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In this work, the dielectric properties of nanocomposites based on poly(2,2,2‐trifluoroethyl methacrylate) copolymer (PMATRIF) and vinylbenzyl‐functionalized montmorillonite (MMT) nanoparticles prepared via in situ free radical polymerization were studied. The effect of different loadings of (MMT) filler (in weight ratios of 1, 3, and 5%) on the molecular dynamics and polarization of PMATRIF was investigated using broadband dielectric spectroscopy from 10−1 to 106 Hz and at temperatures between 20 and 170°C. For PMATRIF matrix, the real part ε′ and the imaginary part ε″ of the dielectric permittivity curves revealed four dielectric processes β, α, αβ, and ionic conduction phenomenon. Furthermore, it was found that incorporating MMT led to an increase in the dielectric losses and generated additional relaxation processes known as Maxwell–Wagner Sillars polarization. Calculation of the activation energy for the different processes revealed that α relaxation followed the Vogel–Fulcher–Tammann–Hesse dependency while the other processes were suitably fitted with the Arrhenius law. In order to probe matrix/MMT interface properties, dielectric strength of the interfacial polarization Δε is calculated by fitting the dielectric permittivity through the known Havriliak–Negami model. POLYM. COMPOS., 40:3333–3341, 2019. © 2018 Society of Plastics Engineers

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