EP1578700A2 - Materiau vitroceramique et son procede de fabrication - Google Patents

Materiau vitroceramique et son procede de fabrication

Info

Publication number
EP1578700A2
EP1578700A2 EP03800164A EP03800164A EP1578700A2 EP 1578700 A2 EP1578700 A2 EP 1578700A2 EP 03800164 A EP03800164 A EP 03800164A EP 03800164 A EP03800164 A EP 03800164A EP 1578700 A2 EP1578700 A2 EP 1578700A2
Authority
EP
European Patent Office
Prior art keywords
joint
solid
mol
component
recited
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP03800164A
Other languages
German (de)
English (en)
Inventor
Dong-Sang Kim
Kerry D. Meinhardt
Bradley R. Johnson
Michael J. Schweiger
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Battelle Memorial Institute Inc
Original Assignee
Battelle Memorial Institute Inc
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Battelle Memorial Institute Inc filed Critical Battelle Memorial Institute Inc
Publication of EP1578700A2 publication Critical patent/EP1578700A2/fr
Withdrawn legal-status Critical Current

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    • 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
    • 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
    • C03C27/00—Joining pieces of glass to pieces of other inorganic material; Joining glass to glass other than by fusing
    • 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
    • C03C8/00—Enamels; Glazes; Fusion seal compositions being frit compositions having non-frit additions
    • C03C8/24—Fusion seal compositions being frit compositions having non-frit additions, i.e. for use as seals between dissimilar materials, e.g. glass and metal; Glass solders
    • C—CHEMISTRY; METALLURGY
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    • C04B37/00—Joining burned ceramic articles with other burned ceramic articles or other articles by heating
    • C04B37/003—Joining burned ceramic articles with other burned ceramic articles or other articles by heating by means of an interlayer consisting of a combination of materials selected from glass, or ceramic material with metals, metal oxides or metal salts
    • C04B37/005—Joining burned ceramic articles with other burned ceramic articles or other articles by heating by means of an interlayer consisting of a combination of materials selected from glass, or ceramic material with metals, metal oxides or metal salts consisting of glass or ceramic material
    • C—CHEMISTRY; METALLURGY
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    • C04B37/00—Joining burned ceramic articles with other burned ceramic articles or other articles by heating
    • C04B37/02—Joining burned ceramic articles with other burned ceramic articles or other articles by heating with metallic articles
    • C04B37/023—Joining burned ceramic articles with other burned ceramic articles or other articles by heating with metallic articles characterised by the interlayer used
    • C04B37/025—Joining burned ceramic articles with other burned ceramic articles or other articles by heating with metallic articles characterised by the interlayer used consisting of glass or ceramic material
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
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    • C04B37/00—Joining burned ceramic articles with other burned ceramic articles or other articles by heating
    • C04B37/04—Joining burned ceramic articles with other burned ceramic articles or other articles by heating with articles made from glass
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/028—Sealing means characterised by their material
    • H01M8/0282—Inorganic material
    • H—ELECTRICITY
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    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0286—Processes for forming seals
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    • C04B2235/3201—Alkali metal oxides or oxide-forming salts thereof
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    • C04B2235/3215—Barium oxides or oxide-forming salts thereof
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    • C04B2235/3217—Aluminum oxide or oxide forming salts thereof, e.g. bauxite, alpha-alumina
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    • C04B2235/3225—Yttrium oxide or oxide-forming salts thereof
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    • C04B2235/3227—Lanthanum oxide or oxide-forming salts thereof
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    • C04B2235/3409—Boron oxide, borates, boric acids, or oxide forming salts thereof, e.g. borax
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    • C04B2235/3418—Silicon oxide, silicic acids or oxide forming salts thereof, e.g. silica sol, fused silica, silica fume, cristobalite, quartz or flint
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    • C04B2235/36—Glass starting materials for making ceramics, e.g. silica glass
    • C04B2235/365—Borosilicate glass
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    • C04B2237/00—Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
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    • C04B2237/10—Glass interlayers, e.g. frit or flux
    • H—ELECTRICITY
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    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M2008/1293—Fuel cells with solid oxide electrolytes
