JPH02153041A - Manufacture of high polymer compounded type rare earth magnet material - Google Patents

Abstract

PURPOSE:To obtain the title magnet material of high capacity by pulverizing an ingot of rare earth elements-transition metals-B series, subjecting it to primary magnetic compacting, thereafter to sintering, to pulverizing, furthermore to secondary magnetic compacting, thereafter to heat treatment under specific conditions and successively impregnating high polymer resin thereto. CONSTITUTION:An R2T14B series ingot constituted of Nd as rare earth elements R, Fe as transition metals T and B is cast, cooled and thereafter pulverized. The powder is formed into a primary magnetic compact and is thereafter sintered, e.g., at 1,030 deg.C in vacuum or in an inert gas. The sintered body is pulverized to regulate its average grain size to the one as large as 1.5 times the average grain size of the sintered body and to <=1mm. The powder of the sintered body is compacted in the magnetic field into a secondary magnetic powder compact, is thereafter subjected to heat treatment at 480 to 1,120 deg.C, is quenched from the above temp., is furthermore reheated to 540 to 800 deg.C and is thereafter impregnated with high polymer resin such as epoxy resin to execute high polymer compounding.

Description

[Detailed Description of the Invention] [Industrial Application Field] The present invention mainly uses rare earth metals (r?), transition metals (T), and boron (B), typified by Nd-Fe-B permanent magnets. R, T1. The present invention relates to a method for manufacturing polymer composite rare earth magnet materials, typically rubber magnets and plastic magnets, using rare earth magnet powder of B (R represents at least one of Y and a rare earth element, and T represents a transition element) system.

[Prior Art] Generally, a polymer composite magnet material is one in which magnet powder is dispersed in a polymer resin, or one in which magnet powder is bound with a polymer resin. This type of magnet material has various properties not found in cast magnets, sintered magnets, etc., such as elasticity and ease of processing, and is used in various fields. A variety of materials have been used as the magnet powder to be dispersed and bound, and in particular, Nd-Fe-B rare earth magnet alloy powder is known to exhibit the most excellent magnetic properties.

However, as mentioned above, this polymer composite rare earth magnet material is made of Nd-Fe-B rare earth magnet alloy powder and non-magnetic resin, so it has poor magnetic properties compared to sintered magnets. It has the disadvantage of being inferior.

For this reason, in the conventional manufacturing method of polymer composite rare earth magnet material using Nd-Fe-B rare earth magnet alloy powder, an alloy ingot obtained by melting the Nd-Fe-B tea raw material is heat-treated. An attempt was made to achieve magnetic properties by pulverizing the powder, mixing the powder with a polymer resin, and then molding it in a magnetic field to make it anisotropic, such as orienting the magnetic powder in the magnetic field. Moreover, it has been considered desirable that the raw material magnet alloy powder used be composed of fine single crystal grains in order to improve crystal grain orientation in a magnetic field.

[Problems to be solved by the invention] However, in the conventional manufacturing method of polymer composite rare earth magnet materials, mechanical stress during crushing causes
The coercive force (fHc) decreases, especially in the region where this alloy powder consists of fine single crystal particles, and the coercive force decreases significantly. Even if it could be used, it had the disadvantage that it would result in a polymer composite magnet with extremely poor magnetic properties.

On the other hand, it is known that pulverization using the liquid quenching method produces an alloy powder with almost no decrease in holding power, but on the other hand, it has the problem that anisotropy cannot be easily achieved. are doing. The present inventors have filed and disclosed an invention for making magnet powder anisotropic by hot working this liquid quenched alloy, but since it requires a large pressing force, However, since it is usually expensive, it is difficult to say that it is industrially useful.

Therefore, in view of the above-mentioned drawbacks, the technical problem of the present invention is to provide a manufacturing method that allows easy switching of existing equipment in the manufacturing process of conventional R-T-B sintered magnet materials, and to utilize the existing equipment as is. Accordingly, it is an object of the present invention to provide a method for manufacturing a polymer composite rare earth magnet material having anisotropy with improved magnetic properties.

