Ceramic sintered body

Abstract

To provide a ceramic sintered body capable of reducing a change in a dielectric loss tangent in a frequency band.SOLUTION: A ceramic sintered body comprises a gahnite crystal phase, an enstatite crystal phase, a quartz crystal phase, a suanite crystal phase, a willemite crystal phase, and a Zn2Al4Si5O18 crystal phase, wherein in an X-ray diffraction pattern, a ratio of an intensity of a peak corresponding to the quartz crystal phase to an intensity of a peak corresponding to the gahnite crystal phase is 0.100 or less, and a ratio of an intensity of a peak corresponding to the willemite crystal phase to an intensity of a peak corresponding to the gahnite crystal phase is 0.120 or less.SELECTED DRAWING: None

Description

[Technical Field]

[0001] The disclosed embodiments relate to a ceramic sintered body. [Background technology]

[0002] In recent years, semiconductor devices have become faster, i.e., operate at higher frequencies. Accordingly, wiring boards on which semiconductor devices are mounted require insulating materials that are compatible with the high-frequency characteristics of the semiconductor devices. Specifically, in order to transmit high-frequency signals to the semiconductor devices, wiring board materials are required to have lower dielectric constants and dielectric loss tangents. As such a material, for example, a glass sintered body made of a glass composition primarily composed of SiO2, Al2O3, and MgO has been proposed.

[0003] For example, a known material for a high-frequency circuit board with a low dielectric constant and dielectric loss tangent in the high-frequency range is a low-temperature fired porcelain composition obtained by molding a mixed powder containing 50 to 99.9 wt % of glass composed of SiO2, Al2O3, MgO, ZnO, and B2O3, 0.01 to 49.9 wt % of zinc oxide, and 0.01 to 49.9 wt % of amorphous silica, and then firing the molded mixture at 800 to 1000°C in a non-oxidizing atmosphere to produce a gahnite crystalline phase, enstatite crystalline phase, SiO2 crystalline phase, Mg2B2O5 crystalline phase, and glass phase, or the above crystalline phases containing a willemite crystalline phase, a ZnO crystalline phase, and a glass phase (see, for example, Patent Document 1). [Prior art documents] [Patent documents]

[0004] [Patent Document 1] Japanese Patent Application Publication No. 9-208298 Summary of the Invention [Problem to be solved by the invention]

[0005] However, in the conventional technology, there is a concern that the relative permittivity or dielectric loss tangent of the material of the wiring board may change significantly in the frequency band of the signal propagating through the semiconductor element.

[0006] Thus, the conventional techniques have room for further improvement in terms of reducing the change in the relative permittivity or dielectric loss tangent of the wiring board material in the frequency band of signals propagating through semiconductor elements.

[0007] One aspect of the embodiment has been made in view of the above, and aims to provide a ceramic sintered body capable of reducing the change in relative dielectric constant across frequency bands.

[0008] Another aspect of the embodiment has been made in view of the above, and aims to provide a ceramic sintered body capable of reducing a change in dielectric loss tangent over a frequency band. [Means for solving the problem]

[0009] A ceramic sintered body according to one aspect of the embodiment includes a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, and a willemite crystalline phase.

[0010] The ceramic sintered body according to another aspect of the embodiment may include a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, and Zn2Al4Si5O 18 The quartz crystal contains a crystalline phase, and in its X-ray diffraction pattern, the ratio of the peak intensity corresponding to the gahnite crystalline phase to the peak intensity corresponding to the quartz crystalline phase is 0.100 or less, and the ratio of the peak intensity corresponding to the willemite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase is 0.120 or less. [Effects of the Invention]

[0011] According to one aspect of the embodiment, it is possible to provide a ceramic sintered body capable of reducing the change in relative dielectric constant across frequency bands.

[0012] According to one aspect of the embodiment, it is possible to provide a ceramic sintered body capable of reducing the change in dielectric loss tangent over a frequency band. [Brief explanation of the drawings]

[0013] [Figure 1] FIG. 1 is a schematic diagram for explaining the X-ray diffraction pattern of a ceramic sintered body. [Figure 2] FIG. 2 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample A. [Figure 3] FIG. 3 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample B. [Figure 4] FIG. 4 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 1. [Figure 5] FIG. 5 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 2. [Figure 6] FIG. 6 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 4. [Figure 7] FIG. 7 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 5. [Figure 8] FIG. 8 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 7. [Figure 9] FIG. 9 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 8. [Figure 10] FIG. 10 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 9. [Figure 11] FIG. 11 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 10. [Figure 12] FIG. 12 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 11. [Figure 13] FIG. 13 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 14. [Figure 14]FIG. 14 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 15. [Figure 15] FIG. 15 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 16. [Figure 16] FIG. 16 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 17. [Figure 17] FIG. 17 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 18. [Figure 18] FIG. 18 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 19. [Figure 19] FIG. 19 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 20. DETAILED DESCRIPTION OF THE INVENTION

[0014] Hereinafter, embodiments for carrying out the ceramic sintered body disclosed in the present application (hereinafter referred to as "embodiments") will be described in detail with reference to the drawings. Note that the ceramic sintered body disclosed in the present application is not limited to these embodiments.

[0015] First Embodiment First, an example of the configuration of the ceramic sintered body according to the first embodiment will be described.

[0016] The ceramic sintered body according to the first embodiment is a sintered body obtained by firing a molded body manufactured from ceramic raw materials. The ceramic sintered body according to the first embodiment may be, for example, porcelain. Here, the porcelain is a glass ceramic material with low water absorption. The ceramic sintered body according to the first embodiment can be used, for example, as an insulating material for a wiring substrate on which a semiconductor element is mounted.

[0017] The ceramic sintered body according to the first embodiment includes a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, and a willemite crystalline phase.

[0018] The crystalline phase contained in the ceramic sintered body according to the first embodiment is identified by, for example, X-ray diffraction. The inclusion of a crystalline phase in the ceramic sintered body according to the first embodiment means, for example, that in the X-ray diffraction pattern of the ceramic sintered body, the count number of a peak corresponding to the crystalline phase relative to the count number of the baseline is 10 or more. Here, the count number in the X-ray diffraction pattern of the ceramic sintered body is the output value of an X-ray diffractometer that measures the X-ray diffraction pattern of the ceramic sintered body.

[0019] The gahnite crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula ZnOAl2O3. The gahnite crystalline phase may be represented as ZnAl2O4. The gahnite crystalline phase may be a composite of ZnOAl2O3 and ZnAl2O4. The enstatite crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula MgSiO3. The quartz crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula SiO2. The suanite crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula Mg2B2O5. The willemite crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula Zn2SiO4.

[0020] However, the ratio of the number of each element in the chemical formula representing the crystalline phase is not limited to the ratio of the number of each element shown in the above chemical formula, and the ratio of the number of each element may be changed as long as the structure of the crystalline phase is maintained. Maintaining the structure of the crystalline phase means, for example, that the crystalline phase can be identified from the X-ray diffraction pattern of the ceramic sintered body.

[0021] The ceramic sintered body according to the first embodiment may contain, for example, a glass phase in addition to the gahnite crystalline phase, enstatite crystalline phase, quartz crystalline phase, suanite crystalline phase, and willemite crystalline phase. The glass phase may include, for example, SiO2, Al2O3, ZnO, MgO, and BO3. The ceramic sintered body according to the first embodiment may consist of, for example, the gahnite crystalline phase, enstatite crystalline phase, quartz crystalline phase, suanite crystalline phase, willemite crystalline phase, and the remainder being the glass phase.

[0022] The ceramic sintered body according to the first embodiment may not contain, for example, a zinc oxide crystalline phase. The absence of a crystalline phase in the ceramic sintered body according to the first embodiment means, for example, that in the X-ray diffraction pattern of the ceramic sintered body, the count number of the peak corresponding to the crystalline phase relative to the count number of the baseline is less than 10.

[0023] According to the ceramic sintered body according to the first embodiment, it is possible to reduce the change in relative dielectric constant across frequency bands.

[0024] The ceramic sintered body according to the first embodiment may have a water absorption rate of 0.1% or less. The water absorption rate of the ceramic sintered body according to the first embodiment is measured by, for example, Archimedes' method.

[0025] In this case, it is possible to further reduce the change in the dielectric constant over the frequency band. For example, the change in the dielectric constant of the ceramic sintered body in the high frequency band from 20 GHz to 67 GHz (ε(67 GHz) - ε(20 GHz)) may be 0.1 or less. ε(20 GHz) is the dielectric constant of the ceramic sintered body at a frequency of 20 GHz. ε(67 GHz) is the dielectric constant of the ceramic sintered body at a frequency of 67 GHz. The dielectric constant of the ceramic sintered body is measured, for example, by a cylindrical cavity resonator method.

