DE19602176C2 - High-temperature fuel cell with a cathode made of a perovskite - Google Patents
High-temperature fuel cell with a cathode made of a perovskiteInfo
- Publication number
- DE19602176C2 DE19602176C2 DE19602176A DE19602176A DE19602176C2 DE 19602176 C2 DE19602176 C2 DE 19602176C2 DE 19602176 A DE19602176 A DE 19602176A DE 19602176 A DE19602176 A DE 19602176A DE 19602176 C2 DE19602176 C2 DE 19602176C2
- Authority
- DE
- Germany
- Prior art keywords
- fuel cell
- perovskite
- phase
- cathode
- temperature fuel
- 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.)
- Expired - Fee Related
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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
- 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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8671—Removing components of defined structure not provided for in B01D53/8603 - B01D53/8668
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01F—COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS
- C01F17/00—Compounds of rare earth metals
- C01F17/30—Compounds containing rare earth metals and at least one element other than a rare earth metal, oxygen or hydrogen, e.g. La4S3Br6
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G51/00—Compounds of cobalt
- C01G51/006—Compounds containing, besides cobalt, two or more other elements, with the exception of oxygen or hydrogen
-
- 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
- C04B35/50—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on rare-earth compounds
-
- 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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/10—Single element gases other than halogens
- B01D2257/104—Oxygen
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/30—Three-dimensional structures
- C01P2002/34—Three-dimensional structures perovskite-type (ABO3)
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/50—Solid solutions
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
- C01P2002/72—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Electrochemistry (AREA)
- Environmental & Geological Engineering (AREA)
- Ceramic Engineering (AREA)
- Biomedical Technology (AREA)
- Life Sciences & Earth Sciences (AREA)
- Geology (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Analytical Chemistry (AREA)
- Manufacturing & Machinery (AREA)
- Health & Medical Sciences (AREA)
- Structural Engineering (AREA)
- Inert Electrodes (AREA)
Description
Die Erfindung bezieht sich auf eine Hochtemperaturbrennstoffzelle mit einer Kathode, die aus einem Perowskiten besteht.The invention relates to a high temperature fuel cell with a cathode consisting of a perovskite.
Es ist bekannt, Perowskite oder perowskitähnliche Strukturen zur Herstellung von Kathoden bei Hochtempe ratur-Brennstoffzellen einzusetzen.It is known to be perovskite or perovskite-like Structures for the production of cathodes at high temperature rature fuel cells.
Brennstoffzellen wandeln chemische Energie in elektri schen Strom um. Ein aus Anode, Elektrolyt und Kathode bestehendes System bewerkstelligt eine solche Umwand lung. An der Kathode wird der Sauerstoff der Luft mit Elektronen beladen und in Oxidionen umgewandelt. Die Oxidionen treten an der Dreiphasengrenze Kathode/ Luft/Elektrolyt in den Elektrolyten ein.Fuel cells convert chemical energy into electri electricity. One made of anode, electrolyte and cathode existing system accomplishes such a conversion lung. The oxygen in the air is also at the cathode Load electrons and convert them into oxide ions. The Oxide ions occur at the three-phase boundary cathode / Air / electrolyte in the electrolyte.
Um einen hohen Stromfluß zu ermöglichen, muß die Ka thode ein guter Elektronenleiter sein. Zur Gewährlei stung eines hohen Sauerstoffaustausches ist die Kathode vorteilhaft porös.To enable a high current flow, the Ka be a good electron conductor. To guarantee A high oxygen exchange is the cathode advantageously porous.
Aufgrund von unterschiedlichen Ausdehnungskoeffizienten der verschiedenen Materialien verhält sich das System Kathode/Elektrolyt mechanisch instabil. Daneben entste hen infolge der hohen Arbeitstemperaturen neue Phasen und chemische Verbindungen, die gleichfalls negativ auf das gewünschten Verhalten des Systems Ka thode/Elektrolyt einwirken. Daher sollte sich das Ka thodenmaterial ferner chemisch inert verhalten und einen ähnlichen Ausdehnungskoeffizienten wie der Elektrolyt aufweisen.Due to different expansion coefficients the system behaves of different materials Mechanically unstable cathode / electrolyte. Next to it hen new phases due to the high working temperatures and chemical compounds that are also negative the desired behavior of the system Ka act on the electrolyte. Therefore, the Ka method material also be chemically inert and a coefficient of expansion similar to that Have electrolyte.
