WO2019112002A1 - 複合磁性粉末、磁性樹脂組成物、磁性樹脂ペースト、磁性樹脂粉末、磁性樹脂スラリー、磁性樹脂シート、金属箔付磁性樹脂シート、磁性プリプレグ及びインダクタ部品 - Google Patents

複合磁性粉末、磁性樹脂組成物、磁性樹脂ペースト、磁性樹脂粉末、磁性樹脂スラリー、磁性樹脂シート、金属箔付磁性樹脂シート、磁性プリプレグ及びインダクタ部品 Download PDF

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WO2019112002A1
WO2019112002A1 PCT/JP2018/044903 JP2018044903W WO2019112002A1 WO 2019112002 A1 WO2019112002 A1 WO 2019112002A1 JP 2018044903 W JP2018044903 W JP 2018044903W WO 2019112002 A1 WO2019112002 A1 WO 2019112002A1
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Prior art keywords
magnetic
powder
magnetic resin
resin composition
resin
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PCT/JP2018/044903
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English (en)
French (fr)
Japanese (ja)
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大三 馬場
佐々木　大輔
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パナソニックＩｐマネジメント株式会社
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Priority to CN201880078778.0A priority Critical patent/CN111466001B/zh
Priority to JP2019558274A priority patent/JP7194909B2/ja
Publication of WO2019112002A1 publication Critical patent/WO2019112002A1/ja

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/12—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 soft-magnetic materials
    • H01F1/14—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 soft-magnetic materials metals or alloys
    • H01F1/20—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 soft-magnetic materials metals or alloys in the form of particles, e.g. powder
    • H01F1/28—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 soft-magnetic materials metals or alloys in the form of particles, e.g. powder dispersed or suspended in a bonding agent

Definitions

  • the present invention relates to composite magnetic powder, magnetic resin composition, magnetic resin paste, magnetic resin powder, magnetic resin slurry, magnetic resin sheet, magnetic resin sheet with metal foil, magnetic prepreg, and inductor component.
  • Patent Document 1 discloses an inductor component including a coiled wiring and a cured product of a resin sheet (hereinafter, magnetic material) that covers the coiled wiring.
  • This resin sheet contains an epoxy resin, a phenoxy resin, a linear elastomer, a curing agent, and an inorganic filler.
  • the content of the inorganic filler is 80 to 98% by mass with respect to the total amount of the resin sheet.
  • the content of the linear elastomer is 0.01 to 0.5 parts by mass with respect to a total of 100 parts by mass of the constituent components of the resin sheet excluding the linear elastomer.
  • the conventional magnetic material as described in Patent Document 1 has a Q value (quality factor, hereinafter referred to as Q value of the magnetic material) indicating a small loss of the magnetic material in a high frequency band (for example, 100 MHz) Low, high loss in high frequency band.
  • Q value of the magnetic material quality factor, hereinafter referred to as Q value of the magnetic material
  • the object of the present invention is to provide a composite magnetic powder, magnetic resin composition, magnetic resin paste, magnetic resin powder, magnetic resin slurry, magnetic resin sheet, magnetic foil with metal foil, which can increase Q value of magnetic material in high frequency band. It is providing a resin sheet, a magnetic prepreg, and an inductor component.
  • the composite magnetic powder according to one aspect of the present invention contains a magnetic powder containing a first powder and a nonmagnetic powder containing a second powder, and the first powder comprises an alloyed iron powder,
  • the second powder comprises at least one of alumina powder and silica powder, and the average particle diameter of the first powder is less than 5 ⁇ m, and at least 3 times and 30 times the average particle diameter of the second powder. It is below.
  • the magnetic resin composition according to one aspect of the present invention contains the composite magnetic powder, and at least one resin selected from the group consisting of a curable resin and a thermoplastic resin.
  • the magnetic resin composition is paste-like.
  • the magnetic resin composition is powdery.
  • the magnetic resin composition further contains a solvent and is in the form of a slurry.
  • the magnetic resin composition is in the form of a sheet.
  • the magnetic resin sheet with metal foil includes the magnetic resin sheet and a metal foil having a thickness of 5 ⁇ m or less laminated on at least one surface of the magnetic resin sheet.
  • the magnetic prepreg according to one aspect of the present invention includes a fibrous base material, and the magnetic resin composition or a semi-cured product of the magnetic resin composition.
  • the inductor component according to one aspect of the present invention includes a coiled wire and an insulating layer covering the coiled wire, and the insulating layer is formed of a cured product or a solidified product of the magnetic resin composition.
  • FIG. 1A is a schematic cross-sectional view for explaining the positional relationship between magnetic particles constituting a first powder and nonmagnetic particles constituting a second powder in the composite magnetic powder of the present invention.
  • FIG. 1B is a schematic cross-sectional view showing a seemingly large lump of large particles in which a plurality of large diameter magnetic particles are formed close to each other.
  • FIG. 1C is a schematic cross-sectional view for explaining the positional relationship between the magnetic particles and the nonmagnetic particles when the average particle diameter of the first powder is less than three times the average particle diameter of the second powder. .
  • FIG. 1A is a schematic cross-sectional view for explaining the positional relationship between magnetic particles constituting a first powder and nonmagnetic particles constituting a second powder in the composite magnetic powder of the present invention.
  • FIG. 1B is a schematic cross-sectional view showing a seemingly large lump of large particles in which a plurality of large diameter magnetic particles are formed close to each other.
  • FIG. 1C is a schematic cross
  • FIG. 1D is a schematic cross-sectional view for explaining the positional relationship between the magnetic particles and the nonmagnetic particles when the average particle diameter of the first powder is more than 30 times the average particle diameter of the second powder.
  • FIG. 2A is a schematic cross-sectional view for describing a part of the method for manufacturing a magnetic resin sheet according to the embodiment of the present invention.
  • FIG. 2B is a schematic cross-sectional view for describing a part of the method of manufacturing a magnetic resin sheet according to the embodiment of the present invention.
  • FIG. 2C is a schematic cross-sectional view for describing a part of the method for manufacturing a magnetic resin sheet according to the embodiment of the present invention.
  • FIG. 3 is a schematic view for explaining the method of measuring the glycin value.
  • FIG. 4 is a schematic cross-sectional view of a magnetic resin sheet with a metal foil according to an embodiment of the present invention.
  • FIG. 5 is a schematic cross-sectional view of a magnetic prepreg according to
  • the present embodiment relates to a composite magnetic powder, and in particular to a composite magnetic powder suitably used as a magnetic material.
  • the composite magnetic powder (hereinafter, composite magnetic powder) according to the present embodiment contains a magnetic powder and a nonmagnetic powder.
  • the magnetic powder comprises a first powder.
  • the first powder comprises an alloyed iron powder.
  • the nonmagnetic powder comprises a second powder.
  • the second powder comprises at least one of alumina powder and silica powder.
  • the average particle size of the first powder is less than 5 ⁇ m and at least 3 times and not more than 30 times the average particle size of the second powder.
  • Magnetic powder is an aggregate of magnetic particles.
  • Nonmagnetic powder is an aggregate of nonmagnetic particles.
  • magnetic particles constituting the first powder are referred to as large-diameter magnetic particles 10
  • nonmagnetic particles constituting the second powder among the nonmagnetic particles are referred to as small-diameter nonmagnetic particles 20.
  • the magnetic particles are particles composed of a substance (magnetic material) that can be made magnetic by an external magnetic field, and representative substances include iron oxide, chromium oxide, cobalt, ferrite and the like.
  • the nonmagnetic particles are particles of a substance which is not contained in the magnetic substance (it is not magnetic even when an external magnetic field is applied).
  • average particle diameter means, in principle, the particle diameter at an integrated value of 50% in a particle size distribution measured based on a particle size distribution measuring device based on a laser scattering / diffraction method, ie 50% volume average particle diameter ( It means D 50 ).
  • an average particle diameter means the average value of the particle diameter measured by scanning electron microscope (SEM) observation.
  • the composite magnetic powder is suitably used as a raw material of a magnetic material of an inductor component (hereinafter, high frequency inductor component) for controlling noise in a high frequency band.
  • the performance of high frequency inductor components can be evaluated by the Q value of the magnetic material.
  • the Q value of the magnetic material As the Q value of the magnetic material is higher, the loss of the magnetic material is smaller and the resistance component R of the inductor is smaller, so the Q value of the inductor is higher and the performance of the high frequency inductor component is higher.
