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WO2010073590A1 - Composite soft magnetic material and method for producing same - Google Patents

Composite soft magnetic material and method for producing same Download PDF

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Publication number
WO2010073590A1
WO2010073590A1 PCT/JP2009/007070 JP2009007070W WO2010073590A1 WO 2010073590 A1 WO2010073590 A1 WO 2010073590A1 JP 2009007070 W JP2009007070 W JP 2009007070W WO 2010073590 A1 WO2010073590 A1 WO 2010073590A1
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WO
WIPO (PCT)
Prior art keywords
powder
sendust alloy
soft magnetic
magnetic material
iron powder
Prior art date
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PCT/JP2009/007070
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French (fr)
Japanese (ja)
Inventor
渡辺宗明
五十嵐和則
Original Assignee
三菱マテリアル株式会社
株式会社ダイヤメット
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Application filed by 三菱マテリアル株式会社, 株式会社ダイヤメット filed Critical 三菱マテリアル株式会社
Priority to JP2010543839A priority Critical patent/JPWO2010073590A1/en
Priority to CN2009801528854A priority patent/CN102264492A/en
Publication of WO2010073590A1 publication Critical patent/WO2010073590A1/en

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    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01FMAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F41/00Apparatus 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
    • H01F41/02Apparatus 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
    • H01F41/0206Manufacturing of magnetic cores by mechanical means
    • H01F41/0246Manufacturing of magnetic circuits by moulding or by pressing powder
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B22CASTING; POWDER METALLURGY
    • B22FWORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F1/00Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
    • B22F1/12Metallic powder containing non-metallic particles
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B22CASTING; POWDER METALLURGY
    • B22FWORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F1/00Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
    • B22F1/16Metallic particles coated with a non-metal
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/02Ferrous alloys, e.g. steel alloys containing silicon
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/06Ferrous alloys, e.g. steel alloys containing aluminium
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01FMAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/12Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials
    • H01F1/14Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys
    • H01F1/20Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder
    • H01F1/22Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder pressed, sintered, or bound together
    • H01F1/24Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder pressed, sintered, or bound together the particles being insulated
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01FMAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/12Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials
    • H01F1/14Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys
    • H01F1/147Alloys characterised by their composition
    • H01F1/14766Fe-Si based alloys
    • H01F1/14791Fe-Si-Al based alloys, e.g. Sendust
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01FMAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/12Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials
    • H01F1/14Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys
    • H01F1/20Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder
    • H01F1/22Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder pressed, sintered, or bound together
    • H01F1/24Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder pressed, sintered, or bound together the particles being insulated
    • H01F1/26Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder pressed, sintered, or bound together the particles being insulated by macromolecular organic substances

Definitions

  • the present invention relates to a composite soft magnetic material obtained by mixing and compacting an insulating iron powder and a sendust alloy powder together with a binder and firing the mixture, and a method for producing the same.
  • This application claims priority based on Japanese Patent Application No. 2008-330597 for which it applied to Japan on December 25, 2008, and uses the content here.
  • Electromagnetic components for electronic devices such as inverters, transformer cores, and choke coils are required to have stricter material properties as electronic devices become smaller and have higher performance.
  • metal magnetic materials such as Sendust alloy and silicon steel, and oxide magnetic materials such as ferrite have been used as soft magnetic materials for such parts.
  • metallic magnetic materials such as Sendust alloy have a high hardness when powdered, and there is a problem that it is difficult to increase the density by powder molding.
  • a metal soft magnetic powder having an insulating coating, and a raw material powder consisting of a lubricant powder and a binder added as needed are filled in a mold cavity. After that, a green compact having a desired shape is produced by pressure molding, and then the green compact is fired to produce a composite soft magnetic material.
  • Sendust alloy has very little plastic deformation when processed at room temperature and can be pulverized by pulverization, but cannot be formed into a plate shape. Therefore, when Sendust alloy powder is molded to produce magnetic parts such as magnetic cores, plastic deformation hardly occurs. Therefore, Sendust alloy powder is simply connected with the added binder. Even if the permeability of the sendust alloy powder itself is high, there is a problem that a high permeability cannot be obtained when a dust core is used.
  • Patent Document 1 Also known is a composite magnetic material obtained by mixing a Sendust alloy powder having an oxide film, a highly compressible soft magnetic metal powder, a soft ferrite powder, and a binder, followed by sintering and sintering.
  • the soft magnetic composite material produced by coating the metal magnetic powder such as Permalloy with an oxide magnetic material such as ferrite has a problem that the magnetic properties deteriorate because the metal and ferrite easily react at the interface between them when heat-treated. Had. Further, in the method of mixing Sendust alloy powder and other soft magnetic metal powder, since Sendust alloy powder is very hard, even if soft magnetic metal powder having good compressibility is mixed, 20 ton / cm 2. A high pressure molding technique of a certain level is required, and there is a problem that only a product having a simple shape such as a cylindrical shape such as a dust core can be obtained.
  • the present invention has been proposed in view of such conventional circumstances, and its purpose is to select iron powders to be mixed with Sendust alloy powder, the range of their addition amount, and the respective particle size ranges.
  • it is made into an optimal composition, while maintaining high saturation magnetic flux density inherent in iron powder, while high permeability, low coercivity, inherent in Sendust alloy powder,
  • the composite soft magnetic material according to the present invention comprises an insulating iron powder, a sendust alloy powder, and a binder mixed and compacted and fired, and the iron powder and the sendust alloy powder are compacted.
  • a fired main phase and a grain boundary phase mainly composed of a binder formed around the main phase are provided, and the proportion of Sendust alloy in the main phase is 5% by mass or more and less than 20% by mass.
  • the saturation magnetic flux density is 1 T or more at a magnetic field of 10 kA / m
  • the coercive force is 260 A / m or less
  • the iron loss (at 0.1 T, 10 kHz) is 20 W / kg or less.
  • the average particle size of the iron main phase formed by compacting and firing the iron powder is 20 to 50 ⁇ m, and the average particle size of the alloy main phase formed by compacting and firing the Sendust alloy powder.
  • the thickness can be 50 to 120 ⁇ m.
  • pure iron powder having an Mg-containing oxide film can be used as the insulated iron powder.
  • the method for producing a composite soft magnetic material according to the present invention comprises a main phase formed by compacting at least mixed compacted and sintered iron powder, sendust alloy powder and binder, and then compacting the iron powder and sendust alloy powder. And a sendust alloy occupying the total mass of the insulated iron powder and sendust alloy powder in producing a composite soft magnetic material having a grain boundary phase mainly composed of a binder formed around the main phase.
  • the addition ratio of the powder is 5 mass% or more and less than 20 mass%
  • the insulated iron powder and Sendust alloy powder are mixed and compacted and fired to obtain a saturation magnetic flux density of 1 T or more at a magnetic field of 10 kA / m, a coercive force.
  • a composite soft magnetic material having 260 A / m or less and iron loss (at 0.1 T, 10 kHz) of 20 W / kg or less is obtained.
  • the addition ratio or blending ratio of Sendust alloy powder is the ratio of Sendust alloy powder to the total mass of Sendust alloy powder and the iron powder insulated with Mg-containing oxide coating or the like. It means a compounding ratio (mass%).
  • the method for producing a composite soft magnetic material according to the present invention is characterized by using an insulated iron powder having an average particle diameter of 20 to 50 ⁇ m and a sendust alloy powder having an average particle diameter of 50 to 120 ⁇ m.
  • the method for producing a composite soft magnetic material according to the present invention is characterized in that pure iron powder insulated with an Mg-containing oxide film is used as the insulated iron powder.
  • the soft magnetic characteristics such as low iron loss, low coercive force, and low eddy current loss of the proper amount of sendust alloy powder are effective.
  • the composite soft magnetic material obtained in the above can be provided.
  • a soft magnetic material can be provided.
  • pure iron powder insulated with an Mg-containing oxide coating is used as the insulated iron powder to ensure high saturation magnetic flux density, low iron loss, low coercive force, and low eddy current loss. It is possible to get to.
  • FIG. 1 is a graph showing the relationship between the blending ratio of sendust alloy powder and the specific resistance in an example of a composite soft magnetic material according to the present invention.
  • FIG. 2 is a diagram showing the relationship between the blending ratio of the sendust alloy powder and the saturation magnetic flux density in the example of the composite soft magnetic material according to the present invention.
  • FIG. 3 is a diagram showing the relationship between the saturation magnetic flux density and the loss in the example of the composite soft magnetic material according to the present invention.
  • FIG. 4 is a diagram showing the relationship between the blending ratio of the sendust alloy powder and the loss in the example of the composite soft magnetic material according to the present invention.
  • FIG. 5 is a diagram showing the relationship between the blending ratio of Sendust alloy powder and mechanical strength in the example of the composite soft magnetic material according to the present invention.
  • a powder compact having a predetermined shape can be obtained by filling the mixed powder obtained by adding and mixing a binder and a lubricant as necessary into a mold cavity of a compacting device, followed by pressure molding. Thereafter, the obtained green compact is fired in a predetermined temperature range, whereby a composite soft magnetic material having a desired shape can be obtained.
  • Insulated pure iron powder used in the present invention is, for example, an Mg-containing oxide in which a Mg—Fe—O ternary oxide deposition film containing (Mg, Fe) O is coated on the surface of pure iron particles.
  • Wet powder-coated pure iron powder, phosphate-coated pure iron powder, or a wet solution such as silica sol-gel solution (silicate) or alumina sol-gel solution is mixed and coated on the surface of pure iron powder, then dried and fired
  • the present invention is not limited to this, and it is possible to widely apply insulated pure iron powder having a structure in which pure iron powder is coated with an insulating coating layer. it can.
  • the Mg-containing oxide-coated pure iron powder coated with the Mg—Fe—O ternary oxide deposited film is obtained, for example, by the following production method (A), (B), (C) or (D). be able to.
