JP2002038245A - Alloy powder for rare earth permanent magnet and method for producing rare earth permanent magnet - Google Patents

Abstract

(57) [Problem] To provide a method for adding Co, Cu, Dy or the like, which can sufficiently utilize a conventional rare earth material alloy without any change, and reduce coarse crystal grains during sintering. An object of the present invention is to achieve high magnetic characteristics without causing generation and a reduction in coercive force. SOLUTION: The present invention is directed to a method for producing R (at least one or more rare earth elements including Y) in an amount of 29 to 33 mass% and boron B0.
8 to 1.2 mass%, combined addition of Ga and Al
a 0.01 to 0.5 mass% and Al 0.01 to 2.
An alloy consisting of 0 mass% and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 2
9-33 mass%, Ga and Al are added in combination
0.01-0.5 mass% and Al 0.01-2.0
An alloy consisting of a mass% and a balance of Fe (a part of Fe is replaced by Co and Cu) is used as a second alloy, and the first alloy powder and the second alloy powder are mixed in a predetermined composition. This is a method for producing a rare earth alloy powder and a rare earth permanent magnet using the same.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

TECHNICAL FIELD The present invention relates to an RTB (R is a rare earth, T is a transition metal, etc., B is boron) alloy powder for permanent magnets, and an RTB permanent magnet using the same. The present invention relates to a method for manufacturing a magnet.

[0002]

2. Description of the Related Art Today, RTB-based permanent magnets are used in a wide range of fields such as various home appliances, information communication devices, computer peripheral devices, and various motors. As the magnets are expanded, the magnets used are required to have further improved magnetic properties, heat resistance, and corrosion resistance.

[0003] R-T-B permanent magnets dissolve a raw material alloy and pulverize, mold, sinter, heat-treat the obtained ingot.
It is manufactured by processing. For the pulverization, wet pulverization using a ball mill or the like is possible, but jet mill pulverization using an inert high-pressure gas is generally used. Since the fine powder obtained in this manner is extremely active, a method of mixing a small amount of oxygen into a pulverized gas stream of a jet mill for stabilization or collecting the fine powder in mineral oil or the like has been adopted. Molding performed in a magnetic field employs both dry molding and wet molding. The sintering is performed in a temperature range of 1000 ° C. to 1150 ° C. in a vacuum or in an inert gas, and the obtained sintered body is generally subjected to one or more heat treatments at an appropriate temperature. is there.

[0004] RTB-based permanent magnets are initially corrosion resistant,
There was a problem that heat resistance was low,
It has been significantly improved by the development of coating techniques such as plating. Improving the corrosion resistance of the magnet material itself is also extremely important for improving the reliability after coating.
Various additional elements have been studied. Elements such as Co and Dy are generally used as these additional elements. Co raises Curie temperature, improves temperature characteristics,
The corrosion resistance is improved by making the R-rich phase an R ₃ Co intermetallic compound. Dy improves the coercive force by increasing the anisotropic magnetic field _HA of the main phase. Further, Cu,
Trace addition elements such as Ga and Al are also used. C
u increases the optimum heat treatment range and contributes to the improvement of the coercive force by co-addition with Co.
3). Further, the addition of Cu changes the grain boundary phase to R-Co-Cu.
It is known that it becomes an intermetallic compound and the corrosion resistance is further increased as compared with the case where only Co is added. It is known that additional elements such as Ga and Al are also effective in improving the coercive force.

As a method of adding Co, Dy, Cu, etc.,
A so-called one-alloy method, which is added at the melting stage of the raw material alloy,
A two-alloy method (mixing method) in which an alloy having a predetermined composition is mixed after coarse pulverization or fine pulverization is used. In the two-alloy method, for the purpose of preventing powder oxidation, elements that contribute to corrosion resistance, such as Co and Dy, are added to the R-rich alloy, and in particular, the R-rich alloy is made into an intermetallic compound having a specific crystal structure. Has been shown to increase the oxidation resistance of the alloy powder
(Japanese Unexamined Patent Publication (Kokai) Nos. 5-182813-182816). Further, there is disclosed a method of adding elements such as Cu, Al, and Ga, which contribute to the improvement of coercive force, to the R-rich alloy side, with the intention of concentrating the elements in the grain boundary phase.

[0006]

The addition of Co, Dy, Cu, etc. is effective in improving the corrosion resistance and heat resistance. However, when using the one-alloy method, adding Co and Cu results in a high residual magnetic flux density. In the composition range where the required Dy is small,
Grain growth tends to occur during sintering, and a large number of coarse crystal grains tend to appear. As a result, there is a problem that the grain size distribution of the main phase crystal grains of the sintered body is widened, and the coercive force and the squareness are likely to be reduced. Further, the two-alloy method is a very attractive method from the viewpoint of high performance. However, if this method is to be implemented on a mass production scale, the following problems are raised. That is,
Main phase alloy with low rare earth content and so-called R rich in rare earth
It is necessary to prepare a rich alloy, and a drastic change of the raw material alloy system is required. Further, since the main phase alloy and the R-rich alloy have different hydrogen storage properties, it is necessary to change the coarse pulverization conditions. In the case of mixing after pulverization, not only must each pulverization condition be separately optimized, but also the process becomes complicated.

According to the present invention, in the method of adding Co, Cu, Dy, etc., a conventional rare earth material alloy can be fully utilized without any change, and coarse crystal grains are generated during sintering and the coercive force is reduced. It is an object of the present invention to provide an alloy powder for an RTB-based permanent magnet and a method for producing an RTB-based permanent magnet, which can achieve high magnetic properties without inducing.

