WO2021256409A1 - ガラスセラミックス及び積層セラミック電子部品 - Google Patents

ガラスセラミックス及び積層セラミック電子部品 Download PDF

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WO2021256409A1
WO2021256409A1 PCT/JP2021/022434 JP2021022434W WO2021256409A1 WO 2021256409 A1 WO2021256409 A1 WO 2021256409A1 JP 2021022434 W JP2021022434 W JP 2021022434W WO 2021256409 A1 WO2021256409 A1 WO 2021256409A1
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weight
glass
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content
ceramic
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PCT/JP2021/022434
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French (fr)
Japanese (ja)
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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 JP2022531783A priority Critical patent/JP7494908B2/ja
Priority to CN202180043343.4A priority patent/CN115916717A/zh
Priority to CN202511652894.7A priority patent/CN121494324A/zh
Publication of WO2021256409A1 publication Critical patent/WO2021256409A1/ja
Priority to US18/065,980 priority patent/US20230117436A1/en
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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
    • C03C14/00—Glass compositions containing a non-glass component, e.g. compositions containing fibres, filaments, whiskers, platelets, or the like, dispersed in a glass matrix
    • C03C14/004—Glass compositions containing a non-glass component, e.g. compositions containing fibres, filaments, whiskers, platelets, or the like, dispersed in a glass matrix the non-glass component being in the form of particles or flakes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
    • H01B3/02—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of inorganic substances
    • H01B3/12—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of inorganic substances ceramics
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    • 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
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    • 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
    • C03C10/0009—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 silica as main constituent
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    • C03C3/00—Glass compositions
    • C03C3/04—Glass compositions containing silica
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    • C03C3/00—Glass compositions
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    • C03C3/062—Glass compositions containing silica with less than 40% silica by weight
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    • 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
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G4/00—Fixed capacitors; Processes of their manufacture
    • H01G4/002—Details
    • H01G4/018—Dielectrics
    • H01G4/06—Solid dielectrics
    • H01G4/08—Inorganic dielectrics
    • H01G4/12—Ceramic dielectrics
    • H01G4/129—Ceramic dielectrics containing a glassy phase, e.g. glass ceramic
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0306—Inorganic insulating substrates, e.g. ceramic, glass
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
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    • B32B2250/00—Layers arrangement
    • B32B2250/24—All layers being polymeric
    • B32B2250/244—All polymers belonging to those covered by group B32B27/36
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    • B32—LAYERED PRODUCTS
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    • B32B2255/00—Coating on the layer surface
    • B32B2255/10—Coating on the layer surface on synthetic resin layer or on natural or synthetic rubber layer
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    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/20—Properties of the layers or laminate having particular electrical or magnetic properties, e.g. piezoelectric
    • B32B2307/202—Conductive
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/70—Other properties
    • B32B2307/724—Permeability to gases, adsorption
    • B32B2307/7242—Non-permeable
    • B32B2307/7246—Water vapor barrier
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/70—Other properties
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    • B32B2457/00—Electrical equipment
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
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    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
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Definitions

  • the present invention relates to glass ceramics and laminated ceramic electronic components.
  • Patent Document 1 describes 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 a low-temperature fired substrate having a basic composition, in which RO and Al 2 O 3 are both in the range of 1 to 25 mol%, and the mol% ratio of SiO 2 / B 2 O 3 is 1.3 or less.
  • glass ceramics containing an aggregate in the glass composition for a low-temperature fired substrate are disclosed.
  • 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 a low-temperature fired substrate described in Patent Document 1 has a mol% ratio of SiO 2 / B 2 O 3 of 1.3 or less, and has a high B (boron) content.
  • Such a glass having a high boron composition can reduce the dielectric loss, but has a problem that the boron content is not stable. Specifically, there arises a problem that boron elutes into a solvent during mixing and grinding, and boron volatilizes during firing. When the boron content decreases due to elution or volatilization, the viscosity of the glass during firing decreases, which causes insufficient sintering.
  • glass in which boron is reduced due to elution or volatilization is chemically unstable and has low moisture resistance and plating solution resistance, which may lead to quality deterioration.
  • the glass ceramics described in Patent Document 1 have a large temperature change of 100 ppm / K or more in dielectric constant, and are difficult to apply to electronic devices such as filters. Further, since the coefficient of thermal expansion is as low as less than 6 ppm / K and the difference in coefficient of thermal expansion from other dielectrics and mounting substrates is large, it is likely to cause quality defects.
