Microfluidic Processing of Piezoelectric and Magnetic Responsive Electroactive Microspheres

[Image: see text] Poly(vinylidene fluoride) (PVDF) combined with cobalt ferrite (CFO) particles is one of the most common and effective polymeric magnetoelectric composites. Processing PVDF into its electroactive phase is a mandatory condition for featuring electroactive behavior and specific (post)processing may be needed to achieve this state, although electroactive phase crystallization is favored at processing temperatures below 60 °C. Different techniques are used to process PVDF–CFO nanocomposite structures into microspheres with high CFO dispersion, with microfluidics adding the advantages of high reproducibility, size tunability, and time and resource efficiency. In this work, magnetoelectric microspheres are produced in a one-step approach. We describe the production of high content electroactive phase PVDF and PVDF–CFO microspheres using microfluidic technology. A flow-focusing polydimethylsiloxane device is fabricated based on a 3D printed polylactic acid master, which enables the production of spherical microspheres with mean diameters ranging from 80 to 330 μm. The microspheres feature internal and external cavernous structures and good CFO distribution with an encapsulation efficacy of 80% and prove to be in the electroactive γ-phase with a mean content of 75%. The microspheres produced using this approach show suitable characteristics as active materials for tissue regeneration strategies and other piezoelectric polymer applications.