Solvent‐Free Synthesis and Processing of Conductive Elastomer Composites for Green Dielectric Elastomer Transducers

Stretchable electrodes are more suitable for dielectric elastomer transducers (DET) the closer the mechanical characteristics of the electrodes and elastomer are. Here, a solvent‐free synthesis and processing of conductive composites with excellent electrical and mechanical properties for transducers are presented. The composites are prepared by in situ polymerization of cyclosiloxane monomers in the presence of graphene nanoplatelets. The low viscosity of the monomer allows for easy dispersion of the filler, eliminating the need for a solvent. After the polymerization, a cross‐linking agent is added at room temperature, the composite is solvent‐free screen‐printed, and the cross‐linking reaction is initiated by heating. The best material shows conductivity σ = 8.2 S cm–1, Young's modulus Y10% = 167 kPa, and strain at break s = 305%. The electrode withstands large strains without delamination, shows no conductivity losses during repeated operation for 500 000 cycles, and has an excellent recovery of electrical properties upon being stretched at strains of up to 180%. Reliable prototype capacitive sensors and stack actuators are manufactured by screen‐printing the conductive composite on the dielectric film. Stack actuators manufactured from dielectric and conductive materials that are synthesized solvent‐free are demonstrated. The stack actuators even self‐repair after a breakdown event. A novel synthetic strategy to obtain stretchable electrodes for dielectric elastomer transducers is presented. Their synthesis from monomers, as well as their processing into devices, is completely solvent‐free. The electrode can be easily screen‐printed on virtually any substrate without interfering and does not delaminate under operation.