EP2332205A1 - Cellule électrochimique haute température et dispositif de cellules électrochimiques correspondant - Google Patents

Cellule électrochimique haute température et dispositif de cellules électrochimiques correspondant

Info

Publication number
EP2332205A1
EP2332205A1 EP09783263A EP09783263A EP2332205A1 EP 2332205 A1 EP2332205 A1 EP 2332205A1 EP 09783263 A EP09783263 A EP 09783263A EP 09783263 A EP09783263 A EP 09783263A EP 2332205 A1 EP2332205 A1 EP 2332205A1
Authority
EP
European Patent Office
Prior art keywords
fuel cell
copper
ods
cell according
anode
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Withdrawn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
EP09783263A
Other languages
German (de)
English (en)
Inventor
Horst Greiner
Alessandro Zampieri
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.)
Siemens AG
Original Assignee
Siemens AG
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 Siemens AG filed Critical Siemens AG
Publication of EP2332205A1 publication Critical patent/EP2332205A1/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • 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
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/04—Making non-ferrous alloys by powder metallurgy
    • C22C1/0425—Copper-based alloys
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/04—Making non-ferrous alloys by powder metallurgy
    • C22C1/05—Mixtures of metal powder with non-metallic powder
    • C22C1/051—Making hard metals based on borides, carbides, nitrides, oxides or silicides; Preparation of the powder mixture used as the starting material therefor
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/10—Alloys containing non-metals
    • C22C1/1084—Alloys containing non-metals by mechanical alloying (blending, milling)
    • 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
    • H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
    • H01M4/8882—Heat treatment, e.g. drying, baking
    • H01M4/8885—Sintering or firing
    • 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
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • H01M4/9025—Oxides specially used in fuel cell operating at high temperature, e.g. SOFC
    • H01M4/9033—Complex oxides, optionally doped, of the type M1MeO3, M1 being an alkaline earth metal or a rare earth, Me being a metal, e.g. perovskites
    • 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
    • H01M4/9066—Metals or alloys specially used in fuel cell operating at high temperature, e.g. SOFC of metal-ceramic composites or mixtures, e.g. cermets
    • 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
    • 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
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
    • H01M8/2425—High-temperature cells with solid electrolytes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F2998/00—Supplementary information concerning processes or compositions relating to powder metallurgy
    • 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
    • H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
    • H01M2004/8684—Negative electrodes
    • 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
    • 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
    • H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
    • 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
    • H01M8/0215—Glass; Ceramic materials
    • 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

