JP2010105174A - Method for producing ceramic structural material - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a method for producing a ceramic structure with which the ceramic structure can be obtained, in which a surface layer body is piled up on and unified with a substrate obtained from ceramic powder whose main components are different from each other, by a simple, locally heatable technique. <P>SOLUTION: The method for producing the ceramic structural material includes: the process A in which, using a substance having a dielectric loss in the frequency of a microwave or a high frequency or a resonance characteristic in the frequency of a supersonic wave as at least one of the ceramic powder and a binder, a substrate molding 1 to be the substrate [1] after baking and a surface layer body molding 2 to be the surface layer body [2] are produced by using a mixture comprising the ceramic powder and the binder; the process B in which the surface layer body molding 2 is piled up on the substrate molding 1, and minute vibration is applied on the interface of them to fuse them together to produce a unified molding 3; and the process for obtaining the ceramic structural material 5 in which the surface layer body [2] is joined to the substrate [1] by degreasing and baking the unified molding 3. <P>COPYRIGHT: (C)2010,JPO&INPIT

Description

  The present invention relates to a method for producing a ceramic structural material in which a surface layer body is laminated and integrated on a substrate obtained from ceramic powders having different main components.

  Conventionally, various methods have been proposed as a method for producing a ceramic structural material. For example, in Patent Document 1, as a method of manufacturing a ceramic member in which a metal member is incorporated along a predetermined plane, a molded body of a first portion of the ceramic member is formed by a uniaxial pressure forming method, and a metal is formed on this surface. Providing a member, then placing the raw material of the second part of the ceramic member on the first molded body and the metal member, forming the second part by a uniaxial pressure molding method to produce a preform, Next, a method for producing a ceramic structural material by hot-press firing the preform is disclosed. Also, in Patent Document 2, as a method for producing a metal member-containing ceramic member, a mixture of a ceramic member raw material and a binder is granulated to obtain a granulated granule, and the granulated granule is molded to form a metal. A method of manufacturing a ceramic structural material by producing a preform with an embedded member and hot pressing the preform is disclosed. Further, Patent Document 3 discloses a method for manufacturing a metal member ceramic member similar to Patent Document 1.

  Further, for example, in Patent Document 4, as a method of manufacturing a multilayer ceramic electronic component, unevenness having a pitch matched to the shape of the electrode ink film on the side where the electrode ink film is not formed on the support on which the electrode ink film is formed. An electrode-embedded ceramic raw sheet produced by applying a ceramic ink on a support including an electrode ink film and drying it is heated on another ceramic raw sheet without peeling from the support. A method is disclosed in which after the pressure bonding, only the support is peeled off, the electrode embedded ceramic raw sheet is transferred onto another ceramic raw sheet, and this is fired.

  Further, for example, in Patent Document 5, as a method for manufacturing a sliding ceramic material, a surface layer made of nitride ceramics containing boron nitride as a sliding surface is applied to a substrate surface made of nitride ceramics, and formed. A method for producing a ceramic structure integrated by firing is disclosed. Specifically, a binder is added to sialon powder, kneaded in methanol, granulated, and then the granulated powder is compacted to produce a molded product, and after degreasing the molded product, the nitrogen atmosphere Pre-sintered and processed the pre-sintered pre-sintered body to form a sliding surface, and the slurry formed by kneading boron nitride powder and sialon powder in methanol on the sliding surface to a predetermined thickness A manufacturing method is disclosed in which, after being applied, dried in air, and then subjected to main sintering in a nitrogen atmosphere, the finish of the sliding surface of the sintered body that has been subjected to main sintering is disclosed.

Further, in Patent Document 6, when bonding objects to be bonded made of ceramics, an Au / Cr vapor deposition film is provided on the bonding surface of each object to be bonded, and a Pb vapor deposition film is provided on one Au / Cr vapor deposition film. Thereafter, a method is disclosed in which both the objects to be bonded are brought into close contact with each other by pressurizing them to thereby press and bond both objects to be bonded to each other.
Japanese Patent Laid-Open No. 10-249843 Japanese Patent Laid-Open No. 10-259059 Japanese Patent Laid-Open No. 11-255566 Japanese Patent Laid-Open No. 3-96206 Japanese Patent Laid-Open No. 5-221756 Japanese Patent Laid-Open No. 10-282073

  However, in the method for manufacturing a ceramic structure material described in Patent Documents 1 to 3, since a ceramic member is formed using a uniaxial pressure forming method, it is difficult to produce a complicated shape. is there. Further, there is a problem that the metal member that becomes a conductor portion needs to have a strength that does not deform during pressure molding.

  Moreover, in the manufacturing method of the ceramic structure material described in Patent Document 4, since the ceramic raw sheet is bonded by thermocompression bonding, heating of the entire ceramic raw sheet is required, and a specific part cannot be heated and bonded. There is a point.

  In addition, in the method for manufacturing a ceramic structure described in Patent Document 5, after firing for temporary sintering, firing for main sintering is performed, and as a result, the firing process is performed twice. There is a problem that productivity is bad.

