WO2023095605A1 - ガラスセラミックス及び電子部品 - Google Patents

ガラスセラミックス及び電子部品 Download PDF

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Publication number
WO2023095605A1
WO2023095605A1 PCT/JP2022/041561 JP2022041561W WO2023095605A1 WO 2023095605 A1 WO2023095605 A1 WO 2023095605A1 JP 2022041561 W JP2022041561 W JP 2022041561W WO 2023095605 A1 WO2023095605 A1 WO 2023095605A1
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Prior art keywords
glass
weight
less
ceramics
ceramic
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English (en)
French (fr)
Japanese (ja)
Inventor
淳 浦川
安隆 杉本
太一 渡邉
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Murata Manufacturing Co Ltd
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Murata Manufacturing Co Ltd
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Priority to JP2023563601A priority Critical patent/JP7758056B2/ja
Priority to CN202280077240.4A priority patent/CN118284586A/zh
Publication of WO2023095605A1 publication Critical patent/WO2023095605A1/ja
Priority to US18/665,639 priority patent/US20240300852A1/en
Anticipated expiration legal-status Critical
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    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C10/00—Devitrified glass ceramics, i.e. glass ceramics having a crystalline phase dispersed in a glassy phase and constituting at least 50% by weight of the total composition
    • C03C10/0018—Devitrified glass ceramics, i.e. glass ceramics having a crystalline phase dispersed in a glassy phase and constituting at least 50% by weight of the total composition containing SiO2, Al2O3 and monovalent metal oxide as main constituents
    • C03C10/0027—Devitrified glass ceramics, i.e. glass ceramics having a crystalline phase dispersed in a glassy phase and constituting at least 50% by weight of the total composition containing SiO2, Al2O3 and monovalent metal oxide as main constituents containing SiO2, Al2O3, Li2O as main constituents
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00—Glass compositions
    • C03C3/04—Glass compositions containing silica
    • C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
    • C03C3/089—Glass compositions containing silica with 40% to 90% silica, by weight containing boron
    • C03C3/091—Glass compositions containing silica with 40% to 90% silica, by weight containing boron containing aluminium
    • C03C3/093—Glass compositions containing silica with 40% to 90% silica, by weight containing boron containing aluminium containing zinc or zirconium
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C10/00—Devitrified glass ceramics, i.e. glass ceramics having a crystalline phase dispersed in a glassy phase and constituting at least 50% by weight of the total composition
    • C03C10/0036—Devitrified glass ceramics, i.e. glass ceramics having a crystalline phase dispersed in a glassy phase and constituting at least 50% by weight of the total composition containing SiO2, Al2O3 and a divalent metal oxide as main constituents
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C10/00—Devitrified glass ceramics, i.e. glass ceramics having a crystalline phase dispersed in a glassy phase and constituting at least 50% by weight of the total composition
    • C03C10/0054—Devitrified glass ceramics, i.e. glass ceramics having a crystalline phase dispersed in a glassy phase and constituting at least 50% by weight of the total composition containing PbO, SnO2, B2O3
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C17/00—Surface treatment of glass, not in the form of fibres or filaments, by coating
    • C03C17/06—Surface treatment of glass, not in the form of fibres or filaments, by coating with metals
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/16—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on silicates other than clay
    • C04B35/18—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on silicates other than clay rich in aluminium oxide
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C2217/00—Coatings on glass
    • C03C2217/20—Materials for coating a single layer on glass
    • C03C2217/25—Metals
    • C03C2217/251—Al, Cu, Mg or noble metals
    • C03C2217/253—Cu

Definitions

  • the present invention relates to glass ceramics and electronic components.
  • a glass-ceramic material that can be fired at a low temperature is known as a ceramic material for ceramic multilayer wiring boards.
  • RO—Al 2 O 3 —B 2 O 3 —SiO 2 (where RO is one or more of the group consisting of MgO, CaO, SrO, BaO, and ZnO)
  • a glass composition for low-temperature fired substrates which has a basic composition, both RO and Al 2 O 3 are in the range of 1 to 25 mol %, and the mol % ratio of SiO 2 /B 2 O 3 is 1.3 or less. and glass ceramics containing aggregates in the glass composition for low-temperature firing substrates.
