Electro-Thermal model of thermal breakdown in multilayered dielectric elastomers

Energy transduction of dielectric elastomers involves minute electrical and mechanical losses, both of which potentially increase the temperature within the elastomer. Thermal breakdown of dielectric elastomers occur when heat generated therein cannot be balanced by heat loss on the surface, which is more likely to occur in stacked dielectric elastomers. In this article an electro-thermal model of a multilayered dielectric elastomer able to predict the possible number of layers in a stack before thermal breakdown occurs is presented. Simulation results show that point of breakdown is greatly affected by an increase in surrounding temperature and applied electric field. Furthermore, if the stack diameter is large, thermal insulation of the cylindrical surface is a valid approximation. Two different expressions for the electrical conductivity are used, and it is concluded that the Frank-Kamenetskii expression is more conservative in prediction of point of breakdown than the Arrhenius expression, except at high surrounding temperature. © 2018 American Institute of Chemical Engineers AIChE J, 65: 859–864, 2019     

Theory progress and applications of dielectric elastomers

This paper summarizes the research progress of dielectric elastomer (DE) and its composite materials, including the introduction of materials, theoretical research development, and typical applications. First of all, the DE composite materials are introduced. Then, the theoretical research development of DEs is summarized. Finally, some applications as well as research prospects about DEs are listed.     

Energy harvesting performance of viscoelastic polyacrylic dielectric elastomers

Viscoelasticity dissipates the mechanical energy, leading to a reduction of energy conversion efficiency in both dielectric elastomer (DE) actuators and generators. By measuring the uniaxial tension-recovery experiments of very-high-bond-based DE, this article quantitatively presents the effect of viscoelasticity on energy harvesting performance of DE generators. By employing a DE strip energy harvester with constant surface charge, an analytical model is established to calculate the generated electrical energy and energy conversion efficiency. Numerical results demonstrate that viscoelasticity has a significant influence on DE energy harvesting performance.     

Glycerol as high‐permittivity liquid filler in dielectric silicone elastomers

A recently reported novel class of elastomers was tested with respect to its dielectric properties. The new elastomer material is based on a commercially available poly(dimethylsiloxane) composition, which has been modified by embedding glycerol droplets into its matrix. The approach has two major advantages that make the material useful in a dielectric actuator. First, the glycerol droplets efficiently enhance the dielectric constant, which can reach astonishingly high values in the composite. Second, the liquid filler also acts as a softener that effectively decreases the elastic modulus of the composite. In combination with very low cost and easy preparation, the two property enhancements lead to an extremely attractive dielectric elastomer material. Experimental permittivity data are compared to various theoretical models that predict relative permittivity changes as a function of filler loading, and the applicability of the models is discussed. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 44153.     

Improvement of actuation performance of dielectric elastomers by barium titanate and carbon black fillers

Dielectric elastomers are promising materials for actuators resembling human muscle. Among elastomers, acrylic rubbers (ACM) have shown good actuation performance but its use is limited by the high operating voltages required. The present work demonstrates that simultaneous incorporation of nanostructured carbon black and dielectric fillers offers an increase in a dielectric permittivity and a suitable modulus of the elastomers matrix, enabling an improved electro‐mechanical actuation performance at low voltages. By the use of reinforcing carbon black and barium titanate in an acrylic elastomer matrix a sixfold increase in the dielectric permittivity was realized. A fine tuning of the actuation stress and, consequently, actuation strain can be done by a judicial selection of the different filler concentrations in the soft rubber matrix. Finally, a synergistic effect of the fillers was observed in the improved actuation performance of the developed materials. This work may pave the way to design dielectric elastomers for actuator fabrication. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 44116.     

Extension limit,polarization saturation,and snap-through instability of dielectric elastomers

A dielectric elastomer is capable of large voltage-induced deformation, particularly when the voltage is applied on the verge of snap-through instability. A model is described which shows that the snap-through instability is markedly affected by both the extension limit of polymer chains and the polarization saturation of dipoles. The model may guide the search for high-performance dielectric elastomer transducers.     

Preparation and electrodeformation of silicone dielectric elastomers containing poly(propylene glycol diacetate) with different molecular weights

In this study, poly(propylene glycol diacetate)s (PPGDAs) with different molecular weights were obtained by the esterification reaction of poly(propylene glycol) and acetic anhydride. We effectively reduced the residual moisture and hydrophilicity of PPGDA. Then, poly(dimethyl siloxane) (PDMS) was modified by the addition of only 5 wt % PPGDA, which possessed a high dielectric constant (k) and a large actuated strain at a low electric field. PPGDA was used to enhance the molecular polarity because of the more polar oxygen atoms and the greater number of ester groups. The great increase in k and the low elastic modulus of the PPGDA–PDMS composites lead to a great increase in the electromechanical sensitivity. When the molecular weight of PPGDA was about 4000, the PPGDA–PDMS composites had the largest actuated strain. As a result, compared to the pure silicone elastomer (8.94%), it exhibited a greater strain of 17.31% at a low electric field of 10.5 V/μm (an increase of ca. 1.94 times). © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45329.     

