JP2006045040A - Composite material having silicon-based ceramic and its manufacturing method - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a composite material having a silicon-based ceramic joined through a joining part having a strong joining strength and having a Ge-concentrated region in the vicinity of a joint interface. <P>SOLUTION: In the composite material in which a silicon-based ceramic member and a member to be joined are joined with the joining part consisting essentially of aluminum and containing 0.1-50 wt.% germanium, a first germanium-concentrated region is formed in the vicinity of a joint interface with the silicon-based ceramic member in the joining part. <P>COPYRIGHT: (C)2006,JPO&NCIPI

Description

The present invention relates to a composite material having Si-based ceramics, particularly Si ₃ N ₄ (silicon nitride), and a method for producing the same.

Silicon nitride (Si ₃ N ₄ ) is excellent in high-temperature strength, has high electrical insulation, and has higher thermal conductivity than alumina, and is therefore used as a heater, a heat sink, and an electrical insulation plate. However, since ceramics are generally difficult to machine, it is important to develop a bonding method in order to obtain a ceramic product having a desired shape.

  It is also possible to manufacture a high-functional product that takes advantage of the high workability of the metal material and the aforementioned advantages of silicon nitride.

Patent Document 1 discloses a ceramic circuit board in which a metal plate containing aluminum as a main component is bonded to at least one main surface of a ceramic substrate such as silicon nitride through a brazing material containing aluminum (Mg) as a main component. Is disclosed. The joint made of such a brazing material has a form in which the Mg is unevenly distributed in the vicinity of the joint interface with the ceramic circuit board.
JP 2001-144433 A

  In the above-mentioned Patent Document 1, Mg added to a brazing material containing Al as a main component exhibits high oxidizability, and the amount of addition is limited, so that a metal plate is bonded to a ceramic member with sufficient bonding strength. It was difficult to do.

  The present invention relates to a composite material in which a Si-based ceramic member and a joining partner member are joined with high strength at a joint portion containing Al as a main component and having a relatively large amount of Ge containing excellent oxidation resistance, and a method for manufacturing the same. provide.

  The present invention is a composite material in which a silicon-based ceramic member and a bonding partner member are bonded together at a bonding portion containing aluminum as a main component and containing 0.1 to 50% by weight of germanium, wherein the bonding portion includes the silicon The present invention provides a composite material characterized in that a first germanium enriched region is formed in the vicinity of a bonding interface with a ceramic member.

  Further, the present invention is a composite material in which a silicon-based ceramic member and a bonding partner member are bonded at a bonding portion containing aluminum as a main component and containing 0.1 wt% to 20 wt% of silicon, The present invention provides a composite material characterized in that a silicon-concentrated region is formed in the vicinity of a bonding interface with a silicon-based ceramic member.

  Further, according to the present invention, a brazing material containing aluminum as a main component and containing germanium in an amount of 0.1% by weight to 50% by weight is interposed between a silicon-based ceramic member and a bonding partner member, and is heated. The present invention provides a method for producing a composite material, which includes a step of forming, between the members, a joint portion in which a germanium concentrated region exists in the vicinity of a joint interface.

  ADVANTAGE OF THE INVENTION According to this invention, the composite material which has Si type ceramics which has a low porosity and has a junction part with high joint strength, and its manufacturing method can be provided.

  Furthermore, by using a brazing material containing Ge, the melting (brazing) temperature of the brazing material can be lowered, and it becomes possible to produce composite materials having Si-based ceramics for various uses.

  Hereinafter, a composite material according to the present invention will be described in detail with reference to the drawings.

(First embodiment)
FIG. 1 is a partially cutaway perspective view showing a composite material having Si-based ceramics according to the first embodiment. The composite material 1 exists in a state in which a silicon-based ceramic member 2 is sandwiched between two bonding partner members 3, and is bonded with a bonding portion 4 interposed between the ceramic member 2 and the two bonding partner members 3. Has the structure.

