JP2023103144A5

JP2023103144A5 -

Info

Publication number: JP2023103144A5
Application number: JP2022013691A
Authority: JP
Filing date: 2022-01-13
Publication date: 2024-01-25

Description

実施例１～１２および比較例１、２、４、７で使用したナノ結晶軟磁性金属扁平粉末の作製には、単ロール法により作製した厚み２０μｍのＦｅ_８３．３Ｓｉ_７．７Ｂ_２．０Ｎｂ_５．７Ｃｕ_１．３（ｗｔ％）組成のアモルファス薄帯を出発原料として用いた。これをＡｒ雰囲気中で実施例１～５と比較例１、２、４は４２０℃で、実施例６～１２と比較例７はそれぞれ２２０℃で１時間脆化処理した後に、ボールミルで７４μｍ以下に粉砕した。次いで粉砕粉末を、アトライターでエタノールを用いた湿式条件により扁平加工した。さらにＡｒ雰囲気中５６０℃で１時間のナノ結晶化処理を行った。 To prepare the nanocrystalline soft magnetic metal flat powder used in Examples 1 to 12 and Comparative Examples 1, 2, 4 , and 7, Fe _83.3 Si _7.7 B _2. An amorphous ribbon having a composition of ₀ Nb _5.7 Cu _1.3 (wt%) was used as a starting material. This was subjected to embrittlement treatment in an Ar atmosphere at 420°C for Examples 1 to 5 and Comparative Examples 1, 2, and 4 , and at 220°C for Examples 6 to 12 and Comparative Example 7 for 1 hour, and then milled with a ball mill to a diameter of 74 μm or less. It was crushed. The pulverized powder was then flattened using an attritor under wet conditions using ethanol. Furthermore, nanocrystallization treatment was performed at 560° C. for 1 hour in an Ar atmosphere.

実施例１～１２、比較例１、２、４、７では得られたナノ結晶軟磁性金属扁平粉末を用い、全固形分に対して５０ｖｏｌ％となるように、耐熱温度１５０℃の熱硬化型アクリルゴム系混合樹脂をトルエンで希釈した樹脂溶液に配合後に分散させて、コーティング用の塗料を作製した。この塗料をコンマコーターで０．０５ｍｍ厚みに塗布し、磁場配向を行った後に５０℃で乾燥し溶剤を除去した。乾燥後のシートを６枚積層して１５０℃で１０ＭＰａの圧力で熱プレスし、厚み０．１５ｍｍの性能評価用の樹脂複合シートを得た。次に外形２０ｍｍ、内径１０ｍｍのドーナツ状に抜き加工し、透磁率と保磁力とコアロスを測定した。各温度での透磁率の実数部（μ’）は１ＭＨｚ、虚数部（μ’’）は１０ＭＨｚで測定した。 In Examples 1 to 12 and Comparative Examples 1, 2, 4 , and 7, the obtained nanocrystalline soft magnetic metal flat powder was used, and a thermosetting type with a heat resistance temperature of 150 ° C. A coating material for coating was prepared by blending an acrylic rubber-based mixed resin into a resin solution diluted with toluene and then dispersing it. This paint was applied to a thickness of 0.05 mm using a comma coater, oriented in a magnetic field, and then dried at 50°C to remove the solvent. Six dried sheets were laminated and hot pressed at 150° C. and a pressure of 10 MPa to obtain a resin composite sheet with a thickness of 0.15 mm for performance evaluation. Next, it was punched into a donut shape with an outer diameter of 20 mm and an inner diameter of 10 mm, and its magnetic permeability, coercive force, and core loss were measured. The real part (μ') of magnetic permeability at each temperature was measured at 1 MHz, and the imaginary part (μ'') was measured at 10 MHz.

