Method for manufacturing a bonded body and a bonded body

Abstract

To provide a method for manufacturing a joined body in which a ceramic member and a cobalt-containing metal member may be simply joined at low cost.SOLUTION: A method of manufacturing a joined body having a ceramic member and a cobalt-containing metal member comprises (1) a step of installing an aluminum-containing metal member on a joint surface of a ceramic member in which the aluminum-containing metal member is installed so that an organosilicon-based polymer is arranged between the ceramic member and the aluminum-containing metal member, and the main chain of the organosilicon-based polymer has a Si-O-Si group, (2) a step of installing a cobalt-containing metal member having 15 mass% or more of cobalt on the aluminum-containing metal member to form an assembly, and (3) a step of heating the assembly to 430°C or more under an inert gas atmosphere or a vacuum atmosphere.SELECTED DRAWING: Figure 4

Description

[Technical field]

[0001] The present invention relates to a method for producing a bonded body and to a bonded body. [Background technology]

[0002] Several methods have been proposed so far as techniques for joining a ceramic member and a cobalt-containing metal member.

[0003] For example, Patent Document 1 proposes a method in which a nickel plating layer is provided on a pre-etched surface of a ceramic member, a silver brazing material is provided on the plating layer, and then the ceramic member and a cobalt-based alloy member are brazed via the silver brazing material.

[0004] Furthermore, Patent Document 2 proposes a method of joining a ceramic member and a cobalt-based alloy member by performing heat treatment in a state in which a nickel-containing foil is placed between the ceramic member and the cobalt-based alloy member. [Prior art documents] [Patent documents]

[0005] [Patent Document 1] Japanese Unexamined Patent Publication No. 60-081072 [Patent Document 2] Japanese Patent Application Laid-Open No. 63-060170 Summary of the Invention [Problem to be solved by the invention]

[0006] Conventional methods require additional processing such as etching the joining surfaces of the ceramic members, plating or brazing the joining surfaces, and the plating and / or brazing processes require the use of expensive metals such as silver and nickel.

[0007] For this reason, in the conventional method, it is difficult to simplify the joining process, and the cost increases.

[0008] The present invention has been made in view of the above background, and an object of the present invention is to provide a method for producing a joined body capable of joining a ceramic member and a cobalt-containing metal member more easily and at lower cost. Another object of the present invention is to provide a joined body in which a ceramic member and a cobalt-containing metal member are joined together, the joined body not containing a metal such as silver and / or nickel. [Means for solving the problem]

[0009] 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 placing a cobalt-containing metal member on the aluminum-containing metal member to form an assembly, which is carried out subsequent to the step (A-1); or (A-1) a step of placing an aluminum-containing metal member on a joining surface of a cobalt-containing metal member; (a-2) a step, carried out subsequent to the step (a-1), of forming an assembly by placing a ceramic member on the aluminum-containing metal member, 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.

[0010] 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. Effect of the Invention

[0011] The present invention can provide a method for producing a joined body capable of joining a ceramic member and a cobalt-containing metal member more simply and at lower cost. Also, the present invention can provide a joined body in which a ceramic member and a cobalt-containing metal member are joined together, the joined body not including a metal such as silver and / or nickel. [Brief description of the drawings]

[0012] [Figure 1] FIG. 2 is a diagram showing an example of a cross section of a bonded body according to one embodiment of the present invention. [Diagram 2] FIG. 11 is a diagram showing an example of a cross section of a bonded body according to another embodiment of the present invention. [Diagram 3] 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. [Figure 4] 1 is a diagram illustrating a flow of a method for producing a bonded body according to an embodiment of the present invention. [Diagram 5] 5A to 5C are diagrams illustrating a flow of a method for producing a bonded body according to another embodiment of the present invention. [Figure 6] 1 is a photograph showing an example of a cross section of a bonded body according to an embodiment of the present invention. [Figure 7] 13 is a photograph showing an example of a cross section of a bonded structure according to another embodiment of the present invention. [Figure 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. [Figure 9] FIG. 9 is a diagram showing the results of line analysis of a cross section of the bonded body shown in FIG. [Figure 10] 13 is a photograph showing an example of a cross section of a bonded structure according to still another embodiment of the present invention. [Figure 11] 11 is a photograph showing an enlarged view of the area within the frame in FIG. 10. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0013] Hereinafter, one embodiment of the present invention will be described.

[0014] As described above, it is difficult to say that the methods proposed so far for joining a ceramic member and a cobalt-containing metal member are low-cost and simple.

[0015] Therefore, the inventors of the present application have been actively engaged in research and development into a technique for properly bonding a ceramic member and a cobalt-containing metal member in a simpler and less costly manner, and as a result, the inventors of the present application have discovered that the ceramic member and the cobalt-containing metal member can be properly bonded by interposing an organosilicon-based polymer and an aluminum-containing metal member between the ceramic member and the cobalt-containing metal member, thereby arriving at the present invention.

[0016] 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 placing a cobalt-containing metal member on the aluminum-containing metal member to form an assembly, which is carried out subsequent to the step (A-1); or (A-1) a step of placing an aluminum-containing metal member on a joining surface of a cobalt-containing metal member; (a-2) a step, carried out subsequent to the step (a-1), of forming an assembly by placing a ceramic member on the aluminum-containing metal member, 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.