  • the glass-ceramics described in Patent Document 1 can achieve an excellent dielectric loss of 20 ⁇ 10 ⁇ 4 or less at 3 GHz.
  • the glass composition for low-temperature firing substrates described in Patent Document 1 has a SiO 2 /B 2 O 3 mol % ratio of 1.3 or less and a high B (boron) content.
  • a glass with a high boron composition can have a low dielectric loss, but has the problem that the boron content is not stable. Specifically, there arise problems such as elution of boron into a solvent during mixing and pulverization, and volatilization of boron during firing. If the boron content decreases due to elution or volatilization, the viscosity of the glass during firing decreases, causing insufficient sintering. Also, glass in which boron has been reduced by elution or volatilization is chemically unstable and has low moisture resistance and plating solution resistance, which may lead to deterioration in quality.
  • the glass ceramics described in Patent Document 1 have a low coefficient of thermal expansion of less than 6 ppm/K, and the difference in coefficient of thermal expansion from other dielectrics and mounting substrates is large, which easily causes quality defects.
  • An object of the present invention is to solve the above problems, and to provide glass-ceramics having a low relative dielectric constant and dielectric loss and a large coefficient of thermal expansion.
  • One embodiment of the glass-ceramic of the present invention is a glass-ceramic containing a glass containing Si, B, Al and Zn, and an aggregate, wherein the glass contains 45% by weight or more and 80% by weight or less, and The aggregate contains 20 wt % or more and 50 wt % or less of SiO 2 , 20 wt % or less of Al 2 O 3 , and 10 wt % or less of ZnO, based on the weight of the glass ceramics.
  • Another embodiment of the glass-ceramic of the present invention is a glass-ceramic containing Si, B, Al and Zn, wherein the SiO2 content is 52.00 wt% or more and 71.58 wt% or less, and B 2O3 content is 6.30 wt% or more and 21.00 wt% or less, Al2O3 content is 7.63 wt% or more and 22.00 wt% or less, ZnO content is 5.04% by weight or more and 17.00% by weight or less, and the Li 2 O content is 0.55% by weight or less.
  • the electronic component of the present invention comprises a glass-ceramic layer that is a sintered body of the glass-ceramic of the present invention.
  • FIG. 1 is a cross-sectional view schematically showing an example of a laminated ceramic electronic component as an electronic component of the present invention.
  • FIG. 2 is a schematic cross-sectional view showing a laminated green sheet (unfired state) produced in the manufacturing process of the laminated ceramic electronic component in FIG.
  • the glass-ceramics and electronic components of the present invention will be described below. It should be noted that the present invention is not limited to the following configurations, and may be modified as appropriate without departing from the gist of the present invention.
  • the present invention also includes a combination of a plurality of individual preferred configurations described below.
  • the glass-ceramics of the present invention are low temperature co-fired ceramic (LTCC) materials.
  • LTCC low temperature co-fired ceramic
  • "low temperature co-fired ceramic material” means a glass-ceramic material that can be sintered at a firing temperature of 1000°C or less.
  • An embodiment of the glass-ceramic of the present invention is a glass-ceramic containing glass containing Si, B, Al and Zn, and an aggregate, wherein the glass is contained in an amount of 45% by weight or more and 80% by weight or less, and the aggregate is 20 wt % or more and 50 wt % or less of SiO 2 , 20 wt % or less of Al 2 O 3 , and 10 wt % or less of ZnO, based on the weight of the glass-ceramics.
  • the glass used in the present invention contains Si, B, Al and Zn.
  • the glass has a SiO 2 content of 15% by weight or more and 65% by weight or less , and a B 2 O 3 content of 11% by weight or more and 30% by weight or less .
  • 2 (SiO 2 /B 2 O 3 ) is 1.21 or more, and the weight ratio of Al 2 O 3 to ZnO (Al 2 O 3 /ZnO) is 0.75 or more and 1.64 or less. is preferred.
  • the content of SiO 2 contained in the glass is preferably 15% by weight or more and 65% by weight or less, more preferably 45% by weight or more and 60% by weight or less.