  • A Pure iron powder is subjected to an oxidation treatment in an oxidizing atmosphere at room temperature to 500 ° C., and then mixed powder obtained by adding and mixing Mg powder to this powder is temperature: 150 to 1100 ° C., pressure When heated in an inert gas atmosphere or vacuum atmosphere of 1 ⁇ 10 ⁇ 12 to 1 ⁇ 10 ⁇ 1 MPa and further heated in an oxidizing atmosphere at a temperature of 50 to 400 ° C.
  • the surface of pure iron powder Mg-containing oxide-coated pure iron particles having an oxide insulating film containing Mg are obtained.
  • B After subjecting the pure iron powder to the oxidation treatment described above, after adding and mixing the silicon monoxide powder, or while mixing, heating in a vacuum atmosphere at a temperature of 600 to 1200 ° C., After adding and mixing Mg powder, or heating while mixing in a vacuum atmosphere at a temperature of 400 to 800 ° C., an Mg—Si containing oxide film is formed on the surface of pure iron powder. A material-coated pure iron powder is obtained.
  • the Mg—Si-containing oxide film is formed on the surface of the pure iron powder.
  • the addition amount of the silicon monoxide powder can be in the range of 0.01 to 1% by mass, and the addition amount of the Mg powder can be in the range of 0.05 to 1% by mass.
  • the vacuum atmosphere may be a vacuum atmosphere at a pressure of 1 ⁇ 10 ⁇ 12 to 1 ⁇ 10 ⁇ 1 MPa.
  • the Mg-containing oxide-coated pure iron particles obtained by these production methods have remarkably excellent coating adhesion of the Mg—Fe—O ternary oxide deposited film containing (Mg, Fe) O, Even if these particles are pressed to produce a green compact, the insulating coating is less likely to be broken and peeled off.
  • the oxide-coated pure iron powder is preferably a powder having an average particle size in the range of 20 to 50 ⁇ m. The reason is that if the average particle size is too small, the compressibility of the powder decreases and the value of the saturation magnetic flux density decreases, which is not preferable. On the other hand, if the average particle size is too large, the eddy current inside the soft magnetic powder is not preferable. This is because the magnetic permeability at a high frequency is likely to increase and decrease.
  • a sendust alloy for example, composition ratio: 10 mass% Si-6 mass% Al-residual Fe
  • a powder having a particle size range of 50 to 120 ⁇ m can be used.
  • the oxide-coated pure iron powder and Sendust alloy powder are each mixed with a binder material containing Si, such as silicone resin as a binder material, and each powder is made into a silicone resin-coated powder. .
  • the temperature is in the range of 150 to 250 ° C, more preferably 200 to 250 ° C. Can be baked and coated in the range of.
  • the temperature is in the range of 80 to 250 ° C., more preferably in the range of 100 to 200 ° C. It can be baked and coated by heating.
  • the baking temperature can be selected from a range of 150 to 250 ° C. A decrease in specific resistance, which is considered to be caused by damage to the insulation coating, is observed, and if it exceeds 250 ° C., the binder material becomes hard and the packing density during molding is decreased, which is not desirable. Even within this range, a baking temperature in the range of 200 to 250 ° C. is more preferable in order to obtain higher density and specific resistance.
  • a temperature range of 80 to 250 ° C can be selected as the baking temperature. If the temperature is outside this range, a decrease in density or variation may be observed during molding. At temperatures exceeding 250 ° C., the specific resistance is decreased, which is not desirable. Even within this range, a baking temperature in the range of 100 to 200 ° C. is more preferable in order to obtain higher density and specific resistance.
  • the ratio of the mass of the Sendust alloy powder coated with the binder material to the total mass of the oxide-coated pure iron powder coated with these binder materials and the Sendust alloy powder coated with the binder material is 5% by mass or more and 20% by mass.
  • These powders are mixed so as to be less than the minimum, accommodated in a mold of a compacting apparatus, and warm-molded into a desired shape with a molding temperature of about 8 to 10 Ton / cm 2 at a mold temperature of 80 to 150 ° C. and consolidated. Let it be the body.
  • the molding pressure of about 8 to 10 Ton / cm 2 used here is much lower than the conventional molding pressure of about 20 Ton / cm 2 used for compacting Sendust alloy powder, and the compacting force used for general powder molding methods.
  • the Sendust alloy powder to produce an excellent composite soft magnetic material according to the present invention even at a general molding pressure.
  • the compact is fired at a temperature of 500 ° C. to 800 ° C. for about 1 hour in a vacuum atmosphere, an inert gas atmosphere (Ar, N 2 ), or in a non-oxidizing atmosphere (H 2 atmosphere) to obtain the desired composite.
  • a soft magnetic material can be obtained.
  • the pure iron powder subjected to insulation treatment is consolidated into an iron main phase
  • Sendust alloy powder is consolidated into a Sendust alloy main phase.
  • the target composite soft magnetic material can be obtained by exhibiting a structure in which a grain boundary phase formed as a result of firing the binder material so as to be present at those grain boundaries with respect to the main phase constituted by.
  • the composite soft magnetic material manufactured as described above has low loss in the high frequency range (10 to 20 kHz), excellent iron loss, hysteresis loss, coercive force, low eddy current loss, and high specific resistance. Has soft magnetic properties. This is because the composite soft magnetic material of the present invention covers pure iron powder with a film of the Mg—Fe—O ternary oxide deposited film containing (Mg, Fe) O having excellent insulation and adhesion.
  • the pure iron powder with a suitable particle size range is mixed with a suitable amount of Sendust alloy powder with a suitable particle size range, consolidated, and fired to form a composite soft magnetic material.
  • the insulation treatment of the pure iron powder is not limited to the above-described coating with the Mg—Fe—O ternary oxide deposited film containing (Mg, Fe) O, and the phosphate-coated pure iron powder, A similar composite soft magnetic material can be obtained also by a film subjected to another insulation treatment.
  • the composite soft magnetic material obtained by mixing pure iron powder and Sendust alloy powder and compacting as described above is mixed with soft pure iron powder in an appropriate blending ratio compared to Sendust alloy, compacted, and fired. Therefore, sufficient magnetic properties can be exhibited at a molding pressure of about 8 to 10 Ton / cm 2 .
  • the composite soft magnetic material of the present invention has a low loss in the high frequency range (10 to 20 kHz) inherent to the sendust alloy powder by setting the addition ratio of the sendust alloy powder in the range of 5% by mass or more and less than 20% by mass. Excellent soft magnetic properties such as low iron loss, hysteresis loss, coercive force, low eddy current loss, and high specific resistance can be obtained.
  • the send rate of the sendust alloy powder is less than the above range, these characteristics cannot be exhibited effectively.
  • the addition ratio of Sendust alloy powder is too large, the amount of pure iron powder decreases, so it becomes difficult to obtain a high saturation magnetic flux density and the pressure required during molding becomes high, and the molding pressure in the above range is good. It becomes difficult to obtain the density.
  • Examples of the electromagnetic circuit component configured using the composite soft magnetic material of the present invention include a magnetic core, a motor core, a generator core, a solenoid core, an ignition core, a reactor core, a transformer core, a choke coil core, and a magnetic sensor core. These are electromagnetic circuit components that can exhibit excellent characteristics in any case. Examples of electric devices incorporating these electromagnetic circuit components include an electric motor, a generator, a solenoid, an injector, an electromagnetically driven valve, an inverter, a converter, a transformer, a relay, or a magnetic sensor system.
  • the composite soft magnetic material of the present invention has the effect of contributing to high efficiency, high performance, small size and light weight of these electric devices.
  • MICROTRAC FRA manufactured by LEED & NORTHRUP was used.
  • pure Mg powder coated with Mg oxide the pure iron powder was heat-treated at 220 ° C. in the atmosphere to form an oxide film on the surface, and 0.3% by mass of Mg powder was added to the soft magnetic powder. Blending and rolling this blended powder with a granulation rolling agitation and mixing device in vacuum at 650 ° C.
  • Insulated pure iron powder As other insulation-coated pure iron powder, iron phosphate-coated iron powder S110i manufactured by Heganes Japan was prepared, and as a comparative sample, pure iron powder having a particle size equivalent to the above was prepared. .
  • the blending ratio of Sendust alloy powder (the blending ratio of Sendust alloy powder in the total mass of oxide-coated pure iron powder and Sendust alloy powder, mass%) is displayed in Table 1, and water density (g / cm 3), the specific resistance ( ⁇ m), ⁇ max, the saturation magnetic flux density when a magnetic field 10kA / m (B 10k a / m: T), the coercive force (Hc: a / m), iron loss (total Table 1 also shows the results of measuring the loss, hysteresis loss, eddy current loss) and mechanical strength (compression crushing strength: N / mm 2 ).
  • FIG. 1 is a graph plotting the relationship between the blending ratio and specific resistance of Sendust alloy powder shown in Table 1. According to the results shown in FIG. 1, the specific resistance value is remarkably low at 0% by mass in the blending ratio of Sendust alloy powder, but the specific resistance value increases rapidly in the sample to which 5% by mass of Sendust alloy powder is added. . Further, when the blending ratio is 20% by mass or more, the reduction ratio of specific resistance increases. Therefore, the blending ratio of Sendust alloy powder is preferably 5% by mass or more and less than 20% by mass.
  • FIG. 2 is a graph plotting the relationship between the blending ratio of Sendust alloy powder shown in Table 1 and the saturation magnetic flux density. According to the results shown in FIG. 2, the saturation magnetic flux density rapidly decreases when the blending ratio is 20% by mass or more. Therefore, the blending ratio of Sendust alloy powder to oxide-coated pure iron powder is preferably 5% by mass or more and less than 20% by mass in order to obtain a saturation magnetic flux density of 1T or more at a magnetic field of 10 kA / m, and a magnetic field of 10 kA / m. In order to obtain a saturation magnetic flux density of 1.1 T, 5 mass% or more and 10 mass% or less are more preferable.
  • FIG. 3 is a graph plotting the relationship between the magnetic flux density and the iron loss at the magnetic field of 10 kA / m shown in Table 1 (when the magnetic flux density is 0.1 T and the frequency is 10 kHz). According to the results shown in FIG. 3, the iron loss can be reduced without reducing the magnetic flux density by blending the sendust alloy powder.
