WO2010059159A1 - Pile à combustible à oxyde solide comportant un support métallique avec revêtement conducteur - Google Patents

Pile à combustible à oxyde solide comportant un support métallique avec revêtement conducteur Download PDF

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Publication number
WO2010059159A1
WO2010059159A1 PCT/US2008/084260 US2008084260W WO2010059159A1 WO 2010059159 A1 WO2010059159 A1 WO 2010059159A1 US 2008084260 W US2008084260 W US 2008084260W WO 2010059159 A1 WO2010059159 A1 WO 2010059159A1
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WO
WIPO (PCT)
Prior art keywords
fuel cell
noble metal
metal coating
recited
steel substrate
Prior art date
Application number
PCT/US2008/084260
Other languages
English (en)
Inventor
Mark R. Jaworowski
Jean Yamanis
Original Assignee
Utc Power Corporation
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 Utc Power Corporation filed Critical Utc Power Corporation
Priority to PCT/US2008/084260 priority Critical patent/WO2010059159A1/fr
Publication of WO2010059159A1 publication Critical patent/WO2010059159A1/fr

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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
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0206—Metals or alloys
    • H01M8/0208—Alloys
    • H01M8/021—Alloys based on iron
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8803—Supports for the deposition of the catalytic active composition
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8825—Methods for deposition of the catalytic active composition
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9041—Metals or alloys
    • H01M4/905—Metals or alloys specially used in fuel cell operating at high temperature, e.g. SOFC
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/92—Metals of platinum group
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/92—Metals of platinum group
    • H01M4/921—Alloys or mixtures with metallic elements
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/92—Metals of platinum group
    • H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
    • 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
    • H01M8/1213—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the electrode/electrolyte combination or the supporting material
    • H01M8/1226—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the electrode/electrolyte combination or the supporting material characterised by the supporting layer
    • 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
    • H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
    • 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

