Vegetable fillers for electric stimuli responsive elastomers

Dielectric elastomer actuators (DEAs) have been studied widely in recent years for artificial muscle applications, but their implementation into production is limited due to high operating voltages required. The actuation behavior of dielectric elastomer under an applied electric field is predicted by Maxwell's pressure and thickness strain equations. According to these equations, the best electromechanical response is achieved when the relative permittivity is high and elastic modulus is low. The potential source for additives increasing the relative permittivity of rubbers can be vegetable powders that have much higher dielectric constant than common elastomers. In the present research, the dielectric and actuation properties of polyacrylate rubber (ACM) were studied after the addition of different vegetable‐based fillers such as potato starch, corn starch, garlic, and paprika. The results were compared to ACM filled with barium titanate. The compounds containing vegetable fillers showed higher relative dielectric permittivity at 1 Hz frequency than the compounds containing barium titanate due to higher interfacial polarization. The actuation studies showed that lower electric fields are required to generate certain actuation forces when the starches and garlic are used in the rubber instead of barium titanate. Therefore, the vegetable‐based fillers can be used to improve actuation performance of DEAs. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45081.     

Plasticized thermoplastic polyurethanes for dielectric elastomers with improved electromechanical actuation

In this article, four different plasticizers are blended in thermoplastic polyurethane (PU) to improve its electromechanical actuation performance. The selected plasticizers include dibutyl phthalate, triphenyl phosphate, polyethylene glycol (PEG), and an unsaturated polyester PMG. The plasticization effect of various plasticizers on the mechanical properties, dielectric properties, and the electromechanical actuation of PU films is carefully characterized and compared. Results demonstrate that the actuated strain under low electric fields and the electromechanical coupling efficiency of PU can be substantially improved by blending with appropriate type and amount of plasticizers. The oligomer‐type plasticizers, PEG and PMG, act more efficiently in the improvement of actuation. An actuated strain in thickness of 1.54%, 140 times higher than that of pure PU, along with an electromechanical coupling efficiency of 0.60 under a low electric field of 5 V/μm was achieved for the PU plasticized with PMG suggesting an attractive approach toward advanced dielectric elastomer actuators. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45123.     

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.     

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.     

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.     

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.     

Enhancement of the actuation performance of dielectric triblock copolymers modified with additives

To enhance actuation performance without prestrain, an elastomeric acrylic triblock copolymer, poly(methyl methacrylate)‐block‐poly(n‐butyl acrylate)‐block‐poly(methyl methacrylate), was modified with two kinds of additives, oligomeric poly(n‐butyl acrylate) and the plasticizer dibutyl sebacate. An actuator modified with those additives showed about 6% strain, whereas the unmodified actuator showed only 1% strain for the same applied electric field without prestrain. In addition, actuation was attained at lower critical electric field strength (625 and 1000 V mm^?1 for modified and unmodified actuators, respectively). Upon increasing the amounts of the additives, the electrically induced actuation velocity and degree of deformation increased. These results are explained by the dielectric and mechanical properties of the elastomers. The dielectric constants for elastomers modified with dibutyl sebacate were larger than those for elastomers modified with oligomeric poly(n‐butyl acrylate). The initial tensile stresses of both of the modified elastomers were much smaller than that of unmodified elastomer. The results provide a route to enhancing actuation performance of dielectric elastomers without prestrain. Copyright © 2011 Society of Chemical Industry     

Enhancement of electromechanical properties of natural rubber by adding barium titanate filler: An electro-mechanical study

Natural rubber is one of the most potential electro-active polymers for sensors, actuators, and energy harvesting applications. Enhancing the characteristic properties of polymers by reinforcing with fillers that possess multifunctional attributes have attracted considerable attention. In the present study, barium titanate reinforced natural rubber composite is prepared by using two-roll mill mixing. Afterwards, mechanical, electrical, and electromechanical properties of the composites are extensively analyzed by reinforcing different amounts of barium titanate into the matrix of natural rubber. The fabricated dielectric composite shows excellent properties such as high dielectric constant, low dielectric losses, high dielectric breakdown strength, and extreme stretchability. It is observed that as the filler loading reaches the value of 11 parts per hundred rubber (phr), maximum agglomeration of the particles occurs. Maximum stretchability and highest ratio of dielectric constant to elastic modulus are obtained at 8 phr of barium titanate fillers and at the loading, a maximum actuation strain of 11.24% is achieved. This study provides a simple, economical, and effective method for preparing enhanced mechanical, electrical, and electromechanical properties of natural rubber composites, facilitating the wide applications of dielectric materials as actuators and generators.     