[0026] For example, the rate of change Δε of the dielectric constant of the ceramic sintered body in the high frequency band of 20 GHz to 67 GHz may be 2% or less, where Δε is (ε(67 GHz)-ε(20 GHz)) / ε(20 GHz).

[0027] In addition, it is possible to reduce the change in the dielectric loss tangent over the frequency band. For example, the change in the dielectric loss tangent of the ceramic sintered body over the high frequency band of 20 GHz to 67 GHz (tan δ(67 GHz) - tan δ(20 GHz)) is 3×10 -4 The dielectric loss tangent of the sintered ceramic body at a frequency of 20 GHz may be as follows: tan δ(20 GHz) is the dielectric loss tangent of the sintered ceramic body at a frequency of 20 GHz. tan δ(67 GHz) is the dielectric loss tangent of the sintered ceramic body at a frequency of 67 GHz. The dielectric loss tangent of the sintered ceramic body is measured, for example, by a cylindrical cavity resonator method.

[0028] For example, the rate of change Δtanδ of the dielectric tangent of the ceramic sintered body in the high frequency band of 20 GHz or more and 67 GHz or less may be 34% or less. Here, the rate of change Δtanδ of the dielectric tangent of the ceramic sintered body in the high frequency band of 20 GHz or more and 67 GHz or less is (tanδ(67 GHz)-tanδ(20 GHz)) / tanδ(20 GHz).

[0029] The ceramic sintered body according to the first embodiment may contain, as main mineral crystal phases, a gahnite crystal phase, an enstatite crystal phase, a quartz crystal phase, a suanite crystal phase, and a willemite crystal phase.

[0030] The content of a certain crystalline phase among all the crystalline phases contained in the ceramic sintered body according to the first embodiment is calculated, for example, by the ratio of the count number of the peak corresponding to that crystalline phase to the count number of all the peaks in the X-ray diffraction pattern of the ceramic sintered body.

[0031] In this case, it is possible to reduce the water absorption rate of the ceramic sintered body, for example, the water absorption rate of the ceramic sintered body may be 0.05% or less.

[0032] Furthermore, the rate of change Δtanδ of the dielectric tangent of the ceramic sintered body in the high frequency band of 20 GHz or more and 67 GHz or less may be 34% or less, and the rate of change Δε of the relative dielectric constant of the ceramic sintered body in the high frequency band of 20 GHz or more and 67 GHz or less may be 1% or less.

[0033] The ceramic sintered body according to the first embodiment may further include an eskolite crystalline phase. The eskolite crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula Cr2O3. However, the ratio of the number of elements in the chemical formula representing the crystalline phase is not limited to the ratio of the number of elements represented by the above chemical formula, and may vary as long as the structure of the crystalline phase is maintained. The ceramic sintered body according to the first embodiment may be composed of, for example, a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, an eskolite crystalline phase, and the remainder being a glass phase.

[0034] In the ceramic sintered body according to the first embodiment, the eskolite crystalline phase exists among the gahnite crystalline phase, the enstatite crystalline phase, the quartz crystalline phase, the suanite crystalline phase, and the willemite crystalline phase. The eskolite crystalline phase contained in the ceramic sintered body has almost no effect on either the relative permittivity or the dielectric loss tangent of the ceramic sintered body. In other words, the eskolite crystalline phase contained in the ceramic sintered body causes almost no chemical change to any of the gahnite crystalline phase, the enstatite crystalline phase, the quartz crystalline phase, the suanite crystalline phase, and the willemite crystalline phase contained in the ceramic sintered body.

[0035] Therefore, the relative dielectric constant and dielectric loss tangent of the ceramic sintered body when it further contains an escolite crystal phase are equivalent to the relative dielectric constant and dielectric loss tangent of the ceramic sintered body when it does not contain an escolite crystal phase.

[0036] When the ceramic sintered body does not contain an eskolite crystal phase, the color tone of the ceramic sintered body is whitish. On the other hand, when the ceramic sintered body further contains an eskolite crystal phase, the color tone of the ceramic sintered body is greenish.

[0037] In this way, by the ceramic sintered body according to the first embodiment further containing an escolite crystal phase, it becomes possible to change the color tone of the ceramic sintered body without substantially changing the relative dielectric constant and dielectric tangent of the ceramic sintered body.

[0038] When the ceramic sintered body is used as an insulating material for a wiring board, the greenish color tone of the ceramic sintered body further containing the escolite crystal phase exhibits higher contrast with the color tone of the conductor than the whiteish color tone of the ceramic sintered body not containing the escolite crystal phase.

[0039] Therefore, a ceramic sintered body further containing an eskolite crystalline phase is more suitable for use as an insulating layer of a wiring board than a ceramic sintered body not containing an eskolite crystalline phase. For example, when a conductor such as copper, nickel, or gold is formed on the surface of an insulating layer made of a ceramic sintered body further containing an eskolite crystalline phase, the visibility of the conductor formed on the insulating layer can be improved. In particular, when the surface of the wiring board is irradiated with light to perform binarization processing of images of the insulating layer and conductor, the accuracy of numerical data regarding the shape and arrangement of the conductor can be improved.

[0040] Next, an example of a method for manufacturing the ceramic sintered body according to the first embodiment will be described. The method for manufacturing the ceramic sintered body according to the first embodiment is not limited to the method for manufacturing the ceramic sintered body described below.

[0041] First, a mixed powder for producing the ceramic sintered body according to the first embodiment is prepared. For example, glass powder, zinc oxide powder, and amorphous silica powder can be used as raw material powders for preparing the mixed powder. Furthermore, chromium oxide powder can be used as the raw material powder for preparing the mixed powder, if necessary. For example, SiO2-Al2O3-ZnO-MgO-B2O3-based glass can be used as the glass powder. For example, the mixed powder for producing the ceramic sintered body is prepared by mixing the raw material powders using a ball mill with alumina balls as the medium.

[0042] Next, a green sheet is produced from the prepared mixed powder. For example, a slurry is prepared by adding an organic vehicle to the prepared mixed powder. As the organic vehicle, for example, a mixture of an organic binder such as butyral resin, a plasticizer such as dibutyl phthalate (DBP), and a solvent such as toluene can be used. The prepared slurry is formed into a sheet, for example, to produce a green sheet.

[0043] Next, a plurality of the prepared green sheets are stacked and pressure-bonded to prepare a green sheet laminate. Examples of pressure and heating conditions include a temperature of about 50° C. and a pressure of about 100 MPa.

[0044] Next, the resulting laminate is heated to perform a degreasing process. Heating conditions for the degreasing process include, for example, a temperature of about 700°C. The laminate is then fired to obtain a ceramic sintered body. Firing conditions include, for example, a maximum temperature of about 925°C, a holding time of about 2 hours, and a moist nitrogen atmosphere.

[0045] <Second embodiment> First, an example of the configuration of the ceramic sintered body according to the second embodiment will be described.

[0046] The ceramic sintered body according to the second embodiment is a sintered body obtained by firing a molded body manufactured from ceramic raw materials. The ceramic sintered body according to the second embodiment may be, for example, porcelain. Here, the porcelain is a glass ceramic material with low water absorption. The ceramic sintered body according to the second embodiment can be used, for example, as an insulating material for a wiring substrate on which a semiconductor element is mounted.

[0047] The ceramic sintered body according to the second embodiment has a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, and Zn2Al4Si5O 18 Contains a crystalline phase.

[0048] The crystalline phase contained in the ceramic sintered body according to the second embodiment is identified by, for example, X-ray diffraction. The inclusion of a crystalline phase in the ceramic sintered body according to the second embodiment means, for example, that in the X-ray diffraction pattern of the ceramic sintered body, the count number of a peak corresponding to the crystalline phase relative to the count number of the baseline is 10 or more. Here, the count number in the X-ray diffraction pattern of the ceramic sintered body is the output value of an X-ray diffractometer that measures the X-ray diffraction pattern of the ceramic sintered body.

[0049] The gahnite crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula ZnOAl2O3. The gahnite crystalline phase may be represented as ZnAl2O4. The gahnite crystalline phase may be a composite of ZnOAl2O3 and ZnAl2O4. The enstatite crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula MgSiO3. The quartz crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula SiO2. The suanite crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula Mg2B2O5. The willemite crystalline phase is, for example, a crystalline phase of a mineral represented by the chemical formula Zn2SiO4. Zn2Al4Si5O 18 The crystalline phase is Zn2Al4Si5O 18 It is the crystalline phase of the mineral represented by the chemical formula Zn2Al4Si5O 18 The crystalline phase is also called zinc aluminum silicate crystalline phase.