[0017] 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.

[0018] In this application, the term "cobalt-containing metal component" refers to a component made of metallic cobalt or a component made of an alloy containing 15 mass % or more of cobalt.

[0019] Moreover, the term "aluminum-containing metal component" refers to a component made of metallic aluminum, or a metal component containing 51 mass % or more of aluminum.

[0020] Furthermore, the term "aluminum-containing metal layer" refers to 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 structure in which the matrix contains 51% by mass or more of aluminum.

[0021] In general, it is difficult to directly bond a cobalt-containing metal member and a ceramic member.

[0022] 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, thereby enabling the cobalt-containing metal member and the ceramic member to be appropriately joined.

[0023] 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.

[0024] The bonding layer is formed by mutual diffusion of the components contained in the aluminum-containing metal member and the components contained in the cobalt-containing metal member. Therefore, a bonding layer can be formed between the aluminum-containing metal member and the cobalt-containing metal member by carrying out a heat treatment while the aluminum-containing metal member and the cobalt-containing metal member are in contact with each other. The aluminum-containing metal member and the cobalt-containing metal member can be appropriately bonded to each other through the bonding layer.

[0025] On the other hand, it is difficult to directly bond an aluminum-containing metal member to a ceramic member. For this reason, in one embodiment of the present invention, an organosilicon-based polymer is interposed between the two. That is, the organosilicon-based polymer is used to form a good bond between the aluminum-containing metal member and the ceramic member.

[0026] The organosilicon polymer used in the present application has a linear main chain of Si-O-Si groups. For example, the organosilicon polymer may be a siloxane polymer. Examples of siloxane polymers include polymethylhydrosiloxane and polymethylphenylsiloxane.

[0027] Such organosilicon-based polymers, when heated under an inert atmosphere, are transformed into silicon-containing compounds that are capable of bonding with aluminum and ceramic components in high temperature environments.

[0028] 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.

[0029] After the bonding process, the organosilicon polymer becomes an aluminum-silicon-oxygen oxide layer, such as an aluminosilicate, and in this application, such an oxide layer is referred to as an "oxide layer."

[0030] Due to the above-mentioned effects, in one embodiment of the present invention, the ceramic member and the cobalt-containing metal member can be appropriately joined.

[0031] It should be noted that the above description merely describes a phenomenon that may occur based on one mechanism currently considered, that is, in the manufacturing method of a joined 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.

[0032] In the method for producing a bonded body according to an embodiment of the present invention, since a complicated process such as a plating process is not performed, the bonded body can be produced easily. Furthermore, since the method for producing a bonded body according to an embodiment of the present invention does not use expensive metal materials such as nickel and / or silver, the production cost can be significantly reduced.

[0033] (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.

[0034] FIG. 1 shows a schematic cross section of a bonded body according to one embodiment of the present invention (hereinafter referred to as a "first bonded body").

[0035] 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 configuration in which the 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.

[0036] 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).

[0037] Moreover, the aluminum-containing metal layer 130 means a metal layer containing 51 mass % or more of aluminum.

[0038] The oxide layer 120 is an aluminum-silicon-oxygen oxide layer, such as an aluminosilicate.

[0039] The bonding layer 140 includes at least aluminum and cobalt. The bonding layer 140 may further include the main metal elements (except cobalt) included in the cobalt-containing metal member 150. For example, when the cobalt-containing metal member 150 is KOVAR, the bonding layer 140 may include iron and nickel. Also, when the aluminum-containing metal layer 130 includes silicon, the bonding layer 140 may further include silicon.

[0040] The first bonding 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 appropriately.

[0041] (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.

[0042] FIG. 2 is a schematic cross-sectional view of a bonded body according to another embodiment of the present invention (hereinafter referred to as a "second bonded body").

[0043] 2, the second bonded body 200 has a configuration 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, compared to the first bonded body 100, the second bonded body 200 has a configuration in which the aluminum-containing metal layer 130 is omitted.

[0044] In practice, the second bonding body 200 is formed in the configuration shown in FIG. 2 by incorporating an aluminum-containing metal component, which serves as a source of the aluminum-containing metal layer, into the oxide layer 220 and the bonding layer 240 during the manufacturing process.

[0045] In the second bonded body 200 as well, the oxide layer 220 to the bonding layer 240 are present between the ceramic member 210 and the cobalt-containing metal member 250. Therefore, in the second bonded body 200 as well, the above-mentioned functions of the oxide layer 220 to the bonding layer 240 enable the ceramic member 210 and the cobalt-containing metal member 250 to be properly bonded to each other.

[0046] (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.

[0047] FIG. 3 is a schematic cross-sectional view of a bonded body according to still another embodiment of the present invention (hereinafter referred to as a "third bonded body").

[0048] 3, the third bonded body 300 has a configuration 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 configuration as the first bonded body 100.

[0049] However, the third bonded body 300 differs from the first bonded body 100 in that it contains a plurality of particulates 360 inside the aluminum-containing metal layer 330. In other words, the aluminum-containing metal layer 330 has a morphology in which the particulates 360 are dispersed in a matrix of an aluminum-based metal (metallic aluminum or an aluminum alloy).

[0050] The shape of the granules 360 is generally spherical in most cases, but is not necessarily required to be spherical.

