CA2594168A1 - Method of producing metal to glass, metal to metal or metal to ceramic connections - Google Patents

Method of producing metal to glass, metal to metal or metal to ceramic connections Download PDF

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Publication number
CA2594168A1
CA2594168A1 CA002594168A CA2594168A CA2594168A1 CA 2594168 A1 CA2594168 A1 CA 2594168A1 CA 002594168 A CA002594168 A CA 002594168A CA 2594168 A CA2594168 A CA 2594168A CA 2594168 A1 CA2594168 A1 CA 2594168A1
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CA
Canada
Prior art keywords
metal
grain size
glass
connections
oxide
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.)
Granted
Application number
CA002594168A
Other languages
French (fr)
Other versions
CA2594168C (en
Inventor
Karsten Agersted Nielsen
Mette Solvang
Peter Halvor Larsen
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.)
Danmarks Tekniskie Universitet
Original Assignee
Technical University Of Denmark
Karsten Agersted Nielsen
Mette Solvang
Peter Halvor Larsen
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 Technical University Of Denmark, Karsten Agersted Nielsen, Mette Solvang, Peter Halvor Larsen filed Critical Technical University Of Denmark
Publication of CA2594168A1 publication Critical patent/CA2594168A1/en
Application granted granted Critical
Publication of CA2594168C publication Critical patent/CA2594168C/en
Expired - Fee Related legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Classifications

    • 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
    • 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
    • C03C27/04—Joining glass to metal by means of an interlayer
    • C03C27/042—Joining glass to metal by means of an interlayer consisting of a combination of materials selected from glass, glass-ceramic or ceramic material with metals, metal oxides or metal salts
    • 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
    • C03C27/04—Joining glass to metal by means of an interlayer
    • 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
    • C03C29/00—Joining metals with the aid of glass
    • 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
    • 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
    • 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
    • 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
    • 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
    • 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
    • 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
    • B32B2311/00—Metals, their alloys or their compounds
    • 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
    • C04B2237/00—Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
    • C04B2237/02—Aspects relating to interlayers, e.g. used to join ceramic articles with other articles by heating
    • C04B2237/10—Glass interlayers, e.g. frit or flux
    • 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
    • C04B2237/00—Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
    • C04B2237/30—Composition of layers of ceramic laminates or of ceramic or metallic articles to be joined by heating, e.g. Si substrates
    • C04B2237/32—Ceramic
    • C04B2237/34—Oxidic
    • C04B2237/343—Alumina or aluminates
    • 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
    • C04B2237/00—Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
    • C04B2237/30—Composition of layers of ceramic laminates or of ceramic or metallic articles to be joined by heating, e.g. Si substrates
    • C04B2237/40—Metallic
    • 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
    • H01M8/10—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
    • 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

Abstract

A method of manufacturing metal to glass, metal to metal and metal to ceramic connections to be used in SOFC applications, said connections being produced as a mixture of a base glass powder and a metal oxide powder. As a result, the inherent properties of the glass used in the composite seals may be altered locally in the metal-coating interface by adding e.g. MgO in order to control the viscosity and wetting, and at the same time maintain the bulk properties such as high coefficient of thermal expansion of the basic glass towards the seal components.

Claims (16)