  • the Q value of the magnetic material at 100 MHz needs to be 20 or more, and preferably 33 or more from the viewpoint of enhancing the performance of the high frequency inductor component.
  • the high frequency band means several tens of MHz or more and several GHz or less.
  • the magnetic material refers to a cured product of a first magnetic resin composition described later or a solidified product of a second magnetic resin composition described later.
  • the Q value of the magnetic material can be determined in the same manner as the method (RF impedance analyzer) described in the examples.
  • the real part ( ⁇ ') at 100 MHz is preferably 6.0 or more in designing a high frequency inductor component.
  • the average particle size of the first powder is at least 3 times and not more than 30 times the average particle size of the second powder.
  • the imaginary part ( ⁇ ′ ′) is low at 100 MHz, and the Q value of the magnetic material can be made 20 or more. This is because adjacent large-diameter magnetic particles 10, 10 are less likely to aggregate, adjacent to each other It is assumed that the main reason is that the electrical insulation of the large-diameter magnetic particles 10 is secured to each other Specifically, in the magnetic material before treatment, as shown in FIG.
  • a plurality of small-diameter nonmagnetic particles 20 are uniformly disposed around one particle and one particle of the magnetic particle 10, and a layer 21 composed of the small-diameter nonmagnetic particles 20 is easily formed on the surface of the large-diameter magnetic particle 10.
  • Each large diameter magnetic particle 10 tends to behave as an independent particle, and the spacing I between adjacent large diameter magnetic particles 10 can be optimized. In other words, as shown in FIG. of The magnetic particles 10, 10 do not seem to behave as a single large particle 11.
  • the second powder is made of at least one of alumina powder and silica powder, so the layer 21 has insulation properties.
  • the inter-particle eddy current flowing across adjacent large-diameter magnetic particles 10 is less likely to occur, and eddy current loss can be further reduced, and it is presumed that the imaginary part ( ⁇ ′ ′) at 100 MHz will be low.
  • Ru The magnetic material before treatment is the state before the magnetic material is cured or solidified, and the first magnetic resin composition before curing, the magnetic resin paste described later, the magnetic resin powder described later, the resin magnetic slurry described later And a magnetic resin sheet described later, a second magnetic resin composition before solidification, and the like.
  • the composite magnetic powder may further contain a powder different from the first powder and the second powder, as long as it is a mixed powder containing the first powder and the second powder. That is, in the particle size distribution measured in terms of volume of the composite magnetic powder, at least two peaks representing the frequency of presence may be present, and three or more peaks may be present.
  • the shapes of the magnetic particles and nonmagnetic particles constituting the composite magnetic powder are not particularly limited, and examples thereof include spheres, ellipsoids, flats, and fractures.
  • the shapes of the magnetic particles and the nonmagnetic particles may be all the same or different. Among them, the shapes of the magnetic particles and the nonmagnetic particles are preferably all spherical. If the shapes of the magnetic particles and the nonmagnetic particles are all spherical, the filling amount of the composite magnetic powder to the magnetic material can be increased.
  • the magnetic material before treatment in which the shape of each magnetic particle and nonmagnetic particle is all spherical and the magnetic material before treatment in which the shape of each magnetic particle and nonmagnetic particle is not all spherical.
  • the former is more excellent in the fluidity of the magnetic material before the treatment.
  • the Q value of the magnetic material at 100 MHz can be further enhanced.
  • Spheres include those having an average sphericity of 0.7 or more.
  • the sphericity of a certain number (preferably 200 or more) of particles is determined, and this average value is taken as the average sphericity.
  • the composite magnetic powder contains magnetic powder.
  • the magnetic powder comprises a first powder and may further comprise other magnetic powders.
  • the magnetic powder is preferably insulated. That is, the surface of each magnetic particle is preferably covered with an electrically insulating film. This makes it possible to lower the imaginary part ( ⁇ ′ ′) at 100 MHz and further increase the Q value of the magnetic material. Further, it is possible to improve the electrical insulation reliability of the magnetic material itself.
  • the imaginary number at 100 MHz The reason why the portion ( ⁇ ′ ′) can be made lower is estimated to be mainly because the insulating coating hardly generates interparticle eddy current flowing between adjacent magnetic particles, and eddy current loss can be further reduced. Be done.
  • a method of the insulation process for example, a method of mixing and drying a magnetic powder and an aqueous solution containing an electrically insulating filler may be mentioned.
  • an electrically insulating filler for example, phosphoric acid, boric acid, magnesium oxide and the like can be used.
  • This electrically insulating film is different from the layer 21 made of the small-diameter nonmagnetic particles 20. When the magnetic particles themselves have electrical insulation, they may not be covered with the electrically insulating film.
  • the mixing ratio of the magnetic powder is preferably 4.0 parts by mass or more and 19.0 parts by mass or less, more preferably 4.0 parts by mass or more and 5.7 parts by mass or less with respect to 1 part by mass of the nonmagnetic powder. More preferably, it is 4.3 parts by mass or more and 5.2 parts by mass or less. If the mixing ratio of the magnetic powder is within the above range, the Q value of the magnetic material at 100 MHz and the flowability of the magnetic material before the treatment can be balanced. This is presumed to be because, as shown in FIG. 1A, the thickness of the layer 21 composed of the nonmagnetic particles 20 disposed around the large diameter magnetic particles 10 can be made thinner, and the spacing I can be made more appropriate.
  • the first powder comprises an alloyed iron powder.
  • the alloyed iron powder is an aggregate of alloyed iron particles.
  • the material of the alloy iron particles is an alloy mainly composed of iron. Examples of the material of the alloy iron particles include Sendust, permendur, silicon steel, permalloy, Fe-Si-Cr alloy and the like. These are high permeability alloy irons.
  • Sendust is an alloy of iron, silicon and aluminum (Fe-Si-Al alloy). Sendust has high saturation magnetic flux density, high permeability, small core loss, and excellent wear resistance.
  • An example of the composition of Sendust is Fe-9.5Si-5.5Al (numerical values are mass%, balance Fe). In the vicinity of this composition region, both of the magnetostriction constant and the magnetic anisotropy constant become approximately zero. Therefore, high permeability and low coercivity can be obtained.
  • Permendur is an alloy based on iron and cobalt. Permendur has the largest saturation flux density among the soft magnetic materials put into practical use.
  • An example of the composition of permendur is Fe-49Co-2V (values are mass%, balance Fe).
  • Silicon steel is an alloy of iron and a small amount of silicon. Silicon steel is also called silicon iron because it does not contain carbon.
  • Permalloy is an alloy of Ni-Fe. Permalloy includes permalloy A, permalloy B, permalloy C, and permalloy D, which are referred to as JIS standards.
  • the average particle size of the first powder is 3 to 30 times the average particle size of the second powder, preferably 3.5 to 20 times, more preferably 4 to 15 times. . If the average particle size of the first powder is less than 3 times the average particle size of the second powder, the imaginary part ( ⁇ ′ ′) may be high at 100 MHz and the Q value of the magnetic material may be less than 20. There is. The reason why the imaginary part ( ⁇ ′ ′) at 100 MHz is high is presumed to be that the layer 21 composed of the small nonmagnetic particles 20 is not easily formed on the surface of the large diameter magnetic particles 10 as shown in FIG. 1C. .
  • the real part ( ⁇ ') may be low at 100 MHz and the Q value of the magnetic material may be less than 20. is there.
  • the fact that the real part ( ⁇ ′) at 100 MHz is lowered is that the layer 21 composed of the small-diameter nonmagnetic particles 20 is easily formed on the surface of the large-diameter magnetic particles 10. It is presumed that the distance I between the particles 10 is too wide.
  • the first powder is a mixed powder obtained by mixing two or more powders having different average particle sizes
  • the average particle size of the first powder indicates the average particle size of the mixed powder.
  • the second powder is a mixed powder in which two or more powders having different average particle sizes are mixed
  • the average particle size of the second powder indicates the average particle size of the mixed powder.
  • the average particle size of the first powder is less than 5 ⁇ m, preferably 0.05 ⁇ m or more and less than 5 ⁇ m, more preferably 0.5 ⁇ m or more and less than 5 ⁇ m.
  • the average particle diameter of the first powder is 5 ⁇ m or more, the imaginary part ( ⁇ ′ ′) at 100 MHz is high, and the Q value of the magnetic material may be less than 20.
