Crosslinking Methodology for Imidazole-Grafted Silicone Elastomers Allowing for Dielectric Elastomers Operated at Low Electrical Fields with High Strains

[Image: see text] For improved actuation at low voltages of dielectric elastomers, a high dielectric permittivity has been targeted for several years but most successful methods then either increase the stiffness of the elastomer and/or introduce notable losses of both mechanical and dielectric nature. For polydimethylsiloxane (PDMS)-based elastomers, most high-permittivity moieties inhibit the sensitive platinum catalyst used in the addition curing scheme. In contrast to the classical addition curing pathway to prepare PDMS elastomers, here, an alternative strategy is reported to prepare PDMS elastomers via the crosslinking reaction between multifunctional imidazole-grafted PDMS with difunctional bis(1-ethylene-imidazole-3-ium) bromide ionic liquid (bis-IL). The prepared IL-elastomer entails uniformly dispersed IL and presents stable mechanical and dielectric properties due to the covalent nature of the crosslinking as opposed to previously reported physical mixing in of ILs. The relative permittivity was improved up to 200% by including the bis-IL in the elastomer, and Young’s modulus was around 0.04 MPa. As a result of the excellent combination of properties, the dielectric actuator developed exhibits an area strain of 20% at 15 V/μm. The novel strategy to prepare PDMS elastomers provides a new paradigm for achieving high-performance dielectric elastomer actuators by a simple methodology.