In this article, the nano-MgO particles were used as inorganic fillers, and polypropylene (PP) polymer was used as a matrix. The nano-MgO/PP composites were prepared by double melt blending. Using the polarization microscope (PLM) test and hot-stage microscope test, the crystalline morphology of PP and nano-MgO/PP with different mass fraction were observed. Using the differential scanning calorimetry (DSC) test, the parameters and crystallinity in the process of isothermal crystallization could be obtained. Additionally, the samples of pure PP and nano-MgO/PP composites were dealt with using a breakdown test and a dielectric frequency spectra test. From the experimental results, nano-MgO particle doping decreased the samples’ crystal size, and the crystalline structure was converted from large spherulites to fascicled crystallization. Additionally, the crystallization rate became fast and crystallinity increased. According to the breakdown test, the nano-MgO particle doping made the composites form small, dense spherulites. The breakdown developed through a longer path, so the composites’ breakdown strength rose greatly. When the mass fraction of nano-MgO particles was 3%, the shape parameter of the composites’ Weibull distribution β was larger, which illustrated that the nano-MgO particles were dispersed uniformly in the PP matrix. According to the dielectric frequency spectra test, the dielectric constant of different nanocomposites were all lower than which of pure PP, but the loss angle tangent values were all higher than which of pure PP.
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