JP7648864B2 - Method for manufacturing a joint body and a joint body - Google Patents

Description

The present invention relates to a method for manufacturing a bonded body and to a bonded body.

To date, several methods have been proposed for joining ceramic components and cobalt-containing metal components.

For example, Patent Document 1 proposes a method in which a nickel plating layer is applied to a pre-etched surface of a ceramic member, a silver brazing material is applied on the plating layer, and then the ceramic member and the cobalt-based alloy member are brazed via the silver brazing material.

Patent Document 2 also proposes a method of joining a ceramic member and a cobalt-based alloy member by placing nickel-containing foil between the ceramic member and the cobalt-based alloy member and then performing heat treatment.

Japanese Patent Application Laid-Open No. 60-081072 Japanese Unexamined Patent Publication No. 63-060170

Conventional methods require additional processing, such as etching the joining surfaces of the ceramic members, plating or brazing the joining surfaces. In addition, these plating and/or brazing processes require the use of expensive metals such as silver and nickel.

As a result, conventional methods have the problem that it is difficult to simplify the joining process and costs increase.

The present invention has been made in view of the above background, and aims to provide a method for manufacturing a bonded body that can bond a ceramic member and a cobalt-containing metal member more easily and at lower cost. In addition, the present invention aims to provide a bonded body in which a ceramic member and a cobalt-containing metal member are bonded, the bonded body not containing metals such as silver and/or nickel.

The present invention provides a method for producing a joined body having a ceramic member and a cobalt-containing metal member, comprising the steps of:
(A-1) a step of placing an aluminum-containing metal member on a joining surface of a ceramic member, the aluminum-containing metal member being placed such that a first organosilicon-based polymer is disposed between the ceramic member and the aluminum-containing metal member;
(A-2) A step of forming an assembly by placing a cobalt-containing metal member on the aluminum-containing metal member, which is carried out following the step (A-1); or (B-1) A step of placing an aluminum-containing metal member on the joining surface of the cobalt-containing metal member;
(A-2) a step, carried out subsequent to the step (A-1), of placing a ceramic member on the aluminum-containing metal member to form an assembly, the ceramic member being placed such that a first organosilicon-based polymer is disposed between the ceramic member and the aluminum-containing metal member;
having
After the step (A-2) or the step (B-2),
(c) heating the assembly to 430° C. or higher in an inert gas atmosphere or a vacuum atmosphere;
having
the first organosilicon polymer has a main chain having Si—O—Si groups;
The cobalt-containing metal component contains 15 mass % or more of cobalt.

The present invention also provides a joined body of a ceramic member and a cobalt-containing metal member, comprising:
The cobalt-containing metal member contains 15 mass % or more of cobalt,
Between the ceramic member and the cobalt-containing metal member, in order from the ceramic member to the cobalt-containing metal member,
an oxide layer including an aluminum-silicon-oxygen oxide;
a bonding layer comprising aluminum and cobalt;
A conjugate is provided, having disposed thereon.

The present invention can provide a method for producing a bonded body that can bond a ceramic member and a cobalt-containing metal member more easily and at lower cost. The present invention can also provide a bonded body in which a ceramic member and a cobalt-containing metal member are bonded together, the bonded body not containing metals such as silver and/or nickel.

FIG. 2 is a diagram showing an example of a cross section of a bonded body according to one embodiment of the present invention. FIG. 11 is a diagram showing an example of a cross section of a bonded body according to another embodiment of the present invention. FIG. 11 is a diagram showing an example of a cross section of a bonded body according to still another embodiment of the present invention. 1 is a diagram illustrating a flow of a method for producing a bonded body according to an embodiment of the present invention. 5A to 5C are diagrams illustrating a flow of a method for producing a bonded body according to another embodiment of the present invention. 1 is a photograph showing an example of a cross section of a bonded body according to an embodiment of the present invention. 13 is a photograph showing an example of a cross section of a bonded structure according to another embodiment of the present invention. 13 is a photograph showing an example of a cross section of a bonded structure according to still another embodiment of the present invention. FIG. 9 is a diagram showing the results of line analysis of a cross section of the bonded body shown in FIG. 8 . 13 is a photograph showing an example of a cross section of a bonded structure according to still another embodiment of the present invention. 11 is a photograph showing an enlarged view of the area enclosed in the frame in FIG. 10 .

One embodiment of the present invention is described below.

As mentioned above, the methods proposed so far for joining ceramic members and cobalt-containing metal members cannot be said to be low-cost and simple.

The inventors of the present application have therefore been actively researching and developing a technology for properly bonding a ceramic member and a cobalt-containing metal member in a simpler and less costly manner. As a result, the inventors of the present application have discovered that by interposing an organosilicon-based polymer and an aluminum-containing metal member between the ceramic member and the cobalt-containing metal member, the ceramic member and the cobalt-containing metal member can be properly bonded together, which led to the present invention.

That is, in one embodiment of the present invention,
A method for manufacturing a joined body having a ceramic member and a cobalt-containing metal member, comprising the steps of:
(A-1) a step of placing an aluminum-containing metal member on a joining surface of a ceramic member, the aluminum-containing metal member being placed such that a first organosilicon-based polymer is disposed between the ceramic member and the aluminum-containing metal member;
(A-2) A step of forming an assembly by placing a cobalt-containing metal member on the aluminum-containing metal member, which is carried out following the step (A-1); or (B-1) A step of placing an aluminum-containing metal member on the joining surface of the cobalt-containing metal member;
(A-2) a step, carried out subsequent to the step (A-1), of placing a ceramic member on the aluminum-containing metal member to form an assembly, the ceramic member being placed such that a first organosilicon-based polymer is disposed between the ceramic member and the aluminum-containing metal member;
having
After the step (A-2) or the step (B-2),
(c) heating the assembly to 430° C. or higher in an inert gas atmosphere or a vacuum atmosphere;
having
the first organosilicon polymer has a main chain having Si—O—Si groups;
The cobalt-containing metal component contains 15 mass % or more of cobalt.

In addition, in one embodiment of the present invention,
A joined body of a ceramic member and a cobalt-containing metal member,
The cobalt-containing metal member contains 15 mass % or more of cobalt,
Between the ceramic member and the cobalt-containing metal member, in order from the ceramic member to the cobalt-containing metal member,
an oxide layer including an aluminum-silicon-oxygen oxide;
a bonding layer comprising aluminum and cobalt;
A conjugate is provided, having disposed thereon.

In this application, "cobalt-containing metal component" means a component made of metallic cobalt or a component made of an alloy containing 15% by mass or more of cobalt.

Also, "aluminum-containing metal component" means a component made of metallic aluminum, or a metal component containing 51% or more by mass of aluminum.

Furthermore, "aluminum-containing metal layer" means a layer containing 51% by mass or more of aluminum. However, as described below, when the "aluminum-containing metal layer" has a matrix and particulate matter dispersed in the matrix, the "aluminum-containing metal layer" has a configuration in which the matrix contains 51% by mass or more of aluminum.