[0050] However, the ratio of the number of each element in the chemical formula representing the crystalline phase is not limited to the ratio of the number of each element shown in the above chemical formula, and the ratio of the number of each element may be changed as long as the structure of the crystalline phase is maintained. Maintaining the structure of the crystalline phase means, for example, that the crystalline phase can be identified from the X-ray diffraction pattern of the ceramic sintered body.

[0051] The ceramic sintered body according to the second embodiment has a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, and Zn2Al4Si5O 18 In addition to the crystalline phase, the ceramic sintered body according to the second embodiment may further include, for example, a glass phase. The glass phase may be, for example, a borosilicate glass phase. The glass phase may include, for example, SiO2, Al2O3, ZnO, MgO, and B2O3. The ceramic sintered body according to the second embodiment may include, for example, a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, Zn2Al4Si5O 18 It may consist of a crystalline phase and the remainder a glassy phase.

[0052] The ceramic sintered body according to the second embodiment may not contain, for example, a zinc oxide crystalline phase. The absence of a crystalline phase in the ceramic sintered body according to the second embodiment means, for example, that in the X-ray diffraction pattern of the ceramic sintered body, the count number of the peak corresponding to the crystalline phase relative to the count number of the baseline is less than 10.

[0053] The ceramic sintered body according to the second embodiment contains, as main mineral crystal phases, a gahnite crystal phase, an enstatite crystal phase, a quartz crystal phase, a suanite crystal phase, a willemite crystal phase, and Zn2Al4Si5O 18 It may contain a crystalline phase.

[0054] The content of a certain crystalline phase among all the crystalline phases contained in the ceramic sintered body according to the second embodiment is calculated, for example, by the ratio of the count number of the peak corresponding to that crystalline phase to the count number of all the peaks in the X-ray diffraction pattern of the ceramic sintered body.

[0055] The ceramic sintered body according to the second embodiment may further contain an eskolite crystalline phase. The eskolite crystalline phase is, for example, a crystalline phase of a mineral expressed by the chemical formula Cr2O3. However, the ratio of the number of elements in the chemical formula representing the crystalline phase is not limited to the ratio of the number of elements shown in the above chemical formula, and the ratio of the number of elements may be changed as long as the structure of the crystalline phase is maintained. The ceramic sintered body according to the second embodiment may further contain, for example, a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, or a Zn2Al4Si5O 18 It may consist of a crystalline phase, an escolite crystalline phase, and the balance a glass phase.

[0056] Next, with reference to FIG. 1, an X-ray diffraction pattern of the ceramic sintered body according to the second embodiment will be roughly described.

[0057] FIG. 1 is a schematic diagram illustrating an X-ray diffraction pattern of a ceramic sintered body. In FIG. 1, the horizontal and vertical axes represent 2θ (degrees) and the number of counts, respectively. 2θ represents the diffraction angle of the diffracted X-rays. θ represents the Bragg angle of the diffracted X-rays. The number of counts is a quantity proportional to the intensity of the diffracted X-rays. The incident X-rays used in the X-ray diffraction device are, for example, Cu-Kα rays. When the incident X-rays are Cu-Kα rays, the range of 2θ is, for example, from 0 degrees to 70 degrees.

[0058] As shown in FIG. 1, the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment includes a peak corresponding to a gahnite crystalline phase, a peak corresponding to an enstatite crystalline phase, a peak corresponding to a quartz crystalline phase, a peak corresponding to a suanite crystalline phase, a peak corresponding to a willemite crystalline phase, and a peak corresponding to a ZnAlSiO 18The X-ray diffraction pattern of the ceramic sintered body according to the second embodiment may include a peak corresponding to the crystalline phase and a peak corresponding to the eskolite crystalline phase. Here, the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment may not include a peak corresponding to the eskolite crystalline phase.

[0059] An X-ray diffraction pattern may include multiple peaks corresponding to a certain crystalline phase. For example, as shown in Fig. 1, an X-ray diffraction pattern may include multiple peaks corresponding to a gahnite crystalline phase. When the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment includes multiple peaks corresponding to a certain crystalline phase, the peak with the maximum intensity (or the maximum count number) among the multiple peaks is used as the peak corresponding to the crystalline phase.

[0060] When the incident X-rays are Cu-Kα rays, the peak corresponding to the gahnite crystalline phase is the peak at 36.8±0.2 degrees 2θ. The peak corresponding to the enstatite crystalline phase is the peak at 28.1±0.2 degrees 2θ. The peak corresponding to the quartz crystalline phase is the peak at 26.6±0.2 degrees 2θ. The peak corresponding to the suanite crystalline phase is the peak at 35.1±0.2 degrees 2θ. The peak corresponding to the willemite crystalline phase is the peak at 34.0±0.2 degrees 2θ. Zn2Al4Si5O 18 The peak at 10.5±0.2 degrees 2θ is used as the peak corresponding to the crystalline phase, and the peak at 33.6±0.2 degrees 2θ is used as the peak corresponding to the escolite crystalline phase.

[0061] In the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment, the ratio of the intensity of the peak corresponding to the quartz crystal phase to the intensity of the peak corresponding to the gahnite crystal phase is 0.100 or less, and the ratio of the intensity of the peak corresponding to the willemite crystal phase to the intensity of the peak corresponding to the gahnite crystal phase is 0.120 or less.

[0062] The ratio of the intensity of the peak corresponding to the quartz crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase may be, for example, the ratio of the maximum count number of the peak corresponding to the quartz crystalline phase to the maximum count number of the peak corresponding to the gahnite crystalline phase. Similarly, the ratio of the intensity of the peak corresponding to the willemite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase may be the ratio of the maximum count number of the peak corresponding to the willemite crystalline phase to the maximum count number of the peak corresponding to the gahnite crystalline phase.

[0063] In this case, it is possible to provide a ceramic sintered body capable of reducing changes in the dielectric loss tangent over a frequency band, and it is possible to provide a ceramic sintered body capable of reducing changes in the relative permittivity and the dielectric loss tangent over a frequency band.

[0064] Here, the relative dielectric constant and dielectric loss tangent of the ceramic sintered body according to the second embodiment are measured by, for example, a cylindrical cavity resonator method or a dielectric rod resonator method.

[0065] Furthermore, it is possible to reduce the dielectric loss tangent of the ceramic sintered body at a specific frequency.It is possible to reduce the relative permittivity and dielectric loss tangent of the ceramic sintered body at a specific frequency.

[0066] In addition, it is possible to reduce the water absorption rate of the ceramic sintered body.

[0067] Here, the water absorption rate of the ceramic sintered body according to the second embodiment is measured by, for example, the Archimedes method.

[0068] Furthermore, in the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment, the ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.140 or less, and the ratio of the intensity of the peak corresponding to the Zn2Al4Si5O 18 The ratio of the intensities of the peaks corresponding to the crystalline phases may be less than or equal to 0.100.

[0069] The ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase may be, for example, the ratio of the maximum count number of the peak corresponding to the enstatite crystalline phase to the maximum count number of the peak corresponding to the gahnite crystalline phase. 18 The ratio of the intensity of the peak corresponding to the crystalline phase to the maximum count number of the peak corresponding to the gahnite crystalline phase is 18 It may also be the ratio of the maximum count number of the peak corresponding to the crystalline phase.

[0070] In this case, it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric loss tangent over a frequency band, and it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric constant over a frequency band and the change in dielectric loss tangent over a frequency band.

[0071] Furthermore, in the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment, the ratio of the intensity of the peak corresponding to the suanite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase may be 0.080 or less.

[0072] The ratio of the intensity of the peak corresponding to the gahnite crystalline phase to the intensity of the peak corresponding to the suanite crystalline phase may be, for example, the ratio of the maximum count number of the peak corresponding to the gahnite crystalline phase to the maximum count number of the peak corresponding to the suanite crystalline phase.

[0073] In this case, it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric loss tangent over a frequency band, and it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric constant over a frequency band and the change in dielectric loss tangent over a frequency band.

[0074] Furthermore, in the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment, the intensity of the peak corresponding to the gahnite crystalline phase is 18 The ratio of the intensities of the peaks corresponding to the crystalline phases may be less than or equal to 0.080.

[0075] In this case, it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric loss tangent over a frequency band, and it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric constant over a frequency band and the change in dielectric loss tangent over a frequency band.

[0076] Furthermore, in the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment, the ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase may be 0.030 or more and 0.110 or less.

[0077] In this case, it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric loss tangent over a frequency band, and it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric constant over a frequency band and the change in dielectric loss tangent over a frequency band.

[0078] Furthermore, it is possible to further reduce the dielectric loss tangent of the ceramic sintered body at a specific frequency.It is possible to further reduce the relative permittivity of the ceramic sintered body at a specific frequency and also to further reduce the dielectric loss tangent of the ceramic sintered body at a specific frequency.