1. A method of manufacturing metal to glass, metal to metal, and metal to ceramic connections and which is able to engineer the boundary phases, so as to obtain a strong bond independent of the metal alloy composition and a protective oxidation scale developed during usecharacterized by said connections being produced to a desired layer thickness as a mixture of a base glass powder and a metal oxide powder, the bonding being provided at elevated temperatures under controlled conditions, wherein the metal oxide powder is selected from the group consisting of:
- 0 to10 wt% boron oxide with a grain size d50 < 2 µm;
- 0 to 10 wt% magnesium oxide with a grain size d50 < 2 µm;
- 0 to 8 wt% sodium and potassium oxides with a grain size d50 < 2 µm;
- 1 to 10 wt% manganese oxide with a grain size d50 < 1.5 µm;
- 1 to 10 wt% nickel oxide with a grain size d50 < 1.5 µm;
- 0 to 10 wt% vanadium oxide with a grain size d50 < 1.5 µm;
- 0 to 5 wt% cobalt oxide with a grain size d50 < 1.5 µm; and - 0 to 5 wt% molybdenum oxide with a grain size d50 < 1.5 µm.
- 0 to 5 wt% copper oxide with a grain size d50 < 1.5 µm.
2. The method according to claim 1, characterized by said connections produced as a base glass powder with addition of metal oxide powders in a binder system being combined with metallic surface coating on the metallic part, said coating being alloyed into the surface by heating in a controlled atmosphere prior to application of the glassy connection layer.
3. The method according to claim 1, characterized by said connections produced as a base glass powder with addition of metal oxide powders in a binder system being combined with metal oxide coatings on the metallic part, said coatings being deposited prior to application of the glassy connection layer.
4. The method according to claim 1, characterized by said connections produced as a base glass powder with additions of the metal oxide powders in a binder system and being combined with metallic surface coatings on the metallic part, which are alloyed into the surface by heating in a controlled atmosphere prior to application of a metal oxide coating on the metallic part, said coating being deposited prior to bringing together the metal and the glassy connection layer.
5. The method according to claim 1, characterized by said connections being produced by coating a composite seal part with a dispersed metal oxide suspension.
6. The method according to claim 1, characterized by said connections being produced by coating a composite seal part with a dispersed metal oxide suspension in combination with metallic surface coatings on the metal components which are alloyed into the surface by heating in a controlled atmosphere prior to bringing together the metal and the seal composite components.
7. The method according to any one of claims 1-6, characterized by the amount of glassy connection layer material per surface area being sufficient to dissolve any protective chromia scale which may develop on the metallic parts.
8. The method according to any one of claims 1-6, characterized by the base glass being selected from glasses of earth alkaline aluminosilicates at compositions resulting in eutectic crystallization behavior, or from sodium aluminosilicates at compositions within the primary crystallization field of Albite, or from magnesium aluminophosphate glasses.
9. The method according to any one of claims 1-6, characterized by metal coatings which are oxidized in situ after application and then controls the scale composition on the metallic part, said metallic part being selected from the following:
- ~Manganese, nickel, and cobalt.
10. The method according to claim 9, wherein said metallic part is selected from the following:

-~<80 µg/cm2 manganese;
- ~<90 µg/cm2 nickel, - ~<40 µg/cm2 cobalt.
11. The method according to any one of claims 1-8, characterized by using a base glass in the glass composite seal with a slow or eutectic crystallization behavior in order to maintain a compliant seal at operating temperatures higher than the glass softening temperature.
12. The method according to claim 10 or 11, characterized by adding high expansion materials said base glass in order to adapt the thermal expansion of the seal composite material to the thermal expansion of the substrate.
13. The method according to claim 12, characterized by said high expansion material being fine grained enough so as to prevent excessive micro cracking of the seal, and is coarse enough so as to prevent excessive reaction and dissolution into the glass matrix.
14. The method according to claim 12, wherein said high expansion material has a grain size of d = 10 - 200 µm.
15. Use of the metal to glass connection components obtained with the method of any of claims 1-to 14 for bonding metal to glass composite, bonding metal to ceramic components or bonding metal to metal components.
16. A method of manufacturing metal to glass, metal to metal, and metal to ceramic connections, characterized by said connections being produced with a mixture comprising a base glass powder and a metal oxide powder having a grain size of 5 µm or less.
CA2594168A 2004-12-28 2005-12-23 Method of producing metal to glass, metal to metal or metal to ceramic connections Expired - Fee Related CA2594168C (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DKPA200402011 2004-12-28
DKPA200402011 2004-12-28
PCT/EP2005/013968 WO2006069753A1 (en) 2004-12-28 2005-12-23 Method of producing metal to glass, metal to metal or metal to ceramic connections

Publications (2)

Publication Number Publication Date
CA2594168A1 true CA2594168A1 (en) 2006-07-06
CA2594168C CA2594168C (en) 2011-02-22

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Family Applications (1)

Application Number Title Priority Date Filing Date
CA2594168A Expired - Fee Related CA2594168C (en) 2004-12-28 2005-12-23 Method of producing metal to glass, metal to metal or metal to ceramic connections

Country Status (10)

Country Link
US (1) US8002166B2 (en)
EP (1) EP1844512B1 (en)
JP (2) JP5639737B2 (en)
KR (1) KR100886882B1 (en)
CN (1) CN100568598C (en)
AU (1) AU2005321530B2 (en)
CA (1) CA2594168C (en)
NO (1) NO20073274L (en)
RU (1) RU2366040C2 (en)
WO (1) WO2006069753A1 (en)

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