Tailoring molecular structure and electromechanical properties of polydimethylsiloxane elastomer for enhanced energy conversion efficiency

Abstract The molecular structure of dielectric elastomers dictates their mechanical, electrical, and properties to react under external stimuli, influencing their suitability for applications such as actuators, sensors, and energy harvesting devices. The molecular structure of polymers can be tailored by incorporating plasticizers and particulate fillers to achieve multifunctional properties. However, achieving a balance between flexibility and maintaining mechanical strength due to incorporation of fillers induced phase separation and compromised intermolecular interactions remains challenging. In the present work, polydimethylsiloxane (PDMS) composites are synthesized using plasticizer and particulate fillers, polyethylene glycol (H‐(OCH 2 CH 2 ) n OH) and titanium diboride (TiB 2 ) respectively in various concentrations using shear mixing and doctor blade casting technique. Molecular structure of synthesized PDMS composite is confirmed by observing peaks of Raman spectra sift, which exhibits robust CO bonds dominating for both fillers. Chain entanglement due to filler incorporation significantly affects the crosslink density of PDMS composite, it increases with the concentration of plasticizer and possesses inverse relation for particulate. Furthermore, interdependence of the filler types and concentration are found on the mechanical as well as electrical properties. The specific deformation energy exhibits a significant increase of 118.9% when comparing particulate to the plasticizer at concentration of 8 wt.%. Although plasticizer increases the actuation strain and energy conversion efficiency but decreases the electrical breakdown voltage in comparison to particulate. By systematically varying fillers concentration, subtle changes in multifunctional properties are achieved. Overall, this investigation provides a framework for tailoring dielectric elastomer composites with desired electromechanical characteristics through the amalgamation of filler types and crosslinking densities, all intricately tied to the molecular architecture for electromechanical sensors. Highlights Filler incorporation changes DE molecular structure and materials properties. Formation of additional bonds and micro‐capacitors in DE enhances capacitance. Actuation strain in DE depends on filler type and concentration. Energy conversion efficiency varies with the concentration of filler.