[0079] Furthermore, in the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment, the ratio of the intensity of the peak corresponding to the willemite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase may be 0.060 or more and 0.090 or less.

[0080] The ratio of the intensity of the peak corresponding to the gahnite crystalline phase to the intensity of the peak corresponding to the willemite crystalline phase may be, for example, the ratio of the maximum count number of the peak corresponding to the willemite crystalline phase to the maximum count number of the peak corresponding to the gahnite crystalline phase.

[0081] In this case, it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric loss tangent over a frequency band, and it is possible to provide a ceramic sintered body capable of further reducing the change in dielectric constant over a frequency band and the change in dielectric loss tangent over a frequency band.

[0082] In the ceramic sintered body according to the second embodiment, the escolite crystal phase is a gahnite crystal phase, an enstatite crystal phase, a quartz crystal phase, a suanite crystal phase, a willemite crystal phase, and Zn2Al4Si5O 18 That is, the escolite crystal phase contained in the ceramic sintered body is present among the gahnite crystal phase, enstatite crystal phase, quartz crystal phase, suanite crystal phase, willemite crystal phase, and Zn2Al4Si5O crystal phase contained in the ceramic sintered body. 18 There is little chemical change to any of the crystalline phases.

[0083] As a result, the eskolite crystal phase contained in the ceramic sintered body has almost no effect on either the dielectric constant or the dielectric loss tangent of the ceramic sintered body. Therefore, the dielectric constant and the dielectric loss tangent of the ceramic sintered body when the ceramic sintered body further contains the eskolite crystal phase are equivalent to the dielectric constant and the dielectric loss tangent of the ceramic sintered body when the ceramic sintered body does not contain the eskolite crystal phase.

[0084] When the ceramic sintered body does not contain an eskolite crystal phase, the color tone of the ceramic sintered body is whitish. On the other hand, when the ceramic sintered body further contains an eskolite crystal phase, the color tone of the ceramic sintered body is greenish.

[0085] In this way, by the ceramic sintered body according to the second embodiment further containing an escolite crystal phase, it becomes possible to change the color tone of the ceramic sintered body without substantially changing the relative dielectric constant and dielectric tangent of the ceramic sintered body.

[0086] When the ceramic sintered body is used as an insulating material for a wiring board, the greenish color tone of the ceramic sintered body further containing the escolite crystal phase exhibits higher contrast with the color tone of the conductor than the whiteish color tone of the ceramic sintered body not containing the escolite crystal phase.

[0087] Therefore, a ceramic sintered body further containing an eskolite crystalline phase is more suitable for use as an insulating layer of a wiring board than a ceramic sintered body not containing an eskolite crystalline phase. For example, when a conductor such as copper, nickel, or gold is formed on the surface of an insulating layer made of a ceramic sintered body further containing an eskolite crystalline phase, the visibility of the conductor formed on the insulating layer can be improved. In particular, when the surface of the wiring board is irradiated with light to perform binarization processing of images of the insulating layer and conductor, the accuracy of numerical data regarding the shape and arrangement of the conductor can be improved.

[0088] Next, an example of a method for manufacturing a ceramic sintered body according to the second embodiment will be described. The method for manufacturing a ceramic sintered body according to the second embodiment is not limited to the method for manufacturing a ceramic sintered body described below.

[0089] First, a mixed powder for producing a ceramic sintered body according to the second embodiment is prepared. Examples of raw material powders for preparing the mixed powder include glass powder, zinc oxide powder, and amorphous silica powder. Furthermore, chromium oxide powder can be used as the raw material powder for preparing the mixed powder, if necessary. Examples of glass powder include borosilicate glass. For example, SiO2-Al2O3-ZnO-MgO-B2O3-based glass can be used. For example, the raw material powders are mixed in a ball mill using alumina balls as the medium to prepare the mixed powder for producing the ceramic sintered body.

[0090] Next, a green sheet is produced from the prepared mixed powder. For example, a slurry is prepared by adding an organic vehicle to the prepared mixed powder. As the organic vehicle, for example, a mixture of an organic binder such as butyral resin, a plasticizer such as dibutyl phthalate (DBP), and a solvent such as toluene can be used. The prepared slurry is formed into a sheet, for example, to produce a green sheet.

[0091] Next, a plurality of the prepared green sheets are stacked and pressure-bonded to prepare a green sheet laminate. Examples of pressure and heating conditions include a temperature of about 50° C. and a pressure of about 100 MPa.

[0092] Next, the resulting laminate is heated to perform a degreasing process. Heating conditions for the degreasing process include, for example, a temperature of about 700°C. The laminate is then fired to obtain a ceramic sintered body. Firing conditions include, for example, a firing temperature of 875°C to 1000°C, a firing time of 1 hour to 2 hours, and a moist nitrogen atmosphere.

[0093] In this way, gahnite crystalline phase, enstatite crystalline phase, quartz crystalline phase, suanite crystalline phase, willemite crystalline phase, Zn2Al4Si5O 18A ceramic sintered body can be obtained that contains a crystalline phase, an escolite crystalline phase, and a glass phase, but does not contain a zinc oxide crystalline phase.

[0094] Methods for realizing the X-ray diffraction pattern of the ceramic sintered body according to the second embodiment include, for example, adjusting the ratio of raw material powders such as glass powder, zinc oxide powder, and amorphous silica powder in the mixed powder and / or the firing temperature.

[0095] One method for achieving an X-ray diffraction pattern in which the ratio of the intensity of the peak corresponding to the quartz crystal phase to the intensity of the peak corresponding to the gahnite crystal phase is 0.100 or less is, for example, to not use crystalline silica powder as the raw material powder.

[0096] One method for achieving an X-ray diffraction pattern in which the ratio of the intensity of the peak corresponding to the willemite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.120 or less is, for example, to prepare a mixed powder so that the proportion of glass powder in the mixed powder is 71 mass% or more.

[0097] A method for realizing an X-ray diffraction pattern in which the ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.140 or less includes, for example, adjusting the firing conditions so that the firing temperature is 980°C or less.

[0098] Zn2Al4Si5O versus the intensity of the peaks corresponding to the gahnite crystalline phase 18 An example of a method for realizing an X-ray diffraction pattern in which the ratio of peak intensities corresponding to crystalline phases is 0.100 or less is to prepare a mixed powder so that the proportion of glass powder in the mixed powder is 83 mass % or less.

[0099] A method for realizing an X-ray diffraction pattern in which the ratio of the intensity of the peak corresponding to the suanite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.080 or less can be exemplified by preparing the mixed powder so that the proportion of glass powder in the mixed powder is 78 mass% or less.

[0100] Zn2Al4Si5O versus the intensity of the peaks corresponding to the gahnite crystalline phase 18 An example of a method for realizing an X-ray diffraction pattern in which the ratio of peak intensities corresponding to crystalline phases is 0.080 or less is to prepare a mixed powder so that the proportion of glass powder in the mixed powder is 78 mass % or less.

[0101] A method for realizing an X-ray diffraction pattern in which the ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.030 or more and 0.110 or less, for example, is to adjust the firing conditions so that the firing temperature is 900°C or more and 950°C or less.

[0102] A method for achieving an X-ray diffraction pattern in which the ratio of the intensity of the peak corresponding to the willemite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.060 or more and 0.090 or less can be, for example, by preparing a mixed powder so that the proportion of glass powder in the mixed powder is 71% by mass or more and 74% by mass or less, the proportion of zinc oxide powder in the mixed powder is 10% by mass or more and 12% by mass or less, and the proportion of amorphous silica powder in the mixed powder is 16% by mass or more and 17% by mass or less. [Example]

[0103] Examples of the present disclosure will be specifically described below, but the present disclosure is not limited to the examples shown below.

[0104] First, a mixed powder for producing the ceramic sintered body according to the example was prepared. Specifically, glass powder, zinc oxide powder, silica powder, and chromium oxide powder were prepared as raw material powders for preparing the mixed powder. The glass powder contained 44 mass% SiO2, 28 mass% Al2O3, 7 mass% ZnO, 11 mass% MgO, and 10 mass% B2O3. The silica powder was amorphous silica powder. The mixed powder for sample A was prepared by mixing raw material powders containing glass powder, zinc oxide powder, and amorphous silica powder in a ball mill using alumina balls as media. Similarly, the mixed powder for sample B was prepared by mixing raw material powders containing glass powder, zinc oxide powder, amorphous silica powder, and chromium oxide powder.

[0105] Table 1 shows the compositions of the mixed powders for Sample A and Sample B. [Table 1]

[0106] As shown in Table 1, the mixed powder for Sample A contained 75% by mass of glass powder, 10% by mass of zinc oxide powder, and 15% by mass of silica powder. As shown in Table 1, the mixed powder for Sample B was prepared by adding 1% by mass of chromium oxide powder to 100% by mass of the mixed powder for Sample A.