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.     

Effect of carbon black on the mechanical and dielectric properties of rubber ferrite composites containing barium ferrite

Fine particles of barium ferrite (BaFe₁₂O₁₉) were synthesized by the conventional ceramic technique. These materials were then characterized by the X‐ray diffraction method and incorporated in the natural rubber matrix according to a specific receipe for various loadings of ferrite. The rubber ferrite composites (RFC) thus obtained have several applications, and have the advantage of molding into complex shapes. For applications such as microwave absorbers, these composites should have an appropriate dielectric strength with the required mechanical and magnetic properties. The N330 (HAF) carbon black has been added to these RFCs for various loadings to modify the dielectric and mechanical properties. In this article we report the effect of carbon black on the mechanical and dielectric properties of these RFCs. Both the mechanical and dielectric properties can be enhanced by the addition of an appropriate amount of carbon black. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 89: 769–778, 2003     

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.     

Electric‐field response behaviors of chitosan/barium titanate composite hydrogel elastomers

Chitosan/barium titanate (BaTiO₃) composite hydrogel elastomers were prepared in the presence or absence of an applied direct‐current (dc) electric field. Scanning electron microscopy was used to observe the microstructure of the elastomers and the dispersion of particles in it. Tests of the storage moduli (Gs) of the elastomers were investigated with a dynamic mechanical analyzer. On this basis, the G increment and increment sensitivity were explored. The results show that the particles were sequentially dispersed, and the values of the G values for the elastomer were higher under an external applied dc electric field; this indicated that the composite elastomers exhibited excellent electric field response. Furthermore, the electric‐field response of the composite elastomers changed with the particle concentration, and the maximum response occurred when the mass fraction of BaTiO₃ was 2.0%. The G value of the composite elastomer with a BaTiO₃ weight percentage of 2.0 increased with increasing electric field; this revealed that the composite elastomer had a positive electric field response. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42094.     

Enhancement of dielectric constants of epoxy thermosets via a fine dispersion of barium titanate nanoparticles

In this study, we examined a facile approach for achieving a fine dispersion of barium titanate (BT) nanoparticles (NPs) in epoxy thermosets. First, the surfaces of BT NPs were modified with poly(ε‐caprolactone) (PCL) via a surface‐initiated ring‐opening polymerization approach. We found that the PCL‐grafted BT NPs were easily dispersed in epoxy thermosets. The fine dispersion of the PCL‐grafted BT NPs in the epoxy thermosets was evidenced by transmission electron microscopy and dynamic mechanical thermal analysis. We found that the organic–inorganic nanocomposites displayed significantly enhanced dielectric constants and low dielectric loss compared to the control epoxy. The nanocomposites containing 14.1 wt % BT NPs possessed dielectric constants as high as at a frequency of 10³ Hz. The dielectric loss was measured to be 0.002 at a frequency of 10³ Hz. The improved dielectric properties are accounted for the fine dispersion of the BT NPs in the epoxy thermosets. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43322.     

Dielectric relaxation behavior of conducting carbon black reinforced ethylene acrylic elastomer vulcanizates

The dielectric relaxation characteristics of conductive carbon black (CCB) reinforced ethylene acrylic elastomer (AEM) vulcanizates have been studied as a function of frequency (10¹–10⁶ Hz) at different filler loading over a wide range of temperatures (30–120°C). The effect of filler loadings on the dielectric permittivity (ε′), loss tangent (tan δ), complex impedance (Z*), and electrical conductivity (σ_ac) were studied. The variation of ε′ with filler loading has been explained based on the interfacial polarization of the fillers within a heterogeneous system. The effect of filler loading on the imaginary (Z″) and real (Z′) part of Z* were distinctly visible, which may be due to the relaxation dynamics of polymer chains at the polymer–filler interface. The frequency dependency of σ_ac has been investigated using percolation theory. The phenomenon of percolation in the composites has been discussed in terms of σ_ac. The percolation threshold (?_crit) occurred in the range of 20–30 phr (parts per hundred) of filler loading. The effect of temperature on tan δ, ε′, σ_ac, and Nyquist plots of CCB‐based AEM vulcanizates has been investigated. The CCB was uniformly dispersed within the AEM matrix as studied from the transmission electron microscope (TEM) photomicrographs. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Electro-thermal and -mechanical model of thermal breakdown in multilayered dielectric elastomers

Multiple breakdown phenomena may take place when operating dielectric elastomers. Thermal breakdown, which occurs due to Joule heating, becomes of special importance when using multilayered stacks of dielectric elastomers, due to the large volume-to-surface-area-ratio. In this article, a 2D axisymmetric finite-element model of a multilayered stack of dielectric elastomers is set up in COMSOL Multiphysics®. Both the electro-thermal and electro-mechanical couplings are considered, allowing for determination of the onset of thermal breakdown. Simulation results show that an entrapped particle in the dielectric elastomer drastically reduces the possible number of layers in the stack. Furthermore, the possible number of layers is greatly affected by the ambient temperature and the applied voltage. The performance of three hyperelastic material models for modeling the elastomer deformation are compared, and it is established that the Gent model yields the most restrictive prediction of breakdown point, while the Ogden model yields the least restrictive estimation.     

