JP6086293B2 - Method for producing RTB-based sintered magnet - Google Patents

Description

  The present invention relates to a method for producing an RTB-based sintered magnet.

  R-T-B sintered magnets (R is at least one of rare earth elements, T is at least one of transition metal elements, and must contain Fe) are known as the most powerful magnets among permanent magnets. It is used for various motors such as a voice coil motor (VCM) of a hard disk drive and a hybrid in-vehicle motor.

The _RTB -based sintered magnet has a _reduced coercive force H _cJ (hereinafter sometimes simply referred to as “H _cJ ”) at high temperatures, causing irreversible thermal demagnetization. In order to avoid irreversible thermal demagnetization, when used for motors, etc., it is required to maintain a high _HcJ even at high temperatures.

In recent years, for the purpose of improving _HcJ of RTB-based sintered magnets, heavy rare earth elements RH such as Dy and Tb are supplied to the surface of RTB-based sintered magnets, and the heavy rare earth elements RH are magnetized. There has been proposed a method for improving H _cJ while suppressing a decrease in residual magnetic flux density B _r (hereinafter, simply referred to as “B _r ”) by diffusing inside.

  In Patent Document 1, a plurality of RTB-based sintered magnet bodies and a plurality of RH diffusion sources containing heavy rare earth elements RH are inserted into a processing chamber so as to be relatively movable and close to or in contact with each other. The RTB-based sintered magnet body and the RH diffusion source are heated while being moved continuously or intermittently in the processing chamber, whereby the heavy rare earth element RH is removed from the RH diffusion source. Is supplied to the surface of the RTB-based sintered magnet body and diffused inside.

International Publication No. 2011/007758

  However, in the diffusion process of Patent Document 1, the RTB-based sintered magnet body and the RH diffusion source are continuously or intermittently moved in the process chamber, so that the process chamber in which these are loaded is used. Rotating, swinging, etc. (hereinafter, sometimes referred to as “rotation”), the R-T-B system sintered magnet body is affected by the impact caused by the contact between the R-T-B system sintered magnet bodies. Chipping may occur.

  Patent Document 1 describes that it is preferable to introduce an agitation auxiliary member into the processing chamber in addition to the RTB-based sintered magnet body and the RH diffusion source. The stirring auxiliary member promotes contact between the RH diffusion source and the RTB-based sintered magnet body, and the heavy rare earth element RH adhering to the stirring auxiliary member is indirectly supplied to the RTB-based sintered magnet body. The role of supplying to. Furthermore, it is described that the stirring assisting member also has a role of preventing chipping due to contact between the RTB-based sintered magnet bodies or between the RTB-based sintered magnet body and the RH diffusion source in the processing chamber. Has been.

  In the diffusion process of Patent Document 1, as a method of charging the RTB-based sintered magnet body, the RH diffusion source, and the stirring auxiliary member into the processing chamber, for example, the RTB-based sintered magnet body, RH A method of collectively loading each of the diffusion source and the stirring assisting member into the processing chamber (hereinafter sometimes referred to as “collective charging process”) is conceivable.

  However, when the batch charging process is performed, the R after the diffusion process of Patent Document 1 is compared with the case where the stirring auxiliary member is not inserted (when only the RTB-based sintered magnet body and the RH diffusion source are used). There was a problem that the magnetic characteristics of the -T-B based sintered magnets varied. As a result of detailed studies on this problem, the present inventors have conventionally used a stirring auxiliary member to promote contact between the RH diffusion source and the RTB-based sintered magnet body. However, when it is actually used, the RTB-based sintered magnet body and the RH diffusion source are difficult to uniformly stir. It turned out that there may be. That is, when the present inventors perform the batch charging process using an agitation auxiliary member, uniform agitation between the RTB-based sintered magnet body and the RH diffusion source may be hindered. I found out the problem. If the RTB-based sintered magnet body and the RH diffusion source are not uniformly stirred, the supply of the heavy rare earth element RH to the RTB-based sintered magnet body will vary, and as a result, The magnetic characteristics of the RTB-based sintered magnet after the diffusion treatment of Patent Document 1 vary.

