Specification
FORM 2
THE PATENTS ACT, 1970
(39 of 1970)
&
THE PATENTS RULES, 2003
COMPLETE SPECIFICATION
[See section 10, Rule 13]
RARE EARTH SINTERED MAGNET, METHOD FOR PRODUCING RARE EARTH
SINTERED MAGNET, ROTOR, AND ROTARY MACHINE;
MITSUBISHI ELECTRIC CORPORATION, A CORPORATION ORGANISED
AND EXISTING UNDER THE LAWS OF JAPAN, WHOSE ADDRESS IS 7-3,
MARUNOUCHI 2-CHOME, CHIYODA-KU, TOKYO 100-8310, JAPAN
THE FOLLOWING SPECIFICATION PARTICULARLY DESCRIBES THE
INVENTION AND THE MANNER IN WHICH IT IS TO BE PERFORMED.
2
DESCRIPTION
TITLE OF THE INVENTION:
RARE EARTH SINTERED MAGNET, METHOD FOR PRODUCING RARE EARTH
SINTERED MAGNET, ROTOR, AND ROTARY MACHINE5
Field
[0001] The present disclosure relates to a rare earth
sintered magnet which is a permanent magnet obtained by
sintering a material containing a rare earth element, a10
method for producing a rare earth sintered magnet, a rotor,
and a rotary machine.
Background
[0002] R-T-B-based permanent magnets having a tetragonal15
R2T14B intermetallic compound as a main phase are known.
Here, the element R is a rare earth element, the element T
is a transition metal element including Fe (iron) or Fe
partially replaced by cobalt (Co), and B is boron. R-T-B-
based permanent magnets are used for various high value-20
added components including industrial motors. In
particular, Nd-Fe-B-based sintered magnets in which the
element R is neodymium (Nd) are used for various components
due to excellent magnetic properties. In addition, because
industrial motors are often used in a high temperature25
environment exceeding 100°C, attempts have been made to
improve coercive force by adding heavy rare earth elements
such as dysprosium (Dy) to Nd-T-B-based permanent magnets.
[0003] In recent years, the production of Nd-Fe-B-based
sintered magnets has been expanded, and the consumption of30
Nd and heavy rare earth elements such as Dy and terbium
(Tb) has been increased. However, Nd and heavy rare earth
elements are expensive and also have a procurement risk due
3
to high distribution unevenness. In view of this, a
possible measure for reducing the consumption of Nd and
heavy rare earth elements is to use other rare earth
elements as the element R, such as cerium (Ce), lanthanum
(La), samarium (Sm), scandium (Sc), gadolinium (Gd),5
yttrium (Y), and lutetium (Lu). However, magnetic
properties are known to be significantly degraded by
substituting these elements for all or a part of Nd.
Therefore, attempts have been conventionally made to
develop technology that allows for prevention of10
degradation of magnetic properties associated with
temperature rise in the case of using these elements for
producing Nd-Fe-B-based sintered magnets.
[0004] For example, Patent Literature 1 discloses a rare
earth magnet alloy including a main phase having a15
tetragonal R2Fe14B crystal structure and mainly composed of
Fe, B, and one or more elements selected from the group
consisting of Nd, La, and Sm, and a crystalline subphase
mainly composed of oxygen (O) and one or more elements
selected from the group consisting of Nd, La, and Sm. In20
the rare earth magnet alloy described in Patent Literature
1, La is segregated in the crystalline subphase, and Sm is
dispersed without segregation in the main phase and the
crystalline subphase. In the rare earth magnet alloy
described in Patent Literature 1, the above-described25
structure form prevents degradation of magnetic properties
associated with temperature rise.
[0005] Patent Literature 2 discloses a rare earth magnet
including a first phase containing a compound represented
by RaTbX, a grain boundary phase which is present at the30
crystal grain boundary of the first phase and has a higher
concentration of the element R than RaTbX, and a second
phase consisting of a single crystal of a compound
4
represented by ScMd. Here, the element R is one or more
rare earth elements including Nd, the element T is one or
more transition metal elements including Fe, and the
element X is one or more elements selected from B and
carbon (C). The element S is one or more rare earth5
elements including Sm, and the element M is one or more
transition metal elements including Co. According to the
technique described in Patent Literature 2, a rare earth
magnet having sufficient magnetic properties even at a high
temperature is obtained.10
[0006] Patent Literature 3 discloses an R-T-B-based
sintered magnet including a first main phase composed of
crystal grains of an R-T-B-based alloy containing a light
rare earth element as the element R, a second main phase
composed of crystal grains of an R-T-B-based alloy15
containing a heavy rare earth element as the element R, a
surface phase surrounding the surfaces of the crystal
grains constituting the first main phase and the second
main phase, and a grain boundary alloy phase present at the
grain boundary triple point. Here, the element T is Fe or20
Fe partially replaced by Co. In the R-T-B-based sintered
magnet described in Patent Literature 3, the concentration
of the heavy rare earth element is lower in the first main
phase and the grain boundary alloy phase than that in the
second main phase and the surface phase. According to the25
technique described in Patent Literature 3, the coercive
force can be effectively improved using rare earth elements
that give a high coercive force.