Characterization of barium titanate reinforced acrylonitrile butadiene rubber composites for flexible electronic applications: influences of barium titanate content

The aim of this study was to develop high dielectric constant flexible polymers with a highly efficient and cost‐effective approach using acrylonitrile butadiene rubber (NBR) as the polymer matrix and barium titanate (BT) as the high dielectric constant filler. The BT powder was synthesized with a solid‐state reaction and was characterized using a particle size analyzer, XRD, SEM and Fourier transform infrared spectroscopy. NBR/BT composites were fabricated using an internal mixer with various BT loadings up to 160 phr. The influence of BT loading on the cure characteristics and mechanical, dynamic mechanical, thermal, dielectric and morphological properties was determined. The incorporation of BT in the NBR matrix shortened scorch time and increased delta torque. The mechanical properties, thermal stability and dielectric constant were greatly improved and increased with BT loading. The results suggest that the reinforcement effect was achieved due to strong hydrogen bonding or polar–polar interactions between NBR matrix and BT filler. This is further corroborated by the good dispersion of BT filler in the NBR matrix observed with SEM imaging. These findings can be applied to produce high‐performance dielectric elastomers. © 2020 Society of Industrial Chemistry     

Influence of fillers and bonding agents on the viscoelasticity of highly filled elastomers

Highly filled elastomers such as solid propellants exhibit a complex nonlinear viscoelastic behavior. This work aimed at determining the influence of binder–filler and filler–filler interactions on the microstructure and the viscoelastic properties of the propellant using a design of experiments method. The influences of the filler fraction and of the filler–binder bonding agents (FBBA) were measured by swelling experiments and prestrained dynamic mechanical analyses. The results showed that FBBA react on the filler surface and concentrate the curing agents in the vicinity of the fillers. The nonlinearity of the viscoelastic behavior originated from filler–filler interactions that created high stress zones between fillers and therefore constrained the movements of the macromolecules of the binder. Filler–binder interactions induced by the FBBA increased the filler effective volume as well as the heterogeneous stress distribution in the microstructure. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40664.     

Mechanical,dielectric, and thermal properties of fluorosilicone rubber composites filled with silica/multiwall carbon nanotube hybrid fillers

In this work, hybrid fillers consist of modified silica (SiO₂) and multiwalled carbon nanotube (MWCNT) were used to improve the mechanical, dielectric, and thermal properties of fluorosilicone (FSR) composites via a direct mechanical mixing method. With the increase of CNT loading in SiO₂/CNT hybrid loading ratio, the tensile properties, dielectric constant, electrical conductivity, and thermal properties all increase without a sharp sacrifice of flexibility. The dielectric constant of FSR-S15/C5 achieved 7,370 @1 kHz, which is about four orders of the FSR-S20, and the dielectric loss remains as low as 0.676 @1 kHz. Therefore, the linkage of SiO₂ and FSR chains not only enhances the interfacial interaction between the fillers and FSR matrix but also decreases the agglomeration of the fillers in matrix. What is more, modified SiO₂ and CNT were designed as the effective hybrid filler to improve the performance of the polymeric matrix through synergic effect.     

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.     

钛酸钡纳米复合材料制备与性能研究

对钛酸钡颗粒进行羟基化和巯基官能化处理,将纳米银粒子成功接枝到钛酸钡颗粒表面制备了x Ag@BT颗粒(x为银质量分数,BT为钛酸钡),并用溶液共混法制备了Ag@BT/PVDF纳米复合材料(PVDF为聚偏氟乙烯)。结果表明,x Ag@BT颗粒为具有草莓结构的纳米颗粒,尺寸为2~16 nm的银粒子成功装饰在钛酸钡颗粒表面;纳米银粒子的引入可以降低复合材料在低频下的介电损耗和电导率,且当纳米银粒子质量分数为1.0%时复合材料的特征击穿强度达到最大值;与传统BT/PVDF纳米复合材料相比,1.0%Ag@BT/PVDF纳米复合材料具有更优良的电性能。