  In order to solve the above-mentioned problem, for example, without changing the speed of rotation of the processing chamber in which the RTB-based sintered magnet body, the RH diffusion source, and the stirring auxiliary member are charged, the time of rotation, etc. However, the diffusion processing time of Patent Document 1 becomes longer, and the mass productivity is greatly deteriorated. Therefore, a method of changing the speed of rotation or the like without changing the time of rotation or the like of the processing chamber can be considered. However, for example, when the speed of rotation or the like is increased, the RTB-based sintered magnet body and the RH diffusion source are uniformly stirred, but the impact due to the contact between the RTB-based sintered magnet bodies is increased. This increases the problem that the function of preventing the chipping of the RTB-based sintered magnet body by the stirring assisting member cannot be sufficiently exerted, and a lot of chips may occur. On the other hand, if the speed of rotation or the like is slowed, the RTB-based sintered magnet body and the RH diffusion source do not uniformly stir, so it is necessary to lengthen the processing time, and there is a problem that mass production efficiency deteriorates. It was.

  Further, in Patent Document 1, as another method for inserting the RTB-based sintered magnet body, the RH diffusion source, and the stirring auxiliary member into the processing chamber, for example, an RTB-based sintered magnet body in advance is used. A method of mixing the RH diffusion source and the stirring auxiliary member uniformly outside the processing chamber and then charging the RH diffusion source and the stirring auxiliary member into the processing chamber (hereinafter sometimes referred to as “preliminary batch mixing processing”) is conceivable. The preliminary batch mixing process can be performed, for example, by a method in which an RTB-based sintered magnet body, an RH diffusion source, and an agitation auxiliary member are charged in a container and the container is rotated. However, even when mixing outside in this way, as in the case of increasing the time of rotation of the processing chamber or changing the speed, a lot of chipping occurs or the processing time becomes longer, resulting in higher mass production efficiency. There was a problem of getting worse.

  The present invention has been made to solve the above problems, and in the diffusion treatment of Patent Document 1, an R-T-B system sintered magnet material (R-T-B system sintered magnet of Patent Document 1 is used. Rt that does not deteriorate the mass production efficiency by reducing the occurrence of chipping of the R-T-B-based sintered magnet material when uniformly stirring the RH diffusion source and the RH diffusion source to prevent variations in magnetic properties An object is to provide a method for producing a B-based sintered magnet.

  The method for producing an RTB-based sintered magnet according to claim 1 includes a plurality of RH diffusion sources (alloys containing heavy rare earth element RH in an amount of 30% by mass to 80% by mass, provided that The element RH is a step of preparing at least one of Dy and Tb, a step of preparing a plurality of stirring auxiliary members, and a plurality of R-T-B system sintered magnet materials (R is at least one of rare earth elements). And a step of preparing a diffusion source-auxiliary member mixture by mixing the RH diffusion source and the stirring auxiliary member, and preparing a diffusion source-auxiliary member mixture; , The step of charging the diffusion source-auxiliary member mixture and the RTB-based sintered magnet material into a processing chamber, and heating and rotating and / or swinging the processing container; A diffusion source and the stirring auxiliary member; Serial R-T-B based sintered magnet material continuously or intermittently moving the characterized in that it comprises a, and performing RH diffusion process.

The present invention according to claim 2 is the method for producing an RTB-based sintered magnet according to claim 1, wherein the weight ratio of the RH diffusion source and the stirring auxiliary member in the diffusion source-auxiliary member mixture is It is characterized by being in the range of 0.8 to 1.2: 1.
According to a third aspect of the present invention, there is provided the method for producing an RTB-based sintered magnet according to the first aspect, wherein the RTB-based sintered magnet material and the diffusion source-auxiliary member mixture are mixed. The weight ratio is in the range of 0.4 to 0.7: 1.

  According to the present invention, in the RH diffusion treatment, the RTB-based sintered magnet material and the RH diffusion source are uniformly stirred to prevent variation in magnetic properties. The production | generation method of the RTB type | system | group sintered magnet which reduces generation | occurrence | production of the chip | tip of a magnet raw material and does not deteriorate mass production efficiency can be provided.

It is process drawing which shows embodiment of the manufacturing method of the RTB type sintered magnet of this invention. It is sectional drawing which shows typically an example of the apparatus used when performing RH spreading | diffusion processing of this invention.