  • the content of the first powder may be appropriately adjusted according to the material of the other magnetic powder, the average particle diameter, etc., and is preferably 20% by mass or more and 100% by mass or less with respect to the total mass of the magnetic powder. Preferably it is 40 mass% or more and 100 mass% or less. If the content of the first powder is within the above range, the real part ( ⁇ ′) can be further improved while maintaining the Q value of the high magnetic material at 100 MHz.
  • the magnetic powder may contain other magnetic powder different from the first powder.
  • the other magnetic powder is an aggregate of other magnetic particles different from the large-diameter magnetic particles 10.
  • pure iron As a material of another magnetic particle, pure iron, a metal oxide, an alloy, resin, etc. can be used, for example.
  • Pure iron is high purity iron of 99.90% by mass or more and 99.95% by mass or less.
  • examples of pure iron include carbonyl iron, armco iron, sponge iron, electrolytic iron and the like.
  • Carbonyl iron is obtained by thermal decomposition of iron carbonyl Fe (CO) 5 .
  • the metal oxide for example, ferrite, magnetite or the like can be used.
  • Ferrite is a general term for ceramics mainly composed of iron oxide, and has insulating properties.
  • As an alloy, nickel, a cobalt base alloy, etc. can be used, for example. Among them, it is preferable to use ferrite as the material of the other magnetic particles.
  • the real part ( ⁇ ′) at 100 MHz can be further improved.
  • the ferrite may be soft ferrite exhibiting soft magnetism or hard ferrite exhibiting ferromagnetism.
  • Examples of the crystal structure of ferrite include spinel ferrite, hexagonal ferrite, garnet ferrite and the like.
  • Spinel ferrite has a spinel type crystal structure, composition formula MeO ⁇ Fe 2 O 3 or MeFe 2 O 4: represented by (Me Zn, Ni, Cu, Mn, Mg, transition metals such as Co). Most of the spinel ferrite is soft ferrite. Specific examples thereof include manganese magnesium ferrite, manganese zinc ferrite, nickel zinc ferrite and copper zinc ferrite. Spinel ferrite is effective as an inductor component for a high frequency circuit because it has a high permeability and a high electrical resistance, so that the eddy current loss in a high frequency region is small.
  • the hexagonal ferrite has a magnetoplumbite type hexagonal crystal structure, and the composition formula is represented by MO ⁇ 6Fe 2 O 3 or MFe 12 O 19 (M: alkaline earth metal such as Ba, Sr, Pb, etc.) .
  • the hexagonal ferrite is also called magnetoplumbite ferrite or M-type ferrite.
  • Hexagonal ferrite is a typical hard ferrite exhibiting a large coercive force because of its large magnetic anisotropy compared to spinel ferrite. Specific examples thereof include barium ferrite and strontium ferrite.
  • the garnet ferrite has a garnet-type crystal structure, and the composition formula is represented by 3R 2 O 3. 5 Fe 2 O 3 or R 3 Fe 5 O 12 (R: rare earth elements such as Y, Sm, Gd, etc.).
  • Garnet ferrite is also called RIG (Rare-earth Iron Garnet, rare earth iron garnet).
  • RIG Rare-earth Iron Garnet, rare earth iron garnet
  • YIG Yttrium Iron Garnet
  • Garnet ferrite is effective as an inductor component for microwaves because the magnetic loss in a high frequency region is small.
  • the average particle size of the other magnetic powder is not particularly limited, and is preferably 0.05 ⁇ m or more and 5 ⁇ m or less, more preferably 0.5 ⁇ m or more and 5 ⁇ m or less. If the average particle size of the other magnetic particle sizes is within the above range, the imaginary part ( ⁇ ′ ′) at 100 MHz can be made lower.
  • the mixing ratio of the other magnetic powder may be appropriately adjusted according to the average particle diameter of the other magnetic powder and the like.
  • the mixing ratio of the other magnetic powder is preferably less than 12% by mass, more preferably 0.5, with respect to the first powder. It is mass% or more and 10 mass% or less.
  • the Q value of the magnetic material at 100 MHz can be made 20 or more, and the magnetic resin sheet obtained Is excellent in fluidity.
  • the composite magnetic powder contains nonmagnetic powder.
  • the nonmagnetic powder includes the second powder and may further include other nonmagnetic powder.
  • the second powder is at least one of silica powder and alumina powder. That is, the composition of the second powder is a composition consisting only of silica powder, a composition consisting only of alumina powder, or a composition consisting of silica powder and alumina powder. Since the silica powder and the alumina powder both have high electrical insulation, the second powder can suppress the flow of eddy current.
  • Silica powder is an aggregate of silica particles.
  • a silica particle a crystalline silica particle, a non-crystalline silica particle, etc. can be used, for example.
  • the silica particles may be porous.
  • Alumina powder is an aggregate of alumina particles.
  • a material of the alumina particles for example, ⁇ -alumina, ⁇ -alumina, ⁇ -alumina, ⁇ -alumina, ⁇ -alumina, ⁇ -alumina and the like can be used.
  • the average particle diameter of the second powder is in accordance with the average particle diameter of the first powder, etc. so that the average particle diameter of the first powder is 3 times to 30 times the average particle diameter of the second powder It is adjusted, preferably 0.05 ⁇ m or more and 5 ⁇ m or less, more preferably 0.5 ⁇ m or more and 2 ⁇ m or less. If the average particle diameter of the second powder is within the above range, the flowability of the magnetic material before the treatment can be easily secured.
  • the content of the second powder may be appropriately adjusted according to the material, average particle diameter, and the like of the other nonmagnetic powder, and is preferably 50% by mass to 100% by mass with respect to the total mass of the nonmagnetic powder. More preferably, they are 70 mass% or more and 100 mass% or less.
  • the nonmagnetic powder may further contain other nonmagnetic powder.
  • the other nonmagnetic powder is an aggregate of other nonmagnetic particles different from the small diameter nonmagnetic particles 20.
  • nonmagnetic particles for example, carbon black, titanium oxide, cerium oxide, tin oxide, tungsten oxide, ZnO, ZrO 2 , SiO 2 , Cr 2 O 3 or the like can be used.
  • the other nonmagnetic powder preferably has electrical insulation. That is, the surface of the other nonmagnetic particles is preferably covered with an electrically insulating film.
  • an electrically insulating film As a method of the insulation treatment, for example, a method of mixing and drying a nonmagnetic powder and an aqueous solution containing an electrically insulating filler may be mentioned.
  • a material of the electrically insulating filler for example, phosphoric acid, boric acid, magnesium oxide and the like can be used.
  • the average particle size of the other nonmagnetic powder is not particularly limited, and may be about the same as the average particle size of the second powder.
  • the magnetic resin composition according to the present embodiment contains a composite magnetic powder, and at least one resin selected from the group consisting of a curable resin and a thermoplastic resin.
  • the magnetic resin composition may be a resin composition containing a curable resin (hereinafter referred to as a first magnetic resin composition), and a resin composition containing a thermoplastic resin (hereinafter referred to as a second magnetic resin) It may be called a composition).
  • the cured product or solidified product of the magnetic resin composition preferably has a Q value of 20 or more at a frequency of 100 MHz. That is, the cured product of the first magnetic resin composition preferably has a Q value of 20 or more at a frequency of 100 MHz, and the solidified product of the second magnetic resin composition has a Q value of 20 or more at a frequency of 100 MHz. Is preferred.
  • the magnetic resin composition can be suitably used as the magnetic material of the high frequency inductor component.
  • the cured product or solidified product of the magnetic resin composition more preferably has a Q value of 33 or more at a frequency of 100 MHz.
  • the first magnetic resin composition contains a composite magnetic powder and a curable resin.
  • the first magnetic resin composition contains a curable resin.
  • curable resins include thermosetting resins and photocurable resins.
  • the first magnetic resin composition may contain only a thermosetting resin, may contain only a photocurable resin, or may contain both a thermosetting resin and a photocurable resin. Good.
  • the photocurable resin is a reactive compound capable of absorbing light and causing a crosslinking reaction.
  • the photocurable resin is not particularly limited as long as it is a photocurable resin.
  • a resin having a polymerizable unsaturated group may be used.
  • photocurable resins include methacrylic resins, acrylic resins, epoxy resins, and oxetane resins.
  • the photocurable resin contained in the first magnetic resin composition may be used alone or in combination of two or more.
  • the photocurable resin may be liquid at room temperature or solid such as powder.
  • methacrylic resins examples include methacrylic acid esters, polymethacrylic acid esters, and ethylene-methacrylic acid copolymers.