Um stabile Keramiken zu erhalten, werden einphasige Strukturen bevorzugt. Die Perowskite werden mit weite ren Oxiden dotiert, um katalytische Eigenschaften und elektronisches Leitfähigkeitsvermögen zu erhöhen. Bisher werden unterschiedlich dotierte AIIIBIIIO3- Perowskite, zum Beispiel Lanthan-Manganite oder Lanthan-Ferrite, dotiert mit Strontium, Eisen oder Cobalt als Kathodenmaterial bevorzugt verwendet (Lit: B. C. H. Steele, State-of-the-Art SOFC Ceramic Materials, ist Europ. SOFC Forum, Oct. 3-7, 1994, Lucerne/Swiss, Proc., p. 375; H. U. Anderson, Defect chemistry of p-type Perowskites, 14th Riso Intern. Symp. on Materials Science, 6-10 Sept. 1993; B. C. H. Steele, Isotopic exchange and optimization of SOFC Cathode materials, 14th Riso Intern. Symp. an Materials Science, 6-10 Sept. 1993).In order to obtain stable ceramics, single-phase structures are preferred. The perovskites are doped with further oxides to increase catalytic properties and electronic conductivity. So far, differently doped A III B III O 3 perovskites, for example lanthanum-manganites or lanthanum ferrites, doped with strontium, iron or cobalt, have been used with preference as the cathode material (Lit: BCH Steele, State-of-the-Art SOFC Ceramic Materials , is Europ. SOFC Forum, Oct. 3-7, 1994, Lucerne / Swiss, Proc., p. 375; HU Anderson, Defect chemistry of p-type Perowskites, 14th Riso Intern. Symp. on Materials Science, 6-10 Sept. 1993; BCH Steele, Isotopic exchange and optimization of SOFC Cathode materials, 14th Riso Intern. Symp. An Materials Science, 6-10 Sept. 1993).
Es ist jedoch bisher nicht möglich, alle genannten An forderungen mit einem Material im ausreichenden Maße zu gewährleisten. Bei sehr guten funktionellen Eigen schaften sind die bekannten Materialien chemisch reak tiv mit anderen in der Konstruktion erforderlichen Ma terialien oder im thermischen Ausdehnungskoeffizienten nicht angepaßt. However, it is not yet possible to do all of the above to a sufficient extent with one material guarantee. With very good functional properties The known materials are chemically reactive tiv with other dimensions required in the construction materials or in the coefficient of thermal expansion not adjusted.
Aufgabe der Erfindung ist die Schaffung einer Hochtemperaturbrennstoffzelle mit einer verbesserten Kathode.The object of the invention is to create a high temperature fuel cell with an improved cathode.
Gelöst wird die Aufgabe durch eine Hochtemperaturbrennstoffzelle mit den Merk malen des Anspruchs.The task is solved by a high-temperature fuel cell with the mark paint the claim.
Ein Mischoxid der Zusammensetzung MIIMIVO3 als Wirtsoxid wird mit einer Dotierung von 5 bis 30 mol% Mx auf dem Platz MIV verwendet. Es entsteht ein Mischoxid der Zusammensetzung MIIMIV(MX)O3-y. Dieses Material scheidet bei erhöhter Temperatur von 600 bis 1000°C und bei erhöhtem Sauerstoffpartialdruck in seiner Umgebung eine zweite Phase, zum Beispiel das Oxid MIIMxO3-z aus. Beim Absinken des Sauerstoffpartialdrucks wird das Oxid reversibel wieder im Mischoxid aufgelöst.A mixed oxide of the composition M II M IV O 3 as the host oxide is used with a doping of 5 to 30 mol% M x on the M IV site . A mixed oxide of the composition M II M IV (M X ) O 3-y is formed . This material separates a second phase, for example the oxide M II M x O 3-z , at an elevated temperature of 600 to 1000 ° C. and at an increased oxygen partial pressure in its environment. When the oxygen partial pressure drops, the oxide is reversibly dissolved again in the mixed oxide.