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    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H01M2300/0071—Oxides
    • H01M2300/0074—Ion conductive at high temperature
    • H01M2300/0077—Ion conductive at high temperature based on zirconium oxide
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the ' present invention is a glass ceramic material and method of making, specifically for use in electrochemical devices such as fuel cells, gas sensors, oxygen or hydrogen pumps/separators, or for sealing any material with a thermal expansion coefficient similar to the seal material.
  • solid electrolyte or “solid oxide ion conducting electrolyte” are interchangable.
  • joint includes the term “seal” because, in this glass-ceramic field, the “seal” joins at least two parts. However, the “joint” may be intermittent thereby not serving as a "seal”.
  • Ceramic materials are being used more often from automobile turbochargers to experimental fuel cells.
  • solid oxide ion conducting electrolytes are useful for oxygen separation and high temperature fuel cells.
  • sealing In a planar design, a gas-tight seal must bond the components together and prevent the mixing of the gas species on both sides of the solid oxide ion conducting electrolyte.
  • a limited number of materials are suitable as a solid oxide ion conducting electrolyte.
  • the most commonly used materials are yttria stabilized zirconia (YSZ), doped ceria, doped bismuth oxide and doped lanthanum gallate.
  • the thermal expansion coefficient (TEC) of these materials can range from 10.1 x 10 " 6 to 14.3 x 10 "6 °C “1 depending on the type of dopant and concentration. Of particular interest are materials having a TEC of 12 x 10 "6 °C "1 or greater.
  • the operating temperature can also range from 700°C to 1000°C depending upon which material is chosen as the electrolyte.
  • the seal material must be tailored to match the electrolyte thermal expansion, maintain a gas tight seal at temperatures ranging from 200 °C to 1200 °C, and not have detrimental chemical interactions with the fuel cell components.
  • the seal material must also be stable at the operating temperature (800-1000°C) for extended periods of time (>9,000 hr) and be electrically insulating. For a solid oxide fuel cell, the seal must be able to survive extremely reducing environments.
  • Borosilicate glasses and glass ceramics have also been considered as potential seal materials. These glasses have been investigated by C. G ⁇ nther et al 2 and K.L. Ley et al 3 for use in solid oxide fuel cells. However, boron will react with a humidified hydrogen atmosphere to form the gaseous species B 2 (OH) 2 and B 2 (OH) 3 at the operating temperature 2 . Therefore, any high boron seal may corrode in a humidified hydrogen environment over time. Glasses with B 2 O 3 as the only glass former have showed up to a 20% weight loss in the humidified hydrogen environment and extensive interactions with fuel cell component materials both in air and wet fuel gas. 1
  • Silica-based glasses and glass-ceramics offer the most promise. They typically have a higher chemical resistance and show minimal interaction with the fuel cell component materials. 1 Unfortunately, these glasses tend to have thermal expansions below the range needed for a sealing material.
  • the present invention is a glass-ceramic compound and method of making that are useful in joining or sealing ceramic components to other ceramic components, to glass components, to metal components, or to combinations thereof (e.g., cermet components). More specifically, the present invention is useful for joining/sealing in an electrochemical cell having at least one solid electrolyte having a first and second side exposed to first and second gas species respectively. The seal is necessary for separating the first and second gas species.
  • the glass-ceramic compound contains at least four metal oxides, M1-M2- M3-M4.
  • M1 is BaO, SrO, CaO, MgO, or combinations thereof.
  • M2 is AI 2 O 3 and is present in the compound in an amount from 2 to 15 mol%.
  • M3 is SiO 2 with up to 50 mol% B 2 O 3 .
  • M4 is either between 0.1 - 7.5 mol% a metal oxide selected from the group of La 2 O 3 , Y2O3, Nd2O3 or combinations thereof, or between 0.1 and 7.5 mol% K 2 O.
  • the composition contain an additional 0.1 to 3 mol %CuO as a wetting agent to assist the bonding of the glass.
  • the compound substantially matches a coefficient of thermal expansion of the solid ceramic component and at least one other solid component that is either ceramic, metal, or a combination thereof, when those components are selected as having a coefficient of expansion in the crystalline phase of 12 or greater 12 x 10 "6 °C "1 as measured from 25 °C to 1000 °C.
  • a series of glass ceramics in the M1- AI 2 O 3 -M3-M4 system can be used to join or seal both tubular and planar ceramic solid oxide fuel cells, oxygen electrolyzers, thermal barrier coatings, as a protective coating for metal substrates used as supports for catalytic particles used for high temperature catalytic reactions, for high temperature super-alloy applications, where it is desirable to coat metal parts with a ceramic material to improve their oxidation resistance,.and in membrane reactors for the production of syngas, commodity chemicals and other products. For high temperature super-alloy applications, it is often necessary to coat metal parts with a ceramic material to improve their oxidation resistance.
