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.
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.
A dicyclic, eight-shaped and a tricyclic, trefoil-shaped poly(THF) both having an alkyne group at the core position (II and III, respectively) have been introduced as versatile core-clickable kyklo-telechelic precursors. The prepolymer II has been prepared by an ESA-CF (electrostatic self-assembly and covalent fixation) process using an assembly (1a/2b), composed of two units of linear poly(THF) having N-phenylpyrrolidinium salt groups carrying one unit of a tetrafunctional carboxylate having an alkyne group as a counteranion. Alternatively, the prepolymer III has been produced through a click process using a cyclic poly(THF) precursor having an azide group (Ia), obtainable also by the ESA-CF technique, with a tripropargylated pentaerythritol derivative (2c) followed by the esterification with 4-pentynoic acid to introduce again an alkyne group. The subsequent click coupling reaction of II and III with a linear telechelic poly(THF) having azide groups (1b) afforded successfully novel tetra-and hexacyclic bridged-spiro hybrid polymer topologies, i.e., double-eight and double-trefoil constructions.
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