This study further investigated the synergistic effect of micro- and nanofiller doping on matrix material space charges and breakdown characteristics. Accordingly, low-density polyethylene (LDPE) was used as the matrix material, and spherical ZnO particles with sizes of 30 nm and 1 µm were used as additives. Micro-ZnO/LDPE, nano-ZnO/LDPE, and micro-nano-ZnO/LDPE composites were prepared through melt blending. The crystalline morphologies of the composites were observed via polarized light microscopy. The composite crystallinity and melting peak temperature were measured via differential scanning calorimetry, and the micro- and nanoparticle dispersions in the matrix were observed via scanning electron microscopy. The test results showed that the particles were uniformly dispersed in the polyethylene matrix. The filler acted as a heterogeneous nucleation agent in the matrix. The crystal size decreased, thereby increasing the crystal quantity. The doping of inorganic ZnO particles improved the composite crystallinity. The ZnO/LDPE composites were subjected to DC breakdown, space charge, and dielectric spectrum tests. When the crystal arrangement of the sample was loose and its size was large, the breakdown process developed along a shorter path, and the field strength of the composite breakdown decreased. The order of AC and DC breakdown field strengths of the samples was as follows: micro-ZnO/LDPE < pure LDPE < micro-nano-ZnO/LDPE < nano-ZnO/LDPE. The DC and AC breakdown field strengths of the micro- and nano-ZnO/LDPE were 4.7% and 3.2% higher than those of the pure LDPE, respectively. Moreover, the DC and AC breakdown field strengths of the nano-ZnO/LDPE were 11.02% and 15.8% higher than those of the pure LDPE, respectively. The doping of inorganic ZnO particles restrained the space charge accumulation, and the residual charges decreased after short-circuit treatment. The dielectric constant of all nanocomposites was lower than that of LDPE, and the dielectric loss of all composites was higher than that of LDPE.
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