Citation List30
Patent Literature
[0007] Patent Literature 1: PCT Patent Application Laid-
open No. 2021/048916
5
Patent Literature 2: Japanese Patent Application
Laid-open No. 2021-9862
Patent Literature 3: Japanese Patent Application
Laid-open No. 2018-174205
5
Summary of Invention
Problem to be solved by the Invention
[0008] However, the rare earth magnet alloy described in
Patent Literature 1, in which Sm is uniformly dispersed in
the main phase and the subphase in the rare earth magnet10
alloy, can prevent degradation of magnetic properties
associated with temperature rise, but may not contribute to
improvement of magnetic properties at room temperature. In
addition, in the rare earth magnet described in Patent
Literature 2, the second phase is composed of a single15
crystal, and the elements present in the second phase do
not differ in concentration. That is, the second phases
distributed in the rare earth magnet have the same
composition at any positions, and are formed of one kind of
compound having a uniform concentration distribution. For20
this reason, the rare earth magnet described in Patent
Literature 2 does not have an optimal structure for
improvement of magnetic properties at room temperature. In
short, the problem is that there is room for further
improvement in magnetic properties. In addition, the R-T-25
B-based sintered magnet described in Patent Literature 3 is
configured to always contain a heavy rare earth element,
which results in a high coercive force. However, there is
a problem in that the residual magnetic flux density
required for industrial motors or the like cannot be30
obtained, which leads to degradation of magnetic
properties. Thus, there has been a demand for a rare earth
sintered magnet that achieves both improvement of magnetic
6
properties at room temperature and prevention of
degradation of magnetic properties associated with
temperature rise.
[0009] The present disclosure has been made in view of
the above, and an object thereof is to obtain a rare earth5
sintered magnet capable of improving magnetic properties at
room temperature and preventing degradation of magnetic
properties associated with temperature rise with reduced
use of Nd and heavy rare earth elements.
10
Means to Solve the Problem
[0010] To solve the problems above and achieve an
object, the present disclosure is directed to a rare earth
sintered magnet satisfying a general formula (Nd, La, Sm)-
Fe-B-M, where element M is one or more elements selected15
from a group consisting of Cu, Al, and Ga, the rare earth
sintered magnet including: a main phase including crystal
grains based on an R2Fe14B crystal structure; a first
subphase that is crystalline and mainly composed of an
oxide phase represented by (Nd, La, Sm)-O; and a second20
subphase that is crystalline and mainly composed of an
oxide phase represented by (Nd, La)-O. A concentration of
Sm is higher in the first subphase than in the second
subphase, and a concentration of the element M is higher in
the second subphase than in the first subphase.25
Effects of the Invention
[0011] The present disclosure can achieve the effect of
improving magnetic properties at room temperature and
preventing degradation of magnetic properties associated30
with temperature rise with reduced use of Nd and heavy rare
earth elements.
7
Brief Description of Drawings
[0012] FIG. 1 is a diagram schematically illustrating an
exemplary sintered structure of a rare earth sintered
magnet according to a first embodiment.
FIG. 2 is a diagram illustrating atomic sites in a5
tetragonal Nd2Fe14B crystal structure.
FIG. 3 is a flowchart illustrating an exemplary
procedure of a method for producing a rare earth magnet
alloy according to a second embodiment.
FIG. 4 is a diagram schematically illustrating the10
method for producing a rare earth magnet alloy according to
the second embodiment.
FIG. 5 is a flowchart illustrating an exemplary
procedure of a method for producing a rare earth sintered
magnet according to the second embodiment.15
FIG. 6 is a cross-sectional view schematically
illustrating an exemplary configuration of a rotor equipped
with a rare earth sintered magnet according to a third
embodiment.
FIG. 7 is a cross-sectional view schematically20
illustrating an exemplary configuration of a rotary machine
according to a fourth embodiment.
