Ceramic/polymer dielectric composites show significant potential for energy storage devices in advanced microelectronic applications. However, an excessive quantity of inorganic nanofillers within the polymeric matrix can lead to a substantially unequal distribution of the electric field, which may impede the improvement of energy storage density. Herein, 0.94Bi0.5Na0.5TiO3-0.06BaTiO3 (BNBT6) nanoparticles were synthesized using a combined solid-phase method followed by sieving. The silane coupling agent KH560 was used to modify the nanoparticles. Additionally, polyphenylene oxide (PPO), polytetrafluoroethylene (PTFE), and perfluoroalkyl (PFA) were utilized as matrices. The surface modification enhanced the interfacial coupling interaction between BNBT6 and the polymers, resulting in a lower concentration of interfacial hole defects. The findings demonstrated that BNBT6@KH560/PPO nanocomposites attained a high Wrec (2.71 J cm−³) and an excellent of η ∼ 81.1 % with 50 wt% BNBT6@KH560 nanofiller at 1550 kV cm−1. Furthermore, the exceptional frequency and thermal stability of BNBT6@KH560/PPO nanocomposites made it a strong contender for future portable energy devices. This work presents a feasible solution for synthesizing high-performance dielectric nanocomposites using straightforward preparation techniques.
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