Magnetoelectric coupling in nonsintered bulk BaTiO3 -- xCoFe2O4 multiferroic composites

Bulk BaTiO3-xCoFe2O4, x = 0.1 – 0.6 magnetoelectric composites were prepared using the phosphate bonded ceramics approach. XRD analysis proved the purity of both phases. The dielectric properties are governed by a series of composition-dependent Maxwell-Wagner relaxations and conductivity at lower frequencies and a phase transition-related anomaly at higher frequencies. A dielectric constant as high as 616 – 9387i is observed at 500 K for BaTiO3-0.6CoFe2O4. The magnetic hysteresis demonstrates a high Ms/Mr ratio of 0.46, which is related to the around 30 nm size of the CoFe2O4 particles. The measured direct magnetoelectric coupling coefficient of 1.1 mV Oe−1 cm−1 is higher than that of the conventionally sintered ceramics and compatible with that of core-shell structures. •Non-sintered phosphate bonded BaTiO3-xCoFe2O4 bulk magnetielectric composites were synthesized.•XRD analysis proved the purity of both phases. The homogenity was verified with SEM and PFM.•The dielectric properties undergoes the Maxwell-Wagner relaxations below 1 MHz and phase transition-related anomaly above.•The magnetoelectric coupling coefficient reaches 1.1 mV Oe−1 cm−1 at 0.5 T.