FIG. 8 is a composition image obtained by analyzing a
cross section of a rare earth sintered magnet according to
Examples 1 to 8 with FE-EPMA.25
FIG. 9 is an element map of Nd obtained by analyzing a
cross section of a rare earth sintered magnet according to
Examples 1 to 8 with FE-EPMA.
FIG. 10 is an element map of O obtained by analyzing a
cross section of a rare earth sintered magnet according to30
Examples 1 to 8 with FE-EPMA.
FIG. 11 is an element map of La obtained by analyzing
a cross section of a rare earth sintered magnet according
8
to Examples 1 to 8 with FE-EPMA.
FIG. 12 is an element map of Sm obtained by analyzing
a cross section of a rare earth sintered magnet according
to Examples 1 to 8 with FE-EPMA.
FIG. 13 is an element map of Cu obtained by analyzing5
a cross section of a rare earth sintered magnet according
to Examples 1 to 8 with FE-EPMA.
FIG. 14 is an element map of Al obtained by analyzing
a cross section of a rare earth sintered magnet according
to Examples 1 to 8 with FE-EPMA.10
FIG. 15 is an element map of Ga obtained by analyzing
a cross section of a rare earth sintered magnet according
to Examples 1 to 8 with FE-EPMA.
Description of Embodiments15
[0013] Hereinafter, a rare earth sintered magnet, a
method for producing a rare earth sintered magnet, a rotor,
and a rotary machine according to embodiments of the
present disclosure will be described in detail with
reference to the drawings.20
[0014] First Embodiment.
FIG. 1 is a diagram schematically illustrating an
exemplary sintered structure of a rare earth sintered
magnet according to the first embodiment. The permanent
magnet according to the first embodiment is a rare earth25
sintered magnet 1 satisfying the general formula (Nd, La,
Sm)-Fe-B-M, and including a main phase 10 including crystal
grains based on an R2Fe14B crystal structure and a subphase
20. The subphase 20 includes a first subphase 21 that is
crystalline and mainly composed of an oxide phase30
represented by (Nd, La, Sm)-O, and a second subphase 22
that is crystalline and mainly composed of an oxide phase
represented by (Nd, La)-O. The element M indicates one or
9
more elements selected from the group consisting of copper
(Cu), aluminum (Al), and gallium (Ga).
[0015] The main phase 10 has a tetragonal R2Fe14B crystal
structure in which the element R is Nd, La, and Sm. That
is, the main phase 10 has the composition formula (Nd, La,5
Sm)2Fe14B. The reason why the element R of the rare earth
sintered magnet 1 having a tetragonal R2Fe14B crystal
structure is rare earth elements consisting of Nd, La, and
Sm is from the calculation of magnetic interaction energy
with the use of a molecular orbital method. The10
calculation shows that a composition in which La and Sm are
added to Nd can produce the rare earth sintered magnet 1
which is practical in that degradation of magnetic
properties associated with temperature rise can be
prevented. In addition, by intentionally segregating La15
and Sm also in the grain boundary that is an example of the
subphase 20, it is possible to make Nd relatively diffused
throughout the main phase 10 so that magnetocrystalline
anisotropy of the main phase 10 is enhanced. Consequently,
a pseudo core-shell structure is formed in which a portion20
having high magnetic anisotropy and a portion having low
magnetic anisotropy exist in the main phase 10. As a
result, the effect of preventing degradation of magnetic
properties associated with temperature rise is further
enhanced.25
[0016] Note that when too much La and Sm are added, it
causes a decrease in the amount of Nd, which is an element
having a high magnetic anisotropy constant and a high
saturation magnetic polarization, which results in
degradation of magnetic properties. Therefore, it is30
preferable to satisfy a>(b+c), where a, b, and c represent
the composition ratios of Nd, La, and Sm, respectively.
[0017] The average grain size of the crystal grains of
10
the main phase 10 is preferably 100 μm or less, and more
preferably 0.1 μm to 50 μm for improving magnetic
properties.
[0018] The crystalline subphase 20 is a generic term for
the first subphase 21 and the second subphase 22 that are5
crystalline, and is present between the main phases 10.
The crystalline first subphase 21 is represented by (Nd,
La, Sm)-O as described above, and the crystalline second
subphase 22 is represented by (Nd, La)-O as described
above. Here, (Nd, La, Sm)-O means that a part of Nd is10
replaced by La and Sm. Note that the elements of the main
components are described in parentheses; therefore, the
first subphase 21 and the second subphase 22 may contain a
small amount of another component. In one example, the
second subphase 22 represented by (Nd, La)-O contains an15
extremely small amount of Sm.