Property reinforcement of silicone dielectric elastomers filled with self‐prepared calcium copper titanate particles

In this article, submicron and micron calcium copper titanate (CCTO) crystallites with different morphologies were successfully designed and prepared by directly thermal treatment method and molten salt method, respectively. Then, the silicone elastomer filled with self‐prepared CCTO particles had high dieletric constant, low dielectric loss, and actuated strain which was greatly improved at low electric field. The dieletric constant at 50 Hz obviously increased from 2.15 for pure silicone elastomer to 4.37 and 4.18 for the submicron and micron CCTO/poly (dimethyl siloxane) (PDMS) composites. The dielectric loss of the composites retained at a low value (less than 0.06). Meanwhile, the elastic modulus of CCTO/PDMS composites was increased slightly only with a good flexibility. Compared to pure silicone elastomer (2.25%), the submicron and micron CCTO/PDMS composites with 2 wt % content exhibited a greater strain of 7.69% and 9.83% at a low electric field of 5 V/μm. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42613.     

Investigation on static and dynamic performance of a hinge configuration with integrated dielectric elastomers

A rigid hinge frame combined with pre‐stretched dielectric elastomer (DE) films can form an active biological agonist–antagonist configuration. In this structure, the DE films undergo a constant deformation under a static voltage as well as specific reciprocating rotation under an alternative voltage. To theoretically investigate the static and dynamic performance, we establish the kinetic equation of the active hinge configuration. The computational static rotary angle exhibits a good fit with the experimental data from literature. Based on this model, static performance of this configuration when DE undergoes uniaxial and pure shear deformation is investigated. Subject to a small perturbation, the configuration may oscillate around the equilibrium state and the natural frequency can be obtained. By varying the pre‐stretch ratios, applied voltage, layer number, and the rotational inertia of the hinge, we can tune the natural frequency at a wide range. When the voltage is sinusoidal and varies continuously, the configuration resonates at multiple frequencies of excitation, known as harmonic and superharmonic resonance. Our research may serve as a guide to optimal design and provide insights into the performance of the hinge configuration, which can effectively expand the structure's application fields. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41630.     

Influences of porous reduction graphene oxide/molybdenum disulfide as filler on dielectric properties,thermal stability,and mechanical properties of natural rubber

A ternary composite system consisting of natural rubber (NR), porous reduced graphene oxide (rPGO), and molybdenum disulfide (MoS₂) was introduced for applying in the dielectric field, of which rPGO and MoS₂ hybrid conductive filler (rPGM) was prepared by an effective and environmentally friendly method-microwave reduction. And the well-dispersed NR composites (NGM) were made by the latex co-precipitation method. Due to the large specific surface area of rPGM itself and the synergistic dispersion of rPGO and MoS₂, it formed many stable interface structures with the NR matrix, which not only made the blend exhibit high elasticity and withstood large deformation as NR but also greatly improved the dielectric, mechanical and thermal stability of the NR matrix. Compared with neat NR, the dielectric constant of nanocomposite increased by 11 times in the presence of rPGM conductive filler, and the leakage current generated by direct contact of fillers was reduced due to the attachment of MoS₂ to the surface of rPGO; when 2% rPGM was added, the NR exhibited the highest tensile strength (21.3 MPa), elongation at break (495%), and abrasion resistance (0.165 cm⁻³); in addition, the thermal stability of the nanocomposite was also improved. These phenomena indicate that rPGM had great potential in conductive fillers and provided a reliable way for NR applications in the field of dielectric elastomers.     