[Means for Solving the Problems] According to the present invention, an R2T14B ingot containing Nd, Fe, and B as main components (R represents at least one of Y and a rare earth element, and T represents a transition element) is crushed. After producing an initial powder, the initial powder is compacted in a first magnetic field to produce a first magnetic powder compact, and the first magnetic powder compact is sintered. a sintering step of producing a sintered body; a sintered body crushing step of pulverizing the sintered body to generate a sintered body crushed powder; a second magnetic field compacting step of producing a second magnetic powder compact, and heat treating the second magnetic powder compact;
A method for producing a polymer composite rare earth magnet material is obtained, which includes a heat treatment step of producing a heat-treated molded body, and a resin composite molding step of composite-molding the heat-treated molded body with a polymer resin.

Further, according to the present invention, the heat treatment step includes heat-treating the secondary magnetic powder compact at a temperature substantially within the range of 1480 to 1120°C to produce a heat-treated compact. A method for manufacturing a molecular composite rare earth magnet material is obtained.

Further, according to the present invention, before the resin composite molding treatment step, the heat-treated molded product is rapidly cooled after maintaining the heat treatment temperature, and then reheated again substantially at a temperature in the range of 540 to 800°C. A method for producing a polymer composite rare earth magnet material is obtained, which is characterized by including a rapid cooling and reheating treatment step.

Further, according to the present invention, before the resin composite molding treatment step, the heat-treated molded product is slowly cooled after maintaining the heat treatment temperature, and then reheated again at a temperature substantially in the range of 1450 to 750°C. A method for producing a polymer composite rare earth magnet material is obtained, which is characterized by including a gradual cooling and reheating treatment step.

Further, according to the present invention, the resin composite molding treatment step includes:
A method for producing a polymer composite rare earth magnet material is obtained, which comprises performing composite molding by impregnating the heat-treated molded body with a polymer resin.

According to the present invention, after an R2 T14B system (R represents at least one of Y and a rare earth element, and T represents a transition element) ingot containing Nd, Fe, and B as main components is pulverized to generate an initial powder. , a first magnetic field compacting step in which the initial powder is compacted in a first magnetic field to produce a first magnetic powder compact, and a sintering step in which the first magnetic powder compact is sintered to produce a sintered body. a sintering process, a sintered body crushing process of pulverizing the sintered body to produce a sintered body crushed powder, and a second magnetic field molding after mixing the sintered body crushed powder with a polymer resin. According to the present invention, the sintered body pulverizing step preferably includes the sintered body pulverized powder. The sintered body is pulverized so that the average grain size of the sintered body is substantially 1.5 times or more as compared to the average crystal grain size of the sintered body, and within 1 mm or less. A method for producing a characteristic polymer composite rare earth magnet material is obtained.

[Summary of the present invention] Various experiments were conducted to demonstrate that the improvement in magnetic properties of the present invention is related to the improvement in 1Hc and Br, and that this is deeply caused by the plurality of oriented crystal grains in the molding powder. The present invention is constituted by the facts discovered as a result of the research.

An outline of the present invention is shown below.

(1) First, an R2T, B-based alloy ingot is pulverized to produce a primary powder, and then subjected to primary compacting in a magnetic field to produce a primary magnetic powder compact.

(2) Next, the obtained primary magnetic powder compact is sintered, thereby producing a sintered body with a high degree of crystal orientation.

(2) Next, the secondary powder is compacted in a secondary magnetic field to produce a secondary magnetic powder compact.

Next, the second magnetic powder compact is heat-treated to obtain a heat-treated compact. At this time, the heat treatment temperature is substantially 148
The temperature should be within the range of 0 to 1120°C.

This shows that heat treatment at 1480°C or higher significantly improves Br and IHc, and heat treatment at 1120°C or higher improves IHc.
This is because the decrease in c becomes significant. This means that mechanical damage and deterioration during crushing cannot be recovered by heat treatment. However, it has been shown that internal distortion can be eliminated by high-temperature heat treatment at 900° C. or higher.

■Here, in order to further improve IHC, the heat-treated molded product is cooled rapidly or slowly after the heat treatment temperature is maintained, and then cooled again.
Substantially, reheating treatment may be performed at a temperature in the range of 540 to 800°C or 450 to 750°C.

Next, the heat-treated molded body is impregnated with a polymer resin to produce an R-T-B polymer composite rare earth magnet material having high magnetic properties.