[0019] In the rare earth sintered magnet 1 according to
the first embodiment, the concentration of Sm is higher in
the first subphase 21 than in the second subphase 22, and
the concentration of the element M is higher in the second20
subphase 22 than in the first subphase 21. In other words,
it means that Sm and the element M are segregated in
different subphases 20. Sm is present at a higher
concentration in the first subphase 21. Thus, Nd in the
Nd-rich phase is relatively diffused throughout the main25
phase 10, which results in improved magnetocrystalline
anisotropy of the main phase 10. Furthermore, Sm also
exists in the crystal grains of the main phase 10, and thus
contributes to improvement of the residual magnetic flux
density by being coupled in the same magnetization30
direction with Fe, a ferromagnetic substance. The element
M is present at a high concentration in the second subphase
22. Thus, the element M forms a nonmagnetic phase that
11
magnetically separates the main phases 10 from each other,
and contributes to improvement of magnetic properties.
Because Sm and the element M are present at a high
concentration in the different subphases 20, it is possible
to improve both the residual magnetic flux density and the5
coercive force.
[0020] In the rare earth sintered magnet 1 according to
the first embodiment, the concentrations of La and Sm
differ between the main phase 10 and the subphase 20: the
sum of the concentrations of La in the first subphase 2110
and the second subphase 22 is equal to or greater than the
concentration of La in the main phase 10, and the sum of
the concentrations of Sm in the first subphase 21 and the
second subphase 22 is equal to or greater than the
concentration of Sm in the main phase 10. Specifically,15
the concentrations of La and Sm in the subphase 20 are
equal to or higher than the concentrations of La and Sm in
the main phase 10. Furthermore, the concentration of La
also differs between the first subphase 21 and the second
subphase 22: the concentration of La in the first subphase20
21 is equal to or higher than the concentration of La in
the second subphase 22.
[0021] Here, given that X represents the concentration
of La contained in the main phase 10, X1 represents the
concentration of La contained in the first subphase 21, X225
represents the concentration of La contained in the second
subphase 22, Y represents the concentration of Sm contained
in the main phase 10, Y1 represents the concentration of Sm
contained in the first subphase 21, and Y2 represents the
concentration of Sm contained in the second subphase 22,30
the relationship of Formula (1) below is satisfied.
[0022] 1<(Y1+Y2)/Y<(X1+X2)/X ··· (1)
[0023] La is present at a high concentration in the
12
grain boundary in the process of production, particularly
in the heat treatment, whereby Nd is relatively diffused
throughout the main phase 10. As a result, in the rare
earth sintered magnet 1 according to the first embodiment,
Nd in the main phase 10 is not consumed at the grain5
boundary, which leads to improve magnetocrystalline
anisotropy. Sm is also present at a higher concentration
in the subphase 20, particularly in the first subphase 21,
than in the main phase 10. Thus, Nd is relatively diffused
throughout the main phase 10 as in the case of La,10
resulting in improved magnetocrystalline anisotropy.
[0024] The rare earth sintered magnet 1 according to the
first embodiment may contain an additive element N that
improves magnetic properties. The additive element N is
one or more elements selected from the group consisting of15
Co, zirconium (Zr), titanium (Ti), praseodymium (Pr),
niobium (Nb), Dy, Tb, manganese (Mn), Gd, and holmium (Ho).
[0025] Therefore, the rare earth sintered magnet 1
according to the first embodiment is expressed by the
general formula (NdaLabSmc)FedBeMfNg, where the additive20
element N is one or more elements selected from the group
consisting of Co, Zr, Ti, Pr, Nb, Dy, Tb, Mn, Gd, and Ho.
It is desirable that a, b, c, d, e, f, and g satisfy the
following relational expressions.
5≤a≤2025
0 second subphase” in structure form, and
the state in which the concentration of the element M is25
higher in the second subphase 22 than in the first subphase
21 is indicated in the item “concentration of element M:
first subphase < second subphase” in structure form. Among
Examples 1 to 8 and Comparative Examples 1 to 6, samples in
which these states were confirmed are indicated by “○”, and30
samples in which these states were not be confirmed are
indicated by “×”.
[0075] In addition, it is confirmed from the intensity
35
ratio of the element maps obtained with the FE-EPMA
analysis that the sum of the concentrations of La in the
first subphase 21 and the second subphase 22 is equal to or
greater than the concentration of La in the main phase 10,
and the sum of the concentrations of Sm in the first5
subphase 21 and the second subphase 22 is equal to or
greater than the concentration of Sm in the main phase 10.