In general, it is difficult to directly join cobalt-containing metal components and ceramic components.

However, in one embodiment of the present invention, an aluminum-containing metal member and an organosilicon-based polymer are used to join the ceramic member and the cobalt-containing metal member, which allows the cobalt-containing metal member and the ceramic member to be appropriately joined.

According to the findings of the present inventors, aluminum can form a good bond with cobalt via a "bonding layer." Therefore, an aluminum-containing metal member and a cobalt-containing metal member can also be bonded to each other via a bonding layer containing aluminum and cobalt formed between them.

This bonding layer is formed by mutual diffusion of components contained in the aluminum-containing metal member and components contained in the cobalt-containing metal member. Therefore, by carrying out heat treatment while the aluminum-containing metal member and the cobalt-containing metal member are in contact with each other, a bonding layer can be formed between the two. Furthermore, the aluminum-containing metal member and the cobalt-containing metal member can be appropriately bonded via this bonding layer.

On the other hand, it is difficult to bond an aluminum-containing metal member and a ceramic member directly to each other. For this reason, in one embodiment of the present invention, an organosilicon-based polymer is interposed between the two. In other words, the organosilicon-based polymer is used to form a good bond between the aluminum-containing metal member and the ceramic member.

The organosilicon-based polymer used in this application has a linear main chain of Si-O-Si groups. For example, the organosilicon-based polymer may be a siloxane-based polymer. Examples of siloxane-based polymers include polymethylhydrosiloxane and polymethylphenylsiloxane.

When such organosilicon-based polymers are heated under an inert atmosphere, they are transformed into silicon-containing compounds that can bond with aluminum and ceramic components in high temperature environments.

Therefore, when a compound containing silicon is formed between a ceramic member and an aluminum-containing metal member in a high-temperature environment, the ceramic member and the aluminum member can be properly joined via the compound containing silicon.

After the bonding process, the organosilicon polymer becomes an aluminum-silicon-oxygen oxide layer, such as an aluminosilicate. In this application, such an oxide layer is referred to as the "oxide layer."

Due to the above effects, in one embodiment of the present invention, a ceramic member and a cobalt-containing metal member can be properly joined.

The above explanation merely describes a phenomenon that may occur based on one mechanism currently under consideration. In other words, in the method for manufacturing a bonded body according to the present invention, a good bond may be formed between the ceramic member and the cobalt-containing metal member as a result of another mechanism.

In the method for manufacturing a joint body according to one embodiment of the present invention, since a complicated process such as a plating process is not performed, the joint body can be manufactured easily. Furthermore, in the method for manufacturing a joint body according to one embodiment of the present invention, since expensive metal materials such as nickel and/or silver are not used, the manufacturing cost can be significantly reduced.

(Conjugate according to one embodiment of the present invention)
Hereinafter, a configuration example of a bonded body according to an embodiment of the present invention will be described in more detail with reference to the drawings.

Figure 1 shows a schematic cross-section of a bonded body according to one embodiment of the present invention (hereinafter referred to as the "first bonded body").

As shown in FIG. 1, the first bonded body 100 has a structure in which a ceramic member 110 and a cobalt-containing metal member 150 are bonded together. More specifically, the first bonded body 100 has a structure in which a ceramic member 110, an oxide layer 120, an aluminum-containing metal layer 130, a bonding layer 140, and a cobalt-containing metal member 150 are laminated in this order.

As mentioned above, the cobalt-containing metal component 150 is made of an alloy containing at least 15% by weight of cobalt. The cobalt-containing metal component 150 may be made of metallic cobalt or a cobalt alloy. One example of a cobalt alloy is KOVAR (17% by weight cobalt-12% by weight nickel-iron alloy).

Also, the aluminum-containing metal layer 130 means a metal layer that contains 51% or more by mass of aluminum.

The oxide layer 120 is an aluminum-silicon-oxygen oxide layer, such as an aluminosilicate.

The bonding layer 140 contains at least aluminum and cobalt. The bonding layer 140 may further contain the major metal elements (except cobalt) contained in the cobalt-containing metal member 150. For example, when the cobalt-containing metal member 150 is KOVAR, the bonding layer 140 may contain iron and nickel. Also, when the aluminum-containing metal layer 130 contains silicon, the bonding layer 140 may further contain silicon.

The first bonded body 100 has an oxide layer 120, an aluminum-containing metal layer 130, and a bonding layer 140 between the ceramic member 110 and the cobalt-containing metal member 150. As described above, the functions of the oxide layer 120 to the bonding layer 140 enable the ceramic member 110 and the cobalt-containing metal member 150 to be bonded properly.

(Conjugate according to another embodiment of the present invention)
Next, with reference to FIG. 2, a configuration example of a bonded body according to another embodiment of the present invention will be described.

Figure 2 shows a schematic cross-section of a bonded body according to another embodiment of the present invention (hereinafter referred to as the "second bonded body").

As shown in FIG. 2, the second bonded body 200 has a structure in which a ceramic member 210, an oxide layer 220, a bonding layer 240, and a cobalt-containing metal member 250 are laminated in this order. That is, the second bonded body 200 has a structure in which the aluminum-containing metal layer 130 is omitted compared to the first bonded body 100.

In practice, the second bonded body 200 is formed in the configuration shown in FIG. 2 by incorporating an aluminum-containing metal component, which serves as the source of the aluminum-containing metal layer, into the oxide layer 220 and the bonding layer 240 during the manufacturing process.

In the second bonded body 200, the oxide layer 220 to the bonding layer 240 are also present between the ceramic member 210 and the cobalt-containing metal member 250. Therefore, in the second bonded body 200, the above-mentioned functions of the oxide layer 220 to the bonding layer 240 allow the ceramic member 210 and the cobalt-containing metal member 250 to be properly bonded together.

(Conjugate according to yet another embodiment of the present invention)
Next, with reference to FIG. 3, a configuration example of a bonded body according to still another embodiment of the present invention will be described.

Figure 3 shows a schematic cross-section of a joint according to yet another embodiment of the present invention (hereinafter referred to as the "third joint").

As shown in FIG. 3, the third bonded body 300 has a structure in which a ceramic member 310, an oxide layer 320, an aluminum-containing metal layer 330, a bonding layer 340, and a cobalt-containing metal member 350 are laminated in this order. That is, the third bonded body 300 has the same layer structure as the first bonded body 100.

However, unlike the first joint body 100, the third joint body 300 contains a plurality of granules 360 inside the aluminum-containing metal layer 330. In other words, the aluminum-containing metal layer 330 has a form in which the granules 360 are dispersed in a matrix of an aluminum-based metal (metallic aluminum or an aluminum alloy).

The shape of the granules 360 is often roughly spherical, but does not necessarily have to be spherical.