  In the present invention, the RH diffusion treatment refers to the diffusion by heating and rotating and / or swinging the treatment chamber charged with the diffusion source-auxiliary member mixture and the RTB-based sintered magnet material. By moving the RH diffusion source and the stirring auxiliary member charged with the source-auxiliary member mixture and the R-T-B system sintered magnet material continuously or intermittently, the heavy rare earth element RH is removed from the RH diffusion source. Is diffused inside while supplying the surface of the RTB-based sintered magnet material.

  In the present invention, the RTB-based sintered magnet before RH diffusion treatment and during the RH diffusion treatment is referred to as an “RTB-based sintered magnet material”, and the RTB-based sintered magnet after the RH diffusion treatment is used. The binding magnets are indicated separately as “RTB-based sintered magnets”. The RTB-based sintered magnet material corresponds to the RTB-based sintered magnet body of Patent Document 1. A mixture obtained by mixing a plurality of RH diffusion sources and a plurality of stirring auxiliary members is referred to as a “diffusion source-auxiliary member mixture”.

An embodiment of the method for producing an RTB-based sintered magnet of the present invention will be described based on the process chart shown in FIG. .
In the present invention, when the RH diffusion process (S6) is performed, the RH diffusion source prepared in the step (S1) of preparing a plurality of RH diffusion sources and the step of preparing a plurality of stirring auxiliary members (S2). The step (S4) of preparing the diffusion source-auxiliary member mixture by mixing the stirring auxiliary member prepared in step S4 is performed, and then the diffusion source-auxiliary member mixture and a plurality of RTB systems A step (S5) of charging the RTB-based sintered magnet material prepared in the step (S3) of preparing the sintered magnet material into the processing chamber is performed. That is, in the present invention, the batch charging process is not performed. In the present invention, after the step (S4) of preparing the diffusion source-auxiliary member mixture by mixing the RH diffusion source and the stirring auxiliary member, the diffusion source-auxiliary member mixture and the RTB-based sintering are performed. By carrying out the step (S5) of charging the magnet material into the processing chamber, the R-T-B system sintered magnet material is not chipped as compared with the batch charging process, without causing the occurrence of chipping in the R-T The B-based sintered magnet material and the RH diffusion source can be uniformly stirred. That is, in the present invention, in order to uniformly stir the RTB-based sintered magnet material and the RH diffusion source, the speed of the rotation of the processing chamber is increased or decreased unlike the batch charging process. There is no need to do. Therefore, without causing the deterioration of mass production efficiency due to the occurrence of chipping of the RTB-based sintered magnet material by increasing the speed of rotation of the processing chamber or the speed of rotation of the processing chamber, etc. Variations in characteristics can be prevented. In the present invention, since the RTB-based sintered magnet material is not mixed, only the RH diffusion source and the stirring auxiliary member are mixed in advance to prepare the diffusion source-auxiliary member mixture. Compared to the case of mixing a B-based sintered magnet material, RH diffusion source, and stirring auxiliary member (preliminary batch mixing process), RH diffusion can be performed without considering chipping of the RTB-based sintered magnet material. The source and the stirring auxiliary member can be mixed in a short time, and as a result, good stirring of the mixture and the R-T-B system sintered magnet material can be realized without requiring a long time.
Note that the order of the step (S1) and the step (S2) is not limited as long as it is performed at least before the step (S4). For example, the step (S1) may be performed after the step (S2). The order of the step (S3) is not limited as long as it is performed at least before the step (S5). For example, it may be performed before the step (S4) or after the step (S4).
Details of each process will be described below.

[Step of preparing a plurality of RH diffusion sources (S1)]
In the step of preparing a plurality of RH diffusion sources (S1), the RH diffusion source is an alloy containing 30% by mass to 80% by mass of heavy rare earth element RH (heavy rare earth element RH is at least one of Dy and Tb). For example, DyFe alloy, TbFe alloy and the like. When the heavy rare earth element RH is less than 30% by mass, the supply amount of the heavy rare earth element RH becomes small and the treatment time becomes very long, which is not suitable for mass production. Moreover, when heavy rare earth element RH exceeds 80 mass%, there exists a possibility of welding with a RTB system sintered magnet raw material. The RH diffusion source may contain at least one of Nd, Pr, La, Ce, Zn, Zr, Sm, and Co as long as the effects of the present invention are not impaired other than Dy, Tb, and Fe.