Furthermore, it is confirmed that the concentration of La
in the first subphase 21 is equal to or higher than the
concentration of La in the second subphase 22.10
[0076] Here, from the intensity ratio of the element
maps obtained through FE-EPMA analysis of the concentration
of La contained in the main phase 10, the first subphase
21, and the second subphase 22 and the concentration of Sm
contained in the main phase 10, the first subphase 21, and15
the second subphase 22, it is confirmed that the
relationship between the concentration of La contained in
the main phase 10, the first subphase 21, and the second
subphase 22 and the concentration of Sm contained in the
main phase 10, the first subphase 21, and the second20
subphase 22 satisfies Formula (1) above.
[0077] Next, the results of measurement of the magnetic
properties in each sample according to Examples 1 to 8 and
Comparative Examples 1 to 6 will be described. The shape
of each sample that is the subject of magnetic measurement25
is a block shape having a length, a width, and a height of
7 mm. The first measurement temperature T1 is 23°C, and
the second measurement temperature T2 is 200°C. 23°C is
room temperature. 200°C is a temperature that can occur as
an environment in which automobile motors and industrial30
motors operate.
[0078] First, the residual magnetic flux density and the
coercive force in each sample according to Examples 1 to 8
36
and Comparative Examples 2 to 6 are determined in
comparison with Comparative Example 1. When the values of
the residual magnetic flux density and the coercive force
of each sample at 23°C are within an allowable measurement
error of 1% compared with the values of Comparative Example5
1, the values are rated as “equivalent”. Values of 1% or
more higher are rated as “good”, and values of 1% or more
lower are rated as “poor”.
[0079] Next, the temperature coefficient α of residual
magnetic flux density is calculated using the residual10
magnetic flux density at the first measurement temperature
T1 of 23°C and the residual magnetic flux density at the
second measurement temperature T2 of 200°C. The
temperature coefficient β of coercive force is calculated
using the coercive force at the first measurement15
temperature T1 of 23°C and the coercive force at the second
measurement temperature T2 of 200°C. The temperature
coefficient of residual magnetic flux density and the
temperature coefficient of coercive force in each sample
according to Examples 1 to 8 and Comparative Examples 2 to20
6 are determined in comparison with Comparative Example 1.
When the values of each sample are within an allowable
measurement error of ±1% compared with the absolute value
|α| of the temperature coefficient of residual magnetic
flux density and the absolute value |β| of the temperature25
coefficient of coercive force in the sample of Comparative
Example 1, the values are rated as “equivalent”. Values of
−1% or more lower are rated as “good”, and values of +1% or
more higher are rated as “poor”. Because the samples
determined to be “good” have a smaller temperature30
coefficient, it is possible to provide the rare earth
sintered magnet 1 having stable magnetic properties even in
a high temperature environment while reducing or preventing
37
degradation of magnetic properties associated with
temperature rise.
[0080] The results of determination of the residual
magnetic flux density, the coercive force, the temperature
coefficient of residual magnetic flux density, and the5
temperature coefficient of coercive force are shown in
Table 3.
[0081] Comparative Example 1 is a sample of the rare
earth sintered magnet 1 prepared in the form of Nd-Fe-B
with the production method according to the second10
embodiment using Nd, Fe, and FeB as raw materials. From
the observation of the structure form of this sample
according to the above-described method, due to the absence
of Sm, it is not confirmed that the concentration of Sm is
higher in the first subphase 21 than in the second subphase15
22. Furthermore, due to the absence of the element M, it
is not confirmed that the concentration of the element M is
higher in the second subphase 22 than in the first subphase
21. The evaluation of the magnetic properties of this
sample with the method described above shows that the20
residual magnetic flux density is 1.3 T and the coercive
force is 1000 kA/m. The temperature coefficients of
residual magnetic flux density and coercive force are
|α|=0.191 %/°C and |β|=0.460 %/°C, respectively. These
values of Comparative Example 1 are used as a reference.25
[0082] Comparative Example 2 is a sample of the rare
earth sintered magnet 1 prepared in the form of (Nd, Dy)-
Fe-B with the production method according to the second
embodiment using Nd, Dy, Fe, and FeB as raw materials.