The main component of the silicon-based ceramics may be silicon-containing ceramics, and the main component is particularly preferably silicon nitride. Examples of the silicon-containing ceramic include silicon nitride (Si ₃ N ₄ ), silicon carbide (SiC), silicon oxide (SiO ₂ ), mullite (Al ₂ O ₃ —SiO ₂ ), and cordierite ((Mg, Fe). ₂ Al ₃ (Si ₅ Al) O ₁₈ ) and sialon (Si ₃ N ₄ .AlN.SiO ₂ .Al ₂ O ₃ ). Silicon nitride is usually used in the form of a sintered body containing a sintering aid such as alumina (Al ₂ O ₃ ), yttria (Y ₂ O ₃ ), magnesium oxide (MgO) or calcium oxide (CaO). For example, these auxiliary components may be a plurality of components such as Al ₂ O ₃ + Y ₂ O ₃ or MgO + Y ₂ O ₃ . Specific examples of silicon nitride sintered bodies containing these auxiliary components include Si ₃ N ₄ -3 wt% Al ₂ O ₃ -5 wt% Y ₂ O ₃ , Si ₃ N ₄ -2 wt% MgO-10 wt% Y ₂ O ₃ and the like.

  Examples of the bonding partner member 3 include ceramics or metal. When the bonding partner member 3 is ceramic, for example, the Si-based ceramic described above is preferable. When the joining partner member 3 is a metal, the joining partner member 3 is desirably made of a material having a melting point of 300 ° C. or higher, preferably 450 ° C. or higher. The joining partner member 3 is desirably made of, for example, a metal containing Al, more preferably Al or an Al alloy.

  The said junction part 4 is an area | region located between the said silicon-type ceramic member 2 and the said other party member 3, and means the area | region where a composition differs with respect to all of these joining members. When a metal is selected as the bonding partner member 3, the composition may gradually change from the bonding interface toward the metal member, and in this case, the region of the bonding portion is not clear. In this case, the region may be determined within the composition range by paying attention to a certain element.

  The joint 4 has a composition containing Al as a main component and Ge in an amount of 0.1 wt% to 50 wt%. The junction 4 is formed with a Ge-enriched region 6 in the vicinity of the junction interface 5 with the silicon-based ceramic member 2.

  Here, the vicinity 5 of the interface corresponds to the distribution region of the concentrated region, and means a region within 500 μm from the bonding interface. Regardless of the thickness of the bonded portion, the distribution region of the concentrated region is preferably 500 μm or less because the strength may decrease when the region exceeds 500 μm.

  The density area, the density of the density area, and the distribution area are determined by the following method.

(A) Judgment of the enriched region Element is measured with an electron probe microanalyzer [(EPMA; electron probe microanalyser) (Shimadzu Corporation, EPMA-1600) from the end face of the ceramic member to the direction of the joining partner member in the cross section of the joint. The two-dimensional distribution of each element is measured, and the concentration region is determined by looking at the distribution of the count number of the corresponding element. The concentration region needs to have a difference in the count number of the corresponding element larger than the measurement error as compared with other regions, and it is desirable to obtain the effect of the present invention that is twice or more.

(B) Determination of concentration in concentrated region First, a plurality of samples with known concentrations are prepared, and EPMA and energy dispersive X-ray spectrometer [(EDX; Energy Dispersive X-ray Spectrometer) ( Shimadzu Corporation, EMAX-2770] is used to perform a quantitative analysis to measure the count number of the corresponding element, and a calibration curve indicating the relationship between the count number of the corresponding element and the concentration of the corresponding element is created from this measurement result. . The concentration of the corresponding element in the actual concentrated region is determined by checking the count number of the corresponding element measured from the EPMA and EDX against this calibration curve. Similarly, the concentration of the junction with the region other than the concentrated region is determined by comparing the count number of the corresponding element with this calibration curve. From these determination results, the magnification of the density of the darkened area relative to the area other than the darkened area is obtained. However, the density of each region is used as an average value at a plurality of locations. Such density magnification is desirably 1.5 times or more, more preferably 2 times or more. If the magnification is less than 1.5 times, it may be difficult to bond the Si-based ceramic member 2 and the bonding partner member 3 with sufficient strength. The upper limit of the concentration of the corresponding element in the concentration region depends on the concentration of the corresponding element contained in the junction.

(C) Judgment of the distribution region of the concentration region In the cross section of the joint, measurement is performed in the region from the distance X and from X to 2X using EPMA from the ceramic member end surface toward the bonding partner member, and the concentration region The distance X when the area ratio (area fraction of the concentrated area with respect to the total area area) reaches 1.5 times is defined as the distribution area of the concentrated area.

