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Toward Low-Energy Spark-Plasma Sintering of Hot-Deformed Nd-Fe-B Magnets

Received: 24 August 2021    Accepted: 13 September 2021    Published: 29 September 2021
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Abstract

High-coercivity Nd-Fe-B permanent magnets are key materials for producing electrical components on the macro- and nanoscale. We present a newly developed, economically efficient method for processing Nd-Fe-B magnets based on spark-plasma sintering (SPS) that makes it possible to retain the technologically essential properties of the magnet, but by consuming about 30% less energy compared to the conventional SPS process. A magnet with an anisotropic microstructure was fabricated from MQU-F commercial ribbons with a low energy consumption (0.37 MJ) during the deformation process and compared to a conventionally prepared hot-deformed magnet that consumed three-times more energy (1.2 MJ). Both magnets were post-annealed at 650°C for 120 min in a vacuum. After the post-annealing process, the low-energy processing (LEP) hot-deformed magnet exhibited a coercivity of 1327 kAm-1, and a remanent magnetization of 1.27 T. In comparison, the high-energy processing (HEP) hot-deformed magnet had a coercivity of 1337 kAm-1 and a remanent magnetization of 1.31 T. A complete microstructural characterization and detailed statistical analyses revealed a better texture orientation for the HEP hot-deformed magnet processed with the larger energy consumption. This texture is the main reason for the difference in the remanent magnetization between the two hot-deformed magnets. The results show that although the LEP hot-deformed magnet was processed with three-times less energy than in a typical hot-deformation process, the maximum energy product is only 8% lower than that of a HEP hot-deformed magnet.

Published in International Journal of Materials Science and Applications (Volume 10, Issue 5)
DOI 10.11648/j.ijmsa.20211005.12
Page(s) 98-107
Creative Commons

This is an Open Access article, distributed under the terms of the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution and reproduction in any medium or format, provided the original work is properly cited.

Copyright

Copyright © The Author(s), 2024. Published by Science Publishing Group

Keywords

Hot-Deformed Nd-Fe-B Magnets, Low-Energy Processing Hot-Deformation Process, Spark-Plasma Sintering, Statistical Analyses, Electron Microscopy

