Fiber dielectric elastomer actuators (DEAs) are potential candidates for the realization of artificial muscles owing to, amongst others, their linear actuation principle. In this work, a polydimethylsiloxane (PDMS) hollow fiber is prepared through a spinning method using the photocurable thiol-ene reaction between a thiol (R-SH) group and a double bond (C=C). The developed PDMS hollow fiber has an external diameter of 463 μm and uniform wall thickness of 78 μm, and presents tensile properties of ~600 % strain at break and 0.22 MPa strength, compared to these of the planar film of 86 % strain at break and 0.14 MPa tensile strength. Fiber DEAs are prepared by using ionic liquid as an inner electrode and ionogel as an electrical outer sheath. Due to the highly transparent PDMS elastomer layer and ionic liquid-based electrodes, the fiber DEA presents a transparency of ~91 % in a visible light spectrum. The fiber DEA exhibits a large linear strain of 9 % at 50 V/μm. Furthermore, the fiber DEA can be assembled into bundles for increased forces. The work presented herein provides a pathway for creating active soft matter with complex architectures to enable fast programmable actuation for multiple applications including invisible robots.
A novel magnetochromic elastomer with a strong and rapid magnetochromic effect has been developed. In the system, citric acid surface-functionalized magnetic nanoparticles (MNPs) are dissolved in poly(ethylene glycol) (PEG-200) and ultrasonicated into an emulsion with polydimethylsiloxane (PDMS) by speedmixing. The MNPs are shown to change from random to field-aligned under an external magnetic field and thus enables an on/off function. The developed elastomer shows a great potential for a wide range of applications, such as sensors and anticounterfeiting labels.
Dielectric elastomers (DEs) have shown a significant potential for actuation applications such as artificial muscles, due to their low weight, fast response, silent operation, and high efficiency. DEs with large actuation strain or low driving voltages are usually incorporated with high permittivity fillers. Ionic liquid (IL) presents a promising improvement on relative permittivity of DEs, however, its aggregation in the elastomer matrix by the physical blending modification has limited the improvement on actuating performances. In this study, a new strategy is developed to prepare high-performance PDMS elastomers by the formation of bis(1-ethylene-imidazole-3-ium) bromide between the PDMS backbones, after which the actuation performance of the IL-modified elastomer is investigated.
Dielectric elastomer actuators (DEAs) are usually operated at high voltage to induce sufficient electric pressure between two compliant electrodes sandwiching the dielectric elastomer. However, a harsh environment (e.g. humid environment combined with high voltage) often induces electrical breakdown (EB) of the DEAs, which results in pinhole formation or even tearing of the device, followed by macroscopic failure. Therefore, it is ideal for DEAs to be self-healing to extend robustness and lifetime, such as observed for biological muscles, which can be healed from injuries by inherent biological processes. Herein, we prepared a soft (Young’s modulus: 187 kPa) polydimethylsiloxane (PDMS) thermoplastic elastomer (TPE) to demonstrate an autonomous self-healing ability. The system exploits hydrogen bonding (H-bonding) in two types of transient cross-linkers: urea group serves as a sacrificial bond under loading and ureidopyrimidone (UPy) serves as a strong, load-carrying crosslinker. The PDMS TPE shows a crossover of the elastic moduli at 119 °C and highly frequency dependent elastic modulus. The DEA is prepared with compliant, corrugated silver electrodes on both sides of a corrugated PDMS TPE film. A maximum actuation strain (6.8 % in longitudinal direction) is achieved at 18.8 V μm-1. A further increase in potential does not increase the actuation strain, but EBs are observed on the electrodes and the actuation is maintained without any detrimental effects to the film despite the previous breakdown. The EBs do not form permanent pinholes, nor do they cause tearing of films. Instead, only the removal of the silver electrode is observed, which is the so-called self-clearing effect commonly observed for metallic electrodes. In combination with the self-clearing effect, the heat generated by the EBs allows the PDMS TPE to soften. The polymer molecules are then capable of flowing into the voids that were created at the initiation of the EBs. As a result, further propagation of the EB is hindered, and instead, an instantaneous and autonomous self-healing of the DEA is observed.