■Meanwhile, the sintered body is crushed to produce sintered body crushed powder,
After mixing this sintered powder with a polymer resin, a second
Next, the material is molded in a magnetic field and then compression molded or injection molded to produce an R-T-B polymer composite rare earth magnet material having high magnetic properties. Here, the sintered body is crushed to produce a secondary powder, the average particle size of which is 1.5 times or more compared to the average crystal grain size of the sintered body, and within the range of 11g1 or less. shall be. By setting this to 1.5 times or more compared to the average grain size of the sintered body, it is possible to improve the holding power due to heat treatment and at the same time
The improvement in r, (BH), , is also significant, and the upper limit is lowered to I
The reason why it is set as III+1 is because if the particle size is larger than this, the homogeneity of the polymer composite rare earth magnet material decreases, and problems such as mold breakage during powder compaction and non-uniformity in fluid production occur. It is.

Note that the average crystal grain size of the sintered body is preferably within the range of 0.5 to 100 μm, but is not limited thereto.

As explained above, by producing a heat-treated molded article according to the present invention and using this, an impregnated mold.

It is possible to provide a wide range of polymer composite rare earth magnet materials such as compression molding molds and injection molding molds.

[Example] Next, an example of the present invention will be described with reference to the drawings.

Example 1 - The polymer composite clay 'M and magnet according to Example 1 of the present invention relates to a case in which a heat-treated molded body is impregnated with a polymer resin.

First, Nd with a purity of 97 wt% (the remainder is rare earth elements other than Nd mainly consisting of Ce and Pr) and ferroboron (B
(approximately 20 wt%) and electrolytic iron, and melted by high frequency heating in an argon atmosphere so that the rare earth element (R) is 33.5%, B is 1.1%, and the balance is Fe. , an alloy ingot was obtained. This ingot was coarsely ground, and then coarsely ground to an average particle size of about 2 μm using a ball mill. This alloy powder is placed in a magnetic field of about 20 KOe.
It was molded into a rectangular parallelepiped in a magnetic field at a pressure of 1 ton/- (
1st magnetic field forming process).

Next, this primary magnetic powder molded body was heated to 1030°C in vacuum.
After being kept at ℃ for 1 hour, the
Hold for a period of time to obtain a sintered body (sintering process). At this time, the density of the sintered body is approximately 7.55 (gr/am”),
The average grain size was about 6 μm.

This sintered body is coarsely ground to 150 meshes or less to produce an alloy powder (sintered body pulverized powder). It was molded into a disc shape in a magnetic field (secondary molding step in a magnetic field).

The obtained secondary magnetic powder compact was heated at 1450℃5500'
C, 700'C, 800℃, 900℃, 1000℃, 1
Heat treatment at temperatures of 050°C, 1100°C, and 1150°C for 1 hour in vacuum and then 1 hour in Ar (
After the heat treatment step), it was rapidly cooled to obtain a heat-treated molded product. The density (G, D,) of these rapidly cooled heat-treated molded bodies is 5.4
It was 0 to 7.00 (gr/an').

Next, these heat-treated molded bodies were evacuated and then impregnated with epoxy resin. Subsequently, the magnet was held at 80° C. for 5 hours to be cured to obtain a polymer composite magnet according to Example 1 (resin composite molding step).

FIG. 1 shows the magnetic properties of the polymer composite rare earth magnet material according to the obtained example.

As a result, within the heat treatment temperature range of 480 to 1120°C,
It can be seen that it exhibits high magnetic properties. In this figure, the horizontal axis is the heat treatment temperature in the molding process, and the vertical axis is the maximum energy product (BH) MAX (MGOe>).

Residual magnetic flux density Br (KG), ci! , magnetic force IHc
(KOe), densities G, D, and (gr-cm-') are shown, respectively.

Here, as a polymer composite rare earth magnet according to a comparative example, the above-mentioned sintered body was aged at 600''C for 2 hours, and then this aged sintered body was used as a sintered body in the same manner as in Example 1. The material was pulverized, molded in a secondary magnetic field, heat treated, and impregnated with epoxy resin to form a polymer composite.

The measured magnetic properties and density of the comparative example are (BH)MAX
4. 0 <MGOe), Br5.
5 (KO).

, 1c 3. 0 (KOe),
G, D, 5. 4 (gr.cm
-'), and it was found that higher magnetic properties were obtained with the polymer composite rare earth magnet of this example than with the comparative example.