  • Solid oxide fuel cells are commonly known and used for generating electricity.
  • conventional solid oxide fuel cells typically include an anode, a cathode, and an electrolyte between the anode and the cathode.
  • a support structure mechanically supports the anode, the cathode, and the electrolyte.
  • the support structure may also serve to supply reactant gas to the anode and conduct electric current to an external circuit.
  • One problem associated with such support structures is that the operating environment is severely corrosive. For instance, the support structure is exposed on one side to a reactant gas oxidant (e.g., air) and on another side to a reactant gas fuel (e.g., hydrogen). This dual exposure produces environmental conditions that change the protective nature of the oxide scale on the oxidant side and can lead to rapid oxidation of common alloys that are used for the support structure, such as ferritic stainless steel. Oxidation of the support structure may diminish the mechanical strength and electrical conductivity.
  • a reactant gas oxidant e.g., air
  • a reactant gas fuel e.g., hydrogen
  • the electrode is typically a ceramic material having a nominal coefficient of thermal expansion of about l lxlO ⁇ 6 /°C, which is considerably different than most alloys.
  • Ferritic stainless steels have a nominal coefficient of thermal expansion of about l lxlO ⁇ 6 /°C and thereby mitigate thermal stresses between the electrode and the support structure due to thermal cycling.
  • alloys with better resistance to oxidation than stainless steel are known, such alloys cannot be directly substituted for the stainless steel because the thermal expansion mismatch with the ceramic material of the electrode may cause damage to the fuel cell due to thermal cycling.
  • An exemplary fuel cell apparatus includes a fuel cell having a solid oxide electrolyte between an anode and a cathode.
  • the fuel cell is disposed on a metallic support that includes a steel substrate and a noble metal coating that is disposed on the steel substrate between the fuel cell and the steel substrate.
  • An exemplary method of processing the fuel cell apparatus includes forming the noble metal coating on the steel substrate of the metallic support, forming the fuel cell on the coated metallic support such that the noble metal coating is between the fuel cell and the steel substrate, and subjecting the metallic support, the noble metal coating, and the electrode to a thermal process during the forming of the fuel cell .
  • Figure 1 illustrates an example fuel cell.
  • Figure 2 illustrates another example fuel cell having a rigidized foil support.
  • Figure 3 illustrates an example method for processing the fuel cell.
  • FIG. 1 schematically illustrates selected portions of an example fuel cell assembly 10, or apparatus.
  • the fuel cell assembly 10 includes a fuel cell unit 12 that operates in a known manner to generate electricity.
  • a fuel cell unit 12 that operates in a known manner to generate electricity.
  • multiple fuel cell units 12 may be stacked in a known manner and sandwiched between collector plates (not shown) in a series arrangement with an external circuit.
  • collector plates not shown
  • this disclosure is not limited to the arrangement of the example fuel cell assembly 10, and the concepts disclosed herein may be applied to other fuel cell arrangements.
  • the fuel cell unit 12 includes a metallic support 14 between a fuel cell 16, which may also be known as an electrode assembly, and a cathode interconnect layer 18.
  • the fuel cell 16 may be a tri-layered arrangement, including a solid oxide electrolyte 20 between a cathode 22 and an anode 24 for providing an electrochemical reaction to generate an electric current.
  • the solid oxide electrolyte 20 may be any type of solid oxide electrolyte, such as ceria (CeO 2 ) doped with rare earth metal oxide(s), gallate (e.g., strontium-doped lanthanum gallate), or stabilized (fully or partially) zirconia.
  • the cathode interconnect layer 18 may be any type of interconnect for conducting electric current and delivering reactant gas to the cathode 22.
  • the metallic support 14 includes a steel substrate 26 and a noble metal coating 28 disposed on the steel substrate 26 between the fuel cell 16 and the steel substrate 26.
  • the noble metal coating 28 may be more resistant to oxidation than the steel substrate 26.
  • the noble metal coating 28 provides a low electronic (Ohmic) resistance path through a chromia scale that may form on the steel substrate 26 during formation of the fuel cell 16.
  • the noble metal coating 28 may include nickel, platinum, palladium, silver, gold, rhodium, iridium, ruthenium, osmium, and combinations thereof.
  • the noble metal coating 28 is a nickel alloy, substantially pure nickel, a mixture of nickel and platinum, or a mixture of nickel and at least one other noble metal selected from platinum, palladium, silver, gold, rhodium, iridium, and ruthenium. In some examples, the noble metal coating 28 includes only the listed example elements and impurities that do not effect the properties of the noble metal coating 28.
  • the noble metal coating 28 provides continuous or discreet metallic electron-conductive pathways though the oxide scale that forms on the steel substrate 26.
  • the noble metal coating 28 maintains a low Ohmic resistance when stainless steel or ferritic stainless steel is used as the steel substrate 26.
  • the steel substrate 26 of the fuel cell assembly 10 may be any type of structure for mechanically supporting the fuel cell 16 and delivering reactant gas to the anode 24, such as a rigidized support or other type of structure.
  • the steel substrate 26 may be comprised of a stainless steel composition, such as CROFER® 22 APU.
  • a stainless steel composition such as CROFER® 22 APU.
  • Such a composition may include about 20-24 wt% chromium, about 0.3-0.8 wt% manganese, about 0.03-0.2 wt% titanium, about 0.04-0.2 wt% lanthanum, and a balance of iron.
  • the stainless steel may have other compositions.
  • the term "about” as used in this description relative to compositions or other values refers to possible variation in the given value, such as normally accepted variations or tolerances.
  • the noble metal coating 28 is relatively thin in comparison to the steel substrate 26 to reduce the influence on the thermal expansion/contraction of the metallic support 14.
  • the thickness of the noble metal coating 28 is such that the thermal expansion/contraction of the steel substrate 26 controls the thermal expansion/contraction of the noble metal coating 28.
  • the thermal expansion/contraction of the overall metallic support 14 is approximately equivalent to the thermal expansion/contraction of the steel substrate 26, even though the metallic support 14 is a composite of the noble metal coating 28 and the steel substrate 26.
  • the metallic support 14 provides the benefit of being highly corrosion resistant (from the noble metal coating 28) while maintaining a nominal coefficient of thermal expansion that is approximately equal to the nominal coefficient of thermal expansion of the fuel cell 16 (from the steel substrate 26).
  • the thickness of the noble metal coating 28 is less than about 10 micrometers (about 393 microinches). In another example the thickness may be less than about 5 micrometers (about 197 microinches) to achieve the thermal expansion/contraction match between the metallic support 14 and the fuel cell 16.
  • FIG. 2 illustrates an example fuel cell assembly 100 that is somewhat similar to the example fuel cell assembly 10 of the previous example.
