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Thermoplastic bonded magnetic composites combine the cost-effectiveness, low mass density, and manufacturing flexibility of conventional thermoplastics with the unique characteristics of magnetic powders/ fillers to form multifunctional magneto polymeric composites that offer superior properties to conventional materials. At elevated temperatures, the magnetic properties change significantly, and the polymer matrix no longer secures the magnetic particles and can rotate freely with respect to an externally applied magnetic field. This often happens at temperatures significantly below the melting point of the polymer. To extend the thermal window of bonded magnets beyond 175 ◦C (the typical temperature of rotors in motors and generators), poly- mers such as polyetheretherketone (PEEK), polyetherimide (PEI), or other high-temperature thermoplastics have been considered suitable binders for magnetic fillers. Another suggested approach is using a surface treatment to increase the adhesion between the polymer matrix and magnetic particles. In this review, the fabrication pro- cesses to make bonded magnets by injection molding and fused filament fabrication were discussed as well as their thermal, mechanical, and magnetic performance obtained via analytical and materials characterization methods. The magnetic properties of bonded permanent magnets manufactured via different techniques were discussed in terms of the most important single magnetic parameter known as “the maximum energy product- (BH)max, which can serve as a performance index for manufacturing bonded magnets. The energy product normalized on cost or mass density are used to provide insight on the performance of bonded magnets for ap- plications driven by cost or inertia. Finally, applications of high-performance thermoplastic-based magnetic composites that can be viable for stringent engineering devices such as sensors, actuators, motors, and generators were highlighted. 

Magnetic Field Assisted Additive Manufacturing (MFAAM) enables 3D printing of magnetic materials of various shapes which exhibit a complex anisotropy energy surface containing contributions generated from different origins such as sample, particle, and agglomerate shape anisotropy, flow and field induced anisotropy, and particle crystal anisotropy. These novel magnet shapes require the need to measure the x, y, and z components of the magnetic dipole moment simultaneously to fully understand the magnetic reversal mechanism and unravel the complex magnetic anisotropy energy surface of 3D printed magnetic composites. This work aims to develop a triaxial vibrating sample magnetometer (VSM) by adding a z-coil set to a pre-existing biaxial VSM employing a modified Mallison coil set. The optimum size and location of the sensing coils were determined by modeling the sensitivity matrix of the z-coil set. The designed coil set was implemented using 3D printed spools, a manual coil winder, and gauge 38 copper wire. A 3D printed strontium ferrite nylon composite sample was used to estimate the sensitivity of the z-coils (50 mV/emu). The results herein are applicable for any VSM using a modified Mallison biaxial coil configuration allowing for a quick implementation on pre-existing systems. 

Magnetic Field Assisted Additive Manufacturing (MFAAM), 3D printing in a magnetic field, has the potential to fabricate high magnetic strength anisotropic bonded magnets. Here, 10, 35, and 54 wt% strontium ferrite bonded magnets using polyamide 12 binder were developed by twin screw compounding process and then printed via MFAAM samples in zero, and in 0.5 Tesla (H parallel to the print direction and print bed). The hysteresis curves were measured using a MicroSense EZ9 Vibrating Sample Magnetometer (VSM) for 3 different mount orientations of the sample on the sample holder to explore the magnetic anisotropy. The samples printed in zero field exhibited a weak anisotropy with an easy axis perpendicular to the print direction. This anisotropy is caused by the effect of shear flow on the orientation of the magnetic platelets in the 3D printer head. For the MFAAM samples, the S values are largest along the print bed normal. This anisotropy is caused by the field. The alignment of the magnetic particles happens when the molten suspension is in the extruder. When the material is printed, it is folded over on the print bed and its easy axis rotates 90° parallel to the print bed normally. Little realignment of the particles happens after it is printed, suggesting a sharp drop in temperature once the composite touches the print bed, indicating that field-induced effects in the nozzle dominate the anisotropy of MFAAM deposited samples. 