In addition, the magnetic properties of the aged sintered body itself in the comparative example are maximum energy product (BH) mAx44, O(MG
Oe), residual magnetic flux density Br13.7 (KG),! magnetic force r
HCl2. O('KOe), the average grain size of the crystal grains is about 6 μm, and the sintered densities G and D.

It was 7.55 (gr-cm-').

Example 2 - A polymer composite rare earth magnet according to Example 2 of the present invention relates to a case in which a heat-treated molded body is rapidly cooled, reheated, and then impregnated with a polymer resin.

First, a secondary magnetic powder molded body formed from the coarse powder of the sintered body produced in Example 1 in a magnetic field was heat treated at 1000°C for 1 hour in vacuum and in Ar, and then rapidly cooled. did.

Next, these heat-treated molded bodies were heated at 500°C to 80°C.
Each sample was held in Ar for 2 hours at 50°C intervals up to 0°C, then rapidly cooled and reheated.

The densities G and D of the obtained molded product after this reheating treatment.

was 6.10 to 6.15 (gr/male).

Thereafter, these compacts were made into polymer composite rare earth magnets in the same manner as in Example 1, and the magnetic properties thereof were measured and are shown in FIG.

As a result, it was confirmed that high magnetic characteristic values could be obtained when the temperature of the reheating treatment was within the range of 540 to 800°C.

As a comparative example, except for the above reheating treatment,
A polymer composite rare earth magnet was produced in the same manner as in this example, and its magnetic properties were measured.

The result is (BH) MAX 21, 5 (MGO
e).

Br9.9 (KG), IHc 8.5 (KOe)
.

G, D, 6.10 (gr/am').

Embodiment 3 - A polymer composite rare earth magnet according to Embodiment 3 of the present invention relates to a case in which a heat-treated molded body is gradually cooled, subjected to reheating treatment, and then impregnated with a polymer resin.

First, a second magnetic powder compact was formed by compacting the sintered powder (-150 mesh or less) produced in Example 1 again in a magnetic field at 1000'C. After being kept in vacuum and Ar gas for 1 hour each, it was cooled in a furnace to 300°C. Note that this furnace cooling rate is approximately -150°C/Hr, 7°C near 1000°C.
Around 00°C, it was about -70°C/Hr; around 1400°C, it was -30°C/Hr.

Next, these heat-treated molded bodies were held at 1450 to 750°C in 50°C increments for 2 hours each, then slowly cooled and reheated. Densities G, D, of the heat-treated molded body subjected to reheating treatment,
is 6.10 to 6.15 (gr/am').

Next, these molded bodies were impregnated with a polymer resin in the same manner as in Example 1 to obtain a polymer composite rare earth magnet, and the magnetic properties were measured. The measured values are shown in Figure 3. .

As a result, it can be seen from FIG. 3 that the polymer composite rare earth magnet according to Example 3 can obtain high magnetic properties when the reheating treatment temperature is within the range of 6150 to 750°C.

For the sake of Hitsu, the magnetic properties and density of a polymer composite rare earth magnet manufactured in the same manner as in this example except for the above-mentioned reheating treatment were (BH) MAX 21-5 (MGOe).
), Br9. 8 (KG),
I Hc 9゜0 (KOe), G, D
, 6.10 (gr/c+n').

Example 4 - A polymer composite rare earth magnet according to Example 4 of the present invention relates to a case in which a heat-treated molded body is impregnated with a polymer resin.

First, using cerium dididium consisting of 5 wt% C6, 15 wt% Pr balance Nd (Nd includes rare earth elements other than Nd), dysprosium, ferroporon, electrolytic iron, electrolytic cobalt, and aluminum, an example was prepared. 1
Similarly, (Ce・Pr-Nd> is 33.0wt%
, Dy is 3.0wt%, Co is 10wt%, AI is 1w
An R-'T'-B ingot containing t% and the balance Fe was obtained.

Next, in the same manner as in Example 1, the powder was pulverized to a uniform particle size of about 2 μm, then compacted in a primary magnetic field, and sintered at 1000°C. The density of this sintered body was 7°50, and the crystal grains had an average grain size of about 5.5 μm.

