EP1665429A2 - Electric contact for high-temperature fuel cells and methods for the production of said contact - Google Patents

Electric contact for high-temperature fuel cells and methods for the production of said contact

Info

Publication number
EP1665429A2
EP1665429A2 EP04762750A EP04762750A EP1665429A2 EP 1665429 A2 EP1665429 A2 EP 1665429A2 EP 04762750 A EP04762750 A EP 04762750A EP 04762750 A EP04762750 A EP 04762750A EP 1665429 A2 EP1665429 A2 EP 1665429A2
Authority
EP
European Patent Office
Prior art keywords
contact
contacting
temperature fuel
metallic
component
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Withdrawn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
EP04762750A
Other languages
German (de)
French (fr)
Inventor
Nikolai Trofimenko
Mihail Kuznecov
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.)
Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV
Original Assignee
Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV
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 Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV filed Critical Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV
Publication of EP1665429A2 publication Critical patent/EP1665429A2/en
Withdrawn legal-status Critical Current

Links

Classifications

    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C26/00—Coating not provided for in groups C23C2/00 - C23C24/00
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C10/00—Solid state diffusion of only metal elements or silicon into metallic material surfaces
    • C23C10/28—Solid state diffusion of only metal elements or silicon into metallic material surfaces using solids, e.g. powders, pastes
    • C23C10/30—Solid state diffusion of only metal elements or silicon into metallic material surfaces using solids, e.g. powders, pastes using a layer of powder or paste on the surface
    • 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
    • H01M8/023—Porous and characterised by the material
    • H01M8/0232—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
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/023—Porous and characterised by the material
    • H01M8/0236—Glass; Ceramics; 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
    • H01M8/023—Porous and characterised by the material
    • H01M8/0241—Composites
    • H01M8/0243—Composites in the form of mixtures
    • 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
    • H01M8/023—Porous and characterised by the material
    • H01M8/0241—Composites
    • H01M8/0245—Composites in the form of layered or coated products
    • 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
    • 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
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T29/00—Metal working
    • Y10T29/49—Method of mechanical manufacture
    • Y10T29/49002—Electrical device making
    • Y10T29/49117—Conductor or circuit manufacturing
    • Y10T29/49204—Contact or terminal manufacturing
    • Y10T29/49208—Contact or terminal manufacturing by assembling plural parts
    • Y10T29/4921—Contact or terminal manufacturing by assembling plural parts with bonding