  Furthermore, in the method for manufacturing a ceramic structure described in Patent Document 6, an Au / Cr vapor deposition film is provided on each of the ceramic objects to be joined, and a Pb film is further provided on one Au / Cr vapor deposition film. There is a problem that the productivity is not good because the pressure welding is carried out by pressing while pressing.

  The present invention has been devised to solve the above-described problems in the prior art, and the object thereof is obtained from ceramic powders each having a different main component in a simple and locally heatable manner. An object of the present invention is to provide a method for manufacturing a ceramic structure in which a ceramic structure in which a surface layer body is laminated and integrated on a substrate is obtained.

  In the method for producing a ceramic structure material of the present invention, at least one of the ceramic powder and the binder is one having a dielectric loss at a microwave or high frequency frequency or having a resonance characteristic at an ultrasonic frequency. A step A for producing a base body molded body that becomes a base body after firing using the mixture containing, and a surface body molded body that becomes a surface layer body after firing using the mixture containing the ceramic powder and the binder; Laminating the surface layer molded body, applying microwave or high frequency or ultrasonic wave, and fusing the interface between the base body molded body and the surface layer molded body to produce an integrated molded body, And degreasing and firing the integrated molded body to obtain a ceramic structure material in which the surface layer body is bonded to the substrate. And it is characterized in and.

  In the method for producing a ceramic structural material of the present invention, in step A, a ceramic green sheet is produced on a support as at least one of the base body molded body and the surface layer body molded body. The green sheet is laminated and fused to produce the integrated molded body.

  The method for producing a ceramic structural material of the present invention is characterized in that, in the step B, only a part of the base body compact and the surface layer compact is fused.

  According to the method for producing a ceramic structural material of the present invention, at least one of the ceramic powder and the binder is one having a dielectric loss at a microwave or high frequency frequency or having a resonance characteristic at an ultrasonic frequency, A step A for producing a substrate molded body that becomes a substrate after firing using a mixture containing a binder, and a surface molded body that becomes a surface layer body after firing using a mixture containing ceramic powder and a binder, and a substrate molded body A step B of laminating the surface layer molded body and applying a microwave or high frequency or ultrasonic wave to fuse the interface between the base body molded body and the surface layer molded body to produce an integrated molded body, And degreasing and firing the integrated molded body to obtain a ceramic structure material in which the surface layer body is bonded to the substrate. From the above, a surface layer molded body is laminated on a base molded body, and microwaves or high frequency by a high frequency welder or ultrasonic waves by an ultrasonic welder is applied, so that there is a dielectric loss in the frequency of the microwave or high frequency or ultrasonic waves One or both of the ceramic powder and the binder having a resonance characteristic at a frequency of 1 and both vibrate finely and generate heat, and the bonding interface between the base molded body and the surface layer molded body can be fused to securely bond the two. Therefore, it is possible to easily and surely obtain a ceramic structural material in which the surface layer body is joined and integrated with a substrate obtained from ceramic powders having different main components.

  Further, according to the method for producing a ceramic structural material of the present invention, in step A, a ceramic green sheet is produced on a support as at least one of a base body molded body and a surface layer body molded body. When producing an integrated molded body by laminating and fusing, rather than indirectly heat fusing the ceramic green sheet using a heater or the like, by using either microwaves, high frequency or ultrasonic waves, Since the ceramic green sheets themselves generate heat and are fused, the ceramic green sheets are excellent in temperature uniformity on the fused surface as compared with the method using indirect heating, and the ceramic green sheets can be easily bonded to each other.

  Further, according to the method for producing a ceramic structure material of the present invention, when only a part of the base body molded body and the surface layer molded body is fused in Step B, the base body molded body and the surface layer body molded body are partially bonded. If the non-adhesive part is removed before or after firing the integrated molded body by partially bonding a surface layer molded body of the same or different material to the base molded body, the surface of the substrate can be removed. In addition, a surface layer body having an arbitrary pattern can be produced without using a technique such as printing, and a three-dimensional molded body having an arbitrary shape can be easily produced.

  Hereinafter, an example of an embodiment of a method for producing a ceramic structural material of the present invention will be described in detail with reference to the drawings.

<First Example of Embodiment>
FIG. 1A to FIG. 1C are cross-sectional views for each process showing a first example of an embodiment of a method for producing a ceramic structural material of the present invention.

  As shown in FIG. 1 (a), the first example of the ceramic structure manufacturing method shown in FIG. 1 has dielectric loss at microwave or high frequency in the ceramic powder and / or binder, or ultrasonic waves. A substrate molded body 1 that becomes a substrate after firing using a mixture containing ceramic powder and a binder, and a surface layer body after firing using a mixture containing ceramic powder and a binder. As shown in FIG. 1B, the surface layer body 2 is laminated on the base body 1, and the surface body body 2 is formed on the base body 1. The laminated molded body 3 is sandwiched between a pair of molds 4a and 4b, and a high frequency is applied from the molds 4a and 4b to the integral molded body 3 using the oscillation source 4 to laminate the laminated substrate structure. By irradiating the interface between the body 1 and the surface layer molded body 2, an integrated molded body 3 in which the base molded body 1 and the surface layer molded body 2 are bonded by applying a minute vibration to the interface between the two and bonding them. The integrated ceramic structure formed by bonding the surface layer body [2] to the base body [1] by degreasing and firing the integrated molded body 3 and the step B to be manufactured as shown in FIG. And a process C for obtaining the material 5.