[0008]

Means for Solving the Problems The present invention has the following features in order to solve the above-mentioned problems. The following (1) to (6) are the cases where the amount of boron B added to the second alloy is made substantially zero by utilizing the combined effect of Ga and Al. The following (7) to (12) use the combined addition effect of Ga and Al to increase the boron B addition amount of the second alloy to 0.8 m.
less than ass%. In addition, the following (13)-
(18) is the case where Al is solely added to make the amount of boron B added to the second alloy substantially zero. The following (19)-
(24) is a case in which Al is solely added, and the amount of boron B added to the second alloy is less than 0.8 mass%. (1) R (at least one or more rare earth elements including Y)
29-33 mass%, boron B 0.8-1.2 mass
%, Ga and Al are added in combination to form Ga 0.01 to 0.5.
An alloy consisting of mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) is 29 to 33 mass%.
Ga and Al are added in combination to make Ga 0.01 to 0.5 ma.
ss% and Al 0.01 to 2.0 mass%, balance Fe
A rare earth alloy powder characterized in that an alloy composed of (a part of Fe is replaced by Co and Cu) is used as a second alloy, and the first alloy powder and the second alloy powder are mixed in a predetermined composition. . (2) The weight ratio of Cu to Co is Cu / Co = 0.02
0.2, wherein the rare earth alloy powder is (1). (3) Two or more kinds of the first alloy powder of the first alloy coarse powder having a different content of heavy rare earth and the first alloy coarse powder having a different boron B content, and the second alloy powder have a predetermined composition. The rare earth alloy powder according to (1), wherein the powder is mixed. (4) R (at least one or more rare earth elements including Y)
29-33 mass%, boron B 0.8-1.2 mass
%, Ga and Al are added in combination to form Ga 0.01 to 0.5.
An alloy consisting of mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) is 29 to 33 mass%.
Ga and Al are added in combination to make Ga 0.01 to 0.5 ma.
ss% and Al 0.01 to 2.0 mass%, balance Fe
An alloy composed of (a part of Fe replaced by Co and Cu) is used as a second alloy, and a rare earth alloy powder in which the first alloy powder and the second alloy powder are mixed in a predetermined composition is molded in a magnetic field, A method for producing a rare earth permanent magnet, characterized by sintering. (5) R (at least one or more rare earth elements including Y)
29-33 mass%, boron B 0.8-1.2 mass
%, Ga and Al are added in combination to form Ga 0.01 to 0.5.
An alloy consisting of mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) is 29 to 33 mass%.
Ga and Al are added in combination to make Ga 0.01 to 0.5 ma.
ss% and Al 0.01 to 2.0 mass%, balance Fe
(A part of Fe is replaced by Co and Cu, and the weight ratio of Cu to Co is Cu / Co = 0.02 to 0.2) is used as a second alloy, and a first alloy powder and a second alloy powder are used. Is a method for producing a rare earth permanent magnet, which comprises molding a rare earth alloy powder mixed with a predetermined composition in a magnetic field, and then sintering. (6) R (at least one or more rare earth elements including Y)
29-33 mass%, boron B 0.8-1.2 mass
%, Ga and Al are added in combination to form Ga 0.01 to 0.5.
mass%, Al 0.01 to 2.0 mass%, and the balance of Fe, wherein the first alloy coarse powder having a different content of heavy rare earths among the R and the first alloy coarse powder having a different boron B content. R (at least one or more rare earth elements including Y) 2
9-33 mass%, Ga and Al are added in combination
0.01-0.5 mass% and Al 0.01-2.0
An alloy consisting of a mass% and a balance of Fe (Fe is partially replaced by Co and Cu) is used as a second alloy, and a rare earth alloy powder in which the first alloy powder and the second alloy powder are mixed to a predetermined composition is subjected to a magnetic field. And then sintering the rare-earth permanent magnet. (7) R (at least one or more rare earth elements including Y)
29-33 mass%, boron B 0.8-1.2 mass
%, Ga and Al are added in combination to form Ga 0.01 to 0.5.
An alloy consisting of mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) is 29 to 33 mass%.
Boron B less than 0.8 mass%, Ga and Al are added in combination to form Ga 0.01 to 0.5 mass% and Al0.01
-2.0 mass%, an alloy consisting of the balance Fe (a part of which is replaced by Co and Cu) is defined as a second alloy, and the first alloy powder and the second alloy powder are mixed in a predetermined composition. It is a rare earth alloy powder characterized. (8) The weight ratio of Cu and Co is Cu / Co = 0.02
The rare earth alloy powder according to (7), which is 0.2. (9) Two or more kinds of the first alloy powder of the first alloy coarse powder different in the content of heavy rare earth and the first alloy coarse powder different in the boron B content of the R, and the second alloy powder have a predetermined composition. The rare earth alloy powder according to (7), wherein the powder is mixed. (10) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
ss%, Ga and Al are added in combination of Ga 0.01 to
0.5 mass% and Al 0.01 to 2.0 mass%
And an alloy consisting of the balance Fe as the first alloy, and R (at least one or more rare earth elements including Y) 29 to 33 mas
s%, boron B less than 0.8 mass%, Ga and Al are added in a combined manner to obtain Ga 0.01 to 0.5 mass% and Al
An alloy consisting of 0.01 to 2.0 mass% and the balance Fe (a part of which is replaced by Co and Cu) is made of a second alloy.
A method for producing a rare earth permanent magnet, comprising forming an alloy, a rare earth alloy powder in which a first alloy powder and a second alloy powder are mixed in a predetermined composition in a magnetic field, and then sintering. (11) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
ss%, Ga and Al are added in combination of Ga 0.01 to
0.5 mass% and Al 0.01 to 2.0 mass%
And an alloy consisting of the balance Fe as the first alloy, and R (at least one or more rare earth elements including Y) 29 to 33 mas
s%, boron B less than 0.8 mass%, Ga and Al are added in a combined manner to obtain Ga 0.01 to 0.5 mass% and Al
0.01 to 2.0 mass%, the balance Fe (part of Fe is replaced by Co and Cu, and the weight ratio of Cu to Co is Cu
/Co=0.02 to 0.2) is a second alloy, and a rare earth alloy powder in which the first alloy powder and the second alloy powder are mixed in a predetermined composition is molded in a magnetic field, and then sintered. A method for producing a rare earth permanent magnet, characterized in that: (12) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
