EP3462465B1 - Seltenerdmagnet - Google Patents

Seltenerdmagnet Download PDF

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Publication number
EP3462465B1
EP3462465B1 EP18194093.3A EP18194093A EP3462465B1 EP 3462465 B1 EP3462465 B1 EP 3462465B1 EP 18194093 A EP18194093 A EP 18194093A EP 3462465 B1 EP3462465 B1 EP 3462465B1
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EP
European Patent Office
Prior art keywords
phase
rare earth
earth magnet
satisfies
molten metal
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Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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Application number
EP18194093.3A
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English (en)
French (fr)
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EP3462465A1 (de
Inventor
Masaaki Ito
Tetsuya Shoji
Masao Yano
Hisazumi Akai
Munehisa Matsumoto
Martin Hoffmann
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
University of Tokyo NUC
Toyota Motor Corp
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University of Tokyo NUC
Toyota Motor Corp
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Priority claimed from JP2018027405A external-priority patent/JP6927906B2/ja
Application filed by University of Tokyo NUC, Toyota Motor Corp filed Critical University of Tokyo NUC
Publication of EP3462465A1 publication Critical patent/EP3462465A1/de
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/032—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials
    • H01F1/04—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys
    • H01F1/047—Alloys characterised by their composition
    • H01F1/053—Alloys characterised by their composition containing rare earth metals
    • H01F1/055—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5
    • H01F1/0555—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 pressed, sintered or bonded together
    • H01F1/0557—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 pressed, sintered or bonded together sintered
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/032—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials
    • H01F1/04—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys
    • H01F1/047—Alloys characterised by their composition
    • H01F1/053—Alloys characterised by their composition containing rare earth metals
    • H01F1/055—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5
    • H01F1/0551—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 in the form of particles, e.g. rapid quenched powders or ribbon flakes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/032—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials
    • H01F1/04—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys
    • H01F1/047—Alloys characterised by their composition
    • H01F1/053—Alloys characterised by their composition containing rare earth metals
    • H01F1/055—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5
    • H01F1/057—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 and IIIa elements, e.g. Nd2Fe14B
    • H01F1/0571—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 and IIIa elements, e.g. Nd2Fe14B in the form of particles, e.g. rapid quenched powders or ribbon flakes
    • H01F1/0575—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 and IIIa elements, e.g. Nd2Fe14B in the form of particles, e.g. rapid quenched powders or ribbon flakes pressed, sintered or bonded together
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/02—Making non-ferrous alloys by melting
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C19/00—Alloys based on nickel or cobalt
    • C22C19/07—Alloys based on nickel or cobalt based on cobalt
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C33/00—Making ferrous alloys
    • C22C33/04—Making ferrous alloys by melting
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C38/00—Ferrous alloys, e.g. steel alloys
    • C22C38/005—Ferrous alloys, e.g. steel alloys containing rare earths, i.e. Sc, Y, Lanthanides
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C38/00—Ferrous alloys, e.g. steel alloys
    • C22C38/10—Ferrous alloys, e.g. steel alloys containing cobalt
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/032—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials
    • H01F1/04—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys
    • H01F1/047—Alloys characterised by their composition
    • H01F1/053—Alloys characterised by their composition containing rare earth metals
    • H01F1/055—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5
    • H01F1/0555—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 pressed, sintered or bonded together
    • H01F1/0558—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 pressed, sintered or bonded together bonded together
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F41/00—Apparatus or processes specially adapted for manufacturing or assembling magnets, inductances or transformers; Apparatus or processes specially adapted for manufacturing materials characterised by their magnetic properties
    • H01F41/02—Apparatus or processes specially adapted for manufacturing or assembling magnets, inductances or transformers; Apparatus or processes specially adapted for manufacturing materials characterised by their magnetic properties for manufacturing cores, coils, or magnets
    • H01F41/0253—Apparatus or processes specially adapted for manufacturing or assembling magnets, inductances or transformers; Apparatus or processes specially adapted for manufacturing materials characterised by their magnetic properties for manufacturing cores, coils, or magnets for manufacturing permanent magnets
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/032—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials
    • H01F1/04—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of hard-magnetic materials metals or alloys
    • H01F1/047—Alloys characterised by their composition
    • H01F1/053—Alloys characterised by their composition containing rare earth metals
    • H01F1/055—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5
    • H01F1/0555—Alloys characterised by their composition containing rare earth metals and magnetic transition metals, e.g. SmCo5 pressed, sintered or bonded together