  • thermal barrier coatings are used in the areospace industry for coating turbine blades and other components.
  • multi-layered coatings are used to address issues of oxygen diffusion as well as thermal expansion mis-match.
  • the present invention is well suited for this application.
  • High temperature catalytic reactions also require the use of protective coatings for metal surfaces.
  • Thin metal substrates are often used as supports for catalytic particles, however at elevated temperatures and pressures, they oxidize and crumble.
  • a protective oxide coating applied to thin metal foils could be used to prolong their life, and could be cheaper and easier to manufacture than an all-ceramic part. These oxide surfaces then become the substrate that holds catalytic particles.
  • the present invention is well suited to be used in this manner.
  • the present invention is further well suited for sealing glass material surfaces also, such as those utilized in the lighting industry.
  • High performance, special application light bulbs require glass to metal seals in order to provide a joint between the filament and the glass bulb.
  • Some of the gasses in these light bulbs are highly corrosive, and since the bulbs get very hot, there are thermal expansion mis-match issues between the electrical contacts for the filament and the glass wall, creating a common failure site for these bulbs.
  • the present invention is well suited to solve this problem.
  • M4 is the maintaining of a substantially constant coefficient of thermal expansion from the glass to crystalline phase.
  • the present invention is a glass-ceramic compound and method of making the glass-ceramic compound.
  • the present invention is useful for joining or sealing between at least two solid ceramic parts, for example a seal in an electrochemical cell having at least one solid electrolyte having a first and second side exposed to first and second gas species respectively.
  • the present invention is also useful for joining or sealing between a solid ceramic component and a metal component or a cermet component. The seal is necessary for separating the first and second gas species during operation, usually at elevated temperatures.
  • the present invention includes a joint between a solid ceramic component and at least one other solid component that is preferably a solid ceramic component, a metal component, or a combination thereof such as a cermet component.
  • the joint has at least four metal oxides of M1-M2-M3-M4.
  • M1 is BaO, SrO, CaO, MgO, or combinations thereof.
  • M2 is AI 2 O 3 .
  • M3 is SiO with up to 50 mol% B 2 O 3 .
  • M4 is either between 0.1 - 7.5 mol% a metal oxide selected from the group of La 2 O 3 , Y 2 O 3 , Nd 2 O 3 or combinations thereof, or between 0.1 and 7.5 mol% K 2 O.
  • the composition contain an additional 0.1 to 3 mol %CuO, which has been shown to provide good wetting, and therefore assists with bonding, while improving, or at a minimum not degrading, the TEC over time.
  • the joint substantially matches a coefficient of thermal expansion of the components comprising the joint.
  • the coefficient of thermal expansion of the joint is 12 x 10 "6 °C "1 or greater as measured from 25 °C to 1000 °C.
  • composition of the joint/seal is preferably in the range wherein M1 is present in an amount from about 20 mol% to about 55 mol%, AI 2 O 3 is present in an amount from about 2 mol% to about 15 mol%, and M3 is present in an amount from about 40 mol% to about 70 mol%.
  • M4 is either between 0.1 - 7.5 mol% a metal oxide selected from the group of La 2 O 3 , Y 2 O 3 , Nd 2 O 3 or combinations thereof, or between 0.1 and 7.5 mol% K 2 O.
  • the composition contain an additional 0.1 to 3 mol %CuO for its wetting properties.
  • substantially the same coefficient of thermal expansion is herein defined as the coefficient of thermal expansion of the seal material within about 30%, preferably within about 16%, more preferably within about 5% of the sealed material.
  • the joint may be used in an electrochemical test cell to join an oxygen ion pump and a test material.
  • the joint may be used in an oxygen generator or a fuel cell to join an oxygen ion conducting electrolyte, for example a zirconia electrolyte, and an interconnect, for example manganite, chromite, metal, and combinations thereof.
  • an oxygen ion conducting electrolyte for example a zirconia electrolyte
  • an interconnect for example manganite, chromite, metal, and combinations thereof.
  • preferred applications are those where electrical resistance is desired, such as solid oxide fuel cells.
  • preferred applications are those where electrical resistance is not critical, such as oxygen generators.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Organic Chemistry (AREA)
  • Materials Engineering (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Manufacturing & Machinery (AREA)
  • Structural Engineering (AREA)
  • Electrochemistry (AREA)
  • Sustainable Energy (AREA)
  • Sustainable Development (AREA)
  • Geochemistry & Mineralogy (AREA)
  • Inorganic Chemistry (AREA)
  • Glass Compositions (AREA)
  • Fuel Cell (AREA)
  • Ceramic Products (AREA)
  • Joining Of Glass To Other Materials (AREA)