Next, the above-mentioned sintered body is coarsely pulverized and formed in a second magnetic field,
Thereafter, heat treatment was performed at 600°C, 800°C, and 1000°C, respectively, and the heat-treated molded product was made of epoxy 1r! A polymer composite magnet was obtained by impregnating it with No. 1 resin. Table 1 shows the measurement results of their magnetic properties.

The measured magnetic properties and density of the polymer composite rare earth magnet material formed through the forming process of impregnating with (BH)h
aAx 4. O (MGOe), Br5.2 (KG),
IHc3.5 (KOe), G, D, 5°50 (gr
/1xr3).

From Table 1, it can be seen that the polymer composite rare earth magnet according to Example 4 had significantly improved magnetic properties compared to Comparative Example 4.

As a comparative example, the above sintered body was subjected to aging treatment at 600°C for 2 hours, then coarsely crushed, molded in a second magnetic field, and impregnated with epoxy resin in the same manner as in this example. , and measured the magnetic properties at that time.

The result is (BH) MAX 33, 5(MGOe
).

Br 1 2. 1 (KG), I
Hc14. 5 (KOe).

As a result, it can be seen that this example has better magnetic properties than the cited example.

Table 1 Below, below, and below: 1 Example 5 - The polymer composite rare earth magnet according to Example 5 of the present invention was produced by mixing the heat-treated compact powder with a polymer resin, and then performing tertiary magnetic field molding. and relates to cases that are compression molded or injection molded.

First, the pulverized sintered powder produced in Example 1 was molded in a second magnetic field, and then heat-treated at 600°C.
It was crushed at 50 mesh or less.

Polymer composite rare earth magnets were produced from this heat-treated compact powder using the following two methods. One is about 25vo I% of epoxy resin mixed into heat-treated molded body powder.
Compression molding was performed in a magnetic field of 0 KOe at a pressure of 7 tons/- while performing tertiary magnetic field molding. The obtained molded body was heated to 110
Hold at ℃ for 1 hour to obtain a polymer composite rare earth magnet.

Another method is to mix 40 vol.
A polymer composite rare earth magnet was obtained by injection molding into a predetermined mold while molding in a tertiary magnetic field applying a magnetic field of .

Table 2 shows the magnetic properties of the polymer composite rare earth magnet.

For comparison purposes, the above sintered body was subjected to aging treatment and then crushed to obtain sintered body pulverized powder. After that, polymer composite rare earth magnets each treated in the same manner as in this example were prepared. Magnet characteristics are also listed.

As a result, from Table 2, it can be seen that the polymer composite rare earth magnet according to the example had significantly improved magnetic properties compared to the comparative example.

Example 6 below - A polymer composite rare earth magnet according to Example 6 of the present invention relates to a case in which the sintered powder was pulverized to have an average particle diameter of 50 μm.

First, using Nd with a purity of 97 wt% (the balance being rare earth elements mainly consisting of Ce and Pr), ferroboron (B content of 20 wt%), and electrolytic iron, rare earth elements (R) were 34.0%, B 1.0%.

An alloy ingot was obtained by melting by high frequency heating in an argon atmosphere so that the remainder was Fe.

After crushing this ingot, use a ball mill to further crush the ingot to an average particle size of about 2 μm. Approximately 20% of this alloy powder
In a magnetic field of 0 KOe, at a pressure of 1 tOn/cIA, it is desired to form a rectangular parallelepiped in a magnetic field (first magnetic field forming step).

Next, this primary magnetic powder molded body was heated at 1000° C. in vacuum.
℃ or 1050'C for 1 hour, and then kept in an argon atmosphere for 3 hours to obtain a sintered body (sintering process). At this time, the sintered density is about 7.55 (gr/am'), and the average crystal grain size of the sintered body at 1000°C is 5 μm,
At 1050°C, it was 10 μm.

This sintered body was heated to 111 μm so that the average grain size was 50 μm.
This alloy powder is crushed into about 200
(Second magnetic field forming step) to form a disk shape in a magnetic field of e and a forming pressure of 5tO11/-.

Next, this secondary magnetic powder compact was heated to 1400°C to 110°C.
Within the range of 0℃, each 100℃ for 1 hour in vacuum.
After being held in Ar for 1 hour, it was rapidly cooled (heat treatment step).