Definitions

  • the invention relates to an electrical contact for high-temperature fuel cells and a method for producing such a contact.
  • the invention relates to an electrical contact for high-temperature fuel cells and to a method aimed at producing such an electrical contact.
  • the electrical contacts according to the invention can preferably be used on the anode side of high-temperature fuel cells, to which the particular fuel, such as hydrogen and suitable low-molecular hydrocarbon compounds, such as natural gas or methane, is supplied for the actual process. Its reducing effect can also be used in a targeted manner.
  • High-temperature fuel cells are often electrically combined to form more complex units, that is to say a plurality of such individual fuel cells, and are connected in series and / or in parallel with one another in order to achieve an increased electrical output power. Fuel cell stacks are formed.
  • the individual respective high-temperature fuel cells are provided with interconnectors, usually so-called biopolar plates.
  • the electrodes of the respective fuel cell that is to say a cathode and also an anode, to be electrically conductively connected to the respective interconnector assigned to them.
  • an oxide layer essentially consisting of chromium oxide very quickly forms.
  • This chromium oxide layer also forms on the surface of the interconnector facing the interior of the fuel cell in the areas in which the nickel network is in contact with the interconnector.
  • the protective layers cannot always compensate for mechanical influences such as vibrations, changes in pressure and tensile stresses, or a sufficiently high resistance to such influences can be achieved, and accordingly the electrically conductive connection is adversely affected in an undesirable manner.
  • this object is achieved with an electrical contact for high-temperature fuel cells, which has the features of claim 1.
  • a manufacturing method for such electrical contacts is defined in claim 14.
  • the electrical contact according to the invention is in the form of a composite which consists of a metallic component and a ceramic component.
  • the metallic component of the composite is formed from at least one metal oxide, this metal oxide also being able to be contained in the contact as it is, ie as a non-reduced chemical compound.
  • the ceramic component of the composite should advantageously be conductive for contacting for oxygen ions.
  • the metallic component of the composite can be formed at least temporarily from NiO, CuO and / or MgO.
  • nickel or copper are the correspondingly reduced metal oxides, and the magnesium oxide which may be present in the composite also remains as such in the finished electrical contact.
  • Zirconium oxide and cerium oxide have been found to be particularly suitable for the ceramic component.
  • the ceramic component of the composite may have been formed solely from zirconium oxide, solely from cerium oxide, but also from both oxides.
  • Stabilized zirconium oxide (Zr0 2 ) 0.92 (Y 2 0 3 ) 0.08 should advantageously be used, but optionally also partially stabilized zirconium oxide (Zr0 2 ) 0.97 (Y2O3) 0.03.
  • cerium oxide this can advantageously be doped with other elements (e.g. Ca, Sr, Gd, Sc).
  • the respective metallic component should be contained with 80 to 100 mass% and the ceramic component with 0 to 20 mass%.
  • the metallic component is contained in highly dispersed form.
  • a particle size of a pure metal or a corresponding metal alloy obtained by reduction compared to the particle size of the starting powder can be achieved within the contact.
  • the contacting formed on or between the electrically conductive elements to be contacted should have a thickness of 2 to 500 ⁇ m in order to be able to guarantee the desired long-term protection while at the same time having a sufficiently high electrical conductivity.
  • the electrical contact can be formed on at least one surface of a metallic network which is arranged between an anode and the interconnector assigned to it in a high-temperature fuel cell.
  • Such a metallic network which, as in the prior art, can also have been formed from nickel, should have been provided with a contact according to the invention at least on the surface which is in contact with the anode.
  • contacting according to the invention can also have been formed over a large area on the corresponding surface of the anode and / or on the surface of the interconnector facing the interior of the fuel cell.
  • a procedure can be followed such that a mixture which is formed from a metallic and a ceramic component is applied to elements which are to be electrically connected to one another but also between such electrically conductive elements.
  • This order is followed by heat treatment and a supply of a reducing agent, the supply of the reducing agent being able to take place after a certain predetermined temperature has been reached.
  • binder components contained in the starting mixture can be driven out.
  • the heat treatment and the reduction can advantageously be carried out in situ within the high-temperature fuel cell, the respective fuel being able to act as a reducing agent.
  • an adhesive diffusion bond can also be formed at the interfaces of the electrically conductive elements to be contacted.
  • both the metallic component and the ceramic component can be deformed are used, it being favorable to mix them together with a binder and, if appropriate, a suitable solvent, such as water and an organic solvent, so that a pasty consistency can be set.
  • a suitable solvent such as water and an organic solvent
  • the mixture can be applied in this pasty form.
  • An order can be made by screen printing technology known per se or by rolling up.
  • a mixture with a suitable consistency can also be applied using the wet powder spray method.
  • the catalytic activity of a high-temperature fuel cell can be improved by a correspondingly achievable increase in the active anode area.
  • the electrical contacting according to the invention is also chemically and thermally resistant in the frequently occurring redox cycles, which also ensures a sufficiently high electrical conductivity in the long term.
  • an increased adhesive strength of the contact can be achieved through the diffusion bond that can be achieved.
  • FIG. 1 shows a schematic representation of a section through a high-temperature fuel cell with an electrical contact formed between a metallic network and the anode of the fuel cell and
  • Figure 2 in a schematic form and enlargement of the electrical contact formed between the metallic network and anode in one example.
  • FIG. 1 A section through a high-temperature fuel cell is shown in schematic form in FIG.
  • a bipolar plate is arranged on the cathode side as an interconnector 6.
  • a further interconnector 5 is arranged on the side of the fuel cell opposite the interconnector 6, in which channels for the supply of a suitable fuel for the operation of the fuel cell by a corresponding one in schematic form Structuring have been trained.
  • a metallic network 4 made of nickel has been placed on the surface of the interconnector 5 which faces the interior of the high-temperature fuel cell and which can also be designed as a bipolar plate.
  • the connection of the metallic network 4 to the interconnector 5 may have been made point by point by welding.
  • the electrical contact 1 was formed on the surface of the metallic network 4 pointing in the direction of the anode 3.
  • FIG. 1 also shows a gas channel between cathode 3 'and interconnector 6 for supplying the oxidizing agent (oxygen or air) required for operating the fuel cell.
  • oxidizing agent oxygen or air
  • the surface of the interconnector 5 pointing in the direction of the interior of the high-temperature fuel cell was previously provided with a protective nickel layer.
  • the mixture containing the aforementioned metallic component and the ceramic component had been applied to the surface of the metallic network 4, here with a layer thickness of 300 ⁇ m and subsequent assembly of the fuel cell, it was put into operation normally, so that early heating, i.e. a quasi heat treatment, the nickel oxide starting powder has been completely reduced to metallic nickel.
  • an adherent, diffusion bond was formed with the magnesium oxide between the anode 3, the metallic network 4 and the electrical contact 1 and also with the stabilized zirconium oxide forming the ceramic component at the respective interfaces.