  • acrylic resins include ethylene-acrylic acid copolymers, ethylene-methyl acrylic acid copolymers, acrylic acid esters, and polyacrylic acid esters.
  • the epoxy resin may be a monofunctional epoxy resin having one epoxy group in one molecule, or a polyfunctional epoxy resin having two or more epoxy groups in one molecule.
  • polyfunctional epoxy resins include polybutadiene epoxy resins, bisphenol A epoxy resins, bisphenol type epoxy compounds such as bisphenol F epoxy resins, naphthalene type epoxy compounds, aliphatic epoxy compounds, biphenyl type epoxy, glycidyl amine type epoxy compounds, Alcohol type epoxy compounds such as hydrogenated bisphenol A type epoxy compounds, epoxy modified silicones, phenol novolac type epoxy compounds, novolac type epoxy compounds such as cresol novolac type epoxy compounds, alicyclic epoxy compounds, heterocyclic epoxy type compounds, many Halogenated epoxy compounds such as functional epoxy compounds, glycidyl ether type epoxy compounds, glycidyl ester type epoxy compounds, brominated epoxy compounds, rubber modified epoxy compounds Including styrene block copolymer, epoxy group-containing polyester compounds, epoxy group-containing polyurethane compound, an epoxy group-containing
  • the oxetane resins may be used alone or in combination of two or more.
  • the first magnetic resin composition may contain a photopolymerization initiator as needed.
  • photopolymerization initiators include photo radical generation initiators and photo acid generation initiators.
  • the first magnetic resin composition preferably contains a photoradical generation initiator.
  • the photo radical generation initiator is not particularly limited as long as it generates radicals to initiate the photopolymerization reaction.
  • the first magnetic resin composition preferably contains a photoacid generation initiator.
  • the photoacid generation initiator is not particularly limited, and may be an ionic photoacid generation initiator or a non-ionic photoacid generation initiator.
  • the first magnetic resin composition preferably contains a thermosetting resin.
  • a thermosetting resin is a reactive compound which can cause a crosslinking reaction by heat.
  • the thermosetting resin for example, bisphenol A epoxy resin, bisphenol F epoxy resin, polyfunctional epoxy resin, biphenyl epoxy resin, cresol novolac epoxy resin, phenol novolac epoxy resin, imide resin can be used.
  • the polyfunctional epoxy resin is a resin having three or more epoxy groups in one molecule.
  • the thermosetting resin contained in the first magnetic resin composition may be used alone or in combination of two or more.
  • the thermosetting resin may be liquid at room temperature or solid such as powder.
  • the content of the thermosetting resin is preferably 75% by mass or more and 100% by mass or less based on the total mass of the resin component in the first magnetic resin composition.
  • the first magnetic resin composition may further contain a curing agent.
  • the curing agent is an additive that cures the thermosetting resin.
  • a curing agent dicyandiamide, a phenol based curing agent, cyclopentadiene, an amine based curing agent, an acid anhydride or the like can be used.
  • the phenolic curing agent has two or more phenolic hydroxyl groups in one molecule.
  • phenol-based curing agent for example, phenol novolak resin, phenol aralkyl resin, naphthalene type phenol resin, bisphenol resin and the like can be used.
  • a bisphenol resin bisphenol A resin, bisphenol F resin etc. can be used, for example.
  • the curing agent may be liquid or solid at normal temperature. The content of the curing agent is preferably 20% by mass or less based on the total mass of the resin component of the first magnetic resin composition.
  • the first magnetic resin composition may further contain a curing accelerator.
  • a curing accelerator for example, tertiary amines, tertiary amine salts, imidazoles, phosphines, phosphonium salts and the like can be used.
  • the imidazole 2-ethyl-4-methylimidazole can be used.
  • the content of the curing accelerator may be appropriately adjusted according to the materials of the thermosetting resin and the curing agent.
  • the first magnetic resin composition may further contain a thermoplastic resin. Thereby, bending followability, elasticity etc. can be provided to the magnetic resin sheet 1 mentioned later.
  • a phenoxy resin etc. can be used as a thermoplastic resin.
  • the content of the thermoplastic resin is preferably 2% by mass or more and 50% by mass or less based on the total mass of the resin component of the first magnetic resin composition.
  • the first magnetic resin composition may further contain a surface treatment agent.
  • a surface treatment agent a silane coupling agent, a dispersing agent, etc. can be used, for example.
  • silane coupling agent for example, 3-glycidyloxypropyltriethoxysilane can be used.
  • the dispersant for example, higher fatty acid phosphates, amine salts of higher fatty acid phosphates, alkylene oxides of higher fatty acid phosphates, and the like can be used.
  • the higher fatty acid phosphate octyl phosphate, decyl phosphate, lauryl phosphate and the like can be used.
  • the content of the surface treatment agent is preferably 0% by mass or more and 30% by mass or less based on the total mass of the resin component of the first magnetic resin composition.
  • the first magnetic resin composition may further contain an elastomer.
  • an elastomer for example, a thermosetting elastomer or a thermoplastic elastomer can be used.
  • the first magnetic resin composition may further contain a solvent.
  • a solvent Methyl ethyl ketone (MEK), N, N-dimethylformamide (DMF), acetone, methyl isobutyl ketone (MIBK) and the like can be used.
  • MEK Methyl ethyl ketone
  • DMF N-dimethylformamide
  • MIBK methyl isobutyl ketone
  • the solvents may be used alone or in combination of two or more. When two or more solvents are mixed, the mixing ratio (mass ratio and volume ratio) is not particularly limited.
  • the content of the composite magnetic powder is preferably 70% by mass or more of the total solid content of the first magnetic resin composition, more preferably 75% by mass or more, particularly preferably 80% by mass or more preferable. If the content of the composite magnetic powder is 70% by mass or more of the total solid content of the magnetic resin composition, the real part ( ⁇ ′) at 100 MHz tends to be 6.0 or more, and the high frequency inductor should be designed well Can.
  • the content of the composite magnetic powder is preferably 99.5% by mass or less, more preferably 99% by mass or less, of the total solid content of the first magnetic resin composition, and 98.5% by mass It is particularly preferred that When the content of the composite magnetic powder is 99.5% by mass or less of the total solid content of the magnetic resin composition, the Q value of the magnetic material tends to be high.
  • the solid content of the magnetic resin composition is the amount obtained by removing the solvent from the magnetic resin composition.
  • a method of preparing the first magnetic resin composition for example, a method of mixing a composite magnetic powder, a curable resin, and as necessary, a curing agent, a curing accelerator, a thermoplastic resin, a surface treatment agent, an elastomer, etc. Etc.
  • the first magnetic resin composition can be in the form of paste, slurry, powder, or sheet
  • the first magnetic resin composition in an appropriate form according to the subsequent steps.
  • the subsequent steps include, for example, a transfer molding step using a mold, and a heating and pressurizing embedded molding step.
  • the second magnetic resin composition (hereinafter, the second magnetic resin composition) contains a composite magnetic powder and a thermoplastic resin.
  • Thermoplastic resins are compounds that soften by heating to the glass transition temperature or melting point and solidify by cooling to a temperature below the glass transition temperature or melting point.
  • a thermoplastic resin nylon etc. can be used, for example.
  • nylon, nylon 6 etc. can be used, for example.
  • the second magnetic resin composition may further contain a curable resin.
  • a curable resin curable resin which the said 1st magnetic resin composition may contain can be used.
  • the content of the curable resin is preferably 2% by mass or more and 50% by mass or less based on the total mass of the resin component of the second magnetic resin composition.
  • the second magnetic resin composition may further contain a surface treatment agent.
  • a surface treatment agent a silane coupling agent, a dispersing agent, etc. can be used, for example.
  • silane coupling agent for example, 3-glycidyloxypropyltriethoxysilane can be used.
  • the dispersant for example, higher fatty acid phosphates, amine salts of higher fatty acid phosphates, alkylene oxides of higher fatty acid phosphates, and the like can be used.
  • the higher fatty acid phosphate octyl phosphate, decyl phosphate, lauryl phosphate and the like can be used.
  • the content of the surface treatment agent is preferably 0% by mass or more and 30% by mass or less based on the total mass of the resin component of the second magnetic resin composition.
  • the second magnetic resin composition may further contain an elastomer.
  • rubber elasticity can be imparted to the solidified product of the second magnetic resin composition.
