EP0739543A1 - Perowskitische elektroden und damit bestückte hochtemperatur-brennstoffzellen - Google Patents
Perowskitische elektroden und damit bestückte hochtemperatur-brennstoffzellenInfo
- Publication number
- EP0739543A1 EP0739543A1 EP95905046A EP95905046A EP0739543A1 EP 0739543 A1 EP0739543 A1 EP 0739543A1 EP 95905046 A EP95905046 A EP 95905046A EP 95905046 A EP95905046 A EP 95905046A EP 0739543 A1 EP0739543 A1 EP 0739543A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- perovskite
- fuel cells
- high temperature
- temperature fuel
- platinum metal
- 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- Withdrawn
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
- 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
-
- 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 an electrode
- Perovskite base with solid electrolyte contact which is particularly suitable for high-temperature fuel cells.
- Solid electrolyte fuel cells usually operate at operating temperatures of around 950 to 1000 ° C. The aim is to lower the operating temperature to approximately 800 ° C.
- ZrO2 (YsZ) stabilized with Y 2 O 3 is generally used as the solid electrolyte.
- the solid electrolyte which in the classic concept also serves as a substrate support and usually has a thickness of 100 to 150 ⁇ m, is coated on both sides with different materials as electrodes (see Fig. 1): Perovskites such as (La 1-x Sr x ) MnO 3 applied, as an anode a Ni / ZrO 2 cermet.
- the aim of the invention is therefore to reduce the chemical interactions between the perovskites serving as electrodes and the solid electrolyte and, if appropriate, to improve the electrochemical properties of the electrodes. This goal is achieved by inhibiting platinum metal doping in the perovskite adjacent to the electrolyte.
- doped electrodes additionally show improved electrochemical properties.
- the doping amounts useful here can go up to over 1%, but are expediently chosen in the range from 10 to 10 3 ppm.
- platinum metals iridium and ruthenium are preferred, which are absorbed by the perovskite in particular in oxidic form.
- the doping can vary over the total volume of the
- platinum metals with high oxide vapor pressure e.g.
- the perovskite e.g. in air or another oxygen-containing atmosphere at elevated temperatures (approx. 600 - 1000 ° C) exposed to the access of the oxide vapor for long periods.
- the desired doping can be achieved by impregnation and heat treatment or by suitable additives already during electrode manufacture.
- perovskite cathodes of high-temperature fuel cells particular attention is paid to the perovskite cathodes of high-temperature fuel cells, but a perovskite provided for the anode can also be doped with platinum metal according to the invention.
- the doping according to the invention is useful for types of perovskite and mixtures such as are provided for fuel cells, such as for example perovskite based on LaMnO 3 , LaCoO 3 , LaFeO 3 ⁇ , LaCrO 3, etc.
- Perovskites based on lanthanum ferrite were examined in particular. Y 2 O 3 -containing ZrO 2 materials are widely used as the solid electrolyte.
- the reduction in reactivity of perovskite electrodes by platinum metal doping can, of course, also be used with other oxide masses serving as solid electrolyte, such as mixed oxides based on Gd, Ce-based and doped BaCeO 3 .
- the invention is not limited to fuel cells, but can be used in all cases of boundary layer structures operated at elevated temperatures, in which material of the perovskite type and high-temperature-resistant oxide materials in particular
- perovskites e.g.
- FIG. 1 shows a diagram for an electrode / electrolyte arrangement of fuel cells
- FIG. 2 shows a graph for the SrZrO 3 formation in a powder mixture of YsZ and perovskite
- Figure 3 is an x-ray diagram for
- Figure 4 is a graph for the cell volume
- Perovskite powders of different compositions were loaded for 48 h or 121 h at 900 ° C together with iridium sheet in air via the gas phase.
- the samples pretreated in this way were mixed with the electrolyte material 8YsZ (with 8 mol% Y2O3 stabilized ZrO 2 ) in equimolar proportions, pressed into pellets and annealed or aged at 1000 ° C. for different times.
- the formation of reaction products (SrZrO 3 or CaZrO 3 ) after 25 h or 48 h exposure was determined with the aid of X-ray diffraction images.
- the results are summarized in Table 1. As can be seen, the samples doped with iridium show a much lower tendency to react with the electrolyte than that untreated samples.
- the time course of the SrZrO 3 formation is plotted in FIG. 2, which clearly shows the difference.
- a perovskite with the composition (La 0.6 Sr 0.4 ) 0.9 Fe 0.8 Co 0.2 O 3- ⁇ was chosen as the starting material, which was calcined for 48 h at 900 ° C in an oxygen atmosphere.
- two samples of the same composition were "outsourced” in the same oxygen atmosphere in the presence of iridium at 900 ° C for 48 h or 121 h.
- the nitrates of the corresponding metal components of the perovskite and Ir (III) oxide (Ir 2 O 3 ) served as starting materials. All components were homogenized in an aqueous solution, dried and then stored in air at 1200 ° C. for 48 h in order to build up the perovskite grid. With the help of a parallel iridium determination using neutron activation analysis and
- the iridium content could be determined to be about 200 ppm in both cases.