表１に実施例１～５、比較例１、２、４、５を示す。実施例１～５は樹脂複合シートのフレキシビリティーを重視して、ナノ結晶金属扁平粉末の平均粒径が２０μｍ～４０μｍ未満で、かつ平均厚みが０．２～１．５μｍ未満で、ナノ結晶化処理後に所定のかさ密度／真密度の扁平粉末が得られるように扁平加工条件を調整した。さらに扁平加工工程で、ナノ結晶化処理後の保磁力が最低となるように、微粉末の発生を抑え、扁平粉末の輪郭が平滑になるように、スラリー濃度、粉砕メディアの衝突エネルギーなどの扁平加工条件を最適化した。同時に、扁平粉末の面内に制御された適度なマイクロクラックを導入した。 Table 1 shows Examples 1 to 5 and Comparative Examples 1, 2, 4, and 5. Examples 1 to 5 focused on the flexibility of the resin composite sheet, and the nanocrystalline metal flat powder had an average particle size of 20 μm to less than 40 μm and an average thickness of 0.2 to less than 1.5 μm, and Flattening conditions were adjusted so that flattened powder with a predetermined bulk density/true density could be obtained after the chemical treatment. Furthermore, in the flattening process, the slurry concentration, the collision energy of the crushing media, etc. Optimized processing conditions. At the same time, moderately controlled microcracks were introduced within the plane of the flat powder.

表２に実施例６～１２、比較例７、１０、１１を示す。実施例６～１２は樹脂複合シートの透磁率を重視して、ナノ結晶軟磁性金属扁平粉末の平均粒径が４０μｍ～１００μｍ未満で、かつ平均厚みが１．５～５μｍ未満で、ナノ結晶化処理後に所定のかさ密度／真密度の扁平粉末が得られるように扁平加工条件を調整した。さらに扁平加工工程で、ナノ結晶化処理後の保磁力が最低となるように、微粉末の発生を抑え、扁平粉末の輪郭が平滑になるように、スラリー濃度、粉砕メディアの衝突エネルギーなどの扁平加工条件を最適化した。同時に、扁平粉末の面内に制御された適度なマイクロクラックを導入した。実施例８～１０では空気分級により、保磁力の高い微粉末と、内在亀裂が磁気ギャップとなり軟磁気特性に影響を及ぼす粗大扁平粉末をそれぞれ５ｗｔ％除去した。 Table 2 shows Examples 6 to 12 and Comparative Examples 7, 10, and 11 . Examples 6 to 12 focused on the magnetic permeability of the resin composite sheet, and the nanocrystalline soft magnetic metal flat powder had an average particle size of 40 μm to less than 100 μm and an average thickness of 1.5 to less than 5 μm, and was nanocrystallized. Flattening conditions were adjusted so that flattened powder having a predetermined bulk density/true density could be obtained after treatment. Furthermore, in the flattening process, the slurry concentration, the collision energy of the crushing media, etc. are adjusted to suppress the generation of fine powder and to make the outline of the flat powder smooth so that the coercive force after nanocrystallization is the lowest. Optimized processing conditions. At the same time, moderately controlled microcracks were introduced within the plane of the flat powder. In Examples 8 to 10, air classification was used to remove 5 wt % of each of fine powder with high coercive force and coarse flat powder in which inherent cracks become magnetic gaps and affect soft magnetic properties.

表１より、実施例１～５はいずれも実数（１ＭＨｚ）および虚数透磁率（１０ＭＨｚ）の温度係数Ｋが－４０℃～１５０℃の範囲で０≦Ｋ１≦０．２０、－０．１０≦Ｋ２≦０．１０、－０．１５≦Ｋ３≦０．０５を満たしており、測定温度の透磁率への影響が軽微である。また、比較例１、２、４よりも高い実数および虚数透磁率を０℃で有しているとともに、コアロスがいずれも低い。比較例５のガスアトマイズ法により作製したＦｅ_８４．８Ａｌ_５．６Ｓｉ_９．６（ｗｔ％）組成の合金粉末を用いた金属扁平粉末では、０℃で透磁率が最大になり、８５℃、１５０℃での透磁率の低下が顕著である。さらに、０℃での透磁率が大幅に不足しているともに、コアロスが高い。 From Table 1, in Examples 1 to 5, the temperature coefficient K of real number (1 MHz) and imaginary number permeability (10 MHz) is 0≦K1≦0.20, -0.10≦ in the range of -40°C to 150°C. K2≦0.10 and -0.15≦K3≦0.05 are satisfied, and the influence of the measured temperature on the magnetic permeability is slight. Further, it has higher real and imaginary magnetic permeability at 0° C. than Comparative Examples 1, 2, and 4 , and all have low core loss. In the flat metal powder using the alloy powder with the composition of Fe _84.8 Al _5.6 Si _9.6 (wt%) produced by the gas atomization method of Comparative Example 5, the magnetic permeability reached its maximum at 0°C, and the magnetic permeability reached the maximum at 85°C. The decrease in magnetic permeability at 150°C is significant. Furthermore, the magnetic permeability at 0° C. is significantly insufficient and the core loss is high.