  • an elastomer a thermosetting elastomer, a thermoplastic elastomer, etc. can be used, for example.
  • the content of the elastomer may be appropriately adjusted depending on the application of the second magnetic resin composition and the like.
  • the second magnetic resin composition may further contain a solvent.
  • a solvent methyl ethyl ketone (MEK), N, N-dimethylformamide (DMF), acetone, methyl isobutyl ketone (MIBK) or the like can be used.
  • MEK methyl ethyl ketone
  • DMF N-dimethylformamide
  • MIBK acetone
  • MIBK methyl isobutyl ketone
  • the solvents may be used alone or in combination of two or more. When two or more solvents are mixed, the mixing ratio (mass ratio and volume ratio) is not particularly limited.
  • the content of the composite magnetic powder is preferably 70% by mass or more of the total solid content of the second magnetic resin composition, more preferably 75% by mass or more, particularly preferably 80% by mass or more preferable.
  • the content of the composite magnetic powder is 70% by mass or more of the total solid content of the magnetic resin composition, the ratio of the composite magnetic powder to the second magnetic resin composition becomes high, and the solidified product with high complex magnetic permeability You can get Further, the content of the composite magnetic powder is preferably 99.5% by mass or less, more preferably 99% by mass or less, of the total solid content of the second magnetic resin composition, and 98.5% by mass It is particularly preferred that When the content of the composite magnetic powder is 99.5% by mass or less of the total solid content of the magnetic resin composition, the flowability of the second magnetic resin composition at the time of molding can be secured, and the complex permeability It is possible to obtain a solidified product with high magnetic permeability.
  • the solid content of the magnetic resin composition is the amount obtained by removing the solvent from the magnetic resin composition.
  • the second magnetic resin composition for example, a method of charging the composite magnetic powder and the thermoplastic resin, and, if necessary, an elastomer into a kneader, and melt-kneading may be mentioned.
  • a kneader for example, a screw extruder, a kneader, a Banbury mixer, a twin-screw kneader, or the like can be used.
  • the second magnetic resin composition obtained may be molded into a desired shape.
  • the second magnetic resin composition may be formed by extrusion molding, injection molding, or the like.
  • the second magnetic resin composition can be in the form of paste, slurry, powder, or sheet
  • the second magnetic resin composition of an appropriate form according to the subsequent steps can be used.
  • the subsequent steps include, for example, a transfer molding step using a mold, and a heating and pressurizing embedded molding step.
  • the magnetic resin composition is paste-like.
  • the pasty state means that the magnetic resin composition has fluidity at room temperature.
  • the magnetic resin composition may be a first magnetic resin composition or a second magnetic resin composition. That is, in the magnetic resin paste, the first magnetic resin composition may be in the form of paste, and the second magnetic resin composition may be in the form of paste.
  • the filling ratio of the magnetic powder in the magnetic resin paste (hereinafter referred to as the content of the magnetic powder) is preferably from 20% by volume to 99% by volume, more preferably from 53% by volume to 95% by volume with respect to the entire solid content of the magnetic resin paste. % Or less. If the content of the magnetic powder is within the above range, the real part ( ⁇ ′) at 100 MHz can be increased, and the flowability of the magnetic resin paste can be easily controlled.
  • the content of the magnetic powder was calculated from the compounding amounts of the respective materials constituting the solid content of the magnetic resin paste and the specific gravities of the respective materials. In the magnetic resin paste, when the magnetic resin composition contains a solvent, the solid content of the magnetic resin paste is the amount obtained by removing the solvent from the magnetic resin composition.
  • a method of preparing a magnetic resin paste for example, at least one liquid type resin selected from the group consisting of a curable resin and a thermoplastic resin is used, and a composite magnetic powder, a liquid type resin, and, if necessary, Examples thereof include methods of mixing a curing agent, a curing accelerator, a surface treatment agent, an elastomer, and the like.
  • the magnetic resin paste when the magnetic resin composition contains a solvent, for example, at least one resin selected from the group consisting of a curable resin and a thermoplastic resin is dissolved in the solvent to obtain a resin solution.
  • a magnetic resin paste can be obtained by mixing the composite magnetic powder and, if necessary, a curing agent, a curing accelerator, a surface treatment agent, an elastomer and the like with the resulting resin solution.
  • the magnetic resin paste may be in the form of a paste in which the magnetic resin composition contains a solvent, or may be in the form of a paste containing no solvent. That is, the first magnetic resin composition may be in the form of a paste containing a solvent, or may be in the form of a paste containing no solvent.
  • the second magnetic resin composition may be in the form of a paste containing a solvent, or may be in the form of a paste containing no solvent.
  • the magnetic resin paste is preferably in the form of a paste in which the magnetic resin composition does not contain a solvent.
  • a solvent since the magnetic resin paste does not contain a solvent, generation of voids can be prevented when the magnetic resin paste is stored or when it is heated.
  • it is possible to reduce the risk of contamination of members and equipment used with the magnetic resin paste by the solvent contained in the magnetic resin paste.
  • a solvent when a solvent is contained in the magnetic resin paste, it may be necessary to deal with explosion-proofing of a dedicated process or apparatus used in the manufacturing process. However, since the magnetic resin paste does not contain a solvent, the manufacturing process can be simplified.
  • the content of the solvent contained in the magnetic resin composition is 5% by mass or less of the total solid content of the magnetic resin composition Is preferable, and 1% by mass or less is more preferable, and 0.5% by mass or less is particularly preferable.
  • methyl ethyl ketone MEK
  • N, N-dimethylformamide DMF
  • acetone methyl isobutyl ketone (MIBK) or the like
  • the solvents may be used alone or in combination of two or more.
  • the mixing ratio mass ratio and volume ratio is not particularly limited.
  • the magnetic resin composition is powdery.
  • the magnetic resin composition may be a first magnetic resin composition or a second magnetic resin composition.
  • the magnetic resin powder may be powdery of the first magnetic resin composition, and the powder of the semi-cured product of the first magnetic resin composition It may be a letter.
  • a semi-cured product is one in which the resin composition is partially cured to such an extent that it can be cured further. That is, a semi-cured product refers to the B-stage state, and refers to the state of the intermediate stage of the curing reaction.
  • the intermediate stage refers to the stage between the varnish state (A stage state) and the completely cured state (C stage state).
  • the thermosetting resin composition when heated, the viscosity gradually decreases, and then curing starts and the viscosity gradually increases.
  • the semi-cured state is a state in which the viscosity starts to increase and before it is completely cured.
  • the average particle diameter of the particles constituting the magnetic resin powder is not particularly limited.
  • a method of preparing a magnetic resin powder for example, a method using an atomizing method using a magnetic resin slurry described later, and at least one resin selected from the group consisting of a composite magnetic powder, a curable resin and a thermoplastic resin
  • the method of mixing powder and a 3-roll mill etc., the method of crushing the magnetic resin sheet mentioned later, etc. are mentioned.
  • the atomizing method is particularly preferred in that individual particles constituting the magnetic resin powder can be made approximately spherical. When the individual particles that make up the magnetic resin powder are substantially spherical, the flowability during the subsequent molding process will be good.
  • the magnetic resin slurry is sprayed in a high temperature (for example, 140 ° C.) environment to form atomized particles, and the magnetic resin powder is prepared by rapidly drying to volatilize the solvent.
  • the first magnetic resin composition has a possibility that the viscosity becomes high because the content of the composite magnetic powder is relatively large.
  • the solvent which is a volatile component is rapidly dissipated and becomes powdery, Good handling of
  • the magnetic resin composition further contains a solvent and is in a slurry form.
  • the slurry state means that the magnetic resin composition contains a solvent and has fluidity at room temperature.
  • the magnetic resin composition may be a first magnetic resin composition or a second magnetic resin composition. That is, the magnetic resin slurry may be in the form of a slurry in which the first magnetic resin composition contains a solvent, and may be in the form of a slurry in which the second magnetic resin composition contains a solvent.
  • methyl ethyl ketone MEK
  • N, N-dimethylformamide DMF
  • acetone methyl isobutyl ketone (MIBK) or the like
  • the solvents may be used alone or in combination of two or more.
  • the mixing ratio mass ratio and volume ratio
  • the content of the solvent in the magnetic resin slurry is not particularly limited.