  If the content of Ge contained in the joint 4 is less than 0.1% by weight, it is difficult to form a desired concentrated region. On the other hand, when the Ge content exceeds 50% by weight, the amount of Ge becomes excessive, and there is a concern that the strength of the bonded portion itself may be reduced due to poor bonding or the like. A more preferable Ge content is 0.5 wt% to 30 wt%.

The joint 4 may further contain 0.1 wt% to 20 wt% of Si. In this case, in the vicinity of the bonding interface 5 with the silicon-based ceramic member 2, in addition to the above-described Ge concentration region (first concentration region),
(1) Si concentration region,
(2) Ge.Si enriched region, and (3) Si enriched region and Ge.Si enriched region,
A second concentrated region selected from is formed.

  The Ge / Si concentration region may be formed by containing Si in a part of the first concentration region.

  In the case where Si is contained in the joint 4, it is difficult to form a desired concentrated region if the Si content is less than 0.1% by weight. On the other hand, if the Si content exceeds 20% by weight, the amount of Si becomes excessive, and the strength of the joint itself may decrease due to poor bonding or the like. A more preferable Si content is 0.2 wt% to 10 wt%.

The joint 4 may further contain 0.05 wt% to 5 wt% of Mg. In this case, in addition to the above-described first concentration region, in the vicinity of the bonding interface 5 with the silicon-based ceramic member 2,
(4) Mg concentration region,
(5) A Ge / Mg enriched region and (6) a third enriched region selected from the Mg enriched region and the Ge / Mg enriched region are formed.

  The Ge / Mg concentration region may be formed by containing Mg in a part of the first concentration region.

  In the case where Mg is contained in the joint 4, it is difficult to form a desired concentrated region if the Mg content is less than 0.05% by weight. On the other hand, if the Mg content exceeds 5% by weight, the amount of Mg becomes excessive, and there is a concern that the strength of the joint part itself is lowered due to poor bonding or the like. A more preferable Mg content is 0.1 wt% to 2 wt%.

  The joint portion 4 may include 0.1 wt% to 20 wt% Si and 0.05 wt% to 5 wt% Mg. In this case, in addition to the first concentration region, the second concentration region and the third concentration region are formed in the vicinity 5 of the bonding interface with the silicon-based ceramic member 2, or these first to first concentration regions are formed. A Ge / Si / Mg concentrated region (fourth concentrated region) is formed in addition to the three concentrated regions.

  In the case where Si and Mg are contained in the joint 4, it is difficult to form a desired concentrated region if the Si content is less than 0.1 wt%. On the other hand, if the Si content exceeds 20% by weight, the amount of Si becomes excessive, and the strength of the joint itself may decrease due to poor bonding or the like. A more preferable Si content is 0.2 wt% to 10 wt%.

  Further, in the case where Si and Mg are contained in the joint portion 4, if the Mg content is less than 0.05% by weight, it becomes difficult to form a desired concentrated region. On the other hand, if the Mg content exceeds 5% by weight, the amount of Mg becomes excessive, and there is a concern that the strength of the joint part itself is lowered due to poor bonding or the like. A more preferable Mg content is 0.1 wt% to 2 wt%.

  Each of the distribution regions of the second, third, and fourth concentrated regions described above corresponds to the vicinity 5 of the bonding interface, which means a region within 500 μm from the bonding interface, like the first Ge concentrated region. The distribution region of these concentrated regions is preferably 500 μm or less because there is a possibility that the strength is lowered when the thickness exceeds 500 μm regardless of the thickness of the joint.

  Furthermore, the joint portion 4 may contain inevitable impurities, and may contain a component derived from the ceramic member 2 or the counterpart member 3.

  Note that each of the above-described concentrated regions exists, for example, in the vicinity of the bonding interface 5 in the form of particles or lumps.

  Next, the manufacturing method of the composite material which has Si type ceramics concerning this invention is demonstrated as an example with reference to FIG.

  First, Ge or an alloy-containing powder is added to the organic adhesive, and the viscous Ge-containing powder is applied to both surfaces of the Si-based ceramic member 2 to form Ge-containing powder layers 9 respectively. Subsequently, a brazing material 8 made of Al as a main component is superposed on the Ge-containing powder layers 9 on both sides of the Si-based ceramic member 2, and a joining material 3 is further superposed on the brazing material 8 to produce a laminate 7. To do.