  • the present invention has been made to solve the above problems, and an object of the present invention is to provide glass ceramics having a low boron content, a small dielectric constant and a small dielectric loss, a small temperature dependence of the dielectric constant, and a large coefficient of thermal expansion. do.
  • One embodiment of the glass ceramics of the present invention is a glass ceramic containing Si, B, Al and Zn-containing glass and an aggregate, and the glass has a SiO 2 content of 20% by weight or more. and 55 wt% or less, B 2 content of O 3 is 15 wt% or more and 30 wt% or less, the weight ratio of SiO 2 to B 2 O 3 (SiO 2 / B 2 O 3) is 1.21 or more, the weight ratio of Al 2 O 3 with respect to ZnO (Al 2 O 3 / ZnO ) is 0.8 or more and 1.3 or less, as the aggregate, the weight of the glass ceramic, 20 wt % Or more and 50% by weight or less SiO 2 , 1% by weight or more and 10% by weight or less of TiO 2 , 3% by weight or less of ZrO 2 and 1% by weight or less of ZnO in the glass. 2.
  • the contents of ZrO 2 , SnO 2 and SrO are all 0% by weight or more and
  • Another embodiment of the glass ceramic of the present invention is a glass ceramic containing Si, B, Al, Zn, Ti and Zr, and has a SiO 2 content of 41.70% by weight or more and 67.48% by weight or less.
  • the B 2 O 3 content is 8.74% by weight or more and 19.50% by weight or less
  • the Al 2 O 3 content is 4.875% by weight or more and 21.125% by weight or less.
  • ZnO content is 5.175% by weight or more and 21.425% by weight or less
  • TiO 2 content is 1% by weight or more and 13.5% by weight or less
  • ZrO 2 content is 6.8. It is characterized in that it is not more than% by weight, the content of SnO 2 is 3.95% by weight or less, and the content of SrO is 3.95% by weight or less.
  • the laminated ceramic electronic component of the present invention is characterized by comprising a glass ceramic layer which is a sintered body of the glass ceramic of the present invention.
  • the present invention it is possible to provide glass ceramics having a low boron content, a small dielectric constant and a small dielectric loss, a small temperature dependence of the dielectric constant, and a large coefficient of thermal expansion.
  • FIG. 1 is a cross-sectional view schematically showing an example of a laminated ceramic 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 the laminated ceramic electronic components of the present invention will be described.
  • the present invention is not limited to the following configuration, and may be appropriately modified without departing from the gist of the present invention.
  • a combination of a plurality of individual preferred configurations described below is also the present invention.
  • the glass ceramics of the present invention are low temperature co-fired ceramics (LTCC) materials.
  • LTCC low temperature co-fired ceramics
  • co-fired ceramic material at low temperature means a glass ceramic material that can be sintered at a firing temperature of 1000 ° C. or lower.
  • One embodiment of the glass ceramics of the present invention is a glass ceramic containing Si, B, Al and Zn-containing glass and an aggregate, and the glass has a SiO 2 content of 20% by weight or more. and 55 wt% or less, B 2 content of O 3 is 15 wt% or more and 30 wt% or less, the weight ratio of SiO 2 to B 2 O 3 (SiO 2 / B 2 O 3) is 1.21 or more, the weight ratio of Al 2 O 3 with respect to ZnO (Al 2 O 3 / ZnO ) is 0.8 or more and 1.3 or less, as the aggregate, the weight of the glass ceramic, 20 wt % Or more and 50% by weight or less SiO 2 , 1% by weight or more and 10% by weight or less of TiO 2 , 3% by weight or less of ZrO 2 and 1% by weight or less of ZnO in the glass. 2.
  • the contents of ZrO 2 , SnO 2 and SrO are all 0% by weight or more and
  • glass 20% by weight or more, includes a SiO 2 of 55 wt% or less, 15 wt% or more, and a B 2 O 3 of 30 wt% or less, B 2 O 3 to weight ratio of SiO 2 (SiO 2 / B 2 O 3) is not less 1.21 or more, the weight ratio of Al 2 O 3 with respect to ZnO (Al 2 O 3 / ZnO ) is 0.8 or more, 1.3 or less , and the as the aggregate, 20% by weight or more, and SiO 2 of 50 wt% or less, 1% by weight or more, and 10 wt% or less of TiO 2, 3 the weight percent of ZrO 2, less 1 wt% Includes ZnO. Further, the contents of TiO 2 , ZrO 2 , SnO 2 and SrO in the glass are all 0% by weight or more and 5% by weight or less.