[0107] Next, a green sheet for sample A was produced from the mixed powder for sample A. Specifically, a slurry for sample A was prepared by adding an organic vehicle to the mixed powder for sample A. The organic vehicle was a mixture of butyral resin as an organic binder, dibutyl phthalate (DBP) as a plasticizer, and toluene as a solvent. A doctor blade-type sheet forming machine was used to form the slurry for sample A into a sheet, thereby producing a green sheet for sample A. Similarly, a green sheet for sample B was produced from the mixed powder for sample B. The thickness of the green sheet for sample A and the green sheet for sample B was 300 μm.

[0108] Next, five green sheets for Sample A were stacked and pressed together using a hydraulic press to produce a laminate for Sample A. The pressure and heating conditions for pressing the five green sheets for Sample A were a temperature of 50°C and a pressure of 5 MPa, respectively. Similarly, five green sheets for Sample B were stacked and pressed together to produce a laminate for Sample B. The size of the laminate for Sample A and the size of the laminate for Sample B were 100 mm × 100 mm × 1.5 mm.

[0109] Next, the laminate for sample A was fired to obtain a ceramic sintered body for sample A. Specifically, the laminate for sample A was degreased at a temperature of 700°C, and then fired at a maximum firing temperature of 925°C for a holding time of 2 hours in a moist nitrogen atmosphere. Similarly, the laminate for sample B was fired to obtain a ceramic sintered body for sample B. The ceramic sintered body for sample A and the ceramic sintered body for sample B each had dimensions of approximately 80 mm × approximately 80 mm × approximately 1.1 mm. The ceramic sintered body for sample A and the ceramic sintered body for sample B were porcelain.

[0110] Next, an X-ray diffraction pattern of the ceramic sintered body of Sample A was obtained using an X-ray diffractometer. The incident X-rays used in the X-ray diffractometer were Cu-Kα rays. By analyzing the X-ray diffraction pattern of the ceramic sintered body of Sample A, the crystalline phase contained in the ceramic sintered body of Sample A was identified.

[0111] FIG. 2 shows the X-ray diffraction pattern of the ceramic sintered body of sample A. In FIG. 2, the horizontal and vertical axes represent 2θ (degrees) and the number of counts, respectively. 2θ represents the diffraction angle of the diffracted X-rays. The range of 2θ is from 0 degrees to 70 degrees. θ represents the Bragg angle of the diffracted X-rays. The number of counts is proportional to the intensity of the diffracted X-rays.

[0112] As shown in FIG. 2, the ceramic sintered body of sample A was confirmed to contain a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, and a willemite crystalline phase. The total content of the gahnite crystalline phase, the enstatite crystalline phase, the quartz crystalline phase, the suanite crystalline phase, and the willemite crystalline phase in all crystalline phases contained in the ceramic sintered body of sample A was confirmed to be 100%. The ceramic sintered body of sample A was confirmed to contain no zinc oxide crystalline phase. Thus, the ceramic sintered body of sample A was confirmed to consist of a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, and the remainder being a glass phase.

[0113] Next, an X-ray diffraction pattern of the ceramic sintered body of Sample B was obtained using an X-ray diffractometer. The incident X-rays used in the X-ray diffractometer were Cu-Kα rays. By analyzing the X-ray diffraction pattern of the ceramic sintered body of Sample B, the crystalline phase contained in the ceramic sintered body of Sample B was identified.

[0114] FIG. 3 shows the X-ray diffraction pattern of the ceramic sintered body of sample B. In FIG. 3, the horizontal and vertical axes represent 2θ (degrees) and the number of counts, respectively. 2θ represents the diffraction angle of the diffracted X-rays. The range of 2θ is from 0 degrees to 70 degrees. θ represents the Bragg angle of the diffracted X-rays. The number of counts is proportional to the intensity of the diffracted X-rays.

[0115] As shown in Figure 3, the ceramic sintered body of sample B was confirmed to contain gahnite, enstatite, quartz, suanite, willemite, and eskolite crystalline phases. The total content of the gahnite, enstatite, quartz, suanite, and willemite crystalline phases in all crystalline phases contained in the ceramic sintered body of sample B was confirmed to be 98.8%. The total content of the eskolite crystalline phase in all crystalline phases contained in the ceramic sintered body of sample B was confirmed to be 0.2%. It was confirmed that the ceramic sintered body of sample B did not contain zinc oxide crystalline phase. Thus, it was confirmed that the ceramic sintered body of sample B consisted of gahnite, enstatite, quartz, suanite, willemite, and eskolite crystalline phases, with the remainder being a glass phase.

[0116] Next, the water absorption rate of the ceramic sintered body of Sample A was measured by Archimedes' method based on JIS-R1601. Similarly, the water absorption rate of the ceramic sintered body of Sample B was measured according to the Archimedes' method.

[0117] Next, the dielectric constant and dielectric loss tangent of the ceramic sintered body of Sample A were measured at frequencies of 20 GHz and 67 GHz using a network analyzer according to the TM011 mode cylindrical cavity resonator method. Here, the size of the ceramic sintered body of Sample A was 50 mm × 50 mm × 1 mm.

[0118] Similarly, the dielectric constant and dielectric loss tangent of the ceramic sintered body of Sample B were measured at frequencies of 20 GHz and 67 GHz using a network analyzer according to the TM011 mode cylindrical cavity resonator method. Here, the size of the ceramic sintered body of Sample B was 50 mm × 50 mm × 1 mm.

[0119] Table 2 shows the water absorption (%) and dielectric properties of the ceramic sintered bodies of Sample A and Sample B. Here, the dielectric properties are the relative permittivity and dielectric loss tangent at frequencies of 20 GHz and 67 GHz, respectively, the rate of change of the relative permittivity in the frequency band from 20 GHz to 60 GHz, and the rate of change of the dielectric loss tangent in the frequency band from 20 GHz to 60 GHz. [Table 2]

[0120] As shown in Table 2, the water absorption rate (%) of the ceramic sintered body of Sample A was 0.05%, and the water absorption rate (%) of the ceramic sintered body of Sample B was 0.02%.

[0121] As shown in Table 2, the relative dielectric constant ε(20GHz) of the ceramic sintered body of Sample A at a frequency of 20GHz was 4.9. The dielectric loss tangent tanδ(20GHz) of the ceramic sintered body of Sample A at a frequency of 20GHz was 9×10 -4 The relative dielectric constant ε(67GHz) of the ceramic sintered body of sample A at a frequency of 67GHz was 4.9. The dielectric loss tangent tanδ(67GHz) of the ceramic sintered body of sample A at a frequency of 67GHz was 12×10 -4 It was.

[0122] Therefore, as shown in Table 2, the rate of change in the dielectric constant of the ceramic sintered body of Sample A in the frequency band from 20 GHz to 60 GHz, Δε (= (ε (67 GHz) - ε (20 GHz)) / ε (20 GHz)), was 0. The rate of change in the dielectric tangent of the ceramic sintered body of Sample A in the frequency band from 20 GHz to 60 GHz, Δtanδ (= (tanδ (67 GHz) - tanδ (20 GHz)) / tanδ (20 GHz)), was 0.333.

[0123] As shown in Table 2, the relative dielectric constant ε(20 GHz) of the ceramic sintered body of Sample B at a frequency of 20 GHz was 4.9. The dielectric loss tangent tanδ(20 GHz) of the ceramic sintered body of Sample B at a frequency of 20 GHz was 9×10 -4 The relative dielectric constant ε(67GHz) of the ceramic sintered body of sample B at a frequency of 67GHz was 4.9. The dielectric loss tangent tanδ(67GHz) of the ceramic sintered body of sample B at a frequency of 67GHz was 12×10 -4 It was.

[0124] Therefore, as shown in Table 2, the rate of change in the dielectric constant of the ceramic sintered body of Sample B in the frequency band from 20 GHz to 60 GHz, Δε (= (ε (67 GHz) - ε (20 GHz)) / ε (20 GHz)), was 0. The rate of change in the dielectric tangent of the ceramic sintered body of Sample B in the frequency band from 20 GHz to 60 GHz, Δtanδ (= (tanδ (67 GHz) - tanδ (20 GHz)) / tanδ (20 GHz)), was 0.333.

[0125] In this way, it was confirmed that the ceramic sintered body according to the embodiment contains a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, and a willemite crystalline phase, thereby making it possible to reduce the change in the relative dielectric constant across the frequency band.