  Furthermore, as an inevitable impurity, at least one of Al, Ti, V, Cr, Mn, Ni, Cu, Ga, Nb, Mo, Ag, In, Hf, Ta, W, Pb, Si, and Bi may be included.

  The shape of the RH diffusion source is arbitrary such as a spherical shape, a linear shape, a plate shape, a block shape, and a powder. In the case of a spherical shape, a linear shape, a plate shape, or a block shape, the diameter can be set to 1.5 mm to 10 mm in the case of a spherical shape, for example. In the case of powder, the particle size can be set in the range of 0.05 mm to 1 mm, for example.

[Step of preparing a plurality of stirring assisting members (S2)]
The stirring assisting member has a role of reducing the occurrence of chipping due to contact between the R-T-B type sintered magnet materials in the processing chamber. The stirring assisting member also serves to indirectly supply the heavy rare earth element RH attached to the stirring assisting member from the RH diffusion source to the RTB-based sintered magnet material. In particular, in the present invention, since the mixture is mixed with the RH diffusion source in advance before charging into the processing chamber to form a diffusion source-auxiliary member mixture, the original role as the stirring auxiliary member during the RH diffusion treatment. Can be fully exhibited.

  In the step (S2) of preparing a plurality of stirring assisting members, the stirring assisting member is at least one of zirconia, silicon nitride, silicon carbide, and boron nitride, or at least one of Mo, W, Ta, Hf, and Zr. Consists of. Moreover, it is preferable that the stirring auxiliary member has a shape that is easy to move in the processing chamber, and examples thereof include a spherical shape, an elliptical shape, and a cylindrical shape having a diameter of 0.5 mm to 3 mm.

[Step of preparing a plurality of RTB-based sintered magnet materials (S3)]
In the step of preparing a plurality of RTB-based sintered magnet materials (S3), an RTB-based sintered magnet material (R is at least one of rare earth elements, and T is at least one of transition metals) Rt-B-based sintered magnet manufactured by a known composition and manufacturing method can be used.

[Step of preparing a diffusion source-auxiliary member mixture (S4)]
A plurality of RH diffusion sources and a plurality of stirring auxiliary members are mixed to prepare a diffusion source-auxiliary member mixture. As a mixing method, a known method may be used, and the method is not particularly limited. For example, a plurality of RH diffusion sources and an agitation auxiliary member may be charged into the mixing tank, and the mixing tank may be rotated at 0.1 to 2 m per second for 10 minutes to 8 hours for mixing.

  In the diffusion source-auxiliary member mixture, the weight ratio of the RH diffusion source and the stirring auxiliary member is preferably in the range of 0.8 to 1.2: 1. If it is less than 0.8, the amount of RH diffusion source charged is small, so the amount of heavy rare earth element RH supplied to the R-T-B system sintered magnet material may be small. As a result, the magnetic properties of the RTB-based sintered magnet after the RH diffusion treatment may deteriorate. Moreover, since the charging amount of the stirring auxiliary member is small when it exceeds 1.2, there may be a lot of chipping due to the contact between the RTB-based sintered magnet materials during the RH diffusion treatment which is the next step. .

[Step of charging the diffusion source-auxiliary member mixture and the RTB-based sintered magnet material into the processing chamber (S5)]
The diffusion source-auxiliary member mixture prepared in advance in the step (S4) and the RTB-based sintered magnet material prepared in the step (S3) are charged into a processing chamber. It is preferable that the RTB-based sintered magnet material and the diffusion source-auxiliary member mixture are charged into the processing chamber in a weight ratio of 0.4 to 0.7: 1. If it is less than 0.4, the amount of R-T-B system sintered magnet material charged is small, so that the processing amount decreases and mass productivity may deteriorate. On the other hand, if it exceeds 0.7, the amount of the diffusion source-auxiliary member mixture charged is small, so that the amount of heavy rare earth element RH supplied to the RTB-based sintered magnet material may be small. As a result, the magnetic properties of the RTB-based sintered magnet after the RH diffusion treatment may deteriorate.

