4D printing of the barium ferrite permanent magnets provides new opportunities for intelligent structure and process innovation of permanent magnets. In this paper, the preparation, filament manufacture, and intelligent printing methods with shape memory/recovery effect are studied for the barium ferrite permanent magnet. Firstly, the PLA/TPU/BaFe12O19 composite materials are developed by adding different contents of ferrite permanent magnet BaFe12O19 powders into the PLA/TPU (polylactic acid/thermoplastic polyurethane) matrix. The weight percentage of the BaFe12O19 is 10–40 wt% with an interval of 10 wt%. Secondly, the composites are pelletized and further extruded to manufacture composite filaments with different BaFe12O19 contents. Scanning electron microscope (SEM) is used for the microstructural analysis. The BaFe12O19 particles are uniformly distributed in the PLA/TPU matrix, and the slight particle agglomeration phenomenon occurs in the composite filaments with 30 and 40 wt% BaFe12O19. The thermal properties of PLA/TPU/BaFe12O19 composite filaments are analyzed by thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). After adding the barium ferrite particles, the glass transition temperature of the composite filaments changes within a small range from 53.5 °C to 55 °C. Thirdly, the filaments are successfully manufactured to magnet parts by the fused deposition modeling (FDM) 3D printing for the tests of mechanical, magnetic, and shape recovery properties. With the increase of the barium ferrite content, the magnetic properties show a rising trend, proving the feasibility of using 3D printing technology to make magnets. The shape memory effects of the printed parts are excellent and the shape recovery ratios show a rising trend, from 85.6 % to 88.9 % under heat contact stimulus and from 88.9 % to 97.8 % under electromagnetic induction non-contact stimulus. Relatively, the parts hold fast response speed due to direct contact with the heat source under the heat stimulus, and the parts hold higher shape recovery ratios due to more heats produced under the electromagnetic induction stimulus. The addition of magnetic particles is helpful to improve the heat transfer ability and provide the possibility of non-contact heat transfer. The magnetic parts with complex structure and intelligent shape memory/recovery effect can be achieved for special application requirements. As a result, the research of this paper expands preparation methods of new magnetic composite materials, explores the manufacture process for intelligent magnets and lays a solid foundation for the development of new permanent magnet devices.
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