References
[1] M. Sagawa, K. Hiraga, H. Yamamoto, and Y. Matsuura, “Permanent magnet materials based on the rare earth-iron-boron tetragonal compounds (invited),” IEEE Trans. Magn., vol. 20, no. 5, pp. 1584–1589, 1984, doi: 10.1109/TMAG.1984.1063214.
[2] J. J. Croat, J. F. Herbst, R. W. Lee, and F. E. Pinkerton, “High-energy product Nd-Fe-B permanent magnets,” Appl. Phys. Lett., vol. 44, no. 1, pp. 148–149, 1984, doi: 10.1063/1.94584.
[3] Yanglong Hou and David J. Sellmyer, Magnetic nanomaterials: Fundamentals synthesis and applications. Wiley-VCH Verlag GmbH, 2017.
[4] T. Zhang et al., “Hot-deformed Nd-Fe-B magnets fabricated by dynamic loading with a high maximum energy product,” Intermetallics, vol. 73, pp. 67–71, 2016, doi: 10.1016/j.intermet.2016.04.001.
[5] T. Saito, M. Fujita, T. Kuji, K. Fukuoka, and Y. Syono, “The development of high performance Nd-Fe-Co-Ga-B die upset magnets,” J. Appl. Phys., vol. 83, no. 11, pp. 6390–6392, 1998, doi: 10.1063/1.367522.
[6] K. Hono and H. Sepehri-Amin, “Strategy for high-coercivity Nd-Fe-B magnets,” Scr. Mater., vol. 67, no. 6, pp. 530–535, 2012, doi: 10.1016/j.scriptamat.2012.06.038.
[7] M. Yue, M. Tian, J. X. Zhang, D. T. Zhang, P. L. Niu, and F. Yang, “Microstructure and magnetic properties of anisotropic Nd-Fe-B magnets produced by spark plasma sintering technique,” Mater. Sci. Eng. B Solid-State Mater. Adv. Technol., vol. 131, no. 1–3, pp. 18–21, 2006, doi: 10.1016/j.mseb.2005.11.010.
[8] U. M. R. Seelam et al., “Coercivity of the Nd-Fe-B hot-deformed magnets diffusion-processed with low melting temperature glass forming alloys,” J. Magn. Magn. Mater., vol. 412, pp. 234–242, 2016, doi: 10.1016/j.jmmm.2016.04.005.
[9] M. Soderžnik, M. Korent, K. Žagar Soderžnik, M. Katter, K. Üstüner, and S. Kobe, “High-coercivity Nd-Fe-B magnets obtained with the electrophoretic deposition of submicron TbF3 followed by the grain-boundary diffusion process,” Acta Mater., vol. 115, pp. 278–284, 2016, doi: 10.1016/j.actamat.2016.06.003.
[10] D. Givord, H. S. Li, and J. M. Moreau, “Magnetic properties and crystal structure of Nd2Fe14B,” Solid State Commun., vol. 50, no. 6, pp. 497–499, 1984, doi: 10.1016/0038-1098(84)90315-6.
[11] X. Tang, H. Sepehri-Amin, T. Ohkubo, and K. Hono, “Suppression of non-oriented grains in Nd-Fe-B hot-deformed magnets by Nb doping,” Scr. Mater., vol. 147, pp. 108–113, 2018, doi: 10.1016/j.scriptamat.2017.12.032.
[12] Y. H. Hou, Y. L. Huang, Z. W. Liu, D. C. Zeng, S. C. Ma, and Z. C. Zhong, “Hot deformed anisotropic nanocrystalline NdFeB based magnets prepared from spark plasma sintered melt spun powders,” Mater. Sci. Eng. B Solid-State Mater. Adv. Technol., vol. 178, no. 15, pp. 990–997, 2013, doi: 10.1016/j.mseb.2013.06.009.
[13] O. Gutfleisch, “Controlling the properties of high energy density permanent magnetic materials by different processing routes,” J. Phys. D. Appl. Phys., vol. 33, no. 17, 2000, doi: 10.1088/0022-3727/33/17/201.
[14] R. K. Mishra, E. G. Brewer, and R. W. Lee, “Grain growth and alignment in hot deformed Nd-Fe-B magnets,” J. Appl. Phys., vol. 63, no. 8, pp. 3528–3530, 1988, doi: 10.1063/1.340731.
[15] R. W. Lee, “Hot-pressed neodymium-iron-boron magnets,” Appl. Phys. Lett., vol. 46, no. 8, pp. 790–791, 1985, doi: 10.1063/1.95884.
[16] R. W. Lee, E. G. Brewer, and N. A. Schaffel, “MAGNETS,” IEEE Trans. Magn., vol. M, no. 5, pp. 1958–1963, 1985.
[17] X. Tang et al., “Relationship between the thermal stability of coercivity and the aspect ratio of grains in Nd-Fe-B magnets: experimental and numerical approaches,” Acta Mater., 2019, doi: 10.1016/J.ACTAMAT.2019.11.038.