When a substrate-bonded silicone dielectric elastomer (DE) is subjected to high voltage, creasing, wrinkling, and cratering instabilities can be formed at the surface of the DE. This deformation, has been already demonstrated for the prevention and detachment of biofouling from the surface of DEs. In this work we add sensing capabilities to the anti-biofouling effect of active DE surfaces. The capacitance of the sensor is measured as a function of applied voltage, and the threshold voltage at which instabilities occur is identified. The formation of instabilities increases the capacitance of the device. When stiff biofouling material attach to the surface of the silicone, the threshold voltage necessary to develop instabilities on the surface of the silicone will increase and this can be used as a measure of attached species to the surface.
Enabling desirable actuations at low voltages for silicone based dielectric elastomer actuators (DEAs) is challenging. Reducing the thickness and increasing the softness of the silicone film are key approaches for this purpose. In this work, a super-stretchable silicone elastomer was characterized and used as DEA. The prepared elastomer can be stretched uniaxially to 2400% strain, allowing a significant thickness reduction through pre-stretches. Besides, it shows a moderate average elastic modulus of 0.32 MPa even at strains of 1000%-1500%. These properties favor its application in DEAs. Actuation results show that the elastomer was not only actuated to a high strain but also actuated at attractive voltages. Specifically, a 1 mm-thick elastomer with a pre-strain of 200%×200% was actuated 45% in area at 4 kV, and a 0.25 mmthick elastomer film with pre-strain of 600%×600% showed a 3% actuation strain at only 120 V. Considering its easy fabrication and excellent actuation performance at low voltages, the elastomer is promising in the application in DEAs.
Dielectric elastomers (DEs) can undergo very large spatial deformations in response to an externally applied electrical field, giving them significant potential as soft actuators. High-performance DEs are usually modified by high-permittivity additives, which are used to lower driving voltages. In this study, a novel high-permittivity soft additive (LMS-EIL) was developed via the combination of high-permittivity ionic liquid (IL) and chloropropyl-silicone, enabling good compatibility with the silicone matrix. The relative dielectric permittivity of the novel silicone oil additive was 9×104 times higher at 0.1Hz compared to pristine chloropropyl-silicone oil. High-permittivity silicone elastomers were then achieved via incorporation of this novel IL-grafted chloropropyl-silicone oil. The relative dielectric permittivity of elastomers modified with 10 parts per hundred rubber (phr) LMS-EIL increased from 3.0 (pure film) to 22 at 0.1Hz, while the Young’s modulus decreased steadily with increasing LMS-EIL concentration. A simplified figure of merit (Fom') was used to evaluate actuation performance, and was shown to be 8.1 for the elastomer incorporated with 10 phr LMS-EIL, indicating excellent potential for use as an actuator.
Slide-ring elastomers consist of mobile cross-links that can rearrange themselves within the network in contrast to conventional elastomers with fixed junctures. This unique feature affects the macroscopic mechanical properties of the sliding elastomers by imparting a distinct sliding elasticity that is caused by the distribution entropy of the sliding crosslinks. Slide-ring silicone elastomers exhibit two distinct time dependent elastic responses that can be credited to the conformational entropy of the polysiloxane chains and the distribution entropy of the threaded rings. In this work, the transition between rubber elasticity of the silicone chains and the sliding elasticity of the rings has been observed through linear viscoelastic studies. The extensional properties of the elastomers further corroborated the presence of two distinct time dependent viscoelastic profiles. This novel network structure presents the potential to design more intricate dielectric elastomer transducers with two distinctive modes of behavior determined by the operational speed of the system.