[0051] These particulates 360 include aluminum and the metal components included in the cobalt-containing metal component 350. For example, if the cobalt-containing metal component 350 is KOVAR, the particulates 360 have a composition including aluminum, cobalt, iron, and nickel.

[0052] Also, needle-shaped precipitates may be present inside some of the grains 360. According to the evaluation by 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 believed to be composed of phases containing iron, cobalt, and nickel, and do not contain aluminum.

[0053] 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 to each other.

[0054] (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.

[0055] (Ceramics 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.

[0056] There is no particular limitation on the shape of the ceramic member 110. The ceramic member 110 may have the shape of, for example, a block, a plate, a rod, a disk, or the like.

[0057] (Oxide layer 120) The oxide layer 120 is primarily composed of an oxide containing aluminum and silicon, and may be, for example, an aluminosilicate.

[0058] The thickness of the oxide layer 120 is not particularly limited, but may be in the range of 10 nm to 100 μm, for example.

[0059] (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.

[0060] As previously mentioned, the aluminum-containing metal layer 130 may include cobalt and aluminum-containing grains 360 (see FIG. 3).

[0061] (Joining 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.

[0062] In at least a portion of the bonding layer 140, the concentration of aluminum may continuously decrease toward the side of 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 the bonding layer 140 contains silicon, silicon may exhibit the same concentration change behavior as aluminum.

[0063] On the other hand, the cobalt concentration may continuously increase 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.

[0064] Furthermore, 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.

[0065] (Cobalt-containing metal member 150) The composition of the cobalt-containing metal component 150 is not particularly limited as long as the cobalt content is 15 mass% or more. The cobalt-containing metal component 150 may be, for example, metallic cobalt or KOVAR (17 mass% cobalt-12 mass% nickel-iron alloy).

[0066] There is no particular limitation on the shape of the cobalt-containing metal member 150. The cobalt-containing metal member 150 may have the shape of, for example, a block, a plate, a rod, a disk, or the like.

[0067] (Method of manufacturing a bonded body according to one embodiment of the present invention) Next, with reference to FIG. 4, an example of a method for producing a joined body having a ceramic member and a cobalt-containing metal member according to one embodiment of the present invention will be described.

[0068] FIG. 4 shows a schematic flow of a method for producing a bonded body having a ceramic member and a cobalt-containing metal member according to one embodiment of the present invention (hereinafter referred to as a "first production method").

[0069] As shown in FIG. 4, the first manufacturing method includes the following steps: (A) applying an organosilicon polymer to 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 member (step S130); (D) placing a cobalt-containing metal member on the aluminum-containing metal member 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.

[0070] It should be noted that step S130 is not necessarily an essential step and may be omitted.

[0071] Each step will be explained in detail below.

[0072] (Step S110) This step corresponds to the first half of (A-1) above.

[0073] First, a ceramic member is prepared.

[0074] The ceramic member is not particularly limited, and may be selected from the group consisting of alumina, silicon nitride, silicon carbide, mullite, zirconia, forsterite, steatite, cordierite, and ferrite, for example.

[0075] Furthermore, the shape of the ceramic member is not particularly limited, and the ceramic member may have the shape of a block, plate, rod, disk, or the like.

[0076] Next, an organosilicon polymer is applied to the joining surfaces of the ceramic members.

[0077] The organosilicon polymer is selected from siloxane polymers having a linear main chain with Si-O-Si groups.

[0078] Examples of siloxane-based polymers are polymethylhydrosiloxane, polymethylphenylsiloxane, polydimethylsiloxane, polysilsesquioxane, and the like.

[0079] The method of 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.

[0080] (Process S120) This step corresponds to the latter half of (A-1) above.

[0081] Next, an aluminum-containing metal member is placed on the ceramic member on which the organosilicon-based polymer has been placed.

[0082] The composition of the aluminum-containing metal member is not particularly limited, so long as it contains 51 mass % or more of aluminum.

[0083] 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.

[0084] The shape of the aluminum-containing metal member is not particularly limited, and the aluminum-containing metal member may have the shape of a block, plate, rod, foil, disk, or the like.

[0085] (Step S130) This step can be included in the above (A-2).

[0086] A second organosilicon-based polymer is then applied over the aluminum-containing metal component.

[0087] The second organosilicon polymer is selected from siloxane polymers having a linear main chain with Si-O-Si groups.

[0088] The second organosilicon based polymer can be the same material as the first organosilicon based polymer, or it can be a different material.

[0089] As mentioned above, step S130 is not necessarily an essential step. However, if this step is performed, the second organosilicon polymer decomposes during the heat treatment in the subsequent step S150 to generate a silane-based gas. When the aluminum-containing metal component comes into contact with the silane-based gas, the oxide film on the surface of the aluminum-containing metal component is easily removed. Therefore, a new surface of the aluminum-containing metal component can be exposed during the joining process.

[0090] As described above, aluminum and cobalt tend to be bonded to each other through an alloy layer formed at the interface, and therefore, when there is little oxide on the surface of the aluminum-containing metal member, the aluminum-containing metal member and the cobalt-containing metal member can be bonded more firmly.

[0091] (Process S140) This step corresponds to the above-mentioned part (A-2).