The density (G, D,) of these heat-treated molded bodies is 5.4 to
It was 6.8 (gr/cm3).

Next, these heat-treated molded bodies were evacuated, impregnated with epoxy resin, and then held at 80° C. for 5 hours to be cured to form a polymer composite magnet. The measurement results of the magnetic properties are shown in FIG. As a result, it was found that high magnetic properties were exhibited by heat treatment at about 450°C to 1100°C.

As a comparative example, the above sintered body was subjected to aging treatment, and then a polymer composite magnet treated in the same manner as in this example was produced, and the magnetic properties thereof were compared. The result is (BH)MA
X 2.5 (MGOe>, Br5, O(KG), I
Hc2. O (KOe), G.

D, 5.40 (gr/cm') Teaf, -0
Example 7 - In the polymer composite rare earth magnet according to Example 7 of the present invention, the average particle size of the sintered body crushed powder is 1/1 of the average crystal grain size of the sintered body.
．． Concerning cases where the increase is 5 times or more.

First, using the sintered body produced in Example 6, the average particle size of the sintered body at 1000°C is 5.10
, 15, 25, 250μm, and 1050℃
In the case of 01, 20.30, 50, 100.5
00tcm (sintered compact crushing step).

Next, the pulverized powder of the sintered body was heated at 600°C for 1 hour in a vacuum.
After being held in Ar for 1 hour and quenched, these heat-treated molded bodies were lightly ground to produce a heat-treated molded powder, and then 20V of epoxy resin was applied.

The mixture was mixed with I% and subjected to secondary magnetic field molding in a magnetic field of about 20 KOe at a molding pressure of 5 tons/- to form a disk shape. This molded body was held at 80° C. for 5 hours to form a polymer composite magnet. The measurement results of this magnetic property are shown in FIG. Note that G and D in the figure are values when only the magnet powder is used, which was determined from the density of the polymer composite magnet by correcting the amount of mixed epoxy resin. The results show that when the value of average pulverized grain size/average crystal grain size of sintered body becomes 1.5 or more, the magnetic properties are significantly improved.

Example 8 - In the polymer composite rare earth magnet according to Example 8 of the present invention, the average grain size of the sintered body crushed 45) powder is 1.5 times or more the average crystal grain size of the sintered body. Concerning a case like this.

The sintered body crushed powder produced in Example 7 was heated to about 20K Oe.
A second magnetic field molding was performed in a magnetic field of 5 ton/- at a molding pressure of 5 ton/- to form a disk shape. This secondary magnetic powder molded body was heated at 1000°C in a vacuum for 1 hour, and then A
After being held for 1 hour in R, it was rapidly cooled to produce a heat-treated molded body. The density (G, D) of these heat-treated molded bodies is 5.8
~6.5 (gr/cm').

Next, in the same manner as in Example 6, impregnated with epoxy resin,
We made a polymer composite magnet and measured its magnetic properties. The results are shown in FIG. The results show that when the value of the average pulverized grain size/the average crystal grain size of the sintered body becomes 1°5 or more, the magnetic properties are significantly improved.

Example 9 - A polymer composite rare earth magnet according to Example 9 of the present invention relates to a case in which the sintered powder was ground to have an average particle size of 50 μm.

First, Nd with a purity of 97wt% (the remainder is other rare earth elements mainly consisting of Ce and Pr) and Dy with a purity of 99w7% or more.
In the same manner as in Example 6, using ferroboron and electrolytic iron, an ingot having a composition of 33.0% (NdO19.Dy0.1), 1.0% B, and the balance Fe was obtained.

Next, this ingot was coarsely crushed and molded in a magnetic field in the same manner as in Example 6 (first magnetic field molding step), 102
Sintering was performed at 0°C or 1080°C. At this time, the average crystal grain size of the sintered body was 7 μm at 1020°C, and 7 μm at 1080°C.
In this case, it was 17 μm.

Next, these sintered bodies were coarsely pulverized to an average particle size of 20 μm, and then heat-treated by holding them at 600° C. in vacuum for 1 hour and in Ar for 94 hours.

Next, these heat-treated molded bodies were crushed, 35 vol.% of polyethylene was mixed, and then 2
Injection molding is performed in a mold while applying a magnetic field of 0 KOe,
Get a polymer composite magnet. The measurement results of the magnetic properties are shown in the third
Shown in the table.