For silicone elastomers used as actuators, softness is key for enabling actuation at low voltages. Recently, an extremely soft (Young’s modulus < 50 kPa) silicone elastomer without cross-links has been reported by Goff et al. Besides its extreme softness, the elastomer was reported to almost completely recover (82%) from a 10-cycle elongation of more than 5000%. This observation challenges conventional elasticity theory of cross-linked elastomers because a network without covalent crosslinks should not be able to strain-recover to such extent. In this work, the elastomer is hypothesized to be formed from concatenated rings through heterodifunctional uni-molecular ring closure. It is found that the elastic properties of this uncross-linked elastomer can be described by the dynamics of concatenated rings, which act as pseudo-crosslinks and pseudo-entanglements. Isolated rings and dangling rings function as external solvents and internal solvents respectively, thereby contributing to the unprecedented softness. The ability to precisely control the ratio between concatenated and dangling rings is expected to lead to even softer dielectric elastomers paving the way forward for ultra-soft robotics without significant mechanical losses.
Based on aligned multi-walled carbon nanotubes (MWCNTs), a highly stretchable and conductive polydimethylsiloxane (PDMS)/ MWCNTs composite fiber has been fabricated through a simple, effective and environmental friendly method. The prepared fiber shows excellent stretchability (up to 360% strain) and conductivity (4 S/m) with only around 2wt% of MWCNTs. In addition, the prepared fiber exhibits increased conductivity under tensile strain and cyclic stretching, which makes it an interesting candidate for a wide variety of applications in electronics. An application as conductive wires demonstrates that the prepared fiber will provide a new possibility for the development of next generation electronics.
Dielectric elastomer (DE) sensors have great potential for applications in soft robotics, wearable devices and medical diagnostic. A novel pressure sensor with remarkably improved force sensing characteristics was obtained through combined usage of polydimethylsiloxane (PDMS) and ionic liquid (IL). The regenerated keratin from wool was added and dispersed homogeneously in the PDMS matrix acting as reinforcing fillers. The influence of the amount of IL on the electro-mechanical properties of the composites was investigated. One obvious result was that the permittivity of the ILcontaining elastomers increased dramatically with the increased amount of IL loaded. Furthermore, the sensitivity of the composite elastomers as pressure sensors was investigated by recording the response of the voltage when a small force is applied to the top surface of the pressure sensor. The elastomers with IL loaded exhibit excellent response of the voltage and the maximum sensitivity of the composite elastomer is 2.64 mV/N.
Biofouling accumulation on synthetic underwater surfaces presents serious economic problem for the marine industry. When a substrate-bonded dielectric elastomer (DE) is subjected to high voltage, deformations in form of creases can be formed at the surface of the DE. This deformation, has been already demonstrated for the prevention and detachment of biofouling from the surface of DEs. In this work, we add sensing capability to the anti-biofouling effect of active DE surfaces. A device consisting of a metallic plate, a Kapton sheet, and a thin silicone membrane is immersed in conductive solution, which acts as one electrode, with the metal plate being the second electrode. Two different conductive solutions were used 3.5 wt% NaCl and 20 wt% NaCl. The surface deformation of the silicone as a function of applied voltage is monitored under microscope in order to verify electrical measurements. Breakdown measurements of the dielectric material in different conductive solutions are also performed. Because the membrane is made from incompressible elastomer and bonded to a rigid substrate, voltages below the creasing threshold create no deformation in the membrane, and therefore no change in capacitance. Above the voltage threshold, creasing instabilities appear at the surface of the silicone, thus increasing the capacitance of the device. Therefore, the capacitance of the sensor is measured as a function of applied voltage, and the voltage at which the capacitance increases is the threshold voltage at which creases occur. Creases are identified when using both 3.5 wt% NaCl and 20 wt% NaCl as top electrode. Theoretical values of creasing voltage deviate from the experimental measurements. Type of conductive solution is shown to have no significant influence on a breakdown voltage.
Slide-ring elastomers have mobile cross-links that can slide on their axial polymers in a manner similar to a pulley on a zip line. This supramolecular network structure imparts unique mechanical properties to the elastomers, such as high deformability and low hysteresis upon cyclic loading, that are often favorable for dielectric elastomer actuators (DEAs). The utilization of this type of dynamic network for actuation has been limited by the low compatibility of slide-ring materials and common elastomer platforms used in DEAs. Here, a synthetic pathway is proposed to allow for incorporation of slide-ring cross-linkers into silicone networks.