  • the content of SiO 2 is 15% by weight or more and 65% by weight or less, it contributes to a decrease in dielectric constant when glass-ceramics including glass are sintered. As a result, stray capacitance and the like associated with higher frequency electrical signals are suppressed.
  • the content of SiO 2 contained in the glass exceeds 65% by weight, it becomes difficult to sinter the glass at 1000° C. or less, and the crystallization temperature rises, making it difficult for ZnAl 2 O 4 crystals to precipitate. occurs.
  • the crystallization temperature exceeds 1000° C., crystals do not precipitate during firing of the glass-ceramics, so the Q value of the glass-ceramics tends to decrease.
  • the content of SiO 2 contained in the glass is less than 15% by weight, the viscosity is too low, making vitrification difficult.
  • the content of B 2 O 3 contained in the glass is preferably 11% by weight or more and 30% by weight or less, more preferably 15% by weight or more and 30% by weight or less.
  • the weight ratio of SiO 2 to B 2 O 3 is preferably 1.21 or more. When the weight ratio is within this range, the proportion of B 2 O 3 in the entire glass is small. Therefore, elution and volatilization of boron from the glass are less likely to occur, and problems such as insufficient sintering and lowering of plating solution resistance are less likely to occur.
  • the weight ratio of SiO 2 to B 2 O 3 is preferably 4 or less.
  • Al 2 O 3 in the glass contributes to improving the chemical stability of the glass.
  • ZnO in the glass forms a crystal phase of ZnAl 2 O 4 together with Al 2 O 3 .
  • the weight ratio of Al 2 O 3 to ZnO is preferably 0.75 or more and 1.64 or less. When the weight ratio is within this range, the content of ZnAl 2 O 4 in the glass is within a preferable range.
  • the glass is crystallized glass and contains ZnAl 2 O 4 which is a crystal phase precipitated from the glass.
  • ZnAl 2 O 4 is a crystal phase precipitated from the glass.
  • the crystallization temperature of the glass is preferably lower than the firing temperature of the glass ceramics.
  • the crystallization temperature of the glass is preferably 1000° C. or lower.
  • the Q value can be increased.
  • the glass may contain Li 2 O as an accessory component.
  • the content of Li 2 O is preferably 1.0% by weight or less.
  • Li 2 O in the glass contributes to lowering the viscosity of the glass.
  • the sinterability of the glass-ceramics is improved.
  • the glass-ceramics of the present invention contain 20% by weight or more and 50% by weight or less of SiO 2 as an aggregate.
  • SiO2 as aggregate is preferably quartz. Since quartz has a low dielectric constant, it can be used as an aggregate to lower the dielectric constant of glass ceramics. Quartz also contributes to increasing the coefficient of thermal expansion when the glass-ceramics are sintered. Glass has a thermal expansion coefficient of about 6 ppm/K, while quartz has a thermal expansion coefficient of about 15 ppm/K. is obtained. Therefore, the difference in thermal expansion with metal materials such as Ag and Cu used as electrodes can be reduced, so the thermal stress generated in the cooling process after sintering is reduced, and internal defects such as cracks around the electrodes are less likely to occur. Also, the reliability of mounting on a mounting substrate (for example, a resin substrate) is enhanced. However, when the amount of quartz added increases, the Q value tends to decrease slightly.
  • the coefficient of thermal expansion of the glass-ceramics can be increased to approach the coefficient of thermal expansion of the conductive layer made of copper, silver, or the like. . If the content of SiO 2 as aggregate is less than 20% by weight, the coefficient of thermal expansion of the glass-ceramics may be too small. When the content of SiO 2 as aggregate exceeds 50% by weight, the coefficient of thermal expansion of the glass-ceramics may increase.
  • Amorphous silica or silica glass may be used as SiO 2 as an aggregate. Since amorphous silica and silica glass have a lower dielectric constant than quartz, the dielectric constant of glass ceramics can be made lower. A plurality of quartz, amorphous silica, and silica glass may be used.
  • the glass-ceramics of the present invention contain 20% by weight or less of Al 2 O 3 as an aggregate.