Control of coefficient of thermal expansion in elastomers using boron nitride

The thermal expansion properties of three commercial elastomers; Pebax®, Estane® and Hytrel® modified with 2.5–10 wt % boron nitride were investigated. The glass transition temperatures of the filled materials were relatively unaffected; however boron nitride did effectively reinforce all the three elastomers as seen by dynamic mechanical analysis and tensile tests. The coefficients of thermal expansion of the composite materials do not obey the rule of mixtures and show a large decrease without the loss of ductility typically associated with filled elastomers. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 102: 5153–5161, 2006     

Effects of metal oxides on the dielectric and mechanical properties of silicone rubber composites

Polysiloxane dielectric elastomers have garnered a considerable deal of attention over the last decade due to their potential as electroactive soft materials. However, the intrinsic low dielectric constant of polysiloxanes has proven a serious limitation in their practical use. In this work, we controlled the dielectric properties of silicone rubber composites by changing the type and content of oxide fillers. The silicone-based dielectric elastomers with a high dielectric constant (5.21@1 kHz), low modulus (1.62 MPa), and high elongation (1100%) were successfully obtained. The effects of different types of metal oxides on the dielectric properties and mechanical properties of the prepared composites are further explored. Due to their excellent comprehensive features, these types of materials are expected to be applied in capacitive sensors, actuators, generators, and beyond.     

Imaging the effect of dielectric breakdown in a multilayered polymer film

The dielectric strength and energy storage capability of poly(vinylidene fluoride‐hexafluoropropylene) copolymer (P[VDF‐HFP]) films are enhanced by interleaving layers of PVDF copolymer with thin layers of polycarbonate (PC). To gain insight into the breakdown processes in such materials, focused ion beam (FIB) milling in conjunction with scanning electron microscopy (SEM) was used to study the effect of a breakdown on the film. FIB can sequentially mill cross sections that are each imaged by SEM. The technique can provide quasi‐3D images across the film and give a detailed view of the damage caused by an electrical breakdown. Here, breakdowns initiated using a needle‐plane electrode configuration were imaged. In homogeneous films, the damage was confined to the small volume at the pinhole site. In 32‐layer 50/50 PC/P[VDF‐HFP] multilayer films, damage extending laterally up to ～ 15 μm into the film along the layer interfaces was seen. In addition to the delamination, layer buckling and distortion were apparent. The damage varied with the sample orientation, but the images indicate that the interfaces play an important role in the breakdown. They suggest that modifying the interface properties can be a strategy to further improve the dielectric strength of multilayer polymer dielectric materials. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Mechanical,dielectric, and electromechanical properties of silicone dielectric elastomer actuators

Silicone elastomer actuators were investigated to develop a simple and industrially scalable product with improved mechanical properties, such as a low modulus, high tearing strength, and good resilience, and enhanced electromechanical actuation properties. Silicone elastomers were fabricated via a hydrosilylation addition reaction with a vinyl‐end‐functionalized poly(dimethyl siloxane) (V), a multivinyl‐functionalized silicone resin, and a crosslinker in the presence of a platinum catalyst. For the larger electromechanical actuation response, the silicone dielectric elastomer actuator had to have a larger molecular weight of poly(dimethyl siloxane), a smaller hardener content, and a resin‐free composition. However, the silicone elastomer actuators needed to include a small amount of resin to improve the tearing strength. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2014 , 131, 40030.     

Novel method for preparation of polyurethane elastomers with improved thermal stability and electrical insulating properties

A novel method was developed for the preparation of polyurethane with enhanced thermal stability and electrical insulation properties via the reaction of epoxy‐terminated polyurethane prepolymer (EPU) and poly(amic acid) (PAA). EPUs were synthesized from the reaction of glycidol with NCO‐terminated polyurethane prepolymers, which were prepared from the reaction of polycaprolactone‐based polyol (CAPA) of different molecular weights and some commercially available diisocyanates including hexamethylene diisocyante, toluene diisocyanate, and 4,4′‐methylene bis(phenyl isocyanate). PAA was prepared from the reaction of equimolar amounts of pyromellitic dianhydride and oxydianiline. The effects of PAA content, the nature of diisocyanate, and the molecular weight of CAPA on the mechanical, thermal, thermomechanical, and electrical properties of the final networks were investigated. The crosslink density of the samples was determined according to an equilibrium swelling method using the Flory–Rehner equation and was correlated to the structure of the final polymers. Gel content and activation energy of network formation in the absence and the presence of a tertiary amine catalyst were also studied. The results showed considerable improvement in the thermal, electrical, and mechanical properties compared to those of other common polyurethanes. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 103: 1776–1785, 2007     

Mechanical and thermal properties of polyurethane elastomers based on hydroxyl‐terminated polybutadienes and biopitch

