A novel method allowing rapid production of reliable composites with increased dielectric constant and high dielectric strength for dielectric elastomer actuators (DEA) is reported. The promising approach using composites of conductive particles and insulating polymers generally suffers from low breakdown fields when applied to DEA devices. The present publication shows how to overcome this deficiency by using conductive polyaniline (PANI) particles encapsulated into an insulating polymer shell prior to dispersion. PANI particles are encapsulated using miniemulsion polymerization (MP) of divinylbenzene (DVB). The encapsulation process is scaled up to approximately 20 g particles per batch. The resulting particles are used as high dielectric constant (ϵ′) fillers. Composites in a polydimethylsiloxane (PDMS) matrix are prepared and the resulting films characterized by dielectric spectroscopy and tensile tests, and evaluated in electromechanical actuators. The composite films show a more than threefold increase in ϵ′, breakdown field strengths above 50 V μm−1, and increased strain at break. These novel materials allow tuning the actuation strain or stress output and have potential as materials for energy harvesting.

A one‐step process for the synthesis of elastomers with high permittivity, excellent mechanical properties and increased electromechanical sensitivity is presented. It starts from a high molecular weight polymethylvinylsiloxane, P1, whose vinyl groups serve two functions: the introduction of polar nitrile moieties by reacting P1 with 3‐mercaptopropionitrile (1) and the introduction of cross‐links to fine tune mechanical properties by reacting P1 with 2,2′‐(ethylenedioxy)diethanethiol (2). This twofold chemical modification furnished a material, C2, with a powerful combination of properties: permittivity of up to 10.1 at 104 Hz, elastic modulus Y10% = 154 kPa, and strain at break of 260%. Actuators made of C2 show lateral actuation strains of 20.5% at an electric field as low as 10.8 V μm–1. Additionally, such actuators can self‐repair after a breakdown, which is essential for an improved device lifetime and an attractive reliability. The actuators can be operated repeatedly and reversibly at voltages below the first breakdown. Due to the low actuation voltage and the large actuation strain applications of this material in commercial products might become reality.

Dielectric elastomer actuators are stretchable capacitors capable of a musclelike actuation when charged. They will one day be used to replace malfunctioning muscles supposing the driving voltage can be reduced below 24 V. This focus here is on polar dielectric elastomers and their behavior under an electric field. Emphasis is placed on all the features that are correlated with the molecular structure, its synthetic realization, and its impact on properties. Regarding the polymer class, the focus, to some degree, is on polysiloxanes because of their attractively low glass transition temperatures. This enables introduction of highly polar groups to the backbone while maintaining soft elastic properties. The goal is to provide a few guidelines for future research in this emerging field that may be useful for those considering entering this fascinating endeavor. Because of the large number of materials available, a few restrictions in the selection have to be applied.

Several polydimethylsiloxane elastomers were developed and investigated regarding their potential use as materials in dielectric elastomer actuators (DEA). A hydroxyl end‐functionalized polydimethylsiloxane was reacted with different crosslinkers and the electromechanical properties of the resulting elastomers were investigated. The silicone showing the best actuation at the lowest electric field was further used as matrix and compounded with encapsulated conductive polyaniline particles. These composites have enhanced properties including increased strain at break, higher dielectric constant as well as, gratifyingly, breakdown fields higher than that of the matrix. One of the newly synthesized composites is compared to the commercially available acrylic foil VHB 4905 (3M) which is currently the most commonly used elastomer for DEA applications. It was found that this material has little hysteresis and can be activated at lower voltages compared to VHB 4905. For example, when the newly synthesized composite was 30% prestrained, a lateral actuation strain of about 12% at 40 V μm−1 was measured while half of this actuation strain at the same voltage was measured for VHB 4905 film that was 300% prestrained. It also survived more than 100 000 cycles at voltages which are close to the breakdown field. Such materials might find applications wherever small forces but large strains at low voltages are required, in, for example, tactile displays.

The low frequency mechanical and dielectric behavior of three different elastomers has been investigated by dynamic mechanical analysis and dielectric spectroscopy, with the aim of accounting for the frequency dependence of the characteristics of the corresponding dielectric elastomer actuators. Satisfactory agreement was obtained between the dynamic response of the actuators and a simple model based on the experimental data for the elastomers, assuming that the relatively large prestrains employed in the actuators to have little influence on the frequency dependence of their effective moduli. It was thus demonstrated that the frequency dependence of the actuator strain is dominated by that of the mechanical response of the elastomer, and that the frequency dependence of the dielectric properties has a relatively minor influence on the actuator performance.