Magnetoelectric microspheres based on piezoelectric poly(vinylidene fluoride) (PVDF) and magnetostrictive
CoFe2O4 (CFO), a novel morphology for polymer-based ME materials, have been developed by an
electrospray process. The CFO nanoparticle content in the (3–7 mm diameter) microspheres reaches
values up to 27 wt%, despite their concentration in the starting solution reaching values up to 70 wt%.
Additionally, the inclusion of magnetostrictive nanoparticles into the polymer spheres has no relevant
effect on the piezoelectric b-phase content (z60%), crystallinity (40%) and the onset degradation
temperature (460–465 C) of the polymer matrix. The multiferroic microspheres show a maximum
piezoelectric response |d33| z 30 pC N1, leading to a magnetoelectric response of D|d33| z 5 pC N1
obtained when a 220 mT DC magnetic field was applied. It is also shown that the interface between
CFO nanoparticles and PVDF (from 0 to 55%) has a strong influence on the ME response of the
microspheres. The simplicity and the scalability of the processing method suggest a large application
potential of this novel magnetoelectric geometry in areas such as tissue engineering, sensors and actuators.