Scalable, cost-efficient synthesis and properties optimization of magnetoelectric cobalt ferrite/barium titanate composites

Cobalt ferrite (CoFe2O4)/barium titanate (BaTiO3) particulate composites exhibiting high magnetoelectric coefficients were synthesized from low-cost commercial precursors using mechanical ball milling followed by high-temperature annealing. CoFe2O4 (20 nm–50 nm) and either cubic or tetragonal BaTiO3 nanoparticle powders were used for the synthesis. It was found that utilizing a 50 nm cubic BaTiO3 powder as a precursor results in a composite with a magnetoelectric coupling coefficient value as high as 4.3 mV/Oe cm, which is comparable to those of chemically synthesized core–shell CoFe2O4–BaTiO3 nanoparticles. The microstructure of these composites is dramatically different from the composite synthesized using 200 nm tetragonal BaTiO3 powder. CoFe2O4 grains in the composite prepared using cubic BaTiO3 powder are larger (by at least an order of magnitude) and significantly better electrically insulated from each other by the surrounding BaTiO3 matrix, which results in a high electrical resistivity material. It is hypothesized that mechanical coupling between larger CoFe2O4 grains well embedded in a BaTiO3 matrix in combination with high electrical resistivity of the material enhances the observed magnetoelectric effect.