  • FIG. 4 is a graph plotting the relationship between the blending ratio of the Sendust alloy powder shown in Table 1 and the loss. According to the result shown in FIG. 4, a blending ratio of less than 20% by mass is preferable for the loss. Moreover, when the blending ratio of Sendust alloy powder is 5 mass% or more and less than 20 mass%, an iron loss (at a magnetic flux density of 0.1 T and a frequency of 10 kHz) of 20 W / kg or less can be realized.
  • FIG. 5 is a graph plotting the relationship between the blending ratio of Sendust alloy powder shown in Table 1 and the mechanical strength. According to the results shown in FIG. 5, it is clear that the crushing strength has a mechanical strength peak between 5 and 10% by mass, but there is no problem in the practical range for the blending ratio of Sendust alloy powder. It turns out that it is.
  • a silicone resin-coated sendust in which 0.5% by mass of a silicone resin is mixed with pure iron powder and then baked at 250 ° C. is mixed with 1% by mass of silicone resin and baked at 200 ° C.
  • the alloy powder was blended so that the blending ratio of the silicone resin-coated Sendust alloy powder in the total mass of the silicone resin-coated pure iron powder and the silicone resin-coated Sendust alloy powder was 7% by mass.
  • the silicone resin-coated Sendust alloy powder obtained by mixing 1% by mass of silicone resin with Sendust alloy powder and baking at 150 ° C. 0.5% by mass of silicone resin is mixed to 150 ° C., 200 ° C., 250 ° C. , And 270 ° C.
  • the blending ratio of the silicone resin-coated Sendust alloy powder occupying the total mass of the silicone resin-coated Sendust alloy powder and the silicone resin-coated Sendiron alloy powder is 7%. %.
  • the baking temperature of the silicone resin with respect to the pure iron powder can be selected in the range of 150 to 250 ° C, more preferably in the range of 200 to 250 ° C.
  • Silicone resin-coated pure iron powder obtained by mixing 0.5% by mass of a silicone resin with pure iron powder and baking at 250 ° C. and 1% by mass of silicone resin were mixed at 50 ° C., 80 ° C., 100 ° C., 150 ° C., The silicone resin-coated Sendust alloy powder occupies the total mass of the silicone resin-coated pure iron powder and the silicone resin-coated Sendust alloy powder. It mix
  • the baking temperature of the silicone resin in the Sendust alloy powder can be selected in the range of 80 to 250 ° C, more preferably in the range of 100 to 200 ° C.
  • the soft magnetic characteristics such as low iron loss, low coercive force, and low eddy current loss of the proper amount of sendust alloy powder are effective.
  • the composite soft magnetic material obtained in the above can be provided.

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Abstract

Disclosed is a composite soft magnetic material which is characterized by being obtained by mixing, compacting and firing an iron powder, which has been subjected to an insulating treatment, a Sendust alloy powder and a binder.  The composite soft magnetic material is also characterized by comprising a main phase in which the iron powder and the Sendust alloy powder are compacted, and a grain boundary phase which is formed around the main phase and is mainly composed of the binder, and by having a ratio of the Sendust alloy in the main phase of 5% by mass or more, but less than 20% by mass, a saturation magnetic flux density at a magnetic field of 10 kA/m of 1 T or more, a coercivity of 260 A/m or less, and an iron loss (at 0.1 T, 10 kHz) of 20 W/kg or less.  Consequently, the composite soft magnetic material has characteristics of the Sendust alloy, namely a high magnetic permeability, low coercivity and low iron loss, while maintaining a high saturation magnetic flux density which is intrinsic to an iron powder.  Also disclosed is a method for producing the composite soft magnetic material.

Description

複合軟磁性材料とその製造方法Composite soft magnetic material and manufacturing method thereof
 本発明は、絶縁処理された鉄粉末とセンダスト合金粉末をバインダーとともに混合圧密し、焼成してなる複合軟磁性材料とその製造方法に関する。
 本願は、2008年12月25日に日本に出願された特願2008-330597号に基づき優先権を主張し、その内容をここに援用する。
The present invention relates to a composite soft magnetic material obtained by mixing and compacting an insulating iron powder and a sendust alloy powder together with a binder and firing the mixture, and a method for producing the same.
This application claims priority based on Japanese Patent Application No. 2008-330597 for which it applied to Japan on December 25, 2008, and uses the content here.
 インバーターやトランスのコア、チョークコイルなどの電子機器用電磁気部品は、電子機器の小型化、高性能化に伴い、より厳しい材料特性が求められるようになってきている。このような部品に用いられる軟磁性材料として、従来、センダスト合金やケイ素鋼などの金属磁性材料、フェライトなどの酸化物磁性材料が使用されてきた。しかし、センダスト合金などの金属磁性材料は、粉末とした場合の硬度が高く、粉末成形により高密度化することが難しい問題がある。
 例えば、粉末成形による高密度複合軟磁性材料の製造では、先ず、絶縁被膜を有する金属軟磁性粉末と、必要に応じて添加される潤滑剤粉末とバインダーからなる原料粉末を金型のキャビティに充填した後、加圧成形することによって目的の形状の圧粉体を作製し、その後、圧粉体を焼成することによって複合軟磁性材料が製造されている。
Electromagnetic components for electronic devices such as inverters, transformer cores, and choke coils are required to have stricter material properties as electronic devices become smaller and have higher performance. Conventionally, metal magnetic materials such as Sendust alloy and silicon steel, and oxide magnetic materials such as ferrite have been used as soft magnetic materials for such parts. However, metallic magnetic materials such as Sendust alloy have a high hardness when powdered, and there is a problem that it is difficult to increase the density by powder molding.
For example, in the production of high-density composite soft magnetic materials by powder molding, first, a metal soft magnetic powder having an insulating coating, and a raw material powder consisting of a lubricant powder and a binder added as needed are filled in a mold cavity. After that, a green compact having a desired shape is produced by pressure molding, and then the green compact is fired to produce a composite soft magnetic material.
 従って、成形に用いる粉末自体の硬度が高い場合、圧粉体として高い圧密度を得ることが困難となり易い問題がある。例えば、センダスト合金は室温で加工する場合、塑性変形が極めて少なく、粉砕による微粉末化は可能であるが、板状には成形できないものである。従って、磁心などの磁気部品を製造するために、センダスト合金粉末を成形しても、ほとんど塑性変形しないから、センダスト合金粉末は添加した結合剤で単純に結びついている状態となっているのみであり、センダスト合金粉末自体の透磁率は高くとも、圧粉磁心とした場合に高い透磁率を得ることができない問題がある。 Therefore, when the hardness of the powder itself used for molding is high, there is a problem that it is difficult to obtain a high pressure density as a green compact. For example, Sendust alloy has very little plastic deformation when processed at room temperature and can be pulverized by pulverization, but cannot be formed into a plate shape. Therefore, when Sendust alloy powder is molded to produce magnetic parts such as magnetic cores, plastic deformation hardly occurs. Therefore, Sendust alloy powder is simply connected with the added binder. Even if the permeability of the sendust alloy powder itself is high, there is a problem that a high permeability cannot be obtained when a dust core is used.
 そこで従来、酸化物磁性材料と金属磁性材料を混合し、複合化して、高性能化しようとする試みがなされている。
 例えば、パーマロイなどの金属磁性粉末をフェライトなどの酸化物磁性材料で被覆し、その後に成形して熱処理する方法が知られている。(特許文献1参照)
 また、酸化被膜を有するセンダスト合金粉末と高圧縮性の軟磁性金属粉末とソフトフェライト粉末とバインダーを混合し、圧密後に焼成処理してなる複合磁性材料が知られている。(特許文献2参照)
Therefore, conventionally, attempts have been made to improve the performance by mixing an oxide magnetic material and a metal magnetic material to form a composite.
For example, a method is known in which a metal magnetic powder such as permalloy is coated with an oxide magnetic material such as ferrite and then molded and heat-treated. (See Patent Document 1)
Also known is a composite magnetic material obtained by mixing a Sendust alloy powder having an oxide film, a highly compressible soft magnetic metal powder, a soft ferrite powder, and a binder, followed by sintering and sintering. (See Patent Document 2)
特開昭56-38402号公報JP-A-56-38402 特開平6-236808号公報JP-A-6-236808
 前記パーマロイなどの金属磁性粉末をフェライトなどの酸化物磁性材料で被覆して製造される軟磁性複合材料は、熱処理するとそれらの界面で金属とフェライトが反応し易いので、磁気特性が劣化するという問題を有していた。
 また、センダスト合金粉末と他の軟磁性金属粉末を混合する方法にあっては、センダスト合金粉末が非常に硬いために、圧縮性の良好な軟磁性金属粉末を混合したとしても、20ton/cm程度の高圧成形技術が必要となり、ダストコアなど、円筒形のような単純な形状の製品しか得られないという問題を有していた。
The soft magnetic composite material produced by coating the metal magnetic powder such as Permalloy with an oxide magnetic material such as ferrite has a problem that the magnetic properties deteriorate because the metal and ferrite easily react at the interface between them when heat-treated. Had.
Further, in the method of mixing Sendust alloy powder and other soft magnetic metal powder, since Sendust alloy powder is very hard, even if soft magnetic metal powder having good compressibility is mixed, 20 ton / cm 2. A high pressure molding technique of a certain level is required, and there is a problem that only a product having a simple shape such as a cylindrical shape such as a dust core can be obtained.
 本発明は、このような従来の事情に鑑みて提案されたものであり、その目的は、センダスト合金粉末に対して混合する鉄粉末の選定と、それらの添加量の範囲、それぞれの粒径範囲を好適に選択し、バインダーの条件等も加味して最適な配合とすることにより、鉄粉末が本来有する高い飽和磁束密度を維持しながら、センダスト合金粉末が本来有する高透磁率、低保磁力、低鉄損失の特性を併せ持つことができるようにした複合軟磁性材料とその製造方法の提供を目的とする。 The present invention has been proposed in view of such conventional circumstances, and its purpose is to select iron powders to be mixed with Sendust alloy powder, the range of their addition amount, and the respective particle size ranges. By suitably selecting and taking into account the conditions of the binder and the like, it is made into an optimal composition, while maintaining high saturation magnetic flux density inherent in iron powder, while high permeability, low coercivity, inherent in Sendust alloy powder, It is an object of the present invention to provide a composite soft magnetic material and a method for manufacturing the same, which can have the characteristics of low iron loss.