Definitions

  • the invention relates to a high-temperature fuel cell (SOFC) according to the preamble of claim 1.
  • SOFC high-temperature fuel cell
  • the invention also relates to an associated, constructed of such fuel cells Brennstoffzellen- anläge.
  • the invention relates to the use of copper in the anodes in the individual fuel cells and as cell connectors in the entire fuel cell system.
  • SOFC S_olid Oxide Fuel Cell
  • Copper also has the tendency to react with nickel even at relatively low temperatures and in particular to form alloys (see state diagram copper-nickel, Hansen / Anderko "Constitution of Binary Alloys" (McGraw-Hill 1958), page 602) when using copper in a In a SOFC generator, all nickel components are always exchanged for copper.
  • the anode In particular in the event that copper-based materials are used to reduce the operating temperature in fuel cells, the anode must also be set to copper. This applies to the SOFCs of different designs, in particular the tubular, HPD or ⁇ cells.
  • cell-to-cell connector materials such as pastes or tapes for their realization
  • cell-to-cell connector materials are also copper-based.
  • the copper-based pastes or slips used to make them, as well as tapes, must be conductive, porous and stable at the operating temperature of the generator, and for comparatively long periods of operation.
  • the contact pastes or the anodes in the corresponding time will be more dense and that the porosity of the materials decreases when copper grains sinter together in the slurry and form larger agglomerates, in a relatively short time even at relatively low temperatures (600 0 C - 700 0 C).
  • relatively low temperatures 600 0 C - 700 0 C.
  • the invention relates to the selection of such copper-based materials for the individual fuel cells - both for the anode and for the materials for connection to the contacts - in which a mechanical alloy of so-called.
  • ODS copper powders with fine oxidic powders i. as dispersion alloy is present (ODS: Oxide-p_ispersion-S_trengthened).
  • the ODS Cu / metal oxide material is produced by mechanical alloying of the different powders.
  • the invention are advantageously such new copper-ferbas elected materials for fuel cells such as the anode layer and anode contact paste is proposed, which advantageously at lower temperatures, particularly in the range 400-700 0 C, or even at moderate operating temperatures, particularly in the range 700-950 0 C, whereby the materials find use for the anodes as well as for all other compounds.
  • the invention proposes the use of copper particles with the finest distributions of certain metal oxides by mechanical alloying.
  • the distribution of metal oxide particles allows a better thermal stability of the copper particles, as confirmed by experimental studies, and leads to a longer life and a slower rate of degradation of the contact slip.
  • the invention is based on the finding that excessive sintering between copper particles, in particular in the anode and contact paste, is avoided and that subsequent compression of the contact pastes in the individual bundles of the fuel cells and thus in the entire generator can be excluded. This should improve the performance, i. the long-term stability of the new fuel cells can be increased.
  • the already mentioned ODS copper / metal oxide powder ie, for example, Cu / doped Zr ⁇ 2 - such.
  • Cu / YSZ or Cu / ScSZ - or Cu / doped Ce0 2 - such as Cu / GDC or Cu / SDC - can be used.
  • Cu / metal oxide combinations with different dispersion material content and grain size can be used.
  • the oxide dispersion should be present with a good distribution in the submicrometer range, for example also in the nano range.
  • All metal oxides are replaceable, but especially the oxides of the electrolyte material in order to avoid possible reactions between the various elements in the long-term operation of the fuel cell system.
  • the dispersion energetically blocks the movement of copper to minimize the specific surface area.
  • the anode layers could be removed with the aid of wet coating methods, eg. As roller coating, screen printing, wet-powder spraying, and be prepared with additional sintering processes.
  • the anode paste or solution / suspension consists of ODS copper powder, electrolyte material, water, binder, plasticizer, and possibly a porous material, eg. As graphite or polymer materials.
  • the contact paste (possibly it could be in the adhesive tape form) consists of the ODS copper powder, water, binder or adhesive materials, such as polyvinyl acetate (PVA) and possibly a plasticizer to control the viscosity, are mixed. Other additives are possible.
  • PVA polyvinyl acetate
  • FIG. 1 shows a micrograph of pure copper powder
  • FIG. 2 shows a micrograph of sintered Cu / SCZ material
  • FIG. 3 shows schematically copper particles with mechanically added metal oxides in extremely fine distribution.
  • Such functional layers with ODS powders can be carried out by applying appropriate materials, for example by spraying liquids, by mechanical application or by preparation via belts.
  • appropriate materials for example by spraying liquids, by mechanical application or by preparation via belts.
  • copper powder can be mixed together with copper / metal oxides already produced by mechanical alloying.
  • the copper particles are denoted by 1, as obtained in a bed of copper powder. It can be seen that pores 2 are present.
  • FIG. 2 shows a composite of Cu / SCSZ 10 mol% after a thermal treatment at 1000 ° for 125 h. It can be seen clearly that the pure copper powder has sintered together to form larger areas 10 and, according to FIG. 1, forms extended agglomerates, while the Cu / ScSZ powder is characterized by a few contact compounds among the particles 10. These contact connections provide electrical conductivity to form a network in the anode that allows electronic conductivity. Ansons- The individual particles appear as discrete regions and substantially unchanged from FIG.
  • FIG. 3 shows a particle 110 which was produced by mechanical alloying.
  • the distribution of substantially smaller metal oxide particles 111 occurs in the larger particle 110 of copper matrix.
  • the metal oxide particles 111 have a diameter of 100 nm, and the matrix particles may have an extension of 1 mm or more. In accordance with FIG. 2, this results in a statistical distribution of the metal oxide particles 111 in the matrix 110.
  • the hybrid particles of copper with mechanically alloyed ODS copper / oxide particles described with reference to FIGS. 1 to 3 are used to build up the anodes of SOFC fuel cells. Furthermore, the material for the contacts can be produced on this basis. This solves the problem that it can lead to copper precipitation during long-term operation of the new fuel cell. As mentioned above, it can be assumed that mechanical alloying for improving material structures is known per se. In connection with high-temperature fuel cells and the
  • the ODS dispersion of metal oxide in metal cores are suitable for the replacement of the previous nickel-based anode in high-temperature fuel cells, if in the fuel cell system, the operating temperature is lowered.
  • the corresponding compounds in pasty or liquid consistency for contacting the individual parts of the fuel cell system may also have corresponding copper / copper oxide-based ODS materials.
  • the use of pastes with copper / metal oxide distributions allows for improved thermal stability and increased lifetime of the SOFC and the individual fuel cells or the fuel cell belt. This results in a considerable cost reduction of the known SOFC generators, which is of highest relevance in practice.
  • the materials described are used in fuel cell, wherein the anode has a thickness of about 1 to 100 microns.
  • the ODS copper powder-based layer as
  • the anode may be infiltrated with additional precursor suspensions - eg, CeO 2 , Co, Ni -, for example, by wet chemical or CVD methods to increase electrochemical activity.
  • the metal oxide-based particles have an order of magnitude of ⁇ 1 ⁇ m and may be in particular in the nanoscale, ie submicrometer range.
  • the ODS material may consist of Cu / ZrO 2 or Cu / doped-Zr0 2, as for example, be Cu / YSZ or Cu / ScSZ, gebil ⁇ det.
  • the ODS may also be formed of Cu / doped CeO 2, such as Cu / GDC or Cu / SDC, or Cu / GDC.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Thermal Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Ceramic Engineering (AREA)
  • Composite Materials (AREA)
  • Fuel Cell (AREA)
  • Inert Electrodes (AREA)