ss%, Ga and Al are added in combination of Ga 0.01 to
0.5 mass% and Al 0.01 to 2.0 mass%
And at least two types of first alloy powder of the first alloy coarse powder having a different content of heavy rare earth and the first alloy coarse powder having a different boron B content in the first alloy. An alloy, R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 mass%
Less than, Ga and Al are added in a combined amount of 0.01 to 0.1 Ga.
5 mass% and Al 0.01 to 2.0 mass%,
An alloy consisting of the balance Fe (a part of which was replaced by Co and Cu) was used as a second alloy, and the first alloy powder and the second alloy were mixed together.
A method for producing a rare earth permanent magnet, comprising forming a rare earth alloy powder in which an alloy powder is mixed in a predetermined composition in a magnetic field, and then sintering. (13) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
An alloy consisting of ss%, 0.01 to 2.0 mass% of Al and the balance of Fe is used as a first alloy, and 29 to 33 mass% of R (at least one or more rare earth elements including Y) is used.
01-2.0 mass%, the balance Fe (part of Fe is Co
And a Cu-substituted alloy) as a second alloy, wherein the first alloy powder and the second alloy powder are mixed in a predetermined composition. (14) The weight ratio of Cu and Co is Cu / Co = 0.02
The rare earth alloy powder according to (13), which is 0.2. (15) Two or more kinds of the first alloy powder of the first alloy coarse powder having a different content of heavy rare earth and the first alloy coarse powder having a different boron B content of the R, and the second alloy powder have a predetermined composition. (13) The rare earth alloy powder according to (13), wherein (16) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
An alloy consisting of ss%, 0.01 to 2.0 mass% of Al and the balance of Fe is used as a first alloy, and 29 to 33 mass% of R (at least one or more rare earth elements including Y) is used.
01-2.0 mass%, the balance Fe (part of Fe is Co
And a Cu-substituted Cu) as a second alloy, a rare earth alloy powder in which the first alloy powder and the second alloy powder are mixed in a predetermined composition is molded in a magnetic field, and then sintered. This is a method for producing a rare earth permanent magnet. (17) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
An alloy consisting of ss%, 0.01 to 2.0 mass% of Al and the balance of Fe is used as a first alloy, and 29 to 33 mass% of R (at least one or more rare earth elements including Y) is used.
01-2.0 mass%, the balance Fe (part of Fe is Co
And Cu, the weight ratio of Cu and Co is Cu / Co
= 0.02 to 0.2) as a second alloy, forming a rare earth alloy powder in which the first alloy powder and the second alloy powder are mixed in a predetermined composition in a magnetic field, and then sintering. This is a method for producing a rare earth permanent magnet. (18) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
An alloy comprising ss%, Al 0.01 to 2.0 mass%, and the balance Fe, wherein the first alloy coarse powder having a different content of heavy rare earths among the R and the first alloy coarse powder having a different boron B content. Two or more of the first alloy powders are defined as a first alloy, and R
(At least one or more rare earth elements including Y) 29 to 3
An alloy consisting of 3 mass%, Al 0.01 to 2.0 mass%, and the balance Fe (a part of Fe is replaced by Co and Cu) is used as a second alloy, and the first alloy powder and the second alloy powder have a predetermined composition. A method for producing a rare earth permanent magnet, comprising forming a mixed rare earth alloy powder in a magnetic field and then sintering. (19) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
An alloy consisting of ss%, Al 0.01 to 2.0 mass% and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B
Less than 0.8 mass%, Al 0.01-2.0 mass
%, The balance being Fe (a part of Fe being replaced by Co and Cu) is used as a second alloy, and the first alloy powder and the second alloy powder are mixed in a predetermined composition. It is an alloy powder. (20) The weight ratio of Cu and Co is Cu / Co = 0.02
The rare earth alloy powder according to (19), which is 0.2. (21) Two or more of the first alloy powder of the first alloy coarse powder having a different content of heavy rare earth and the first alloy coarse powder having a different boron B content in the R, and the second alloy powder have a predetermined composition. (19) is the rare earth alloy powder described in (19). (22) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
An alloy consisting of ss%, Al 0.01 to 2.0 mass% and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B
Less than 0.8 mass%, Al 0.01-2.0 mass
%, And a balance of Fe (a part of Fe is replaced by Co and Cu) is used as a second alloy, and a rare earth alloy powder in which the first alloy powder and the second alloy powder are mixed in a predetermined composition is applied in a magnetic field. A method for producing a rare earth permanent magnet, which comprises forming and then sintering. (23) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
An alloy consisting of ss%, Al 0.01 to 2.0 mass% and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B
Less than 0.8 mass%, Al 0.01-2.0 mass
%, The balance Fe (a part of Fe is replaced by Co and Cu,
(The weight ratio of Cu and Co is Cu / Co = 0.02 to 0.2)
A rare earth alloy powder obtained by mixing a first alloy powder and a second alloy powder in a predetermined composition in a magnetic field, and then sintering the rare earth alloy powder. It is. (24) R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.2 ma
an alloy consisting of ss%, Al 0.01 to 2.0 mass%, and the balance of Fe, wherein the first alloy coarse powder having a different content of heavy rare earth in the R and the first alloy coarse powder having a different boron B content. Two or more of the first alloy powders are defined as a first alloy, and R
(At least one or more rare earth elements including Y) 29 to 3
3 mass%, boron B less than 0.8 mass%, Al
An alloy consisting of 0.01 to 2.0 mass% and the balance Fe (a part of Fe was replaced with Co and Cu) was used as a second alloy, and the first alloy powder and the second alloy powder were mixed to a predetermined composition. This is a method for producing a rare earth permanent magnet, which comprises molding a rare earth alloy powder in a magnetic field and then sintering.