These granules 360 contain aluminum and the metal components contained in the cobalt-containing metal component 350. For example, if the cobalt-containing metal component 350 is KOVAR, the granules 360 have a composition that includes aluminum, cobalt, iron, and nickel.

In addition, needle-shaped precipitates may be present inside some of the granules 360. According to the evaluation of the present inventors, when the cobalt-containing metal component 350 is KOVAR, these needle-shaped precipitates present in the aluminum-containing metal layer 330 are thought to be composed of phases containing iron, cobalt, and nickel, and do not contain aluminum.

Here, in the third bonded body 300 as well, the oxide layer 320, the aluminum-containing metal layer 330, and the bonding layer 340 are present between the ceramic member 310 and the cobalt-containing metal member 350. Therefore, in the third bonded body 300 as well, the above-mentioned functions of the oxide layer 320 to the bonding layer 340 allow the ceramic member 310 and the cobalt-containing metal member 350 to be properly bonded together.

(About each component)
Next, each component included in the bonded body according to one embodiment of the present invention will be described in more detail. Note that, here, each component will be described using the first bonded body 100 shown in FIG. 1 as an example. Therefore, the reference symbols shown in FIG. 1 will be used to represent each component. However, it will be clear to those skilled in the art that the following description can be applied as is or with some modifications to the second bonded body 200 and the third bonded body 300.

(Ceramic member 110)
The material of the ceramic member 110 is not particularly limited as long as it is ceramic. The ceramic member 110 may be selected from the group consisting of, for example, alumina, silicon nitride, silicon carbide, mullite, zirconia, forsterite, steatite, cordierite, and ferrite.

The shape of the ceramic member 110 is not particularly limited. The ceramic member 110 may have a shape such as a block, a plate, a rod, or a disk.

(Oxide layer 120)
The oxide layer 120 is primarily composed of an oxide containing aluminum and silicon, and may be, for example, an aluminosilicate.

The thickness of the oxide layer 120 is not particularly limited, but may be, for example, in the range of 10 nm to 100 μm.

(Aluminum-containing metal layer 130)
The aluminum-containing metal layer 130 is a metal layer containing aluminum in an amount of 51 mass % or more. The aluminum-containing metal layer 130 may contain silicon in addition to aluminum.

As previously mentioned, the aluminum-containing metal layer 130 may include particulate matter 360 containing cobalt and aluminum (see FIG. 3).

(Bonding layer 140)
The bonding layer 140 contains at least aluminum and cobalt. The bonding layer 140 may further contain a metal element other than cobalt contained in the cobalt-containing metal member 150. The bonding layer 140 may further contain a metal element other than aluminum contained in the aluminum-containing metal layer 130.

In at least a portion of the bonding layer 140, the concentration of aluminum may continuously decrease toward the cobalt-containing metal member 150. Similarly, metal elements other than aluminum contained in the aluminum-containing metal layer 130 may also exhibit the same behavior as cobalt. For example, when silicon is contained in the bonding layer 140, silicon may exhibit the same concentration change behavior as aluminum.

On the other hand, the cobalt concentration may increase continuously toward the cobalt-containing metal component 150. Metal elements other than cobalt contained in the cobalt-containing metal component 150 may also behave in a similar manner to cobalt.

Also, for example, when the cobalt-containing metal member 150 is KOVAR, the total amount of cobalt, iron, and nickel at the center position of the thickness of the bonding layer 140 may be 20 mass% or more.

(Cobalt-containing metal member 150)
The composition of the cobalt-containing metal member 150 is not particularly limited as long as the cobalt content is 15 mass % or more. The cobalt-containing metal member 150 may be, for example, metallic cobalt or KOVAR (a 17 mass % cobalt-12 mass % nickel-iron alloy).

The shape of the cobalt-containing metal member 150 is not particularly limited. The cobalt-containing metal member 150 may have a shape such as a block, a plate, a rod, or a disk.

(Method of manufacturing a bonded body according to one embodiment of the present invention)
Next, an example of a method for manufacturing a joined body having a ceramic member and a cobalt-containing metal member according to one embodiment of the present invention will be described with reference to FIG.

Figure 4 shows a schematic flow diagram of a method for manufacturing a joint having a ceramic member and a cobalt-containing metal member according to one embodiment of the present invention (hereinafter referred to as the "first manufacturing method").

As shown in FIG. 4, the first manufacturing method includes the following steps:
(A) a step of placing an organosilicon-based polymer on a joining surface of a ceramic member (step S110);
(B) placing an aluminum-containing metal member on the ceramic member on which the organosilicon-based polymer is placed (step S120);
(C) placing a second organosilicon-based polymer on the aluminum-containing metal component (step S130);
(D) placing a cobalt-containing metal component on the aluminum-containing metal component on which the second organosilicon-based polymer has been placed to form an assembly (step S140);
(E) heating the assembly to 430° C. or higher under an inert gas atmosphere or a vacuum atmosphere (step S150);
has.

Note that step S130 is not necessarily a required step and may be omitted.

Each step is explained in detail below.

(Step S110)
This step corresponds to the first half of (A-1) above.

First, the ceramic components are prepared.

The ceramic member is not particularly limited. For example, the ceramic member may be selected from the group consisting of alumina, silicon nitride, silicon carbide, mullite, zirconia, forsterite, steatite, cordierite, and ferrite.

The shape of the ceramic member is not particularly limited, and the ceramic member may have a shape such as a block, plate, rod, or disk.

Next, an organosilicon polymer is applied to the joining surfaces of the ceramic components.

The organosilicon polymer is selected from siloxane polymers whose main chain has a linear Si-O-Si group.

Examples of siloxane-based polymers include polymethylhydrosiloxane, polymethylphenylsiloxane, polydimethylsiloxane, polysilsesquioxane, etc.

The method for applying the organosilicon polymer is not particularly limited. The organosilicon polymer may be applied to the joining surface of the ceramic member by, for example, a coating method. Examples of the coating method include a dipping method, a spin coater method, and a spray method.

(Step S120)
This step corresponds to the latter half of (A-1) above.

Next, an aluminum-containing metal member is placed on top of the ceramic member on which the organosilicon polymer is placed.

The composition of the aluminum-containing metal component is not particularly limited, so long as it contains 51% or more by mass of aluminum.

For example, the aluminum-containing metal member may be metallic aluminum or an aluminum alloy. The aluminum alloy may contain, for example, silicon. The aluminum alloy may be, for example, an aluminum-Si alloy, or may be, for example, silumin containing about 12 mass% silicon.

The shape of the aluminum-containing metal component is not particularly limited, and the aluminum-containing metal component may have a shape such as a block, plate, rod, foil, or disk.

(Step S130)
This step can be included in the above (A-2).

A second organosilicon-based polymer is then placed on top of the aluminum-containing metal member.

The second organosilicon polymer is selected from siloxane polymers having a linear main chain with Si-O-Si groups.