[Step of performing RH diffusion treatment (S6)]
By heating and rotating and / or swinging the processing chamber charged with the diffusion source-auxiliary member mixture and the RTB-based sintered magnet material in the step (S5), the diffusion source-auxiliary By continuously or intermittently moving the RH diffusion source, the stirring auxiliary member, and the RTB-based sintered magnet material charged by the member mixture, the heavy rare earth element RH is transferred from the RH diffusion source to the R- While supplying the surface of the TB-based sintered magnet material, an RH diffusion treatment is performed to diffuse the inside. FIG. 2 is a cross-sectional view schematically showing an example of an apparatus used when performing the RH diffusion treatment of the present invention. First, the lid 5 in FIG. 2 is removed from the processing chamber 4, the diffusion source-auxiliary member mixture and a plurality of RTB-based sintered magnet materials 1 are charged into the processing chamber 4, and the lid 5 is processed again. Install in chamber 4. Next, the inside of the processing chamber 4 is decompressed by the exhaust device 6. Then, after the internal pressure of the processing chamber 4 is sufficiently reduced, heating by the heater 7 is performed while the processing chamber 4 is rotated by the motor 8. By the rotation of the processing chamber 4, the RH diffusion source 2, the stirring auxiliary member 3 and the RTB-based sintered magnet material 1 charged by the diffusion source-auxiliary member mixture are uniformly stirred as shown in the figure. As a result, the intended RH diffusion process can be performed smoothly.

  The processing chamber 4 is made of stainless steel, but is not limited to this, and has heat resistance of 1000 ° C. or more, and reacts with the R—T—B system sintered magnet material 1, the RH diffusion source 2, and the stirring auxiliary member 3. Any material that is difficult to do is optional. For example, an alloy containing at least one of Nb, Mo, and W may be used. Further, an Fe—Cr—Al alloy or an Fe—Cr—Co alloy may be used. The processing chamber 4 is provided with a lid 5 that can be opened and closed or removed. Further, projections are provided on the inner wall of the processing chamber 4 so that the RTB-based sintered magnet material 1, the RH diffusion source 2, and the stirring auxiliary member 3 can move efficiently. Further, the cylindrical shape of the processing chamber 4 may have an oval or polygonal cross section. The processing chamber 4 is connected to the exhaust device 6. The inside of the processing chamber 4 can be depressurized or pressurized by the exhaust device 6. An inert gas can be inserted into the processing chamber 4 from a gas supply device (not shown).

  The processing chamber 4 is heated by a heater 7 disposed on the outer periphery thereof. By heating the processing chamber 4, the RTB-based sintered magnet material 1, the RH diffusion source 2, and the stirring auxiliary member 3 housed therein are also heated. The processing chamber 4 is rotatably supported and can be rotated by the motor 8 during heating by the heater 7. For example, the peripheral speed of the inner wall surface of the processing chamber 4 is set to 0.01 m or more so that the RTB-based sintered magnet material 1 and the RH diffusion source 2 are not welded. It is preferable. Moreover, it is preferable to set to 0.5 m or less per second so that the RTB-based sintered magnet material in the processing chamber does not vigorously come into contact with each other due to rotation.

  The inside of the processing chamber 4 during heating is preferably in an inert atmosphere. The “inert atmosphere” in the present invention includes a vacuum or an inert gas atmosphere. The “inert gas” is a rare gas such as argon (Ar), for example, but chemically between the RTB-based sintered magnet material 1, the RH diffusion source 2, and the stirring auxiliary member 3. Any gas that does not react is included in the “inert gas” in the present invention. The pressure in the processing chamber 4 is preferably 1 kPa or less. In the present invention, since the RTB-based sintered magnet material 1 and the RH diffusion source 2 are close to or in contact with each other, the diffusion amount of the heavy rare earth element RH can be increased. is there.

  In the RH diffusion treatment of the present invention, it is preferable to maintain the temperature of the RTB-based sintered magnet material 1 and the RH diffusion source 2 within a range of 500 ° C. or higher and 850 ° C. or lower, and 700 ° C. or higher and 850 ° C. or lower. It is more preferable to be within the range The temperature range is such that the R—T—B system sintered magnet material 1 and the RH diffusion source 2 move relatively close to each other or come into contact with each other while the heavy rare earth element RH is sintered in the R—T—B system. This is a preferable temperature range that diffuses inward through the grain boundary layer of the internal structure of the magnet material, and the diffusion into the RTB-based sintered magnet material is efficiently performed. The holding time of the RH diffusion treatment in the present invention can be determined in consideration of the charged amount and shape of the RTB-based sintered magnet material 1, the RH diffusion source 2, and the stirring auxiliary member 3. The holding time is 10 minutes to 72 hours, preferably 1 hour to 14 hours.