(Operation) The present invention solves the above-mentioned problems by using Co, Cu, Dy, B
As a result of studying the method of addition and the amount of rare earth, Co, Cu
The first alloy is a conventional alloy having a rare earth content that does not contain a second alloy, which has a rare earth content that is basically equal to that of the first alloy and contains substantially no B or is less than the first alloy. By adding a specific ratio of Co and Cu to the mixture, finely pulverizing and sintering these alloy coarse powders, so that the conventional rare earth material alloy can be fully utilized without any change, and the coarseness during sintering can be increased Without causing the generation of crystal grains and a decrease in coercive force,
It has been found that improvement in corrosion resistance and heat resistance and high magnetic properties can be achieved. Further, Dy,
It has been found that the method of mixing a plurality of alloy coarse powders having different compositions such as B with the second alloy makes it possible to easily adjust the components only by changing the mixing ratio.

That is, the present invention relates to a method for producing R (at least one or more rare earth elements including Y) of 29 to 33 mass%,
0.8-1.2 mass%, Al 0.01-2.0 ma
An alloy consisting of ss%, the balance of Fe and unavoidable impurities was defined as a first alloy, and the amount of R substantially equal to that of the first alloy, B0.8
less than mass%, Al 0.01 to 2.0 mass%, balance Fe (Fe is partially substituted with Co and Cu)
And an alloy consisting of unavoidable impurities as a second alloy,
R in which the alloy powder and the second alloy powder are mixed in a predetermined composition
-It is a TB alloy powder. Further, R (at least one or more rare earth elements including Y) 29 to 33 mass%, B
0.8-1.2 mass%, Al 0.01-2.0 ma
An alloy consisting of ss%, Ga 0.01 to 0.5 mass%, balance Fe and unavoidable impurities is defined as a first alloy, and the R amount is substantially equal to the first alloy, B is less than 0.8 mass%, A
l0.01-2.0 mass%, Ga0.01-0.5
The alloy consisting of mass%, the balance Fe (a part of Fe was replaced by Co and Cu), and unavoidable impurities
The alloy is an RTB-based alloy powder in which a first alloy powder and a second alloy powder are mixed in a predetermined composition. Also, Cu
And the weight ratio of Co to Cu / Co = 0.02 to 0.2. Further, it is an RTB-based alloy powder in which two or more first alloy powders having different heavy rare earth contents and a second alloy powder are mixed in a predetermined composition. Further, these RTB-based alloy powders are molded in a magnetic field,
This is a method for producing an RTB-based permanent magnet that is then sintered.

[0011]

BEST MODE FOR CARRYING OUT THE INVENTION In the present invention, R includes Y
Nd, Pr, Dy with at least one rare earth element
Is preferred. Nd and Dy alone may be used, but a mixture of Nd and Pr
A compound may be used instead of Nd. First pass to be the subject
If the R of gold is less than 29 mass%, the liquid phase is insufficient.
Sintering failure, residual flux above 33 mass%
Since the density is reduced, the addition amount is 29 mass% to 33 m
ass%. B of the first alloy is less than 0.8 mass%
Then R₂T ₁₇Due to the appearance of the phase, the coercive force suddenly decreases,
If it exceeds 1.2 mass%, a B-rich phase which is a non-magnetic phase
Becomes too large, and the residual magnetic flux density decreases.
0.8 to 1.2 mass%. Al and Al
When Al and Ga are added, the amount of Al and Ga is Al0.
01-2.0 mass%, Ga 0.01-0.5mass
s%. Al shows an effect of improving coercive force, but 0.0
If it is less than 1 mass%, the effect is not sufficient and 2.0 m
When it exceeds ass%, the decrease in residual magnetic flux density is greatly preferred.
I don't. Similarly, the coercive force of Ga is improved by its addition.
However, if less than 0.01 mass%, the effect is not
It is sufficient, and when it exceeds 0.5 mass%, the coercive force is improved.
The effect is saturated and the residual magnetic flux density decreases. Departure
In the light, Ga and Al are more effective when added in combination.
is there.