Ceramic powders used for the base body 1 and the surface layer body 2 produced in step A include alumina (Al ₂ O ₃ ), zirconia (Zr ₂ O ₃ ), tungsten carbide (WC), silicon nitride (Si ₃ N ₄ ), various cermets, boron nitride (BN) and the like can be selected from ceramic powders. In the present invention, ceramic powders having different main components are selected for the base molded body 1 and the surface layer molded body 2. As a combination of the ceramic powders of the base body compact 1 and the surface layer compact 2, for example, tungsten carbide (WC) is used as the base compact 1, and silicon nitride (Si ₃ N ₄ ) is used as the surface compact 2. In this case, when silicon nitride (Si ₃ N ₄ ) is used as the substrate molded body 1 and boron nitride (BN) is used as the surface layer molded body 2, alumina (Al ₂ O ₃ ) is used as the substrate molded body 1, and the surface layer body is used. In some cases, cermet is used as the molded body 2.
Among these, as those having dielectric loss at microwave or high-frequency frequencies or having resonance characteristics at ultrasonic frequencies, for example, tungsten carbide (WC) or various cermets for a frequency of 1 MHz. It has dielectric loss, and silicon nitride (Si ₃ N ₄ ) or various cermets have resonance characteristics with respect to the frequency of 1 kHz of ultrasonic waves, and each generates self-heating.

In the first example shown in FIG. 1, as a combination of ceramic powders of the base body 1 and the surface layer body 2, for example, silicon nitride (Si ₃ N ₄ ) is used as the base body 1, and surface layer molding is performed. By using boron nitride (BN) as the body 2 and co-firing them, the boron nitride (BN) was bonded to the silicon nitride (Si ₃ N ₄ ) as the substrate [1] with the surface layer body [2]. The ceramic structural material 5 can be easily produced.

  Examples of the resin that can be used as the binder include thermoplastic resins such as vinyl chloride, acrylic, polypropylene, polycarbonate, polyacetal, polyimide, polyethylene, tetrafluoroethylene, butyral, and paraffin wax. Among these, those having a dielectric loss at a frequency with respect to microwaves or high frequencies or having resonance characteristics at a frequency with respect to ultrasonic waves include polyethylene, polypropylene, and tetrafluoroethylene for microwaves. Etc. For high frequencies, nylon, paraffin wax, acrylic, polyimide, and the like can be given. For ultrasonic waves, nylon, acrylic, polyethersulfone, polyetherimide, and the like can be given.

  As a method for producing the substrate molded body 1 and the surface layer molded body 2 using these ceramic powder and binder, methods such as extrusion molding, powder press molding, injection molding or casting molding can be used. What is necessary is just to use a suitable method according to the shape of the base | substrate molded object 1 or the surface layer molded object 2 to be made.

  As a method of producing the base molded body 1 and the surface layer molded body 2, extrusion molding, powder press molding, injection molding, cast molding, or the like can be used as appropriate. Further, as will be described later, at least one of the base molded body 1 and the surface layer molded body 2 may be produced as a ceramic green sheet by a tape molding method or the like.

  In step B shown in FIG. 1B, as a means for applying fine vibrations to the interface between the base molded body 1 and the surface layer molded body 2 by being applied to the integrated molded body 3, microwaves, high frequencies or ultrasonic waves are used. Use. By using these, the ceramic powder and / or binder contained in the base molded body 1 and the ceramic powder and / or binder contained in the surface layer molded body 2 are subjected to dielectric loss or microwave frequency against microwave or high frequency. By giving the resonance characteristics, the base molded body 1 and the surface layer molded body 2 generate internal heat, and the interface between the base molded body 1 and the surface layer molded body 2 is fused, whereby the base molded body 1 is bonded. Since the surface layer molded body 2 can be stably and surely fused, the surface layer body [2] can be easily and reliably joined and integrated with the base body [1] obtained from ceramic powders having different main components after firing. It is possible to obtain a ceramic structure material 5 obtained by converting the structure.

  In order to apply a microwave to the integrated molded body 3, the surface molded body 2 is laminated on the base molded body 1 and set in the microwave irradiation apparatus, and the surface molded body is formed on the base molded body 1. What is necessary is just to irradiate a microwave on the conditions which can fuse | fuse the body 2, what is necessary is just to use a high frequency welder in order to apply a high frequency, and what is necessary is just to use an ultrasonic welder in order to apply an ultrasonic wave. Each frequency is preferably 1 GHz to 30 GHz for microwaves, 1 MHz to 300 MHz for high frequencies, and 1 kHz to 30 kHz for ultrasonic waves. The irradiation time is suitably 1 to 10 seconds for any of microwave, high frequency, and ultrasonic waves.

