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Dielectric polymer nanocomposites are considered as one of the most promising insulation material candidates for future capacitive energy storage applications, providing tailorability of charge trapping and transport properties at the nanometric level which is a key for increased dielectric performance of biaxially oriented polypropylene (BOPP) for metallized film capacitors in high-voltage direct current (HVDC) applications. In this study, a comprehensive investigation of morphology and dielectric performance of pilot-scale BOPP nanocomposites with hexamethyldisilazane (HMDS)-treated hydrophobic fumed silica nanoparticles was carried out, providing critical perspectives on the performance and challenges of PNCs for thin film capacitors also in a broader context. In non-oriented cast films, incorporation of nanosilica modified the crystallization kinetics and α/β-crystalline spherulitic morphology of polypropylene and reduced the accumulation of space charge under a DC electric field. The nanocomposites exhibited promising dispersion characteristics in the nano-scale, however, the low amount of micron-sized agglomerates inherently present in commercial fumed silica persisted in the compounds which can become critical for thin film applications. Subsequently, biaxial-stretching-induced morphology development and dielectric properties of silica-BOPP nanocomposites were evaluated, highlighting the role of precursor morphology and film processing in the silica-BOPP film morphology, defects and dielectric performance. Charge trapping and transport properties of silica-BOPP films were investigated by isothermal and thermally stimulated techniques under high DC electro-thermal stresses, indicating profound modification of the trap density of states brought about by nanosilica. This resulted in more homogeneous space charge distribution and reduced temperature- and field dependent DC conductivity at 100 °C in comparison to neat BOPP under moderate field stresses (

New potential High Voltage Direct Current (HVDC) cable insulation materials based on nanocomposites are developed in this study. The nanocomposites are produced by blending of polypropylene (PP), propylene-ethylene copolymer (PP–HI) and a modified fumed silica (A-silica) in a concentration of 1 and 2 wt %. The A-silica is successfully modified with (3-aminopropyl)triethoxysilane (APTES) via a solvent-free method, as proven by infrared spectroscopy, thermogravimetry and transmission electron microscope mapping. A-silica in the polymer matrix acts as a nucleating agent resulting in an increase of the crystallization temperature of the polymers and a smaller crystal size. Moreover, the silica addition modified the crystals morphology of the unfilled PP/PP-HI blend. The composite containing A-silica with 2 wt% contains bigger-size silica clusters than the composite filled with 1 wt%. The composite with the higher A-silica concentration shows lower space charge accumulation and a lower charge current value. Besides, much deeper traps and lower trap density are observed in the composite with 2 wt% A-silica addition compared to the one with a lower concentration. Surprisingly, the presence of silica clusters with dimensions of more than 200 nm exhibit a positive effect on reducing the space charge accumulation. However, the real cause of this improvement might be due to change of the electron distribution stemming from the amine-amine hydrogen bond formation, or the change of the chain mobility due to the presence of occluded polymer macromolecules constrained inside the high structure silica clusters. Both phenomena may lead to a higher energetic barrier of charge de-trapping, thus increasing the depth of the charge traps. publishedVersion

This study compares different polymer-nanofiller blends concerning their suitability for application as insulating thermoplastic composites for High Voltage Direct Current (HVDC) cable application. Two polymer blends, PP/EOC (polypropylene/ethylene-octene copolymer) and PP/PP-HI (polypropylene/ propylene - ethylene copolymer) and their nanocomposites filled with 2 wt.% of fumed silica modified with 3-aminopropyltriethoxysilane were studied. Morphology, thermal stability, crystallization behavior dynamic relaxation, conductivity, charge trap distribution and space charge behavior were studied respectively. The results showed that the comprehensive performance of the PP/PP-HI composite is better than the one of the PP/EOC composite due to better polymer miscibility and flexibility, as well as lower charging current density and space charge accumulation. Nanosilica addition improves the thermal stability and dielectric properties of both polymer blends. The filler acts as nucleating agent increasing the crystallization temperature, but decreasing the degree of crystallinity. Dynamic mechanical analysis results revealed three polymer relaxation transitions: PP glass transition ( $\beta$ ), weak crystal reorientation ( $\alpha 1$ ) and melting ( $\alpha 2$ ). The nanosilica introduced deep traps in the polymer blends and suppressed space charge accumulation, but slightly increased the conductivity. A hypothesis for the correlation of charge trap distribution and polymer chain transition peaks is developed: In unfilled PP/EOC and PP/PP-HI matrices, charges are mostly located at the crystalline-amorphous interface, whereas in the filled PP/EOC/silica and PP/PP-HI /silica composites, charges are mostly located at the nanosilica-polymer interface. Overall, the PP/PP-HI (55/45) nanocomposite with 2 wt.% modified silica and 0.3 wt.% of antioxidants making it $a$ promising material for PP based HVDC cable insulation application with $a$ reduced space charge accumulation and good mechanical properties.