The second organosilicon-based polymer may be the same material as the first organosilicon-based polymer or a different material.

As mentioned above, step S130 is not necessarily an essential step. However, if this step is performed, the second organosilicon-based polymer decomposes during the heat treatment in the subsequent step S150, generating a silane-based gas. When the aluminum-containing metal component comes into contact with this silane-based gas, the oxide film on the surface of the aluminum-containing metal component is easily removed. Therefore, the newly formed surface of the aluminum-containing metal component can be exposed during the joining process.

As mentioned above, aluminum and cobalt tend to bond to each other through an alloy layer formed at the interface. Therefore, if there is little oxide on the surface of the aluminum-containing metal component, the aluminum-containing metal component and the cobalt-containing metal component can be joined more firmly.

(Step S140)
This step corresponds to the above-mentioned part (A-2).

Next, a cobalt-containing metal member is placed on the aluminum-containing metal member on which the second organosilicon-based polymer is placed, forming an assembly.

As mentioned above, the composition of the cobalt-containing metal component is not particularly limited as long as it contains 15 mass% or more of cobalt.

The cobalt-containing metal component may be, for example, cobalt metal or a cobalt alloy. The cobalt alloy may be, for example, a cobalt-iron-nickel based alloy such as KOVAR. KOVAR is an alloy containing 17% by weight cobalt, 12% by weight nickel, and the remainder iron.

The shape of the cobalt-containing metal component is not particularly limited, and the cobalt-containing metal component may have a shape such as a block, plate, rod, foil, or disk.

(Step S150)
This step corresponds to the above step (c).

Next, the assembly formed in step S140 is heat treated for the joining process. This produces a joined body in which the ceramic member and the cobalt-containing metal member are joined.

The heat treatment is carried out in an atmosphere substantially free of oxygen, such as an inert gas atmosphere or a vacuum atmosphere. If the heat treatment is carried out in an oxygen-containing environment, such as an air atmosphere, the oxides on the surface of the aluminum-containing metal member may not be sufficiently reduced. In this case, it may be difficult to obtain good bonding between the ceramic member and the aluminum-containing metal member, and between the aluminum-containing metal member and the cobalt-containing metal member.

The inert gas atmosphere may be, for example, an atmosphere of argon, helium, and/or nitrogen. The degree of vacuum in the vacuum atmosphere is, for example, -0.08 MPa or less when the atmospheric pressure is 0 MPa.

The heat treatment temperature is 430°C or higher. It is preferable that the heat treatment temperature is, for example, 700°C or lower. In particular, it is preferable that the heat treatment temperature is in the range of 540°C to 660°C.

The heat treatment time varies depending on the heat treatment temperature, but may be in the range of, for example, 15 minutes to 2 hours.

Heat treating the assembly changes the organosilicon polymer and forms an oxide layer between the ceramic member and the aluminum-containing metal member.

Typically, the oxide layer is composed of an oxide of the aluminum-silicon-oxygen system.

In addition, by heat treating the assembly, a bonding layer is formed between the aluminum-containing metal component and the cobalt-containing metal component.

This bonding layer is essentially an "alloy layer" formed by mutual diffusion of components contained in the aluminum-containing metal member and components contained in the cobalt-containing metal member, and contains at least aluminum and cobalt.

In addition, at least a portion of this bonding layer has a gradient portion in which the aluminum concentration and the cobalt concentration are gradient.

In the inclined portion, the aluminum concentration gradually decreases toward the cobalt-containing metal component side, while the cobalt concentration gradually increases toward the cobalt-containing metal component side. In the inclined portion, metals other than aluminum contained in the aluminum-containing metal component may also behave in a similar manner to aluminum. Also, metals other than cobalt contained in the cobalt-containing metal component may also behave in a similar manner to cobalt.

For example, if the aluminum-containing metal member contains silicon, the silicon concentration may gradually decrease toward the cobalt-containing metal member. Also, if the cobalt-containing metal member is KOVAR, the iron and nickel concentrations may gradually increase toward the cobalt-containing metal member in the sloped portion of the bonding layer.

In this way, the bonding layer is usually formed as an alloy layer in which the components of the aluminum-containing metal member and the cobalt-containing metal member are mutually diffused. When the cobalt-containing metal member is KOVAR, the sum of the concentrations of cobalt, iron, and nickel in the central portion of the bonding layer thickness may be 20 mass% or more.

Depending on the heat treatment conditions, the aluminum-containing metal components in the assembly may disappear completely. In this case, a structure is obtained in which the bonding layer is disposed directly on the oxide layer (see Figure 2).

The above steps produce a bonded body in which the ceramic member and the cobalt-containing metal member are well bonded.

The first manufacturing method does not require a complicated process such as a plating process, and therefore can easily manufacture a joint body. In addition, the first manufacturing method does not require expensive metal materials such as nickel and/or silver, and therefore can significantly reduce manufacturing costs.

In the first manufacturing method, the organosilicon polymer is placed on the ceramic member in step S110. Then, an aluminum-containing metal member is placed on the ceramic member.

However, alternatively, an organosilicon polymer may be applied to the aluminum-containing metal component at the required location, and then the aluminum-containing metal component may be placed on the ceramic component.

In other words, the timing of application of the organosilicon-based polymer is not particularly limited, and the organosilicon-based polymer may be applied to either the ceramic member or the aluminum-containing metal member. Alternatively, the organosilicon-based polymer may be applied to both the ceramic member and the aluminum-containing metal member, and then the two members may be superimposed.

In the first manufacturing method, the second organosilicon-based polymer is placed on the aluminum-containing metal member in step S130. Then, the cobalt-containing metal member is placed on the aluminum-containing metal member.

Alternatively, however, a second organosilicon-based polymer may be applied to the corresponding portion of the cobalt-containing metal component, and then the cobalt-containing metal component may be applied over the aluminum-containing metal component.

This process corresponds to steps (a-1) and (a-2) above.

That is, the timing of application of the second organosilicon-based polymer is not particularly limited, and the second organosilicon-based polymer may be applied to either the aluminum-containing metal member or the cobalt-containing metal member. Alternatively, the second organosilicon-based polymer may be applied to both the aluminum-containing metal member and the cobalt-containing metal member, and then the two members may be superimposed on each other.

It will be clear to those skilled in the art that various other modifications are possible.

(Method of manufacturing a bonded body according to another embodiment of the present invention)
Next, an example of a method for manufacturing a joined body having a ceramic member and a cobalt-containing metal member according to another embodiment of the present invention will be described with reference to FIG.

Figure 5 shows a schematic flow diagram of a method for manufacturing a joint having a ceramic member and a cobalt-containing metal member according to another embodiment of the present invention (hereinafter referred to as the "second manufacturing method").