  • the glass-ceramics of the present invention may not contain Al 2 O 3 as an aggregate.
  • Al 2 O 3 as an aggregate contributes to low dielectric loss and high mechanical strength when the glass-ceramics are sintered.
  • the addition of Al 2 O 3 increases the Q value.
  • the bending strength is increased, and by using Al 2 O 3 as an aggregate, a glass-ceramic having a bending strength exceeding 150 MPa can be obtained.
  • the bending strength of the glass ceramics is preferably high because it affects the strength of the electronic component. In particular, 150 MPa or more is more preferable.
  • the reason why the bending strength is improved is that the addition of Al 2 O 3 as an aggregate promotes precipitation of ZnAl 2 O 4 from the glass.
  • the crystal phase contains Al 2 O 3 having a high Q value and a high strength.
  • Cristobalite crystals are a kind of SiO 2 crystals, but since they undergo a phase transition at about 280° C., if cristobalite crystals precipitate during the sintering process of glass-ceramics, their volume will change significantly in a high-temperature environment, reducing reliability. From this point of view as well, the glass-ceramics preferably do not contain cristobalite crystals.
  • not containing cristobalite crystals means that the content of cristobalite crystals is below the detection limit. Presence or absence of precipitation of cristobalite crystals is confirmed by crystal structure analysis such as X-ray diffraction (XRD).
  • the amount of Al 2 O 3 added is preferably 1% by weight or more.
  • the addition of Al 2 O 3 increases the dielectric constant of the glass-ceramics. Therefore, the amount of Al 2 O 3 added as an aggregate is preferably 10% by weight or less. Also, if the amount of Al 2 O 3 added as an aggregate exceeds 20% by weight, sintering of the glass-ceramics is hindered.
  • the glass-ceramics of the present invention contain ZnO of 10% by weight or less as an aggregate.
  • the glass-ceramics of the present invention may not contain ZnO as an aggregate.
  • ZnO is included as an aggregate, sinterability can be improved.
  • the amount of ZnO added is preferably 1.0% by weight or more, more preferably 2.5% by weight or more. However, if the amount of ZnO added as an aggregate exceeds 10% by weight, the dielectric constant of the glass-ceramics increases. Also, Zn 2 SiO 4 (willemite) may be generated during firing due to the addition of ZnO.
  • the glass-ceramics of the present invention preferably contain SiO 2 , ZnAl 2 O 4 and Al 2 O 3 as crystal phases. Since SiO 2 , ZnAl 2 O 4 , and Al 2 O 3 are included as crystal phases in the glass-ceramics after firing, the dielectric constant is small, the dielectric loss is small, the Q value is high, the coefficient of thermal expansion is large, and the It becomes glass-ceramics with high strength. Quartz is preferred as the SiO2 crystal phase, and garnite is preferred as the ZnAl2O4 crystal phase . The inclusion of these crystal phases can be confirmed by crystal structure analysis such as X-ray diffraction (XRD).
  • XRD X-ray diffraction
  • the glass-ceramic of the present invention preferably has a dielectric constant of 5.0 or less, more preferably 4.5 or less, and even more preferably 4.3 or less.
  • the dielectric constant of glass-ceramics is determined as measured at 6 GHz or 30 GHz.
  • a dielectric constant at 6 GHz can be measured by a perturbation method.
  • the dielectric constant at 30 GHz can be measured by the TE 011 mode cavity resonator method based on JIS R 1641.
  • the present invention it is possible to provide glass-ceramics having a low boron content, a low dielectric constant and dielectric loss, a high Q value, and a large coefficient of thermal expansion. Furthermore, by including Al 2 O 3 as an aggregate, the Q value can be increased and the bending strength can be improved.
  • the glass and the Aggregates can be distinguished or separated.
  • elemental analysis such as wavelength dispersive X-ray analysis (WDX), energy dispersive X-ray analysis (EDX), inductively coupled plasma atomic emission spectrometry (ICP), etc.
  • WDX wavelength dispersive X-ray analysis
  • EDX energy dispersive X-ray analysis
  • ICP inductively coupled plasma atomic emission spectrometry
  • SiO 2 content as glass and the SiO 2 content as aggregate can be measured respectively. The same applies to other elements.