Abstract

An electric contact for high-temperature fuel cells and to methods for the production of said contacts. The aim of the invention is to enable long-term use at high operating temperatures of up to 950 °C, offering high electrical conductivity and being able to be produced at low cost. The inventive electric contact is produced from a composite consisting of a metal component and a ceramic component. The metal component is, preferably, formed with at least one metal oxide.

Description

Elektrische Kontaktierung für Hochtemperaturbrennstoffzellen sowie Verfahren zur Herstellung einer solchen KontaktierungElectrical contacting for high-temperature fuel cells and method for producing such contacting
Die Erfindung betrifft eine elektrische Kontaktierung für Hochtemperaturbrennstoffzellen sowie ein Verfahren zur Herstellung einer solchen Kontaktierung.The invention relates to an electrical contact for high-temperature fuel cells and a method for producing such a contact.
Die Erfindung betrifft eine elektrische Kontaktierung für Hochtemperaturbrennstoffzellen sowie ein auf die Herstellung einer solchen elektrischen Kontaktierung gerichtetes Verfahren. Die erfindungsgemäßen elektrischen Kontaktierungen können bevorzugt auf der Anodenseite von Hochtemperaturbrennstoffzellen einge- setzt werden, an der der jeweilige Brennstoff, wie z.B. Wasserstoff und geeignete niedermolekulare KohlenwasserstoffVerbindungen, wie Erdgas oder Methan, für den eigentlichen Prozess zugeführt wird. Dabei kann auch dessen reduzierende Wirkung gezielt ausge- nutzt werden. Hochtemperaturbrennstoffzellen werden häufig zu komplexeren Einheiten also mehrere solcher einzelnen Brennstoffzellen elektrisch zusammengefasst und dabei in Reihe und/oder parallel miteinander verschaltet, um eine erhöhte elektrische Ausgangsleistung zu erreichen. Es werden dabei BrennstoffZellenstapel (Stacks) gebildet.The invention relates to an electrical contact for high-temperature fuel cells and to a method aimed at producing such an electrical contact. The electrical contacts according to the invention can preferably be used on the anode side of high-temperature fuel cells, to which the particular fuel, such as hydrogen and suitable low-molecular hydrocarbon compounds, such as natural gas or methane, is supplied for the actual process. Its reducing effect can also be used in a targeted manner. High-temperature fuel cells are often electrically combined to form more complex units, that is to say a plurality of such individual fuel cells, and are connected in series and / or in parallel with one another in order to achieve an increased electrical output power. Fuel cell stacks are formed.
In diesen Fällen sind die einzelnen jeweiligen Hochtemperaturbrennstoffzellen mit Interkonnektoren, üblicherweise so genannte biopolare Platten, versehen.In these cases, the individual respective high-temperature fuel cells are provided with interconnectors, usually so-called biopolar plates.
Hierzu ist es erforderlich, dass die Elektroden der jeweiligen Brennstoffzelle, also eine Kathode und auch eine Anode, elektrisch leitend mit dem jeweiligen ihnen zugeordneten Interkonnektor elektrisch leitend verbunden werden.For this purpose, it is necessary for the electrodes of the respective fuel cell, that is to say a cathode and also an anode, to be electrically conductively connected to the respective interconnector assigned to them.
Für die elektrisch leitende Verbindung einer Anode mit einem Interkonnektor ist beispielsweise aus DE 196 49 457 Cl bekannt, ein flexibel verformbares Netzwerk aus Nickel zwischen Interkonnektor und Anode einzusetzen, das mit dem Interkonnektor und der Anode zu kontaktieren ist.For the electrically conductive connection of an anode to an interconnector, it is known, for example from DE 196 49 457 Cl, to use a flexibly deformable network of nickel between the interconnector and anode, which is to be contacted with the interconnector and the anode.