[0092] Next, a cobalt-containing metal member is placed on the aluminum-containing metal member on which the second organosilicon-based polymer has been placed, thereby forming an assembly.

[0093] As described above, the composition of the cobalt-containing metal member is not particularly limited as long as it contains 15 mass % or more of cobalt.

[0094] 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, which is an alloy containing 17% by weight cobalt, 12% by weight nickel, and the remainder iron.

[0095] The shape of the cobalt-containing metal member is not particularly limited, and the cobalt-containing metal member may have a shape such as a block, plate, rod, foil, or disk.

[0096] (Process S150) This step corresponds to part (c) above.

[0097] Next, the assembly constructed in step S140 is heat-treated for bonding, thereby producing a bonded body in which the ceramic member and the cobalt-containing metal member are bonded together.

[0098] The heat treatment is carried out in an atmosphere substantially free of oxygen, for example, 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.

[0099] The inert gas atmosphere may be, for example, an atmosphere of argon, helium, and / or nitrogen, etc. The degree of vacuum in the vacuum atmosphere is, for example, −0.08 MPa or less when the atmospheric pressure is 0 MPa.

[0100] The heat treatment temperature is 430° C. or higher. The heat treatment temperature is preferably, for example, 700° C. or lower. In particular, the heat treatment temperature is preferably in the range of 540° C. to 660° C.

[0101] 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.

[0102] Heat treating the assembly converts the organosilicon polymer to form an oxide layer between the ceramic member and the aluminum-containing metal member.

[0103] Typically, the oxide layer is made of an oxide of the aluminum-silicon-oxygen system.

[0104] Furthermore, by subjecting the assembly to a heat treatment, a bonding layer is formed between the aluminum-containing metal member and the cobalt-containing metal member.

[0105] 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.

[0106] The bonding layer also has at least a portion having a gradient in aluminum concentration and a gradient in cobalt concentration.

[0107] 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 behave similarly to aluminum. Also, metals other than cobalt contained in the cobalt-containing metal component may behave similarly to cobalt.

[0108] For example, if the aluminum-containing metal component includes silicon, the silicon concentration may gradually decrease toward the cobalt-containing metal component, and if the cobalt-containing metal component is KOVAR, the iron and nickel concentrations may gradually increase toward the cobalt-containing metal component in the gradient portion of the bonding layer.

[0109] 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 total concentration of cobalt, iron, and nickel may be 20 mass% or more in the central portion of the bonding layer thickness.

[0110] Depending on the heat treatment conditions, the aluminum-containing metal member 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).

[0111] Through the above steps, a bonded body is manufactured in which the ceramic member and the cobalt-containing metal member are bonded well to each other.

[0112] In the first manufacturing method, since a complicated process such as a plating process is not performed, the bonded body can be manufactured easily. In addition, since the first manufacturing method does not use expensive metal materials such as nickel and / or silver, the manufacturing cost can be significantly reduced.

[0113] In the first manufacturing method, the organosilicon polymer is placed on the ceramic member in step S110, and then an aluminum-containing metal member is placed on the ceramic member.

[0114] However, alternatively, the 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.

[0115] That is, the timing of application of the organosilicon polymer is not particularly limited, and the organosilicon polymer may be applied to either the ceramic member or the aluminum-containing metal member, or the organosilicon polymer may be applied to both the ceramic member and the aluminum-containing metal member, and then the two members may be laminated together.

[0116] In the first manufacturing method, the second organosilicon-based polymer is placed on the aluminum-containing metal component in step S130, and then the cobalt-containing metal component is placed on the aluminum-containing metal component.

[0117] Alternatively, however, a second organosilicon-based polymer may be applied to the cobalt-containing metal component in question, and then the cobalt-containing metal component may be applied over the aluminum-containing metal component.

[0118] This step corresponds to the above steps (a-1) and (a-2).

[0119] That is, the timing of applying the second organosilicon polymer is not particularly limited, and the second organosilicon polymer may be applied to either the aluminum-containing metal member or the cobalt-containing metal member. Alternatively, the second organosilicon 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.

[0120] It will be apparent to those skilled in the art that various other modifications are possible.

[0121] (Method of manufacturing a bonded body according to another embodiment of the present invention) Next, with reference to FIG. 5, an example of a method for producing a joined body having a ceramic member and a cobalt-containing metal member according to another embodiment of the present invention will be described.

[0122] FIG. 5 shows a schematic flow of a manufacturing method of a bonded body having a ceramic member and a cobalt-containing metal member according to another embodiment of the present invention (hereinafter referred to as a "second manufacturing method").

[0123] As shown in FIG. 5, the second manufacturing method includes: (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.

[0124] The second manufacturing method can be effectively used particularly when the aluminum-containing metal member is in particulate form, and therefore, in the following description, each step will be described using the case where the aluminum-containing metal member is in particulate form as an example.

[0125] However, it will be apparent to those skilled in the art that the second manufacturing method can be similarly applied to an aluminum-containing metal member in the form of a block, plate, bar, foil, disk, or the like.

[0126] (Step S210) This step corresponds to the above-mentioned part (A-1).

[0127] First, the ceramic member as shown in the first manufacturing method is prepared. Also, the aluminum-containing metal member is prepared. The aluminum-containing metal member may have the composition as described above.