As a result, it can be seen that the sample with an average crystal grain size of 7 μIn, in which the value of average crushed grain size/average crystal grain size of sintered body is 1.5 or more, has significantly improved magnetic properties.

Table 1 Example 10 - The polymer composite rare earth magnet according to Example 10 of the present invention is as follows:
This example relates to a case in which the sintered compact powder was ground to have an average particle size of 50 μm.

First, 5 wt% Ce, 15 wt% Pr, and the balance Nd (
However, other rare earth elements were included as Nd. ) consisting of cerium dididium and ferroboron.

Using electrolytic iron, electrolytic cobalt, balt and aluminum,
In the same manner as in Example 6, <Ce-Pr-Nd) was set to 35.
0wt%, B 1.1wt%, Co 10wt%, AI
An ingot having a composition of 1 wt% Fe and the balance Fe was obtained.

Next, in the same manner as in Example 6, the ingot was crushed, molded in a magnetic field, and sintered at 1000°C and 1050°C.

The average grain size of these sintered bodies is approximately 8. c.
zm was 17 μm at 1050°C.

Next, after pulverizing these sintered bodies to an average particle size of 20 μm,
In the same manner as in Example 6, molding was performed in a second magnetic field, and the temperature was 600 °C and 9
After heat treatment at 00°C, it was impregnated with epoxy resin to form a polymer composite magnet.

The results are shown in Table 4.

As a result, it can be seen that the sample with an average crystal grain size of 8 μm, in which the value of average crushed grain size/average crystal grain size of sintered body is 1.5 or more, has significantly improved magnetic properties.

As explained in the examples below, R2 having anisotropy
It can be seen that by using the sintered compact powder produced by pulverizing the T14B sintered alloy, it can be applied to a wide range of manufacturing methods for polymer composite magnets, such as impregnation type, compression molding type, and injection molding type. In addition, by making the average particle size of the sintered body crushed powder 1.5 times or more the average crystal grain size of the sintered body, a remarkable improvement in magnetization and growth could be realized.

In addition, in the above examples, h-Nd-Fe-B system, Nd-
Dy-Fe-B system, Ce-Pr-Nd-Co-AI-F
Although only the e-B system has been described, a portion of Nd may be replaced by Y and other rare earth elements, such as Gd.

By substituting Tb, Ho, etc., by substituting a part of Fe with other transition metals such as Mn, Cr, Ni, etc., or by substituting part of B with other semimetals such as St, C, etc. Even if the substitution is made, the composition of the magnet alloy is one in which Nd-FeB is a part of the main component, and the compound system of the magnet is one in which R2T14B, represented by the Nd2Fe+<B system, contributes to magnetism. For example, it can be easily inferred that the effects of the present invention can be fully expected. In addition, in this example, epoxy resin and polyethylene were used as polymer composite resins.
Although we have considered this, any substance is included in the present invention as long as it is a polymeric resin, rubber, metal, etc. that is present inside the molded product and contributes to improving the strength of the molded product. can be easily understood by those skilled in the art.

Furthermore, the same type of effect can be expected even if powder compaction is repeated three or more times.

[Effects of the Invention] As explained above, according to the present invention, high-performance RTs having anisotropy such as impregnation molds, compression molding molds, injection molding molds, etc.
- The B-beam polymer composite rare earth magnet and its manufacturing method can be easily realized without making large-scale changes to existing processes and equipment, and are extremely useful industrially.

[Brief explanation of the drawing]