In Step B in which the surface layer body 2 is laminated on the base body 1 and fused to produce the integrated body 3, the entire surface of the interface between the base body 1 and the surface body 2 is not necessarily fused. However, only a part of the interface between the base molded body 1 and the surface layer molded body 2 may be fused. When only a part is fused, for example, a surface layer molded body 2 made of tungsten carbide (WC) and a binder having an arbitrary shape is superposed on a base molded body 1 made of silicon nitride (Si ₃ N ₄ ) and a binder. A method of obtaining an integrated molded body 3 by bonding a surface layer molded body 2 to a base molded body 1 by applying a high frequency or an ultrasonic wave after being laminated and sandwiched between molds 4a and 4b, or silicon nitride ( A green sheet made of tungsten carbide (WC), which becomes the surface layer formed body 2, and a binder is laminated on the substrate formed body 1 made of Si ₃ N ₄ ) and a binder, and the dies 4a, 4b having arbitrary shapes are stacked. An ultrasonic wave or a high frequency wave is applied, and an arbitrary shape portion of the green sheet, which is the surface layer molded body 2, is transferred to the base body molded body 1. How to obtain a molded product 3.

  In this way, when only a part of the base body molded body 1 and the surface layer body molded body 2 is fused, the surface layer body molded body 2 can be decorated in any shape on the base body molded body 1, or any other function It is possible to easily form a shape showing

  In the case of the integrated molded body 3 in which the base body [1] and the surface layer body [2] have different functions and the function is required for a large area, such as a sliding ceramic structural material, the base body It is preferable to fuse the entire surface of the interface between the molded body 1 and the surface layer molded body 2.

  In step C, a degreasing step is provided before the firing step. Specifically, according to the kind of ceramic powder, the heat degreasing process of 400 degreeC for 2 hours is implemented with respect to the integrated molded object 3 produced at the process B, for example in air | atmosphere atmosphere or nitrogen atmosphere. Thereafter, for example, by firing in an oxidizing atmosphere or a non-oxidizing atmosphere, the ceramic structural material 5 which is a sintered body in which the surface layer [2] is joined and integrated to the base [1] obtained from ceramic powders having different main components. Can be obtained.

  About the obtained ceramic structural material 5, you may give an external shape process and a finishing process so that it may become a desired shape or surface state as needed.

In such a first example, for example, silicon nitride (Si ₃ N ₄ ) is used as the base molded body 1, and tungsten carbide (WC) is used as the surface layer molded body 2, and the sintered body is integrally joined. After the ceramic structural material 5 is manufactured, the ceramic structural material 5 for the sliding portion can be manufactured by subjecting the surface to polishing, R processing, or external processing according to the shape of the sliding portion. .

<Second Example of Embodiment>
2 (a) to 2 (c) are cross-sectional views for each process showing a second example of the embodiment of the method for producing a ceramic structural material of the present invention.

  As shown in FIG. 2 (a), the second example of the method for producing a ceramic structure material shown in FIG. 2 has dielectric loss at microwave or high frequency in the ceramic powder and / or binder, or ultrasonic waves. A substrate molded body 11 that becomes a substrate after firing using a mixture containing ceramic powder and a binder is prepared using a material having resonance characteristics at a frequency of the surface layer and a surface layer body after firing using a mixture containing ceramic powder and a binder. As shown in FIG. 2B, the surface layer molded body 12 is laminated on the substrate molded body 11, and the surface layer molded body 12 is laminated on the substrate molded body 11. In this example, the oscillator 14a is brought into contact with the surface layer molded body 12 side, and an ultrasonic wave is applied from the oscillator 14a to the integrated molded body 13 using the oscillation source 14 to By irradiating the interface between the molded body 11 and the surface layer molded body 12, the substrate molded body 11 and the surface layer molded body 12 are bonded to each other by applying a minute vibration to the interface between the two. Step B for producing the molded body 13 and the integrated molded body 13 are degreased and fired, whereby the surface layer body [12] is joined to the base body [11] as shown in FIG. And a step C of obtaining a structured ceramic structural material 15.

  This second example is the same as the first example shown in FIG. 1 except for the difference in configuration in step B shown in FIG.

In such a second example, for example, a silicon nitride (Si ₃ N ₄ ) is used as the substrate molded body 11, and boron nitride (BN) is used as the surface layer molded body 12. After the ceramic structural material 15 is produced, the ceramic structural material 15 for the sliding portion can be produced by subjecting the surface to polishing, R processing, or external processing according to the shape of the sliding portion.

  According to the second example as described above, it is not necessary to sandwich the substrate molded body 11 and the surface layer molded body 12 with a mold, and the adhesion between the substrate molded body 11 and the surface layer molded body 12 is possible. This has the advantage of increasing the degree of freedom in selecting the binder type.

<Third Example of Embodiment>
FIGS. 3A to 3D are cross-sectional views for each process showing a third example of the embodiment of the method for producing a ceramic structural material of the present invention.