[0126] Next, mixed powders for producing ceramic sintered bodies according to the examples and comparative examples were prepared. Specifically, glass powder, zinc oxide powder, amorphous silica powder, crystalline silica powder, and chromium oxide powder were prepared as raw material powders for preparing the mixed powders. The glass powder contained 44 mass% SiO2, 28 mass% Al2O3, 7 mass% ZnO, 11 mass% MgO, and 10 mass% B2O3. The raw material powders were mixed in a ball mill using alumina balls as media to prepare the mixed powders for Samples 1 to 20.

[0127] Table 3 shows the composition (mass %) of the mixed powder, the firing temperature (° C.), and the firing time (hours) for Samples 1 to 20. [Table 3]

[0128] As shown in Table 3, the mixed powders for Samples 1, 2, 5-7, 9-12, 14-17, and 19 contained glass powder, zinc oxide powder, and amorphous silica powder. As shown in Table 3, the mixed powders for Samples 3, 4, 8, and 13 contained glass powder, zinc oxide powder, amorphous silica powder, and chromium oxide powder. As shown in Table 3, the mixed powder for Sample 18 contained glass powder, zinc oxide powder, and crystalline silica powder. As shown in Table 3, the mixed powder for Sample 20 contained glass powder, zinc oxide powder, amorphous silica powder, and crystalline silica powder.

[0129] Next, green sheets for Samples 1 to 20 were produced from the mixed powders for Samples 1 to 20, respectively. Specifically, slurries for Samples 1 to 20 were prepared by adding an organic vehicle to the mixed powders for Samples 1 to 20. The organic vehicle was a mixture of butyral resin as an organic binder, dibutyl phthalate (DBP) as a plasticizer, and toluene as a solvent. The slurries for Samples 1 to 20 were formed into sheets using a doctor blade sheet forming machine, thereby producing green sheets for Samples 1 to 20, respectively. The thickness of the green sheets for Samples 1 to 20 was 300 μm.

[0130] Next, five green sheets for each of Samples 1 to 20 were stacked and pressed together using a hydraulic press to produce a laminate for each of Samples 1 to 20. The pressure and heating conditions for pressing the five green sheets for each of Samples 1 to 20 were a temperature of 50°C and a pressure of 5 MPa, respectively. The size of the laminate for Samples 1 to 20 was 100 mm x 100 mm x 1.5 mm.

[0131] Next, the laminates for Samples 1 to 20 were fired to obtain ceramic sintered bodies for Samples 1 to 20, respectively. Specifically, the laminates for Samples 1 to 20 were degreased at 700°C, and then fired in a wet nitrogen atmosphere. As shown in Table 3, the firing temperature for Samples 1, 2, 4, 5, 7 to 11, 14, and 16 to 20 was 925°C. As shown in Table 3, the firing temperatures for Samples 3, 6, 12, 13, and 15 were 900°C, 950°C, 975°C, 875°C, and 1000°C, respectively. As shown in Table 3, the firing time for Samples 1 to 6 and Samples 9 to 20 was 1 hour. As shown in Table 3, the firing temperature for Samples 7 and 8 was 2 hours. The size of the ceramic sintered bodies for Samples 1 to 20 was approximately 80 mm × approximately 80 mm × approximately 1.1 mm. The ceramic sintered bodies for Samples 1 to 20 were porcelain.

[0132] Next, an X-ray diffractometer was used to obtain X-ray diffraction patterns of the ceramic sintered bodies for Samples 1 to 20. The incident X-rays used in the X-ray diffractometer were Cu-Kα rays.

[0133] First, the X-ray diffraction patterns of the ceramic sintered bodies of Samples 1 to 20 were analyzed to identify the crystalline phases corresponding to the peaks contained in the X-ray diffraction patterns of the ceramic sintered bodies of Samples 1 to 20.

[0134] Specifically, the peak at 36.8 degrees 2θ was identified as a peak corresponding to the gahnite crystalline phase. The peak at 28.1 degrees 2θ was identified as a peak corresponding to the enstatite crystalline phase. The peak at 26.6 degrees 2θ was identified as a peak corresponding to the quartz crystalline phase. The peak at 35.1 degrees 2θ was identified as a peak corresponding to the suanite crystalline phase. The peak at 34.0 degrees 2θ was identified as a peak corresponding to the willemite crystalline phase. The peak at 10.5 degrees 2θ was identified as a peak corresponding to the Zn2Al4Si5O 18The peak at 33.6 degrees 2θ was identified as the peak corresponding to the eskolite crystalline phase.

[0135] The ceramic sintered bodies of samples 1 to 20 consisted of gahnite crystalline phase, enstatite crystalline phase, quartz crystalline phase, suanite crystalline phase, willemite crystalline phase, Zn2Al4Si5O 18 It was confirmed that the crystalline phases contained in the ceramic sintered bodies of samples 1 to 20 were gahnite, enstatite, quartz, suanite, willemite, and Zn2Al4Si5O 18 It was confirmed that the total content of the crystalline phase, escolite crystalline phase, and zinc oxide crystalline phase was 100%. It was confirmed that the ceramic sintered bodies of Samples 1 to 20 did not contain zinc oxide crystalline phase. Thus, the ceramic sintered bodies of Samples 1 to 20 contained a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, Zn2Al4Si5O 18 It was confirmed that the powder consisted of a crystalline phase, an escolite crystalline phase, and a glass phase as the remainder.

[0136] FIG. 4 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 1. FIG. 5 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 2. FIG. 6 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 4. FIG. 7 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 5. FIG. 8 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 7. FIG. 9 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 8. FIG. 10 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 9. FIG. 11 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 10. FIG. 12 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 11. FIG. 13 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 14. FIG. 14 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 15. FIG. 15 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 16. FIG. 16 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 17. FIG. 17 is a graph showing the X-ray diffraction pattern of the ceramic sintered body of Sample 18. FIG. 18 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 19. FIG. 19 is a diagram showing the X-ray diffraction pattern of the ceramic sintered body of Sample 20. In FIGS. 4 to 19, the horizontal and vertical axes represent 2θ (degrees) and the number of counts, respectively. 2θ represents the diffraction angle of the diffracted X-rays. The range of 2θ is equal to or greater than 0 degrees and equal to or less than 70 degrees. θ represents the Bragg angle of the diffracted X-rays. The number of counts is an amount proportional to the intensity of the diffracted X-rays.

[0137] As shown in Figures 4 to 19, the ceramic sintered bodies of Samples 1, 2, 4, 5, 7 to 11, and 14 to 20 consisted of a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, and Zn2Al4Si5O 18It was confirmed that all the crystalline phases contained in the ceramic sintered bodies of Samples 1, 2, 4, 5, 7-11, and 14-20 were gahnite, enstatite, quartz, suanite, willemite, and Zn2Al4Si5O 18 It was confirmed that the total content of the crystalline phase and the escolite crystalline phase was 100%. It was confirmed that the ceramic sintered bodies of Samples 1, 2, 4, 5, 7 to 11, and 14 to 20 did not contain any zinc oxide crystalline phase. Thus, the ceramic sintered bodies of Samples 1, 2, 4, 5, 7 to 11, and 14 to 20 contained a gahnite crystalline phase, an enstatite crystalline phase, a quartz crystalline phase, a suanite crystalline phase, a willemite crystalline phase, Zn2Al4Si5O 18 It was confirmed that the powder consisted of a crystalline phase, an escolite crystalline phase, and a glass phase as the remainder.

[0138] Next, the X-ray diffraction patterns of the ceramic sintered bodies of Samples 1 to 20 were analyzed, and the maximum counts of each peak included in the X-ray diffraction patterns of the ceramic sintered bodies of Samples 1 to 20 were obtained as the intensity of each peak. That is, the intensity of the peak corresponding to the gahnite crystalline phase, the intensity of the peak corresponding to the enstatite crystalline phase, the intensity of the peak corresponding to the quartz crystalline phase, the intensity of the peak corresponding to the suanite crystalline phase, the intensity of the peak corresponding to the willemite crystalline phase, and the intensity of the peak corresponding to the Zn2Al4Si5O 18 The intensities of the peaks corresponding to the crystalline phase and the intensities of the peaks corresponding to the escolite crystalline phase were obtained.

[0139] Next, from the obtained peak intensities, the ratio of the peak intensity corresponding to each crystalline phase to the peak intensity corresponding to the gahnite crystalline phase was calculated. That is, the ratio of the peak intensity corresponding to the enstatite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase, the ratio of the peak intensity corresponding to the quartz crystalline phase to the peak intensity corresponding to the gahnite crystalline phase, the ratio of the peak intensity corresponding to the suanite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase, the ratio of the peak intensity corresponding to the willemite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase, and the ratio of the peak intensity corresponding to the Zn2Al4Si5O crystalline phase to the peak intensity corresponding to the gahnite crystalline phase. 18 The ratio of the intensities of the peaks corresponding to the crystalline phases and the ratio of the intensities of the peaks corresponding to the eskolite crystalline phase to the intensities of the peaks corresponding to the gahnite crystalline phase were calculated.