Biopitch is a renewable source of polyol obtained from Eucalyptus tar distillation, which was studied as an active component of polyurethane (PU). The polymerization occurred in one step, with a mixture of biopitch and hydroxyl‐terminated polybutadiene polyols reacted with 4‐4′‐diphenyl methane diisocyanate in the presence of dibutyltin dilaurate. Solid‐state ¹³C‐NMR, IR spectroscopy, elemental analysis, and thermal analysis [thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC)] were used to characterize the biopitch. The biopitch sample showed an aromatic and oxygenated structure with great thermal stability at high temperatures. Multiphasic PUs were synthesized and characterized by IR spectroscopy (attenuated total reflectance), elemental analysis, thermal analysis (TGA and DSC), mechanical assays (tensile strength, elongation at break, toughness, hardness, and resilience), and water absorption resistance (ASTM D 570‐81). In a comparative study of the synthesized elastomers, biopitch content increased tensile strength and hardness and decreased thermal stability, elongation at break, and water absorption. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 88: 759–766, 2003     

Silicone rubbers for dielectric elastomers with improved dielectric and mechanical properties as a result of substituting silica with titanium dioxide

One prominent method of modifying the properties of dielectric elastomers (DEs) is by adding suitable metal oxide fillers. However, almost all commercially available silicone elastomers are already heavily filled with silica to reinforce the otherwise rather weak silicone network and the resulting metal oxide filled elastomer may contain too much filler. We therefore explore the replacement of silica with titanium dioxide to ensure a relatively low concentration of filler. Liquid silicone rubber (LSR) has relatively low viscosity, which is favorable for loading inorganic fillers. In the present study, four commercial LSRs with varying loadings of silica and one benchmark room-temperature vulcanizable rubber (RTV) were investigated. The resulting elastomers were evaluated with respect to their dielectric permittivity, tear and tensile strengths, electrical breakdown, thermal stability and dynamic viscosity. Filled silicone elastomers with high loadings of nano-sized titanium dioxide (TiO₂) particles were also studied. The best overall performing formulation had 35 wt.% TiO₂ nanoparticles in the POWERSIL® XLR LSR, where the excellent ensemble of relative dielectric permittivity of 4.9 at 0.1 Hz, breakdown strength of 160 V µm^?1, tear strength of 5.3 MPa, elongation at break of 190%, a Young’s modulus of 0.85 MPa and a 10% strain response (simple tension) in a 50 V μm^?1 electric field was obtained.     

Dynamic viscoelasticity and phenomenological model of electrorheological elastomers

Electrorheological elastomers (EREs) present a tunable viscoelasticity with the application of an electric field. For their application, it is necessary to investigate the viscoelasticity of the EREs under various loading conditions and establish an accurate constitutive model. In this study, anisotropic silicone‐rubber‐based EREs with 30 vol % TiO₂–urea core–shell particles were prepared under an orientation electric field. We evaluated their viscoelasticities by testing their shear stress–shear strain hysteresis loops under various electric fields, frequencies, and strain amplitudes. On the basis of the experimental data, a nonlinear, revised Bouc–Wen phenomenological model was established, and the parameters in the model were identified. The results indicate that the revised model could accurately describe the viscoelastic properties of the EREs within a low frequency. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45407.     

Electromechanical instability in silicone‐ and acrylate‐based dielectric elastomers

Electromechanical instability (EMI) is regarded as a significant factor in preventing dielectric elastomers (DEs) from achieving large voltage‐induced deformations. In this study, the strain‐stiffening effect was used to control the occurrence of EMI in DEs. The results show that the stretching ratio required to provide a feasible strain‐stiffening effect in silicone rubber (SR) was smaller than that needed for a commercial DE material, VHB 4910. The experimental data were compared with currently used models for the simulation of EMI in DEs. We found that EMI could be eliminated in the deformation of these elastomers when prestretching was used. Through the application of a prestretching ratio of above 2.0, EMI was suppressed in both the VHB 4910 and SR samples. The findings of this research are of great significance in the maximization of the electromechanical performance of DE materials. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 45733.     

Maximum actuation strain for dissipative dielectric elastomers with simultaneous effect of prestretch and temperature

A dielectric elastomer can generate giant deformation by the voltage actuation, but the deformation is often hindered by the electromechanical instability and “snap‐through deformation,” which may lead to electrical breakdown. In this study, for the first time, the mathematical model is established for dissipative dielectric elastomers in the dynamic model with simultaneous effect of prestretch and temperature in order to achieve maximum actuation strain. The deformation of the dissipative dielectric elastomer: VHB 4905/4910 is investigated for the two simple actuation methods: constant and ramping voltage actuation, respectively. The best combined conditions of voltage and prestretch to obtain a large deformation at different operating temperatures are studied in detail. Under the best combined conditions, the influences of three factors: voltage, prestretch, and temperature on the maximum actuation strain are analyzed. This study should offer a great help in the design of dielectric elastomer actuators, and give the guidance to the accomplishment of the large deformation of dissipative dielectric elastomer actuators. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 45850.