From the observation of the structure form of this sample30
according to the above-described method, due to the absence
of Sm, it is not confirmed that the concentration of Sm is
higher in the first subphase 21 than in the second subphase
38
22. Furthermore, due to the absence of the element M, it
is not confirmed that the concentration of the element M is
higher in the second subphase 22 than in the first subphase
21. The evaluation of the magnetic properties of this
sample with the method described above shows that the5
residual magnetic flux density is “poor”, the coercive
force is “good”, the temperature coefficient of residual
magnetic flux density is “equivalent”, and the temperature
coefficient of coercive force is “equivalent”. This result
indicates that the coercive force is improved by10
substituting Dy having high magnetocrystalline anisotropy
for a part of Nd.
[0083] Comparative Example 3 is a sample of the rare
earth sintered magnet 1 prepared in the form of Nd-Fe-B-M
with the production method according to the second15
embodiment using Nd, Fe, FeB, and further the element M as
raw materials. From the observation of the structure form
of this sample according to the above-described method, due
to the absence of Sm, it is not confirmed that the
concentration of Sm is higher in the first subphase 21 than20
in the second subphase 22. In addition, despite the
addition of the element M, the first subphase 21 and the
second subphase 22 are not formed due to the absence of Sm,
and it is not confirmed that the concentration of the
element M is higher in the second subphase 22 than in the25
first subphase 21. The evaluation of the magnetic
properties of this sample with the method described above
shows that the residual magnetic flux density is
“equivalent”, the coercive force is “good”, the temperature
coefficient of residual magnetic flux density is30
“equivalent”, and the temperature coefficient of coercive
force is “equivalent”. This result reflects the fact that
the crystal grain boundary is made non-magnetic by the
39
element M, and the coercive force is improved, but the
concentration of Sm and the concentration of the element M
in the subphase 20 do not accord with an appropriate
structure form due to the absence of La and Sm.
[0084] Comparative Example 4 is a sample of the rare5
earth sintered magnet 1 prepared in the form of (Nd,Dy)-Fe-
B-M with the production method according to the second
embodiment using Nd, Dy, Fe, FeB, and further the element M
as raw materials. From the observation of the structure
form of this sample according to the above-described10
method, due to the absence of Sm, it is not confirmed that
the concentration of Sm is higher in the first subphase 21
than in the second subphase 22. In addition, despite the
addition of the element M, the first subphase 21 and the
second subphase 22 are not formed due to the absence of Sm,15
and it is not confirmed that the concentration of the
element M is higher in the second subphase 22 than in the
first subphase 21. The evaluation of the magnetic
properties of this sample with the method described above
shows that the residual magnetic flux density is “poor”,20
the coercive force is “good”, the temperature coefficient
of residual magnetic flux density is “equivalent”, and the
temperature coefficient of coercive force is “equivalent”.
This result reflects the fact that a part of Nd is replaced
by Dy having high magnetocrystalline anisotropy, and the25
crystal grain boundary is made non-magnetic by M, whereby
the coercive force is improved, but the concentration of Sm
and the concentration of the element M in the subphase 20
do not accord with an appropriate structure form due to the
absence of La and Sm.30
[0085] Comparative Example 5 is a sample of the rare
earth sintered magnet 1 prepared in the form of (Nd, La,
Sm)-Fe-B with the production method according to the second
40
embodiment using Nd, La, Sm, Fe, and FeB as raw materials.
