journal article·2026-04Open access

Processing-induced magnetic softening in high-loading printable composites for additive manufacturing

Gloria Guerrero-Muñoz, Jorge Revuelta-Losada, Jia Yan Law, Elisa Guisado-Arenas, Luis M. Moreno-Ramírez, Manuel Sanchez-Poncela, Victorino Franco

Abstract

Abstract Additive manufacturing (AM) of magnetic composites has traditionally been limited by trade-offs between filler loading, filament quality, processability, and functional performance. Yet, processing-driven advances in AM can redefine this design space, enabling unprecedented filler loadings, broader material compatibility, and scalable fabrication beyond conventional flexible metastructures. Here, we introduce a versatile feedstock-engineering strategy that fabricates magnetic composite filaments with high filler contents while maintaining homogeneity, printability, and performance. By systematically comparing three polymer matrices with two classes of soft magnetic powders, we report the critical interplay among matrix chemistry, filler morphology, and processing conditions, achieving magnetic filaments at high loadings (up to 61 wt% in rigid and 52 wt% in flexible systems), well above commercial standards (~ 40 wt%). Polyethylene terephthalate yields rigid, defect-free filaments at high loadings, whereas thermoplastic polyurethane uniquely enables mechanically flexible, magnetically functional filaments. Structural analyses confirm uniform filler dispersion and preservation of the amorphous or crystalline characters of the powders, while magnetic characterization uncovers an unexpected processing-induced magnetic softening: extrusion reduces coercivity relative to raw powders. This counterintuitive softening transforms extrusion from a passive fabrication step into a functional design tool. Proof-of-concept flexible demonstrations, including flexible actuators and magnetic grippers, exhibit magnetic field-responsive deformation and flux-guided manipulation, validating multifunctionality. The results establish a new design principle, processing-induced property enhancement, which enables AM of magnetically active yet mechanically compliant and reconfigurable systems for soft robotics and electromagnetic control. This scalable, polymer-independent method expands material and functional options for engineering multifunctional composites with structural integrity, mechanical flexibility, and enhanced functionality.
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Research context

OpenAlex topics: Advanced Sensor and Energy Harvesting Materials · Additive Manufacturing and 3D Printing Technologies · Micro and Nano Robotics

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References (45)

