The search for new materials and compositions, in which the phenomena of ferrimagnetism and ferroelectricity are closely coupled, is of great technological interest. In the present study, composite systems of (BaTiO3)(100-x)%/(CoNb0·02Fe1·98O4)x% where x = 0, 2, 5, 10, 20, and 100% were produced. Initially, BaTiO3 (BTO) was made by sol-gel combustion approach and CoFe1·98Nb0·02O4 (CoFeNbO) was made by hydrothermal method. Both compounds were then combined via solid-state reaction route to form the composite systems. According to X-ray diffraction, the pristine BTO and CoNbFeO display tetragonal and cubic structures, respectively, and all composite systems consisted of the cubic phase for BTO and spinel phase for CoNbFeO. Scanning electron microscopy showed a decrease in grain size (from 0.552 μm to 0.194 μm) and porosity (from 18.65% to 4.57%) as the CoNbFeO content increases from x = 0 to x = 20%, respectively. The influence of magnetic CoNbFeO content on the magnetic, ferroelectric, magnetoelectric coefficient, electric, and dielectric properties of composite systems has been investigated. The ferromagnetic and ferroelectric natures of diverse composite systems are reflected via the registered M-H and P-E loops at ambient temperature. A steady increase in magnetic parameters such as saturation magnetization and remanent magnetization is observed as the spinel ferrite CoNbFeO content increases. Similarly, the values of the electric coercivity increased from 1.65 kV/cm for x = 0% to 3.99 kV/cm for x = 20%. The frequency-dependent dielectric and electrical measurements were also investigated at various temperatures. By raising the measurement temperature, the dielectric polarization was found to increase for composite systems with x > 2%. Interestingly, the tangent loss was reduced for different composite systems in comparison to pristine BTO and CoNbFeO materials. The lowest tangent loss values were noticed for x = 5% composite system. All composite systems revealed good magnetoelectric coupling with coupling coefficient magnitudes up to a maximum value of ∼22.5 mV/cm.Oe, indicating that they can be potential candidates for use in advanced multifunctional electric devices.
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