Novel insights into the electromechanical failure of dielectric elastomers are presented. Measurements are conducted by coupling a high-speed camera to electrical breakdown strength equipment. It is shown that the breakdown behavior is far from simple since the thin elastomer film undergoes complex dimensional changes before the breakdown. Multiple geometries of the electrodes were investigated and different behaviors were observed. The breakdown patterns were categorized and the underlying theory behind this complex process will be presented.
Soft, stretchable and light-weight transducers are most sought after for research on advanced applications like stretchable electronics, soft robotics and energy harvesters. Stretchable electronics require elastomers that have high elongation at break, high dielectric permittivity and high breakdown strength. Commercial silicone elastomer formulations often do not encompass all the necessary properties required to function effectively as stretchable transducers but they are used out of familiarity. In this study, most commonly used commercial silicone formulations are formulated with different stoichiometry and also blends of these formulations are made in order to manipulate their resulting properties. The properties of these blends like ultimate stress and strain, Young’s modulus, dielectric permittivity and breakdown strength are investigated and mapped to identify those that have the best suited properties for fabricating soft stretchable devices. On a research level, Sylgard 184, Sylgard 186, Ecoflex 00-50, Ecoflex 00-30 and Ecoflex 00-10 are widely used for fabricating such soft devices and hence they will be worked upon in this study. The elastomers obtained using the methods of mixing illustrated here can act as a starting point for conceptualizing the feasibility of a product on research level.
Silicone elastomers are widely used due to the favourable properties, such as flexibility, durable dielectric insulation, barrier properties against environmental contaminants and stress-absorbing properties over a wide range of temperatures ≈ -100°C to 250°C. Additionally they are mechanically reliable over millions of deformation cycles, which makes them ideal candidates for dielectric elastomers and stretchable electronics. In research on dielectric elastomers and other emerging technologies, the most common silicone elastomer utilized is Sylgard 184. One of the main advantages of this formulation is the low viscosity which allows for easy processing resulting in almost defect-free samples. Furthermore, its curing is robust and not as sensitive to poisoning as other silicone elastomer formulations. Commonly, the shortcomings of the final properties of Sylgard 184 are overcome by mixing the base polymer and the curing agent in non‐stoichiometric ratios and also by blending it with softer types of commercially available elastomers. Researchers rarely formulate their own tailor‐made silicone elastomers, probably due to the scarcity of information in literature on how to do this. This report aims to equip the beginners in silicone research with knowledge on how to prepare silicone elastomers with specific properties without compromising the mechanical integrity of the elastomer and thereby avoiding mechanical failure. Here the main focus is put on designing and formulating soft, reliable, and reproducible elastomers.
Silicone elastomers have been heavily investigated as candidates for dielectric elastomers and are as such almost ideal candidates with their inherent softness and compliance but they suffer from low dielectric permittivity. This shortcoming has been sought optimized by many means during recent years. However, optimization with respect to the dielectric permittivity solely may lead to other problematic phenomena such as premature electrical breakdown. In this work, we investigate the electrical breakdown phenomena of various types of permittivity-enhanced silicone elastomers. Two types of silicone elastomers are investigated and different types of breakdown are discussed. Furthermore the use of voltage stabilizers in silicone-based dielectric elastomers is investigated and discussed.