[0128] As described above, the aluminum-containing metal member used in the second production method is in the form of particles. The particulate aluminum-containing metal member 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.

[0129] Next, the particulate aluminum-containing metal component is thoroughly mixed with the organosilicon polymer to prepare a slurry.

[0130] If the organosilicon polymer is a liquid, a solvent may be used in preparing the slurry, although this is not necessarily required.

[0131] As the solvent, for example, an organic solvent such as an alcohol, for example methanol and ethanol, or an ester may be used.

[0132] Next, the prepared slurry is applied to the joining surfaces of the ceramic members.

[0133] The method for applying the slurry is not particularly limited. For example, the slurry may be applied to the joining surfaces of the ceramic members or the cobalt-containing metal members by a method such as screen printing.

[0134] (Process S220) This step corresponds to the above-mentioned part (A-2).

[0135] Next, a cobalt-containing metal member is placed on the slurry applied to the joining surfaces of the ceramic members to form an assembly.

[0136] (Step S230) This step corresponds to part (c) above.

[0137] Next, the assembly is heat-treated to produce a bonded body under the same conditions as in the first manufacturing method described above.

[0138] By the 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.

[0139] Furthermore, by subjecting the assembly to a heat treatment, an interdiffusion reaction between cobalt and aluminum occurs on the surface of the cobalt-containing metal member that is in contact with the slurry, forming the above-mentioned bonding layer.

[0140] Furthermore, among the particulate aluminum-containing metal components contained in the initial slurry, the particles that were not used in the reaction form an aluminum-containing metal layer.

[0141] 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.

[0142] Here, in the second production method, when particulate aluminum-containing metal members are used, there is a high tendency for a bonded body having the configuration as shown in FIG. 3 described above to be produced.

[0143] That is, a structure is obtained in which particles containing cobalt and aluminum are dispersed in the matrix of the aluminum-containing metal layer.

[0144] It will be apparent to those skilled in the art that the second manufacturing method has the same advantages as the first manufacturing method.

[0145] That is, the second manufacturing method also makes it possible to easily manufacture a bonded body. Moreover, the second manufacturing method does not use expensive metal materials such as nickel and / or silver, and therefore the manufacturing cost can be significantly reduced.

[0146] In the second manufacturing method, instead of steps S210 to S220, a slurry containing an aluminum-containing metal component may be applied to the joining surface of the cobalt-containing metal component, and then a ceramic component may be placed on the joining surface of the cobalt-containing metal component on which the slurry has been applied, to form an assembly.

[0147] This step corresponds to the above steps (a-1) and (a-2).

[0148] The above describes the methods for producing a bonded body by taking the first and second production methods as examples. However, the above description is merely an example, and it is clear to those skilled in the art that similar effects can be obtained by partially changing the above-mentioned method or adding other steps.

[0149] For example, in the above description, the ceramic member is first prepared, and necessary members are sequentially placed thereon to produce the joined body, but the conversely, the cobalt-containing metal member may be first prepared, and necessary members may be sequentially placed thereon to produce the joined body. EXAMPLES

[0150] Examples of the present invention will be described below, but the present invention is not limited to these examples.

[0151] (Example 1) A bonded body of a ceramic member and a cobalt-containing metal member was produced by the following method.

[0152] First, an alumina plate (purity 90% or more) having dimensions of 20 mm length × 20 mm width × 0.32 mm thickness was prepared as a ceramic member. A pure cobalt plate (manufactured by Nilaco Corporation) having dimensions of 15 mm length × 15 mm width × 1 mm thickness was prepared as a cobalt-containing metal member. Furthermore, a pure aluminum plate (manufactured by Nilaco Corporation) having dimensions of 10 mm length × 10 mm width × 0.1 mm thickness was prepared as an aluminum-containing metal member.

[0153] Next, the aluminum-containing metal member was immersed in a polysiloxane (KF-54; manufactured by Shin-Etsu Silicones) solution to apply polysiloxane to both sides of the aluminum-containing metal member.

[0154] Next, an aluminum-containing metal member and a cobalt-containing metal member were placed in this order on the joining surface (one surface measuring 20 mm long x 20 mm wide) of the ceramic member to form an assembly.

[0155] Next, the obtained assembly was heat-treated. The heat treatment conditions were an inert atmosphere at 700° C. for 15 minutes. As a result, a bonded body was obtained. Hereinafter, this bonded body is referred to as "bonded body according to Example 1."

[0156] In the joined body of Example 1, the ceramic member and the cobalt-containing metal member were joined well.

[0157] (Example 2) A bonded body of a ceramic member and a cobalt-containing metal member was produced by the following method.

[0158] 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 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 silumin (aluminum-12 wt% Si alloy) plate with dimensions of 10 mm length x 5 mm width x 0.08 mm thickness was prepared as the aluminum-containing metal member.

[0159] 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.

[0160] Next, an aluminum-containing metal member was immersed in this solution, and polysiloxane was applied to both sides of the aluminum-containing metal member.

[0161] Next, an aluminum-containing metal member and a cobalt-containing metal member were placed in this order on the joining surface (one surface measuring 20 mm long x 20 mm wide) of the ceramic member to form an assembly.

[0162] Next, the obtained assembly was heat-treated. The heat treatment conditions were 580° 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 2.”

[0163] In the joined body of Example 2, the ceramic member and the cobalt-containing metal member were joined well.

