Inorganic and organic materials based polymer nanocomposite (PNC) films, comprising silica (SiO2) nanoparticles as inorganic filler and the polymer blend of poly(ethylene oxide) (PEO) and poly(vinyl pyrrolidone) (PVP) as organic matrix (i.e., (PEO–PVP)-x wt% SiO2; x = 0, 1, 3 and 5) have been prepared by the solution-casting method. These PNC films are characterized by employing the scanning electron microscopy (SEM), X-ray diffractometer (XRD), Fourier transform infrared (FTIR) spectroscopy, and the dielectric relaxation spectroscopy (DRS). The effect of SiO2 nanofiller on the spherulite and porous morphology, miscibility of the polymers, PEO crystallite size, the degree of crystallinity, polymer–polymer and polymer-nanoparticle interactions, and from 20 Hz to 1 MHz range dielectric and electrical dispersion behaviour and also the structural dynamics of these PNC materials have been investigated. The porous morphology, structures of miscible phases, and the PEO crystallite length greatly alter with the incorporation of merely 1 wt% SiO2 in the polymer blend matrix which further changes with the increase of nanofiller concentration up to 5 wt%. The real part of complex permittivity over the radio frequency range (20 kHz–1 MHz) for these PNC films is found about 2 and their dielectric loss tangent values below 0.03, at the room temperature, which are significantly low. The contribution of interfacial polarization effect at lower audio frequencies enhances the complex permittivity of these materials linearly in the range 2 to 4 with the decrease of frequency from 1 kHz to 20 Hz confirming their frequency tunable dielectric behaviour. The dielectric study of 3 wt% SiO2 containing PNC film in the temperature range 30–60 °C reveals its thermally activated dielectric characteristics, and the temperature dependent values of dielectric relaxation time and dc electrical conductivity obey the Arrhenius behaviour with activation energies in the range 0.2–0.3 eV. The dielectric and electrical parameters ascertain the promising applications of these PNC films in the development of novel electroactive functional materials, and also their use as the dielectric substrate and electrical insulating polymeric nanodielectrics for the fabrication of flexible-type naturally degradable organoelectronic devices.
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