- the perovskite obtained was mixed in an equimolar ratio with YsZ, pressed into pellets and aged at 1000 ° C for 72 hours. The result is shown in Tab. 1.
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Inert Electrodes (AREA)
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE4400540A DE4400540C2 (de) | 1994-01-11 | 1994-01-11 | Perowskitische Elektroden insbesondere für Hochtemperatur-Brennstoffzellen |
DE4400540 | 1994-01-11 | ||
PCT/DE1995/000026 WO1995019053A1 (de) | 1994-01-11 | 1995-01-10 | Perowskitische elektroden und damit bestückte hochtemperatur-brennstoffzellen |
Publications (1)
Publication Number | Publication Date |
---|---|
EP0739543A1 true EP0739543A1 (de) | 1996-10-30 |
Family
ID=6507700
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP95905046A Withdrawn EP0739543A1 (de) | 1994-01-11 | 1995-01-10 | Perowskitische elektroden und damit bestückte hochtemperatur-brennstoffzellen |
Country Status (7)
Country | Link |
---|---|
US (1) | US5824429A (ja) |
EP (1) | EP0739543A1 (ja) |
JP (1) | JPH09507335A (ja) |
AU (1) | AU694471B2 (ja) |
DE (1) | DE4400540C2 (ja) |
NO (1) | NO962900L (ja) |
WO (1) | WO1995019053A1 (ja) |
Families Citing this family (17)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE19547700C2 (de) * | 1995-12-20 | 1998-09-17 | Forschungszentrum Juelich Gmbh | Elektrodensubstrat für eine Brennstoffzelle |
DE19547701C2 (de) * | 1995-12-20 | 2000-01-20 | Forschungszentrum Juelich Gmbh | Elektrode-Elektrolyt-System aus oxidischem Material |
DE19605086C1 (de) * | 1996-02-12 | 1997-06-26 | Siemens Ag | Hochtemperatur-Brennstoffzelle und aus solchen bestehender Hochtemperatur-Brennstoffzellenstapel |
JPH09238367A (ja) * | 1996-02-29 | 1997-09-09 | Matsushita Electric Ind Co Ltd | テレビジョン信号送信方法,テレビジョン信号送信装置,テレビジョン信号受信方法,テレビジョン信号受信装置,テレビジョン信号送信受信方法,テレビジョン信号送信受信装置 |
DE19640926C1 (de) * | 1996-10-04 | 1998-01-15 | Dornier Gmbh | Elektrode für eine elektrochemische Zelle, Elektroden-Elektrolyteinheit und zugehöriges Herstellungsverfahren |
ATE198519T1 (de) | 1997-09-11 | 2001-01-15 | Sulzer Hexis Ag | Elektrochemisch aktives element zu einer festoxidbrennstoffzelle |
ATE349777T1 (de) * | 1999-10-08 | 2007-01-15 | Fuelcell Energy Ltd | Kompositelektroden für festkörperelektrochemische vorrichtungen |
US6565737B2 (en) * | 2000-12-14 | 2003-05-20 | Battelle Memorial Institute | Method and apparatus for selectively removing oxygen using a non-catalytic electrode in an electrochemical cell |
WO2002056399A2 (en) * | 2001-01-12 | 2002-07-18 | Global Thermoelectric Inc. | Redox solid oxide fuel cell |
US6620535B2 (en) * | 2001-05-09 | 2003-09-16 | Delphi Technologies, Inc. | Strategies for preventing anode oxidation |
EP1289035A2 (en) * | 2001-08-29 | 2003-03-05 | Matsushita Electric Industrial Co., Ltd. | Composite electrode for reducing oxygen |
US7045244B2 (en) * | 2002-06-10 | 2006-05-16 | Hewlett-Packard Development Company, L.P. | Fuel cells utilizing non-porous nanofilm microchannel architecture |
JP4601896B2 (ja) * | 2002-10-30 | 2010-12-22 | 富士通セミコンダクター株式会社 | 半導体装置及びその製造方法 |
US7758992B2 (en) * | 2002-11-15 | 2010-07-20 | Battelle Memorial Institute | Copper-substituted perovskite compositions for solid oxide fuel cell cathodes and oxygen reduction electrodes in other electrochemical devices |
US20040214070A1 (en) * | 2003-04-28 | 2004-10-28 | Simner Steven P. | Low sintering lanthanum ferrite materials for use as solid oxide fuel cell cathodes and oxygen reduction electrodes and other electrochemical devices |
DE10351955A1 (de) * | 2003-11-07 | 2005-06-16 | Forschungszentrum Jülich GmbH | Kathodenwerkstoff für eine Hochtemperatur-Brennstoffzelle (SOFC) sowie eine daraus herstellbare Kathode |
US7157165B2 (en) * | 2003-11-18 | 2007-01-02 | Uchicago Argonne, Llc | Iron-based perovskite cathodes for solid oxide fuel cells |
Family Cites Families (16)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3671323A (en) * | 1970-01-12 | 1972-06-20 | Westinghouse Electric Corp | Hydrophobic layers for gas diffusion electrodes |