 上記目的を達成するために、本発明に係る複合軟磁性材料は、絶縁処理された鉄粉末とセンダスト合金粉末とバインダーが混合圧密され、焼成されてなり、前記鉄粉末とセンダスト合金粉末が圧密され焼成された主相と、前記主相の周囲に生成されたバインダーを主体とする粒界相とが具備されてなり、前記主相に占めるセンダスト合金の割合が5質量%以上、20質量%未満であり、磁場10kA/m時の飽和磁束密度1T以上、保磁力260A/m以下、鉄損(0.1T、10kHz時)20W/kg以下であることを特徴とする。
 本発明に係る複合軟磁性材料において、前記鉄粉末を圧密し焼成してなる鉄主相の平均粒径を20~50μm、センダスト合金粉末を圧密し焼成してなる合金主相の平均粒径を50~120μmとすることができる。
 本発明に係る複合軟磁性材料において、絶縁処理された鉄粉末として、Mg含有酸化物被膜を具備してなる純鉄粉末を用いることができる。
In order to achieve the above object, the composite soft magnetic material according to the present invention comprises an insulating iron powder, a sendust alloy powder, and a binder mixed and compacted and fired, and the iron powder and the sendust alloy powder are compacted. A fired main phase and a grain boundary phase mainly composed of a binder formed around the main phase are provided, and the proportion of Sendust alloy in the main phase is 5% by mass or more and less than 20% by mass. The saturation magnetic flux density is 1 T or more at a magnetic field of 10 kA / m, the coercive force is 260 A / m or less, and the iron loss (at 0.1 T, 10 kHz) is 20 W / kg or less.
In the composite soft magnetic material according to the present invention, the average particle size of the iron main phase formed by compacting and firing the iron powder is 20 to 50 μm, and the average particle size of the alloy main phase formed by compacting and firing the Sendust alloy powder. The thickness can be 50 to 120 μm.
In the composite soft magnetic material according to the present invention, pure iron powder having an Mg-containing oxide film can be used as the insulated iron powder.
 本発明に係る複合軟磁性材料の製造方法は、絶縁処理された鉄粉末とセンダスト合金粉末とバインダーを少なくとも混合圧密し、焼成することにより、前記鉄粉末とセンダスト合金粉末を圧密してなる主相と、前記主相の周囲に形成されたバインダーを主体とする粒界相とを具備した複合軟磁性材料を製造するにあたり、絶縁処理された鉄粉末とセンダスト合金粉末の質量の総和に占めるセンダスト合金粉末の添加割合を5質量%以上、20質量%未満として、絶縁処理された鉄粉末およびセンダスト合金粉末を混合圧密し、焼成することにより、磁場10kA/m時の飽和磁束密度1T以上、保磁力260A/m以下、鉄損(0.1T、10kHz時)20W/kg以下の複合軟磁性材料を得ることを特徴とする。
 本明細書において、特に断りのない限り、センダスト合金粉末の添加割合または配合比とは、Mg含有酸化物被膜等により絶縁処理された鉄粉末とセンダスト合金粉末の質量の総和に占めるセンダスト合金粉末の配合比(質量%)を意味する。
 本発明に係る複合軟磁性材料の製造方法は、平均粒径20~50μmの絶縁処理された鉄粉末を用い、平均粒径50~120μmのセンダスト合金粉末を用いることを特徴とする。
 本発明に係る複合軟磁性材料の製造方法は、絶縁処理された鉄粉末として、Mg含有酸化物被膜により絶縁処理された純鉄粉末を用いることを特徴とする。
The method for producing a composite soft magnetic material according to the present invention comprises a main phase formed by compacting at least mixed compacted and sintered iron powder, sendust alloy powder and binder, and then compacting the iron powder and sendust alloy powder. And a sendust alloy occupying the total mass of the insulated iron powder and sendust alloy powder in producing a composite soft magnetic material having a grain boundary phase mainly composed of a binder formed around the main phase. When the addition ratio of the powder is 5 mass% or more and less than 20 mass%, the insulated iron powder and Sendust alloy powder are mixed and compacted and fired to obtain a saturation magnetic flux density of 1 T or more at a magnetic field of 10 kA / m, a coercive force. A composite soft magnetic material having 260 A / m or less and iron loss (at 0.1 T, 10 kHz) of 20 W / kg or less is obtained.
In the present specification, unless otherwise specified, the addition ratio or blending ratio of Sendust alloy powder is the ratio of Sendust alloy powder to the total mass of Sendust alloy powder and the iron powder insulated with Mg-containing oxide coating or the like. It means a compounding ratio (mass%).
The method for producing a composite soft magnetic material according to the present invention is characterized by using an insulated iron powder having an average particle diameter of 20 to 50 μm and a sendust alloy powder having an average particle diameter of 50 to 120 μm.
The method for producing a composite soft magnetic material according to the present invention is characterized in that pure iron powder insulated with an Mg-containing oxide film is used as the insulated iron powder.
 本発明によれば、絶縁処理した鉄粉末が有する高い飽和磁束密度を維持しながら、適量混合したセンダスト合金粉末が有する低鉄損と低い保磁力と少ない渦電流損失のような軟磁気特性を有効に得た複合軟磁性材料を提供することができる。さらに、本発明によれば、従来のセンダスト合金粉末の成形に必要としていた高い成形力を要することなく一般的な粉末成形に必要な程度の圧力で圧密成形が可能で上述の特性を発揮できる複合軟磁性材料を提供することができる。
 また、本発明において、絶縁処理した鉄粉末として、Mg含有酸化物被膜により絶縁処理された純鉄粉末を用いることにより、高い飽和磁束密度と低鉄損と低い保磁力と少ない渦電流損失を確実に得ることが可能である。
According to the present invention, while maintaining the high saturation magnetic flux density of the insulated iron powder, the soft magnetic characteristics such as low iron loss, low coercive force, and low eddy current loss of the proper amount of sendust alloy powder are effective. The composite soft magnetic material obtained in the above can be provided. Furthermore, according to the present invention, a composite that can be compacted at a pressure required for general powder molding without exhibiting the high molding force required for the conventional Sendust alloy powder molding and can exhibit the above-described characteristics. A soft magnetic material can be provided.
In the present invention, pure iron powder insulated with an Mg-containing oxide coating is used as the insulated iron powder to ensure high saturation magnetic flux density, low iron loss, low coercive force, and low eddy current loss. It is possible to get to.
図1は、本発明に係る複合軟磁性材料の実施例において、センダスト合金粉末の配合比と比抵抗の関係を示す図である。FIG. 1 is a graph showing the relationship between the blending ratio of sendust alloy powder and the specific resistance in an example of a composite soft magnetic material according to the present invention. 図2は、本発明に係る複合軟磁性材料の実施例において、センダスト合金粉末の配合比と飽和磁束密度の関係を示す図である。FIG. 2 is a diagram showing the relationship between the blending ratio of the sendust alloy powder and the saturation magnetic flux density in the example of the composite soft magnetic material according to the present invention. 図3は、本発明に係る複合軟磁性材料の実施例において、飽和磁束密度と損失の関係を示す図である。FIG. 3 is a diagram showing the relationship between the saturation magnetic flux density and the loss in the example of the composite soft magnetic material according to the present invention. 図4は、本発明に係る複合軟磁性材料の実施例において、センダスト合金粉末の配合比と損失との関係を示す図である。FIG. 4 is a diagram showing the relationship between the blending ratio of the sendust alloy powder and the loss in the example of the composite soft magnetic material according to the present invention. 図5は、本発明に係る複合軟磁性材料の実施例において、センダスト合金粉末の配合比と機械強度との関係を示す図である。FIG. 5 is a diagram showing the relationship between the blending ratio of Sendust alloy powder and mechanical strength in the example of the composite soft magnetic material according to the present invention.
 以下、本発明を適用した複合軟磁性材料とその製造方法について詳細に説明する。
 本発明を用いて複合軟磁性材料を製造するには、例えばプレス成型機などの圧密装置を用い、複合軟磁性材料の原料粉末として例えばMgO系絶縁被膜付き純鉄粉末と、センダスト合金粉末に、バインダーと必要に応じて潤滑剤を添加し混合した混合粉末を圧密装置の金型のキャビティに充填した後に、加圧成形することによって所定形状の圧粉体を得ることができる。その後、得られた圧粉体を所定の温度範囲で焼成することにより目的の形状の複合軟磁性材料を得ることができる。
Hereinafter, a composite soft magnetic material to which the present invention is applied and a manufacturing method thereof will be described in detail.
In order to produce a composite soft magnetic material using the present invention, for example, using a compacting device such as a press molding machine, as a raw material powder of the composite soft magnetic material, for example, pure iron powder with an MgO-based insulating coating, and Sendust alloy powder, A powder compact having a predetermined shape can be obtained by filling the mixed powder obtained by adding and mixing a binder and a lubricant as necessary into a mold cavity of a compacting device, followed by pressure molding. Thereafter, the obtained green compact is fired in a predetermined temperature range, whereby a composite soft magnetic material having a desired shape can be obtained.