High driving voltages currently limit the commercial potential of dielectric elastomers (DEs). One method used to lower driving voltage is to increase dielectric permittivity of the elastomer. A novel silicone elastomer system with high dielectric permittivity was prepared through the synthesis of siloxane copolymers, thereby allowing for the attachment of high dielectric permittivity molecules through copper-catalyzed azide-alkyne 1,3-dipolar cycloaddition (CuAAC). The synthesized copolymers allow for a high degree of chemical freedom, as several parameters can be varied during the preparation phase. Thus, the space between the functional groups can be varied, by using different dimethylsiloxane spacer units between the dipolar molecules. Furthermore, the degree of functionalization can be varied accurately by changing the feed of dipolar molecules. As a result, a completely tunable elastomer system, with respect to functionalization, is achieved. It is investigated how the different functionalization variables affect essential DE properties, including dielectric permittivity, dielectric loss, elastic modulus and dielectric breakdown strength, and the optimal degree of chemical functionalization, where these important properties are not significantly compromised, is also determined. Thus, the best overall properties were obtained for a silicone elastomer prepared with 5.6 wt% of the dipolar molecule 1-ethynyl-4-nitrobenzene. Here, a high increase in dielectric permittivity (~70%) was obtained without compromising other vital DE properties such as elastic modulus, gel fraction, dielectric and viscous loss and electrical breakdown strength.
Dielectric elastomers (DEs) have many favourable properties. The obstacle of high driving voltages, however, limits the commercial viability of the technology at present. Driving voltage can be lowered by decreasing the Young’s modulus and increasing the dielectric permittivity of silicone elastomers. A decrease in Young’s modulus, however, is often accompanied by the loss of mechanical stability and thereby the lifetime of the DE. New soft elastomer matrices with high dielectric permittivity and low Young’s modulus, with no loss of mechanical stability, were prepared by two different approaches using chloropropyl-functional silicone polymers. The first approach was based on synthesised chloropropyl-functional copolymers that were cross-linkable and thereby formed the basis of new silicone networks with high dielectric permittivity (e.g. a 43% increase). These networks were soft without compromising other important properties of DEs such as viscous and dielectric losses as well as electrical breakdown strength. The second approach was based on the addition of commercially available chloropropyl-functional silicone oil to commercial LSR silicone elastomer. Two-fold increase in permittivity was obtained by this method and the silicone oil decreased the Young’s modulus significantly. The viscous losses, however, also increased with increasing content of silicone oil. Cross-linkable chloropropyl-functional copolymers offer a new silicone elastomer matrix that could form the basis of dielectric elastomers of the future, whereas the chloropropyl silicone oil approach is an easy tool for improvement of the properties of existing commercial silicone elastomers.
The energy density of dielectric elastomers (DEs) is sought increased for better exploitation of the DE technology since an increased energy density means that the driving voltage for a certain strain can be lowered in actuation mode or alternatively that more energy can be harvested in generator mode. One way to increase the energy density is to increase dielectric permittivity of the elastomer. A novel silicone elastomer system with high dielectric permittivity was prepared through the development of interpenetrating networks from ionically assembled silicone polymers and covalently crosslinked silicones. The system has many degrees of freedom since the ionic network is formed from two polymers (amine and carboxylic acid functional, respectively) of which the chain lengths can be varied, as well as the covalent silicone elastomer with many degrees of freedom arising from amongst many the varying content of silica particles. A parameter study is performed to elucidate which compositions are most favorable for the use as dielectric elastomers. The elastomers were furthermore shown to be self-repairing upon electrical breakdown.
Liquid silicone rubbers (LSRs) have been shown to possess very favorable properties as dielectric electroactive polymers
due to their very high breakdown strengths (up to 170 V/μm) combined with their fast response, relatively high tear
strength, acceptable Young’s modulus as well as they can be filled with permittivity enhancing fillers. However, LSRs
possess large viscosity, especially when additional fillers are added. Therefore both mixing and coating of the required
thin films become difficult. The solution so far has been to use solvent to dilute the reaction mixture in order both to
ensure better particle dispersion as well as allowing for film formation properties. We show that the mechanical
properties of the films as well as the electrical breakdown strength can be affected, and that the control of the amount of
solvent throughout the coating process is essential for solvent borne processes. Another problem encountered when
adding solvent to the highly filled reaction mixture is the loss of tension in the material upon large deformations. These
losses are shown to be irreversible and happen within the first large-strain cycle.
