WO2017080935A1 - Procédé de fabrication d'un matériau magnétique et machine électrique - Google Patents

Procédé de fabrication d'un matériau magnétique et machine électrique Download PDF

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Publication number
WO2017080935A1
WO2017080935A1 PCT/EP2016/076770 EP2016076770W WO2017080935A1 WO 2017080935 A1 WO2017080935 A1 WO 2017080935A1 EP 2016076770 W EP2016076770 W EP 2016076770W WO 2017080935 A1 WO2017080935 A1 WO 2017080935A1
Authority
WO
WIPO (PCT)
Prior art keywords
metal
alloy
phase
hard magnetic
magnetic phase
Prior art date
Application number
PCT/EP2016/076770
Other languages
German (de)
English (en)
Inventor
Holger Wuest
Lars BOMMER
Juergen Oberle
Arne Huber
Witold Pieper
Stefan HINDERBERGER
Original Assignee
Robert Bosch Gmbh
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Robert Bosch Gmbh filed Critical Robert Bosch Gmbh
Priority to CN201680065417.3A priority Critical patent/CN108352232A/zh
Publication of WO2017080935A1 publication Critical patent/WO2017080935A1/fr

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Classifications

    • 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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F3/00—Manufacture of workpieces or articles from metallic powder characterised by the manner of compacting or sintering; Apparatus specially adapted therefor ; Presses and furnaces
    • B22F3/12—Both compacting and sintering
    • B22F3/16—Both compacting and sintering in successive or repeated steps
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C28/00—Alloys based on a metal not provided for in groups C22C5/00 - C22C27/00
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C30/00—Alloys containing less than 50% by weight of each constituent
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C33/00—Making ferrous alloys
    • 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
    • C22C38/14—Ferrous alloys, e.g. steel alloys containing titanium or zirconium
    • 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
    • C22C38/16—Ferrous alloys, e.g. steel alloys containing copper
    • 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
    • H01F41/0266—Moulding; Pressing
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F2998/00—Supplementary information concerning processes or compositions relating to powder metallurgy
    • B22F2998/10—Processes characterised by the sequence of their steps
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F2999/00—Aspects linked to processes or compositions used in powder metallurgy