  • Another embodiment of the glass-ceramic of the present invention is a glass-ceramic containing Si, B, Al and Zn, wherein the SiO2 content is 52.00 wt% or more and 71.58 wt% or less, and B 2O3 content is 6.30 wt% or more and 21.00 wt% or less, Al2O3 content is 7.63 wt% or more and 22.00 wt% or less, ZnO content is 5.04% by weight or more and 17.00% by weight or less, and the Li 2 O content is 0.55% by weight or less.
  • the SiO2 content is preferably 60% by weight or more
  • the B2O3 content is preferably 15% by weight or less
  • the Al2O3 content is preferably 15% by weight or less
  • the ZnO content is preferably 12% by weight or less.
  • Another embodiment of the glass-ceramics of the present invention corresponds to a part of the glass-ceramics in which the contents of Si, B, Al and Zn are defined without distinguishing between the glass and the aggregate. . Therefore, another embodiment of the glass-ceramic of the present invention has the effect exhibited by one embodiment of the glass-ceramic of the present invention.
  • the electronic component of the present invention comprises a glass-ceramic layer that is a sintered body of the glass-ceramic of the present invention.
  • the electronic component of the present invention for example, a laminate having a plurality of glass ceramic layers that are sintered bodies of the glass ceramics of the present invention, a laminated ceramic substrate using the laminate, and a chip mounted on the ceramic substrate and laminated ceramic electronic components.
  • the electronic component of the present invention has a low dielectric constant and a low dielectric loss because it includes the glass ceramic layer which is a sintered body of the glass ceramic of the present invention.
  • a laminate comprising a plurality of glass ceramic layers, which is a sintered body of glass ceramics of the present invention, can be used for, for example, a ceramic multilayer substrate for communication and a laminated dielectric filter.
  • the electronic component of the present invention has a low relative dielectric constant and dielectric loss and a high Q value, and is particularly suitable as an electronic component used in the millimeter wave band.
  • the coefficient of thermal expansion of the glass-ceramic layer is preferably 6 ppm/K or more.
  • the dielectric constant of the glass-ceramic layer is preferably 4.5 or less.
  • the Q value of the glass-ceramic layer is preferably 800 or more.
  • the bending strength of the glass ceramic layer is preferably 150 MPa or more.
  • the electronic component of the present invention has an electrode made of a metal containing Cu, and the content of Cu contained in the glass ceramic layer is preferably 0.5% by weight or less in terms of CuO.
  • Cu When Cu is used as an electrode, diffusion of Cu occurs from the electrode into the glass ceramics. Cu diffused from the electrode may change the sinterability of the glass-ceramics around the electrode, causing defects such as voids. Such problems can be prevented by adding a small amount of CuO as an aggregate to the glass ceramics. Cu may be added more than 0.5% by weight in terms of CuO, but in that case, deposition of Cu tends to occur in the glass ceramics, so there is a concern that shorts may occur between electrodes when used as an electronic component. There is
  • FIG. 1 is a cross-sectional view schematically showing an example of a laminated ceramic electronic component as the electronic component of the present invention.
  • the electronic component 2 includes a laminate 1 formed by laminating a plurality of glass ceramic layers 3 (five layers in FIG. 1), and chip components 13 and 14 mounted on the laminate 1.
  • the laminate 1 is also a laminated ceramic substrate.
  • the glass-ceramic layer 3 is a sintered body of the glass-ceramic of the present invention. Therefore, an electronic device comprising a laminated body 1 in which a plurality of glass ceramic layers 3 are laminated, a laminated ceramic substrate using the laminated body 1, and chip components 13 and 14 mounted on the laminated ceramic substrate (laminated body 1) All of the components 2 are electronic components of the present invention.
  • the compositions of the plurality of glass ceramic layers 3 may be the same or different, but are preferably the same.
  • the laminate 1 may further have a conductor layer.
  • the conductor layer constitutes, for example, passive elements such as capacitors and inductors, and connection wiring for electrical connection between elements.
  • Such conductor layers include conductor layers 9, 10, 11 and via hole conductor layer 12 as shown in FIG.