[0164] (Example 3) In the same manner as in Example 1, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0165] However, in this Example 3, a silicon carbide plate (with a purity of 70% or more) having dimensions of 10 mm in length × 10 mm in width × 5 mm in 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 in length × 5 mm in width × 3 mm in thickness was used as the cobalt-containing metal member.

[0166] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "joint according to Example 3."

[0167] In the joined body of Example 3, the ceramic member and the cobalt-containing metal member were joined well.

[0168] (Example 4) In the same manner as in Example 3, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0169] 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.

[0170] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "joint according to Example 4."

[0171] In the joined body of Example 4, the ceramic member and the cobalt-containing metal member were joined well.

[0172] (Example 5) In the same manner as in Example 1, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0173] However, in this Example 5, a KOVAR plate (cobalt content: 17% by mass; manufactured by Nilaco Corporation) was used as the cobalt-containing metal member.

[0174] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "joint according to Example 5."

[0175] In the joined body of Example 5, the ceramic member and the cobalt-containing metal member were joined well.

[0176] (Example 6) In the same manner as in Example 5, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0177] However, in this Example 6, a silumin (aluminum-12 wt % Si alloy) plate having dimensions of 10 mm length × 5 mm width × 0.08 mm thickness was used as the aluminum-containing metal member.

[0178] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "the joint according to Example 6."

[0179] In the joined body of Example 6, the ceramic member and the cobalt-containing metal member were joined well.

[0180] (Example 7) In the same manner as in Example 6, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0181] However, in this Example 7, silicon carbide (with a purity of 70% or more) having dimensions of 10 mm length×10 mm width×5 mm thickness was used as the ceramic member.

[0182] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "joint according to Example 7."

[0183] In the joined body of Example 7, the ceramic member and the cobalt-containing metal member were joined well.

[0184] (Example 8) A bonded body of a ceramic member and a cobalt-containing metal member was produced by the following method.

[0185] First, an alumina plate (purity 90% or more) having dimensions of 20 mm length × 20 mm width × 0.32 mm thickness was prepared as the ceramic member, and a KOVAR plate (cobalt content 17% by mass; manufactured by Nilaco Corporation) having dimensions of 15 mm length × 15 mm width × 1 mm thickness was used as the cobalt-containing metal member.

[0186] The aluminum-containing metal member was produced using a slurry containing -63 μm silumin powder (aluminum-12 wt % Si alloy, product name: silumin alloy; manufactured by Mitsuwa Chemicals).

[0187] 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 the silumin powder in the slurry was 65% by mass.

[0188] Next, the above-mentioned slurry was applied onto the joining surface (one surface measuring 20 mm long x 20 mm wide) of the ceramic member, and a cobalt-containing metal member was placed thereon to form an assembly.

[0189] Next, the obtained assembly was heat-treated. The heat treatment conditions were an inert atmosphere at 700° C. for 15 minutes. As a result, a bonded body was obtained. Hereinafter, this bonded body is referred to as “bonded body according to Example 8.”

[0190] In the joined body of Example 8, the ceramic member and the cobalt-containing metal member were joined well.

[0191] (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.

[0192] However, in this Example 9, aluminum powder (average particle size 5 μm, purity 99%) was used as the aluminum-containing metal member in the slurry. The concentration of the aluminum powder in the slurry was 65 mass %.

[0193] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "the joint according to Example 9."

[0194] In the joined body of Example 9, the ceramic member and the cobalt-containing metal member were joined well.

[0195] In addition, when a similar experiment was carried out using the aluminum powder contained in the paste with an average particle size of 10 μm, the same results were obtained.

[0196] (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.

[0197] However, in this Example 10, a mullite plate having dimensions of 15 mm length × 15 mm width × 2 mm thickness was used as the ceramic member, and aluminum powder (average particle size 5 μm, purity 99%) was used as the aluminum-containing metal member in the slurry.

[0198] The heat treatment conditions were an inert atmosphere at 700° C. for 60 minutes. As a result, a bonded body was obtained. Hereinafter, this bonded body is referred to as “bonded body according to Example 10.”

[0199] In the joined body of Example 10, the ceramic member and the cobalt-containing metal member were joined well.

[0200] (Example 11) In the same manner as in Example 10, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0201] However, in this Example 11, a zirconia plate was used as the ceramic member.

[0202] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "joint according to Example 11."

[0203] In the joined body of Example 11, the ceramic member and the cobalt-containing metal member were joined well.

[0204] (Example 12) In the same manner as in Example 10, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0205] However, in this Example 12, a forsterite plate was used as the ceramic member.

[0206] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "joint according to Example 12."

[0207] In the joined body of Example 12, the ceramic member and the cobalt-containing metal member were joined well.

[0208] (Example 13) In the same manner as in Example 10, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0209] However, in this Example 13, a steatite plate was used as the ceramic member.

[0210] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "joint according to Example 13."

[0211] In the joined body of Example 13, the ceramic member and the cobalt-containing metal member were joined well.

[0212] (Example 14) In the same manner as in Example 10, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0213] However, in this Example 14, a cordierite plate was used as the ceramic member.

[0214] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "joint according to Example 14."

[0215] In the joined body of Example 14, the ceramic member and the cobalt-containing metal member were joined well.