Mittels des anspruchsgemäßen Kathodenmaterials lassen sich Eigen schaften der zwei Phasen addieren, etwa die chemische Reaktionsstabilität und thermische Ausdehnung der Wirtsphase mit der hohen elektrischen Leitfähigkeit und Sauerstoffaustauschfähigkeit der temporär auftretenden zweiten Phase. Die Wiederauflösung der zweiten Phase sorgt vorteilhaft für eine Regeneration der ka talytischen Fähigkeiten der zweiten Phase. Aufheiz- und Abkühlungszyklen verursachen aufgrund des Auflösungs vermögens keine mechanischen Probleme zwischen der Wirts- und der zweiten Phase.By means of the sophisticated cathode material you can create your own Add the properties of the two phases, for example the chemical one Reaction stability and thermal expansion of the Host phase with high electrical conductivity and Oxygen exchange ability of the temporarily occurring second phase. The redissolution of the second phase ensures regeneration of the ka second stage analytical skills. Heating and Cooling cycles cause due to the dissolution have no mechanical problems between the Host and the second phase.
Es kommt darauf an, solche Materialzusammensetzungen zu wählen, die unter den Temperatur- und pO2-Bedingungen, unter denen sie die Funktion ausüben sollen, die gefor derten Eigenschaften zeigen.It is important to choose such material compositions that show the required properties under the temperature and pO 2 conditions under which they are to perform the function.
Als Wirtsmaterialien sind AIIBIVO3-Perowskite vorgese hen, da diese eine hohe Redoxstabilität und chemische Verträglichkeit mit anderen Materialien aufweisen. Zwar ist ihre elektronische Leitfähigkeit und katalytische Wirksamkeit für Reaktionen mit Sauerstoff relativ ge ring. Dieser Nachteil wird jedoch durch die temporär auftretende Phase kompensiert, da diese das gewünschte Leitfähigkeitsverhalten und die gewünschte katalytische Wirkung ergänzt.A II B IV O 3 perovskites are provided as host materials, since they have high redox stability and chemical compatibility with other materials. Their electronic conductivity and catalytic effectiveness for reactions with oxygen are relatively low. However, this disadvantage is compensated for by the temporarily occurring phase, since this complements the desired conductivity behavior and the desired catalytic effect.
Als die temporäre Phase bildende Übergangsmetallkat ionen eignen sich insbesondere Co, Ti, Fe oder Mn, mit denen in entsprechender Menge dotiert wird. Elektrische Leitfähigkeit und katalytische Wirksamkeit, die das Wirtsmaterial nicht im ausreichendem Maße besitzt, wer den bei dieser Wahl in besonders hohem Maße ergänzt. Es kann dem Fachmann überlassen bleiben, optimale Kom binationen für den jeweiligen Anwendungsfall mittels einiger, weniger Versuche auszuwählen. As the transition metal cat forming the temporary phase Ions are particularly suitable for Co, Ti, Fe or Mn which are endowed in the appropriate amount. Electrical Conductivity and catalytic effectiveness that the Who owns host material is not sufficient supplemented to a particularly high degree in this election. It can be left to the specialist to determine optimal com combinations for the respective application a few, fewer attempts to choose.
Es zeigen:Show it:
Fig. 1: Röntgendiagramme für eine SrCe0,8Co0,2O3-y- Probe Fig. 1: X-ray diagrams for a SrCe 0.8 Co 0.2 O 3-y sample
Fig. 2: katalytische Wirksamkeit von SrCe0,8Co0,2O3-y Fig. 2: Catalytic activity of SrCe 0.8 Co 0.2 O 3-y
Fig. 3: Leitfähigkeitsverhalten bei Ausscheidung/ Auf lösung der zweiten Phase Fig. 3: Conductivity behavior in the case of excretion / solution of the second phase
Fig. 1 zeigt Röntgendiagramme für eine aus SrCe0,8Co0,2O3-y bestehende Probe. Diese wurde 30 Stunden bei 1200°C in Luft (Kurve a), dann in N2/2% H2 für 20 Stunden bei 1250°C (Kurve b) reduziert sowie 20 Stunden lang bei 1200°C in Luft reoxidiert (Kurve c). Das Diagramm verdeutlicht Bedingungen für das Auftreten bzw. Wiederauflösen der zweiten Phase. Der zugehörige Peak der zweiten Phase ist in Fig. 1 mit einem * markiert. Gemäß Kurve a tritt dieser Peak und somit die zweite Phase auf, dieser verschwindet gemäß Kurve b und tritt dann in Kurve c wieder auf. Fig. 1 shows X-ray diagrams for one of SrCe 0.8 Co 0.2 O 3-y existing sample. This was reduced for 30 hours at 1200 ° C in air (curve a), then in N2 / 2% H 2 for 20 hours at 1250 ° C (curve b) and reoxidized for 20 hours at 1200 ° C in air (curve c) . The diagram illustrates conditions for the occurrence or redissolution of the second phase. The associated peak of the second phase is marked with an * in FIG. 1. According to curve a, this peak and thus the second phase occurs, this disappears according to curve b and then reappears in curve c.
