Polymer nanodielectrics characterized by good flexibility, processability, low dielectric loss and high dielectric permittivity are materials of interest for wearable electronic devices and intelligent textiles, and are highly in demand in robotics. In this study, an easily scalable and environmentally friendly method was applied to obtain polysiloxane/nanosilica nanocomposites with a large content of nanofiller, of up to 30% by weight. Nanosilica was dispersed both as individual particles and as agglomerates; in nanocomposites with a lower amount of filler, the former prevailed, and at over 20 wt% nanosilica the agglomerates predominated. An improvement of both the tensile strength and modulus was observed for nanocomposites with 5-15 wt% nanosilica, and a strong increase of the storage modulus was observed with the increase of nanofiller concentration. Furthermore, an increase of the storage modulus of up to seven times was observed in the nanocomposites with 30 wt% nanosilica. The tensile modulus was well fitted by models that consider the aggregation of nanoparticles and the role of the interface. The dielectric spectra showed an increase of the real part of the complex relative permittivity with 33% for 30 wt% nanosilica in nanocomposites at a frequency of 1 KHz, whereas the loss tangent values were lower than 0.02 for all tested nanodielectrics in the radio frequency range between 1 KHz and 1 MHz. The polysiloxane-nanosilica nanocomposites developed in this work showed good flexibility; however, they also showed increased stiffness along with a stronger dielectric response than the unfilled polysiloxane, which recommends them as dielectric substrates for wearable electronic devices.
Keywords: DMA; dielectric properties; flexible electronics; nanocomposites; polysiloxanes; silica nanoparticles.