  • like reference numerals designate like elements where appropriate, and reference numerals with the addition of one-hundred or multiples thereof designate modified elements.
  • the modified elements are understood to incorporate the same features and benefits of the corresponding original elements.
  • the fuel cell assembly 100 includes a stack of fuel cell units 112 that operate in a known manner to generate electricity.
  • Each of the fuel cell units 112 includes a metallic support 114 (e.g. a rigidized foil support) between the fuel cell 16 and a cathode interconnect layer 118.
  • the cathode interconnect 118 includes channels 118a, such as channels formed from a corrugated sheet of expanded metal.
  • the cathode interconnect 118 may be a porous structure, such as a woven filament structure.
  • the cathode interconnect 118 may be bonded to the fuel cell 16 and to the metallic support 114, such as by diffusion bonding, welding, or brazing.
  • the cathode interconnect 118 may be fabricated from a suitable alloy, such as stainless steel or a nickel alloy.
  • the metallic support 114 includes a steel substrate 126 and a noble metal coating 128 on the steel substrate 126 (e.g., on the surfaces).
  • the noble metal coating 128 may be formed only the side of the metallic support adjacent the fuel cell 16 or, alternatively, be applied to substantially all of the exposed surfaces of the metallic support 114.
  • the noble metal coating 128 may be of similar thickness as described above such that the metallic support 114 provides the benefit of being highly corrosion resistant (from the noble metal coating 128) while maintaining a nominal coefficient of thermal expansion that is approximately equal to the nominal coefficient of thermal expansion of the fuel cell 16 (from the steel substrate 126), as described above.
  • the steel substrate 126 includes a separator sheet 136, a perforated support sheet 138 adjacent to the fuel cell 16, and a porous layer 140 located between the separator sheet 136 and the perforated support sheet 138.
  • the porous layer 140 provides an electrical connection between the separator sheet 136 and the perforated support sheet 138.
  • the separator sheet 136, the perforated support sheet 138, and the porous layer 140 may be bonded together using diffusion welding, welding, brazing, or any other suitable process.
  • the noble metal coating 128 may be applied onto the perforated support sheet 138 of the steel substrate 126 either before or after the bonding.
  • the perforated support sheet 138 may be a thin sheet, such as a foil.
  • the perforated support sheet 138 is not limited to any particular thickness, but in a few examples, the thickness may be 5-100 micrometers (197-3937 microinches). In a further example, the thickness may be approximately 15-50 micrometers (591-1969 microinches).
  • the perforated support sheet 138 may be fabricated using any suitable method, including laser drilling, electron beam drilling, chemical etching, or micromachining. In another example, the perforated support sheet 138 may be fabricated as disclosed in United States Application
  • the separator sheet 136 is of similar thickness as the perforated support sheet 138, but is solid and continuous rather than perforated.
  • the porous layer 140 includes first filaments 142a generally arranged transversely relative to second filaments 142b.
  • the first filaments 142a and the second filaments 142b are woven metal wires, such as a square-woven mesh.
  • the gaps between the first filaments 142a and the second filaments 142b provide open space for the flow of the reactant gas through the porous layer 140 to the anode 24.
  • FIG. 3 illustrates an example method 200 for processing the fuel cell assembly 10 or 100 of the previous examples, including steps 202, 204 and 206.
  • Step 202 includes forming the noble metal coating 28 or 128 on the steel substrate 26 or 126 of the metallic support 14 or 114.
  • any suitable type of deposition process may be used to form the noble metal coating 28 or 128, such as sintering, spraying, electroplating, or electrophoresis.
  • a noble metal powder may be deposited onto the steel substrate 26 or 126 and subsequently sintered to form the noble metal coating 28 or 128.
  • the composition of the noble metal powder corresponds to the desire composition of the noble metal coating 28.
  • the noble metal powder used to form the noble metal coating 28 or 128 has an average particle size of about 1-10 micrometers (about 39.4-394 microinches). Using a relatively coarse particle size of about 1-10 micrometers facilitates a reduction in alloying between the noble metal and the underlying steel that may otherwise form undesired intermetallic phases.
  • the sintering of the noble metal coating 28 or 128 may be conducted under a reducing atmosphere, such as a nitrogen or hydrogen atmosphere, to facilitate avoidance of oxidation of the noble metal and avoidance of formation of an oxide scale on the steel substrate 26 or 126.
  • a reducing atmosphere such as a nitrogen or hydrogen atmosphere
  • Step 204 may be used to form the fuel cell 16 onto the metallic support 14 or 114.
  • the cathode 22, the anode 24, and the solid oxide electrolyte 20 may be comprised of ceramic materials that may be formed using suitable ceramic processing techniques known in the art.
  • the cathode 22, the anode 24, and the solid oxide electrolyte 20 may be deposited using slip casting, tape casting, screen printing, electrophoretic deposition, or spin coating and then subsequently sinter under elevated temperatures.
  • the fuel cell 16 may also be deposited using other methods, including thermal plasma spraying, electron beam physical vapor deposition, sputtering, or chemical vapor deposition.
  • Step 206 includes subjecting the metallic support 14 or 114, the noble metal coating 28 or 128, and the fuel cell 16 to a thermal process.
  • the thermal process may be a heating step to sinter the ceramic materials of the fuel cell 16, heat that results from the selected forming technique of the fuel cell 16 (e.g., thermal plasma spraying), or both.
  • the thermal process may involve heating the metallic support 14 or 114, the noble metal coating 28 or 128, and the fuel cell 16 at a prescribed temperature for a prescribed amount of time to densify the ceramic materials.
  • step 206 may be conducted under a controlled atmosphere having a relatively high oxygen partial pressure, such as an oxygen partial pressure that is greater than ambient (about 160 torr or 312 millibar).
  • the controlled atmosphere may also include inert carrier gases.
  • the oxygen partial pressure may be ten to fifteen times the ambient oxygen partial pressure. Using a relatively high oxygen partial pressure provides the benefit of facilitating avoidance of chemical reduction of the solid oxide material of the fuel cell 16.
  • the noble metal coating 28 or 128 protects the underlying steel substrate 26 or 126 from forming such an oxide scale during step 206 to thereby facilitate maintaining mechanical integrity and electrical conductivity of the metallic support 14.
  • the noble metal material of the noble metal coating 28 or 128 is generally unharmed by the oxygen and does not form an oxide scale.
  • the noble metal coating 28 or 128 may form a dendritic or filament type of structure that perpendicularly extends into the surface of the steel substrate 26 to facilitate maintaining a good electrical path between the fuel cell 16 and the metallic support 14 or 114.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Fuel Cell (AREA)