In Fig. 2, ist die O2-Abgabe des Materials SrCe0,8Co0,2O3-y unter verschiedenen Temperatur- und pO2-Bedingungen als Größe für die katalytische Wirksamkeit charakterisiert. Der Sauerstoffgehalt (3 - y) in Mol in der Probe SrCe0,8Co0,2O3-y ist als Funktion der Temperatur und des Sauerstoffpartialdrucks dargestellt. Die katalytische Wirksamkeit ist an der austauschbaren Sauerstoffmenge y gegenüber unterschiedlichen O2- Partialdrücken des Umgebungsgases erkennbar.In Fig. 2, the O 2 release of the material SrCe 0.8 Co 0.2 O 3-y under different temperature and pO 2 conditions is characterized as a parameter for the catalytic activity. The oxygen content (3 - y) in mol in the sample SrCe 0.8 Co 0.2 O 3-y is shown as a function of the temperature and the oxygen partial pressure. The catalytic effectiveness can be seen from the exchangeable amount of oxygen y in relation to different O 2 partial pressures of the ambient gas.
Fig. 3 zeigt eine sprunghafte Änderung der elektrischen Leitfähigkeit in der SrCe0,8Co0,2O3-y-Probe, die innerhalb von 30 Sekunden bei Umschaltung des umgebenden Gases von reduzierender Atmosphäre G auf oxidierende Atmosphäre L auftritt. In Luft L wird die zweite Phase ausgeschieden. In reduzierender Gasatmosphäre G bei einem Druck von 10-15 atm löst sich die zweite Phase auf. Fig. 3 shows an abrupt change in electrical conductivity in the SrCe 0.8 Co 0.2 O 3-y -probe that occurs within 30 seconds after switching of the surrounding gas of reducing atmosphere to an oxidizing atmosphere G L. The second phase is eliminated in air L. The second phase dissolves in a reducing gas atmosphere G at a pressure of 10 -15 atm.
Materialzusammensetzungen, die sich insbesondere für
den Einsatz als Kathode in einer Hochtemperatur-
Brennstoffzelle eignen, sind:
Material compositions that are particularly suitable for use as a cathode in a high-temperature fuel cell are:
Claims (1)
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
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DE19602176A DE19602176C2 (en) | 1996-01-23 | 1996-01-23 | High-temperature fuel cell with a cathode made of a perovskite |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
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DE19602176A DE19602176C2 (en) | 1996-01-23 | 1996-01-23 | High-temperature fuel cell with a cathode made of a perovskite |
Publications (2)
Publication Number | Publication Date |
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DE19602176A1 DE19602176A1 (en) | 1997-08-07 |
DE19602176C2 true DE19602176C2 (en) | 1999-01-07 |
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DE19602176A Expired - Fee Related DE19602176C2 (en) | 1996-01-23 | 1996-01-23 | High-temperature fuel cell with a cathode made of a perovskite |
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DK1356535T3 (en) * | 2000-11-14 | 2006-10-02 | Forskningsct Riso | Dimensionally stable electronic or mixed conductive material |
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1996
- 1996-01-23 DE DE19602176A patent/DE19602176C2/en not_active Expired - Fee Related
Non-Patent Citations (1)
Title |
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Chem. abstr. 121(1994) Ref.-Nr. 38790n * |
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Free format text: HAART, LAMBERTUS G.J. DE, DR., HEERLEN, NL NAOUMIDIS, ARISTIDES, DR., 52428 JUELICH, DE TESKE, KLAUS, DR., 01129 DRESDEN, DE ULLMANN, HELMUT, PROF.DR., 01277 DRESDEN, DE TROFIMENKO, NIKOLAI, DR., 01069 DRESDEN, DE PAULSEN, JENS, 01219 DRESDEN, DE MECKEL, GUDRUN, 01309 DRESDEN, DE |
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Ipc: H01M 8/12 |
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