Dielectric elastomers are being developed for use in actuators, sensors and generators to be used in various applications,
such as artificial eye lids, pressure sensors and human motion energy generators. In order to obtain maximum efficiency,
the devices are operated at high electrical fields. This increases the likelihood for electrical breakdown significantly.
Hence, for many applications the performance of the dielectric elastomers is limited by this risk of failure, which is
triggered by several factors. Amongst others thermal effects may strongly influence the electrical breakdown strength.
In this study, we model the electrothermal breakdown in thin PDMS based dielectric elastomers in order to
evaluate the thermal mechanisms behind the electrical failures. The objective is to predict the operation range of PDMS
based dielectric elastomers with respect to the temperature at given electric field. We performed numerical analysis with
a quasi-steady state approximation to predict thermal runaway of dielectric elastomer films. We also studied
experimentally the effect of temperature on dielectric properties of different PDMS dielectric elastomers. Different films
with different percentages of silica and permittivity enhancing filler were selected for the measurements. From the
modeling based on the fitting of experimental data, it is found that the electrothermal breakdown of the materials is
strongly influenced by the increase in both dielectric permittivity and conductivity.
A new approach based on silicone interpenetrating networks with orthogonal chemistries has been investigated with
focus on developing soft and flexible elastomers with high energy densities and small viscous losses. The
interpenetrating networks are made as simple two pot mixtures as for the commercial available silylation based
elastomers such as Elastosil RT625. The resulting interpenetrating networks are formulated to be softer than RT625 to
increase the actuation caused when applying a voltage due to their softness combined with the significantly higher
permittivity than the pure silicone elastomers.
The research on soft elastomers with high dielectric permittivity for the use as dielectric electroactive polymers (DEAP)
has grown substantially within the last decade. The approaches to enhance the dielectric permittivity can be categorized
into three main classes: 1) Mixing or blending in high permittivity fillers, 2) Grafting of high permittivity molecules onto
the polymer backbone in the elastomer, and 3) Encapsulation of high permittivity fillers. The approach investigated here
is a new type of encapsulation which does not interfere with the mechanical properties to the same content as for the
traditionally applied thermoplastic encapsulation. The properties of the elastomers are investigated as function of the
filler content and type. The dielectric permittivity, dielectric loss, conductivity, storage modulus as well as viscous loss
are compared to elastomers with the same amounts of high permittivity fillers blended into the elastomer, and it is found
that the encapsulation provides a technique to enhance some of these properties.
The development of elastomer materials with a high dielectric permittivity has attracted increased interest over the last years due to their use in for example dielectric electroactive polymers. For this particular use, both the electrically insulating properties - as well as the mechanical properties of the elastomer - have to be tightly controlled in order not to destroy favorable elastic properties by the addition of particles. In the following, expanded graphite in low concentrations (up to 5 wt%) are investigated as a possible candidate as filler materials in very soft elastomers, which by the addition of traditional fillers in the necessary amounts would either lose their stability or their softness. Furthermore the influence of several mixing procedures on the electrical and mechanical properties is investigated.
To our knowledge no known technologies or processes are commercially available for embossing microstructures and
sub-micron structures on elastomers like silicones in large scale production of films. The predominantly used
technologies to make micro-scale components for micro-fluidic devices and microstructures on PDMS elastomer are 1)
reaction injection molding 2) UV lithography and 3) photolithography, which all are time-consuming and not suitable for
large scale productions. A hot-embossing process to impart micro-scale corrugations on an addition curing vinyl
terminated PDMS (polydimethyl siloxane) film, which is thermosetting elastomer, was established based on the existing
and widely applied technology for thermoplasts. We focus on hot-embossing as it is one of the simplest, most costeffective
and time saving methods for replicating structures for thermoplasts. Addition curing silicones are shown to
possess the ability to capture and retain an imprint made on it 10-15 minutes after the gel-point at room temperature. This
property is exploited in the hot-embossing technology.