  Next, the obtained laminate 7 is placed in a vacuum furnace and heated in a vacuum while applying a load from above the uppermost bonding partner member 3, so that the bonding partner member 3 is attached to both surfaces of the ceramic member 2. The composite material 1 is manufactured by joining through the joint portion 4. In this joining, a hot press is employed when a joining surface pressure of 1 MPa is applied, and a weight is placed when a joining surface pressure of 0.01 MPa is applied. Here, the bonding surface pressure is a value obtained by dividing the load at the time of bonding by the area of the bonded portion.

  According to the manufacturing method described above, a composite material in which two members are bonded at the bonding portion 4 where the germanium concentration region exists in the vicinity 5 of the bonding interface with the ceramic member 2 is obtained. The first Ge-enriched region 6 is formed in the vicinity 5 of the bonding interface 4 of the bonding part 4 when Ge is present at a concentration exceeding the solid solubility limit of Ge in Al. It can be considered that the ceramic member 2 has a chemical property similar to that of silicon, and is therefore unevenly distributed on the ceramic member 2 side.

  Next, another method for producing a composite material having Si-based ceramics according to the present invention will be described with reference to FIG. In this method, the above-described composite material is manufactured except that the Ge-containing powder layer 9 is not interposed between the Si-based ceramic member 2 and the brazing material 8 and the brazing material 8 is directly disposed on both surfaces of the Si-based ceramic member 2. It is the same as the method.

  The brazing material 8 preferably has the following composition.

  (I) A brazing material containing 0.1 to 50% by weight, preferably 5 to 50% by weight, more preferably 10 to 30% by weight of Ge, with the balance being substantially Al.

  (Ii) A brazing material containing substantially 1 to 20% by weight of silicon in addition to Ge of the above (i), preferably 4 to 15% by weight, and the balance being substantially Al.

  (Iii) A brazing material containing 0.1 to 5% by weight, preferably 0.5 to 3% by weight of Mg in addition to Ge of (i), with the balance being substantially Al.

  (Iv) A brazing material containing 0.1 to 5% by weight, preferably 0.5 to 3% by weight of Mg in addition to Ge and Si of (ii), with the balance being substantially Al.

  In the production of a composite material, when forming a joint including at least one of Si and Mg in addition to Ge, these alloy powders are mixed with an adhesive, and this is interposed between the members and subjected to heat treatment. Also good.

(Second Embodiment)
The composite material according to the second embodiment joins a Si-based ceramic member and a joining partner member at a joint having a composition containing Al as a main component and containing 0.1 wt% to 20 wt% of Si. Has a Si-enriched region in the vicinity of the bonding interface with the Si-based ceramic member.

  Here, the vicinity 5 of the interface corresponds to the distribution region of the concentrated region, and means a region within 500 μm from the bonding interface. The distribution region of the concentrated region is preferably 500 μm or less because there is a concern that the strength may decrease if it exceeds 500 μm regardless of the thickness of the joint. The density region, the density of the density region, and the method for determining the distribution region are the same as those in the first embodiment, and the density of the density of the density region is 1.5 times or more, preferably 2.0 times or more. It is desirable that

  When the Si content is less than 0.1% by weight, a desired concentrated region is not formed. When the Si content exceeds 20% by weight, the Si amount becomes excessive and the strength of the joint itself may be reduced due to poor bonding or the like. . A more preferable Si content is 0.2 wt% to 10 wt%.

The joint 4 may further contain 0.05 wt% to 5 wt% of Mg. In this case, in addition to the Si concentration region described above in the vicinity of the bonding interface 5 with the silicon-based ceramic member 2,
(7) Mg concentration region,
(8) A Si / Mg concentrated region, and (9) a concentrated region selected from the Mg concentrated region and the Si / Mg concentrated region are formed.

  The Si / Mg enriched region may be formed by containing the same amount of Mg in a part of the Si enriched region.

  In the case where Mg is contained in the joint portion, it is difficult to form a desired concentrated region if the Mg content is less than 0.05% by weight. On the other hand, if the Mg content exceeds 5% by weight, the amount of Mg becomes excessive, and there is a concern that the strength of the joint part itself is lowered due to poor bonding or the like. A more preferable Mg content is 0.1 wt% to 2 wt%.

  The joint portion of the second embodiment may contain inevitable impurities and may contain a component derived from a ceramic member or a counterpart member.

  Each of the concentrated regions described above is present in the vicinity of the bonding interface, for example, in the form of particles or lumps.

