core-shell engineering of conductive fillers toward enhanced dielectric properties: a universal polarization mechanism in polymer conductor composites.Adv Mater2023;35:2207829

[75] Hussain A,Jawaid J.Interface-engineered core-shell nanoparticle embedded polymer nanocomposite demonstrating low voltage and temperature dependent tunable dielectric response.J Mater Chem A2025;13:30587-98

[76] Guo Y,Wu S.Enhanced tunable dielectric properties of Ba_0.6Sr_0.4TiO₃/PVDF composites through dual-gradient structural engineering.J Alloys Compd2022;920:166034

[77] Wang P,Sun Z,Bi J.Carrier gradient core-double shell structure with heterojunction transition layer for significantly enhancing dielectric properties.Chem Eng J2024;496:153968

[78] Wu W,Qiang Z.Inserting insulating barriers into conductive particle channels: a new paradigm for fabricating polymer composites with high dielectric permittivity and low dielectric loss.Compos Sci Technol2021;216:109070

[79] Guo R,Zhai D.Ultrahigh energy density in dielectric nanocomposites by modulating nanofiller orientation and polymer crystallization behavior.Adv Powder Mater2024;3:100212

[80] Pabba DP,Thiam A.Magnetic field assisted high performance triboelectric nanogenerators based on P(VDF-HFP)/NiFe₂O₄ nanofiber composite.Ceram Int2024;50:4178-89

[81] Li Z,Khuje S.Solution-shearing of dielectric polymer with high thermal conductivity and electric insulation.Sci Adv2021;7:eabi7410 PMCID:PMC8480926

[82] Wang L,Zhou X,Zhou K.Sandwich-structured all-organic composites with high breakdown strength and high dielectric constant for film capacitor.Compos Part A Appl Sci Manuf2019;117:369-76

[83] Shi Y,Plamthottam R.A processable, high-performance dielectric elastomer and multilayering process.Science2022;377:228-32

[84] Su Y,Lan J.A highly stretchable dielectric elastomer based on core-shell structured soft polymer-coated liquid-metal nanofillers.Chem Commun2020;56:11625-8

[85] Tang C,Dong L.In-situ confined transformation of Ti₃C₂T_x in electrospun SiC fiber matrix for optimized conductive loss and polarization loss.Chem Eng J2025;521:166507

[86] Zhang L,Wang C,Zhang H.Highly sensitive capacitive flexible pressure sensor based on a high-permittivity MXene nanocomposite and 3D network electrode for wearable electronics.ACS Sens.2021;6:2630-41

[87] Chen Y,Hu F.Microstructured polyfluoroacrylate elastomeric dielectric layer for highly stretchable wide-range capacitive pressure sensors.ACS Appl Mater Interfaces2023;15:58700-10

[88] Feng ZP,Qin J.Ultrasmall barium titanate nanoparticles modulated stretchable dielectric elastomer sensors with large deformability and high sensitivity.InfoMat2023;5:e12413

[89] Peng J,Dong H.Dielectric elastomer actuators with low driving voltages and high mechanical outputs enabled by a scalable ultra-thin film multilayering process.Adv Funct Mater2024;34:2411801

[90] Huang J,Liu R,Guo D.Polyvinyl chloride-based dielectric elastomer with high permittivity and low viscoelasticity for actuation and sensing.Nat Commun2023;14:1483 PMCID:PMC10023783

[91] Shi L,Lu S.Dielectric gels with ultra-high dielectric constant, low elastic modulus, and excellent transparency.NPG Asia Mater2018;10:821-6

[92] Tang T,Shen Z.Compressible polymer composites with enhanced dielectric temperature stability.Adv Mater2023;35:2209958

[93] Li T,Sun W.Constructing fluorinated triphenyl in carbonate copolymers toward flexible high energy-storable dielectric films with enhanced thermal resistance.Nano Energy2024;130:110105

[94] Kim SH,Avila R.Strain-invariant stretchable radio-frequency electronics.Nature2024;629:1047-54

[95] Hu W,Li J,Xie Z.New dielectric elastomers with variable moduli.Adv Funct Mater2015;25:4827-36

[96] Hu J,Wei T,Wan X.Low-voltage organic field-effect transistors using a phosphocholine-based polyampholyte dielectric.Macromolecules2025;58:5618-26

[97] Sun Q,Chen C,Mu Y.Functional zwitterionic polyurethanes as gate dielectrics for organic field-effect transistors.Adv Elect Mater2024;11:2400578

[98] Li W,Zhou Q,Liu Z.Harmonizing elastic modulus and dielectric constant of elastomers for improved pressure sensing performance.ACS Appl Mater Interfaces2024;16:32727-38

[99] He J,Xiao Y.Intrinsically anisotropic dielectric elastomer fiber actuators.ACS Materials Lett2022;4:472-9

[100] Yang L.High-performance electrically responsive artificial muscle materials for soft robot actuation.Acta Biomater2024;185:24-40

[101] Wang R,Xiao J.Multilayer assembly of dielectric actuators based on a reversibly crosslinkable silicone elastomer.Adv Funct Mater2025;36:e09974

[102] Zhang Y,Yu W.Dielectric elastomer with covalently charged interpenetrated polyacrylate network for large actuation strain under low driving electric field.Chem Eng J2025;520:165877

[103] Shu L,Zhang X.Partitioning polar-slush strategy in relaxors leads to large energy-storage capability.Science2024;385:204-9

[104] Zhang T,Yin C.Recent progress in polymer dielectric energy storage: from film fabrication and modification to capacitor performance and application.Prog Mater Sci2023;140:101207

[105] Cao Z,Sun F.Depolymerizable thermosetting dielectric elastomers toughened by sacrificial hydrogen bonds for sustainable capacitive strain-sensor.Adv Funct Mater2025;35:2505979

[106] Jiang Y,Wang Y.High energy harvesting performances silicone elastomer via filling soft dielectric with stretching deformability.Adv Mater2023;35:2300246

[107] Wang Z,Wang Y.Enhancing the energy conversion efficiency of dielectric elastomer generators via elastic energy storage and recovery.Appl Energy2025;379:124854

[108] Duan L,Li CH.A dielectric elastomer actuator that can self-heal integrally.ACS Appl Mater Interfaces2020;12:44137-46

[109] Yang D,Yang R.A rational design of bio-derived disulfide CANs for wearable capacitive pressure sensor.Adv Mater2024;36:2403880

[110] Madsen FB,Skov AL.Self-healing, high-permittivity silicone dielectric elastomer.ACS Macro Lett.2016;5:1196-200

[111] Zhang Y,Zhang R.Electrical and mechanical self-healing in high-performance dielectric elastomer actuator materials.Adv Funct Mater2019;29:1808431

[112] Huang B,Zhao Y.Efficient self-repairing high permittivity cyanosilicone dielectric elastomers.Polymer2023;280:126047

[113] Tan MWM,Lee PS.Rugged soft robots using tough, stretchable, and self-healable adhesive elastomers.Adv Funct Mater2021;31:2103097

[114] Wang H,Leng D,Ning H.Accelerating the discovery and optimization of metal-organic framework materials via machine learning.Adv Colloid Interface Sci2025;346:103671