Elastomers currently used as transducers have not been designed with this specific application in mind and there is therefore a need for new target engineered materials to bring down driving voltages and increase actuator performance. A proposed method of optimization involves the development of new types of interpenetrating polymer networks (IPNs) to be used as dielectric elastomer (DE) transducers. This work demonstrates the use of polypropylene glycol (PPG) as a novel DE material. The IPNs formed were shown to exhibit excellent thermal stability and mechanical properties including lower tendency for viscous dissipation with higher dielectric permittivity compared to state of the art polydimethylsiloxane (PDMS) materials.
We demonstrate that the force output and work density of polydimethylsiloxane (PDMS) based dielectric elastomer transducers can be significantly enhanced by the addition of high permittivity titanium dioxide nanoparticles which was also shown by Stoyanov et al[1] for pre-stretched elastomers and by Carpi et al for RTV silicones[2]. Furthermore the elastomer matrix is optimized to give very high breakdown strengths. We obtain an increase in the dielectric permittivity of a factor of approximately 2 with a loading of 12% TiO2 particles compared to the pure modified silicone elastomer with breakdown strengths remaining more or less unaffected by the loading of TiO2 particles. Breakdown strengths were measured in the range from approximately 80-150 V/μm with averages of the order of 120-130 V/μm for the modified silicone elastomer with loadings ranging from 0 to 12%.
Polydimethylsiloxane (PDMS) elastomers are excellent materials for dielectric electroactive polymers (DEAPs) due to
their high efficiency and fast response. PDMS suffers, however, from low dielectric permittivity and high voltages are
therefore required when the material is used for DEAP actuators. In order to improve the dielectric properties of PDMS a
novel system is developed where push-pull dipoles are grafted to a new silicone compatible cross-linker. The grafted
cross-linkers are prepared by reaction of two different push-pull dipole alkynes as well as a fluorescent alkyne with the
new azide-functional cross-linker by click chemistry. The dipole cross-linkers are used to prepare PDMS elastomers of
various chains lengths providing different network densities. The functionalized cross-linkers are incorporated
successfully into the networks and are well distributed as determined by the fluorescent functional cross-linker and
fluorescence microscopy. The thermal, mechanical and electro-mechanical properties of PDMS elastomers of 0 wt% to
3.6 wt% of push-pull dipole cross-linker are investigated. An increase in the dielectric permittivity of 19 % at only
0.46 wt% of pure push-pull dipole is observed. Furthermore, the dielectric losses are found to be very low while the
electrical breakdown strengths are high and adequate for DEAP applications.
KEYWORDS: Data modeling, Silicon, Polymers, Protactinium, Finite element methods, Data storage, Electroluminescence, Neodymium, Chemical engineering, Mechanical engineering
Mechanical characterization of soft elastomers is usually done either by traditional shear rheometry in the linear
viscoelastic (LVE) regime (i.e. low strains) or by extensional rheology in the nonlinear regime. However, in many
commercially available rheometers for nonlinear extensions the measurements rely on certain assumptions such as a
predefined shape alteration and are very hard to perform on soft elastomers in most cases. The LVE data provides
information on important parameters for DEAP purposes such as the Young's modulus and the tendency to viscous
dissipation (at low strains only) but provides no information on the strain hardening or softening effects at larger strains,
and the mechanical breakdown strength. Therefore it is obvious that LVE can not be used as the single mechanical
characterization tool in large strain applications. We show how the data set of LVE, and large amplitude oscillating
elongation (LAOE)1 and planar elongation2,3 make the ideal set of experiments to evaluate the mechanical performance
of DEAPs. We evaluate the mechanical performance of several soft elastomers applicable for DEAP purposes such as
poly(propyleneoxide) (PPO) networks3,4 and traditional unfilled silicone (PDMS) networks5.