Show source-provided references
1. Lazarus N, Bedair SS (2016) Improved power transfer to wearable systems through stretchable magnetic composites. Appl Phys A-Mater Sci Process 122:543. https://doi.org/10.1007/s00339-016-0067-y10.1007/s00339-016-0067-y ↗
2. Wu S, Hu W, Ze Q, Sitti M, Zhao R (2020) Multifunctional magnetic soft composites: a review. Multifunctional Mater 3:042003. https://doi.org/10.1088/2399-7532/abcb0c10.1088/2399-7532/abcb0c ↗
3. Díaz-García Á, Law JY, Cota A, Bellido-Correa A, Ramírez-Rico J, Schäfer R, Franco V (2020) Novel procedure for laboratory scale production of composite functional filaments for additive manufacturing. Mater Today Commun 24:101049. https://doi.org/10.1016/j.mtcomm.2020.10104910.1016/j.mtcomm.2020.101049 ↗
4. Díaz-García Á, Law JY, Felix M, Guerrero A, Franco V (2022) Functional, thermal and rheological properties of polymer-based magnetic composite filaments for additive manufacturing. Mater Design 219:110806. https://doi.org/10.1016/j.matdes.2022.11080610.1016/j.matdes.2022.110806 ↗
5. Díaz-García Á, Revuelta J, Moreno-Ramírez LM, Law JY, Mayer C, Franco V (2022) Additive manufacturing of magnetocaloric (La,Ce)(Fe,Mn,Si)13–H particles via polymer-based composite filaments. Compos Commun 35:101352. https://doi.org/10.1016/j.coco.2022.10135210.1016/j.coco.2022.101352 ↗
6. Díaz-García Á, Law JY, Żrodowski Ł, Morończyk B, Wróblewski R, Franco V (2024) Polymer‐based filaments with embedded magnetocaloric Ni‐Mn‐Ga Heusler alloy particles for additive manufacturing. Polym Compos 45:5333. https://doi.org/10.1002/pc.2813010.1002/pc.28130 ↗
7. Zhang Z, Heron JT, Pena-Francesch A (2023) Adaptive Magnetoactive Soft Composites for Modular and Reconfigurable Actuators. Adv Funct Mater 33:2215248. https://doi.org/10.1002/adfm.20221524810.1002/adfm.202215248 ↗
8. Bhatta A, McKenzie TF, DeFeo JR, Casey J, Yenugonda V, Mukaddaskhonov S, Toromani G, Pathak AK, Khan M (2025) Exploring the magnetic and magnetocaloric properties of PLA composite filaments of Mn0.5Fe0.5Ni0.95Cr0.05Si0.95Al0.05 for additive manufacturing. AIP Adv 15. https://doi.org/10.1063/9.000094210.1063/9.0000942 ↗
9. Abbasi M, Váz P, Silva J, Martins P (2025) Head-to-Head Evaluation of FDM and SLA in Additive Manufacturing: Performance, Cost, and Environmental Perspectives. Appl Sci 15:2245. https://doi.org/10.3390/app1504224510.3390/app15042245 ↗
10. Kafle A, Luis E, Silwal R, Pan HM, Shrestha PL, Bastola AK (2021) 3D/4D Printing of Polymers: Fused Deposition Modelling (FDM), Selective Laser Sintering (SLS), and Stereolithography (SLA). Polymers 13:3101. https://doi.org/10.3390/polym1318310110.3390/polym13183101 ↗
11. Monfared V, Bakhsheshi-Rad HR, Ramakrishna S, Razzaghi M, Berto F (2021) A Brief Review on Additive Manufacturing of Polymeric Composites and Nanocomposites. Micromachines 12:704. https://doi.org/10.3390/mi1206070410.3390/mi12060704 ↗
12. Giannotta N, Sala G, Bianchini C, Torreggiani A (2023) A Review of Additive Manufacturing of Soft Magnetic Materials in Electrical Machines. Machines 11:702. https://doi.org/10.3390/machines1107070210.3390/machines11070702 ↗
13. Zhou L, Miller J, Vezza J, Mayster M, Raffay M, Justice Q, Al Tamimi Z, Hansotte G, Sunkara LD, Bernat J (2024) Additive Manufacturing: A Comprehensive Review. Sensors-Basel 24:2668. https://doi.org/10.3390/s2409266810.3390/s24092668 ↗
14. Huber C, Mitteramskogler G, Goertler M, Teliban I, Groenefeld M, Suess D (2020) Additive Manufactured Polymer-Bonded Isotropic NdFeB Magnets by Stereolithography and Their Comparison to Fused Filament Fabricated and Selective Laser Sintered Magnets. Materials 13:1916. https://doi.org/10.3390/ma1308191610.3390/ma13081916 ↗