As shown in FIG. 5, the second manufacturing method includes the following steps:
(A) applying a slurry containing an organosilicon polymer and an aluminum-containing metal member to a joining surface of a ceramic member (step S210);
(B) placing a cobalt-containing metal component on the slurry containing the organosilicon polymer and the aluminum-containing metal component to form an assembly (step S220);
(C) heating the assembly to 430° C. or higher under an inert gas atmosphere or a vacuum atmosphere (step S230);
has.

The second manufacturing method can be particularly useful when the aluminum-containing metal component is in particulate form. Therefore, in the following description, each step will be explained using the example of the aluminum-containing metal component in particulate form.

However, it will be apparent to those skilled in the art that the second manufacturing method can be similarly applied to aluminum-containing metal components in the form of blocks, plates, rods, foils, disks, etc.

(Step S210)
This step corresponds to the above-mentioned part (A-1).

First, a ceramic member is prepared as described in the first manufacturing method. An aluminum-containing metal member is also prepared. The aluminum-containing metal member may have a composition as described above.

As described above, the aluminum-containing metal component used in the second manufacturing method is particulate. The particulate aluminum-containing metal component has an average particle size in the range of 1 μm to 500 μm, for example. The average particle size is preferably in the range of 5 μm to 100 μm.

Next, the particulate aluminum-containing metal components are thoroughly mixed with the organosilicon polymer to prepare a slurry.

If the organosilicon polymer is liquid, a solvent may be used when preparing the slurry, although this is not necessarily required.

The solvent may be, for example, an alcohol such as methanol and ethanol, or an organic solvent such as an ester.

Next, the prepared slurry is applied to the joining surfaces of the ceramic components.

The method of applying the slurry is not particularly limited. For example, the slurry may be applied to the joining surface of the ceramic member or the cobalt-containing metal member by a method such as screen printing.

(Step S220)
This step corresponds to the above-mentioned part (A-2).

Next, a cobalt-containing metal component is placed on top of the slurry applied to the joining surfaces of the ceramic components to form an assembly.

(Step S230)
This step corresponds to the above step (c).

Next, the assembly is heat treated to produce a bonded body. The heat treatment conditions are the same as those in the first manufacturing method described above.

By heat treatment, the organosilicon polymer contained in the slurry reacts with the particulate aluminum-containing metal member to form an oxide layer between the ceramic member and the aluminum-containing metal member. As mentioned above, in most cases, the oxide layer is composed of an aluminum-silicon-oxygen oxide.

In addition, by heat treating the assembly, an interdiffusion reaction between cobalt and aluminum occurs on the surface of the cobalt-containing metal component that comes into contact with the slurry, forming the bonding layer described above.

Furthermore, an aluminum-containing metal layer is formed from particles of the particulate aluminum-containing metal components contained in the initial slurry that were not used in the reaction.

As a result, the ceramic member and the cobalt-containing metal member are joined via the oxide layer and the joining layer, and a joined body can be produced.

Here, when particulate aluminum-containing metal components are used in the second manufacturing method, there is a high tendency for a bonded body having the configuration shown in Figure 3 described above to be manufactured.

In other words, a structure is obtained in which particles containing cobalt and aluminum are dispersed in the matrix of the aluminum-containing metal layer.

It will be clear to those skilled in the art that the second manufacturing method provides the same advantages as the first manufacturing method.

In other words, the second manufacturing method also makes it possible to easily manufacture a joint body. Furthermore, the second manufacturing method does not use expensive metal materials such as nickel and/or silver, so manufacturing costs can be significantly reduced.

In the second manufacturing method, instead of steps S210 to S220, a slurry containing an aluminum-containing metal member may be applied to the joining surface of the cobalt-containing metal member, and then a ceramic member may be placed on the joining surface of the cobalt-containing metal member on which the slurry has been applied, to form an assembly.

This process corresponds to parts (a-1) and (a-2) above.

The above describes the methods for manufacturing a bonded body using the first and second manufacturing methods as examples. However, the above description is merely an example, and it will be clear to those skilled in the art that similar effects can be obtained by modifying part of the above-mentioned method or adding other steps.

For example, in the above description, the joined body is manufactured by first preparing the ceramic member and then sequentially placing the necessary members on top of it. However, the joined body may also be manufactured by the opposite process, that is, first preparing the cobalt-containing metal member and then sequentially placing the necessary members on top of it.

The following describes examples of the present invention. However, the present invention is not limited to these examples.

(Example 1)
A bonded body of a ceramic member and a cobalt-containing metal member was produced by the following method.

First, an alumina plate (purity 90% or more) with dimensions of 20 mm length x 20 mm width x 0.32 mm thickness was prepared as the ceramic member. A pure cobalt plate (manufactured by Nilaco Corporation) with dimensions of 15 mm length x 15 mm width x 1 mm thickness was prepared as the cobalt-containing metal member. Furthermore, a pure aluminum plate (manufactured by Nilaco Corporation) with dimensions of 10 mm length x 10 mm width x 0.1 mm thickness was prepared as the aluminum-containing metal member.

Next, the aluminum-containing metal component was immersed in a polysiloxane (KF-54; manufactured by Shin-Etsu Silicones) solution, and polysiloxane was applied to both sides of the aluminum-containing metal component.

Next, an aluminum-containing metal member and a cobalt-containing metal member were placed in this order on the joining surface of the ceramic member (one surface measuring 20 mm long x 20 mm wide) to form an assembly.

Next, the resulting assembly was heat-treated. The heat treatment conditions were 700°C in an inert atmosphere for 15 minutes. This resulted in a bonded body. Hereinafter, this bonded body will be referred to as "bonded body according to Example 1."

In the bonded body of Example 1, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 2)
A bonded body of a ceramic member and a cobalt-containing metal member was produced by the following method.

As the ceramic member, a silicon nitride plate (purity 90% or more) with dimensions of 20 mm length x 20 mm width x 0.32 mm thickness was prepared. As the cobalt-containing metal member, a pure cobalt plate (manufactured by Nilaco Corporation) with dimensions of 15 mm length x 15 mm width x 1 mm thickness was prepared. As the aluminum-containing metal member, a silumin (aluminum-12 wt% Si alloy) plate with dimensions of 10 mm length x 5 mm width x 0.08 mm thickness was prepared.

Next, polysiloxane (YR-3370; manufactured by Momentive Performance Japan) was dissolved in an ethanol solvent to prepare a solution. The concentration of polysiloxane in the solution was 0.1 mol/L.

Next, an aluminum-containing metal component was immersed in the solution, and polysiloxane was applied to both sides of the aluminum-containing metal component.

Next, an aluminum-containing metal member and a cobalt-containing metal member were placed in that order on the joining surface of the ceramic member (one surface measuring 20 mm long x 20 mm wide) to form an assembly.

Next, the resulting assembly was heat-treated. The heat treatment conditions were 580°C and 60 minutes in an inert atmosphere. This resulted in a bonded body. Hereinafter, this bonded body will be referred to as "bonded body according to Example 2."