Abstract

L'invention concerne des cellules électrochimiques haute température fonctionnant à des températures entre 500 et 7000 °C, des matériaux à base de cuivre destinés aux composants et les compositions à base desdits matériaux. Les matériaux à base de cuivre sont des hybrides composés de poudres de cuivre et d'autres poudres oxydiques. Ces hybrides sont notamment produits par alliage mécanique. Le dispositif de cellules électrochimiques fabriqué selon l'invention présente une stabilité à long terme dans la plage de travail concernée et ne présente aucun dépôt de cuivre souvent observé sur les dispositifs habituels.
EP09783263A 2008-09-30 2009-09-22 Cellule électrochimique haute température et dispositif de cellules électrochimiques correspondant Withdrawn EP2332205A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102008049607A DE102008049607A1 (de) 2008-09-30 2008-09-30 Hochtemperatur-Brennstoffzelle und zugehörige Brennstoffzellenanlage
PCT/EP2009/062236 WO2010037665A1 (fr) 2008-09-30 2009-09-22 Cellule électrochimique haute température et dispositif de cellules électrochimiques correspondant

Publications (1)

Publication Number Publication Date
EP2332205A1 true EP2332205A1 (fr) 2011-06-15

Family

ID=41403131

Family Applications (1)

Application Number Title Priority Date Filing Date
EP09783263A Withdrawn EP2332205A1 (fr) 2008-09-30 2009-09-22 Cellule électrochimique haute température et dispositif de cellules électrochimiques correspondant

Country Status (4)

Country Link
US (1) US20110223509A1 (fr)
EP (1) EP2332205A1 (fr)
DE (1) DE102008049607A1 (fr)
WO (1) WO2010037665A1 (fr)

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102539204B (zh) * 2011-10-19 2013-09-11 深圳市金洲精工科技股份有限公司 一种pcb切片的制作方法及pcb切片
CN109175391B (zh) * 2018-10-24 2020-12-15 北京航空航天大学 一种原位合成纳米氧化物颗粒弥散强化合金的方法
US11539053B2 (en) * 2018-11-12 2022-12-27 Utility Global, Inc. Method of making copper electrode
US11453618B2 (en) * 2018-11-06 2022-09-27 Utility Global, Inc. Ceramic sintering

Family Cites Families (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5312582A (en) * 1993-02-04 1994-05-17 Institute Of Gas Technology Porous structures from solid solutions of reduced oxides
DE19630004C2 (de) * 1996-07-25 2001-11-08 Mtu Friedrichshafen Gmbh Anodenstromkollektor für eine Schmelzkarbonatbrennstoffzelle
JP3924772B2 (ja) * 2000-11-16 2007-06-06 三菱マテリアル株式会社 固体電解質型燃料電池の空気極集電体
EP1671391A2 (fr) * 2003-09-17 2006-06-21 Tiax LLC Dispositifs electrochimiques et composants de ceux-ci
US7767358B2 (en) * 2005-05-31 2010-08-03 Nextech Materials, Ltd. Supported ceramic membranes and electrochemical cells and cell stacks including the same
US20070117006A1 (en) * 2005-11-22 2007-05-24 Zhongliang Zhan Direct Fabrication of Copper Cermet for Use in Solid Oxide Fuel Cell
JP5170815B2 (ja) * 2006-07-04 2013-03-27 日産自動車株式会社 固体電解質型燃料電池ユニット及びスタック

Also Published As

Publication number Publication date
US20110223509A1 (en) 2011-09-15
WO2010037665A1 (fr) 2010-04-08
DE102008049607A1 (de) 2010-04-01

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