Definitions

  • the present disclosure relates to a rare earth magnet and a production method thereof.
  • the present disclosure relates to a rare earth magnet containing a magnetic phase having a composition represented by RT 5 (R is a rare earth element, and T is a transition metal element), and a production method thereof.
  • Patent Literature 1 Japanese Unexamined Patent Publication
  • Sm is high in rarity among rare earth elements, it is attempted to replace part or whole of Sm with a rare earth element lower in rarity than Sm.
  • the gist thereof is as follows.
  • the value of w may be 0.01 or more, 0.02 or more, 0.03 or more, 0.04 or more, or 0.05 or more.
  • the value of w may be low as long as the purity of raw materials of Ce and La is not excessively increased, and the value of w may be 0.09 or less, 0.08 or less, 0.07 or less, or 0.06 or less.
  • ⁇ -Co phase, ⁇ -Fe phase, and ⁇ -(Co, Fe) phase are less likely to be formed as well.
  • ⁇ -(Co, Fe) phase indicates a phase where part of Co of ⁇ -Co phase is replaced with Fe.
  • the value of v is 20.9 at% or less, a magnetic phase larger in the rare earth element content than 1-5 phase, that is, 1-2 phase and 2-7 phase, etc., is less likely to be formed, as a result, 1-5 phase is readily stabilized.
  • the value of v is preferably 20.0 at% or less, more preferably 19.0 at% or less, still more preferably 18.0 at% or less.
  • M represents one or more members selected from the group consisting of a transition metal element other than Co and Fe, Ga, Al, Zn, and In, and an unavoidable impurity element.
  • Cu among the transition metal elements and Ga, Al, Zn, and In can reduce the melting point of a crystal grain boundary of the magnetic phase. Consequently, the crystal grain boundary readily turns into a liquid phase during temperature rise, and therefore the sintering (including liquid-phase sintering) temperature can be lowered.
  • the value of z may be 0 at%, it is difficult not to contain an unavoidable impurity element at all, or a significant rise in the production cost is caused. For this reason, the value of z may be 0.1 at% or more, 0.2 at% or more, or 0.4 at% or more.
  • x may be 0.3 or more, 0.6 or more, or 0.7 or more, and y may be 0.1 or more, 0.2 or more, 0.3 or more.
  • y when y is 0.3 or more, the content of Fe decreases, making production of CeFe 2 phase difficult, and the enhancement of saturation magnetization can be more stabilized.
  • 1-5 phase is likely to be stabilized as the formation energy is smaller, when the formation energy is small to a certain extent, the phase is stabilized to a degree not causing a problem in practice. Accordingly, x may be 0.9 or less, 0.85 or less, or 0.80 or less, and y may be 0.9 or less, 0.8 or less, or 0.7 or less.
  • the molten metal can be cooled at a predetermined rate according a strip casting method by using a quenching apparatus 10 illustrated in Fig. 3 .
  • a quenching apparatus 10 illustrated in Fig. 3 .
  • raw materials are melted in a melting furnace 11 to prepare a molten metal 12 having the composition above.
  • the molten metal 12 is supplied to a tundish 13 at a fixed supply rate.
  • the molten metal 12 supplied to the tundish 13 is supplied to a cooling roll 14 from an end of the tundish 13 due to its own weight.
  • the rare earth magnet of the present disclosure and the production method thereof are described more specifically below by referring to Examples and Comparative Examples. However, the rare earth magnet of the present disclosure and the production method thereof are not limited to the conditions employed in the following Examples.
  • the ribbon was coarsely pulverized to obtain a powder, and the presence or absence of 1-5 phase was confirmed by X-ray diffraction (XRD) analysis of the powder.
  • XRD X-ray diffraction
  • Table 1 The results are shown in Table 1.
  • Reference Example 1 was quoted from J.J. Zhang et al., JMMM, 324(2012), pp. 3272-3275 .
  • Fig. 1 a diagram showing the results of Table 1 together in a formation energy map is illustrated
  • Fig. 2 a diagram showing the results of Table 1 together in a total magnetic moment map is illustrated.
  • the formation energy map and the total magnetic moment map were created by the methods described above.
  • the XRD analysis results for the samples of Examples 1 to 5 and for the samples of Comparative Examples 1 to 4 are shown in Fig. 4 and Fig. 5 , respectively. With respect to the analysis results of each sample of Figs.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Hard Magnetic Materials (AREA)