 本発明において用いる絶縁処理済みの純鉄粉末とは、例えば、(Mg,Fe)Oを含むMg-Fe-O三元系酸化物堆積膜が純鉄粒子の表面に被覆形成されたMg含有酸化物被覆純鉄粉末、もしくはリン酸塩被覆純鉄粉末、またはシリカのゾルゲル溶液(シリケート)もしくはアルミナのゾルゲル溶液などの湿式溶液を添加し混合して純鉄粉末表面に被覆したのち乾燥して焼成した酸化ケイ素もしくは酸化アルミニウム被覆純鉄粉末などを用いることができるが、これらに限られるものではなく、絶縁被覆層で純鉄粉末を被覆した構造の絶縁処理済み純鉄粉末を広く適用することができる。 Insulated pure iron powder used in the present invention is, for example, an Mg-containing oxide in which a Mg—Fe—O ternary oxide deposition film containing (Mg, Fe) O is coated on the surface of pure iron particles. Wet powder-coated pure iron powder, phosphate-coated pure iron powder, or a wet solution such as silica sol-gel solution (silicate) or alumina sol-gel solution is mixed and coated on the surface of pure iron powder, then dried and fired However, the present invention is not limited to this, and it is possible to widely apply insulated pure iron powder having a structure in which pure iron powder is coated with an insulating coating layer. it can.
 前記Mg-Fe-O三元系酸化物堆積膜を被覆したMg含有酸化物被覆純鉄粉末は、例えば以下の(A)、(B)、(C)または(D)の製造方法にて得ることができる。
 (A)純鉄粉末に酸化雰囲気中で室温~500℃に保持する酸化処理を施した後、この粉末にMg粉末を添加し混合して得られた混合粉末を温度:150~1100℃、圧力:1×10-12~1×10-1MPaの不活性ガス雰囲気または真空雰囲気中で加熱し、さらに必要に応じて酸化雰囲気中、温度:50~400℃で加熱すると、純鉄粉末表面にMgを含む酸化絶縁被膜を有するMg含有酸化物被覆純鉄粒子が得られる。
 (B)純鉄粉末に前述の酸化処理を施した後、一酸化ケイ素粉末を添加し混合した後、または混合しながら、真空雰囲気中、温度:600~1200℃保持の条件で加熱し、さらにMg粉末を添加し混合した後または混合しながら真空雰囲気中、温度:400~800℃保持の条件で加熱すると、純鉄粉末の表面にMg-Si含有酸化膜が形成されたMg-Si含有酸化物被膜純鉄粉末が得られる。
The Mg-containing oxide-coated pure iron powder coated with the Mg—Fe—O ternary oxide deposited film is obtained, for example, by the following production method (A), (B), (C) or (D). be able to.
(A) Pure iron powder is subjected to an oxidation treatment in an oxidizing atmosphere at room temperature to 500 ° C., and then mixed powder obtained by adding and mixing Mg powder to this powder is temperature: 150 to 1100 ° C., pressure When heated in an inert gas atmosphere or vacuum atmosphere of 1 × 10 −12 to 1 × 10 −1 MPa and further heated in an oxidizing atmosphere at a temperature of 50 to 400 ° C. as necessary, the surface of pure iron powder Mg-containing oxide-coated pure iron particles having an oxide insulating film containing Mg are obtained.
(B) After subjecting the pure iron powder to the oxidation treatment described above, after adding and mixing the silicon monoxide powder, or while mixing, heating in a vacuum atmosphere at a temperature of 600 to 1200 ° C., After adding and mixing Mg powder, or heating while mixing in a vacuum atmosphere at a temperature of 400 to 800 ° C., an Mg—Si containing oxide film is formed on the surface of pure iron powder. A material-coated pure iron powder is obtained.
 (C)純鉄粉末に前述の酸化処理を施した後、一酸化ケイ素粉末およびMg粉末を同時に添加し混合した後、または混合しながら、真空雰囲気中、温度:400~1200℃保持の条件で加熱すると、純鉄粉末の表面にMg-Si含有酸化物膜が形成されたMg-Si含有酸化物被膜軟磁性粉末が得られる。
 (D)純鉄粉末に前述の酸化処理を施した後、Mg粉末を添加し混合した後、または混合しながら、真空雰囲気中、温度:400~800℃保持の条件で加熱すると純鉄粉末の表面にMg含有酸化膜が形成されたMg含有酸化物被覆純鉄粉末が得られる。
 この粉末にさらに一酸化ケイ素粉末を添加し混合した後、または混合しながら、真空雰囲気中、温度:600~1200℃保持の条件で加熱すると、純鉄粉末の表面にMg-Si含有酸化物膜が形成されたMg-Si含有酸化物被覆軟磁性粉末が得られる。
 前記一酸化ケイ素粉末の添加量は0.01~1質量%の範囲内にすることができ、前記Mg粉末の添加量を0.05~1質量%の範囲内にすることができる。前記真空雰囲気は圧力:1×10-12~1×10-1MPaの真空雰囲気とすることができる。
(C) After subjecting the pure iron powder to the above-described oxidation treatment, the silicon monoxide powder and the Mg powder are simultaneously added and mixed, or while mixing, in a vacuum atmosphere at a temperature of 400 to 1200 ° C. When heated, an Mg—Si-containing oxide-coated soft magnetic powder in which an Mg—Si-containing oxide film is formed on the surface of pure iron powder is obtained.
(D) After the above-described oxidation treatment is applied to pure iron powder, after adding and mixing Mg powder or while mixing, heating in a vacuum atmosphere at a temperature of 400 to 800 ° C., the pure iron powder An Mg-containing oxide-coated pure iron powder having a Mg-containing oxide film formed on the surface is obtained.
After further adding and mixing the silicon monoxide powder to this powder and heating it in a vacuum atmosphere at a temperature of 600 to 1200 ° C., the Mg—Si-containing oxide film is formed on the surface of the pure iron powder. Thus, an Mg—Si-containing oxide-coated soft magnetic powder with a formed thereon can be obtained.
The addition amount of the silicon monoxide powder can be in the range of 0.01 to 1% by mass, and the addition amount of the Mg powder can be in the range of 0.05 to 1% by mass. The vacuum atmosphere may be a vacuum atmosphere at a pressure of 1 × 10 −12 to 1 × 10 −1 MPa.
 これらの製造方法により得られたMg含有酸化物被覆純鉄粒子は、(Mg,Fe)Oを含むMg-Fe-O三元系酸化物堆積膜の被覆密着性が格段に優れたものとなり、この粒子をプレス成形して圧粉体を作製しても絶縁被膜が破壊され剥離することが少ない。
 前述の酸化物被覆純鉄粉末は平均粒径:20~50μmの範囲内にある粉末を使用することが好ましい。その理由は、平均粒径が小さすぎると、粉末の圧縮性が低下し、飽和磁束密度の値が低下するので好ましくなく、一方、平均粒径が大きすぎると、軟磁性粉末内部の渦電流が増大して高周波における透磁率が低下するおそれを生じやすいことによるものである。
The Mg-containing oxide-coated pure iron particles obtained by these production methods have remarkably excellent coating adhesion of the Mg—Fe—O ternary oxide deposited film containing (Mg, Fe) O, Even if these particles are pressed to produce a green compact, the insulating coating is less likely to be broken and peeled off.
The oxide-coated pure iron powder is preferably a powder having an average particle size in the range of 20 to 50 μm. The reason is that if the average particle size is too small, the compressibility of the powder decreases and the value of the saturation magnetic flux density decreases, which is not preferable. On the other hand, if the average particle size is too large, the eddy current inside the soft magnetic powder is not preferable. This is because the magnetic permeability at a high frequency is likely to increase and decrease.
 前記酸化物被覆純鉄粉末に加え、センダスト合金(例えば、組成比:10質量%Si-6質量%Al-残Fe)粉末を用意する。このセンダスト合金粉末として50~120μmの粒径範囲の粉末を用いることができる。
 これらの粉末を用意したならば、酸化物被覆純鉄粉末とセンダスト合金粉末にそれぞれバインダー材としてのシリコーンレジンなどのSiを含むバインダー材を個々に混合し、それぞれの粉末をシリコーン樹脂被覆粉末とする。
 酸化物被覆純鉄粉末にバインダー材を被覆するには、0.01~1質量%程度のバインダー材を添加して攪拌混合被覆した後、150~250℃の範囲、より好ましくは200~250℃の範囲に加熱して焼付け被覆することができる。センダスト合金粉末にバインダー材を被覆するには、0.05~3質量%程度のバインダー材を添加して攪拌混合被覆した後、80~250℃の範囲、より好ましくは100~200℃の範囲に加熱して焼付け被覆することができる。
In addition to the oxide-coated pure iron powder, a sendust alloy (for example, composition ratio: 10 mass% Si-6 mass% Al-residual Fe) powder is prepared. As this Sendust alloy powder, a powder having a particle size range of 50 to 120 μm can be used.
Once these powders are prepared, the oxide-coated pure iron powder and Sendust alloy powder are each mixed with a binder material containing Si, such as silicone resin as a binder material, and each powder is made into a silicone resin-coated powder. .
In order to coat the oxide-coated pure iron powder with the binder material, about 0.01 to 1% by mass of the binder material is added and stirred and coated, and then the temperature is in the range of 150 to 250 ° C, more preferably 200 to 250 ° C. Can be baked and coated in the range of. In order to coat the binder material on the Sendust alloy powder, after adding about 0.05 to 3% by mass of the binder material and stirring and coating, the temperature is in the range of 80 to 250 ° C., more preferably in the range of 100 to 200 ° C. It can be baked and coated by heating.
 酸化物被覆純鉄粉末にバインダー材を被覆して焼き付ける場合、焼付け温度として、150~250℃の範囲を選択できるが、この範囲を外れると150℃以下では成形時にバインダー材が剥離し、酸化物絶縁被覆を損傷することが原因と思われる比抵抗の低下が見られ、また、250℃を越えるとバインダー材が硬くなり、成形時の充填密度に低下が見られるので望ましくない。また、この範囲内であっても、より高い密度と比抵抗を得るために、200~250℃の範囲の焼付け温度がより好ましい。
 センダスト合金粉末にバインダー材を被覆して焼き付ける場合、焼付け温度として、80~250℃の範囲を選択できるが、この範囲を外れると80℃以下であると成形時に密度の低下やばらつきが見られること、250℃を超える温度では比抵抗の低下が見られるので望ましくない。また、この範囲内であっても、より高い密度と比抵抗を得るために、100~200℃の範囲の焼付け温度がより好ましい。
When the oxide-coated pure iron powder is baked with a binder material, the baking temperature can be selected from a range of 150 to 250 ° C. A decrease in specific resistance, which is considered to be caused by damage to the insulation coating, is observed, and if it exceeds 250 ° C., the binder material becomes hard and the packing density during molding is decreased, which is not desirable. Even within this range, a baking temperature in the range of 200 to 250 ° C. is more preferable in order to obtain higher density and specific resistance.
