Aluminum nanoparticle/acrylate copolymer nanocomposites for dielectric elastomers with high dielectric constants

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Dielectric elastomers are useful for large-strain actuation and energy harvesting. Their application has been limited by their low dielectric constants and consequently high driving voltage. Various fillers with high dielectric constants have been incorporated into different elastomer systems to improve the actuation strain, force output and energy density of the compliant actuators and generators. However, agglomeration may happen in these nanocomposites, resulting in a decrease of dielectric strength, an increase of leakage current, and in many instances the degree of enhancement of the dielectric constant. In this work, we investigated aluminum nanoparticles as nanofillers for acrylate copolymers. This metallic nanoparticle was chosen because the availability of free electrons could potentially provide an infinite value of dielectric constant as opposed to dielectric materials including ferroelectric nanocrystals. Moreover, aluminum nanoparticles have a self-passivated oxide shell effectively preventing the formation of conductive path. The surfaces of the aluminum nanoparticles were functionalized with methacrylate groups to assist the uniform dispersion in organic solutions and additionally enable copolymerization with acrylate copolymer matrix during bulk polymerization, and thus to suppress large range drifting of the nanoparticles. The resulting Al nanoparticle-acrylate copolymer nanocomposites were found to exhibit higher dielectric constant and increased stiffness. The leakage current under high electric fields were significantly lower than nanocomposites synthesized without proper nanoparticle surface modification. The dielectric strengths of the composites were comparable with the pristine polymers. In dielectric actuation evaluation, the actuation force output and energy specific work density were enhanced in the nanocomposites compared to the pristine copolymer.