[0140] Table 4 shows the ratio of the intensity of the peak corresponding to each crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase for Samples 1 to 20. [Table 4]

[0141] As shown in Table 4, among Samples 1 to 20, for Samples 1 to 16, the ratio of the peak intensity corresponding to the quartz crystalline phase to the peak intensity corresponding to the gahnite crystalline phase was 0.100 or less, and the ratio of the peak intensity corresponding to the willemite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase was 0.120 or less. On the other hand, for Samples 18 and 20, the ratio of the peak intensity corresponding to the quartz crystalline phase to the peak intensity corresponding to the gahnite crystalline phase exceeded 0.100. For Samples 17 and 19, the ratio of the peak intensity corresponding to the willemite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase exceeded 0.120.

[0142] As shown in Table 4, among samples 1 to 16, for samples 1 to 14, the ratio of the peak intensity corresponding to the enstatite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase was 0.140 or less, and the ratio of the peak intensity corresponding to the Zn2Al4Si5O 18 The ratio of the intensity of the peak corresponding to the Zn2Al4Si5O crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase was 0.100 or less. On the other hand, for sample 15, the ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase was more than 0.140. For sample 16, the ratio of the intensity of the peak corresponding to the Zn2Al4Si5O crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase was 18 The ratio of the intensities of the peaks corresponding to the crystalline phase was greater than 0.100.

[0143] As shown in Table 4, among Samples 1 to 14, the ratio of the peak intensity corresponding to the suanite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase was 0.080 or less for Samples 1 to 13. On the other hand, for Sample 14, the ratio of the peak intensity corresponding to the suanite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase exceeded 0.080.

[0144] As shown in Table 4, among samples 1 to 14, samples 1 to 13 show that the Zn2Al4Si5O 18 The ratio of the peak intensity corresponding to the crystalline phase to that of the Zn2Al4Si5O 18 The ratio of the intensities of the peaks corresponding to the crystalline phase was greater than 0.080.

[0145] As shown in Table 4, among Samples 1 to 13, for Samples 1 to 11, the ratio of the peak intensity corresponding to the enstatite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase was 0.030 or more and 0.110 or less. On the other hand, for Sample 12, the ratio of the peak intensity corresponding to the enstatite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase exceeded 0.110. For Sample 13, the ratio of the peak intensity corresponding to the enstatite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase was less than 0.030.

[0146] As shown in Table 4, among Samples 1 to 20, the ratio of the peak intensity corresponding to the willemite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase for Samples 1 and 2 was 0.060 or more and 0.090 or less. On the other hand, the ratio of the peak intensity corresponding to the willemite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase for Samples 3 to 16, Sample 18, and Sample 20 was less than 0.060. For Samples 17 and 19, the ratio of the peak intensity corresponding to the willemite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase exceeded 0.090.

[0147] Next, the water absorption of the ceramic sintered bodies of Samples 1 to 20 was measured by the Archimedes method based on JIS-R1601.

[0148] Next, using a network analyzer according to the TM011 mode cylindrical cavity resonator method, the relative permittivity ε (20 GHz) and dielectric loss tangent tanδ (20 GHz) of the ceramic sintered compacts at a frequency of 20 GHz, and the relative permittivity ε (67 GHz) and dielectric loss tangent tanδ (67 GHz) of the ceramic sintered compacts at a frequency of 67 GHz were measured for Samples 3, 4, 6 to 8, 12, 13, and 15. Here, the size of the ceramic sintered compacts for Samples 3, 4, 6 to 8, 12, 13, and 15 was 50 mm × 50 mm × 1 mm.

[0149] Next, using a network analyzer according to the TE011 mode dielectric cylinder resonator method, the relative permittivity ε (20 GHz) and dielectric loss tangent tanδ (20 GHz) of the sintered ceramic compacts at a frequency of 20 GHz, and the relative permittivity ε (67 GHz) and dielectric loss tangent tanδ (67 GHz) of the sintered ceramic compacts at a frequency of 67 GHz were measured for Samples 1, 2, 5, 9 to 11, 14, and 16 to 20. Here, the size of the sintered ceramic compacts for Samples 1, 2, 5, 9 to 11, 14, and 16 to 20 was a cylinder with a diameter of 4.4 mm and a height of 2.2 mm.

[0150] Next, the rate of change in relative dielectric constant with respect to frequency, Δε / Δf, in the frequency band from 20 GHz to 60 GHz was calculated from the measured ε(20 GHz) and ε(67 GHz) for Samples 1 to 20. Here, Δε and Δf are defined as Δε=ε(67 GHz)-ε(20 GHz) and Δf=67 GHz-20 GHz, respectively.

[0151] Next, the rate of change of the dielectric tangent with respect to frequency, Δtanδ / Δf, in the frequency band from 20 GHz to 60 GHz was calculated from the measured tanδ (20 GHz) and tanδ (67 GHz) for Samples 1 to 20. Here, Δtanδ and Δf are defined as Δtanδ = tanδ (67 GHz) - tanδ (20 GHz) and Δf = 67 GHz - 20 GHz, respectively.

[0152] Table 5 shows the water absorption (%) and dielectric properties of the ceramic sintered bodies of Samples 1 to 20. Here, the dielectric properties are ε (20 GHz), tan δ (20 GHz), ε (67 GHz), tan δ (67 GHz), Δε / Δf (×10 -10 sec), and Δtanδ / Δf(×10 -13 seconds). [Table 5]

[0153] As shown in Table 5, among samples 1 to 20, the water absorption (%) of the ceramic sintered bodies of samples 1 to 16 was 0.10% or less. Furthermore, the water absorption (%) of the ceramic sintered bodies of samples 1 to 12 and samples 14 to 16 was 0.05% or less. On the other hand, the water absorption (%) of the ceramic sintered bodies of samples 17 to 20 exceeded 0.10%.

[0154] Thus, it was confirmed that the water absorption rate of the ceramic sintered body can be reduced by ensuring that in the X-ray diffraction pattern, the ratio of the peak intensity corresponding to the quartz crystal phase to the peak intensity corresponding to the gahnite crystal phase is 0.100 or less, and the ratio of the peak intensity corresponding to the willemite crystal phase to the peak intensity corresponding to the gahnite crystal phase is 0.120 or less.

[0155] As shown in Table 5, ε(20 GHz) and ε(67 GHz) for Samples 1 to 20 were 5.0 or less. As shown in Table 5, tan δ(20 GHz) for Samples 1 to 20 was 18.0×10 -4 As shown in Table 5, the tan δ (67 GHz) for samples 1 to 20 was 27.0 × 10 -4 It was as follows.

[0156] As shown in Table 5, among samples 1 to 20, tan δ (67 GHz) for samples 1 to 14 was 18.0 × 10 -4 On the other hand, the tan δ (67 GHz) for samples 15 to 20 was 19.0 × 10 -4 That was all.

[0157] Thus, in the X-ray diffraction pattern, the ratio of the intensity of the peak corresponding to the quartz crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.100 or less, the ratio of the intensity of the peak corresponding to the willemite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.120 or less, the ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.140 or less, and the ratio of the intensity of the peak corresponding to the Zn2Al4Si5O crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.150 or less. 18 It was confirmed that the dielectric loss tangent of the ceramic sintered body at a specific frequency can be further reduced by keeping the ratio of the peak intensities corresponding to the crystalline phase at 0.100 or less.

[0158] As shown in Table 5, among samples 1 to 14, the tan δ (67 GHz) of samples 1 to 11 was 15.0 × 10 -4 On the other hand, the tan δ (67 GHz) for samples 12 to 14 was 16.0 × 10 -4 That was all.

[0159] In this way, it was confirmed that the dielectric loss tangent of the ceramic sintered body at a specific frequency can be further reduced by setting the ratio of the peak intensity corresponding to the enstatite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase in the X-ray diffraction pattern to be 0.030 or more and 0.110 or less.

[0160] As shown in Table 5, the Δε / Δf values ​​for samples 1 to 20 were 0.1 × 10 -10 It was less than a second.

[0161] As shown in Table 5, among samples 1 to 20, Δtanδ / Δf for samples 1 to 16 was 0.14×10 -13 On the other hand, Δtanδ / Δf for samples 17 to 20 was 0.15×10 -13 It was more than a second.

