Room-temperature multiferroic (magnetoelectric–magnetodielectric) coupling properties of hybrid microwave-sintered (1 − x)BaZr_0.25Ti_0.75O₃ − xCo_0.9Ni_0.1Fe₂O₄ lead-free electromagnetic composites

This paper reports on the systematic investigation of the room-temperature magnetoelectric and magnetodielectric coupling coefficients on adding ferromagnetic phase (xCo_0.9Ni_0.1Fe₂O₄, where x = 0.1, 0.2, 0.3, and 0.4) to the non-toxic lead-free ferroelectric phase (BaZr_0.25Ti_0.75O₃) prepared via efficient, ultrafast, eco-friendly hybrid microwave sintering at 1100 °C. Rietveld’s refinement of the observed diffraction patterns reflects mixed-phase cubic and tetragonal crystal symmetries with space group Pm3m and P4mm for the ferroelectric phase and cubic Fd-3m for a ferromagnetic phase in each composite which was further verified through micro-Raman spectroscopy. Ferroelectric-ferrite composite at x = 0.2, i.e., 0.8(BaZr_0.25Ti_0.75O₃) − 0.2(Co_0.9Ni_0.1Fe₂O₄), had highest magnetoelectric and magnetodielectric coupling coefficients α_ME= 2.71 mV / cm Oe and MD (%) = 5.19 at 1 kHz applied frequency, respectively. The existence of both ferroelectric and magnetic phases in each composite was confirmed using P–E and M–H hysteresis loops, respectively. This study provides an efficient alternative approach for developing multiferroic composites for various technological applications.