In the bonded body of Example 2, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 3)
In the same manner as in Example 1, a joint consisting of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 3, a silicon carbide plate (with a purity of 70% or more) having dimensions of 10 mm length x 10 mm width x 5 mm thickness was used as the ceramic member, and a samarium-cobalt magnet (cobalt content 66% by mass; manufactured by Santoku Co., Ltd.) having dimensions of 5 mm length x 5 mm width x 3 mm thickness was used as the cobalt-containing metal member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 3."

In the bonded body of Example 3, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 4)
In the same manner as in Example 3, a joint consisting of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 4, an alumina plate (with a purity of 90% or more) was used as the ceramic member, and a silumin (aluminum-12 wt% Si alloy) plate was used as the aluminum-containing metal member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 4."

In the bonded body of Example 4, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 5)
In the same manner as in Example 1, a joint consisting of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 5, KOVAR plate (cobalt content 17% by mass; manufactured by Nilaco Corporation) was used as the cobalt-containing metal member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 5."

In the bonded body of Example 5, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 6)
In the same manner as in Example 5, a joint of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 6, a silumin (aluminum-12 wt% Si alloy) plate with dimensions of 10 mm length x 5 mm width x 0.08 mm thickness was used as the aluminum-containing metal member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 6."

In the bonded body of Example 6, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 7)
In the same manner as in Example 6, a joint consisting of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 7, silicon carbide (with a purity of 70% or more) with dimensions of 10 mm length x 10 mm width x 5 mm thickness was used as the ceramic member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 7."

In the bonded body of Example 7, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 8)
A bonded body of a ceramic member and a cobalt-containing metal member was produced by the following method.

First, an alumina plate (purity 90% or more) with dimensions of 20 mm length x 20 mm width x 0.32 mm thickness was prepared as the ceramic member. In addition, a KOVAR plate (cobalt content 17% by mass; manufactured by Nilaco Corporation) with dimensions of 15 mm length x 15 mm width x 1 mm thickness was used as the cobalt-containing metal member.

The aluminum-containing metal component was made using a slurry containing -63 μm silumin powder (aluminum-12 wt% Si alloy, product name: silumin alloy; manufactured by Mitsuwa Chemicals).

Next, the silumin powder was added to the solvent and thoroughly stirred to prepare a slurry. The solvent was prepared by dissolving polysiloxane (YR-3370; manufactured by Momentive Performance Japan) in 2-(2-n-butoxyethoxy)ethyl acetate. The concentration of silumin powder in the slurry was 65% by mass.

Next, the aforementioned slurry was applied to the joining surface of the ceramic member (one surface measuring 20 mm long x 20 mm wide), and a cobalt-containing metal member was placed on top to form an assembly.

Next, the resulting assembly was heat-treated. The heat treatment conditions were 700°C and 15 minutes in an inert atmosphere. This resulted in a bonded body. Hereinafter, this bonded body will be referred to as "bonded body according to Example 8."

In the bonded body of Example 8, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 9)
In the same manner as in Example 8, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 9, aluminum powder (average particle size 5 μm, purity 99%) was used as the aluminum-containing metal component in the slurry. The concentration of aluminum powder in the slurry was 65 mass%.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 9."

In the bonded body of Example 9, the ceramic member and the cobalt-containing metal member were bonded well.

The same experiment was carried out with the aluminum powder in the paste having an average particle size of 10 μm, and similar results were obtained.

(Example 10)
In the same manner as in Example 8, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 10, a mullite plate having dimensions of 15 mm length x 15 mm width x 2 mm thickness was used as the ceramic member. Also, aluminum powder (average particle size 5 μm, purity 99%) was used as the aluminum-containing metal member in the slurry.

Furthermore, the heat treatment conditions were 700°C and 60 minutes in an inert atmosphere. As a result, a bonded body was obtained. Hereinafter, this bonded body is referred to as "bonded body according to Example 10."

In the bonded body of Example 10, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 11)
In the same manner as in Example 10, a joint of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 11, a zirconia plate was used as the ceramic member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 11."

In the bonded body of Example 11, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 12)
In the same manner as in Example 10, a joint of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 12, a forsterite plate was used as the ceramic member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 12."

In the bonded body of Example 12, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 13)
In the same manner as in Example 10, a joint of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 13, a steatite plate was used as the ceramic member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 13."

In the bonded body of Example 13, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 14)
In the same manner as in Example 10, a joint of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 14, a cordierite plate was used as the ceramic member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 14."

In the bonded body of Example 14, the ceramic member and the cobalt-containing metal member were bonded well.

(Example 15)
In the same manner as in Example 10, a joint of a ceramic member and a cobalt-containing metal member was produced.

However, in this Example 15, a ferrite plate was used as the ceramic member.

After heat treatment of the assembly, a joint was obtained. Hereinafter, this joint is referred to as "joint relating to Example 15."

In the bonded body of Example 15, the ceramic member and the cobalt-containing metal member were bonded well.

The manufacturing conditions for each joint are summarized in Table 1 below.

（評価）
各例に係る接合体を用いて、各種評価を実施した。

(evaluation)
Using the joints according to each example, various evaluations were carried out.

First, a cross section of the bonded body of Example 2 was observed using a scanning electron microscope.

Figure 6 shows an example of a cross section of the joint in Example 2.

In the case of the bonded body of Example 2, it was found that the aluminum-containing metal member had almost completely disappeared. In other words, it was found that the bonded body had a cross-sectional configuration as shown in Figure 2 above, with the ceramic member, oxide layer, bonding layer, and cobalt-containing metal member arranged in that order.

No defects, particularly cracks or voids, were found in the oxide layer or bonding layer.

An elemental analysis of the oxide layer was performed using a simple elemental analyzer. As a result, it was found that the oxide layer contained an aluminosilicate phase. It was also found that the bonding layer contained both aluminum and cobalt.

It was found that in part of the bonding layer, the aluminum concentration continuously decreased toward the cobalt-containing metal component, and conversely, the cobalt concentration continuously increased toward the cobalt-containing metal component.

Almost the same results were obtained with the joint in Example 1.

On the other hand, in the case of the bonded body of Example 5, the layer structure of the bonded body has a cross-sectional structure as shown in Figure 1 above, and it was found to be composed of, in order from the ceramic member side, an oxide layer, an aluminum-containing metal layer, a bonding layer, and a cobalt-containing metal member.

No defects, particularly cracks or voids, were found in the oxide layer or bonding layer.

Elemental analysis of the oxide layer was performed using a simple elemental analyzer. The results showed that the oxide layer contained an aluminosilicate phase. It was also found that the bonding layer contained iron and nickel in addition to aluminum and cobalt.

In part of the bonding layer, it was found that the aluminum concentration continuously decreased toward the cobalt-containing metal component, while the concentrations of cobalt, iron, and nickel continuously increased toward the cobalt-containing metal component.

Figure 7 shows an example of a cross section of the joint according to Example 6.