[18] J. Liu et al., “Grain size dependence of coercivity of hot-deformed Nd-Fe-B anisotropic magnets,” Acta Mater., vol. 82, pp. 336–343, 2015, doi: 10.1016/j.actamat.2014.09.021.
[19] X. D. Xu et al., “Comparison of coercivity and squareness in hot-deformed and sintered magnets produced from a Nd-Fe-B-Cu-Ga alloy,” Scr. Mater., vol. 160, pp. 9–14, 2019, doi: 10.1016/j.scriptamat.2018.09.028.
[20] H. Sepehri-Amin, Y. Une, T. Ohkubo, K. Hono, and M. Sagawa, “Microstructure of fine-grained Nd-Fe-B sintered magnets with high coercivity,” Scr. Mater., vol. 65, no. 5, pp. 396–399, 2011, doi: 10.1016/j.scriptamat.2011.05.006.
[21] J. Liu et al., “Effect of Nd content on the microstructure and coercivity of hot-deformed Nd-Fe-B permanent magnets,” Acta Mater., vol. 61, no. 14, pp. 5387–5399, 2013, doi: 10.1016/j.actamat.2013.05.027.
[22] M. Soderžnik, B. Ambrožič, K. Žagar Soderžnik, and M. Korent, “Limits of grain boundary engineering in nanocrystalline Nd-Fe-B melt-spun ribbons,” Mater. Lett., vol. 264, pp. 20–22, 2020, doi: 10.1016/j.matlet.2020.127338.
[23] J. Liu, H. Sepehri-Amin, T. Ohkubo, K. Hioki, A. Hattori, and K. Hono, “Microstructure evolution of hot-deformed Nd-Fe-B anisotropic magnets,” J. Appl. Phys., vol. 115, no. 17, pp. 15–18, 2014, doi: 10.1063/1.4867960.
[24] M. Soderžnik et al., “Magnetization reversal process of anisotropic hot-deformed magnets observed by magneto-optical Kerr effect microscopy,” J. Alloys Compd., vol. 771, pp. 51–59, 2019, doi: 10.1016/j.jallcom.2018.08.231.
[25] L. H. Lewis, Y. Zhu, D. O. Welch, and L. Henderson, “Evidence for reversal by nucleation in REFeB dieupset magnets Evidence for reversal by nucleation in RE-Fe-B die-upset,” vol. 6235, no. 1994, pp. 9–12, 2012, doi: 10.1063/1.358291.
[26] H. Sepehri-Amin et al., “Microstructure and temperature dependent of coercivity of hot-deformed Nd-Fe-B magnets diffusion processed with Pr-Cu alloy,” Acta Mater., vol. 99, pp. 297–306, 2015, doi: 10.1016/j.actamat.2015.08.013.
[27] K. Hioki, T. Takano, and T. Yamamoto, “Influence of Process Conditions on the Magnetic Properties for Hot Deformed Magnets,” Denki-Seiko [Electric Furn. Steel], vol. 79, no. 2, pp. 119–125, 2008, doi: 10.4262/denkiseiko.79.119.
[28] M. Korent et al., “Magnetic properties and microstructure evolution of hot-deformed Nd-Fe-B magnets produced by low-pressure spark-plasma sintering,” J. Magn. Magn. Mater., vol. 515, no. July, pp. 2–7, 2020, doi: 10.1016/j.jmmm.2020.167279.
[29] J. Trapp and B. Kieback, “Fundamental principles of spark plasma sintering of metals: part I–Joule heating controlled by the evolution of powder resistivity and local current densities,” Powder Metall., vol. 62, no. 5, pp. 297–306, 2019, doi: 10.1080/00325899.2019.1653532.
[30] J. W. Carson and B. H. Pittenger, “Advanced Aluminum Powder Metallurgy Alloys and Composites,” ASM Handb. Vol. 7 Powder Met. Technol. Appl., vol. 7, pp. 287–301, 1998, doi: 10.1361/asmhba00015.
[31] Z. H. Zhang, Z. F. Liu, J. F. Lu, X. B. Shen, F. C. Wang, and Y. D. Wang, “The sintering mechanism in spark plasma sintering - Proof of the occurrence of spark discharge,” Scr. Mater., vol. 81, pp. 56–59, 2014, doi: 10.1016/j.scriptamat.2014.03.011.
[32] N. Chawake, L. D. Pinto, A. K. Srivastav, K. Akkiraju, and B. S. Murty, “On Joule heating during spark plasma sintering of metal powders,” Scr. Mater., vol. 93, pp. 52–55, 2014, doi: 10.1016/j.scriptamat.2014.09.003.
[33] X. Q. Li, L. Li, K. Hu, Z. C. Chen, S. G. Qu, and C. Yang, “Microstructure and magnetic properties of anisotropic Nd-Fe-B magnets prepared by spark plasma sintering and hot deformation,” Trans. Nonferrous Met. Soc. China (English Ed., vol. 24, no. 10, pp. 3142–3151, 2014, doi: 10.1016/S1003-6326(14)63453-1.
