Development of the magnetodielectric properties of BaTiO3-CoFe2O4 multiferroic composites

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The lead-free x CoFe2O4 – (1-x) BaTiO3 (x= 0, 0.075, 0.15, 0.225, and 1) composites have been prepared via the solid-state process. The composites' microstructure, dielectric, ferroelectric, ferromagnetic, and magnetodielectric (MD) properties were investigated. Notably, XRD analysis indicates a decrease in the tetragonality factor (cT/aT) of the BTO phase, accompanied by an expansion of the unit cell as x increases from 7.5 to 22.5 wt.%. According to the FESEM images, the CoFe2O4 (CFO) grains are uniformly distributed in the matrix with the formation of no impurity phase. The optimal dielectric properties (dielectric constant (εr) ∼ 2018 and dielectric loss factor (tan δ) ∼ 0.16) and ferroelectric characteristics (saturation polarization (PS) ∼ 12 μC/cm2 and remnant polarization (Pr) ∼ 10 μC/cm2) are achieved at x=7.5 wt.%, attributed to the minimal presence of the non-ferroelectric CFO phase. By increasing the ferrite content (up to 22.5 wt.%), the ferroelectric properties of the samples showed a gradual diminution. Also, from x=7.5 to 22.5 wt.%, a sharp increase in the saturation magnetization (from 3.75 to 11.3 emu/g) and remnant magnetization (from 0.93 to 2.35 emu/g) values was observed, while the coercivity diminished from 475.8 to ∼ 272 Oe. The simultaneous observation of two ferroic characteristic hysteresis loops validated the multiferroicity of the composites (x=7.5, 15, and 22.5 wt.%). The maximum MD constant (4.68%) was measured for x=22.5 wt.% composite at the applied magnetic field of 7 kOe.