  In FIG. 2, the processing chamber 4 is configured to rotate. In the present invention, the processing chamber 4 is prevented from welding the RTB-based sintered magnet material 1 and the RH diffusion source 2 during the RH diffusion processing. If the RTB-based sintered magnet material 1 and the RH diffusion source 2 can move continuously or intermittently within 4, the processing chamber 4 may be swung rather than rotated. Rotation and swinging operations may be performed together.

  When the RH diffusion source 2, the stirring auxiliary member 3, and the RTB-based sintered magnet material 1 are separated after the RH diffusion treatment, the RH diffusion source 2 and the stirring auxiliary member 3 are not separated, the RH diffusion source 2, It is preferable to separate the stirring auxiliary member 3 and the R-T-B system sintered magnet material 1. Thereby, the RH diffusion source 2 and the stirring auxiliary member 3 that are not separated during the next RH diffusion treatment can be used as a diffusion source-auxiliary part mixture. The separation method may be performed by a known method, and the method is not particularly limited. For example, it may be separated by vibration with a punching metal.

After the step (S6), for the RTB-based sintered magnet after the RH diffusion treatment, a treatment for homogenizing the diffused heavy rare earth element RH (hereinafter referred to as “homogenization heat treatment”). May be added). The homogenization heat treatment is performed within a range of 700 ° C. or more and 1000 ° C. or less of the RTB-based sintered magnet in a situation where the heavy rare earth element RH is not supplied from the RH diffusion source 2 to the RTB-based sintered magnet. Heat with. More preferably, it is performed within a range of 850 ° C. or higher and 1000 ° C. or lower. As a result, the diffusion of the heavy rare earth element RH occurs in the RTB-based sintered magnet, so that the heavy rare earth element RH diffuses deeply from the surface side of the RTB-based sintered magnet. It is possible to increase H _cJ . The time for performing the homogenization heat treatment is, for example, 10 minutes to 72 hours. Preferably it is 1 to 12 hours.

  Furthermore, after the step (S6) or after the homogenization treatment, a heat treatment may be performed for the purpose of improving the magnetic properties of the RTB-based sintered magnet. This heat treatment is the same as the heat treatment performed after sintering in a known method for producing a R-T-B sintered magnet material. Known conditions may be employed for the heat treatment atmosphere, the heat treatment temperature, and the like.

  The present invention will be described in more detail with reference to examples, but the present invention is not limited to the examples.

Example 1
A plurality of DyFe alloys containing 60% by mass of Dy were prepared as RH diffusion sources. The DyFe alloy had a spherical shape and a particle size of 1.5 mm to 2.5 mm. In addition, a plurality of zirconia balls having a diameter of 5 mm were prepared as stirring assist members. Further, Nd 22.3%, Pr 6.2%, Dy 4.0%, B 1.0%, Co 0.9%, Cu 0.1%, Al 0.2%, Ga 0.1%, balance Fe (unit: mass%) An RTB-based sintered magnet material having the following composition was prepared and prepared by a known method. The dimensions of the RTB-based sintered magnet material are 7 mm × 7 mm × 20 mm, and the magnetic properties of the product obtained by heat-treating the RTB-based sintered magnet material at 500 ° C. for 1 hour are: B _r = 1.35T and H _cJ = 1730 kA / m.

  First, the RH diffusion source and the stirring auxiliary member were put into a cylindrical mixing tank having the same diameter as that of the processing chamber, and mixed at 0.2 m per second for 30 minutes to prepare a diffusion source-auxiliary member mixture. The mixing ratio was 1: 1 by weight.