[0216] (Example 15) In the same manner as in Example 10, a bonded body of a ceramic member and a cobalt-containing metal member was produced.

[0217] However, in this Example 15, a ferrite plate was used as the ceramic member.

[0218] After heat treatment of the assembly, a joint was obtained, which will hereinafter be referred to as "joint according to Example 15."

[0219] In the joined body of Example 15, the ceramic member and the cobalt-containing metal member were joined well.

[0220] Table 1 below shows the manufacturing conditions for each bonded body.

[0221] [Table 1] (evaluation) Using the joints according to each example, various evaluations were carried out.

[0222] First, a cross section of the bonded body according to Example 2 was observed using a scanning electron microscope.

[0223] FIG. 6 shows an example of a cross section of the bonded body according to Example 2.

[0224] It was found that the aluminum-containing metal member had almost completely disappeared in the case of the joined body of Example 2. That is, it was found that the joined body had a cross-sectional configuration as shown in Fig. 2 above, and the ceramic member, the oxide layer, the joining layer, and the cobalt-containing metal member were arranged in this order.

[0225] No defects such as cracks or voids were observed in the oxide layer and the bonding layer.

[0226] The oxide layer was analyzed using a simple elemental analyzer, and it was found to contain an aluminosilicate phase in the oxide layer, and both aluminum and cobalt in the bonding layer.

[0227] It was found that in a portion of the bonding layer, the aluminum concentration continuously decreased toward the cobalt-containing metallic component, and conversely, the cobalt concentration continuously increased toward the cobalt-containing metallic component.

[0228] In the case of the bonded body of Example 1, substantially the same results were obtained.

[0229] On the other hand, in the case of the bonded body of Example 5, the layer structure of the bonded body had a cross-sectional structure as shown in Figure 1 above, and it was found to be composed of, from the ceramic member side, an oxide layer, an aluminum-containing metal layer, a bonding layer, and a cobalt-containing metal member.

[0230] No defects such as cracks or voids were observed in the oxide layer and the bonding layer.

[0231] An elemental analysis of the oxide layer was performed using a simple elemental analyzer. The results showed that the oxide layer contained an aluminosilicate phase, and that the bonding layer contained iron and nickel in addition to aluminum and cobalt.

[0232] It was found that in a portion of the bonding layer, the concentration of aluminum decreased continuously toward the cobalt-containing metallic component, while conversely the concentrations of cobalt, iron, and nickel increased continuously toward the cobalt-containing metallic component.

[0233] FIG. 7 shows an example of a cross section of the bonded body according to Example 6.

[0234] It was found that the aluminum-containing metal member had almost completely disappeared in the case of the bonded body of Example 6. That is, the bonded body had a cross-sectional structure as shown in FIG.

[0235] No defects such as cracks or voids were observed in the oxide layer and the bonding layer.

[0236] An elemental analysis of the oxide layer was performed using a simple elemental analyzer. The results showed that the oxide layer contained an aluminosilicate phase, and that the bonding layer contained aluminum, silicon, cobalt, iron, and nickel.

[0237] It was found that in a portion of the bonding layer, the concentrations of aluminum and silicon decreased continuously toward the cobalt-containing metallic component, whereas the concentrations of cobalt, iron and nickel increased continuously toward the cobalt-containing metallic component.

[0238] FIG. 8 shows an example of a cross section of the bonded body according to Example 7.

[0239] In the case of the bonded body of Example 7, it was found that the layer structure of the bonded body had a cross-sectional structure as shown in Figure 1 above, and was composed of, from the ceramic member side, an oxide layer, an aluminum-containing metal layer, a bonding layer, and a cobalt-containing metal member.

[0240] No defects such as cracks or voids were observed in the oxide layer and the bonding layer.

[0241] An elemental analysis of the oxide layer was performed using a simple elemental analyzer. The results showed that the oxide layer contained an aluminosilicate phase, and that the bonding layer contained aluminum, silicon, cobalt, iron, and nickel.

[0242] Fig. 9 shows the results of line analysis of a cross section of the bonded body according to Example 7. In the figure, the horizontal axis corresponds to each cross section position in Fig. 8. For example, point A is a position approximately at the center of the thickness of the aluminum-containing metal layer, point B1 is a position approximately at the interface between the aluminum-containing metal layer and the bonding layer, point B2 is a position inside the bonding layer, point B3 is a position approximately at the interface between the bonding layer and the cobalt-containing metal member, and point C is a position inside the cobalt-containing metal member.

[0243] From this result, it is found 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 member, and conversely, in the same region, the concentrations of cobalt, iron, and nickel gradually increase toward the cobalt-containing metal member.

[0244] In the bonded structure of Example 7, element concentration analysis was performed at approximately the center position in the thickness direction of the bonding layer (see point D in FIG. 8). The results are shown in Table 2.

[0245] [Table 2] It was found that the cobalt+iron+nickel content exceeded 20 mass % at approximately the center of the thickness of the bonding layer.

[0246] Fig. 10 shows an example of a cross section of the bonded body according to Example 8. Fig. 11 shows an enlarged photograph of the area enclosed by the square in Fig. 10.