In the case of the joint in Example 6, it was found that the aluminum-containing metal member had almost completely disappeared. In other words, the joint had a cross-sectional configuration as shown in Figure 2 above.

No defects, particularly cracks or voids, were found in the oxide layer or bonding layer.

Elemental analysis of the oxide layer was performed using a simple elemental analyzer. The results showed that the oxide layer contained an aluminosilicate phase. Additionally, the bonding layer was found to contain aluminum, silicon, cobalt, iron, and nickel.

In some parts of the bonding layer, the concentrations of aluminum and silicon decreased continuously toward the cobalt-containing metal component. Conversely, the concentrations of cobalt, iron, and nickel were found to increase continuously toward the cobalt-containing metal component.

Figure 8 shows an example of a cross section of the joint according to Example 7.

In the case of the bonded body of Example 7, the layer structure of the bonded body has a cross-sectional structure as shown in Figure 1 above, and it was found to be composed of, in order from the ceramic member side, an oxide layer, an aluminum-containing metal layer, a bonding layer, and a cobalt-containing metal member.

No defects, particularly cracks or voids, were found in the oxide layer or bonding layer.

Elemental analysis of the oxide layer was performed using a simple elemental analyzer. The results showed that the oxide layer contained an aluminosilicate phase. Additionally, the bonding layer was found to contain aluminum, silicon, cobalt, iron, and nickel.

Figure 9 shows the results of line analysis of the cross section of the joint of Example 7. In the figure, the horizontal axis corresponds to each cross section position in Figure 8. For example, point A is approximately the center of the thickness of the aluminum-containing metal layer, point B1 is approximately the interface between the aluminum-containing metal layer and the joint layer, point B2 is a position inside the joint layer, point B3 is approximately the interface between the joint layer and the cobalt-containing metal member, and point C is a position inside the cobalt-containing metal member.

From these results, it can be seen that in the bonding layer, at least in the region from point B1 to point B2, the aluminum concentration gradually decreases toward the cobalt-containing metal component. Conversely, in the same region, the concentrations of cobalt, iron, and nickel gradually increase toward the cobalt-containing metal component.

For the bonded body of Example 7, element concentration analysis was performed at approximately the center position of the thickness of the bonded layer (see point D in Figure 8). The results are shown in Table 2.

接合層の厚さの略中央部分では、コバルト＋鉄＋ニッケルの含有量は、２０質量％を超えることがわかった。

It was found that the cobalt+iron+nickel content exceeded 20 mass % at approximately the center of the thickness of the bonding layer.

Figure 10 shows an example of a cross section of the bonded body according to Example 8. Figure 11 shows an enlarged photograph of the area enclosed by the square in Figure 10.

In the case of the bonded body of Example 8, the layer structure of the bonded body has a cross-sectional structure as shown in Figure 3 described above, and it was found to be composed of, in order from the ceramic member side, an oxide layer, an aluminum-containing metal layer, a bonding layer, and a cobalt-containing metal member.

It was also confirmed that the aluminum-containing metal layer contained roughly spherical granules, and as shown in Figure 11, it was found that needle-shaped precipitates were formed inside some of the spherical granules.
The roughly spherical particles were subjected to elemental analysis, and the results are shown in Table 3 below.

表３から、略球状の粒状物は、アルミニウム、コバルト、鉄、およびニッケルを含むことが確認された。

From Table 3, it was confirmed that the approximately spherical particles contained aluminum, cobalt, iron, and nickel.

Elemental analysis of the oxide layer was performed using a simple elemental analyzer. As a result, it was found that the oxide layer contained an aluminosilicate phase.

The bonding layer was also found to contain aluminum, silicon, cobalt, iron and nickel. Table 4 below shows the elemental analysis results measured at point E in Figure 10.

例８に係る接合体においても、酸化物層および接合層には、特にクラックやボイド等の欠陥は認められなかった。

In the bonded body of Example 8, no defects such as cracks or voids were observed in the oxide layer and the bonding layer.

Table 5 below shows the cross-sectional structure of the joints in each example.

表５において、「Ｉ」は、前述の図１に示したような、アルミニウム含有金属層を含む断面構造を意味する。また、「ＩＩ」は、前述の図２に示したような、アルミニウム含有金属層が実質的に認められない断面構造を意味し、「ＩＩＩ」は、前述の図３に示したような、アルミニウム含有金属層の内部に球状の粒状物が分散された断面構造を意味する。

In Table 5, "I" refers to a cross-sectional structure including an aluminum-containing metal layer as shown in Figure 1. "II" refers to a cross-sectional structure in which an aluminum-containing metal layer is not substantially observed as shown in Figure 2, and "III" refers to a cross-sectional structure in which spherical particles are dispersed within the aluminum-containing metal layer as shown in Figure 3.

As described above, it was found that there were three types of cross-sectional layer structures in the bonded bodies of Examples 1 to 15. It was also confirmed that in the bonded bodies of Examples 1 to 15, the ceramic member and the cobalt-containing metal member were well bonded via the layer between them.

In addition, measurements using a simplified elemental analyzer confirmed that the aluminum content in the aluminum-containing metal layer exceeded 51 mass% in each of the joints of Example 2, Example 7, and Example 8.

(Example 16)
A bonded body in which a cobalt-containing metal member was disposed on both sides of a ceramic member was produced by the following method.

First, an alumina plate (purity 90% or more) with dimensions of 20 mm length x 20 mm width x 0.32 mm thickness was prepared as the ceramic member. In addition, two KOVAR plates (cobalt content 17% by mass; manufactured by Nilaco Corporation) with dimensions of 15 mm length x 15 mm width x 1 mm thickness were prepared as the cobalt-containing metal member (referred to as "cobalt-containing metal member A" and "cobalt-containing metal member B" respectively). Furthermore, two pure aluminum plates (manufactured by Nilaco Corporation) with dimensions of 10 mm length x 10 mm width x 0.1 mm thickness were prepared as the aluminum-containing metal member (referred to as "aluminum-containing metal member A" and "aluminum-containing metal member B" respectively).

Next, the aluminum-containing metal member A was immersed in the first solution. The aluminum-containing metal member B was immersed in the second solution. The first solution was a polysiloxane K (KF-54; manufactured by Shin-Etsu Silicones). The second solution was prepared by dissolving polysiloxane H (H44; manufactured by Wacker Chemie) in an ethanol solvent. The concentration of polysiloxane H in the second solution was 0.1 mol/L.

Next, an aluminum-containing metal member A and a cobalt-containing metal member A were placed in this order on one of the joining surfaces of the ceramic member (surface measuring 20 mm long x 20 mm wide). An aluminum-containing metal member B and a cobalt-containing metal member B were placed in this order on the other joining surface of the ceramic member (surface measuring 20 mm long x 20 mm wide), forming an assembly.