[0162] Thus, it was confirmed that, in the X-ray diffraction pattern, the ratio of the peak intensity corresponding to the quartz crystal phase to the peak intensity corresponding to the gahnite crystal phase is 0.100 or less, and the ratio of the peak intensity corresponding to the willemite crystal phase to the peak intensity corresponding to the gahnite crystal phase is 0.120 or less, thereby making it possible to reduce the change in the dielectric loss tangent of the ceramic sintered body over the frequency band.Furthermore, it was confirmed that it is possible to reduce the change in the relative permittivity and dielectric loss tangent of the ceramic sintered body over the frequency band.

[0163] As shown in Table 5, among samples 1 to 16, Δtanδ / Δf for samples 1 to 14 was 0.13×10 -13 On the other hand, Δtanδ / Δf for Samples 15 and 16 was 0.14×10 -13 It was seconds.

[0164] Thus, in the X-ray diffraction pattern, the ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.140 or less, and the ratio of the intensity of the peak corresponding to the Zn2Al4SiO5O 18 It was confirmed that by keeping the ratio of the peak intensities corresponding to the crystalline phase at 0.100 or less, it is possible to further reduce the change in the dielectric loss tangent of the ceramic sintered body over the frequency band. Furthermore, it was confirmed that it is possible to further reduce the change in the relative permittivity of the ceramic sintered body over the frequency band and also the change in the dielectric loss tangent of the ceramic sintered body over the frequency band.

[0165] As shown in Table 5, among samples 1 to 14, Δtanδ / Δf for samples 1 to 13 was 0.11 × 10 -13 On the other hand, Δtanδ / Δf for sample 14 was 0.13×10 -13 It was seconds.

[0166] Thus, it was confirmed that when the ratio of the peak intensity corresponding to the suanite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase in the X-ray diffraction pattern is 0.080 or less, it is possible to further reduce the change in the dielectric loss tangent of the ceramic sintered body over the frequency band. Furthermore, it was confirmed that it is possible to further reduce the change in the relative permittivity of the ceramic sintered body over the frequency band and also the change in the dielectric loss tangent of the ceramic sintered body over the frequency band.

[0167] In addition, in the X-ray diffraction pattern, the intensity of the peak corresponding to the gahnite crystal phase is 18 It was confirmed that by keeping the ratio of the peak intensities corresponding to the crystalline phase at 0.080 or less, it is possible to further reduce the change in the dielectric loss tangent of the ceramic sintered body over the frequency band. Furthermore, it was confirmed that it is possible to further reduce the change in the relative permittivity of the ceramic sintered body over the frequency band and also the change in the dielectric loss tangent of the ceramic sintered body over the frequency band.

[0168] As shown in Table 5, among samples 1 to 13, Δtanδ / Δf for samples 1 to 11 is 0.09 × 10 -13 On the other hand, Δtanδ / Δf for Samples 12 and 13 was 0.11×10 -13 It was seconds.

[0169] Thus, it was confirmed that when the ratio of the peak intensity corresponding to the enstatite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase in the X-ray diffraction pattern is 0.030 or more and 0.110 or less, it is possible to further reduce the change in the dielectric loss tangent of the ceramic sintered body over the frequency band. Furthermore, it was confirmed that it is possible to further reduce the change in the relative permittivity of the ceramic sintered body over the frequency band and also the change in the dielectric loss tangent of the ceramic sintered body over the frequency band.

[0170] As shown in Table 5, among samples 1 to 11, Δtanδ / Δf for samples 1 and 2 was 0.07×10 -13 On the other hand, Δtanδ / Δf for samples 3 to 11 was 0.08×10 -13 It was more than a second.

[0171] Thus, it was confirmed that when the ratio of the peak intensity corresponding to the willemite crystalline phase to the peak intensity corresponding to the gahnite crystalline phase in the X-ray diffraction pattern is 0.060 or more and 0.090 or less, it is possible to further reduce the change in the dielectric loss tangent of the ceramic sintered body over the frequency band. Furthermore, it was confirmed that it is possible to further reduce the change in the relative permittivity of the ceramic sintered body over the frequency band and also the change in the dielectric loss tangent of the ceramic sintered body over the frequency band.

[0172] The present technology can be configured as follows: (1) including gahnite crystalline phase, enstatite crystalline phase, quartz crystalline phase, suanite crystalline phase, and willemite crystalline phase; Sintered ceramic body. (2) further comprising an escolite crystalline phase, The ceramic sintered body according to (1) above. (3) further comprising a glass phase, The ceramic sintered body according to (1) or (2). (4) Does not contain zinc oxide crystalline phase, The ceramic sintered body according to any one of (1) to (3). (5) The water absorption rate is less than 0.1%. The ceramic sintered body according to any one of (1) to (4). (6) The water absorption rate is 0.05% or less. The ceramic sintered body according to (5) above.

[0173] The present technology can also be configured as follows: (1) Gahnite crystal phase, enstatite crystal phase, quartz crystal phase, suanite crystal phase, willemite crystal phase, and Zn2Al4Si5O 18 containing a crystalline phase, In the X-ray diffraction pattern, a ratio of the intensity of the peak corresponding to the gahnite crystalline phase to the intensity of the peak corresponding to the quartz crystalline phase is 0.100 or less; the ratio of the intensity of the peak corresponding to the willemite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.120 or less; Sintered ceramic body. (2) In the X-ray diffraction pattern, a ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.140 or less; The intensity of the peaks corresponding to the gahnite crystalline phase relative to the intensity of the Zn2Al4Si5O 18 the ratio of the intensities of the peaks corresponding to the crystalline phase is less than or equal to 0.100; The ceramic sintered body according to (1) above. (3) In the X-ray diffraction pattern, the ratio of the intensity of the peak corresponding to the suanite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.080 or less. The ceramic sintered body according to (2) above. (4) In the X-ray diffraction pattern, the intensity of the peak corresponding to the gahnite crystalline phase is 18 the ratio of the intensities of the peaks corresponding to the crystalline phase is less than or equal to 0.080; The ceramic sintered body according to (2) or (3). (5) In the X-ray diffraction pattern, the ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.030 or more and 0.110 or less. The ceramic sintered body according to (3) or (4). (6) In the X-ray diffraction pattern, the ratio of the intensity of the peak corresponding to the willemite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.060 or more and 0.090 or less. The ceramic sintered body according to any one of (1) to (5). (7) further comprising an escolite crystalline phase, The ceramic sintered body according to any one of (1) to (6). (8) further comprising a glass phase, The ceramic sintered body according to any one of (1) to (7). (9) Does not contain zinc oxide crystalline phase, The ceramic sintered body according to any one of (1) to (8).

[0174] Further advantages and modifications will readily occur to those skilled in the art. Therefore, the invention in its broader aspects is not limited to the specific details and representative embodiments shown and described above. Accordingly, various modifications may be made without departing from the spirit or scope of the general inventive concept as defined by the appended claims and their equivalents.

Claims

1. Gahnite crystalline phase, enstatite crystalline phase, quartz crystalline phase, suanite crystalline phase, willemite crystalline phase, and Zn ２ Al ４ Si ５ O １８ containing a crystalline phase, In the X-ray diffraction pattern, a ratio of the intensity of a peak corresponding to the quartz crystalline phase to the intensity of a peak corresponding to the gahnite crystalline phase is 0.100 or less; the ratio of the intensity of the peak corresponding to the willemite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.120 or less; Sintered ceramic body.

2. In the X-ray diffraction pattern, a ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.140 or less; The Zn relative to the intensity of the peak corresponding to the gahnite crystalline phase ２ Al ４ Si ５ O １８ the ratio of the intensities of the peaks corresponding to the crystalline phase is 0.100 or less; The ceramic sintered body according to claim 1 .

3. In the X-ray diffraction pattern, the ratio of the intensity of a peak corresponding to the suanite crystalline phase to the intensity of a peak corresponding to the gahnite crystalline phase is 0.080 or less. The ceramic sintered body according to claim 2.

4. In the X-ray diffraction pattern, the Zn relative to the intensity of the peak corresponding to the gahnite crystalline phase ２ Al ４ Si ５ O １８ The ratio of the intensities of the peaks corresponding to the crystalline phase is 0.080 or less. The ceramic sintered body according to claim 2.

5. In the X-ray diffraction pattern, the ratio of the intensity of the peak corresponding to the enstatite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.030 or more and 0.110 or less. The ceramic sintered body according to claim 3 or 4.

6. In the X-ray diffraction pattern, the ratio of the intensity of the peak corresponding to the willemite crystalline phase to the intensity of the peak corresponding to the gahnite crystalline phase is 0.060 or more and 0.090 or less. The ceramic sintered body according to claim 1 .

7. further comprising an escolite crystalline phase, The ceramic sintered body according to claim 1 .

8. further comprising a glass phase, The ceramic sintered body according to claim 1 .

9. Does not contain zinc oxide crystalline phase, The ceramic sintered body according to claim 1 .

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