JP2003293005A - HYDRIDE-COATED Fe-Ni SOFT MAGNETIC ALLOY POWDER AND MANUFACTURING METHOD - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide hydride-coated Fe-Ni soft magnetic alloy powder and its manufacturing method. <P>SOLUTION: In the hydride-coated Fe-Ni soft magnetic alloy powder, the surface of Fe-Ni soft magnetic alloy powder is coated with hydride of rare-earth elements including Y, Zr hydride, Ti hydride, Hf hydride, V hydride, Ta hydride or Pd hydride (hereinafter referred to as metal hydride). In the method for manufacturing the hydride-coated Fe-Ni soft magnetic alloy powder, the surface of the Fe-Ni soft magnetic alloy powder is coated with the metal hydride by a high-speed impact method or a binder method by using the Fe-Ni soft magnetic alloy powder having 10 to 150 μm average particle size and powder of the metal hydride having 1 to 10 μm average particle size. <P>COPYRIGHT: (C)2004,JPO

Description

Detailed Description of the Invention

[0001]

This invention relates to a hydride-coated Fe-
The present invention relates to a Ni-based soft magnetic alloy powder and a method for producing the same.

[0002]

2. Description of the Related Art Generally, a soft magnetic sintered material obtained by sintering Fe-Ni based soft magnetic alloy powder is used for a magnetic head case, a magnetic shield case, a magnetic shield room, an iron core of various transformers, a stepping motor step for a watch. -It is known that it is used for a yoke and the like. This Fe-
The soft magnetic sintered material obtained by sintering Ni-based soft magnetic alloy powder has excellent corrosion resistance, but has a low specific resistance, and when this is used as a magnetic core, eddy current loss occurs and effective permeability decreases. Therefore, it cannot be used for high frequencies. In order to avoid this, silica, titanium oxide, alumina, boron oxide, iron oxide, on the surface of the Fe-Ni soft magnetic alloy powder,
A high-resistance layer-coated soft magnetic powder coated with a substance having a large specific resistance such as a metal oxide such as ferrite having a spinel structure, a nitride, a fluoride, a chloride, a bromide, and an iodide is prepared. Fe-N by sintering soft magnetic powder
Silica having a large specific resistance at the grain boundary of the i-based soft magnetic alloy powder,
Composite soft magnetic sintered material having a structure in which titanium oxide, alumina, boron oxide, iron oxide, metal oxide such as ferrite having a spinel structure, nitride, fluoride, chloride, bromide, iodide, etc. are interposed. Is already known, and this composite soft magnetic sintered material has a large resistance value due to the interposition of a substance having a large specific resistance between Fe-Ni soft magnetic alloy powders, which causes an eddy current loss. Has been able to be used for high frequencies since it has dropped significantly.

A composite soft magnetic sintered material having a structure in which a substance having a large specific resistance is present between the Fe--Ni soft magnetic alloy powder is a Fe--Ni soft magnetic alloy powder containing silica,
Titanium oxide, alumina, boron oxide, iron oxide, metal oxides such as ferrite, nitrides, fluorides, chlorides, bromides, colloids consisting of iodide are mixed to produce a high resistance layer-coated soft magnetic powder, It is made by sintering this high resistance layer-coated soft magnetic powder. Among the composite soft magnetic sintered materials obtained by sintering these high-resistance layer-coated soft magnetic powders, a high-performance material obtained by coating the surface of Fe—Ni soft magnetic alloy powder with a ferrite layer having a spinel structure. The composite soft magnetic sintered material, which has a structure in which Fe-Ni soft magnetic alloy powders obtained by sintering the resistance layer-coated soft magnetic powders are separated by a ferrite layer, is particularly excellent in high frequency characteristics and is the most noticeable. There is.

[0004]