BR7902625A (pt) * | 1978-05-04 | 1979-11-27 | Du Pont | Aperfeicoamento em sensor de concentracao de oxigenio |
DE2837118C2 (de) * | 1978-08-25 | 1982-05-19 | Dornier System Gmbh, 7990 Friedrichshafen | Poröse Oxidelektroden für elektrochemische Hochtemperaturzellen |
US4631238A (en) * | 1985-01-18 | 1986-12-23 | Westinghouse Electric Corp. | Cobalt doped lanthanum chromite material suitable for high temperature use |
DE3610363A1 (de) * | 1986-03-27 | 1987-10-01 | Kernforschungsz Karlsruhe | Verfahren zum kontinuierlichen ueberwachen von konzentrationen von gasfoermigen bestandteilen in gasgemischen, ausgenommen o(pfeil abwaerts)2(pfeil abwaerts) |
JPH01105472A (ja) * | 1987-10-16 | 1989-04-21 | Mitsubishi Heavy Ind Ltd | 固体電解質燃料電池 |
US4895576A (en) * | 1988-04-15 | 1990-01-23 | Westinghouse Electric Corp. | Method of doping interconnections for electrochemical cells |
US4885078A (en) * | 1988-12-07 | 1989-12-05 | Westinghouse Electric Corp. | Devices capable of removing silicon and aluminum from gaseous atmospheres |
JPH03112059A (ja) * | 1989-09-27 | 1991-05-13 | Osaka Gas Co Ltd | 固体電解質燃料電池 |
JPH03112057A (ja) * | 1989-09-27 | 1991-05-13 | Osaka Gas Co Ltd | 固体電解質燃料電池 |
ES2100877T5 (es) * | 1989-12-27 | 2004-03-16 | The Standard Oil Company | Reactores electroquimicos y membranas de varios componentes utiles para reacciones de oxidacion. |
JP3134882B2 (ja) * | 1990-03-30 | 2001-02-13 | 東燃ゼネラル石油株式会社 | ランタンクロマイト系複合酸化物と用途 |
JPH0412457A (ja) * | 1990-04-27 | 1992-01-17 | Tonen Corp | 高温型燃料電池 |
JPH04230955A (ja) * | 1990-05-31 | 1992-08-19 | Tonen Corp | 高温型燃料電池 |
DE4116734C1 (ja) * | 1991-05-23 | 1992-10-15 | Abb Patent Gmbh, 6800 Mannheim, De | |
US5543239A (en) * | 1995-04-19 | 1996-08-06 | Electric Power Research Institute | Electrode design for solid state devices, fuel cells and sensors |
-
1994
- 1994-01-11 DE DE4400540A patent/DE4400540C2/de not_active Expired - Fee Related
-
1995
- 1995-01-10 EP EP95905046A patent/EP0739543A1/de not_active Withdrawn
- 1995-01-10 US US08/682,508 patent/US5824429A/en not_active Expired - Fee Related
- 1995-01-10 WO PCT/DE1995/000026 patent/WO1995019053A1/de not_active Application Discontinuation
- 1995-01-10 JP JP7518270A patent/JPH09507335A/ja active Pending
- 1995-01-10 AU AU13821/95A patent/AU694471B2/en not_active Ceased
-
1996
- 1996-07-10 NO NO962900A patent/NO962900L/no unknown
Non-Patent Citations (1)
Title |
---|
See references of WO9519053A1 * |
Also Published As
Publication number | Publication date |
---|---|
NO962900D0 (no) | 1996-07-10 |
AU1382195A (en) | 1995-08-01 |
JPH09507335A (ja) | 1997-07-22 |
NO962900L (no) | 1996-07-10 |
US5824429A (en) | 1998-10-20 |
AU694471B2 (en) | 1998-07-23 |
WO1995019053A1 (de) | 1995-07-13 |
DE4400540A1 (de) | 1995-07-13 |
DE4400540C2 (de) | 1995-10-12 |
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Legal Events
Date | Code | Title | Description |
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PUAI | Public reference made under article 153(3) epc to a published international application that has entered the european phase |
Free format text: ORIGINAL CODE: 0009012 |
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17P | Request for examination filed |
Effective date: 19960710 |
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AK | Designated contracting states |
Kind code of ref document: A1 Designated state(s): AT BE CH DE DK ES FR GB GR IE IT LI LU MC NL PT SE |
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17Q | First examination report despatched |
Effective date: 19971126 |
|
STAA | Information on the status of an ep patent application or granted ep patent |
Free format text: STATUS: THE APPLICATION IS DEEMED TO BE WITHDRAWN |
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18D | Application deemed to be withdrawn |
Effective date: 19980929 |