  As shown in FIG. 3 (a), the third example of the method for manufacturing a ceramic structure material shown in FIG. 3 has dielectric loss at microwave or high-frequency frequency in at least one of ceramic powder and binder, or ultrasonic waves. Using at least one of the base molded body 21 and the surface layer molded body 22, in this example, the surface layer molded body 22 is formed on the resin film as the support 26 with ceramic powder, a binder, and A ceramic green sheet prepared by tape-molding a slurry containing a solvent and a base-molded body 21 using a mixture containing ceramic powder and a binder, in this example, a ceramic obtained by tape-molding a slurry containing ceramic powder, a binder and a solvent. As shown in FIG. 3 (b), the process A is prepared as a green sheet. In addition, the ceramic green sheet of the surface layer molded body 22 produced on the support 26 is adhered and laminated on the ceramic green sheet of the base molded body 21, and the surface layer body on the support 26 is laminated on the base molded body 21. An integrated molded body 23 in which the molded body 22 is laminated is sandwiched between a pair of electrodes 24a and 24b, and microwaves, high frequencies, or ultrasonic waves are applied from the electrodes 24a and 24b to the integrated molded body 23 using the oscillation source 24 and laminated. By irradiating the interface between the molded body 21 and the surface layer molded body 22, a fine vibration is applied to the interface between the two so as to fuse them, as shown in FIG. As shown in FIG. 3 (d), after forming the integrated molded body 23 with the surface layer molded body 22 bonded thereto, the support 26 is peeled off from the integrated molded body 23, and then degreased and fired. As shown in FIG. 3D, the surface layer body [22] is bonded to the base body [21]. That is intended to include a step C to obtain a ceramic structural material 25 that is integrated.

  This third example also differs from the first example shown in FIG. 1 except for the difference that a ceramic green sheet is used for the base molded body 21 and a ceramic green sheet formed on the support 26 is used for the surface layer molded body 22. It is the same.

  In the third example shown in FIG. 3, in step B, the surface layer compact 22 is produced as a ceramic green sheet on the support 26, and this ceramic green sheet is directly laminated on the base compact 21 and melted. The ceramic green sheet of the surface layer molded body 22 is placed on the base body molded body 21, and high frequency or ultrasonic waves are applied by the method shown in FIG. The ceramic green sheet of the body molded body 22 and the base body molded body 21 are bonded. Thereafter, the ceramic green sheet of the surface layer molded body 22 having a weak adhesive force may be transferred from the support 26 to the base molded body 21 by peeling the ceramic green sheet of the surface layer molded body 22 from the support 26. .

  The solvent for producing the ceramic green sheet as the base molded body 21 or the surface layer molded body 22 is not particularly limited as long as it dissolves the binder resin. For example, toluene, xylene, ethanol , Isopropanol, methyl isobutyl ketone, terpineol, ethyl carbitol, butyl carbitol acetate, and the like can be selected. When a resin film is used as the support 26, it can be appropriately selected from polyethylene terephthalate, polyamide, polyetherimide, vinyl chloride and the like. Further, as the support 26, various metal plates and various papers may be used in addition to the resin film.

In such a third example, for example, alumina (Al ₂ O ₃ ) is used as the base molded body 21 and zirconia (ZrO ₂ ) is used as the surface layer molded body 22, and functions such as wear resistance are required. After producing the ceramic structural material 25, which is a sintered body in which the surface layer (22) is joined and integrated only in the part, surface polishing, R processing, or external processing is performed according to the shape that requires wear resistance. By applying, the wear-resistant ceramic structural material 25 can be produced.

  According to the third example, it is possible to transfer the surface layer molded body 22 onto the base body molded body 21 in a short time as a thin sheet without directly printing or the like. Become.

  The manufacturing method of the ceramic structure material of the present invention shown as each example as described above has, as the ceramic structure material, for example, a ceramic structure material used for a sliding portion such as a ceramic roll and a current-carrying portion such as a far infrared heater. The present invention can be applied to the production of various ceramic structural materials, including ceramic structural materials made of silicon nitride used for ceramic structural materials, ceramic balls, heat-resistant ceramic parts, and the like.

  Hereinafter, the specific example of the manufacturing method of the ceramic structure material of this invention is demonstrated.

Example 1
Using a compound containing Si ₃ N ₄ powder as a ceramic powder and vinyl chloride as a binder (dielectric loss with respect to 1 MHz: 6 × 10 ⁻³ ) in the ratio shown in Table 1, a rectangular parallelepiped shape of 5 mm × 5 mm × 35 mm is formed by injection molding. A base molded body was prepared. Further, by using a compound containing Si ₃ N ₄ powder as a ceramic powder and paraffin wax (dielectric loss with respect to 1 MHz: 2 × 10 ⁻⁴ ) as a binder at a ratio shown in Table 1, injection molding is performed to have a size of 5 mm × 5 mm × 35 mm. A rectangular parallelepiped surface layer molded body was produced.