  Next, the RTB-based sintered magnet material and the diffusion source-auxiliary member mixture are charged into the processing chamber at a weight ratio of 0.5: 1, and the processing chamber is evacuated. Inert gas (Ar gas) was introduced. The pressure of the inert gas was 1 Pa. The treatment chamber was heated and rotated to perform the RH diffusion treatment. The processing chamber was rotated at a peripheral speed of 0.03 m per second. The temperature of the RTB-based sintered magnet material and the diffusion source-auxiliary member mixture was heated to 850 ° C. and held for 4 hours. The RTB-based sintered magnet after the RH diffusion treatment was subjected to a homogenization heat treatment with an inert gas pressure of 10 kPa and a temperature of 850 ° C., to prepare an RTB-based sintered magnet. .

Example 2
R-T-B system in the same manner as in Example 1 except that the RH diffusion source and the stirring auxiliary member were mixed at a weight ratio of 0.8: 1 to prepare a diffusion source-auxiliary member mixture. A sintered magnet was produced.

Example 3
R-T-B system in the same manner as in Example 1 except that the RH diffusion source and the stirring auxiliary member were mixed at a weight ratio of 1.2: 1 to prepare a diffusion source-auxiliary member mixture. A sintered magnet was produced.

Example 4
The RTB system is the same as that of Example 1 except that the RTB system sintered magnet material and the diffusion source-auxiliary member mixture are mixed at a weight ratio of 0.4: 1. A sintered magnet was produced.

Example 5
The RTB system is the same as that of Example 1 except that the RTB system sintered magnet material and the diffusion source-auxiliary member mixture are mixed at a weight ratio of 0.7: 1. A sintered magnet was produced.

Example 6
R-T-B system in the same manner as in Example 1 except that the RH diffusion source and the stirring auxiliary member were mixed at a weight ratio of 0.7: 1 to prepare a diffusion source-auxiliary member mixture. A sintered magnet was produced.

Example 7
R-T-B system in the same manner as in Example 1 except that the RH diffusion source and the stirring auxiliary member were mixed at a weight ratio of 1.3: 1 to produce a diffusion source-auxiliary member mixture. A sintered magnet was produced.

Example 8
The RTB system is the same as that of Example 1 except that the RTB system sintered magnet material and the diffusion source-auxiliary member mixture are mixed at a weight ratio of 0.3: 1. A sintered magnet was produced.

Example 9
The RTB system is the same as that of Example 1 except that the RTB system sintered magnet material and the diffusion source-auxiliary member mixture are mixed at a weight ratio of 0.8: 1. A sintered magnet was produced.

Comparative Example 1
Except that the RTB-based sintered magnet material, RH diffusion source, and stirring assisting member are collectively charged into the processing chamber at a weight ratio of 1: 1: 1 (the batch charging process). Produced an RTB-based sintered magnet in the same manner as in Example 1.

Comparative Example 2
An RTB-based sintered magnet was produced in the same manner as in Comparative Example 1 except that the processing chamber was rotated at a peripheral speed of 0.05 m per second.

Comparative Example 3
R-T-B system sintered magnet material, RH diffusion source, and stirring auxiliary member are added to the mixing tank at a ratio of 1: 1: 1 by weight, and mixed at 0.2 m per second for 30 minutes. An R-T-B system sintered magnet was produced in the same manner as in Example 1 except that it was charged into the treatment chamber (preliminary batch mixing treatment).

Comparative Example 4
The RTB-based sintered magnet material and the stirring auxiliary member are mixed at a weight ratio of 1: 1 to prepare a mixture, and the RH diffusion source and the mixture are mixed at a weight ratio of 0.5: An RTB-based sintered magnet was produced in the same manner as in Example 1 except that it was charged into the processing chamber at a rate of 1.

Comparative Example 5
The RTB-based sintered magnet material and the RH diffusion source are mixed at a weight ratio of 1: 1 to prepare a mixture, and the stirring auxiliary member and the mixture are mixed at a weight ratio of 0.5: An RTB-based sintered magnet was produced in the same manner as in Example 1 except that it was charged into the processing chamber at a rate of 1.

Comparative Example 6
The same as Example 1 except that the R-T-B system sintered magnet material and the RH diffusion source were charged into the processing chamber at a weight ratio of 1: 1 without using the stirring auxiliary member. An RTB-based sintered magnet was produced by this method.