15. Strong D, Kay M, Conner B, Wakefield T, Manogharan G (2018) Hybrid manufacturing – integrating traditional manufacturers with additive manufacturing (AM) supply chain. Additive Manuf 21:159. https://doi.org/10.1016/j.addma.2018.03.01010.1016/j.addma.2018.03.010 ↗
16. Jacob J, Pejak Simunec D, Kandjani AEZ, Trinchi A, Sola A (2024) A Review of Fused Filament Fabrication of Metal Parts (Metal FFF): Current Developments and Future Challenges. Technologies 12:267. https://doi.org/10.3390/technologies1212026710.3390/technologies12120267 ↗
17. Bollig LM, Patton MV, Mowry GS, Nelson-Cheeseman BB (2017) Effects of 3-D Printed Structural Characteristics on Magnetic Properties. Ieee T Magn 53:1. https://doi.org/10.1109/TMAG.2017.269803410.1109/TMAG.2017.2698034 ↗
18. Bollig LM, Hilpisch PJ, Mowry GS, Nelson-Cheeseman BB (2017) 3D printed magnetic polymer composite transformers. J Magn Magn Mater 442:97. https://doi.org/10.1016/j.jmmm.2017.06.07010.1016/j.jmmm.2017.06.070 ↗
19. Liu H, Wang F, Wu W, Dong X, Sang L (2023) 4D printing of mechanically robust PLA/TPU/Fe3O4 magneto-responsive shape memory polymers for smart structures. Compos Part B: Eng 248:110382. https://doi.org/10.1016/j.compositesb.2022.11038210.1016/j.compositesb.2022.110382 ↗
20. Thomas JL, Andrew HM, Thomas AH, Brittany BN-C (2019) Dispersion of particulate in solvent cast magnetic thermoplastic polyurethane elastomer composites. AIMS Mater Sci 6:354. https://doi.org/10.3934/matersci.2019.3.35410.3934/matersci.2019.3.354 ↗
21. Andrew HM, Thomas MC, Nathan AF, Thomas JL, John EW, Brittany BN-C (2019) Thermoplastic magnetic elastomer for fused filament fabrication. AIMS Mater Sci 6:363. https://doi.org/10.3934/matersci.2019.3.36310.3934/matersci.2019.3.363 ↗
22. Rochman A, Delia S (2024) Additive Manufacturing of Thermoplastic Polyurethane Elastomers: A Review. Reference Module in Materials Science and Materials Engineering: Elsevier; 2024. https://doi.org/10.1016/B978-0-323-95486-0.00100-910.1016/B978-0-323-95486-0.00100-9 ↗
23. Su K-H, Su C-Y, Shih W-L, Lee F-T (2023) Improvement of the Thermal Conductivity and Mechanical Properties of 3D-Printed Polyurethane Composites by Incorporating Hydroxylated Boron Nitride Functional Fillers. Materials 16:356. https://doi.org/10.3390/ma1601035610.3390/ma16010356 ↗
24. Huber C, Cano S, Teliban I, Schuschnigg S, Groenefeld M, Suess D (2020) Polymer-bonded anisotropic SrFe12O19 filaments for fused filament fabrication. J Appl Phys 127. https://doi.org/10.1063/1.513949310.1063/1.5139493 ↗
25. Slapnik J, Pulko I, Rudolf R, Anžel I, Brunčko M (2021) Fused filament fabrication of Nd-Fe-B bonded magnets: Comparison of PA12 and TPU matrices. Additive Manuf 38:101745. https://doi.org/10.1016/j.addma.2020.10174510.1016/j.addma.2020.101745 ↗
26. Gonzalez-Gutierrez J, Cano S, Schuschnigg S, Kukla C, Sapkota J, Holzer C (2018) Additive Manufacturing of Metallic and Ceramic Components by the Material Extrusion of Highly-Filled Polymers: A Review and Future Perspectives. Materials 11:840. https://doi.org/10.3390/ma1105084010.3390/ma11050840 ↗
27. Waheed S, Cabot JM, Smejkal P, Farajikhah S, Sayyar S, Innis PC, Beirne S, Barnsley G, Lewis TW, Breadmore MC, Paull B (2019) Three-Dimensional Printing of Abrasive, Hard, and Thermally Conductive Synthetic Microdiamond–Polymer Composite Using Low-Cost Fused Deposition Modeling Printer. Acs Appl Mater Inter 11:4353. https://doi.org/10.1021/acsami.8b1823210.1021/acsami.8b18232 ↗
28. Wang F-H, You C-Y, Tian N, Liu H-G, Zhang J, Zhu X-P (2024) 3D printing of soft magnetic materials: From printing to applications. J Alloy Compd 990:174486. https://doi.org/10.1016/j.jallcom.2024.17448610.1016/j.jallcom.2024.174486 ↗
29. Khatri B, Lappe K, Noetzel D, Pursche K, Hanemann T (2018) A 3D-Printable Polymer-Metal Soft-Magnetic Functional Composite—Development and Characterization. Materials 11:189. https://doi.org/10.3390/ma1102018910.3390/ma11020189 ↗