However, a conventional high resistance layer-coated soft magnetic powder obtained by coating a ferrite layer having a spinel structure on the surface of an Fe-Ni soft magnetic alloy powder is sintered at high temperature to increase the density. If it is attempted to raise it, the ferrite layer will be decomposed or destroyed so that a sufficient resistance value cannot be obtained, and the actual sintering must be carried out at less than 900 ° C. If it is sintered at such a low temperature, the Fe--Ni-based soft magnetic Although the ferrite layer formed on the surface of the alloy powder is extremely less decomposed or destroyed, the density of the obtained composite soft magnetic sinter is decreased due to the low sintering temperature, and therefore the mechanical strength, especially There was a drawback that the folding force was reduced. On the other hand, a layer made of a highly resistant material having excellent heat resistance such as silica, titanium oxide, alumina, boron oxide, nitride, fluoride, chloride, bromide, and iodide is provided between the grains of the Fe-Ni soft magnetic alloy powder. A composite soft magnetic sintering material having a structure in which Fe-Ni soft magnetic alloy powders are formed and isolated from each other,
Silica, titanium oxide, alumina, boron oxide, nitride,
High resistance materials such as fluorides, chlorides, bromides, and iodides are stable against heat, so even if they are sintered at high temperatures, the high resistance material powders are not decomposed or destroyed during sintering, but Fe The Ni-based soft magnetic alloy powder and the high-resistance substance powder such as silica, titanium oxide, alumina, boron oxide, nitride, fluoride, chloride, bromide, and iodide hardly diffuse and solid-solve during sintering, Therefore, these high-resistance substance powders have a drawback that a composite soft magnetic sintered material having sufficient mechanical strength cannot be obtained because they interfere with the joining of the Fe-Ni soft magnetic alloy powders. However, in recent years
These composite soft magnetic sinters are about to be used in parts such as solenoid valves and plungers that are subject to vibration or shock. There is also a demand for a high-strength, composite soft magnetic sinter that can be used for parts that are subject to impact and that has excellent magnetic properties.

[0005]

Therefore, the present inventors have
Research was conducted to obtain a composite soft magnetic sintered material having high strength, high density, and high resistance. As a result, (a) on the surface of the Fe—Ni soft magnetic alloy powder, a hydride of a rare earth element containing Y (hereinafter referred to as R), a hydride of Zr, a hydride of Ti, a hydride of Hf, V Hydride, Ta hydride or Pd hydride (hereinafter, these are referred to as metal hydrides) are coated to form a hydride-coated Fe-Ni soft magnetic alloy powder, which is then pressed into a non-oxidizing atmosphere. After sintering at a temperature of 900 to 1300 ° C.,
In the composite soft magnetic sintered material obtained by the hydrogenation treatment by heating at a temperature of 150 to 800 ° C. in a hydrogen atmosphere, the metal hydride is present in the grain boundary of the Fe—Ni soft magnetic alloy powder. A composite soft magnetic sintered material having the above structure is obtained, and since the metal hydride coating has a high specific resistance value, a composite soft magnetic sintered material having high resistance is obtained. Since it is sintered at high temperature, it has high density and high strength compared with the composite soft magnetic sintered material having iron oxide or ferrite layer, while silica, titanium oxide, alumina, boron oxide, nitride, fluorine Mechanical strength as compared with the conventional composite soft magnetic sinter material in which a layer made of a highly resistant material having excellent heat resistance such as fluoride, chloride, bromide and iodide is formed at the grain boundary of Fe-Ni soft magnetic alloy powder. Improve, (b) Said sinter After the completion, in the heat treatment step of heat treatment in a hydrogen atmosphere, the degree of hydrogenation of the metal hydride can be adjusted by adjusting the amount of hydrogen contained in the hydrogen atmosphere, and thereby the Fe—Ni soft magnetic alloy. It can be used in a wide frequency range from low frequency to high frequency because the amount of hydrogenation in metal hydride intervening at the grain boundary of the powder can be adjusted and the resistance value of the composite soft magnetic sintered material can be adjusted accordingly. Research results were obtained, such as obtaining a possible composite soft magnetic sintered material.

The present invention has been made on the basis of the results of such research. (1) A hydride-coated Fe-Ni-based soft material obtained by coating the surface of Fe-Ni-based soft magnetic alloy powder with a metal hydride. It is characterized by a magnetic alloy powder.

The Fe—Ni soft magnetic alloy powder has an average particle diameter of 10 to 100 μm, and the surface of the Fe—Ni soft magnetic alloy powder is preferably coated with a metal hydride. Fe− having an average particle size of 10 to 100 μm
Ni-based soft magnetic alloy powder is commonly used Fe-N
It is an i-based soft magnetic alloy powder and is not particularly novel.
Therefore, the present invention provides (2) average particle size: 10 to 10
It is characterized by a hydride-coated Fe-Ni-based soft magnetic alloy powder in which the surface of 0-μm Fe-Ni-based soft magnetic alloy powder is coated with a metal hydride.