Beim Betrieb einer so ausgebildeten Brennstoffzelle bildet sich sehr schnell eine im Wesentlichen aus Chromoxid bestehende Oxidschicht . Diese Chromoxid- schicht bildet sich auf der in das Innere der Brennstoffzelle weisenden Oberfläche des Interkonnektors auch in den Bereichen aus, in denen das Nickelnetzwerk mit dem Interkonnektor im berührenden Kontakt steht .When operating a fuel cell designed in this way, an oxide layer essentially consisting of chromium oxide very quickly forms. This chromium oxide layer also forms on the surface of the interconnector facing the interior of the fuel cell in the areas in which the nickel network is in contact with the interconnector.
Dementsprechend erhöhen sich die elektrischen Wider- stände und Übergangswiderstände, was zu einer erheblichen Reduzierung der elektrischen Leitfähigkeit führt, die wiederum eine Reduzierung des Wirkungsgrades einer solchen Hochtemperaturbrennstoffzelle zur Folge hat .Accordingly, the electrical resistances levels and contact resistance, which leads to a considerable reduction in the electrical conductivity, which in turn results in a reduction in the efficiency of such a high-temperature fuel cell.
Eine solche Oxidschicht beeinträchtigt aber auch durch Verschweißen erhaltene Verbindungspunkte eines Nickelnetzwerkes mit dem Interkonnektor, wobei eine Unterwanderung der Schweißpunkte mit dem gebildeten Chromoxid zu verzeichnen ist .However, such an oxide layer also impairs the connection points of a nickel network obtained by welding with the interconnector, with an undermining of the welding points with the chromium oxide being formed.
In DE 198 36 352 AI wird zur Vermeidung der Ausbildung und Unterwanderung mit solchen Oxidschichten vorgeschlagen, eine dünne Schutzschicht aus reinem Nickel auszubilden. Schutzschichten aus Nickel mit anderen Elementen sind auch aus DE 199 13 873 AI bekannt .In DE 198 36 352 AI to avoid the formation and infiltration with such oxide layers it is proposed to form a thin protective layer of pure nickel. Protective layers made of nickel with other elements are also known from DE 199 13 873 AI.
Auch mit solchen Schutzschichten können nicht alle beim der Technik vorhandenen Nachteile beseitigt werden.Even with such protective layers, not all of the disadvantages existing in technology can be eliminated.
Außerdem können mit den Schutzschichten auch mechani- sehe Einflüsse wie Schwingungen, Druckänderungen und Zugspannungen nicht immer ausgeglichen werden bzw. ein ausreichend großer Widerstand gegen solche Einflüsse erreicht werden, und dementsprechend wird auch wieder die elektrisch leitende Verbindung in uner- wünschter Form beeinträchtigt.In addition, the protective layers cannot always compensate for mechanical influences such as vibrations, changes in pressure and tensile stresses, or a sufficiently high resistance to such influences can be achieved, and accordingly the electrically conductive connection is adversely affected in an undesirable manner.
Des Weiteren treten Probleme durch die erheblichen Temperaturdifferenzen und den beim Betrieb von Brennstoffzellen auftretenden Redox-Zyklen auf.Furthermore, problems arise due to the considerable temperature differences and the redox cycles that occur during the operation of fuel cells.
Es ist daher Aufgabe der Erfindung, eine dahingehend verbesserte elektrische Kontaktierung für Hochtemperaturbrennstoffzellen zur Verfügung zu stellen, die bei erhöhten Betriebstemperaturen bis hin zu 950 °C dauerhaft eine erhöhte elektrische Leitfähigkeit si- chert und dabei gleichzeitig einfach und kostengünstig hergestellt werden kann.It is therefore an object of the invention, one in this regard to provide improved electrical contacting for high-temperature fuel cells which, at elevated operating temperatures up to 950 ° C., ensures increased electrical conductivity in the long term and at the same time can be produced simply and inexpensively.
Erfindungsgemäß wird diese Aufgabe mit einer elektrischen Kontaktierung für Hochtemperaturbrennstoffzel- len, die die Merkmale des Anspruchs 1 aufweist, gelöst. Ein Herstellungsverfahren für solche elektrischen Kontaktierungen wird mit dem Patentanspruch 14 definiert .According to the invention, this object is achieved with an electrical contact for high-temperature fuel cells, which has the features of claim 1. A manufacturing method for such electrical contacts is defined in claim 14.
