Elastomers based on polynorbornene with polar polysiloxane brushes for soft transducer applications

Abstract

Elastomers based on cross‐linked bottlebrush polymers combine an extreme softness at low strains with a strain‐stiffening effect, which makes them attractive as active components in dielectric elastomer actuators (DEA). Their main disadvantage concerns the small relative permittivity, which lies in the range of 3.5, requiring relatively high driving voltage in actuators. We synthesized a bottlebrush polymeric elastomer with polar brushes, which exhibit an enhanced dielectric permittivity of 4.4. Anionic ring‐opening polymerization of a polar cyclosiloxane afforded telechelic polar brushes, while ring‐opening polymerization of a norbornene macromonomer gave a bottlebrush polymer which was cross‐linked to elastomers by a thiol‐ene reaction. Elastomers with a small elastic modulus below 100 kPa, strain at break exceeding 100%, attractive elasticity, and small mechanical loss factors (tanδ) were achieved. Temperature‐dependent impedance measurements revealed a transition temperature of ‐95 °C and an interfacial polarization. The multigram scale synthesis demonstrates the potential for scaling up, which opens the door to broader applications of these materials beyond actuators, such as capacitive sensors, batteries, and electroluminescent devices. Notably, these devices operate at extremely low voltages where the dielectric breakdown does not limit their functionality, but still, the softness and the increased dielectric permittivity are a plus.