Abstract

L'invention concerne un appareil de pile à combustible comprenant une électrode comportant un électrolyte à oxyde solide entre une anode et une cathode. L'électrode est disposée sur un support métallique qui comprend un substrat d'acier et un revêtement de métal noble qui est disposé sur le substrat d'acier entre l'électrode et le substrat d'acier.
PCT/US2008/084260 2008-11-21 2008-11-21 Pile à combustible à oxyde solide comportant un support métallique avec revêtement conducteur WO2010059159A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
PCT/US2008/084260 WO2010059159A1 (fr) 2008-11-21 2008-11-21 Pile à combustible à oxyde solide comportant un support métallique avec revêtement conducteur

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
PCT/US2008/084260 WO2010059159A1 (fr) 2008-11-21 2008-11-21 Pile à combustible à oxyde solide comportant un support métallique avec revêtement conducteur

Publications (1)

Publication Number Publication Date
WO2010059159A1 true WO2010059159A1 (fr) 2010-05-27

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Application Number Title Priority Date Filing Date
PCT/US2008/084260 WO2010059159A1 (fr) 2008-11-21 2008-11-21 Pile à combustible à oxyde solide comportant un support métallique avec revêtement conducteur

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6794075B2 (en) * 2000-10-25 2004-09-21 Ceres Power Limited Fuel cells
US7338729B2 (en) * 2003-07-24 2008-03-04 Nissan Motor Co., Ltd. Fuel cell collector structure and solid oxide fuel cell stack using the same
US7422815B2 (en) * 2000-04-19 2008-09-09 Toyota Jidosha Kabushiki Kaisha Fuel cell separator, manufacturing method thereof and fuel cell

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7422815B2 (en) * 2000-04-19 2008-09-09 Toyota Jidosha Kabushiki Kaisha Fuel cell separator, manufacturing method thereof and fuel cell
US6794075B2 (en) * 2000-10-25 2004-09-21 Ceres Power Limited Fuel cells
US7338729B2 (en) * 2003-07-24 2008-03-04 Nissan Motor Co., Ltd. Fuel cell collector structure and solid oxide fuel cell stack using the same

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