  • the glass contains 40% by weight or more and 55% by weight or less of SiO 2 .
  • the glass contains 40% by weight or more and 55% by weight or less of SiO 2 , it contributes to a decrease in the dielectric constant when the glass ceramics are sintered. As a result, stray capacitance and the like due to high frequency of the electric signal are suppressed.
  • the content of SiO 2 exceeds 55% by weight, problems such as difficulty in sintering at 1000 ° C. or lower and difficulty in precipitation of ZnAl 2 O 4 crystals occur, but the content of SiO 2 is 55. Since it is less than% by weight, the above problem does not occur.
  • the content of SiO 2 is less than 20% by weight, the viscosity is too low and vitrification becomes difficult.
  • B 2 O 3 in the glass contributes to the decrease in glass viscosity. Therefore, the sintered body of glass-ceramics becomes dense.
  • Glass constituting the glass ceramics of the present invention B 2 O content of 3 15% by weight or more, a 30% by weight or less, the weight ratio of SiO 2 to B 2 O 3 (SiO 2 / B 2 O 3 ) it is, since it is 1.21 or more, the proportion of B 2 O 3 in the total glass is small. Therefore, the elution and volatilization of boron from the glass is unlikely to occur, and problems such as insufficient sintering and deterioration of plating solution resistance are unlikely to occur.
  • the weight ratio of SiO 2 to B 2 O 3 (SiO 2 / B 2 O 3) is 1.21 or more and 3.67 or less. If the weight ratio of SiO 2 to B 2 O 3 (SiO 2 / B 2 O 3) is in the above range, hardly occurs elution or volatilization of boron from the glass. If the weight ratio of SiO 2 to B 2 O 3 (SiO 2 / B 2 O 3) is less than 1.21, and B 2 O 3 is too large relative to the SiO 2, elution and evaporation of boron tends to occur become.
  • Al 2 O 3 in the glass contributes to the improvement of the chemical stability of the glass.
  • Zn in the glass forms ZnAl 2 O 4 together with Al.
  • the weight ratio of Al 2 O 3 with respect to ZnO is 0.8 or more, if it is 1.3 or less, the content of the ZnAl 2 O 4 in the glass is the preferred range.
  • the weight ratio of Al 2 O 3 with respect to ZnO is less than 0.8, ZnO is too much, Q value is the inverse of the dielectric loss is reduced.
  • the glass may contain an auxiliary component.
  • an auxiliary component As the subcomponent, at least one metal selected from the group consisting of alkali metals, alkaline earth metals and other metals is preferable.
  • the alkali metal preferably contains at least one of Li, Na and K.
  • the alkaline earth metal preferably contains at least one of Be, Mg, Ca, Sr and Ba.
  • the other metal preferably contains at least one of Ti, Zr and Sn.
  • the total content of the auxiliary components is preferably 0.1% by weight or more and 5% by weight or less of the total weight of the glass.
  • the crystallization of the glass is promoted, which contributes to the reduction of the dielectric loss.
  • the glass may contain at least one oxide selected from the group consisting of TiO 2 , ZrO 2 , SnO 2 and SrO.
  • the content of TiO 2 , ZrO 2 , SnO 2 and SrO in the glass is 0% by weight or more and 5% by weight or less.
  • the value of the relative permittivity becomes too large.
  • the value of the relative permittivity becomes too large.
  • the Sn content in the glass exceeds 5% by weight in terms of oxide, the Q value becomes too low. If the Sr content in the glass exceeds 5% by weight in terms of oxide, the Q value becomes too low.
  • the glass ceramics of the present invention contain 40% by weight or more and 50% by weight or less of SiO 2 as an aggregate. Quartz is preferable as the SiO 2 as an aggregate. Quartz contributes to increasing the coefficient of thermal expansion when the glass ceramics are sintered. Since the coefficient of thermal expansion of glass is about 6 ppm / K, while the coefficient of thermal expansion of quartz is about 15 ppm / K, the high coefficient of thermal expansion when the glass ceramics are sintered due to the inclusion of quartz. Is obtained. Therefore, compressive stress is generated in the cooling process after sintering, and the mechanical strength (for example, the bending strength) is increased. In addition, reliability at the time of mounting on a mounting board (for example, a resin board) is enhanced.