[34] T. Tomše et al., “A spark-plasma-sintering approach to the manufacture of anisotropic Nd-Fe-B permanent magnets,” J. Magn. Magn. Mater., vol. 502, no. October 2019, 2020, doi: 10.1016/j.jmmm.2020.166504.
[35] Y. Zhang et al., “Squareness factors of demagnetization curves for multi-main-phase Nd-Ce-Fe-B magnets with different Ce contents,” J. Magn. Magn. Mater., vol. 487, no. May, 2019, doi: 10.1016/j.jmmm.2019.165355.
[36] S. Liu, N. H. Kang, L. Feng, S. H. Lee, J. H. Yu, and J. G. Lee, “Anisotropic Nanocrystalline Nd-Fe-B-Based Magnets Produced by Spark Plasma Sintering Technique,” IEEE Trans. Magn., vol. 51, no. 11, pp. 18–21, 2015, doi: 10.1109/TMAG.2015.2439672.
[37] Z. H. Hu, J. Li, L. H. Chu, and Y. Liu, “Effect of hot deformation temperature on the magnetic and mechanical properties of NdFeB magnets prepared by spark plasma sintering,” J. Magn. Magn. Mater., vol. 323, no. 1, pp. 104–107, 2011, doi: 10.1016/j.jmmm.2010.08.040.
[38] X. Tang, H. Sepehri-Amin, T. Ohkubo, K. Hioki, A. Hattori, and K. Hono, “Coercivities of hot-deformed magnets processed from amorphous and nanocrystalline precursors,” Acta Mater., vol. 123, pp. 1–10, 2017, doi: 10.1016/j.actamat.2016.10.026.
[39] F. Wang, W. Shen, J. Fan, J. Du, K. Chen, and J. P. Liu, “Strong texture in nanograin bulk Nd-Fe-B magnets via slow plastic deformation at low temperatures,” Nanoscale, vol. 11, no. 13, pp. 6062–6071, 2019, doi: 10.1039/C9NR00107G.
[40] M. Zhu and W. Li, “Texture formation mechanism and constitutive equation for anisotropic thermorheological rare-earth permanent magnets,” AIP Adv., vol. 7, no. 5, 2017, doi: 10.1063/1.4978700.
[41] L. Li and C. D. Graham, “The Origin of Crystallographic Texture Produced During Hot Deformation in Rapidly-Quenched NdFeB Permanent Magnets,” IEEE Trans. Magn., vol. 28, no. 5, pp. 2130–2132, 1992, doi: 10.1109/20.179419.
[42] M. Leonowicz and H. A. Davies, “Effect of Nd content on induced anisotropy in hot deformed FeNdB magnets,” Mater. Lett., vol. 19, no. 5–6, pp. 275–279, 1994, doi: 10.1016/0167-577X(94)90170-8.
[43] E. Castle, R. Sheridan, W. Zhou, S. Grasso, A. Walton, and M. J. Reece, “High coercivity, anisotropic, heavy rare earth-free Nd-Fe-B by Flash Spark Plasma Sintering,” Sci. Rep., vol. 7, no. 1, pp. 1–12, 2017, doi: 10.1038/s41598-017-11660-9.
[44] H. R. Cha, K. W. Jeon, J. H. Yu, H. W. Kwon, Y. Do Kim, and J. G. Lee, “Coercivity enhancement of hot-deformed Nd-Fe-B magnet by grain boundary diffusion process using the reaction of NdHxand Cu nanopowders,” J. Alloys Compd., vol. 693, pp. 744–748, 2017, doi: 10.1016/j.jallcom.2016.09.167.
[45] W. Yin, R. Chen, X. Tang, J. Ju, and A. Yan, “Effect of pressless heat treatment on the magnetic performance and microstructure of hot-deformed Nd-Fe-B magnet,” J. Magn. Magn. Mater., vol. 482, no. September 2018, pp. 9–13, 2019, doi: 10.1016/j.jmmm.2019.03.045.
[46] E. A. Périgo, H. Takiishi, C. C. Motta, and R. N. Faria, “Microstructure and squareness factor: A quantitative correlation in (Nd, Pr)FeB sintered magnets,” J. Appl. Phys., vol. 102, no. 11, 2007, doi: 10.1063/1.2821756.
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    Matic Korent, Marko Soderznik, Urska Rocnik, Sandra Drev, Kristina Zuzek Rozman, et al. (2021). Toward Low-Energy Spark-Plasma Sintering of Hot-Deformed Nd-Fe-B Magnets. International Journal of Materials Science and Applications, 10(5), 98-107. https://doi.org/10.11648/j.ijmsa.20211005.12