From the observation of the structure form of this sample
according to the above-described method, the two types of
subphases 20, namely the first subphase 21 and the second
subphase 22, are not confirmed due to the absence of M5
despite the addition of Sm, and the concentration of Sm is
uniformly dispersed in the main phase 10 and the subphase
20. Furthermore, because the two types of subphases 20 are
not present, it is not confirmed that the first subphase 21
is higher than the second subphase 22. Furthermore, due to10
the absence of the element M, it is not confirmed that the
concentration of the element M is higher in the second
subphase 22 than in the first subphase 21. The evaluation
of the magnetic properties of this sample with the method
described above shows that the residual magnetic flux15
density is “poor”, the coercive force is “poor”, the
temperature coefficient of residual magnetic flux density
is “good”, and the temperature coefficient of coercive
force is “good”. This result reflects the fact that the
presence of La and Sm in the main phase 10 or the subphase20
20 gives a good result in the temperature coefficient of
the magnetic properties, but the two types of subphases 20
are not present, and the concentration of Sm and the
concentration of the element M in these subphases 20 do not
accord with an appropriate structure form.25
[0086] Comparative Example 6 is a sample of the rare
earth sintered magnet 1 prepared in the form of (Nd, La,
Sm)-Fe-B-N with the production method according to the
second embodiment using Nd, La, Sm, Fe, and FeB, and
further one or more additive elements N selected from the30
group consisting of Co, Zr, Ti, Pr, Nb, Dy, Tb, Mn, Gd, and
Ho as raw materials. From the observation of the structure
form of this sample according to the above-described
41
method, the two types of subphases 20, namely the first
subphase 21 and the second subphase 22, are not confirmed
due to the absence of the element M despite the addition of
Sm, and the concentration of Sm is uniformly dispersed in
the main phase 10 and the subphase 20. Furthermore,5
because the two types of subphases 20 are not present, it
is not confirmed that the first subphase 21 is higher than
the second subphase 22. Furthermore, due to the absence of
the element M, it is not confirmed that the concentration
of the element M is higher in the second subphase 22 than10
in the first subphase 21. The evaluation of the magnetic
properties of this sample with the method described above
shows that the residual magnetic flux density is “good”,
the coercive force is “poor”, the temperature coefficient
of residual magnetic flux density is “good”, and the15
temperature coefficient of coercive force is “good”. The
presence of La and Sm in the main phase 10 or the subphase
20 gives a good result in the temperature coefficient of
the magnetic properties. In addition, the magnetic flux
density is improved by the effect of the additive element N20
such as Co, which is a magnetic material. However, the
result reflects the fact that the two types of subphases 20
are not present, and the concentration of Sm and the
concentration of the element M in these subphases 20 do not
accord with an appropriate structure form.25
[0087] Examples 1 to 7 are samples of the rare earth
sintered magnet 1 prepared in the form of (Nd, La, Sm)-Fe-
B-M with the production method according to the second
embodiment using Nd, La, Sm, Fe, FeB, and further the
element M as raw materials. From the observation of the30
structure form of these samples according to the above-
described method, it is confirmed that the concentration of
Sm is higher in the first subphase 21 than in the second
42
subphase 22. Furthermore, it is confirmed that the
concentration of the element M is higher in the second
subphase 22 than in the first subphase 21. The evaluation
of the magnetic properties of these samples with the method
described above shows that the residual magnetic flux5
density is “good”, the coercive force is “good”, the
temperature coefficient of residual magnetic flux density
is “good”, and the temperature coefficient of coercive
force is “good”.
[0088] Example 8 is a sample of the rare earth sintered10
magnet 1 prepared in the form of (Nd, La, Sm)-Fe-B-M with
the production method according to the second embodiment
using Nd, La, Sm, Fe, FeB, the element M, and further the
additive element N as raw materials. From the observation
of the structure form of this sample according to the15
above-described method, it is confirmed that the
concentration of Sm is higher in the first subphase 21 than
in the second subphase 22. Furthermore, it is confirmed
that the concentration of the element M is higher in the
second subphase 22 than in the first subphase 21. The20
evaluation of the magnetic properties of these samples with
the method described above shows that the residual magnetic
flux density is “good”, the coercive force is “good”, the
temperature coefficient of residual magnetic flux density
is “good”, and the temperature property evaluation of25
coercive force is “good”. This indicates that the obtained
effect is not influenced by the addition of the additive
element N as long as a proper structure form is formed.
[0089] The samples of Examples 1 to 8 are the rare earth
sintered magnets 1 satisfying the general formula (Nd, La,30
Sm)-Fe-B-M and including: the main phase 10 including
crystal grains based on an R2Fe14B crystal structure; the
first subphase 21 that is crystalline and mainly composed
43
of an oxide phase represented by (Nd, La, Sm)-O; and the
second subphase 22 that is crystalline and mainly composed
of an oxide phase represented by (Nd, La)-O. As described
above, in the rare earth sintered magnets 1 according to
Examples 1 to 8, the concentration of Sm is higher in the5
first subphase 21 than in the second subphase 22, and the
concentration of the element M is higher in the second
subphase 22 than in the first subphase 21. As a result,
these rare earth sintered magnets 1 are capable of
improving magnetic properties at room temperature and10
reducing or preventing degradation of magnetic properties
associated with temperature rise with reduced use of Nd and
heavy rare earth elements, which are expensive and have a
procurement risk due to high distribution unevenness,
compared with the rare earth sintered magnet satisfying Nd-15
Fe-B.
[0090] The configurations described in the above-
mentioned embodiments indicate examples. The embodiments
can be combined with another well-known technique and with
each other, and some of the configurations can be omitted20
or changed in a range not departing from the gist.