The Fe—Ni soft magnetic alloy powder coated with hydride of the present invention mechanically mixes and stirs the Fe—Ni soft magnetic alloy powder and the metal hydride to obtain the Fe—Ni soft magnetic alloy powder and the metal hydrogen. Of the Fe-Ni-based soft magnetic alloy powder by applying a mechanical energy to the surface of the Fe-Ni soft magnetic alloy powder (hereinafter, this method is referred to as a high-speed impact method) You can

By this high-speed impact method, hydride-coated Fe-
The metal hydride used in the method for producing the Ni-based soft magnetic alloy powder may be a powder, but is not particularly limited to the powder and may be a lump. The reason is that metal hydrides are easier to grind than Fe-Ni-based soft magnetic alloy powders. Therefore, when metal hydrides are added to Fe-Ni-based soft magnetic alloy powders and a high-speed impact method is applied, the metal hydrides are Ground into finer powder, while hard Fe-Ni
Since the average particle diameter of the soft magnetic alloy powder hardly changes, the metal hydride is Fe-Ni during the high-speed impact method.
This is because the fine soft powder is pulverized before the soft magnetic alloy powder and the surface of the Fe-Ni soft magnetic alloy powder is coated with metal hydride. However, if the metal hydride is finer than the Fe—Ni soft magnetic alloy powder, the production of the hydride-coated Fe—Ni soft magnetic alloy powder by the high-speed impact method becomes faster. Therefore, the Fe-Ni-based soft magnetic alloy powder used in the production of the hydride-coated Fe-Ni-based soft magnetic alloy powder by this high-speed impact method has an average particle size of:
Fe-Ni soft magnetic alloy powder of 10 to 100 μm is used, while metal hydride powder has a finer average particle size: 1 to 10 μm than Fe-Ni soft magnetic alloy powder. It is more preferable to use a compound powder. Therefore, according to the present invention, (3) the surface of the Fe—Ni soft magnetic alloy powder is coated with the metal hydride by subjecting the mixture of the Fe—Ni soft magnetic alloy powder and the metal hydride to a high-speed impact method. 1) or a method for producing a hydride-coated Fe-Ni-based soft magnetic alloy powder according to (2),
It is characterized by

Further, the binder and the metal hydride powder are added to the Fe-Ni soft magnetic alloy powder, and the mixture is stirred and dried to coat the surface of the Fe-Ni soft magnetic alloy powder with the metal hydride powder with the binder. The surface of the Fe—Ni soft magnetic alloy powder can be coated with a metal hydride by a solidifying method (hereinafter referred to as a binder method).
Therefore, according to the present invention, (4) a binder and a metal hydride powder are added to the Fe—Ni soft magnetic alloy powder,
Fe-N by a binder method in which it is dried and solidified after stirring
The method for producing a hydride-coated Fe-Ni-based soft magnetic alloy powder according to (1) or (2) above, wherein the surface of the i-based soft magnetic alloy powder is coated with a metal hydride.

By this binder method, hydride-coated Fe
-To produce Ni-based soft magnetic alloy powder, average particle size: 1
Fe-Ni-based soft magnetic alloy powder of 0-100 μm with Fe-
Finer average particle size than Ni-based soft magnetic alloy powder: 1
It is preferable to use a metal hydride powder of 10 μm. The reason is that in the binder method, when the metal hydride is added in a lump for kneading with the binder, the metal hydride is less likely to be crushed like the high-speed impact method,
Therefore, if the metal hydride is added in a lump form, the metal hydride will not be sufficiently crushed and the particle size will vary,
This is because the surface of the Fe—Ni soft magnetic alloy powder is not uniformly covered with the metal hydride. Therefore, the present invention has (5) an average particle diameter of 10 to 100 μm, which is relatively finer than the Fe—Ni soft magnetic alloy powder and the Fe—Ni soft magnetic alloy powder. The hydride-coated Fe-Ni soft magnetic alloy according to (1) or (2), wherein the metal hydride powder is mixed and stirred with a binder, and the surface of the Fe-Ni soft magnetic alloy powder is coated with the metal hydride by a binder method. It is characterized by a method for producing powder.

In order to manufacture a composite soft magnetic sintered material using the hydride-coated Fe-Ni type soft magnetic alloy powder of the present invention, the hydride-coated Fe- described in (1) or (2) above is used.
Ni-based soft magnetic alloy powder is compacted, sintered in a non-oxidizing atmosphere at a temperature of 900 to 1300 ° C., and then hydrogenated at a temperature of 150 to 800 ° C. in a hydrogen atmosphere. Is obtained by In this case, the step of hydrogenating by heating at a temperature of 150 to 800 ° C. in a hydrogen atmosphere can be replaced by setting the atmosphere to be a hydrogen atmosphere in the step of cooling after sintering.