Claims (16)

  1. Seltenerdmagnet mit einer Zusammensetzung, die durch folgende Formel dargestellt wird: (CexLa(1-x-w)R'w)v(CoyFe(1-y))(100-v-z)Mz, wobei R' ein oder mehrere Seltenerdelemente außer Ce und La ist,
    M ein oder mehrere Mitglieder darstellt, die aus der Gruppe ausgewählt sind, die aus einem Übergangsmetallelement außer Co und Fe, Ga, Al, Zn und In und einem unvermeidlichen Verunreinigungselement besteht,
    0 < x < 1,0,
    0 < y < 1,0,
    0 ≥ w ≥ 0,1,
    7,1 ≥ v ≥ 20,9 und
    0 ≥ z ≥ 8,0,
    und der in der Formel die Beziehung y ≤ -3x + 1,7 erfüllt.
  2. Seltenerdmagnet nach Anspruch 1, der ferner in der Formel die Beziehung y ≥ - 1,25x + 1,25 erfüllt.
  3. Seltenerdmagnet nach Anspruch 1 oder 2, wobei x 0,3 ≥ x ≥ 0,9 erfüllt.
  4. Seltenerdmagnet nach Anspruch 1 oder 2, wobei x 0,6 ≥ x ≥ 0,9 erfüllt.
  5. Seltenerdmagnet nach einem der Ansprüche 1 bis 4, wobei y 0,1 ≥ y ≥ 0,9 erfüllt.
  6. Seltenerdmagnet nach einem der Ansprüche 1 bis 4, wobei y 0,1 ≥ y ≥ 0,7 erfüllt.
  7. Seltenerdmagnet nach einem der Ansprüche 1 bis 4, wobei y 0,3 ≥ y ≥ 0,9 erfüllt.
  8. Seltenerdmagnet nach einem der Ansprüche 1 bis 4, wobei y 0,3 ≥ y ≥ 0,7 erfüllt.
  9. Verfahren zur Herstellung eines Seltenerdmagneten, das Folgendes umfasst:
    Herstellen eines geschmolzenen Metalls mit einer Zusammensetzung, die durch folgende Formel dargestellt wird:
    (CexLa(1-x-w)R'w)v(CoyFe(1-y))(100-v-z)Mz, wobei R' ein oder mehrere Seltenerdelemente außer Ce und La ist,
    M ein oder mehrere Mitglieder darstellt, die aus der Gruppe ausgewählt sind, die aus einem Übergangsmetallelement außer Co und Fe, Ga, Al, Zn und In und einem unvermeidlichen Verunreinigungselement besteht,
    0 < x < 1,0,
    0 < y < 1,0,
    0 ≥ w ≥ 0,1,
    7,1 ≥ v ≥ 20,9 und
    0 ≥ z ≥ 8,0, und der in der Formel die Beziehung y ≤ -3x + 1,7 erfüllt, und
    Abkühlen des geschmolzenen Metalls mit einer Rate von 1 × 102 bis 1 × 107 K/sek, um ein Band zu erhalten.
  10. Verfahren nach Anspruch 9, wobei in der Formel ferner die Beziehung y ≥ -1,25x + 1,25 erfüllt ist.
  11. Verfahren nach Anspruch 9 oder 10, wobei x 0,3 ≥ x ≥ 0,9 erfüllt.
  12. Verfahren nach Anspruch 9 oder 10, wobei x 0,6 ≥ x ≥ 0,9 erfüllt.
  13. Verfahren nach einem der Ansprüche 9 bis 12, wobei y 0,1 ≥ y ≥ 0,9 erfüllt.
  14. Verfahren nach einem der Ansprüche 9 bis 12, wobei y 0,1 ≥ y ≥ 0,7 erfüllt.
  15. Verfahren nach einem der Ansprüche 9 bis 12, wobei y 0,3 ≥ y ≥ 0,9 erfüllt.
  16. Verfahren nach einem der Ansprüche 9 bis 12, wobei y 0,3 ≥ y ≥ 0,7 erfüllt.
EP18194093.3A 2017-09-29 2018-09-12 Seltenerdmagnet Active EP3462465B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2017191466 2017-09-29
JP2018027405A JP6927906B2 (ja) 2017-09-29 2018-02-19 希土類磁石

