In this paper, we are reporting structural, dielectric, ferroelectric and magnetic properties of polycrystalline composites (ferrite and ferroelectric) of PZT (PbZr0.55Ti0.45O3) + CNFO (Co0.8Ni0.2Fe2O4). The sample with composition x CNFO + (1-x) PZT (x = 0.00, 0.05, 0.10, 0.15 and 1.00) were prepared using the solid state double sintering method. Here the ratio x: (1-x) of two components is by weight. X-ray diffraction (XRD) studies show that lattice constant and tetragonality decreases with increasing ferrite content. Dielectric constant was found to decrease with increase in amount of CNFO. The value of tangent loss (tanδ) was reasonably low (< 0.04) for all the samples. Ferroelectric and ferrimagnetic behavior was confirmed by observing P-E and M-H hysteresis loop, respectively. The room temperature magnetoelectric coupling coefficient (α = dE/dH) was measured as a function of applied DC magnetic field. The value of α was observed to be maximum (855 μV/(cm.Oe)) at DC magnetic field of 1.7 kOe for sample with 5% CNFO. Value of piezoelectric coefficient ‘d33’ decreases from 133 to 60 pC/N.
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