  • the conductor layers 9, 10, 11 and the via-hole conductor layer 12 preferably contain Ag or Cu as a main component.
  • Ag or Cu As a main component.
  • the conductor layer 9 is arranged inside the laminate 1 . Specifically, the conductor layer 9 is arranged at the interface between the glass ceramic layers 3 .
  • the conductor layer 10 is arranged on one main surface of the laminate 1 .
  • the conductor layer 11 is arranged on the other main surface of the laminate 1 .
  • the via-hole conductor layers 12 are arranged so as to penetrate the glass ceramic layer 3, and electrically connect the conductor layers 9 in different layers, electrically connect the conductor layers 9 and 10, It plays a role of electrically connecting the layers 9 and 11 .
  • the laminate 1 is manufactured, for example, as follows.
  • (A) Preparation of glass The content of SiO2 is 15% by weight or more and 65% by weight or less, and the content of B2O3 is 11% by weight or more and 30% by weight or less .
  • 2 (SiO 2 /B 2 O 3 ) is 1.21 or more, and the weight ratio of Al 2 O 3 to ZnO (Al 2 O 3 /ZnO) is 0.75 or more and 1.64 or less.
  • a glass is prepared by mixing SiO 2 , B 2 O 3 , Al 2 O 3 and ZnO and optionally added auxiliary components (Li 2 O, etc.) as follows.
  • the glass-ceramics of the present invention are prepared by mixing glass with SiO 2 , Al 2 O 3 and ZnO as aggregates and other aggregates (such as CuO) added as necessary. do.
  • (C) Production of green sheet The glass-ceramic of the present invention is mixed with a binder, a plasticizer and the like to prepare a ceramic slurry. Then, the ceramic slurry is formed on a substrate film (eg, polyethylene terephthalate (PET) film) and then dried to produce a green sheet.
  • a substrate film eg, polyethylene terephthalate (PET) film
  • FIG. 2 is a schematic cross-sectional view showing a laminated green sheet (unfired state) produced in the manufacturing process of the laminated ceramic electronic component in FIG.
  • the laminated green sheet 21 is formed by laminating a plurality of green sheets 22 (five in FIG. 2).
  • the green sheet 22 becomes the glass ceramic layer 3 after firing.
  • Conductor layers including the conductor layers 9 , 10 , 11 and the via-hole conductor layer 12 may be formed on the laminated green sheet 21 .
  • the conductor layer can be formed by screen printing, photolithography, or the like using a conductive paste containing Ag or Cu.
  • the sintering temperature of the laminated green sheet 21 is not particularly limited as long as it is a temperature at which the glass ceramics of the present invention constituting the green sheet 22 can be sintered.
  • the firing atmosphere of the laminated green sheet 21 is not particularly limited, but when a material such as Ag that is difficult to oxidize is used as the conductor layers 9, 10, 11 and the via-hole conductor layer 12, an air atmosphere is preferable. When using a material that is easily oxidized, a low-oxygen atmosphere such as a nitrogen atmosphere is preferable. Also, the atmosphere for firing the laminated green sheet 21 may be a reducing atmosphere.
  • the laminated green sheet 21 may be fired while sandwiched between the restraining green sheets.
  • the constraining green sheet mainly contains an inorganic material (for example, Al 2 O 3 ) that does not substantially sinter at the sintering temperature of the glass-ceramic of the present invention that constitutes the green sheet 22 . Therefore, the constraining green sheet does not shrink when the laminated green sheet 21 is fired, and acts to suppress the shrinkage of the laminated green sheet 21 in the main surface direction. As a result, the dimensional accuracy of the obtained laminate 1 (in particular, the conductor layers 9, 10, 11 and the via-hole conductor layer 12) is enhanced.
  • Chip components 13 and 14 may be mounted on the laminate 1 while being electrically connected to the conductor layer 10 .
  • the electronic component 2 having the laminate 1 is configured.
  • the chip components 13 and 14 include, for example, LC filters, capacitors, inductors, and the like.
  • the electronic component 2 may be mounted on a mounting board (for example, a mother board) so as to be electrically connected via the conductor layer 11 .