  • the filling ratio of the magnetic powder in the magnetic resin slurry (hereinafter referred to as the content of the magnetic powder) is preferably from 20% by volume to 99% by volume, more preferably from 53% by volume to 95% by volume with respect to the entire solid content of the magnetic resin slurry. % Or less. If the content of the magnetic powder is in the above range, the real part ( ⁇ ′) at 100 MHz can be increased, and the flowability of the magnetic resin sheet can be easily controlled.
  • the content of the magnetic powder was calculated from the compounding amounts of the respective materials constituting the solid content of the magnetic resin slurry and the specific gravities of the respective materials.
  • the solid content of the magnetic resin slurry is the amount obtained by removing the solvent from the magnetic resin slurry.
  • the magnetic resin slurry for example, at least one resin selected from the group consisting of a curable resin and a thermoplastic resin is dissolved in a solvent to obtain a resin solution, and the composite magnetic powder is added to the obtained resin solution And kneading, and if necessary, a curing agent, a curing accelerator, a surface treatment agent, an elastomer and the like are finally added and stirred to be uniform.
  • the magnetic resin composition is in the form of a sheet.
  • the magnetic resin composition may be a first magnetic resin composition or a second magnetic resin composition.
  • the first magnetic resin composition in the magnetic resin sheet 1, the first magnetic resin composition may be in the form of a sheet, and the semi-cured product of the first magnetic resin composition It may be sheet-like.
  • the size of the magnetic resin sheet 1 may be appropriately adjusted according to the application of the magnetic resin sheet 1.
  • the thickness of the magnetic resin sheet 1 is preferably 10 ⁇ m or more and 500 ⁇ m or less, more preferably 50 ⁇ m or more and 300 ⁇ m or less.
  • the greenness value which shows the fluidity of the magnetic resin sheet 1 is preferably 60% or more and 95% or less, more preferably 70% or more and less than 90%.
  • the green resin value of the magnetic resin sheet 1 is within the above range, for example, when molding a laminated board in which the magnetic resin sheet 1 is laminated on the main surface of the wiring substrate having the wiring formed on the main surface by lamination or press And the magnetic resin sheet 1 having appropriate fluidity can sufficiently embed the wiring, and the magnetic resin sheet 1 flows too much, and the laminator or the press machine may be contaminated by the magnetic resin sheet 1 protruding. Can be avoided.
  • the Grinis value can be measured in the same manner as the method described in the examples.
  • the amount of volatilization of the magnetic resin sheet 1 is preferably 1% by mass or less, more preferably 0.2% by mass or less.
  • the magnetic resin sheet 1 and the cover film are repeatedly refrigerated or refrigerated storage of the magnetic resin sheet 1 whose surface is covered with a cover film and return to normal temperature. Between the above, it is possible to prevent the occurrence of a spot pattern due to the evaporation of the solvent in the magnetic resin sheet 1 or to prevent the flowability of the magnetic resin sheet 1 from becoming too high.
  • the amount of volatilization can be measured in the same manner as the method described in the examples.
  • the magnetic resin sheet 1 is in the form of a sheet, it is easy to form a large area with a magnetic material having a uniform thickness, and is useful as a material for printed wiring boards which is difficult in the form of powder or paste. Since the magnetic resin sheet 1 is a semi-cured product, it can be used, for example, when embedding and forming a circuit of a printed wiring board by heating and pressurizing while performing vacuum drawing.
  • the magnetic resin sheet 1 As a method of manufacturing the magnetic resin sheet 1, for example, as shown in FIGS. 2A to 2C, a method of applying a magnetic resin slurry on a film 2 to form a magnetic resin slurry layer 3 and drying or heating may be mentioned.
  • the film 2 for example, a polyethylene terephthalate (PET) film, a metal foil or the like can be used.
  • PET polyethylene terephthalate
  • the thickness of the film 2 is not particularly limited. It is preferable that the surface of the film 2 to which the magnetic resin slurry layer 3 is applied be subjected to release treatment in advance. Moreover, you may produce the magnetic resin sheet 1 by apply
  • the magnetic resin sheet 30 with metal foil As shown in FIG. 4, the magnetic resin sheet 30 with metal foil according to the present embodiment (hereinafter, the magnetic resin sheet 30 with metal foil) is laminated on the magnetic resin sheet 1 and at least one surface of the magnetic resin sheet 1. And the metal foil 8 having a thickness of 5 ⁇ m or less.
  • the magnetic resin sheet 30 with metal foil has a two-layer structure including the magnetic resin sheet 1 and the metal foil 8 laminated on one side of the magnetic resin sheet 1.
  • the magnetic resin sheet 30 with metal foil may have a three-layer structure including the magnetic resin sheet 1 and two metal foils 8 laminated on both sides of the magnetic resin sheet 1.
  • the magnetic resin sheet 30 with metal foil may have another layer between the magnetic resin sheet 1 and the metal foil 8.
  • the first magnetic resin composition may be in the form of a sheet, or may be in the form of a sheet of a semi-cured product of the first magnetic resin composition, and the second magnetic The resin composition may be in the form of a sheet.
  • the thickness of the magnetic resin sheet 30 with metal foil is preferably 10 ⁇ m or more and 800 ⁇ m or less.
  • a material of metal foil copper, silver, aluminum, nickel, stainless steel etc. can be used, for example.
  • the thickness of the metal foil is preferably 0.5 ⁇ m or more and 300 ⁇ m or less.
  • the magnetic resin sheet 30 As a method of adjusting the magnetic resin sheet 30 with metal foil, for example, a method of forming the metal foil 8 on one side or both sides of the magnetic resin sheet 1 by physical vapor deposition can be mentioned. As a physical vapor deposition method, a vacuum evaporation method, an ion plating method, sputtering method etc. are mentioned, for example. Alternatively, the magnetic resin sheet 30 may be produced by applying a magnetic resin slurry or magnetic resin paste onto the metal foil 8 using a bar coater or the like, and drying or heating it.
  • the magnetic prepreg 40 (hereinafter, magnetic prepreg 40) according to the present embodiment includes a fibrous base material 42 and a semi-cured product of the magnetic resin composition 41 or the magnetic resin composition 41, as shown in FIG.
  • Examples of the magnetic prepreg 40 include those in which the fibrous base material 42 is present in the magnetic resin composition 41 or the semi-cured product of the magnetic resin composition 41.
  • the magnetic prepreg 40 comprises a semi-cured product of the magnetic resin composition 41 or the magnetic resin composition 41 and a fibrous base material 42 present in the semi-cured product of the magnetic resin composition 41 or the magnetic resin composition 41; Equipped with Since the magnetic prepreg 40 includes the fibrous base material 42, the magnetic prepreg 40 is more excellent in bending strength and the like than the magnetic resin sheet 1.
  • the magnetic resin composition may be a first magnetic resin composition or a second magnetic resin composition. That is, the magnetic prepreg 40 may include the one before curing the first resin composition and the fibrous base material 42, and the semi-cured product of the first resin composition and the fibrous base material 42 may be provided. The magnetic prepreg 40 may also include the second resin composition and the fibrous base material 42.
  • the thickness of the magnetic prepreg is preferably 10 ⁇ m or more and 500 ⁇ m or less.
  • the fibrous base material 42 for example, woven fabric (cross), non-woven fabric, pulp paper, linter paper, etc. can be used.
  • the woven fabric for example, organic fiber cloth such as glass cloth, aramid cloth and polyester cloth, graphite cloth and the like can be used.
  • the non-woven fabric for example, an organic fiber non-woven fabric such as a glass non-woven fabric, an aramid non-woven fabric and a polyester non-woven fabric, a graphite non-woven fabric, an inorganic (for example, magnesium oxide) non-woven fabric can be used.
  • a glass cloth a magnetic prepreg 40 with excellent mechanical strength can be obtained.
  • the fibrous base material 42 it is preferable to use a flattened glass cloth as the fibrous base material 42.
  • Specific examples of the flattening processing include a method of pressing the glass cloth flat by continuously pressing the glass cloth with a press roll under an appropriate pressure.
  • the thickness of the fibrous base material 42 is not particularly limited, and for example, one having a thickness of 0.02 mm or more and 0.3 mm or less can be used.
  • the magnetic resin composition 41 may be prepared in the form of a varnish and used in order to impregnate the fibrous base material 42 which is a base material for forming the magnetic prepreg 40. . That is, you may use the resin varnish in which the magnetic resin composition 41 was prepared in varnish form.
  • Such resin varnish can be prepared, for example, as follows.