When baking is performed by coating a sendust alloy powder with a binder material, a temperature range of 80 to 250 ° C can be selected as the baking temperature. If the temperature is outside this range, a decrease in density or variation may be observed during molding. At temperatures exceeding 250 ° C., the specific resistance is decreased, which is not desirable. Even within this range, a baking temperature in the range of 100 to 200 ° C. is more preferable in order to obtain higher density and specific resistance.
 これらのバインダー材を被覆した酸化物被覆純鉄粉末とバインダー材を被覆したセンダスト合金粉末の質量の総和に占める、バインダー材を被覆したセンダスト合金粉末の質量の割合が5質量%以上、20質量%未満となるよう、これら粉末を混合し、圧密装置の金型に収容して金型温度80~150℃にて8~10Ton/cm程度の成形圧力で目的の形状に温間成形して圧密体とする。
 ここで用いる8~10Ton/cm程度の成形圧力は、センダスト合金粉末の圧密に使用する従来の20Ton/cm程度の成形圧力よりも格段に低く、一般的な粉末成形法に利用する圧密力と同等レベルなので、一般的な成形圧力であってもセンダスト合金粉末を利用して本発明に係る優れた複合軟磁性材料の製造に利用できる。
 その後、この圧密体を500℃~800℃の温度で1時間程度、真空雰囲気あるいは不活性ガス雰囲気(Ar、N2)中、または、非酸化雰囲気(H雰囲気)において焼成して目的の複合軟磁性材料を得ることができる。
 前述の圧密処理と焼成処理によって、絶縁処理を施した純鉄粉末は圧密されて鉄主相となり、センダスト合金粉末は圧密されてセンダスト合金主相となり、それらの鉄主相とセンダスト合金主相とが構成する主相に対してそれらの粒界に存在するようにバインダー材が焼成された結果として生成する粒界相が存在する組織を呈し、目的の複合軟磁性材料を得ることができる。
The ratio of the mass of the Sendust alloy powder coated with the binder material to the total mass of the oxide-coated pure iron powder coated with these binder materials and the Sendust alloy powder coated with the binder material is 5% by mass or more and 20% by mass. These powders are mixed so as to be less than the minimum, accommodated in a mold of a compacting apparatus, and warm-molded into a desired shape with a molding temperature of about 8 to 10 Ton / cm 2 at a mold temperature of 80 to 150 ° C. and consolidated. Let it be the body.
The molding pressure of about 8 to 10 Ton / cm 2 used here is much lower than the conventional molding pressure of about 20 Ton / cm 2 used for compacting Sendust alloy powder, and the compacting force used for general powder molding methods. Therefore, it is possible to use the Sendust alloy powder to produce an excellent composite soft magnetic material according to the present invention even at a general molding pressure.
Thereafter, the compact is fired at a temperature of 500 ° C. to 800 ° C. for about 1 hour in a vacuum atmosphere, an inert gas atmosphere (Ar, N 2 ), or in a non-oxidizing atmosphere (H 2 atmosphere) to obtain the desired composite. A soft magnetic material can be obtained.
By the above-described consolidation treatment and firing treatment, the pure iron powder subjected to insulation treatment is consolidated into an iron main phase, and Sendust alloy powder is consolidated into a Sendust alloy main phase. The target composite soft magnetic material can be obtained by exhibiting a structure in which a grain boundary phase formed as a result of firing the binder material so as to be present at those grain boundaries with respect to the main phase constituted by.
 以上説明の如く製造された複合軟磁性材料は、高周波域(10~20kHz)において低損失であり、鉄損、ヒステリシス損、保磁力が低く、渦電流損失が少なく、比抵抗が高いという優れた軟磁気特性を有する。これは、本発明の複合軟磁性材料が、純鉄粉末を絶縁性、密着性共に優れた前述の(Mg,Fe)Oを含むMg-Fe-O三元系酸化物堆積膜の被膜で覆い、好適な粒径範囲とした純鉄粉末に対し、好適な粒径範囲の適量のセンダスト合金粉末を混合し、圧密し、焼成して複合軟磁性材料としているので、圧密体として焼成した状態であっても、純鉄粉末が有する高い飽和磁束密度を維持しながら、センダスト合金が有する高透磁率、低保磁力、低鉄損失の特性を発揮できるからである。
 なお、純鉄粉末の絶縁処理は、前述の(Mg,Fe)Oを含むMg-Fe-O三元系酸化物堆積膜による被膜に限られるものではなく、リン酸塩被覆純鉄粉末など、他の絶縁処理を施した被膜によっても同様の複合軟磁性材料を得ることができる。
The composite soft magnetic material manufactured as described above has low loss in the high frequency range (10 to 20 kHz), excellent iron loss, hysteresis loss, coercive force, low eddy current loss, and high specific resistance. Has soft magnetic properties. This is because the composite soft magnetic material of the present invention covers pure iron powder with a film of the Mg—Fe—O ternary oxide deposited film containing (Mg, Fe) O having excellent insulation and adhesion. The pure iron powder with a suitable particle size range is mixed with a suitable amount of Sendust alloy powder with a suitable particle size range, consolidated, and fired to form a composite soft magnetic material. This is because the high permeability, low coercive force, and low iron loss characteristics of the sendust alloy can be exhibited while maintaining the high saturation magnetic flux density of the pure iron powder.
In addition, the insulation treatment of the pure iron powder is not limited to the above-described coating with the Mg—Fe—O ternary oxide deposited film containing (Mg, Fe) O, and the phosphate-coated pure iron powder, A similar composite soft magnetic material can be obtained also by a film subjected to another insulation treatment.
 前記の如く純鉄粉末とセンダスト合金粉末を混合して圧密焼成してなる複合軟磁性材料は、センダスト合金に比べて軟質の純鉄粉末を適切な配合比で混合し、圧密し、焼成してなるので、8~10Ton/cm程度の成形圧力で充分な磁気特性を発揮することができる。
 本発明の複合軟磁性材料は、センダスト合金粉末の添加割合を5質量%以上、20質量%未満の範囲としたことにより、センダスト合金粉末が本来有する高周波域(10~20kHz)において低損失であり、鉄損、ヒステリシス損、保磁力が低く、渦電流損失が少なく、比抵抗が高いという優れた軟磁気特性を得ることができる。センダスト合金粉末の添加割合が前述の範囲を下回るとこれらの特性を有効に発揮することができなくなる。また、センダスト合金粉末の添加割合が多すぎると純鉄粉末の量が少なくなるので、高い飽和磁束密度を得難くなるとともに、成形時に必要な圧力が高くなり、前述の範囲の成形圧力では良好な密度が得難くなる。
The composite soft magnetic material obtained by mixing pure iron powder and Sendust alloy powder and compacting as described above is mixed with soft pure iron powder in an appropriate blending ratio compared to Sendust alloy, compacted, and fired. Therefore, sufficient magnetic properties can be exhibited at a molding pressure of about 8 to 10 Ton / cm 2 .
The composite soft magnetic material of the present invention has a low loss in the high frequency range (10 to 20 kHz) inherent to the sendust alloy powder by setting the addition ratio of the sendust alloy powder in the range of 5% by mass or more and less than 20% by mass. Excellent soft magnetic properties such as low iron loss, hysteresis loss, coercive force, low eddy current loss, and high specific resistance can be obtained. If the send rate of the sendust alloy powder is less than the above range, these characteristics cannot be exhibited effectively. In addition, if the addition ratio of Sendust alloy powder is too large, the amount of pure iron powder decreases, so it becomes difficult to obtain a high saturation magnetic flux density and the pressure required during molding becomes high, and the molding pressure in the above range is good. It becomes difficult to obtain the density.
 本発明の複合軟磁性材料を用いて構成される電磁気回路部品として、例えば、磁心、電動機コア、発電機コア、ソレノイドコア、イグニッションコア、リアクトルコア、トランスコア、チョークコイルコアまたは磁気センサコアなどが挙げられ、これらは、いずれにおいても優れた特性を発揮し得る電磁気回路部品である。
 これら電磁気回路部品を組み込んだ電気機器には、電動機、発電機、ソレノイド、インジェクタ、電磁駆動弁、インバータ、コンバータ、変圧器、継電器、または磁気センサシステム等がある。本発明の複合軟磁性材料は、これら電気機器の高効率高性能化や小型軽量化に寄与するという効果を有する。
Examples of the electromagnetic circuit component configured using the composite soft magnetic material of the present invention include a magnetic core, a motor core, a generator core, a solenoid core, an ignition core, a reactor core, a transformer core, a choke coil core, and a magnetic sensor core. These are electromagnetic circuit components that can exhibit excellent characteristics in any case.
Examples of electric devices incorporating these electromagnetic circuit components include an electric motor, a generator, a solenoid, an injector, an electromagnetically driven valve, an inverter, a converter, a transformer, a relay, or a magnetic sensor system. The composite soft magnetic material of the present invention has the effect of contributing to high efficiency, high performance, small size and light weight of these electric devices.
 以下、実施例により本発明の効果をより明らかなものとする。なお、本発明は、以下の実施例に限定されるものではなく、その要旨を変更しない範囲で適宜変更して実施することができる。 Hereinafter, the effects of the present invention will be made clearer by examples. In addition, this invention is not limited to a following example, In the range which does not change the summary, it can change suitably and can implement.