Next, the resulting assembly was heat-treated. The heat treatment conditions were 700°C and 15 minutes in an inert atmosphere. This resulted in a bonded body. Hereinafter, this bonded body will be referred to as "bonded body according to Example 16."

In the bonded body of Example 16, both the ceramic member and the cobalt-containing metal member A, and the ceramic member and the cobalt-containing metal member B were bonded well.

(Example 17)
A joint in which ceramic members were disposed on both sides of a cobalt-containing metal member was produced by the following method.

First, two silicon nitride plates (purity 90% or more) with dimensions of 20 mm length x 20 mm width x 0.32 mm thickness were prepared as ceramic members (referred to as "ceramic member A" and "ceramic member B" respectively). In addition, a KOVAR plate (cobalt content 17% by mass; manufactured by Nilaco Corporation) with dimensions of 15 mm length x 15 mm width x 1 mm thickness was prepared as a cobalt-containing metal member. Furthermore, two pure aluminum plates (manufactured by Nilaco Corporation) with dimensions of 10 mm length x 10 mm width x 0.1 mm thickness were prepared as aluminum-containing metal members (referred to as "aluminum-containing metal member C" and "aluminum-containing metal member D" respectively).

Next, aluminum-containing metal member C and aluminum-containing metal member D were each immersed in a polysiloxane (KF-54; manufactured by Shin-Etsu Silicones) solution.

Next, an aluminum-containing metal member C and a ceramic member A were placed in this order on one of the joining surfaces (a surface measuring 20 mm long x 20 mm wide) of the cobalt-containing metal member. An aluminum-containing metal member D and a ceramic member B were placed in this order on the other joining surface (a surface measuring 15 mm long x 15 mm wide) of the cobalt-containing metal member to form an assembly.

Next, the resulting assembly was heat-treated. The heat treatment conditions were 700°C and 15 minutes in an inert atmosphere. This resulted in a bonded body. Hereinafter, this bonded body will be referred to as "bonded body according to Example 17."

In the bonded body of Example 17, the cobalt-containing metal member and ceramic member A, and the cobalt-containing metal member and ceramic member B were both bonded well.

REFERENCE SIGNS LIST 100 First bonded body 110 Ceramic member 120 Oxide layer 130 Aluminum-containing metal layer 140 Bonding layer 150 Cobalt-containing metal member 200 Second bonded body 210 Ceramic member 220 Oxide layer 240 Bonding layer 250 Cobalt-containing metal member 300 Third bonded body 310 Ceramic member 320 Oxide layer 330 Aluminum-containing metal layer 340 Bonding layer 350 Cobalt-containing metal member 360 Particulate matter

Claims (15)

A method for manufacturing a joined body having a ceramic member and a cobalt-containing metal member, comprising the steps of:
(A-1) a step of placing an aluminum-containing metal member on a joining surface of a ceramic member, the aluminum-containing metal member being placed such that a first organosilicon-based polymer is disposed between the ceramic member and the aluminum-containing metal member;
(A-2) A step of forming an assembly by placing a cobalt-containing metal member on the aluminum-containing metal member, which is carried out following the step (A-1); or (B-1) A step of placing an aluminum-containing metal member on the joining surface of the cobalt-containing metal member;
(A-2) a step, carried out subsequent to the step (A-1), of placing a ceramic member on the aluminum-containing metal member to form an assembly, the ceramic member being placed such that a first organosilicon-based polymer is disposed between the ceramic member and the aluminum-containing metal member;
having
After the step (A-2) or the step (B-2),
(c) heating the assembly to 430° C. or higher in an inert gas atmosphere or a vacuum atmosphere;
having
the first organosilicon polymer has a main chain having Si—O—Si groups;
The cobalt-containing metal component contains 15 mass % or more of cobalt. In the step (A-2), the cobalt-containing metal member is disposed such that a second organosilicon-based polymer is disposed between the aluminum-containing metal member and the cobalt-containing metal member; or, in the step (A-1), the aluminum-containing metal member is disposed such that a second organosilicon-based polymer is disposed between the aluminum-containing metal member and the cobalt-containing metal member;
The method according to claim 1 , wherein the second organosilicon polymer has a main chain having Si—O—Si groups. The method of claim 2, wherein the second organosilicon-based polymer is the same as the first organosilicon-based polymer. The aluminum-containing metal member is in a plate or powder form ,
When the aluminum-containing metal member is in the form of a plate, in the step (A-1), the aluminum-containing metal member is immersed in a liquid containing the first organosilicon polymer and then placed on the ceramic member ;
4. The method according to claim 1, wherein when the aluminum-containing metal member is in powder form, the step (A-1) is carried out by applying a slurry containing the first organosilicon polymer and the aluminum-containing metal member to the joining surface of the ceramic member . The aluminum-containing metal member is in a plate or powder form ,
When the aluminum-containing metal member is in the form of a plate, in the step (a-1), the aluminum-containing metal member is immersed in a liquid containing the second organosilicon-based polymer and then placed on the cobalt-containing metal member ;
4. The method according to claim 2 or 3, wherein when the aluminum-containing metal member is in powder form, the step (i-1) is carried out by applying a slurry containing the second organosilicon-based polymer and the aluminum-containing metal member to the joining surface of the cobalt-containing metal member . The method according to any one of claims 1 to 5 , wherein the cobalt-containing metal component is a cobalt-iron-nickel based alloy component. The method according to claim 1 , wherein the aluminum-containing metal component comprises an aluminum alloy containing 51 mass % or more of aluminum. The method according to claim 1 , wherein the ceramic member is selected from the group consisting of alumina, silicon nitride, silicon carbide, mullite, zirconia, forsterite, steatite, cordierite, and ferrite. A joined body of a ceramic member and a cobalt-containing metal member,
The cobalt-containing metal member contains 15 mass % or more of cobalt,
Between the ceramic member and the cobalt-containing metal member, in order from the ceramic member to the cobalt-containing metal member,
an oxide layer including an aluminum-silicon-oxygen oxide;
a bonding layer comprising aluminum and cobalt;
are arranged in a junction. The joined body according to claim 9 , wherein in at least a portion of the joining layer, the aluminum concentration decreases while the cobalt concentration increases toward the cobalt-containing metal member. The joined body according to claim 9 or 10 , wherein the cobalt-containing metal member is a cobalt-iron-nickel based alloy member. 12. The joined body according to claim 11 , wherein the total amount of cobalt, iron, and nickel at a center position in the thickness of the joining layer is 20 mass % or more. The bonded body according to claim 9 , further comprising an aluminum-containing metal layer between the oxide layer and the bonding layer. 14. The joined body according to claim 13 , wherein particulate matter containing aluminum and cobalt is dispersed in the aluminum-containing metal layer. 15. The joined body according to claim 9 , wherein the ceramic member is selected from the group consisting of alumina, silicon nitride, silicon carbide, mullite, zirconia, forsterite, steatite, cordierite, and ferrite.

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