  Next, the manufacturing method of the composite material which concerns on 2nd Embodiment is demonstrated as an example.

  A laminate is prepared by superimposing a brazing material containing Al as a main component directly on both surfaces of a Si-based ceramic member, and further superimposing a bonding partner material on these brazing materials.

  Next, the obtained laminate is placed in a vacuum furnace and heated in a vacuum while applying a load from above the uppermost mating member, and the mating member is bonded to both surfaces of the ceramic member via the joint. To produce a composite material. In this joining, a hot press is employed when a joining surface pressure of 1 MPa is applied, and a weight is placed when a joining surface pressure of 0.01 MPa is applied.

  The Si-enriched region is formed in the vicinity of the bonding interface 5 of the bonding portion 4 when Si is present at a concentration exceeding the solid solubility limit of Si in Al. This is probably because it is unevenly distributed on the ceramic member 2 side so as to be compatible with silicon of No. 2.

  Examples of the present invention will be described below.

Example 1
First, a viscous Ge-containing powder was prepared by adding Ge powder having an average particle size of 25 μm to a binder obtained by diluting an acrylic resin with alcohol. Subsequently, as shown in FIG. 2 described above, a plate-like Si of 30 × 30 × 0.6 mm containing ₃ % by weight of Al ₂ O ₃ and 5% by weight of Y ₂ O ₃ as a sintering aid. _The viscous Ge-containing powder was applied to both surfaces of the ₃ N ₄ sintered body 2 to form a Ge powder layer 9 having a Ge weight of 0.02 g. Subsequently, foils (brazing material) 8 made of Al-12Si and having a thickness of 30 μm were stacked on both sides of the Ge powder layer 9 on both sides of the Si ₃ N ₄ sintered body 2. Further, on these brazing materials 8, No. stipulated in JIS4000. The laminate 7 was formed by stacking 30 × 30 × 0.5 mm Al plates (joining counterpart members) 3 of A1050P.

Next, after the laminate 7 was installed in a vacuum furnace, a joining surface pressure of 0.01 MPa was applied from above the uppermost Al plate, and the gas in the vacuum furnace was exhausted to 3 × 10 ^−2. The composite material was manufactured by setting the pressure at Pa and heating at 575 ° C. for 1 hour. According to the composition analysis of EDX, the concentration of the region other than the concentrated region was 6 wt% Ge, 1 wt% Si, and the balance was substantially Al.

The composite material was cut in a direction perpendicular to the vicinity of the bonding interface, polished, and then photographed with an electron microscope reflected electron beam image. A photograph of this electron microscope reflected electron beam image is shown in FIG. As a result of analyzing the white area | region of the center part of FIG. 4 using EPMA, this area | region was the concentration area | region which has a composition of Al-Ge. In addition, the presence of a concentrated region having an Al—Si—O composition in the vicinity of the bonding interface was confirmed. These concentrated regions were distributed in a range of 100 μm from the joint interface with the Si ₃ N ₄ sintered body 2.

  As a result of measuring the Ge concentration in the concentrated region based on the method (b) described above, the concentration was 3 to 6 times that in the other region of the joint. Similarly, with respect to silicon, the Si concentration in the concentrated region was an average four times that in the other regions of the junction.

The porosity was determined by dividing the length of the void existing in an arbitrary visual field at the interface between the Si ₃ N ₄ sintered body 2 and the bonding portion 4 by the bonding length within the visual field. As a result, the porosity was 2% or less.

In Example 1 as described above, a concentrated region having a composition of Al—Ge and Al—Si—O is formed in the vicinity of the bonding interface at the bonding portion, so that Si ₃ N ₄ is supported by the low porosity. A composite material in which the sintered body and the Al plate are joined with high strength can be obtained.

(Example 2)
First, an alloy powder in which an acrylic resin is diluted with alcohol, Ge powder having an average particle size of 45 μm, 15 wt% Si, 8 wt% Si, 1 wt% Mg, and the balance is substantially Al is added. Mg-containing alloy powder was prepared. Subsequently, as shown in FIG. 2 described above, a plate-like Si of 30 × 30 × 0.6 mm containing ₃ % by weight of Al ₂ O ₃ and 5% by weight of Y ₂ O ₃ as a sintering aid. _The viscous Ge, Si and Mg-containing alloy powders were applied to both surfaces of the ₃ N ₄ sintered body 2 to form Ge, Si and Mg-containing alloy powder layers 9 each having a thickness of 70 μm. Subsequently, on the both surfaces of the Ge powder layer 9 on both surfaces of the Si ₃ N ₄ sintered body 2, No. 3 specified in JIS4000. The laminate 7 was formed by stacking 30 × 30 × 0.5 mm Al plates (joining counterpart members) 3 of A1050P.