  • a mounting board for example, a resin board
  • the coefficient of thermal expansion of glass ceramics can be increased to approach the coefficient of thermal expansion of a conductive layer made of copper, silver or the like. If the content of quartz as an aggregate is less than 20% by weight, the coefficient of thermal expansion may be too small. If the content of quartz as an aggregate exceeds 50% by weight, the coefficient of thermal expansion may be too large.
  • the glass ceramics of the present invention contain 1% by weight or more and 10% by weight or less of TiO 2 as an aggregate.
  • TiO 2 has a negatively large temperature coefficient (TCC) of relative permittivity.
  • SiO 2 has a very large TCC. Therefore, by containing TiO 2 of 1% by weight or more and 10% by weight or less as the aggregate, the temperature dependence of the relative permittivity can be controlled to about 60 ppm / K. If the content of TiO 2 as an aggregate is less than 1% by weight and exceeds 10% by weight, the TCC cannot be adjusted to a desired value.
  • the glass ceramics of the present invention contain 3% by weight or less of ZrO 2 as an aggregate. Dielectric loss can be reduced by containing 3% by weight or less of ZrO 2 as an aggregate with respect to the weight of the glass ceramics. If ZrO 2 as an aggregate is contained in an amount of more than 3% by weight, the relative permittivity becomes too large.
  • the content of ZrO 2 as an aggregate with respect to the weight of the glass ceramics is 0% by weight or more, preferably 0.1% by weight or more, and more preferably 1% by weight or more.
  • the glass ceramics of the present invention contain 1% by weight or less of ZnO as an aggregate. Sinterability can be improved by containing 1% by weight or less of ZnO as an aggregate with respect to the weight of the glass ceramics. In addition, the volatile component of ZnO in the glass can be supplemented. If ZnO as an aggregate is contained in an amount of more than 1% by weight, the moisture resistance is lowered.
  • the content of ZnO as an aggregate with respect to the weight of the glass ceramics is 0% by weight or more, preferably 0.1% by weight or more.
  • the glass and the glass can be obtained by a method of analyzing an electron diffraction pattern with a scanning electron microscope (SEM) or a transmission electron microscope (TEM), or a method of eluting the glass portion with hydrogen fluoride or the like. Aggregates can be distinguished or separated. By performing elemental analysis such as wavelength dispersive X-ray analysis (WDX), energy dispersive X-ray analysis (EDX), and inductively coupled plasma emission spectroscopy (ICP) on the distinguished or separated glass and aggregate. , Glass and aggregate composition can be measured respectively. By the above method, the content of SiO 2 as glass and the content of SiO 2 as an aggregate can be measured, respectively. The same applies to other elements.
  • SEM scanning electron microscope
  • TEM transmission electron microscope
  • ICP inductively coupled plasma emission spectroscopy
  • Another embodiment of the glass ceramic of the present invention is a glass ceramic containing Si, B, Al, Zn, Ti and Zr, and has a SiO 2 content of 41.70% by weight or more and 67.48% by weight or less.
  • the B 2 O 3 content is 8.74% by weight or more and 19.50% by weight or less
  • the Al 2 O 3 content is 4.875% by weight or more and 21.125% by weight or less.
  • ZnO content is 5.175% by weight or more and 21.425% by weight or less
  • TiO 2 content is 1% by weight or more and 13.5% by weight or less
  • ZrO 2 content is 6.8. It is characterized in that it is not more than% by weight, the content of SnO 2 is 3.95% by weight or less, and the content of SrO is 3.95% by weight or less.
  • the content of Si, B, Al, Zn, Ti, Zr, Sn and Sr is determined without distinguishing between the glass and the aggregate in one embodiment of the glass ceramic.
  • another embodiment of the glass ceramics of the present invention is substantially the same as one embodiment of the glass ceramics of the present invention, and has the same effect.
  • the laminated ceramic electronic component of the present invention is characterized by comprising a plurality of glass ceramic layers which are sintered bodies of the glass ceramic of the present invention.
  • the laminated ceramic electronic component of the present invention is, for example, a laminated body having a plurality of glass ceramic layers which is a sintered body of the glass ceramic of the present invention, a laminated ceramic substrate using the laminated body, and mounted on the ceramic substrate. Examples include chip parts and electronic parts provided with ceramics. Since the laminated ceramic electronic component of the present invention includes a plurality of glass ceramic layers which are sintered bodies of the glass ceramic of the present invention, it has a low dielectric constant and a low dielectric loss.
  • the laminate provided with a plurality of glass-ceramic layers which is a sintered body of the glass ceramic of the present invention, can be used, for example, for a communication ceramic multilayer substrate or a laminated dielectric filter.