Table 1 shows the results of Examples 1 to 9 and Comparative Examples 1 to 6. “Occurrence of chipping” indicates the number of chipping in the RTB-based sintered magnet after the RH diffusion treatment. When the part missing due to the chip was equivalent to 1 mm square, the chip was counted as having a chip. In addition, it has been confirmed in advance that there is no chip in the RTB-based sintered magnet material before the RH diffusion treatment. “H _cJ variation” indicates the difference between the maximum H _cJ value and the minimum H _cJ value _obtained by randomly measuring 20 pieces in a plurality of R-T-B sintered magnets after processing. . “Number of treatments” indicates the number of RTB-based sintered magnet materials used in Examples 1 to 9 and Comparative Examples 1 to 6, respectively. “H _cJ ” indicates an average value of H _{cJ obtained} by randomly measuring 20 R-T-B sintered magnets after the RH diffusion treatment. “B _r ” represents an average value of _{Br obtained by} measuring 20 R-T-B sintered magnets after the RH diffusion treatment at random.

As shown in Table 1, a diffusion source-auxiliary member mixture is prepared by mixing the RH diffusion source and the stirring auxiliary member according to the present invention, and the diffusion source-auxiliary member mixture and the RTB-based sintered magnet are prepared. In each of Examples 1 to 9, in which the raw material was charged into the processing chamber and subjected to the RH diffusion treatment, there was almost no “ _breakage ” and “H _cJ variation” was small. On the other hand, Comparative Example 1 in which each of the RH diffusion source, the stirring auxiliary member, and the R-T-B system sintered magnet material was collectively charged into the processing chamber (the batch charging process) " _HcJ variation" is large, although there is no "occurrence". In Comparative Example 2 in which the number of revolutions in the processing chamber was changed, “H _cJ variation” was improved. However, since the rotational speed was increased, many “occurrence of chipping” were confirmed. In addition, Comparative Example 3 in which the RTB-based sintered magnet material, the RH diffusion source, and the stirring auxiliary member were mixed in the mixing tank and then charged into the processing chamber (preliminary batch mixing process) Many occurrences were confirmed. The chipping of Comparative Example 3 occurred due to the impact caused by the contact between the RTB-based sintered magnet materials at the time of preparing the mixture in the mixing tank, and was not generated in the RH diffusion treatment process. Therefore, it is conceivable to reduce “occurrence of chipping” by slowing the rotation speed of the mixing tank, but this is not preferable because the production efficiency is greatly reduced. Furthermore, a comparison was made by mixing the R-T-B system sintered magnet material and the stirring auxiliary member, or the R-T-B system sintered magnet material and the RH diffusion source before charging the processing chamber. In Examples 4 and 5, many occurrences of chipping were confirmed. These also had chipping due to the impact caused by the contact between the RTB-based sintered magnet materials at the time of producing the mixture. Furthermore, in Comparative Example 6, since there was no stirring auxiliary member, many “occurrence of chipping” was confirmed due to the impact caused by the contact between the RTB-based sintered magnet materials.

DESCRIPTION OF SYMBOLS 1 RTB type sintered magnet raw material 2 RH diffusion source 3 Stirring auxiliary member 4 Processing chamber 5 Lid 6 Exhaust device 7 Heater 8 Motor

Claims (1)

Preparing a plurality of RH diffusion sources (an alloy containing heavy rare earth element RH 30% by mass or more and 80% by mass or less, wherein heavy rare earth element RH is at least one of Dy and Tb);
Preparing a plurality of stirring auxiliary members;
Preparing a plurality of RTB-based sintered magnet materials (R is at least one kind of rare earth elements, T is at least one kind of transition metal elements, and necessarily contains Fe);
Mixing the RH diffusion source and the stirring auxiliary member, and preparing a diffusion source-auxiliary member mixture in which the weight ratio of the RH diffusion source and the stirring auxiliary member is in the range of 0.8 to 1.2: 1. When,
Charging the diffusion source-auxiliary member mixture and the RTB -based sintered magnet material into a processing chamber in a weight ratio of 1: 0.4 to 0.7 ;
By heating and rotating and / or swinging the processing chamber , the RH diffusion source, the stirring auxiliary member, and the RTB-based sintered magnet material are moved continuously or intermittently to cause the RH to move. A step of performing a diffusion treatment;
The manufacturing method of the RTB type | system | group sintered magnet containing this.

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