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    ACS Style

    Matic Korent; Marko Soderznik; Urska Rocnik; Sandra Drev; Kristina Zuzek Rozman, et al. Toward Low-Energy Spark-Plasma Sintering of Hot-Deformed Nd-Fe-B Magnets. Int. J. Mater. Sci. Appl. 2021, 10(5), 98-107. doi: 10.11648/j.ijmsa.20211005.12

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    AMA Style

    Matic Korent, Marko Soderznik, Urska Rocnik, Sandra Drev, Kristina Zuzek Rozman, et al. Toward Low-Energy Spark-Plasma Sintering of Hot-Deformed Nd-Fe-B Magnets. Int J Mater Sci Appl. 2021;10(5):98-107. doi: 10.11648/j.ijmsa.20211005.12

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  • @article{10.11648/j.ijmsa.20211005.12,
      author = {Matic Korent and Marko Soderznik and Urska Rocnik and Sandra Drev and Kristina Zuzek Rozman and Saso Sturm and Spomenka Kobe and Kristina Zagar Soderznik},
      title = {Toward Low-Energy Spark-Plasma Sintering of Hot-Deformed Nd-Fe-B Magnets},
      journal = {International Journal of Materials Science and Applications},
      volume = {10},
      number = {5},
      pages = {98-107},
      doi = {10.11648/j.ijmsa.20211005.12},
      url = {https://doi.org/10.11648/j.ijmsa.20211005.12},
      eprint = {https://article.sciencepublishinggroup.com/pdf/10.11648.j.ijmsa.20211005.12},
      abstract = {High-coercivity Nd-Fe-B permanent magnets are key materials for producing electrical components on the macro- and nanoscale. We present a newly developed, economically efficient method for processing Nd-Fe-B magnets based on spark-plasma sintering (SPS) that makes it possible to retain the technologically essential properties of the magnet, but by consuming about 30% less energy compared to the conventional SPS process. A magnet with an anisotropic microstructure was fabricated from MQU-F commercial ribbons with a low energy consumption (0.37 MJ) during the deformation process and compared to a conventionally prepared hot-deformed magnet that consumed three-times more energy (1.2 MJ). Both magnets were post-annealed at 650°C for 120 min in a vacuum. After the post-annealing process, the low-energy processing (LEP) hot-deformed magnet exhibited a coercivity of 1327 kAm-1, and a remanent magnetization of 1.27 T. In comparison, the high-energy processing (HEP) hot-deformed magnet had a coercivity of 1337 kAm-1 and a remanent magnetization of 1.31 T. A complete microstructural characterization and detailed statistical analyses revealed a better texture orientation for the HEP hot-deformed magnet processed with the larger energy consumption. This texture is the main reason for the difference in the remanent magnetization between the two hot-deformed magnets. The results show that although the LEP hot-deformed magnet was processed with three-times less energy than in a typical hot-deformation process, the maximum energy product is only 8% lower than that of a HEP hot-deformed magnet.},
     year = {2021}
    }
    

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  • TY  - JOUR
    T1  - Toward Low-Energy Spark-Plasma Sintering of Hot-Deformed Nd-Fe-B Magnets
    AU  - Matic Korent
    AU  - Marko Soderznik
    AU  - Urska Rocnik
    AU  - Sandra Drev
    AU  - Kristina Zuzek Rozman
    AU  - Saso Sturm
    AU  - Spomenka Kobe
    AU  - Kristina Zagar Soderznik
    Y1  - 2021/09/29
    PY  - 2021
    N1  - https://doi.org/10.11648/j.ijmsa.20211005.12
    DO  - 10.11648/j.ijmsa.20211005.12
    T2  - International Journal of Materials Science and Applications
    JF  - International Journal of Materials Science and Applications
    JO  - International Journal of Materials Science and Applications
    SP  - 98
    EP  - 107
    PB  - Science Publishing Group
    SN  - 2327-2643
    UR  - https://doi.org/10.11648/j.ijmsa.20211005.12
    AB  - High-coercivity Nd-Fe-B permanent magnets are key materials for producing electrical components on the macro- and nanoscale. We present a newly developed, economically efficient method for processing Nd-Fe-B magnets based on spark-plasma sintering (SPS) that makes it possible to retain the technologically essential properties of the magnet, but by consuming about 30% less energy compared to the conventional SPS process. A magnet with an anisotropic microstructure was fabricated from MQU-F commercial ribbons with a low energy consumption (0.37 MJ) during the deformation process and compared to a conventionally prepared hot-deformed magnet that consumed three-times more energy (1.2 MJ). Both magnets were post-annealed at 650°C for 120 min in a vacuum. After the post-annealing process, the low-energy processing (LEP) hot-deformed magnet exhibited a coercivity of 1327 kAm-1, and a remanent magnetization of 1.27 T. In comparison, the high-energy processing (HEP) hot-deformed magnet had a coercivity of 1337 kAm-1 and a remanent magnetization of 1.31 T. A complete microstructural characterization and detailed statistical analyses revealed a better texture orientation for the HEP hot-deformed magnet processed with the larger energy consumption. This texture is the main reason for the difference in the remanent magnetization between the two hot-deformed magnets. The results show that although the LEP hot-deformed magnet was processed with three-times less energy than in a typical hot-deformation process, the maximum energy product is only 8% lower than that of a HEP hot-deformed magnet.
    VL  - 10
    IS  - 5
    ER  - 

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Author Information
  • Department for Nanostructured Materials, Jozef Stefan Institute, Ljubljana, Slovenia

  • Department for Nanostructured Materials, Jozef Stefan Institute, Ljubljana, Slovenia

  • Department for Nanostructured Materials, Jozef Stefan Institute, Ljubljana, Slovenia

  • Center for Electron Microscopy and Microanalysis, Jozef Stefan Institute, Ljubljana, Slovenia

  • Department for Nanostructured Materials, Jozef Stefan Institute, Ljubljana, Slovenia

  • Department for Nanostructured Materials, Jozef Stefan Institute, Ljubljana, Slovenia

  • Department for Nanostructured Materials, Jozef Stefan Institute, Ljubljana, Slovenia

  • Department for Nanostructured Materials, Jozef Stefan Institute, Ljubljana, Slovenia

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