  • the coefficient of thermal expansion of the glass-ceramic layer is preferably 6 ppm / K or more.
  • the relative permittivity of the glass-ceramic layer is preferably 6 or less.
  • the Q value of the glass-ceramic layer is preferably 500 or more.
  • the temperature characteristic (TCC) of the relative permittivity of the glass-ceramic layer is preferably -100 ppm / K or more and +100 ppm / K or less.
  • FIG. 1 is a cross-sectional view schematically showing an example of the laminated ceramic electronic component of the present invention.
  • the electronic component 2 includes a laminated body 1 in which a plurality of glass-ceramic layers 3 (five layers in FIG. 1) are laminated, and chip components 13 and 14 mounted on the laminated body 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 electron including 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).
  • the component 2 is a laminated ceramic electronic component of the present invention.
  • the composition of the plurality of glass-ceramic layers 3 may be the same as each other or different from each other, but it is preferable that they are the same as each other.
  • the laminated body 1 may further have a conductor layer.
  • the conductor layer for example, constitutes a passive element such as a capacitor or an inductor, or constitutes a connection wiring that bears an electrical connection between the elements.
  • Such a conductor layer includes conductor layers 9, 10, 11 and a 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 laminated body 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 laminated body 1.
  • the conductor layer 11 is arranged on the other main surface of the laminated body 1.
  • the via hole conductor layer 12 is arranged so as to penetrate the glass-ceramic layer 3, and can electrically connect the conductor layers 9 of different layers to each other, electrically connect the conductor layers 9 and 10, and conduct conductors. It plays a role of electrically connecting the layers 9 and 11.
  • the laminated body 1 is manufactured as follows, for example.
  • the glass is prepared by mixing the sub-ingredients added as needed.
  • the glass ceramics of the present invention are prepared by mixing glass with SiO 2 , TiO 2 , ZrO 2 and ZnO as aggregates.
  • (C) Preparation of green sheet The glass ceramic of the present invention is mixed with a binder, a plasticizer, etc. to prepare a ceramic slurry. Then, the ceramic slurry is molded on a base film (for example, a polyethylene terephthalate (PET) film) and then dried to produce a green sheet.
  • a base film for example, a 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.
  • the laminated green sheet 21 may be formed with a conductor layer including conductor layers 9, 10, 11 and a via hole conductor layer 12.
  • the conductor layer can be formed by a screen printing method, a photolithography method, or the like using a conductive paste containing Ag or Cu.
  • the firing temperature of the laminated green sheet 21 is not particularly limited as long as the glass ceramics of the present invention constituting the green sheet 22 can be sintered, and may be, for example, 1000 ° C. or lower.
  • the firing atmosphere of the laminated green sheet 21 is not particularly limited, but when a material that is difficult to oxidize such as Ag is used as the conductor layers 9, 10, 11 and the via hole conductor layer 12, an air atmosphere is preferable, and Cu or the like is preferable. When a material that easily oxidizes is used, a low oxygen atmosphere such as a nitrogen atmosphere is preferable. Further, the firing atmosphere of the laminated green sheet 21 may be a reducing atmosphere.
  • the laminated green sheet 21 may be fired while being sandwiched between the restraining green sheets.
  • the restraining green sheet contains, as a main component, an inorganic material (for example, Al 2 O 3 ) that is substantially not sintered at the sintering temperature of the glass ceramics of the present invention constituting the green sheet 22. Therefore, the restraining green sheet does not shrink during firing of the laminated green sheet 21, 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 laminated body 1 (particularly, the conductor layers 9, 10, 11 and the via hole conductor layer 12) is improved.
  • Chip parts 13 and 14 may be mounted on the laminated body 1 in a state of being electrically connected to the conductor layer 10. As a result, the electronic component 2 having the laminated body 1 is configured.
  • Examples of the chip components 13 and 14 include LC filters, capacitors, inductors, and the like.
  • the electronic component 2 may be mounted on a mounting board (for example, a motherboard) so as to be electrically connected via the conductor layer 11.
  • a mounting board for example, a motherboard
  • the "central particle size” means the central particle size D 50 measured by the laser diffraction / scattering method.
  • the glasses G6 to G9, G12, G13, G19, G21, G23, and G25 marked with * in Table 1 are not the glasses constituting the glass ceramics of the present invention.
  • the SiO 2 content of the glass G6 exceeds 55% by weight.