The effect of different fillers on the mechanical and dielectric properties of soft elastomers has been investigated. It was
found that the addition of a small amount of silica fillers would increase the Young's modulus significantly but not
simultaneously increase the tear strength sufficiently for processing as thin films. Addition of nanoclay and barium
titanate nanoparticles to the soft elastomers was shown to be very favorable for the enhancement of the dielectric
properties without increasing the Young's modulus significantly and could be used for DEAP material in e.g. microprocessing
where the tear strength is not crucial for processing. However, for elastomer film processing it is suggested
that a combination of the nanoclay or barium titanate with either silica particles or bimodal networks would give the
right tear strength together with the desired increased dielectric permittivity.
Commercial elastomer materials are available for dielectric electroactive polymer (DEAP) purposes but the applied
commercial elastomers have not been developed with the specific application in mind. It is therefore obvious that
optimization of the elastomer material should be possible. In this study we focus on optimization of the mechanical
properties of the elastomer and show that it is possible to lower the elastic modulus and still not compromise the other
required mechanical properties such as fast response, stability, low degree of viscous dissipation and high extensibility.
The elastomers are prepared from a vinyl-terminated polydimethyl siloxane (PDMS) and a 4-functional crosslinker by a
platinum-catalyzed hydrosilylation reaction between the two reactants. Traditionally, elastomers based on
hydrosilylation are prepared via a 'one-step two-pot' procedure (with a mix A and a mix B mixed in a given ratio). An
alternative network formulation method is adopted in this study in order to obtain an elastomeric system with controlled
topology - a so-called bimodal network. Bimodal networks are synthesized using a 'two-step four-pot' mixing procedure
which results in a nonhomogeneous network structure which is shown to lead to novel mechanical properties due to the
low extensibility of the short chains and the high extensibility of the long chains. The first ensures stability and the last
retards the rupture process thereby combining two desired properties for DEAP purposes without necessarily
compromising the viscous dissipation.
Several elastomers are prepared and tested for the linear viscoelastic behaviour, i.e. behaviour in the small-strain limit
(up to approximately 10% strain). The bimodal networks are, however, capable of extensions up to several times their
initial length but the focus here is the small-strain limit.
When using polymeric networks to EAP material, certain
requirements need to be fulfilled or at least partly fulfilled.
The networks need to be strong since the driving voltage goes as
the thickness of the film to the second power, but on the other
hand the networks need to be soft and flexible in order to provide
sufficiently motion. Several network parameters can be altered in
order to alter the network properties but it turns out that the
most obvious parameter - the chain length of the network reactants
- has moderately influence at molecular lengths above the
entanglement length only. The inter-chains entanglements dominate
the properties rather than the actual crosslinks. Since chain
lengths below the entanglement length result in hard networks, the
chain length alone does not constitute a tunable parameter.
Therefore, it is obvious to focus on controlling the
entanglements. One way to do this is to make the network in
solution and afterwards remove the solvent. This way the
entanglement contribution is lowered because network chains will
be surrounded by solvent molecules and therefore the number of
trapped entanglements between network chains will be lowered. The
chain length can then be used as an easily tunable parameter.
Dielectric elastomer actuators consist of an elastomer film sandwiched between compliant electrodes. They work as electrostatic actuators: when a large electric field is applied over the electrodes, the rubber is compressed and the elastomer film elongates in the film plane. The performance of dielectric elastomer actuators (DEA), when a constant potential is applied, is expressed in a universal equation where a combination of the elastomers materials properties enters through a single parameter - a figure of merit. The expansion of the actuator is related to the applied potential for a particular actuator geometry: an actuator that expands under constant width. The derivation takes finite elasticity of the elastomers into account. The figure of merit can be used as guide to optimizing elastomer properties for dielectric elastomer actuators. For very highly pre-strained elastomers, the equations no longer hold. Elastomers with optimal properties are not commercially available. Typical elastomers for electric applications, encapsulation of electronics take an example, show at least one materials property that diminish their performance in DEA. Elastomers are mapped in a diagram expressing the property space for DEA.
Dynamical properties of dielectric elastomer actuators depend upon both electric and mechanical properties of the elastomer. The viscoelastic mechanical properties are intimately connected to network structure of the elastomer. The connection between network structure and the various relaxation times for the rubber that determines its viscoelastic properties are described.
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