Next, after the laminate 7 was installed in a vacuum furnace, a joining surface pressure of 0.01 MPa was applied from above the uppermost Al plate, and the gas in the vacuum furnace was exhausted to 3 × 10 ^−2. The composite material was manufactured by setting the pressure at Pa and heating at 575 ° C. for 1 hour. According to the composition analysis of EDX, the concentration of the region other than the concentrated region was Ge 4 wt%, Si 1 wt%, and the balance was substantially Al (Mg was not detectable).

An electron microscope reflected electron beam image in the vicinity of the bonding interface of the composite material was taken. As a result, it was confirmed that in addition to the concentrated region having the Al—Ge composition, the concentrated region was formed in the vicinity of the junction interface as shown in the photograph of the reflected electron beam image shown in FIG. As a result of analyzing the white region and the slightly white region in FIG. 5 using EPMA, the white region is a concentrated region having an Al—Ge composition, and the slightly white region is a concentrated region having an Al—Si composition. Met. Although both regions were trace amounts, both Mg and O were concentrated, and it was confirmed that there were partially concentrated regions having compositions of Al-Ge-Mg and Al-Si-O. These concentrated regions were distributed in a range of 100 μm from the joint interface with the Si ₃ N ₄ sintered body 2.

  As a result of measuring the Ge concentration in the concentrated region based on the method (b) described above, the concentration was 2 to 5 times that in the other region of the joint. Similarly, with respect to silicon, the Si concentration in the concentrated region was twice as high as the average of other regions in the junction. Further, when the porosity was measured in the same manner as in Example 1, the porosity was within 2%.

In Example 2 as described above, a concentrated region having a composition of Al—Ge, Al—Si, Al—Ge—Mg, and Al—Si—O is formed at the joint, so that it is supported by the low porosity. In addition, it is possible to obtain a composite material in which the Si ₃ N ₄ sintered body and the Al plate are joined with high strength.
(Example 3)
On both sides of a 30 × 30 × 0.6 mm plate-like Si ₃ N ₄ sintered body containing ₃ % by weight of Al ₂ O ₃ and 5% by weight of Y ₂ O ₃ as a sintering aid, Al— A foil (brazing material) made of 12Si and having a thickness of 30 μm was stacked. Further, on these brazing filler metals, No. stipulated in JIS4000. A laminate of A1050P, 30 × 30 × 0.5 mm Al plates (joining mating members), was stacked.

Next, after the laminate was installed in a vacuum furnace, a hot press was used on the uppermost Al plate to apply a bonding surface pressure of 1 MPa, and the gas in the vacuum furnace was evacuated to 3 × 10 ⁻² Pa. The composite was produced by setting to pressure and heating at 595 ° C. for 1 hour. According to the composition analysis of EDX, the concentration in the region other than the concentrated region was 2% by weight of Si, and the balance was substantially Al.

  As a result of analyzing the vicinity of the joint interface of the composite material using EPMA, it was confirmed that an Al-Si concentrated region was present.

As a result of measuring the Si concentration in the concentrated region based on the method (b) described above, the concentration was three times that in the other regions of the joint. This concentrated region was distributed in a range of 100 μm from the bonding interface with the Si ₃ N ₄ sintered body. Further, when the porosity was measured in the same manner as in Example 1, the porosity was within 2%.

In such Example 3, since an Al-Si concentrated region is formed in the joint, a composite material in which the Si ₃ N ₄ sintered body and the Al plate are joined with high strength as supported by the low porosity. Can be obtained.

  In the composite materials of Examples 1 to 3 described above, a concentrated region having a composition of Al—Ge, Al—Si, Al—Si—O, or Al—Ge—Mg is formed. As a result, the wettability of the brazing material with respect to the ceramics was improved, and a good joint interface vicinity with a low porosity was obtained.