Abstract

L'invention porte sur un matériau vitrocéramique permettant de lier un élément céramique solide à au moins un autre élément solide. Il s'agit d'un mélange du type M1-M2-M3-M4, où M1 est BaO, SrO, CaO, MgO, ou leur combinaison, M2 est Al2O3, présent à raison de 2 à 15 mole %, M3 est SiO2 avec jusqu'à 50 mole % de B203 et un oxyde métallique choisi parmi La2O3, Y2O3, Nd2O3 ou leur combinaison, ou entre 0,1 et 7,5 mole % de K2O. Dans le cas d'oxydes métalliques du groupe La2O3, Y2O3, Nd2O3 ou de leur combinaison, il est préférable d'ajouter au mélange de 0,1 à 3 mole % de CuO. Dans tous les cas, le matériau vitrocéramique en phase cristalline présente un coefficient de dilatation thermique, correspondant à celui des électrolytes solides, de 12 x 10-6 °C-1 mesuré de 25 °C à 1000 °C, et ne se dégrade pas malgré des cycles thermiques répétés. La série des vitrocéramiques du système M1-Al2O3-M3-M4 de l'invention peut servir à joindre ou étanchéifier des piles à combustible tubulaires ou planes à oxyde solide, des électrolyseurs d'oxygène ou des réacteurs à membrane de production gaz de synthèse, de produits chimiques, ou d'autres produits.
EP03800164A 2003-01-03 2003-12-23 Materiau vitroceramique et son procede de fabrication Withdrawn EP1578700A2 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
US336297 1994-11-08
US33629703A 2003-01-03 2003-01-03
PCT/US2003/041230 WO2004063110A2 (fr) 2003-01-03 2003-12-23 Materiau vitroceramique et son procede de fabrication

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EP1578700A2 true EP1578700A2 (fr) 2005-09-28

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EP (1) EP1578700A2 (fr)
JP (1) JP2006512275A (fr)
AU (1) AU2003299892A1 (fr)
CA (1) CA2512083A1 (fr)
WO (1) WO2004063110A2 (fr)

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Also Published As

Publication number Publication date
WO2004063110A3 (fr) 2004-10-21
AU2003299892A8 (en) 2004-08-10
JP2006512275A (ja) 2006-04-13
WO2004063110A2 (fr) 2004-07-29
CA2512083A1 (fr) 2004-07-29
AU2003299892A1 (en) 2004-08-10
WO2004063110B1 (fr) 2004-12-09

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