30. Mazeeva A, Masaylo D, Razumov N, Konov G, Popovich A (2023) 3D Printing Technologies for Fabrication of Magnetic Materials Based on Metal–Polymer Composites: A Review. Materials 16:6928. https://doi.org/10.3390/ma1621692810.3390/ma16216928 ↗
31. ArcelorMittalPowders AdamIQ M300 - AISI 18Ni 300 | W. Nr 1.2709 | DIN X3NiCoMoTi 18-9-5 | UNS K93120 [cited 2025]. Available from: https://powders.arcelormittal.com/adamiq-m300-steel-powder
32. Sánchez-Poncela M, Van-Steenberge N, Gatti F, Rodríguez S (2021) inventorsMetal powder for Additive Manufacturing
33. ASTM_International., ASTM D790-17 (2017) Standard Test Methods for Flexural Properties of Unreinforced and Reinforced Plastics and Electrical Insulating Materials. ASTM International, West Conshohocken, PA
34. ASTM_International., ASTM D695-15 (2015) Standard Test Method for Compressive Properties of Rigid Plastics. ASTM International, West Conshohocken, PA
35. Omeire GC, Iwe MO, Nwosu JN (2013) Influence of Extrusion Variables on the Residence Time and Throughput of a Single Screw Extruder. Curr J Appl Sci Technol 3:277. https://doi.org/10.9734/BJAST/2014/225210.9734/BJAST/2014/2252 ↗
36. Darnal A, Shahid Z, Deshpande H, Kim J, Muliana A (2023) Tuning mechanical properties of 3D printed composites with PLA:TPU programmable filaments. Compos Struct 318:117075. https://doi.org/10.1016/j.compstruct.2023.11707510.1016/j.compstruct.2023.117075 ↗
37. Krapež D, Jusufagić M, Obućina M, Kitek Kuzman M, Kariž M (2025) Effect of Filament Material and Printing Temperature on 3D Printing Extrusion Force. Appl Sci 15:2046. https://doi.org/10.3390/app1504204610.3390/app15042046 ↗
38. Shanmugam V, Babu K, Kannan G, Mensah RA, Samantaray SK, Das O (2024) The thermal properties of FDM printed polymeric materials: A review. Polym Degrad Stab 228:110902. https://doi.org/10.1016/j.polymdegradstab.2024.11090210.1016/j.polymdegradstab.2024.110902 ↗
39. García Díez A, Pereira N, Tubio CR, Vilas-Vilela JL, Costa CM, Lanceros-Mendez S (2023) Magnetic Polymer Actuators with Self-Sensing Resistive Bending Response Based on Ternary Polymer Composites. ACS Appl Electron Mater 5:3426. https://doi.org/10.1021/acsaelm.3c0043210.1021/acsaelm.3c00432 ↗
40. Pigliaru L, Rinaldi M, Ciccacci L, Norman A, Rohr T, Ghidini T, Nanni F (2020) 3D printing of high performance polymer-bonded PEEK-NdFeB magnetic composite materials. Funct Compos Mater 1:4. https://doi.org/10.1186/s42252-020-00006-w10.1186/s42252-020-00006-w ↗
41. Wu Z, Wang Q, Huang J, Yue Y, Chen D, Shi Y, Su B (2022) The soft NdFeB/Ecoflex composites for soft robot with a considerable magnetostimulated shrinkability. Compos Sci Technol 217:109129. https://doi.org/10.1016/j.compscitech.2021.10912910.1016/j.compscitech.2021.109129 ↗
42. Arora N, Dua S, Singh VK, Singh SK, Senthilkumar T (2024) A comprehensive review on fillers and mechanical properties of 3D printed polymer composites. Mater Today Commun 40:109617. https://doi.org/10.1016/j.mtcomm.2024.10961710.1016/j.mtcomm.2024.109617 ↗
43. Franco V, Conde CF, Conde A (1998) Effect of the Si/B ratio on the magnetic anisotropy distribution of Fe73.5Si22.5-xBxCu1Nb3 (x = 7, 9, 16) alloys along nanocrystallization. J Appl Phys 84:5108. https://doi.org/10.1063/1.36880710.1063/1.368807 ↗
44. Amirov A, Omelyanchik A, Murzin D, Kolesnikova V, Vorontsov S, Musov I, Musov K, Khashirova S, Rodionova V (2022) 3D Printing of PLA/Magnetic Ferrite Composites: Effect of Filler Particles on Magnetic Properties of Filament. Processes 10:2412. https://doi.org/10.3390/pr1011241210.3390/pr10112412 ↗
45. Gloeckle C, Konkol T, Jacobs O, Limberg W, Ebel T, Handge UA (2020) Processing of Highly Filled Polymer–Metal Feedstocks for Fused Filament Fabrication and the Production of Metallic Implants. Materials 13:4413. https://doi.org/10.3390/ma1319441310.3390/ma13194413 ↗