  Furthermore, in the joint part of the composite material of Example 2, the wettability is greatly improved by forming a concentrated region having a composition of Al—Ge—Mg and Al—Si—O in the vicinity of the joint interface, and the weight is about It became possible to join even with a small pressure. Thereby, it becomes possible to create a composite material without using a special pressing device such as a hot press, and the manufacturing cost can be reduced. In addition, the inclusion of Ge in the joint as in Examples 1 and 2 makes it possible to lower the brazing temperature than when using a joint that does not contain Ge. Even when the temperature is lowered, a concentrated region of Al—Si—O can be sufficiently formed, and cost reduction can be achieved and the range of products that can be processed can be expanded.

The partial notch perspective view which shows the composite material which has Si type ceramics concerning this invention. The disassembled perspective view which shows the manufacturing method of the composite material which has Si type ceramics concerning this invention. The disassembled perspective view which shows the other manufacturing method of the composite material which has Si type ceramics concerning this invention. The photograph of the electron microscope reflection electron beam image of the joint interface vicinity of the composite material which has Si type ceramics manufactured according to Example 1 of this invention. The photograph of the electron microscope reflection electron beam image of the joint interface vicinity of the composite material which has Si type ceramics manufactured according to Example 2 of this invention.

Explanation of symbols

  DESCRIPTION OF SYMBOLS 1 ... Composite material, 2 ... Ceramic member, 3 ... Joining partner member, 4 ... Joint part, 5 ... Joint interface vicinity, 6 ... Concentration area | region.

Claims (14)

A silicon-based ceramic member and a joining partner member are composite materials joined at a joint portion containing aluminum as a main component and containing 0.1 to 50% by weight of germanium,
The composite material according to claim 1, wherein a first germanium-enriched region is formed in the vicinity of the joint interface with the silicon-based ceramic member.   The joint further includes 0.1 wt% to 20 wt% silicon, and in addition to the first germanium concentrated region, a silicon concentrated region and a germanium / silicon concentration in the vicinity of the joint interface of the silicon-based ceramic member. The composite material according to claim 1, wherein at least one second thickening region selected from the thickening region is further formed.   The composite material according to claim 2, wherein the silicon concentration region has a composition of silicon-aluminum-oxygen.   The joint further includes 0.05 wt% to 5 wt% magnesium, and in addition to the first germanium concentrated region, a magnesium concentrated region and a germanium / magnesium concentrated concentration in the vicinity of the joint interface of the silicon-based ceramic member. The composite material according to claim 1, wherein at least one third concentration region selected from the concentration region is further formed.   The bonding material further includes 0.1 wt% to 20 wt% silicon and 0.05 wt% to 5 wt% magnesium. In addition to the first germanium concentration region, the bonding material includes the silicon-based ceramic member. At least one second concentration region selected from a silicon concentration region and a germanium / silicon concentration region, and at least one third concentration region selected from a magnesium concentration region and a germanium / magnesium concentration region in the vicinity of the bonding interface. The composite material according to claim 1, further comprising:   The composite material according to claim 2, wherein at least a part of the first germanium concentration region further contains silicon.   6. The composite material according to claim 2, wherein the germanium / silicon concentrated region is formed in a part of the first germanium concentrated region.   The composite material according to claim 4, wherein at least a part of the first germanium concentration region further contains magnesium.   The composite material according to claim 4, wherein the germanium / magnesium concentration region is formed in a part of the first germanium concentration region.   The germanium / silicon concentration region is formed in a part of the first germanium concentration region, and the germanium / magnesium concentration region is formed in a remaining part of the first germanium concentration region. The composite material according to claim 5. A silicon-based ceramic member and a bonding partner member are composite materials bonded together at a bonding portion containing aluminum as a main component and 0.1 wt% to 20 wt% of silicon,
The composite material according to claim 1, wherein a silicon-concentrated region is formed in the vicinity of a joint interface with the silicon-based ceramic member. The composite material according to claim 1, wherein the silicon-based ceramic is silicon nitride (Si ₃ N ₄ ).   The composite material according to claim 1, wherein the joining partner member is aluminum or an aluminum alloy.   A brazing material containing aluminum as a main component and 0.1 to 50% by weight of germanium is interposed between the silicon-based ceramic member and the bonding partner member, and is heated in the vicinity of the bonding interface with the silicon-based ceramic member by heating. The manufacturing method of the composite material characterized by including the process of forming the junction part in which the concentration area | region exists between the said members.

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