The free volume effects on the dielectric properties of the polymer are ambiguous, and the quantitative effect of free volume on the dielectric properties has rarely been systematically studied, especially in the high-elastic state dipolar (HESD) polymer. In this work, the free volume of dipolar poly(vinylidene fluoride) (PVDF) is regulated by the addition of Al2O3, which greatly increase the size of free volume holes. Then the effect of free volume on the dielectric properties of PVDF/Al2O3 composites is discussed. The greatly enlarged size of free volume holes is believed to potentially generate disparate effects on dielectric constant under different frequencies in such kinds of HESD polymer-based composites, bringing about more remarkable frequency dependence of the dielectric constant. The influence of atomic-scale microstructure based on free volume further clarifies the free volume effects on the dielectric properties and provides valuable insights for the research of dielectric behaviour of polymer composites, which is constructive to design novel dielectric materials and further optimize the dielectric properties of dipolar dielectric polymer composites.
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