Definitions

  • the present invention relates to an easily implementable and cost-reduced method for producing a magnetic material having excellent magnetic properties. Furthermore, the invention relates to an electrical machine with high power density.
  • High energy product (BH) max magnetic materials often consist of a Nd2Fei4B hard magnetic phase and a neodymium rich one
  • Grain boundary phase and are usually produced by sintering.
  • the grain boundary phase allows liquid-gas sintering to achieve high sintering densities.
  • the liquid phase sintering is based on the fact that the liquid phase during sintering shows a high solubility for the elements of the hard magnetic phase, so that by solution and
  • Re-deposition processes grow large magnetic grains at the expense of small grains and create a faceted, globular grain structure. This improves the coercive force of the magnetic material.
  • a disadvantage is the high cost of the neodymium element.
  • An improvement in the cost structure is achieved by CeFenTi-based hard magnets.
  • analogous liquid phase sintering using a melt of Ce and Fe and Ti fractions results in the formation of CeFe 2 by reaction of the liquid phase with CeFenTi.
  • the hard magnetic phase has poor magnetic properties due to the high amount of CeFe 2 deposited since the grains of the hard magnetic phase are attacked and the formation of the faceted grain structure important for the magnetic properties is restricted. Disclosure of the invention
  • the inventive method for producing a magnetic material according to the main claim overcomes these disadvantages. It will be a
  • Hard magnetic phase are magnetically decoupled by the formation of a grain boundary phase, so that the magnetic material has a high
  • the hard magnetic phase contains at least one element Z which is selected from one or more rare earth metals (RE) and / or yttrium.
  • RE rare earth metals
  • iron, titanium and at least one further element X are contained in the hard magnetic phase.
  • the hard magnetic phase has the following formula:
  • the element X or mixtures of the elements listed above to X can substitute Fe or Ti. The proportion in At% of element X (sum of e + f) is then subtracted from the At% content of Fe or Ti.
  • Z a is understood to mean that one or more
  • the hard magnetic phase according to the invention is a
  • Hard magnetic phase formed according to the invention mentioned elements is significantly cost-reduced compared to a neodymium-rich hard magnetic phase, but still characterized by a high coercive force. this will supported by the fact that the hard magnetic grains are very well magnetically decoupled by the grain boundary phase produced according to the invention.
  • the grain boundary phase comprises at least one metal M and has a melting range below the peritectic temperature of the hard magnetic phase.
  • the method for producing the magnetic material described above comprises a step of hot pressing and / or hot working.
  • crystallographic axes arise in the direction of the applied force.
  • Hot forming can be followed by hot pressing.
  • the novel hot-pressing and / or hot-forming process produces a nanocrystalline magnetic material with outstanding magnetic properties in a process-technically simple manner and thus without high technical or energy-related expense Get properties.
  • a first alloy of a stoichiometric mixture of Elements of the hard magnetic phase to be produced as well as the at least one metal M are produced here.
  • "Stoichiometric" means that the elements of the hard magnetic phase to be produced are proportionately mixed with each other as they subsequently also exist in the hard magnetic phase
  • the metal M has a melting range below the peritectic temperature of produced
  • Hard magnetic phase which is reflected in the melting range of the grain boundary phase. If several metals M are used, they are present in the form of an alloy or are further processed into an alloy which has a melting range which is below the peritectic temperature of the hard magnet phase to be produced.
  • the first alloy becomes so
  • nanocrystalline is understood as meaning particles and grains having a particle size of less than 500 nm.
  • the grains and particles have a particle size of less than 100 nm and in particular from 30 to 50 nm.
  • the nanocrystalline first alloy is then pulverized and the resulting powder, ie the powdered first alloy, precompressed by hot pressing as described above and hot worked at a temperature at or above the melting range of the metal M and below the peritectic temperature of the hard magnetic phase.
  • the hot pressing may advantageously be carried out at pressures around 500 MPa and also at a temperature at or above the melting range of the metal M (or the alloy of the metals M) and below the peritectic temperature of the hard magnetic phase.
  • Hot forming is preferably carried out at pressures around 100 MPa.
  • the magnetic material obtained by the specified method in addition to a high energy product and a high remanence, also has a high coercive force.
  • a so-called multi-alloying is used.
  • a second alloy of a stoichiometric mixture of Produced elements of the hard magnetic phase to be produced and then processed so that the second alloy has a nanocrystalline structure.
  • the obtained nanocrystalline second alloy is then pulverized.
  • nanocrystalline is understood as meaning particles and grains having a particle size of less than 500 nm.
  • At least one metal M is provided, wherein the metal M has a melting range below the peritectic temperature of the hard magnetic phase to be produced. If several metals M are used, they are in the form of an alloy or are processed to an alloy which has a melting range which is below the peritectic temperature of the hard magnet phase to be produced.
  • the metal M or the alloy of the metals M is then likewise further processed so that the metal M or the alloy of the metals M has a nanocrystalline structure.
  • the nanocrystalline material obtained from the metal M / from the metals M is then pulverized.
  • Hot pressing and hot working the hot pressed mixture at a temperature at or above the melting range of the metal M (or the alloy of the metals M) and below the peritectic temperature of the hard magnetic phase.
  • the processing of the metal M, the first alloy and / or the second alloy to a metal M or an alloy with nanocrystalline structure by melt spinning, high energy milling or mechanical alloying carried out. These methods are easy to apply and allow nanocrystalline structures with maximum grain sizes below 100 nm.
  • Grain boundary diffusion includes a first step of applying at least one metal M having a melting range below the peritectic temperature of the hard magnetic phase to the surface of the hot-worked magnetic material.
  • the metal M is preferably identical to the metal M of the grain boundary phase. This also applies to the use of several metals M. This is followed by a temperature treatment at or above the melting range of the metal M, whereby the metal M diffuses into the magnetic material along the grain boundaries.
  • the rare earth metal used in combination with cerium is advantageously selected from: La, Nd, Pr or Sm. Mixtures of these elements are also possible.
  • the transition metal is at least one element selected from the group consisting of: Co, Ni and Mn.
  • the hard magnetic phase has a ThMni2 structure.
  • the melting range of the grain boundary phase is below 1 100 ° C, preferably below 900 ° C and more preferably below 600 ° C. This facilitates the dissolution and elimination processes.
  • the grains of the hard magnetic phase are less affected and the structure of the forming grains is particularly faceted and globular. To improve the wetting of the hard magnetic grains during the
  • Dissolution process for example during hot pressing and / or during
  • the grain boundary phase contains at least one element selected from the group consisting of: Ag, Ga, Cu, Ce, Al, Si, Nd, Y, Pr, Sm, and La.
  • a grain boundary phase has proven that at least one alloy of: Mg 9 3Nd 7 , Cu 3 oNd 7 o, Cu 2 8La 7 2, Cu 2 8Sm 7 2, CaerA, NdGa 6 , CuAl 2 , Mg 4 iNd 5 ,
  • Al 3 Ca 8 LaFe, Fe 2 Ti, CuCe, Cu 2 Ce, AICu, Al 2 Cu, Al 8 Cu 4 Ce, Al 4 CuCe, CeAl, CeFe, CeFe 2 , CeGa, CeSi, CeZn, CeSn, CeAg, AICuCe, SmCu, SmCu 2 , SmCu 4 , SmCuO, SmCu6, Nd 2 Cu and NdCu.
  • these alloys When these alloys are used, for example, for processing by hot pressing and / or hot forming, they do not show a strong reaction with the elements of the hard magnetic phase, but have a high solubility for the elements of the hard magnetic phase, so that the dissolution and precipitation processes are promoted, which a highly globular and faceted grain structure of the hard magnetic phase leads.
  • the solubility of the elements of the hard magnetic phase in the grain boundary phase at low temperature is lower, since during cooling a high proportion of hard magnetic phase is formed by precipitation.
  • the grains of the hard magnetic phase are not attacked, whereby the magnetic properties are improved.
  • Eutectic CeCu alloys have a eutectic at about 407 ° C.
  • copper significantly improves the wetting of the hard magnetic grains compared to a commonly used cerium melt without copper.
  • a part of the hard magnetic grains is released during processing by hot pressing and / or hot forming in the liquid-forming grain boundary phase.
  • Upon cooling depending on the composition and cooling conditions, e.g.
  • Eutectic Al-Cu-Ce alloys have a eutectic at about 550 ° C.
  • a melt of this eutectic alloy has a good wetting ability during processing by hot pressing and / or hot forming.
  • Part of the hard magnetic grains dissolves in the melt of the forming grain boundary phase.
  • phases such as CuCe, Cu 2 Ce, Fe 2 Ti, A Cu, AlCl 2 Ce, AUCuCe or CeFe 2 form directly from the melt. The formation of CeFe2 is significantly reduced.
  • La does not form binary phases with any of the elements Fe, Ce and Ti, whereby the hard magnetic grains of the hard magnetic phase are not attacked.
  • the magnetic material is essentially free of boron, except for unavoidable technical amounts.
  • An addition of boron to the elements of the hard magnetic phase is thus advantageously not carried out.
  • an electric machine which is designed in particular as an electric motor, stator or generator.
  • the electric machine comprises at least one magnetic material produced as described above and is characterized by a high
  • FIG. 1 shows a schematic sectional view of a microstructure of a magnetic produced according to an advantageous embodiment of the method according to the invention
  • FIG. 1 shows a magnetic material 1 which has a hard magnetic phase 2 and a grain boundary phase 3.
  • Hard magnetic phase 2 consists of hard magnetic grains 4, which through the
  • Grain boundary phase 3 separated and thus also be decoupled magnetically.
  • the hard magnetic phase 2 contains at least one element Z.
  • the element Z contains at least one rare earth element RE and / or yttrium. If one
  • the hard magnetic phase 2 contains at least one transition metal TM, iron and titanium.
  • the hard magnetic phase 2 can be described by the following formula:
  • TMbFe c -eTide-fXe + f Z a TMbFe c -eTide-fXe + f
  • a 7 to 9 at%
  • b ⁇ 41 at%
  • d 7 to 9 at%
  • the grain boundary phase 3 contains at least one metal M and has one
  • Hard magnet phase 2 is located.
  • the magnetic material 1 is characterized by a high coercive field strength, a high remanence and a high maximum energy product (BH) max.
  • the first alloy was then further processed to have a nanocrystalline structure. Then, the first alloy was pulverized.
  • the powder of the first alloy was precompressed by hot pressing and then hot worked.
  • the magnetic grains consisting of the elements of the hard magnetic phase and the Grain boundary phase were obtained, compressed.
  • the magnetic grains were magnetically isotropic and thus had no preferred magnetic direction.
  • Subsequent hot working transformed the magnetically isotropic material into a magnetically anisotropic high energy product.
  • the magnetic preferred direction is indicated in Figure 1 by the arrows.

