Fused Deposition Modeling of Polymer-Based Magnetic Composites from Recycled Permanent Magnets of Discarded Hard Drives

Polymer-based composites with magnetic properties are promising materials that are able to combine the usual polymer features (low density, high electrical resistance, enhanced flexibility, and processability, etc.) with magnetic properties typically associated with ferro- or ferrimagnetic metals, alloys or metal oxide. The combination of recycled NdFeB powders with additive manufacturing techniques based on material extrusion enables the production of magnetic composites. The novelty of this approach lies in the use of 3D printing supported by an external magnetic field, which is used to align the particles during the printing process and thus improve the final magnetic properties. This approach represents a sustainable strategy for the recovery of electronic waste, converting it into high-value-added magnetic materials intended for additive manufacturing applications. Micrometric particles made of a Neodymium–Iron–Boron (NdFeB) alloy are compounded with a flexible thermoplastic matrix made of polybutylene adipate-co-terephthalate (PBAT). The NdFeB alloy is recovered from permanent magnets of obsolete hard drives and is demagnetized, ground to powder under an inert atmosphere, and finally sieved to a particle size below 50 µm. The obtained powder is mixed with the polymer using a twin-screw extruder. The composite material containing the NdFeB particles is then processed to obtain a calibrated filament, used for the fused deposition modeling (FDM) three-dimensional (3D) printing of magnetic composites. To improve the composite’s ferromagnetic behavior, the particles were aligned along the stacking direction of the layers during the 3D FDM process by printing directly onto a permanent magnet placed on the build plate. Composites containing up to 50% by weight of recycled NdFeB powder were successfully processed using FDM technology, exhibiting increased stiffness, with the storage modulus rising from 123 to 178 MPa at 20 °C, while magnetic field-assisted printing increased the remanence from 11 to 28 emu/g and improved the reduced remanence from 0.21 to 0.49, corresponding to an estimated fourfold improvement in the magnetic energy product.