The lead-free x NiFe2O4 – (1-x) BaTiO3 (x = 0, 0.05, 0.1, 0.15) multiferroic composites were prepared via the solid-state sintering technique. Microstructure, multiferroic, and magnetodielectric properties of composites were investigated. According to the XRD data (from x = 5 to 15 wt%), the tetragonality factor (cT/aT) and unit cell volume of the BaTiO3 (BTO) crystal system diminished. Based on SEM images, ferromagnetic NiFe2O4 (NFO) grains are uniformly dispersed in the ferroelectric BTO matrix without additional reaction in the interfaces of two phases. The highest values of dielectric (dielectric constant (εr) ∼ 1905 and dielectric loss factor (tan δ) ∼ 0.049) and ferroelectric properties (saturation polarization (PS) ∼ 13 μC/cm2 and remnant polarization (Pr) ∼ 10 μC/cm2) are attained for x = 5 wt% due to the lowest NFO (non-ferroelectric) concentration. Also, with increasing ferrite concentration (up to 15 wt%), the ferroelectric properties of the composites show a gradual decrease. The saturation magnetization (MS) values rise due to increasing ferrite concentration (from 2 to 5 emu/g for x = 5 to 15 wt%). Moreover, coercivity (HC) drops from 150 to 110 Oe. The simultaneous observation of the ferroelectric and ferromagnetic characteristic hysteresis loops confirmed the multiferroic effect for x = 5, 10, and 15 wt%. The highest magnetodielectric constant (3 %) is obtained for x = 15 wt% multiferroic composite at the applied magnetic field of 6 kOe.
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