FIG. 1 shows the heat treatment temperature of a compact in a magnetic field of a sintered coarse powder of a polymer composite rare earth magnet material according to Example 1 of the present invention, the compact density (G, D,), and magnetic properties (Br, r
Figure 2 shows the relationship between reheating treatment temperature and magnetic properties (Br, + Hc + (BH) MAX Figure 3 shows the relationship between reheating treatment temperature and magnetic properties (Br, +Hc, (BH), Ax), Figure 4 shows the relationship between the heat treatment temperature of the sintered ingot powder magnetic field neutral form and the magnet of the polymer composite magnet in Example 6 of the present invention, G, D, and the solid line (0
Mark) indicates the characteristics of a sample in which the average crystal grain size of the sintered body was 5 μm, and the broken line (Δ mark) was 10 μm. Figure 5 shows the average pulverized particle size of the sintered body crushed powder/average crystal grain size of the sintered body in Example 7, and the characteristics of the polymer composite magnet using the same, and the solid line in Figure 1 ( 0 mark) indicates that the average grain size of the sintered body is 5 μm, and the broken line (Δ mark) indicates 10 μm.
The characteristics of the sample using m are shown below. Figure 6 shows the average pulverized particle size of the sintered body crushed powder/average crystal grain size of the sintered body in Example 8, and the characteristics of the polymer composite magnet using the same, and the solid line in Figure 2 ( 0 mark) indicates the characteristics of a sample in which the average crystal grain size of the sintered body was 5 μIn, and the broken line (△ mark) was 10 μm. Figure 2: Reheating temperature (°C) Figure 3: Reheating temperature (°C) Figure 3: Reheating temperature (°C) Heat treatment temperature (°Q)

Claims (7)

[Claims] 1. R_2T_ containing Nd, Fe, and B as main components
1_4B system (R is at least one of Y and a rare earth element,
T represents a transition element. ) A first magnetic field compaction step of pulverizing the ingot to produce an initial powder, and then compacting the initial powder in a first magnetic field to produce a first magnetic powder compact; and the first magnetic powder compaction. a sintering process of sintering the sintered body to produce a sintered body; a sintered body crushing process of crushing the sintered body to generate a sintered body crushed powder; and a second process of the sintered body crushed powder. a second magnetic field compacting step of forming in a magnetic field to produce a second magnetic powder compact; a heat treatment step of heat-treating the second magnetic powder compact to produce a heat-treated compact; and the heat-treated compact. A method for manufacturing a polymer composite rare earth magnet material, comprising a resin composite molding step of composite molding a polymer resin with a polymer resin. 2. In the method for producing a polymer composite rare earth magnet material according to claim 1, in the heat treatment step, the secondary magnetic powder compact is substantially heat treated at a temperature within a range of 480 to 1120°C. , a method for producing a polymer composite rare earth magnet material, the method comprising producing a heat-treated molded body. 3. In the method for producing a polymer composite rare earth magnet material according to claim 1 or 2, before the resin composite molding step, the heat-treated molded product is rapidly cooled after maintaining the heat treatment temperature, and then substantially A method for producing a polymer composite rare earth magnet material, comprising a rapid cooling and reheating step of reheating in the range of 540 to 800°C. 4. In the method for manufacturing a polymer composite rare earth magnet material according to claim 1 or 2, before the resin composite molding step, the heat-treated molded product is slowly cooled after maintaining the heat treatment temperature, and then substantially A method for producing a polymer composite rare earth magnet material, comprising a gradual cooling and reheating step of reheating in a range of 450 to 750°C. 5. In the method for producing a polymer composite rare earth magnet material according to any one of claims 1 to 4, the resin composite molding treatment step includes composite molding by impregnating the heat-treated molded body with a polymer resin. A method for producing a characteristic polymer composite rare earth magnet material. 6. R_2T_ containing Nd, Fe, and B as main components
1_4B system (R is at least one of Y and a rare earth element,
T represents a transition element. ) A first magnetic field compaction step of pulverizing the ingot to produce an initial powder, and then compacting the initial powder in a first magnetic field to produce a first magnetic powder compact; and the first magnetic powder compaction. a sintering process of sintering the body to produce a sintered body; a sintered body crushing process of crushing the sintered body to generate a sintered body crushed powder; heat-treating the sintered body crushed powder; a heat treatment step of producing a heat-treated molded body, pulverizing the heat-treated molded body to generate a heat-treated molded body powder, mixing the heat-treated molded body powder with a polymer resin, and then molding in a second magnetic field; A method for producing a polymer composite rare earth magnet material, characterized by compression molding or injection molding. 7. In the method for producing a polymer composite rare earth magnet material according to claim 6, in the sintered body pulverizing step, the average particle size of the sintered body pulverized powder is substantially equal to the average crystal grain of the sintered body. A method for producing a polymer composite rare earth magnet material, comprising pulverizing the sintered body so that the diameter is 1.5 times or more and 1 mm or less.