Publications (2)

Publication Number Publication Date
EP3462465A1 EP3462465A1 (de) 2019-04-03
EP3462465B1 true EP3462465B1 (de) 2022-02-16

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EP18194093.3A Active EP3462465B1 (de) 2017-09-29 2018-09-12 Seltenerdmagnet

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EP (1) EP3462465B1 (de)
KR (1) KR102077147B1 (de)
CN (1) CN109585107B (de)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110148507B (zh) * 2019-05-23 2020-10-16 钢铁研究总院 一种含REFe2相的晶界扩散铈磁体及其制备方法

Family Cites Families (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2258780A1 (de) * 1971-12-14 1973-06-28 Goldschmidt Ag Th Verfahren zum herstellen von permanentmagneten auf der basis von kobalt-seltene erden-legierungen
US4144105A (en) * 1974-08-13 1979-03-13 Bbc Brown, Boveri & Company, Limited Method of making cerium misch-metal/cobalt magnets
JPS5927756A (ja) * 1982-08-03 1984-02-14 Tohoku Metal Ind Ltd 薄板永久磁石材料の製造方法
US4664723A (en) * 1984-11-09 1987-05-12 Sumitomo Metal Mining Company Limited Samarium-cobalt type magnet powder for resin magnet
JPH04371556A (ja) 1991-06-17 1992-12-24 Shin Etsu Chem Co Ltd 希土類磁石合金及び希土類永久磁石
JPH08191006A (ja) * 1994-11-08 1996-07-23 Toshiba Corp 磁性材料
US7713360B2 (en) * 2004-02-26 2010-05-11 Shin-Etsu Chemical Co., Ltd. Rare earth permanent magnet
CN101064206A (zh) * 2007-03-23 2007-10-31 中南大学 颗粒尺寸小于20nm的SmCo7永磁合金的制备方法
JP4764526B2 (ja) * 2008-05-30 2011-09-07 株式会社東芝 永久磁石およびその製造方法、モータ用永久磁石および永久磁石モータ
JP6319808B2 (ja) * 2015-09-17 2018-05-09 トヨタ自動車株式会社 磁性化合物及びその製造方法

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Publication number Publication date
EP3462465A1 (de) 2019-04-03
CN109585107B (zh) 2021-01-26
KR20190038299A (ko) 2019-04-08
CN109585107A (zh) 2019-04-05
KR102077147B1 (ko) 2020-02-13

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