  • Glass G7 is, B 2 O 3 content exceeds 30% by weight.
  • Glass G9 is, B 2 O 3 content is less than 15 wt%.
  • Glass G12 is the weight ratio of Al 2 O 3 with respect to ZnO (Al 2 O 3 / ZnO ) is less than 0.8.
  • Glass G13 is the weight ratio of Al 2 O 3 with respect to ZnO (Al 2 O 3 / ZnO ) is greater than 1.3.
  • Glass G19 has a TiO 2 content of more than 5% by weight.
  • Glass G21 is, ZrO 2 content exceeds 5 wt%.
  • the glass G23 has a SnO 2 content of more than 5% by weight.
  • the glass G25 has an SrO content of more than 5% by weight.
  • the laminated green sheet was calcined at 980 ° C. for 60 minutes in a reducing atmosphere, and the obtained fired body was a laminated body L1 to have a plurality of glass ceramic layers which are sintered bodies of glass ceramics. It is L38.
  • the laminated bodies L6, L7, L8, L9, L12, L13, L22, L23, L25, L27, L28, L30, L32, L34, L36, and L38 marked with * in Table 2 are the glass ceramics of the present invention. It is not a laminated body using.
  • Network analyzer Keysight 8757D
  • Signal generator Keysight Synthesized Sweeper 83751
  • Resonator Self-made jig (resonance frequency: 6GHz) Prior to the measurement, the cable loss was measured by connecting the network analyzer and the signal generator. The resonator was calibrated using a standard substrate (quartz, dielectric constant: 3.73, Q value: 4545 @ 6 GHz, thickness: 0.636 mm).
  • the laminate provided with the glass-ceramic layer which is the sintered body of the glass-ceramic of the present invention, has a low relative permittivity even though it uses glass having a boron content of 30 wt% or less. It can be seen that the Q value is high, the temperature dependence of the relative permittivity is small, and the coefficient of thermal expansion is large. In addition, there were no problems associated with elution or volatilization of boron.
  • the laminated body L6 was insufficiently sintered. It is considered that this is because the glass G6 having a SiO 2 content of more than 55% by weight was used, so that the sintering did not proceed sufficiently at 980 ° C.
  • the laminated body L7 had insufficient moisture resistance. This is because the content of B 2 O 3 is a glass G7 exceeding 30 wt% is believed that such as boron elution or volatilization occurs in the manufacturing process.
  • the laminated body L8 had insufficient moisture resistance.
  • the laminated body L13 had a low Q value. This is because the weight ratio of Al 2 O 3 with respect to ZnO (Al 2 O 3 / ZnO ) is a glass G13 exceeding 1.3, the viscosity of the glass ends up increasing, to obtain a dense sintered body It is probable that it was not possible.
  • the laminate L22 was insufficiently sintered. It is considered that this is because the content of SiO 2 as an aggregate exceeds 50% by weight.
  • the laminated body L23 had a low coefficient of thermal expansion ⁇ .
  • the laminated body L25 had a high relative permittivity. It is considered that this is because the content of ZrO 2 as an aggregate exceeds 3% by weight.
  • the laminated body L27 does not have sufficient moisture resistance. It is considered that this is because the content of ZnO as an aggregate exceeds 1% by weight.
  • the TCC of the laminated body L28 is too small. It is considered that this is because the content of TiO 2 , which is a negative material for TCC, as an aggregate was too high.
  • the TCC of the laminated body L30 is too large.
  • TCC does not contain TiO 2 , which is a negative material, as an aggregate, so that TCC becomes too large.
  • the laminated body L32 had a high relative permittivity. It is considered that this is because the content of TiO 2 in the glass exceeds 5% by weight.
  • the laminated body L34 had a high relative permittivity. It is considered that this is because the content of ZrO 2 in the glass exceeds 5% by weight.
  • the laminated body L36 had a low Q value. It is considered that this is because the content of SnO 2 in the glass exceeded 5% by weight.
  • the laminated body L38 had a low Q value. It is considered that this is because the content of SrO in the glass exceeded 5% by weight.

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WO2014038230A1 (ja) * 2012-09-10 2014-03-13 日本碍子株式会社 ガラス－セラミックス複合材料
JP2016128361A (ja) * 2013-03-26 2016-07-14 日本碍子株式会社 ガラス−セラミックス複合材料

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WO2025028148A1 (ja) * 2023-07-28 2025-02-06 株式会社村田製作所 低温焼成セラミック及び電子部品

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