  Next, the surface layer body is overlaid and laminated on the base body, and is sandwiched between a pair of molds as shown in FIG. 1 (b), and a high frequency is applied under conditions of 1 MHz and 0.4 A by a high frequency welder. Then, fine vibration was applied to the interface between the base body molded body and the surface layer molded body for 3 seconds to be fused and bonded to produce an integrated molded body. Then, a 200 g weight was hung on the base molded body side of the integrated molded body and the integrated molded body was lifted to manually perform a peel test between the base molded body and the surface layer molded body to confirm the state of adhesion.

  Next, the integrated molded body was heated, degreased, and then fired to obtain a sintered body as Example 1 which is a ceramic structural material in which a surface layer body is bonded to a substrate. The heating and degreasing conditions were 400 ° C. for 2 hours and the firing conditions were 1800 ° C. for 3 hours.

(Example 2)
Using a powder containing Al ₂ O ₃ powder as ceramic powder and paraffin wax (resonance characteristics with respect to 1 kHz: 2 × 10 ⁻⁴ ) as a binder at a ratio shown in Table 1, by powder press molding, 5 mm × 5 mm × 35 mm A rectangular parallelepiped shaped base molded body was produced. In addition, a rectangular parallelepiped shape of 5 mm × 5 mm × 35 mm was formed by injection molding using a compound containing ZrO ₂ powder as ceramic powder and polyethylene as a binder (resonance characteristics with respect to 1 kHz: 2 × 10 ⁻⁴ ) in the ratio shown in Table 1. A surface layer molded body was produced.

  Next, the surface layer body is overlaid and laminated on the base body body, and an oscillator is brought into contact with the surface layer body as shown in FIG. 2 (b). Was applied to the interface between the base body molded body and the surface layer molded body for 3 seconds to be fused and bonded to produce an integrated molded body. Then, similarly, a peel test was manually performed between the base body molded body and the surface layer molded body to confirm the state of adhesion.

  Next, this integrated molded body was heated to degrease and then fired to obtain a sintered body as Example 2 which is a ceramic structural material formed by bonding a surface layer body to a base. The heating and degreasing conditions were 400 ° C. for 2 hours, and the firing conditions were 1600 ° C. and 2 hours.

(Example 3)
Using a powder containing Si ₃ N ₄ powder as a ceramic powder and polypropylene as a binder (dielectric loss with respect to 1 MHz: 2 × 10 ⁻⁴ ) in a ratio shown in Table 1, by powder press molding, 5 mm × 5 mm × 35 mm A rectangular parallelepiped base molded body was produced. Moreover, as a surface layer molded body, a slurry prepared using a mixture containing BN powder as a ceramic powder and an acrylic resin (dielectric loss with respect to 1 MHz: 2 × 10 ⁻² ) as a binder and toluene as a solvent at a ratio shown in Table 1. Was used to produce a ceramic green sheet having a dry film thickness of 50 μm and dimensions of 200 mm × 150 mm on a PET film as a support.

  Next, as shown in FIG. 3 (b), a ceramic green sheet as a surface layer molded body is laminated on a base molded body together with a support and sandwiched between a pair of molds, and the conditions of 1 MHz and 0.5 A by a high frequency welder. And applying a high frequency to the interface between the substrate molded body and the surface layer molded body for 2 seconds to fuse and bond, and then peel off the PET film as a support to form the substrate molded body and An integrated molded body in which the surface body molded body was integrated was produced. Then, using a cross-cut peel tester, a peel test was manually performed between the base molded body and the surface layer molded body to confirm the state of adhesion.

  Subsequently, this integrated molded body was heated and degreased, and then fired to obtain a sintered body as Example 3 which is a ceramic structural material formed by bonding a surface layer body to a base. The heating and degreasing conditions were 400 ° C. for 2 hours and the firing conditions were 1800 ° C. for 3 hours.

Example 4
Using a compound containing Al ₂ O ₃ powder (dielectric loss with respect to 1 MHz: 4 × 10 ⁻⁴⁾ as a ceramic powder and a fluororesin (dielectric loss with respect to 1 MHz: less than 3 × 10 ⁻⁴ ) as a binder at a ratio shown in Table 1, A base molded body having a rectangular parallelepiped shape of 5 mm × 5 mm × 35 mm was produced by injection molding, and ZrO ₂ powder as a ceramic powder and paraffin wax (dielectric loss with respect to 1 MHz: 2 × 10 ⁻⁴ ) as shown in Table 1. A 5 mm × 5 mm × 35 mm cuboid-shaped surface layer molded body was produced by injection molding using the compound contained in a proportion.

  Next, the surface layer body is overlaid and laminated on the base body, and is sandwiched between a pair of molds as shown in FIG. 1 (b), and a high frequency is applied under conditions of 1 MHz and 0.4 A by a high frequency welder. Then, fine vibration was applied to the interface between the base body molded body and the surface layer molded body for 3 seconds to be fused and bonded to produce an integrated molded body. Then, a 200 g weight was hung and lifted on the base molded body side of the integrally molded body, and a peel test was manually performed between the base molded body and the surface layer molded body to confirm the state of adhesion.

