Integrating nano- to micro-sized dielectric fillers to elastomer matrices to form dielectric composites is one of the commonly utilized methods to improve the performance of dielectric elastomer actuators (DEAs). Barium titanate (BaTiO3) is among the widely used ferroelectric fillers for this purpose; however, calcium copper titanate CaCu3Ti4O12 (CCTO) has the potential to outperform such conventional fillers. Despite their promising performance, CCTO-based dielectric composites for DEA application are studied to a relatively lower degree. Particularly, the composites are characterized for a comparably small particle loading range, while critical DEA properties such as breakdown strength and nonlinear elasticity are barely addressed in the literature. Thus, in this study, CCTO was paired with polydimethylsiloxane (CH3)3SiO[Si(CH3)2O]nSi(CH3)3 (PDMS), Sylgard 184, to gain a comprehensive understanding of the effects of particle loading and size on the dielectric composite properties important for DEA applications. The dielectric composites’ performance was described through the figures of merit (FOMs) that consider materials’ Young’s modulus, dielectric permittivity, and breakdown strength. The optimum amounts of the ferroelectric filler were determined through the FOMs to maximize composite DEA performance. Lastly, electromechanical testing of the pre-stretched CCTO-composite DEA validated the improved performance over the plain elastomer DEA, with deviations from prediction attributed to the studied composites’ nonlinearity.

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