  • a mounting board for example, a mother board
  • the thickness of the fired sample was measured, and the dielectric constant and Q value (reciprocal of dielectric loss) at 6 GHz were measured by the perturbation method.
  • the following instruments were used to measure the dielectric constant and Q value.
  • a dielectric constant of 5.0 or less and a Q value of 500 or more were considered good.
  • Network analyzer Keysight 8757D
  • Signal generator Keysight Synthesized Sweeper 83751
  • Resonator self-made jig (resonant frequency: 6 GHz)
  • the cable loss was measured by connecting the network analyzer and the signal generator. Further, the resonator was calibrated using a standard substrate (made of quartz, dielectric constant: 3.73, Q value: 4545@6 GHz, thickness: 0.636 mm).
  • Thermal expansion coefficient ⁇ For each of the ceramics L1 to L29, a dilatometer TD5000SE (manufactured by Netsch) was used to determine the thermal expansion coefficient ⁇ in the temperature range from room temperature to 600°C. A thermal expansion coefficient ⁇ of 6.0 ppm/K or more was considered good.
  • the laminate having the glass ceramic layer which is the sintered body of the glass ceramics of the present invention, has a low dielectric constant, a high Q value (low dielectric loss), and a large coefficient of thermal expansion. Recognize.
  • L6 had a low coefficient of thermal expansion ⁇ . This is believed to be due to the SiO2 content of the aggregate being less than 20% by weight.
  • L7 was undersintered. This is probably because the glass content is less than 45% by weight and the aggregate SiO 2 is more than 50% by weight. This is probably because L12 was also insufficiently sintered and the glass content was less than 45% by weight.
  • L13 is also insufficiently sintered, which is considered to be due to the Al 2 O 3 aggregate exceeding 20% by weight.
  • L21 has a high dielectric constant and a low Q value. This is probably because ZnO in the aggregate exceeds 10% by weight.
  • each glass-ceramic has a small dielectric constant even at a millimeter wave band frequency (approximately 30 GHz), and a high Q value is obtained.
  • the dielectric constant is 4.5 or less and the Q value is 800 or more.
  • the glass-ceramics of the present invention are materials suitable for electronic parts for millimeter wave bands.
  • the contents of Si, B, Al and Zn are specified without distinguishing between the glass and the aggregate in one embodiment of the glass ceramics.
  • the ratio of each element in the glass-ceramics in the above examples can be calculated from the glass compositions shown in Table 1 and the glass-ceramics compositions in Table 2.
  • Each element is represented as an oxide.
  • Table 4 shows examples of the ratio of each element in several glass-ceramics calculated in this way.
  • the glass-ceramics of the present invention have a low content of B 2 O 3 as glass-ceramics, so boron is less likely to be eluted from the glass-ceramics after firing, and the glass-ceramics are resistant to plating solutions. It is difficult to cause problems such as deterioration of sexuality.
  • the dielectric constant can be lowered.
  • the glass-ceramics preferably contain 60% by weight or more of SiO 2 , 15% by weight or less of B 2 O 3 , 15% by weight or less of Al 2 O 3 , and 12% by weight or less of ZnO. As a result, the dielectric constant can be made 5 or less, and further 4.5 or less.

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  • Ceramic Engineering (AREA)
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  • Compositions Of Oxide Ceramics (AREA)
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WO2024257630A1 (ja) * 2023-06-16 2024-12-19 株式会社村田製作所 ガラスセラミックス構造体及び電子部品

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JPS60235744A (ja) * 1984-05-04 1985-11-22 Asahi Glass Co Ltd セラミック基板用組成物
JPS6117441A (ja) * 1984-07-02 1986-01-25 コーニング　グラス　ワークス ＺｎＯを含有するムライトガラスセラミツク
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JP7758056B2 (ja) 2021-11-25 2025-10-22 株式会社村田製作所 ガラスセラミックス及び電子部品
WO2024257630A1 (ja) * 2023-06-16 2024-12-19 株式会社村田製作所 ガラスセラミックス構造体及び電子部品
JPWO2024257630A1 (https=) * 2023-06-16 2024-12-19

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