  Subsequently, this integrated molded body was heated and degreased, and then fired to obtain a sintered body as Example 4 which is a ceramic structural material formed by bonding a surface layer body to a substrate. The heating and degreasing conditions were 400 ° C. for 2 hours, and the firing conditions were 1600 ° C. and 2 hours.

(Example 5)
Using a compound containing Si ₃ N ₄ powder as a ceramic powder and acrylic as a binder (resonance characteristics with respect to 1 kHz: 4 × 10 ⁻² ) in a ratio shown in Table 1, a rectangular parallelepiped shape of 5 mm × 5 mm × 35 mm is formed by injection molding. A base compact was produced. Further, a rectangular parallelepiped of 5 mm × 5 mm × 35 mm is formed by injection molding using a compound containing Si ₃ N ₄ powder as ceramic powder and nylon (resonance characteristic with respect to 1 kHz: 2 × 10 ⁻² ) as a binder at a ratio shown in Table 1. A shaped surface layer body was produced.

  Next, a surface layer molded body is laminated and laminated on this base molded body, and is sandwiched between a pair of molds as shown in FIG. 1 (b), and an ultrasonic wave is applied under a condition of 1 kHz by a high frequency welder. A fine vibration was applied to the interface between the base body molded body and the surface body molded body for 3 seconds to melt and bond to form an integrated molded body. Then, a 200 g weight was hung and lifted on the base molded body side of the integrally molded body, and a peel test was manually performed between the base molded body and the surface layer molded body to confirm the state of adhesion.

  Subsequently, this integrated molded body was heated and degreased, and then fired to obtain a sintered body as Example 5 which is a ceramic structural material formed by bonding a surface layer body to a substrate. The heating and degreasing conditions were 400 ° C. for 2 hours and the firing conditions were 1800 ° C. for 3 hours.

(Comparative Example 1)
Using a compound containing Si ₃ N ₄ powder as a ceramic powder and a phenol resin (dielectric loss: 0 to 1 MHz: 0) as a binder at a ratio shown in Table 2, a rectangular body-shaped base molded body of 5 mm × 5 mm × 35 mm is formed by injection molding. Was made. Further, by using a compound containing Si ₃ N ₄ powder as a ceramic powder and paraffin wax (dielectric loss with respect to 1 MHz: 2 × 10 ⁻⁴ ) as a binder at a ratio shown in Table 2, injection molding is performed to have a size of 5 mm × 5 mm × 35 mm. A rectangular parallelepiped surface layer molded body was produced.

  Next, the surface layer body is overlaid and laminated on the base body, and is sandwiched between a pair of molds as shown in FIG. 1 (b), and a high frequency is applied under conditions of 1 MHz and 0.4 A by a high frequency welder. Then, a fine vibration was applied to the interface between the base molded body and the surface layer molded body for 3 seconds to produce an integrated molded body. Then, similarly, a peel test was manually performed between the base body molded body and the surface layer molded body to confirm the state of adhesion.

  Next, this integrated molded body was heated to degrease and then fired to obtain a sintered body as Comparative Example 1, which is a ceramic structural material formed by bonding a surface layer body to a substrate. The heating and degreasing conditions were 500 ° C. for 8 hours, and the firing conditions were 1800 ° C. for 3 hours.

(Comparative Example 2)
Using a compound containing Si ₃ N ₄ powder as a ceramic powder and a phenol resin (resonance characteristics with respect to 1 kHz: 0) as a binder at a ratio shown in Table 2, a rectangular base-shaped body molded body of 5 mm × 5 mm × 35 mm is formed by injection molding. Was made. Further, by using a compound containing Si ₃ N ₄ powder as a ceramic powder and paraffin wax (dielectric loss with respect to 1 MHz: 2 × 10 ⁻⁴ ) as a binder at a ratio shown in Table 2, injection molding is performed to have a size of 5 mm × 5 mm × 35 mm. A rectangular parallelepiped surface layer molded body was produced.

  Next, the surface layer body is overlaid and laminated on the base body body, and an oscillator is brought into contact with the surface layer body as shown in FIG. 2 (b). Was applied to the interface between the substrate molded body and the surface layer molded body for 3 seconds to produce an integrated molded body. Then, similarly, a peel test was manually performed between the base body molded body and the surface layer molded body to confirm the state of adhesion.

  Next, the integrated molded body was heated, degreased, and then fired to obtain a sintered body of Comparative Example 2, which is a ceramic structural material formed by bonding a surface layer body to a substrate. The heating and degreasing conditions were 500 ° C. for 8 hours, and the firing conditions were 1800 ° C. for 3 hours.

(Comparative Example 3)
Using a compound containing Si ₃ N ₄ powder as a ceramic powder and a polyether ether ketone resin (dielectric loss: 0 for 1 MHz: 0) as a binder in a ratio shown in Table 2, a rectangular parallelepiped shape of 5 mm × 5 mm × 35 mm is formed by injection molding. A base compact was produced. In addition, a rectangular parallelepiped shape of 5 mm × 5 mm × 35 mm is formed by injection molding using a compound containing Si ₃ N ₄ powder as ceramic powder and polyether ketone resin (dielectric loss with respect to 1 MHz: 0) in a ratio shown in Table 2 as a binder. A surface layer molded body was prepared.

