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The synthesis of novel dielectric elastomers that show a muscle-like actuation when exposed to a low electric field represents a major challenge in materials science. Silicone elastomers modified with polar side groups are among the most attractive dielectrics for such a purpose because of their high polarizability over a wide temperature and frequency range. Nitroaniline (NA) has a strong dipole moment, and therefore, its incorporation into silicone networks should allow the formation of elastomers with increased dielectric permittivity. However, incorporation of a large amount of NA into silicone needed to increase the dielectric permittivity is still challenging. In this work, we present the synthesis of polysiloxane elastomers modified with a large fraction of the nitroaniline (NA) polar group, following two different synthetic strategies. Both approaches allowed the formation of homogenous elastomers at the molecular level. These yellowish materials have a dielectric permittivity three times higher as compared to the reported NA-modified silicones. Additionally, they have excellent mechanical properties with low viscoelastic losses and a strain at break reaching 300%. Furthermore, the mechanical properties of these elastomers can be easily tuned by the content of cross-linkers used. The developed elastomers are highly stable in electromechanical tests and show an actuation strain of 8% at unprecedentedly low electric fields of 7.5 V/μm. The combination of properties such as high dielectric permittivity, large strain at break, low viscoelastic losses, fast and reversible actuation, and actuation at low electric fields is crucial for the new generation of dielectric elastomer materials that will find their way in applications ranging from artificial muscles, soft robots, sensors, and haptic displays to electronic skin.

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