  • each component soluble in a solvent which contains at least one resin selected from the group consisting of a curable resin and a thermoplastic resin in the magnetic resin composition 41, is charged into a solvent and dissolved. At this time, heating may be performed as necessary. Thereafter, a component which does not dissolve in the solvent, including the composite magnetic powder, is added and dispersed to a predetermined dispersed state using a ball mill, bead mill, planetary mixer, roll mill or the like to obtain a varnish-like composition. Be prepared.
  • the solvent used here the same solvents as those described above as the solvent which can be contained in the magnetic resin composition can be used.
  • the resin varnish in which the magnetic resin composition 41 is prepared in the form of varnish may be used, and the magnetic resin paste which is the paste-like magnetic resin composition 41 described above, A magnetic resin slurry which is a slurry-like magnetic resin composition 41 may be used.
  • the fibrous base material 42 contains the magnetic resin composition 41 prepared in a varnish form, the magnetic resin paste containing the magnetic resin composition 41, or the magnetic resin composition 41. And a method of impregnating and drying the magnetic resin slurry.
  • the magnetic resin composition 41 can be impregnated into the fibrous base material 42 by immersion, coating, and the like. Immersion, application, etc. may be repeated several times and impregnated as needed. In addition, by repeating impregnation using a magnetic resin paste or magnetic resin slurry containing a plurality of magnetic resin compositions 41 or magnetic resin compositions 41 having different compositions and concentrations, the final desired composition and impregnation amount are obtained. It is also possible to adjust.
  • a first magnetic resin composition containing a thermosetting resin as the magnetic resin composition 41
  • desired heating conditions for example, You may heat at 80 degreeC or more and 180 degrees C or less for 1 minute or more and 10 minutes or less. By heating, the magnetic prepreg 40 provided with the semi-cured product of the first magnetic resin composition can be obtained.
  • the inductor component (hereinafter, inductor component) according to the present embodiment includes a coiled wire and an insulating layer covering the coiled wire, and the insulating layer is a cured product of the first magnetic resin composition or a second
  • the magnetic resin composition of the present invention is molded with a solidified product (hereinafter sometimes referred to as a magnetic material).
  • a solidified product hereinafter sometimes referred to as a magnetic material.
  • the Q value of the magnetic material at 100 MHz of the insulating layer tends to be high. It can be suitably used as a high frequency inductor component.
  • the inductor component of the present embodiment can be particularly suitably used as a high frequency inductor component.
  • high frequency inductor components include coils, inductors, filters, reactors, and transformers.
  • applications of such inductor components include components of noise filters, components of impedance matching circuits, and the like.
  • the noise filter include a low pass filter and a common choke coil.
  • the structure of the inductor component may be appropriately adjusted in accordance with the application of the inductor component, and examples thereof include a wire wound type, a laminated type, and a film type.
  • the size of the inductor component may be appropriately adjusted according to the application of the inductor component, and when used as a substantially cubic high frequency inductor component, preferably 15 mm or less ⁇ 15 mm or less ⁇ 10 mm or less in height is there.
  • the shape of the coiled wiring may be appropriately selected according to the application of the inductor component.
  • the spiral shape may be planarly formed, or the spiral shape may be three-dimensionally formed.
  • the winding structure may be a horizontal winding structure or a vertical winding structure.
  • the beginning and end of the coiled wire are used by being electrically connected to different external electrode terminals.
  • a material of the coiled wiring for example, Ag, Au, Cu, Ag—Pd, Ni or the like can be used.
  • the insulating layer covers the coiled wire except for the beginning and the end of the coiled wire.
  • the raw material of the insulating layer is the first magnetic resin composition or the second magnetic resin composition.
  • the method of manufacturing the inductor component may be appropriately selected according to the configuration of the inductor component according to the application of the inductor component, and for example, the coiled wiring is continuously formed three-dimensionally by the printing method, sheet method, etc. Methods are included.
  • a magnetic resin sheet or a sheet of a second magnetic resin composition hereinafter collectively referred to as a green sheet
  • a conductive paste constituting a coiled wiring are alternately printed and laminated, and the inside of the inductor component is formed.
  • the sheet method is a method of forming through holes in a green sheet, printing and filling a conductive paste, and laminating.
  • Alloy iron powder 1 (“AW2-08 / PF5KG” manufactured by Epson Atomics Co., Ltd., representative composition: Fe-Si-Cr, average particle diameter: 4 ⁇ m, particle shape: all spherical, insulation treatment: available)
  • Alloy iron powder 2 (“AW2-08 / PF3KG” manufactured by Epson Atomics Co., Ltd., representative composition: Fe-Si-Cr, average particle diameter: 3 ⁇ m, particle shape: all spherical, insulation treatment: available)
  • Alloy powder (“AW2-08 / PF8KG” manufactured by Epson Atomics Co., Ltd., representative composition: Fe-Si-Cr, average particle diameter: 5 ⁇ m, particle shape: all spherical, insulation treatment: available)
  • Pure iron powder (“CIP FM” manufactured by BASF Japan Ltd., representative composition: Fe, average particle diameter: 2 ⁇ m, particle shape: all
  • the Grinis value was determined as follows. 1) A magnetic sheet having a thickness of 200 ⁇ m was punched out using a 60 mm ⁇ mold, and a polyethylene terephthalate film was peeled off to prepare a test plate 4. 2) As shown in FIG. 3, a release PET film 5 with a thickness of 75 ⁇ m and a SUS plate 6 with a thickness of 1.8 mm were laminated in this order on both sides of the test plate 4 to obtain a sample set. 3) The sample set was molded by pressing from above and below at an actual pressure of 2.0 Mpa for 10 minutes under atmospheric pressure using a hot plate 7 whose press hot plate temperature was set to 135 ° C.
  • the viscosity of the magnetic resin paste was measured using a rheometer "AR 2000 ex” manufactured by TA Instruments. Specifically, the gap between the upper and lower 25 mm diameter parallel plates is set to 300 ⁇ m, and after filling the magnetic resin paste there, the temperature balance time is set for 2 minutes at room temperature, and the rotation speed is 0.2 rpm. Viscosity measurement was performed. In addition, viscosity measurement at a rotation speed of 2.0 rpm was performed in the same manner.
  • the thixotropic index of the magnetic resin paste was calculated according to the following formula using the values of 0.2 rpm viscosity and 2.0 rpm viscosity measured in the measurement of [2.0 rpm viscosity] described above.
  • Thixo index 0.2 rpm viscosity / 2.0 rpm viscosity
  • DMA-Tg The DMA-Tg of the magnetic resin sheet was measured using a viscoelastic spectrometer "DMS 100" manufactured by Seiko Instruments Inc. Specifically, dynamic viscoelasticity measurement (DMA) is performed with a tension module at a frequency of 10 Hz, and the temperature at which tan ⁇ shows a maximum when the temperature is raised from room temperature to 320 ° C. at a temperature increase rate of 5 ° C./min is DMA -Tg.
  • DMA dynamic viscoelasticity measurement
  • the surface resistance value was measured using "R8340A” manufactured by ADVANTEST in accordance with Standard ASTM D257. Specifically, a test piece (50 mm ⁇ 50 mm ⁇ 1 mm t) is placed between the front electrode (25 mm ⁇ ) and the front electrode consisting of the main electrode and concentric electrodes (inside diameter 38 mm ⁇ , outer diameter 50 mm ⁇ ) and the back electrode (50 mm ⁇ ). It arranges and it measured on the following setting conditions. Setting conditions: Applied voltage 100V, charge time 60 seconds, discharge time 0.1 seconds
  • the real part ( ⁇ ′) and the imaginary part ( ⁇ ′ ′) are obtained from the measured initial magnetization curve, and the obtained real part ( ⁇ ′) and the imaginary part ( ⁇ ′ ′) give the loss factor (Tan ⁇ ) and the Q value of the magnetic material Was calculated.
  • the real part ( ⁇ ′) is preferably 6.0 or more in terms of the design of the high frequency inductor component. In order to function as a high frequency inductor component, it is essential that the Q value of the magnetic material is 20 or more. Furthermore, in order to exhibit good performance as a high frequency inductor component, it is preferable that the Q value of the magnetic material is 33 or more.
  • Examples 1 to 6 In Examples 1 to 6, the content of the magnetic powder is different, and the content of the magnetic powder showing a real part ( ⁇ ') appropriate for functioning as a high frequency inductor component, ie, the real part ( ⁇ ') at 100 MHz is We examined the content of magnetic powder showing 6.0 or more.