In the present invention, R is Y, Ce,
La, Pr, Nd, Sm, Gd, Ho, Er, Yb, L
It is one or more of u. Further, the Fe-Ni-based soft magnetic alloy powder for producing the composite soft magnetic sintered material having high strength, high density and high resistance of the present invention is obtained by the atomization method,
Fe-Ni produced by either electrolytic method or reduction method
Soft magnetic alloy powders can be used. The Fe-Ni-based soft magnetic alloy powder used in this invention is JIS 25
Fe-N having the composition defined by 31-99
This is a powder of an i-based soft magnetic alloy, and this JIS 2531-
Fe-Ni-based soft magnetic alloy powder specified in 99 is
It has a composition containing 30 to 80% by mass of Ni and the balance of Fe and unavoidable impurities, but other N.
i: 70 to 85%, Mo: 0.5 to 5%, Cu: 1 to 7
%, And the balance is Fe-Ni soft magnetic alloy powder having a composition consisting of Fe and inevitable impurities. Other generally known soft magnetic Fe-Ni alloy powders may be used. it can.

[0014]

BEST MODE FOR CARRYING OUT THE INVENTION Example 1 As a raw material powder, an atomized Fe—Ni soft magnetic alloy having an average particle size of 55 μm, a composition of Ni: 45% and the balance of Fe and inevitable impurities was atomized. A powder is prepared, and further, each has a Y hydride powder, an La hydride powder, a Ce hydride powder, an Nd hydride powder, an Sm hydride powder, and a Zr hydride, each having an average particle diameter of 3 μm. Powder, Ti hydride powder, Hf hydride powder, V hydride powder, Ta hydride powder or Pd
The hydride powder of was prepared. The hydride powder of Y, L
a hydride powder, Ce hydride powder, Nd hydride powder, Sm hydride powder, Zr hydride powder, T
i hydride powder, Hf hydride powder, V hydride powder, Ta hydride powder or Pd hydride powder in a high-speed impact device having a rotatable blade together with Fe-Ni soft magnetic alloy atomized powder. After charging, the number of rotations of the blade: 6000 r.p.m. p. m. The hydride powder of the present invention was removed by removing the hydride powder left uncoated by mixing and stirring by rotating for 3 minutes at 37 ° C. and sieving.
-Ni-based soft magnetic alloy powder (hereinafter referred to as the present invention powder) 1
~ 11 were produced. 6 tons of these powders 1 to 11 of the present invention
Vertical: 40 mm by applying molding pressure of n / cm ² .
A compacted body having dimensions of width: 10 mm and thickness: 5 mm is molded, and the obtained compacted body is subjected to 1100 in an inert gas atmosphere.
Sintered at a temperature of ℃, 800 ℃ in the cooling process after sintering
Hydrogen was supplied so that the atmosphere became a hydrogen atmosphere at the time of cooling, and this hydrogen atmosphere was kept at least at 150 ° C. until it was hydrogenated to prepare a composite soft magnetic sintered material.

Conventional Example 1 For comparison, Fe-Ni soft magnetic alloy atomized powder
On the surface of (Mn₁₇Zn ₁₆Fe₆₇)₃O_FourConventional coated
Ferrite-coated Fe-Ni soft magnetic alloy powder (hereinafter
Prepared powder) and prepared this conventional powder at 6 ton / c
m²By applying molding pressure of: vertical: 40 mm, horizontal: 1
0 mm, thickness: molding a compact having a dimension of 5 mm,
By sintering the obtained compact at 800 ° C, it becomes grain boundaries.
A composite soft magnetic sintered material having a ferrite phase was produced.

The relative density and transverse rupture strength of the thus obtained composite soft magnetic sintered material were measured, and the results are shown in Table 1. Furthermore, the magnetic flux density, resistance value and frequency: 1
The relative permeability at a high frequency of 00 KHz was measured, and the results are shown in Table 1.