The R of the second alloy is basically equal to that of the first alloy, but may be slightly shifted due to alloy procurement or lot variation. The composition range is the same as that of the first alloy and R29
３３33 mass%. The B content of the second alloy is 0.8 ma
If it is ss% or more, the effect of suppressing the generation of coarse particles is reduced, and the coercive force is reduced and the squareness is deteriorated. Therefore, although it is less than 0.8 mass%, B is preferably not added. Although Ga and Al of the second alloy are basically equal to those of the first alloy, they may be slightly shifted due to the procurement of the alloy or variations in lots. When Al or Al, Ga is added, the composition range is the same as that of the first alloy and Al0.01.
~ 2.0 mass%, Ga0.01 ~ 0.5 mass%
And In the present invention, it is more effective to add Ga and Al in combination. The addition amounts of Co and Cu in the second alloy are not particularly limited, and can be set based on the relationship between the addition amount and the mixing ratio in the final composition.
Can be set according to the purpose. On the other hand, the second
The compounding ratio of the alloys is as follows: first alloy: second alloy = 99: 1 to 7
0:30 is preferable, but this is not particularly limited.

The weight ratio of Cu and Co is such that Cu / Co is 0.0
If it is less than 2, the effect of expanding the heat treatment temperature range is small,
If it exceeds 0.2, the residual magnetic flux density and the squareness are reduced in a very common composition of about 2 mass% of Co. Therefore, Cu / Co is set to 0.02 to 0.2.

The first alloy coarse powder in the present invention is not limited to a single composition. That is, a first alloy coarse powder having a different amount of heavy rare earths such as Dy and Tb, a first alloy coarse powder having a different B amount, and a second alloy coarse powder to which Co and Cu are added are added to these two or more types. You may mix and mix. In this case, Dy
And B can be easily adjusted only by changing the compounding ratio.

[0015]

DESCRIPTION OF THE PREFERRED EMBODIMENTS Hereinafter, specific embodiments of the present invention will be shown, and the contents of the present invention will be described in detail. (Example 1) Nd25.3mass%, Pr7.0mass
s%, B 1.0 mass%, Al 0.07 mass%,
An alloy consisting of the balance Fe was cast by a strip casting method. This alloy is placed in a processing vessel and is placed in a vacuum at 1000 ° C.
After a heat treatment of × 2 h, the mixture was crushed by a hydrogen storage method to obtain a raw material coarse powder (described in Table 1, alloy A). In addition, Nd18.
6 mass%, Pr5.2 mass%, Dy8.5 ma
ss%, Co20 mass%, Cu1 mass%, Al
An alloy consisting of 0.07 mass% and the balance of Fe was similarly used as a raw material coarse powder (described in Table 1, alloy I). These two kinds of alloy coarse powders are alloy A 90 mass%, alloy I 10 mass%
In a V-type mixer, and mixed for 15 minutes. This mixed coarse powder was pulverized by a jet mill using a nitrogen high-pressure gas so as to have an average particle size of 4.7 μm. While orienting the obtained mixed fine powder in a magnetic field of 0.6 MA / m, 1.
It was molded at a pressure of 0 Ton / cm ² . The obtained molded body is heated at 1060 ° C., 1080 ° C., or 110 ° C. in vacuum.
Sintering was performed at 0 ° C. × 2 hours. Next, these sintered bodies were subjected to a heat treatment at 900 ° C. × 1 hour in an Ar atmosphere, and further subjected to a heat treatment at 480 ° C. × 1 hour. After observing the appearance of the sintered body, the magnetic properties were measured. Table 1 shows the magnetic properties, the sintering temperature, and the results of the appearance observation when the squareness is the highest. Good values were obtained for the magnetic properties. At this time, the sintering temperature was 1100 ° C., and no coarse particles were observed.

(Comparative Example 1) N, which is the final composition of this example,
d24.6 mass%, Pr 6.85 mass%, Dy
0.85 mass%, B0.9 mass%, Co2ma
ss%, Cu 0.1 mass%, Al 0.07 mass
% And the balance of Fe was cast by a strip casting method, and pulverized, sintered and heat-treated in the same manner as in Example 1. After observing the appearance of the obtained sintered body, the magnetic properties were measured, and the results of the magnetic properties, sintering temperature and appearance observation when the squareness was the highest are shown in Table 1. 1060 ° C, 1080
The optimum sintering temperature was 1,080 ° C. out of 1,100 ° C., but Hcj was lower than that of Example 1, and coarse grains were observed. Also, the sample at 1060 ° C. was clearly insufficiently sintered.

(Comparative Example 2) Using the alloys R and S shown in Table 1, coarse pulverization was performed in the same manner as in Example 1, and after mixing to obtain the final composition, fine pulverization, sintering and heat treatment were performed. Where C
o and Cu were uniformly added to both alloys, and Dy was added to alloy S. After observing the appearance of the obtained sintered body, the magnetic properties were measured, and the results of the magnetic properties, sintering temperature and appearance observation when the squareness was the highest are shown in Table 1. Hcj was lower than in Example 1, and coarse particles were observed.

(Comparative Example 3) Using the alloys C and Q shown in Table 1, coarsely pulverized in the same manner as in Example 1, mixed to obtain a final composition, then finely pulverized, sintered and heat-treated. Where D
y, Co and Cu were added to the alloy Q, and B was uniformly added to both alloys. After observing the appearance of the obtained sintered body, the magnetic properties were measured, and the results of the magnetic properties, sintering temperature and appearance observation when the squareness was the highest are shown in Table 1. Hcj is Example 1
Lower than that of Comparative Examples 1 and 2, and coarse grains were observed.