  • the resin solution was obtained by mixing bisphenol A epoxy resin, trifunctional epoxy resin, polyfunctional epoxy resin, phenoxy resin, MEK and DMF at the mixing ratio shown in Table 1. Alloy iron 2 (average particle diameter: 3 ⁇ m) and alumina (average particle diameter: 0.7 ⁇ m) are added to the obtained resin solution at the mixing ratio shown in Table 1 and kneaded, and dicyandiamide, imidazole 1, silane cup.
  • the magnetic resin slurry was obtained by adding the ring agent 1 and the dispersing agent and stirring the mixture uniformly.
  • the magnetic resin slurry obtained was applied to the surface of the polyethylene terephthalate film subjected to the releasing treatment and dried to obtain a magnetic resin sheet in a B-stage state having a thickness of 200 ⁇ m.
  • the grin value, the amount of volatile, DMA-Tg, the surface resistance value and the magnetic property were measured. The results are shown in Table 1.
  • the real part ( ⁇ ') and the imaginary part ( ⁇ ") increase, while the Q value and the grin value of the magnetic material tend to decrease.
  • the real part ( ⁇ ') and the glycini value are most well balanced in the example 4 in which the content of the magnetic powder is 53.0% by volume. .
  • Example 7 and 8 and Comparative Examples 1 to 4 In Examples 7 and 8 and Comparative Examples 1 and 2, while maintaining the content (53.0% by volume) of the magnetic powder of Example 4, the particle size ratio of the first powder to the second powder (hereinafter referred to simply as The particle size ratio satisfying the Q value of the magnetic material which is essential to function as a high frequency inductor component is changed by changing the particle size ratio), that is, the particle size ratio of 20 or more of the Q value of the magnetic material at 100 MHz is examined.
  • the Comparative Example 3 and Comparative Example 4 do not contain the first powder.
  • magnetic resin slurries were obtained in the same manner as in [Examples 1 to 6] except that the raw materials were blended at the blending ratio shown in Table 2. Using the obtained magnetic resin sheet, the grin value, the amount of volatile, DMA-Tg, the surface resistance value and the magnetic property were measured. The results are shown in Table 2.
  • the real part ( ⁇ ') and the glycin value tended to decrease as the particle size ratio increased.
  • the imaginary part ( ⁇ ′ ′) decreases as the particle size ratio increases, and tends to be substantially constant when the particle size ratio exceeds 4.3 (Example 4).
  • the Q value of the magnetic material is the particle size As the ratio increases, it increases, and the particle size ratio tends to decrease when it exceeds 4.3 (Example 4)
  • the Q value of the magnetic material does not contain the alloy iron powder. Was less than 20.
  • the Q value of the magnetic material was less than 20 because the average particle size of the alloyed iron powder was not less than 5 ⁇ m.
  • the magnetic material having the highest Q value and the good Grinis value among Example 4 was Example 4 having a particle size ratio of 4.3.
  • Example 9 to 13 While maintaining the content (53.0% by volume) and the particle size ratio (4.3) of the magnetic powder of Example 4, the mass ratio of magnetic powder to nonmagnetic powder (hereinafter referred to as mass ratio)
  • mass ratio The first mass ratio satisfying the Q value of the magnetic material exhibiting good performance as a high frequency inductor component, that is, the mass ratio of the magnetic material at 100 MHz of 33 or more was examined.
  • Comparative Example 5 contains no nonmagnetic powder.
  • a magnetic resin slurry was obtained in the same manner as in [Examples 1 to 6] except that the raw materials were blended at the blending ratio shown in Table 3.
  • the grin value, the amount of volatile, DMA-Tg, the surface resistance value and the magnetic property were measured. The results are shown in Table 3.
  • Examples 14 and 15 In Examples 14 and 15, while maintaining the particle size ratio at 4.3 and the mass ratio at 6.0, ferrite powder is added as another magnetic powder, and the Q value change of the magnetic material by the addition of the ferrite powder is determined. Examined. Specifically, magnetic resin slurries were obtained in the same manner as in [Examples 1 to 6] except that the raw materials were blended at the blending ratio shown in Table 4. Using the obtained magnetic resin sheet, the grin value, the amount of volatile, DMA-Tg, the surface resistance value and the magnetic property were measured. The results are shown in Table 4.
  • Example 16 a magnetic resin paste was obtained without containing a solvent. Specifically, the magnetic resin paste was obtained by mixing the raw materials shown in Table 5 at the mixing ratio shown in Table 5 and kneading so as to be uniform. For mixing and kneading of the raw materials, known mixers and kneaders were used.
  • the thixotropic index of Example 16 produced without containing a solvent was 3.8, and the Q value was 20 or more. From this result, even if the magnetic resin composition is a paste-like magnetic resin paste containing no solvent, it has excellent fluidity and satisfies the Q value of the magnetic material which is essential to function as a high frequency inductor component. all right.
  • the composite magnetic powder of the first aspect according to the present invention contains a magnetic powder containing a first powder and a nonmagnetic powder containing a second powder.
  • the first powder comprises alloyed iron powder and the second powder comprises at least one of alumina powder and silica powder.
  • the average particle size of the first powder is less than 5 ⁇ m and is at least 3 times and not more than 30 times the average particle size of the second powder.
  • the Q value of the magnetic material in the high frequency band can be increased.
  • the mixing ratio of the magnetic powder is 4 parts by mass to 19 parts by mass with respect to 1 part by mass of the nonmagnetic powder.
  • the second aspect it is possible to balance the Q value of the magnetic material at 100 MHz and the flowability of the magnetic material before processing.
  • the magnetic powder of the third aspect according to the present invention in the first or second aspect, the magnetic powder is subjected to an insulation treatment.
  • the Q value of the magnetic material can be made higher.
  • the magnetic resin composition of the fourth aspect according to the present invention is at least one resin selected from the group consisting of the composite magnetic powder of any one of the first to third aspects, a curable resin and a thermoplastic resin. And.
  • a magnetic material having a high Q value in a high frequency band can be obtained.
  • the content of the composite magnetic powder is 70% by mass or more and 99.5% by mass or less of the total solid content of the magnetic resin composition .
  • a magnetic material that can be suitably used for high frequency inductor applications can be obtained.
  • the cured product or solidified product of the magnetic resin composition has a Q value at a frequency of 100 MHz of 20 or more.
  • a magnetic material that can be suitably used for high frequency inductor applications can be obtained.
  • the magnetic resin composition of any one of the fourth to sixth aspects is paste-like.
  • a magnetic material having good fluidity can be obtained.
  • the magnetic resin composition of any one of the fourth to sixth aspects is powdery.
  • a powdery magnetic material can be obtained.
  • the magnetic resin composition according to any one of the fourth to sixth aspects further contains a solvent and is in the form of a slurry.
  • a magnetic material having good flowability can be obtained.
  • the magnetic resin composition according to any one of the fourth to sixth aspects is in the form of a sheet.
  • a magnetic material having a uniform thickness can be obtained.
  • the magnetic resin sheet according to the eleventh aspect of the present invention has a thickness of 10 ⁇ m to 500 ⁇ m in the tenth aspect.
  • a magnetic material having a constant thickness can be obtained.
  • a magnetic resin sheet with metal foil according to a twelfth aspect of the present invention is a metal foil having a thickness of 5 ⁇ m or less laminated on at least one surface of the magnetic resin sheet according to the tenth or eleventh aspect and the magnetic resin sheet.
  • a magnetic material with a metal foil can be obtained.
  • a magnetic prepreg according to a thirteenth aspect of the present invention comprises a fibrous base material and a semi-cured product of the magnetic resin composition or the magnetic resin composition according to any one of the fourth to sixth aspects.
  • the inductor component according to the fourteenth aspect of the present invention includes a coiled wire and an insulating layer covering the coiled wire, and the insulating layer is the magnetic resin composition according to any one of the fourth to sixth aspects. It is molded with a cured product or solidified product of
  • an inductor component that can be suitably used as a high frequency inductor component can be obtained.

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  • Chemical & Material Sciences (AREA)
  • Dispersion Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Soft Magnetic Materials (AREA)
PCT/JP2018/044903 2017-12-08 2018-12-06 複合磁性粉末、磁性樹脂組成物、磁性樹脂ペースト、磁性樹脂粉末、磁性樹脂スラリー、磁性樹脂シート、金属箔付磁性樹脂シート、磁性プリプレグ及びインダクタ部品 WO2019112002A1 (ja)

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