[0247] In the case of the bonded body of Example 8, it was found that the layer structure of the bonded body had a cross-sectional structure as shown in Figure 3 described above, and was composed of, from the ceramic member side, an oxide layer, an aluminum-containing metal layer, a bonding layer, and a cobalt-containing metal member.

[0248] 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.

[0249] [Table 3] From Table 3, it was confirmed that the approximately spherical particles contained aluminum, cobalt, iron, and nickel.

[0250] The oxide layer was subjected to elemental analysis using a simple elemental analyzer, and the result showed that the oxide layer contained an aluminosilicate phase.

[0251] 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.

[0252] [Table 4] In the bonded body of Example 8, no defects such as cracks or voids were observed in the oxide layer and the bonding layer.

[0253] Table 5 below shows the cross-sectional structure of the bonded bodies according to each example.

[0254] [Table 5] 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.

[0255] Thus, it was found that there were three types of cross-sectional layer structures in the joined bodies of Examples 1 to 15. It was also confirmed that in the joined bodies of Examples 1 to 15, the ceramic members and the cobalt-containing metal members were well joined via the layer therebetween.

[0256] In addition, measurements using a simple elemental analyzer confirmed that the aluminum content in the aluminum-containing metal layer exceeded 51 mass% in each of the joined bodies of Examples 2, 7, and 8.

[0257] (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.

[0258] First, an alumina plate (purity 90% or more) having dimensions of 20 mm length x 20 mm width x 0.32 mm thickness was prepared as a ceramic member. In addition, two KOVAR plates (cobalt content 17% by mass; manufactured by Nilaco Corporation) having dimensions of 15 mm length x 15 mm width x 1 mm thickness were prepared as cobalt-containing metal members (referred to as "cobalt-containing metal member A" and "cobalt-containing metal member B" respectively). Furthermore, two pure aluminum plates (manufactured by Nilaco Corporation) having 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 A" and "aluminum-containing metal member B" respectively).

[0259] 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 Silicone Co., Ltd.) solution. The second solution was prepared by dissolving polysiloxane H (H44; manufactured by Wacker Chemie Co., Ltd.) in an ethanol solvent. The concentration of polysiloxane H in the second solution was 0.1 mol / L.

[0260] 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 (a surface measuring 20 mm in length × 20 mm in width) of the ceramic member. An aluminum-containing metal member B and a cobalt-containing metal member B were placed in this order on the other joining surface (a surface measuring 20 mm in length × 20 mm in width) of the ceramic member to form an assembly.

[0261] Next, the obtained assembly was heat-treated. The heat treatment conditions were an inert atmosphere at 700°C for 15 minutes. As a result, a bonded body was obtained. Hereinafter, this bonded body is referred to as "bonded body according to Example 16."

[0262] In the joined 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 joined well.

[0263] (Example 17) A bonded assembly in which ceramic members were disposed on both sides of a cobalt-containing metal member was produced by the following method.

[0264] 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).

[0265] 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.

[0266] Next, an aluminum-containing metal member C and a ceramic member A were placed in this order on one of the bonding surfaces (a surface measuring 20 mm in length × 20 mm in width) 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 bonding surface (a surface measuring 15 mm in length × 15 mm in width) of the cobalt-containing metal member to form an assembly.

[0267] Next, the obtained assembly was heat-treated. The heat treatment conditions were an inert atmosphere at 700° C. for 15 minutes. As a result, a bonded body was obtained. Hereinafter, this bonded body is referred to as “bonded body according to Example 17.”

[0268] In the joined body of Example 17, the cobalt-containing metal member and the ceramic member A, and the cobalt-containing metal member and the ceramic member B were both joined well. [Explanation of symbols]

[0269] 100 First zygote 110 Ceramic materials 120 Oxide layer 130 Aluminum-containing metal layer 140 Bonding layer 150 Cobalt-containing metal components 200 Second zygote 210 Ceramic Materials 220 Oxide layer 240 Bonding layer 250 Cobalt-containing metal components 300 The third conjugate 310 Ceramic materials 320 Oxide layer 330 Aluminum-containing metal layer 340 Bonding layer 350 Cobalt-containing metal components 360 Particulate matter

Claims

1. 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 placing a cobalt-containing metal member on the aluminum-containing metal member to form an assembly, which is carried out subsequent to the step (A-1); or (A-1) a step of placing an aluminum-containing metal member on a joining surface of a 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.

2. In the step (A-2), the cobalt-containing metal component is disposed such that a second organosilicon-based polymer is disposed between the aluminum-containing metal component and the cobalt-containing metal component; or In the step (a-1), the aluminum-containing metal member is placed 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.

3. The method of claim 2 , wherein said second organosilicon based polymer is the same as said first organosilicon based polymer.

4. 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.

5. 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; The manufacturing 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.

6. 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.

7. The method according to claim 1 , wherein the aluminum-containing metal component comprises an aluminum alloy containing 51 mass % or more of aluminum.

8. 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.

9. 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.

10. 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.

11. The joined body according to claim 9 or 10, wherein the cobalt-containing metal member is a cobalt-iron-nickel based alloy member.

12. 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.

13. The bonded body according to claim 9 , further comprising an aluminum-containing metal layer between the oxide layer and the bonding layer.

14. 14. The joined body according to claim 13, wherein particulate matter containing aluminum and cobalt is dispersed in the aluminum-containing metal layer.

15. 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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