 Mg酸化物被覆純鉄粉末として粒径D50(=20μm~50μm)の粉末と、センダスト合金(組成比:10質量%Si-6質量%Al-残Fe)粉末粒径としてD50(=50μm~120μm)の粉末を用意した。粒径の測定には、LEED&NORTHRUP社製のMICROTRAC FRAを使用した。
 Mg酸化物被覆純鉄粉末として、純鉄粉末に対して大気中220℃にて加熱処理を行って表面に酸化膜を形成し、この軟磁性粉末に対して0.3質量%のMg粉末を配合し、この配合粉末を造粒転動攪拌混合装置によって、真空中、650℃にて1時間転動することにより膜厚30nmの(Mg,Fe)Oで示されるMg含有酸化物被膜を形成した絶縁処理済み純鉄粉末を用いた。
 他の絶縁被覆純鉄粉末として、へガネスジャパン製リン酸鉄被覆鉄粉S110iを用意し、比較例試料として、上記と同等の粒径を有する、被覆を施していない純鉄粉末を用意した。
Powder with particle size D50 (= 20 μm to 50 μm) as pure Mg powder coated with Mg oxide and D50 (= 50 μm to 120 μm) as sendust alloy (composition ratio: 10 mass% Si-6 mass% Al-residual Fe) powder particle diameter ) Powder was prepared. For measurement of the particle size, MICROTRAC FRA manufactured by LEED & NORTHRUP was used.
As pure Mg powder coated with Mg oxide, the pure iron powder was heat-treated at 220 ° C. in the atmosphere to form an oxide film on the surface, and 0.3% by mass of Mg powder was added to the soft magnetic powder. Blending and rolling this blended powder with a granulation rolling agitation and mixing device in vacuum at 650 ° C. for 1 hour forms an Mg-containing oxide film of (Mg, Fe) O with a film thickness of 30 nm Insulated pure iron powder was used.
As other insulation-coated pure iron powder, iron phosphate-coated iron powder S110i manufactured by Heganes Japan was prepared, and as a comparative sample, pure iron powder having a particle size equivalent to the above was prepared. .
 これらの粉末にバインダー材としてのシリコーン樹脂を0.5質量%添加混合し、250℃にて焼き付け、また、センダスト合金粉末にはシリコーン樹脂を1質量%添加混合し、150℃に加熱して焼き付けを行った。引き続いてこれらの各粉末のうち、Mg酸化物被覆純鉄粉末とセンダスト合金粉末を、センダスト合金粉末の割合において、0質量%、5質量%、7質量%、10質量%、20質量%、および50質量%の割合で各々混合し分けた試料を準備し、これらの各試料を成形温度150℃、8Ton/cmの成形圧力で外形35mm、内径25mm、高さ5mmのリング形状に圧密し、各試料を作成した。 Add 0.5% by mass of a silicone resin as a binder material to these powders and bake at 250 ° C., and add 1% by mass of silicone resin to Sendust alloy powder and heat to 150 ° C. for baking. Went. Subsequently, among these powders, Mg oxide-coated pure iron powder and Sendust alloy powder in the proportion of Sendust alloy powder are 0 mass%, 5 mass%, 7 mass%, 10 mass%, 20 mass%, and Samples mixed and divided at a ratio of 50% by mass were prepared, and each of these samples was consolidated into a ring shape having an outer shape of 35 mm, an inner diameter of 25 mm, and a height of 5 mm at a molding temperature of 150 ° C. and a molding pressure of 8 Ton / cm 2 , Each sample was made.
 得られた試料について、センダスト合金粉末の配合比(酸化物被覆純鉄粉末とセンダスト合金粉末の質量の総和に占めるセンダスト合金粉末の配合比、質量%)を表1に表示するとともに、各試料の水中密度(g/cm)、比抵抗(μΩm)、μmax、磁場10kA/m時の飽和磁束密度(B10kA/m:T)、保磁力(Hc:A/m)、鉄損(全損、ヒステリシス損、渦電流損失)、機械強度(圧環強度:N/mm)を測定した結果を表1に併せて示す。 For the obtained samples, the blending ratio of Sendust alloy powder (the blending ratio of Sendust alloy powder in the total mass of oxide-coated pure iron powder and Sendust alloy powder, mass%) is displayed in Table 1, and water density (g / cm 3), the specific resistance (μΩm), μmax, the saturation magnetic flux density when a magnetic field 10kA / m (B 10k a / m: T), the coercive force (Hc: a / m), iron loss (total Table 1 also shows the results of measuring the loss, hysteresis loss, eddy current loss) and mechanical strength (compression crushing strength: N / mm 2 ).
Figure JPOXMLDOC01-appb-T000001
Figure JPOXMLDOC01-appb-T000001
 図1は表1に示すセンダスト合金粉末の配合比と比抵抗の関係をプロットした図である。図1に示す結果によれば、センダスト合金粉末の配合比において、0質量%では著しく比抵抗の値が低いが、センダスト合金粉末を5質量%添加した試料で比抵抗の値が急激に高くなる。また、配合比が20質量%以上になると比抵抗の低下割合が大きくなる。従って、センダスト合金粉末の配合比は5質量%以上、20質量%未満が好ましい。 FIG. 1 is a graph plotting the relationship between the blending ratio and specific resistance of Sendust alloy powder shown in Table 1. According to the results shown in FIG. 1, the specific resistance value is remarkably low at 0% by mass in the blending ratio of Sendust alloy powder, but the specific resistance value increases rapidly in the sample to which 5% by mass of Sendust alloy powder is added. . Further, when the blending ratio is 20% by mass or more, the reduction ratio of specific resistance increases. Therefore, the blending ratio of Sendust alloy powder is preferably 5% by mass or more and less than 20% by mass.
 図2は表1に示すセンダスト合金粉末の配合比と飽和磁束密度の関係をプロットした図である。図2に示す結果によれば、飽和磁束密度については配合比20質量%以上になると急激に低下する。従って、酸化物被覆純鉄粉末に対するセンダスト合金粉末の配合比は、磁場10kA/m時の飽和磁束密度1T以上とするためには、5質量%以上、20質量%未満が好ましく、磁場10kA/m時の飽和磁束密度1.1Tを得るためには5質量%以上、10質量%以下がより好ましい。 FIG. 2 is a graph plotting the relationship between the blending ratio of Sendust alloy powder shown in Table 1 and the saturation magnetic flux density. According to the results shown in FIG. 2, the saturation magnetic flux density rapidly decreases when the blending ratio is 20% by mass or more. Therefore, the blending ratio of Sendust alloy powder to oxide-coated pure iron powder is preferably 5% by mass or more and less than 20% by mass in order to obtain a saturation magnetic flux density of 1T or more at a magnetic field of 10 kA / m, and a magnetic field of 10 kA / m. In order to obtain a saturation magnetic flux density of 1.1 T, 5 mass% or more and 10 mass% or less are more preferable.
 図3は表1に示す磁場10kA/m時の磁束密度と鉄損(磁束密度0.1T、周波数10kHz時)の関係をプロットした図である。図3に示す結果によれば、センダスト合金粉末の配合により磁束密度を低下させることなく、鉄損を低減することができる。
 図4は表1に示すセンダスト合金粉末の配合比と損失との関係をプロットした図である。図4に示す結果によれば、配合比20質量%未満が損失については好ましい。また、センダスト合金粉末の配合比において5質量%以上、20質量%未満において、鉄損(磁束密度0.1T、周波数10kHz時)20W/kg以下を実現できる。
FIG. 3 is a graph plotting the relationship between the magnetic flux density and the iron loss at the magnetic field of 10 kA / m shown in Table 1 (when the magnetic flux density is 0.1 T and the frequency is 10 kHz). According to the results shown in FIG. 3, the iron loss can be reduced without reducing the magnetic flux density by blending the sendust alloy powder.
FIG. 4 is a graph plotting the relationship between the blending ratio of the Sendust alloy powder shown in Table 1 and the loss. According to the result shown in FIG. 4, a blending ratio of less than 20% by mass is preferable for the loss. Moreover, when the blending ratio of Sendust alloy powder is 5 mass% or more and less than 20 mass%, an iron loss (at a magnetic flux density of 0.1 T and a frequency of 10 kHz) of 20 W / kg or less can be realized.
 図5は表1に示すセンダスト合金粉末の配合比と機械強度との関係をプロットした図である。図5に示す結果によれば、圧環強度については配合比5~10質量%の間に機械強度のピークを有することが明らかであるが、センダスト合金粉末の配合比について実用域で問題のない強度であることが判る。 FIG. 5 is a graph plotting the relationship between the blending ratio of Sendust alloy powder shown in Table 1 and the mechanical strength. According to the results shown in FIG. 5, it is clear that the crushing strength has a mechanical strength peak between 5 and 10% by mass, but there is no problem in the practical range for the blending ratio of Sendust alloy powder. It turns out that it is.
 次に、純鉄粉末にシリコーン樹脂を0.5質量%混合して250℃で焼き付けたシリコーン樹脂被覆純鉄粉末に対し、シリコーン樹脂を1質量%混合して200℃で焼き付けたシリコーン樹脂被覆センダスト合金粉末を、シリコーン樹脂被覆純鉄粉末とシリコーン樹脂被覆センダスト合金粉末の質量の総和に占める、シリコーン樹脂被覆センダスト合金粉末の配合比が7質量%となるように配合した。これらを混合して成形温度150℃、8Ton/cmの成形圧力で圧密し、その後、500℃あるいは650℃にて焼成して各試料を作成した。各試料の比抵抗の測定値を以下の表2に示す。 Next, a silicone resin-coated sendust in which 0.5% by mass of a silicone resin is mixed with pure iron powder and then baked at 250 ° C. is mixed with 1% by mass of silicone resin and baked at 200 ° C. The alloy powder was blended so that the blending ratio of the silicone resin-coated Sendust alloy powder in the total mass of the silicone resin-coated pure iron powder and the silicone resin-coated Sendust alloy powder was 7% by mass. These were mixed and compacted at a molding temperature of 150 ° C. and a molding pressure of 8 Ton / cm 2 , and then fired at 500 ° C. or 650 ° C. to prepare each sample. The measured values of the specific resistance of each sample are shown in Table 2 below.