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

Abstract

L'invention concerne un procédé de fabrication d'un matériau magnétique, comprenant une phase magnétique dure (2) et une phase de limite de grains (3), la phase magnétique dure (2) comprenant au moins un élément Z, choisi parmi : un ou plusieurs métaux de terres rares (RE) et/ou l'yttrium ; le fer et le titane et la phase magnétique dure (2) présente la formule suivante : ZaTMbFec-eTid-fXe+f, TM étant au moins un métal de transition, a = 7 à 9 % atomique, b ≤ 41 % atomique, c ≥ 41 % atomique, d = 7 à 9 % atomique, X est choisi dans le groupe constitué de : Mo, V, Ta, Nb, Cr, Si, B, Zr, AI, W, Pd et P, e+f = 0 à 4,5 % atomique, le métal des terres rares (RE) contient au moins 3,5 % atomique de Cer et a+b+(c-e)+(d-f)+(e+f) = 100 % atomique et la phase de limite de grains (3) comprenant au moins un métal M et présentant une zone de fusion inférieure à la température péritectique de la phase magnétique dure (2). Le procédé comprend une étape de pression à chaud et/ou de mise en forme à chaud.
PCT/EP2016/076770 2015-11-10 2016-11-07 Procédé de fabrication d'un matériau magnétique et machine électrique WO2017080935A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN201680065417.3A CN108352232A (zh) 2015-11-10 2016-11-07 制造磁性材料的方法和电机

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102015222075.3 2015-11-10
DE102015222075.3A DE102015222075A1 (de) 2015-11-10 2015-11-10 Verfahren zu Herstellung eines magnetischen Materials und elektrische Maschine

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WO2017080935A1 true WO2017080935A1 (fr) 2017-05-18

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DE (1) DE102015222075A1 (fr)
WO (1) WO2017080935A1 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113652594A (zh) * 2021-08-02 2021-11-16 自贡硬质合金有限责任公司 一种难熔金属基合金及其制备方法

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CN108352232A (zh) 2018-07-31

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