The magnetic anisotropy of strontium ferrite (SF)/PA12 filament, a popular hard magnetic ferrimagnetic composites that is used for 3D-printing of permanent magnets, is studied by vibrating sample magnetometry. The studied filaments have a composition of SF/PA-12 thermoplastic composite with a 40% wt.  ratio of SF. SF particles are non-spherical platelets with an average diameter of 1.3 um and a diameter to thickness ratio of 3. Filaments are produced by a twin-screw extruder and have a diameter of 1.5 mm. SEM images show that the SF particles are homogeneously distributed through the filament. VSM measurements on different parts of the filaments show that the outer part of the cylindrical filament has a higher anisotropy, and the core is mostly isotropic. This conclusion is consistent with computational work by others which suggest that particle alignment predominantly takes place near the walls of the extruder die where shear flow is maximum. Additional hysteresis curve measurement of the outer cylindrical part of the filament parallel to the r and ϕ directions indicates that the squareness of the hysteresis curve (S) is larger in the r-direction. This indicates that the outer surface of the filament has a strong easy axis in the r-direction. We conclude that the SF platelets line up parallel to the walls of the extrusion die. 

The primary advantage of the high energy ball milling (HEBM) process is its ability to synthesize a homogeneous mixture with submicron (up to nanoscale) particle size. This approach is a viable process for particle size reduction and grain refinement of magnetic powders, which affects their domain structure and by extension the resulting magnetic properties. In this research, we designed a 9-ball milling experiment by keeping the rotational speed constant at 300rpm and varying the ball-to-powder ratio of 5:1, 8:1, and 10:1 for 6hrs, lOhrs, and 14hrs milling times. The strontium ferrite magnetic powders subjected to HEBM were analyzed for crystallite size and behavior via XRD, particle size reduction via SEM/ImageJ software/originLabPro, and magnetic performance via powder-based VSM measurement. The magnetic performance of the ball-milled strontium ferrite powders shows a good combination of appreciable increment in the S-values (a ratio of the remanence to saturation magnetization) and a considerable decline in coercivity (<10% decrease) at 6hrs of milling duration. The particle size obtained at 6hr-8:1BPR is 0.59 µm with about 44% reduction from the 1.05 µm particle size of the unmilled strontium ferrites, which is within the reported single-domain particle critical size (0.5 µm - 0.65 µm). The particle size reduction of 0.59 µm at 6hr-8: lBPR would be beneficial in enabling strong interfacial bonding when the ball­milled strontium ferrite powders are used in polymer-bonded magnets. 

Bonded magnetic composites combine the cost-effectiveness, low density, and manufacturing flexibility of conventional polymer binders with the unique magnetic characteristics of magnetic powders/fillers to form multifunctional magneto polymeric composites that offer superior properties to conventional sintered magnets. In this study, a co-rotating twin screw extruder was used to fabricate 20 and 40 wt.% strontium ferrite/polyamide 4.6 bonded magnetic composites viable for fused filament fabrication 3D printing. The characterization conducted on the bonded magnetic composites was scanning electron microscopy, simultaneous differential thermogravimetry, and vibrating sample magnetometry. The microstructure of the bonded composite exhibited a uniform platelet morphology of the strontium ferrite magnetic particles. There was no observable depreciation in the melting transitions, which suggests a thermally resistant magnetic composite. An appreciable increment in % crystallinity of 13 and 20% for 20wt. % and 40wt. % strontium ferrites bonded magnets were observed. This is attributable to the heterogeneous nucleation phenomenon, where the metal powders act as nucleation sites for increased crystalline domains. The bonded composite exhibited significant magnetic anisotropy, with the remanence (Mr), which is the most important property for magnetic application significantly increasing to 49.8% along the easy direction in comparison to the hard axis. This suggests the viability of the fabricated bonded composites in viable in producing anisotropic bonded magnetic devices, which are considered to exhibit stronger magnetic properties.