Example 2 Alloy A and alloy K shown in Table 1
And finely pulverized, sintered and heat-treated after mixing to obtain the final composition. here,
Dy, Co, Cu are added to alloy K and B is 0.4 mass
%. Alloy K is the second alloy of the present invention. After observing the appearance of the obtained sintered body, the magnetic properties were measured, and the results of the magnetic properties, sintering temperature and appearance observation when the squareness was the highest are shown in Table 1. Good magnetic properties were obtained as in Example 1. At this time, the sintering temperature was 1100 ° C., and no coarse particles were observed.

Example 3 Alloy A and Alloy L shown in Table 1
And finely pulverized, sintered and heat-treated after mixing to obtain the final composition. here,
Dy, Co, Cu are added to alloy L and B is 0.7 mass
%. Alloy L is the second alloy of the present invention. After observing the appearance of the obtained sintered body, the magnetic properties were measured, and the results of the magnetic properties, sintering temperature and appearance observation when the squareness was the highest are shown in Table 1. Good magnetic properties were obtained as in Example 1. At this time, the sintering temperature was 1100 ° C., and no coarse particles were observed.

Example 4 Using the alloys B, C, and I shown in Table 1, coarsely pulverized in the same manner as in Example 1, mixed to obtain a final composition, finely pulverized, sintered and heat-treated. Done. Here, Dy, Co, and Cu were added to the alloy I and B was not added. Alloy I is the second alloy of the present invention. After observing the appearance of the obtained sintered body, the magnetic properties were measured, and the results of the magnetic properties, sintering temperature and appearance observation when the squareness was the highest are shown in Table 1. Good magnetic properties were obtained as in Example 1. At this time, the sintering temperature was 1100 ° C., and no coarse particles were observed.

(Example 5) Using the alloys B, C, D and J shown in Table 1, coarsely pulverized in the same manner as in Example 1, mixed to a final composition, finely pulverized and sintered. And heat treatment. Here, Co and Cu were added to the alloy J and B was not added. Alloy J is the second alloy of the present invention. Dy was added in alloy D, which is one of the first alloys of the present invention. After observing the appearance of the obtained sintered body, the magnetic properties were measured, and the results of the magnetic properties, sintering temperature and appearance observation when the squareness was the highest are shown in Table 1. Good magnetic properties were obtained as in Example 1. At this time, the sintering temperature was 1100 ° C., and no coarse particles were observed.

Comparative Example 4 The alloy T and the alloy U shown in Table 1 were roughly pulverized in the same manner as in Example 1, mixed to obtain a final composition, then finely pulverized, sintered and heat-treated. Where D
y, Co, and Cu were added to the R-rich alloy U, and B was not added. Alloy U is not the second alloy of the present invention. After observing the appearance of the obtained sintered body, the magnetic properties were measured, and the results of the magnetic properties, sintering temperature and appearance observation when the squareness was the highest are shown in Table 1. Good magnetic properties were obtained as in Example 1. At this time, the sintering temperature was 1100 ° C., and no coarse particles were observed. From these results, Examples 1 to
The magnetic properties obtained in Example 5 are based on the conventional two alloy method (Comparative Example 4)
It turns out that it is equivalent to.

(Examples 6 to 10 and Comparative Examples 5 to 8) In the compositions of the first alloys A to D, the second alloys I to L, and the comparative alloys P to U, alloys containing 0.1 mass% of Ga were used. It was newly manufactured, and was referred to as first alloys A ′ to D ′, second alloys I ′ to L ′, and comparative alloys P ′ to U ′. Examples 1 to 5, Comparative Examples 1 to
A sintered body was prepared in the same manner as in Example 4, and after observing the appearance of the sintered body, the magnetic properties were measured. Table 2 shows the results of the magnetic properties, sintering temperatures and appearance observations in the case of the highest squareness. The optimum sintering temperature and the appearance of coarse grains are the same as those in Table 1, but it can be confirmed that the level of Hcj is improved by about 0.2 MA / m. The composite addition effect of Ga is obtained.

[0025]

[Table 1]

[0026]

[Table 2]

[0027]

According to the present invention, in the method of adding Co, Cu, Dy, etc., the conventional rare earth material alloy can be fully utilized without any change, and coarse crystal grains are generated during sintering. In addition, high magnetic properties can be achieved without lowering the coercive force.

──────────────────────────────────────────────────続 き Continued on the front page (51) Int.Cl. ⁷ Identification symbol FI Theme coat ゛ (Reference) H01F 1/06 H01F 41/02 G 1/08 1/04 H 41/02 1/06 A

Claims (24)