Claims

A nanocrystalline soft magnetic metal flat powder in which the nanocrystalline particles have a particle size of 5 nm to less than 30 nm and a crystallinity of 65% to less than 95%, and the aspect ratio of the powder with a particle size around the average particle size D50 is 20. temperature coefficient of magnetic permeability of a resin composite sheet or a molded resin composite composition using the nanocrystalline soft magnetic metal flat powder with a coercive force of 20 A/m to less than 150 A/m. Kn (n is 1, 2, 3) is represented by the following formulas (1), (2), and (3) in the range of -40°C to 150°C, 0≦K1≦0.20, -0.10≦ A nanocrystalline soft magnetic metal flat powder, characterized in that K2≦0.10, -0.15≦K3≦0.05.
K1=(μ(0℃)−μ(−40℃))/μ(−40℃) (1)
K2=(μ(85℃)−μ(−40℃))/μ(−40℃) (2)
K3=(μ(150℃)−μ(−40℃))/μ(−40℃) (3)
μ: magnetic permeability (μ': real magnetic permeability, μ'': imaginary magnetic permeability), μ (0℃): magnetic permeability at 0℃

The nanocrystalline soft magnetic metal flat powder according to claim 1, wherein the nanocrystalline powder has an average particle size D50 of 20 μm to less than 40 μm and an average thickness around the D50 average particle size of 0.2 μm to less than 1.5 μm. A nanocrystalline soft magnetic metal flat powder characterized in that the coercive force of the resin composite sheet is from 20 A/m to less than 100 A/m.

The nanocrystalline soft magnetic metal flat powder according to claim 1, wherein the average particle size D50 is 40 μm to less than 100 μm and the average thickness around the D50 average particle size is 1.5 μm to less than 5 μm, A nanocrystalline soft magnetic metal flat powder, characterized in that the coercive force of a resin composite sheet using the metal flat powder is from 20 A/m to less than 80 A/m.

A method for producing a nanocrystalline soft magnetic metal flat powder according to any one of claims 1 to 3, comprising:
A step of embrittling a Fe-based amorphous alloy foil strip serving as a raw material at a temperature below the nanocrystallization temperature,
A step of pulverizing after the embrittlement treatment to obtain a raw material powder for flattening;
A step of performing flattening in the presence of distilled water or an organic solvent, and introducing controlled moderate microcracks within the plane of the raw material powder for flattening during the flattening;
The flat powder obtained after the flattening process is heat-treated at a temperature higher than the crystallization temperature in a nitrogen gas atmosphere, an inert gas atmosphere, or a vacuum to generate a nanocrystalline phase, so that the flat powder undergoes volume shrinkage due to nanocrystallization. 1. A method for producing flat nanocrystalline soft magnetic metal powder, the method comprising the step of self-rupturing to reduce the diameter.

It is made of the flat nanocrystalline soft magnetic metal powder according to any one of claims 1 to 3 and a resin, has a coercive force of 20 A/m to less than 100 A/m, and further has an outer diameter of 20 mm - an inner diameter of 10 mm and a thickness of 0.15 mm. A resin composite sheet characterized by having a core loss of 50 to less than 300 kW/m ³ when measured using a stack of three ring-shaped samples under conditions of Bm and frequency of 50 mT to 100 kHz.

A product made of the flat nanocrystalline soft magnetic metal powder according to any one of claims 1 to 3 and a resin, molded to have an outer diameter of 12.8 mm - an inner diameter of 7.5 mm and a thickness of 5 mm, has a Bm and a frequency of 50 mT. A resin composite composition for molding, characterized in that the core loss is less than 100 to 600 kW/m ³ when measured at -100 kHz.