This research is driven by a desire to create composite films that combine the ferrimagnetic capabilities of pure and La/Nd substituted Sr3Co2Fe24O41 Z-hexaferrites with the multifunctional features of ferroelectric polymers. A flexible magnetoelectric (ME) polymer composite films, with Sr3Co2Fe24O41 (SF), Sr2.85La0.15Co2Fe24O41(SF–La) and Sr2.85Nd0.15Co2Fe24O41 (SF-Nd) as the ferrimagnetic material and poly vinylidene fluoride-hexafluoropropylene (PH) as a ferroelectric component, were synthesized using solution casting method. In the current case, two steps have been used to synthesize ferroelectric and ferrimagnetic composites films: first, SF, SF-La and SF-Nd hexaferrite samples were synthesized using solid state reaction method and then 20% weight percentage of these hexaferrites were incorporated into the PH matrix using solution casting method to form composite film. In order to find the traces of collaborative interactions between the two phases, the structural, magnetic, and ferroelectric properties of these composite samples have been studied. The XRD data confirm the formation of SF, SF-La and SF-Nd hexaferrite dispersed in a piezoelectric copolymer PH matrix. The changes in the ferroelectric properties in different magnetic fields demonstrated the existence of ME coupling in the composite films. The inclusion of PH enhanced the magnetoelectric coupling of composite films. The maximal value of magnetoelectric coupling coefficient (αME) observed is 0.213, 1.227, 3.403 and 9.797 mV cm−1 Oe−1 for SF, PHSF, PHSF-La and PHSF-Nd, respectively. There is approximately 46-time increase in the maximum value of magnetoelectric coupling coefficient (αME) in PHSF-Nd (9.797 mV/cm.Oe) composites as compare to pure SF (0.213 mV/cm.Oe).
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