[0017]

[Table 1]

From the results shown in Table 1, the powders of the present invention 1 to
The composite soft magnetic sintered material prepared in No. 11 is comparable to the composite soft magnetic sintered material prepared by the conventional powder having a ferrite phase in the grain boundary in the magnetic characteristics and the resistance value, It can be seen that the composite soft magnetic sintered material produced in No. 11 has a higher density and higher mechanical strength than the composite soft magnetic sintered material produced by the conventional powder.

Example 2 An atomized powder of an Fe-Ni soft magnetic alloy prepared in Example 1 having an average particle size of 55 μm, a composition of Ni: 45%, and the balance being Fe and inevitable impurities. , Y hydride powder, La hydride powder, Ce hydride powder, each having a fine average particle size: 3 μm
Nd hydride powder, Sm hydride powder, Zr hydride powder, Ti hydride powder, Hf hydride powder,
V hydride powder, Ta hydride powder or Pd hydride powder was blended in an amount of 2% each, and polyvinyl alcohol as a binder: 0.05%, balance: Fe-
Ni-based soft magnetic alloy was blended to become atomized powder,
This compounded powder was charged into a processing device having a rotatable stirring blade, and the stirring blade was rotated at a rotation speed of 1000 r. p. m. The mixture is agitated by rotating for 20 minutes to prepare Fe-Ni-based soft magnetic alloy powders of the present invention (hereinafter referred to as the present invention powders) 12 to 22, and these powders are 6 ton / cm.
By applying molding pressure of ² , length: 40 mm, width: 10
mm, thickness: when forming a compact having dimensions of 5 mm, sintering the obtained compact at a temperature of 1150 ° C. in an inert gas atmosphere, and cooling to 800 ° C. in the cooling step after sintering Hydrogen was supplied so that the atmosphere became a hydrogen atmosphere, and this hydrogen atmosphere was kept at least at 150 ° C. until it was hydrogenated to produce a composite soft magnetic sintered material.

The relative density and the transverse rupture strength of the thus obtained composite soft magnetic sintered material were measured, and the results are shown in Table 1. Further, the magnetic flux density, the resistance value and the frequency: 1
The relative magnetic permeability was measured at a high frequency of 00 KHz, and the results are shown in Table 2.

[0021]

[Table 2]

The composite soft magnetic sintered materials prepared from the powders 12 to 22 of the present invention shown in Table 2 are compared with the composite soft magnetic sintered materials prepared from the conventional powder shown in Table 1 having a ferrite phase at the grain boundary. In addition, the magnetic properties and resistance values are comparable to each other, and the composite soft magnetic sintered material produced by the powders 12 to 22 of the present invention has a higher density than the composite soft magnetic sintered material produced by the conventional powders. In addition, it can be seen that the mechanical strength is higher.

[0023]

INDUSTRIAL APPLICABILITY The present invention can provide a composite soft magnetic sintered material having a high density, excellent mechanical strength, and high relative permeability at high frequencies, and brings excellent effects in the electric and electronic industries. Is.

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Claims (5)

[Claims] 1. A Fe-Ni-based soft magnetic alloy powder having Y on the surface thereof.
Rare earth element hydride containing, Zr hydride, Ti hydride, Hf hydride, V hydride, Ta hydride or Pd hydride (hereinafter these are referred to as metal hydride) is coated. Fe-Ni based soft magnetic alloy powder coated with hydride. 2. Fe-Ni having an average particle size of 10 to 100 μm.
A hydride-coated Fe-Ni soft magnetic alloy powder, characterized in that the surface of the soft magnetic alloy powder is coated with a metal hydride. 3. Fe-Ni having an average particle size of 10 to 100 μm.
3. The metal hydride is coated on the surface of the Fe—Ni soft magnetic alloy powder by mixing and stirring the soft magnetic alloy powder and the metal hydride and applying mechanical energy. Hydride coated Fe-Ni
Method for producing soft magnetic alloy powder. 4. A method for coating a surface of Fe—Ni soft magnetic alloy powder with metal hydride by adding metal hydride powder and a binder to Fe—Ni soft magnetic alloy powder, stirring and drying and solidifying. The method for producing the hydride-coated Fe-Ni-based soft magnetic alloy powder according to claim 1 or 2. 5. The Fe-Ni based soft magnetic alloy powder has an average particle diameter of 10 to 100 μm, the metal hydride powder has an average particle diameter of 1 to 10 μm, and the average particle of the metal hydride powder. The method of producing a hydride-coated Fe-Ni-based soft magnetic alloy powder according to claim 4, wherein the diameter is relatively finer than the average particle diameter of the metal hydride powder.