Figure JPOXMLDOC01-appb-T000002
Figure JPOXMLDOC01-appb-T000002
 表2に示す結果によれば、良好な鉄損(数値が小)とし、ヒステリシス損を下げるためには、焼成温度は高い方が好ましく、焼成温度500℃にて良好な比抵抗が得られるが、より良好な鉄損を得るには、650℃の焼成温度が好ましい。 According to the results shown in Table 2, in order to achieve good iron loss (small numerical value) and lower hysteresis loss, a higher firing temperature is preferable, and a good specific resistance can be obtained at a firing temperature of 500 ° C. In order to obtain better iron loss, a firing temperature of 650 ° C. is preferable.
 次に、センダスト合金粉末にシリコーン樹脂を1質量%混合して150℃で焼き付けたシリコーン樹脂被覆センダスト合金粉末に対し、シリコーン樹脂を0.5質量%混合して、150℃、200℃、250℃、および270℃で、それぞれ焼き付けたシリコーン樹脂被覆絶縁鉄粉を、そのシリコーン樹脂被覆センダスト合金粉末とシリコーン樹脂被覆絶縁鉄粉の質量の総和に占める、シリコーン樹脂被覆センダスト合金粉末の配合比が7質量%になるように配合した。これらをそれぞれ成形温度150℃、8Ton/cmの成形圧力で圧密し、その後、650℃にて焼成して各試料を作成した。各試料の密度、比抵抗および鉄損の測定値を以下の表3に示す。 Next, with respect to the silicone resin-coated Sendust alloy powder obtained by mixing 1% by mass of silicone resin with Sendust alloy powder and baking at 150 ° C., 0.5% by mass of silicone resin is mixed to 150 ° C., 200 ° C., 250 ° C. , And 270 ° C., the blending ratio of the silicone resin-coated Sendust alloy powder occupying the total mass of the silicone resin-coated Sendust alloy powder and the silicone resin-coated Sendiron alloy powder is 7%. %. These were consolidated at a molding temperature of 150 ° C. and a molding pressure of 8 Ton / cm 2 , and then fired at 650 ° C. to prepare each sample. The measured values of density, specific resistance and iron loss of each sample are shown in Table 3 below.
Figure JPOXMLDOC01-appb-T000003
Figure JPOXMLDOC01-appb-T000003
 表3に示す試験結果によれば、純鉄粉末に対するシリコーン樹脂の焼付け温度は150~250℃の範囲を選択できるが、より好ましくは、200~250℃の範囲である。 According to the test results shown in Table 3, the baking temperature of the silicone resin with respect to the pure iron powder can be selected in the range of 150 to 250 ° C, more preferably in the range of 200 to 250 ° C.
 純鉄粉末にシリコーン樹脂を0.5質量%混合して250℃で焼き付けたシリコーン樹脂被覆純鉄粉末と、シリコーン樹脂を1質量%混合して、50℃、80℃、100℃、150℃、200℃、250℃、および270℃で、それぞれ焼き付けたシリコーン樹脂被覆センダスト合金粉末を、そのシリコーン樹脂被覆純鉄粉末とシリコーン樹脂被覆センダスト合金粉末の質量の総和に占める、シリコーン樹脂被覆センダスト合金粉末の配合比が7質量%になるように配合した。これらをそれぞれ成形温度150℃、8Ton/cmの成形圧力で圧密し、その後、650℃にて焼成して各試料を作成した。各試料の密度、比抵抗および鉄損の測定値を以下の表4に示す。 Silicone resin-coated pure iron powder obtained by mixing 0.5% by mass of a silicone resin with pure iron powder and baking at 250 ° C. and 1% by mass of silicone resin were mixed at 50 ° C., 80 ° C., 100 ° C., 150 ° C., The silicone resin-coated Sendust alloy powder occupies the total mass of the silicone resin-coated pure iron powder and the silicone resin-coated Sendust alloy powder. It mix | blended so that a compounding ratio might be 7 mass%. These were consolidated at a molding temperature of 150 ° C. and a molding pressure of 8 Ton / cm 2 , and then fired at 650 ° C. to prepare each sample. The measured values of density, specific resistance, and iron loss of each sample are shown in Table 4 below.
Figure JPOXMLDOC01-appb-T000004
Figure JPOXMLDOC01-appb-T000004
 表4に示す試験結果によれば、センダスト合金粉末におけるシリコーン樹脂の焼付け温度は80~250℃の範囲を選択できるが、より好ましくは、100~200℃の範囲である。 According to the test results shown in Table 4, the baking temperature of the silicone resin in the Sendust alloy powder can be selected in the range of 80 to 250 ° C, more preferably in the range of 100 to 200 ° C.
 以上説明の試験結果から、本発明を実施することで、純鉄粉末にセンダスト合金粉末を添加し、8Ton/cmの成形圧力で圧密することによって、磁場10kA/m時の飽和磁束密度1T以上、保磁力260A/m以下、鉄損(0.1T、10kHz時)20W/kg以下である優れた軟磁気特性の複合軟磁性材料を製造できることが明らかになった。 From the test results described above, by implementing the present invention, by adding Sendust alloy powder to pure iron powder and compacting with a molding pressure of 8 Ton / cm 2 , saturation magnetic flux density of 1 T or more at a magnetic field of 10 kA / m or more. It was revealed that a composite soft magnetic material having excellent soft magnetic properties having a coercive force of 260 A / m or less and an iron loss (at 0.1 T, 10 kHz) of 20 W / kg or less can be produced.
 本発明によれば、絶縁処理した鉄粉末が有する高い飽和磁束密度を維持しながら、適量混合したセンダスト合金粉末が有する低鉄損と低い保磁力と少ない渦電流損失のような軟磁気特性を有効に得た複合軟磁性材料を提供することができる。 According to the present invention, while maintaining the high saturation magnetic flux density of the insulated iron powder, the soft magnetic characteristics such as low iron loss, low coercive force, and low eddy current loss of the proper amount of sendust alloy powder are effective. The composite soft magnetic material obtained in the above can be provided.

Claims (6)

  1.  絶縁処理された鉄粉末とセンダスト合金粉末とバインダーが混合圧密され、焼成されてなり、前記鉄粉末とセンダスト合金粉末が圧密され焼成された主相と、前記主相の周囲に生成されたバインダーを主体とする粒界相とが具備されてなり、前記主相に占めるセンダスト合金の割合が5質量%以上、20質量%未満であり、磁場10kA/m時の飽和磁束密度1T以上、保磁力260A/m以下、鉄損(0.1T、10kHz時)20W/kg以下であることを特徴とする複合軟磁性材料。 Insulated iron powder, Sendust alloy powder, and binder are mixed, consolidated, and fired. A grain boundary phase as a main component, the proportion of Sendust alloy in the main phase is 5 mass% or more and less than 20 mass%, a saturation magnetic flux density of 1 T or more at a magnetic field of 10 kA / m, and a coercive force of 260 A. / M or less, iron loss (at 0.1 T, 10 kHz) 20 W / kg or less, composite soft magnetic material,
  2.  絶縁処理された鉄粉末とセンダスト合金粉末が圧密され焼成された主相において、鉄主相の平均粒径が20~50μm、センダスト合金主相の平均粒径が50~120μmであることを特徴とする請求項1に記載の複合軟磁性材料。 In the main phase in which the insulated iron powder and Sendust alloy powder are consolidated and fired, the average particle size of the iron main phase is 20 to 50 μm, and the average particle size of the Sendust alloy main phase is 50 to 120 μm. The composite soft magnetic material according to claim 1.
  3.  絶縁処理された鉄粉末が、Mg含有酸化物被膜を具備してなる純鉄粉末であることを特徴とする請求項1または2に記載の複合軟磁性材料。 3. The composite soft magnetic material according to claim 1, wherein the insulated iron powder is a pure iron powder comprising an Mg-containing oxide film.
  4.  絶縁処理された鉄粉末とセンダスト合金粉末とバインダーを少なくとも混合圧密し、焼成することにより、前記鉄粉末とセンダスト合金粉末を圧密し焼成してなる主相と、前記主相の周囲に生成されたバインダーを主体とする粒界相とを具備した複合軟磁性材料を製造するにあたり、
     絶縁処理された鉄粉末とセンダスト合金粉末の質量の総和に占めるセンダスト合金粉末の添加割合を5質量%以上、20質量%未満として、絶縁処理された鉄粉末およびセンダスト合金粉末を混合圧密し、焼成することにより、磁場10kA/m時の飽和磁束密度1T以上、保磁力260A/m以下、鉄損(0.1T、10kHz時)20W/kg以下の複合軟磁性材料を得ることを特徴とする複合軟磁性材料の製造方法。
    Insulated iron powder, Sendust alloy powder and binder are mixed and compacted at least, and then fired to produce a main phase formed by compacting and firing the iron powder and Sendust alloy powder, and around the main phase. In producing a composite soft magnetic material having a grain boundary phase mainly composed of a binder,
    The ratio of addition of Sendust alloy powder to the total mass of insulated iron powder and Sendust alloy powder is 5% by mass or more and less than 20% by mass, and the insulated iron powder and Sendust alloy powder are mixed and consolidated and fired. Thus, a composite soft magnetic material having a saturation magnetic flux density of 1 T or more at a magnetic field of 10 kA / m, a coercive force of 260 A / m or less, and an iron loss (at 0.1 T, 10 kHz) of 20 W / kg or less is obtained. A method for producing a soft magnetic material.
  5.  平均粒径20~50μmの絶縁処理された鉄粉末を用い、平均粒径50~120μmのセンダスト合金粉末を用いることを特徴とする請求項4に記載の複合軟磁性材料の製造方法。 5. The method for producing a composite soft magnetic material according to claim 4, wherein an insulated iron powder having an average particle size of 20 to 50 μm is used and a sendust alloy powder having an average particle size of 50 to 120 μm is used.
  6.  絶縁処理された鉄粉末として、Mg含有酸化物被膜により絶縁処理された純鉄粉末を用いることを特徴とする請求項4または5に記載の複合軟磁性材料の製造方法。 6. The method for producing a composite soft magnetic material according to claim 4, wherein pure iron powder insulated with an Mg-containing oxide coating is used as the insulated iron powder.
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