Reference Signs List
[0091] 1 rare earth sintered magnet; 10 main phase; 20
subphase; 21 first subphase; 22 second subphase; 3125
crucible; 32 molten alloy; 33 tundish; 34 single roll;
35 solidified alloy; 36 tray container; 37 rare earth
magnet alloy; 100 rotor; 101 rotor core; 102 magnet
insertion hole; 120 rotary machine; 130 stator; 131
teeth; 132 winding.30
44
We Claim :
[Claim 1] A rare earth sintered magnet satisfying a general
formula (Nd, La, Sm)-Fe-B-M, where element M is one or more
elements selected from a group consisting of Cu, Al, and
Ga, the rare earth sintered magnet comprising:5
a main phase including crystal grains based on an
R2Fe14B crystal structure;
a first subphase that is crystalline and mainly
composed of an oxide phase represented by (Nd, La, Sm)-O;
and10
a second subphase that is crystalline and mainly
composed of an oxide phase represented by (Nd, La)-O,
wherein
a concentration of Sm is higher in the first subphase
than in the second subphase, and15
a concentration of the element M is higher in the
second subphase than in the first subphase.
[Claim 2] The rare earth sintered magnet according to claim
1, wherein20
a sum of concentrations of La in the first subphase
and the second subphase is equal to or greater than a
concentration of La in the main phase, and
a sum of concentrations of Sm in the first subphase
and the second subphase is equal to or greater than a25
concentration of Sm in the main phase.
[Claim 3] The rare earth sintered magnet according to claim
1 or 2, wherein a concentration of La in the first subphase
is equal to or higher than a concentration of La in the30
second subphase.
[Claim 4] The rare earth sintered magnet according to any
45
one of claims 1 to 3, wherein a>(b+c) is satisfied, where
a, b, and c represent composition ratios of Nd, La, and Sm,
respectively.
[Claim 5] The rare earth sintered magnet according to any5
one of claims 1 to 4, wherein 1<(Y1+Y2)/Y<(X1+X2)/X is
satisfied, where X represents the concentration of La
contained in the main phase, X1 represents the
concentration of La contained in the first subphase, X2
represents the concentration of La contained in the second10
subphase, Y represents the concentration of Sm contained in
the main phase, Y1 represents the concentration of Sm
contained in the first subphase, and Y2 represents the
concentration of Sm contained in the second subphase.
15
[Claim 6] The rare earth sintered magnet according to any
one of claims 1 to 5, further comprising: one or more
additive elements N selected from a group consisting of Co,
Zr, Ti, Pr, Nb, Dy, Tb, Mn, Gd, and Ho.
20
[Claim 7] A method for producing the rare earth sintered
magnet according to any one of claims 1 to 6, the method
comprising:
a melting step of melting a raw material of a rare
earth magnet alloy containing an element constituting the25
rare earth sintered magnet;
a pulverizing step of pulverizing the rare earth
magnet alloy satisfying (Nd, La, Sm)-Fe-B-M;
a molding step of preparing a molded body by molding
powder of the rare earth magnet alloy;30
a sintering step of preparing a sintered body by
holding the molded body at a sintering temperature in a
range of 900°C to 1300°C for a period of time in a range of
46
0.1 hours to 10 hours;
a primary aging step of holding the sintered body at a
primary aging temperature that is a temperature lower than
the sintering temperature;
a secondary aging step of holding the sintered body at5
a secondary aging temperature that is a temperature lower
than the primary aging temperature; and
a cooling step of cooling at a temperature lower than
the secondary aging temperature.
10
[Claim 8] The method for producing a rare earth sintered
magnet according to claim 7, wherein, in the first aging
step, the sintered body is held at a temperature of 700°C
or higher but lower than 900°C for 0.1 hours to 10 hours.
15
[Claim 9] The method for producing a rare earth sintered
magnet according to claim 7 or 8, wherein, in the second
aging step, the sintered body is held at a temperature of
450°C or higher but lower than 700°C for 0.1 hours to 10
hours.20
[Claim 10] The method for producing a rare earth
sintered magnet according to any one of claims 7 to 9,
wherein, in the cooling step, the sintered body is held at
a temperature of 200°C or higher but lower than 450°C for25
0.1 hours to 5 hours.
[Claim 11] A rotor comprising:
a rotor core; and
the rare earth sintered magnet according to any one of30
claims 1 to 6 provided in the rotor core.
[Claim 12] A rotary machine comprising:
47
the rotor according to claim 11; and
an annular stator facing the rotor and including, on
an inner surface on a side where the rotor is placed, teeth
protruding toward the rotor and windings provided on the
teeth.5