Effect of the Two-Dimensional Magnetostrictive Fillers of CoFe2O4-Intercalated Graphene Oxide Sheets in 3-2 Type Poly(vinylidene fluoride)-Based Magnetoelectric Films

In the last decade, magnetoelectric (ME) polymer films have been developed by including zero-dimensional or one-dimensional magnetostrictive fillers in a piezoelectric polymer matrix. Existing reports on ME polymer films reveal that the shape of the magnetostrictive fillers is a critical determinant of the polymeric phase conformation, strain transfer between the piezoelectric and magnetostrictive phases, and dipole alignment in the films. In this study, to investigate the effect of two-dimensional (2D) magnetostrictive fillers on piezoelectric, magnetic, and magnetoelectric responses, 3-2 type ME films were prepared using CoFe2O4-intercalated graphene oxide (CFO-i-GO) fillers and poly(vinylidene fluoride) (PVDF) polymers. The 2D fillers of CFO-i-GO were hydrothermally synthesized by CFO intercalation into the interlayers of GO sheets with different lateral sizes, which were controlled by ultrasonication treatment. It was found that the large-lateral-size GO (LGO), medium-lateral-size GO (MGO), and small-lateral-size GO (SGO) fillers in the PVDF-based ME films exhibited a lateral size effect on CFO intercalation, polymeric phase conformation, dipole alignment, and magnetoelectric responses. A maximum ME coefficient (αME) of 3.0 mV/cm∙Oe was achieved with a strong linearity (r2) of 0.9992 at an off-resonance frequency (f) of 1 kHz and applied direct current (dc) magnetic field (Hdc) of ± 1000 Oe. The 3-2 type polymer-based ME films with reliable ME responses have potential for use in high-feasibility ME devices for biomedical sensing applications.