  Next, the surface layer body is overlaid and laminated on the base body, and is sandwiched between a pair of molds as shown in FIG. 1 (b), and a high frequency is applied under conditions of 1 MHz and 0.4 A by a high frequency welder. Then, fine vibration was applied to the interface between the base body molded body and the surface layer body molded body for 3 seconds to produce an integrated molded body. Then, similarly, a peel test was manually performed between the base body molded body and the surface layer molded body to confirm the state of adhesion.

  Subsequently, this integrated molded body was heated and degreased, and then fired to obtain a sintered body as Comparative Example 3, which is a ceramic structural material formed by bonding a surface layer body to a base. The heating and degreasing conditions were 500 ° C. for 8 hours, and the firing conditions were 1800 ° C. for 3 hours.

  For each example obtained as described above, the results of the manual peeling test between the base molded body of the integrated molded body and the surface layer molded body, and the bonding interface of the sintered body held over the fluorescent lamp Table 3 shows the results of confirming the presence or absence of peeling by visually confirming the transmitted light.

  As shown in Table 3, in Example 1 to Example 5, there was no peeling in the integrated molded body, and even in the sintered body, the light transmission of the fluorescent lamp at the bonding interface could not be confirmed, and peeling occurred. There wasn't. Thereby, it was confirmed that the surface layer body was satisfactorily bonded to the base body, and that the functions necessary as an integrated ceramic structure material could be achieved.

  On the other hand, Comparative Example 1 and Comparative Example 2 use a phenol resin as a binder constituting the base molded body, and had a dielectric loss of 0 at a frequency of 1 MHz and a resonance characteristic of 0 at a frequency of 1 kHz. Heat generation did not occur in the molded body itself, and adhesion due to fusion between the base body molded body and the surface layer molded body did not occur at the time of the integrated molded body, and peeling occurred. Also, in the sintered body, peeling occurred at the bonding interface between the base body and the surface layer body, and a gap was generated, so that the transmitted light of the fluorescent lamp could be confirmed, and the functions necessary as an integrated ceramic structure material were sufficient. It was something that could not be fulfilled.

  In Comparative Example 3, polyether ketone resin was used as a binder for producing the base molded body and the surface layer molded body, and the dielectric loss was 0 at a frequency of 1 MHz and the resonance characteristics were 0 at a frequency of 1 kHz. Heat generation did not occur in the base molded body itself and the surface layer molded body itself, and adhesion due to fusion between the base molded body and the surface layer molded body did not occur at the time of the integrated molded body, and peeling occurred. Also, in the sintered body, peeling occurred at the bonding interface between the base body and the surface layer body, and a gap was generated, so that the transmitted light of the fluorescent lamp could be confirmed, and the functions necessary as an integrated ceramic structure material were sufficient. It was something that could not be fulfilled.

(A)-(c) is sectional drawing for every process which shows the 1st example of embodiment of the manufacturing method of the ceramic structure material of this invention, respectively. (A)-(c) is sectional drawing for every process which shows the 2nd example of embodiment of the manufacturing method of the ceramic structure material of this invention, respectively. (A)-(c) is sectional drawing for every process which shows the 3rd example of embodiment of the manufacturing method of the ceramic structure material of this invention, respectively.

Explanation of symbols

1,11,21 ... Base molded body 2,12,22 ... Surface layer molded body 3,13,23 ... Integrated molded body 4,14,24 ... Oscillation sources 4a, 4b ... Mold
14a ・ ・ ・ Oscillator
24a, 24b ... Electrodes [1], [11], [21] ... Base [2], [12], [22] ... Surface layer bodies 5, 15, 25 ... Ceramic structure material
26 ... Support

Claims (3)

At least one of ceramic powder and binder having dielectric loss at microwave or high frequency frequency or having resonance characteristics at ultrasonic frequency, and a substrate that becomes a substrate after firing with a mixture containing ceramic powder and binder Step A for producing a molded body, and producing a surface layer molded body that becomes a surface layer body after firing using a mixture containing ceramic powder and a binder,
The surface layer molded body is laminated on the base body molded body, and microwave, high frequency or ultrasonic wave is applied to fuse the interface between the base body molded body and the surface layer molded body to produce an integrated molded body. Step B,
And a step C of obtaining a ceramic structure material in which a surface layer body is bonded to a substrate by degreasing and firing the integrated molded body.   In the step A, a ceramic green sheet is produced on a support as at least one of the base body molded body and the surface layer molded body, and in the step B, the ceramic green sheets are laminated and fused to form the integrated component. 2. The method of manufacturing a ceramic structure according to claim 1, wherein a shape is produced.   3. The method for manufacturing a ceramic structure material according to claim 1, wherein in the step B, only a part of the base body compact and the surface layer compact is fused.

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