[Claims] 1. The method according to claim 1, wherein at least one of the rare earth elements including R (Y
29-33 mass%, boron B 0.8-1.2
mass%, Ga and Al are added in combination to obtain Ga0.01.
0.5 mass% and Al 0.01 to 2.0 mass
%, The alloy consisting of the balance Fe being the first alloy, and R (at least one or more rare earth elements including Y)
33 mass%, Ga and Al are added in combination to obtain Ga 0.
01-0.5 mass% and Al 0.01-2.0 ma
An alloy consisting of ss% and the balance Fe (a part of Fe is replaced by Co and Cu) is used as a second alloy, and the first alloy powder and the second alloy powder are mixed in a predetermined composition. Rare earth alloy powder. 2. The weight ratio between Cu and Co is Cu / Co = 0.
2. The rare earth alloy powder according to claim 1, wherein the ratio is from 02 to 0.2. 3. A method according to claim 1, wherein the first and second alloy powders include a first alloy coarse powder having a different content of heavy rare earth elements and a first alloy coarse powder having a different boron B content. The rare earth alloy powder according to claim 1, wherein the rare earth alloy powder is mixed in a predetermined composition. 4. The method of claim 1, wherein at least one of the rare earth elements including R (Y
29-33 mass%, boron B 0.8-1.2
mass%, Ga and Al are added in combination to obtain Ga0.01.
0.5 mass% and Al 0.01 to 2.0 mass
%, The alloy consisting of the balance Fe being the first alloy, and R (at least one or more rare earth elements including Y)
33 mass%, Ga and Al are added in combination to obtain Ga 0.
01-0.5 mass% and Al 0.01-2.0 ma
An alloy consisting of ss% and the balance Fe (a part of Fe is replaced by Co and Cu) is used as a second alloy, and a rare earth alloy powder in which a first alloy powder and a second alloy powder are mixed in a predetermined composition is subjected to a magnetic field. And then sintering the rare earth permanent magnet. 5. At least one of R (Y-containing rare earth elements)
29-33 mass%, boron B 0.8-1.2
mass%, Ga and Al are added in combination to obtain Ga0.01.
0.5 mass% and Al 0.01 to 2.0 mass
%, The alloy consisting of the balance Fe being the first alloy, and R (at least one or more rare earth elements including Y)
33 mass%, Ga and Al are added in combination to obtain Ga 0.
01-0.5 mass% and Al 0.01-2.0 ma
ss%, balance Fe (part of Fe is replaced by Co and Cu, and the weight ratio of Cu to Co is Cu / Co = 0.
The alloy consisting of 2) is a second alloy, and the first alloy powder and the second alloy
A method for producing a rare earth permanent magnet, comprising forming a rare earth alloy powder in which an alloy powder is mixed in a predetermined composition in a magnetic field, and then sintering. 6. At least one of R (Y) -containing rare earth elements
29-33 mass%, boron B 0.8-1.2
mass%, Ga and Al are added in combination to obtain Ga0.01.
0.5 mass% and Al 0.01 to 2.0 mass
%, The balance being Fe, wherein two or more of the first alloy powder of the first alloy coarse powder having a different content of heavy rare earth and the first alloy coarse powder having a different boron B content in the R are used as the first alloy powder. 1
R (at least one or more rare earth elements including Y)
33 mass%, Ga and Al are added in combination to obtain Ga 0.
01-0.5 mass% and Al 0.01-2.0 ma
An alloy consisting of ss% and the balance Fe (a part of Fe is replaced by Co and Cu) is used as a second alloy, and a rare earth alloy powder in which a first alloy powder and a second alloy powder are mixed in a predetermined composition is subjected to a magnetic field. And then sintering the rare earth permanent magnet. 7. At least one of R (Y-containing rare earth elements)
29-33 mass%, boron B 0.8-1.2
mass%, Ga and Al are added in combination to obtain Ga0.01.
0.5 mass% and Al 0.01 to 2.0 mass
%, The alloy consisting of the balance Fe being the first alloy, and R (at least one or more rare earth elements including Y)
33 mass%, boron B less than 0.8 mass%, Ga
And Al are added in combination to make Ga 0.01 to 0.5 mass%.
And Al 0.01 to 2.0 mass%, and the balance Fe (F
a rare earth alloy powder characterized in that an alloy consisting of a part of e with Co and Cu) is used as a second alloy, and the first alloy powder and the second alloy powder are mixed in a predetermined composition. 8. When the weight ratio of Cu and Co is Cu / Co = 0.
The rare earth alloy powder according to claim 7, wherein the ratio is from 02 to 0.2. 9. Two or more of first alloy powders of the first alloy coarse powder having a different content of heavy rare earths in R, and first alloy coarse powders having a different boron B content, and a second alloy powder, The rare earth alloy powder according to claim 7, which is mixed to a predetermined composition. 10. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
2 mass%, Ga and Al are combined and Ga0.0
1-0.5 mass% and Al 0.01-2.0mass
s%, the alloy consisting of the balance Fe as the first alloy, and R (at least one or more rare earth elements including Y)
33 mass%, boron B less than 0.8 mass%, Ga
And Al are added in combination to make Ga 0.01 to 0.5 mass%.
And Al 0.01 to 2.0 mass%, and the balance Fe (F
e is replaced with Co and Cu) as a second alloy, and a rare earth alloy powder in which the first alloy powder and the second alloy powder are mixed in a predetermined composition is molded in a magnetic field. A method for producing a rare earth permanent magnet, comprising: 11. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
2 mass%, Ga and Al are combined and Ga0.0
1-0.5 mass% and Al 0.01-2.0mass
s%, the alloy consisting of the balance Fe as the first alloy, and R (at least one or more rare earth elements including Y)
33 mass%, boron B less than 0.8 mass%, Ga
And Al are added in combination to make Ga 0.01 to 0.5 mass%.
And Al 0.01 to 2.0 mass%, and the balance Fe (F
e is replaced with Co and Cu, and an alloy consisting of Cu and Co at a weight ratio of Cu / Co = 0.02 to 0.2) is defined as a second alloy, and the first alloy powder and the second alloy powder are A method of manufacturing a rare earth permanent magnet, comprising: forming a rare earth alloy powder mixed in a predetermined composition in a magnetic field, and then sintering the powder. 12. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
