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Ni0.5Zn0.5Fe2O4-BaTiO3 (NZFO-BTO) magnetoelectric composite ceramics with  different molar ratios (mNZFO:mBTO = 1:1.5, 1.5:1 and 2:1, defined as  N1B1.5, N1.5B1 and N2B1, respectively) were prepared successfully by using a  joint hydrothermal method and sol-gel technique and sintering at 1000 °C.  Meanwhile, the dielectric, ferroelectric and magnetic properties of the  composites were investigated. The presence of bi-phase structure in the  composites was verified with X-ray diffraction analyses. The scanning  electron microscopy images and energy dispersion spectrum results confirmed  that the bulk-like grains (2 to 5 μm) and spherelike grains (_0.5 μm) could  be attributed to NZFO and BTO, respectively. The dielectric constant and  loss increased with increasing NZFO/BTO molar ratio because the carrier  concentration of NZFO is higher than that of BTO. Thus, the dielectric  constant of the N2B1 ceramics is more than 7800 at low frequency of 100Hz  and room temperature, while only less than 2000 for the N1B1.5 composite.  Two peaks can be observed in the temperature dependence of the dielectric  constant curves. One is near 120 °C, which corresponds to the Curie  temperature of BTO, while the other peak occurs at about 320 °C,  corresponding to the relaxation polarization. The remanent polarization  increases with increasing the content of ferroelectric BTO. The maximum  value at 1 kHz was observed for the N1B1.5 sample and it is larger than 4.5  μC/cm2, while the minimal value was obtained for the N2B1 composite and is  only 1.2 μC/cm2. Magnetic properties were also measured and it was observed  that magnetization increases with increasing the molar ratio. The largest  saturation magnetization has the N2B1 composite (_51.74 emu/g) due to the  larger concentration of NZFO phase. However, the sample N1B1.5 shows the  largest coercive field due to the highest interface interaction. This study  provides guidelines for the fabrication of NZFO-BTO magnetoelectric  composite ceramics.

Effects of molar ratio on dielectric, ferroelectric and magnetic properties of Ni0.5Zn0.5Fe2O4-BaTiO3 composite ceramics