2 mass%, Ga and Al are combined and Ga0.0
1-0.5 mass% and Al 0.01-2.0mass
s%, the balance being Fe, the first alloy coarse powder having a different content of heavy rare earths among the R, and boron B
R (at least one or more rare earth elements including Y) 29-
33 mass%, boron B less than 0.8 mass%, Ga
And Al are added in combination to make Ga 0.01 to 0.5 mass%.
And Al 0.01 to 2.0 mass%, and the balance Fe (F
e is replaced with Co and Cu) as a second alloy, and a rare earth alloy powder in which the first alloy powder and the second alloy powder are mixed in a predetermined composition is molded in a magnetic field. A method for producing a rare earth permanent magnet, comprising: 13. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
An alloy consisting of 2 mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 29 to
33 mass%, Al 0.01 to 2.0 mass%, balance Fe (Fe is partially substituted with Co and Cu)
A rare earth alloy powder characterized in that an alloy consisting of: is a second alloy, wherein the first alloy powder and the second alloy powder are mixed in a predetermined composition. 14. The weight ratio of Cu and Co is Cu / Co =
14. The rare earth alloy powder according to claim 13, wherein the ratio is 0.02 to 0.2. 15. The first alloy powder of the first alloy coarse powder having a different content of heavy rare earth in the R and the first alloy powder of the first alloy coarse powder having a different boron B content, and the second alloy powder, 14. The rare earth alloy powder according to claim 13, which is mixed to a predetermined composition. 16. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
An alloy consisting of 2 mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 29 to
33 mass%, Al 0.01 to 2.0 mass%, balance Fe (Fe is partially substituted with Co and Cu)
A rare earth alloy powder in which a first alloy powder and a second alloy powder are mixed in a predetermined composition in a magnetic field, and then sintering the rare earth alloy powder, the method comprising: . 17. R (at least one kind of rare earth element including Y) 29 to 33 mass%, boron B 0.8 to 1.
An alloy consisting of 2 mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 29 to
An alloy consisting of 33 mass%, Al 0.01 to 2.0 mass%, and the balance Fe (a part of Fe is replaced by Co and Cu, and the weight ratio of Cu to Co is Cu / Co = 0.02 to 0.2) A method for producing a rare earth permanent magnet, comprising forming a rare earth alloy powder in which a first alloy powder and a second alloy powder are mixed in a predetermined composition as a second alloy in a magnetic field, and then sintering the rare earth alloy powder. 18. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
An alloy consisting of 2 mass%, Al 0.01 to 2.0 mass%, and the balance being Fe, wherein the first alloy coarse powder having a different content of heavy rare earth in the R and the first alloy coarse powder having a different boron B content. R (at least one or more rare earth elements including Y) 29-
33 mass%, Al 0.01 to 2.0 mass%, balance Fe (Fe is partially substituted with Co and Cu)
A rare earth alloy powder in which a first alloy powder and a second alloy powder are mixed in a predetermined composition in a magnetic field, and then sintering the rare earth alloy powder, the method comprising: . 19. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
An alloy consisting of 2 mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 29 to
33 mass%, boron B less than 0.8 mass%, Al
An alloy composed of 0.01 to 2.0 mass% and the balance Fe (a part of Fe is replaced by Co and Cu) is used as a second alloy, and the first alloy powder and the second alloy powder are mixed in a predetermined composition. Rare earth alloy powder. 20. The weight ratio of Cu and Co is Cu / Co =
20. The rare earth alloy powder according to claim 19, wherein the value is 0.02 to 0.2. 21. Two or more of the first alloy powder of the first alloy coarse powder having a different content of heavy rare earths in the R and the first alloy coarse powder having a different boron B content, and the second alloy powder, The rare earth alloy powder according to claim 19, wherein the rare earth alloy powder is mixed with a predetermined composition. 22. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
An alloy consisting of 2 mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 29 to
33 mass%, boron B less than 0.8 mass%, Al
An alloy consisting of 0.01 to 2.0 mass% and the balance Fe (a part of Fe was replaced by Co and Cu) was used as a second alloy, and the first alloy powder and the second alloy powder were mixed in a predetermined composition. A method for producing a rare earth permanent magnet, comprising forming a rare earth alloy powder in a magnetic field and then sintering the rare earth alloy powder. 23. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
An alloy consisting of 2 mass%, Al 0.01 to 2.0 mass%, and the balance Fe is used as a first alloy, and R (at least one or more rare earth elements including Y) 29 to
33 mass%, boron B less than 0.8 mass%, Al
0.01 to 2.0 mass%, the balance Fe (part of Fe is replaced by Co and Cu, and the weight ratio of Cu and Co is Cu /
(Co = 0.02 to 0.2) is used as a second alloy, and a rare earth alloy powder in which the first alloy powder and the second alloy powder are mixed in a predetermined composition is molded in a magnetic field, and then sintered. A method for producing a rare earth permanent magnet, comprising: 24. R (at least one or more rare earth elements including Y) 29 to 33 mass%, boron B 0.8 to 1.
An alloy consisting of 2 mass%, Al 0.01 to 2.0 mass%, and the balance being Fe, wherein the first alloy coarse powder having a different content of heavy rare earth in the R and the first alloy coarse powder having a different boron B content. R (at least one or more rare earth elements including Y) 29-
33 mass%, boron B less than 0.8 mass%, Al
An alloy consisting of 0.01 to 2.0 mass% and the balance Fe (a part of Fe was replaced by Co and Cu) was used as a second alloy, and the first alloy powder and the second alloy powder were mixed in a predetermined composition. A method for producing a rare earth permanent magnet, comprising forming a rare earth alloy powder in a magnetic field and then sintering the rare earth alloy powder.