Vorteilhafte Ausgestaltungsformen und Weiterbildungen der Erfindung können mit den in den untergeordneten Ansprüchen bezeichneten Merkmalen erreicht werden.Advantageous refinements and developments of the invention can be achieved with the features specified in the subordinate claims.
Die erfindungsgemäße elektrische Kontaktierung ist dabei in Form eines Komposits, das aus einer metallischen Komponente und einer keramischen Komponente besteht, ausgebildet.The electrical contact according to the invention is in the form of a composite which consists of a metallic component and a ceramic component.
Sie kann an aber auch zwischen elektrisch leitend miteinander zu verbindenden Elementen von Brennstoffzellen angeordnet und ausgebildet sein.However, it can also be arranged and formed on elements of fuel cells to be connected to one another in an electrically conductive manner.
Die metallische Komponente des Komposits ist mindestens aus einem Metalloxid gebildet, wobei dieses Me- talloxid auch unverändert, also als nicht reduzierte chemische Verbindung in der Kontaktierung enthalten sein kann.The metallic component of the composite is formed from at least one metal oxide, this metal oxide also being able to be contained in the contact as it is, ie as a non-reduced chemical compound.
Es besteht aber auch die Möglichkeit, dass in der Kontaktierung durch Reduktion von Metalloxiden gebildete reine Metall oder Legierungen enthalten sind. In Vorteilhafterweise sollte die keramische Komponente des Komposits für die Kontaktierung für SauerstoffIonen leitend sein.However, there is also the possibility that pure metal or alloys formed by the reduction of metal oxides are contained in the contact. In The ceramic component of the composite should advantageously be conductive for contacting for oxygen ions.
Wie bereits angedeutet, kann die metallische Komponente des Komposits zumindest temporär aus NiO, CuO und/oder MgO gebildet sein. In diesem Fall stellen dann das Nickel oder auch das Kupfer die entsprechend reduzierten Metalloxide dar, und das in einem gegebe- nenfalls im Komposit enthaltenen Magnesiumoxid bleibt als solches auch in der fertigen elektrischen Kontaktierung enthalten.As already indicated, the metallic component of the composite can be formed at least temporarily from NiO, CuO and / or MgO. In this case, nickel or copper are the correspondingly reduced metal oxides, and the magnesium oxide which may be present in the composite also remains as such in the finished electrical contact.
Als besonders geeignet für die keramische Komponente haben sich Zirkonoxid und Ceroxid herausgestellt. Dabei kann die keramische Komponente des Komposits allein aus Zirkonoxid, allein aus Ceroxid, aber auch aus beiden Oxiden gemeinsam gebildet worden sein. Vorteilhaft sollte stabilisiertes Zirkonoxid (Zr02) 0,92 (Y203) 0,08 gegebenenfalls aber auch partiell stabilisiertes Zirkonoxid (Zr02) 0,97 (Y2O3) 0,03 eingesetzt werden.Zirconium oxide and cerium oxide have been found to be particularly suitable for the ceramic component. The ceramic component of the composite may have been formed solely from zirconium oxide, solely from cerium oxide, but also from both oxides. Stabilized zirconium oxide (Zr0 2 ) 0.92 (Y 2 0 3 ) 0.08 should advantageously be used, but optionally also partially stabilized zirconium oxide (Zr0 2 ) 0.97 (Y2O3) 0.03.
Im Falle von Ceroxid kann dieses vorteilhaft mit an- deren Elementen (z.B. Ca, Sr, Gd, Sc) dotiert sein.In the case of cerium oxide, this can advantageously be doped with other elements (e.g. Ca, Sr, Gd, Sc).
In dem die elektrische Kontaktierung ausbildenden Komposit sollte die jeweilige metallische Komponente mit 80 bis 100 Masse-% und die keramische Komponente mit 0 bis 20 Masse-% enthalten sein.In the composite forming the electrical contact, the respective metallic component should be contained with 80 to 100 mass% and the ceramic component with 0 to 20 mass%.
Wünschenswert und vorteilhaft ist es außerdem, wenn die metallische Komponente, zumindest Teile dieser Komponente, in hochdispergierter Form enthalten ist.It is also desirable and advantageous if the metallic component, at least parts of this component, is contained in highly dispersed form.
Das kann über eine feine Vermahlung von entsprechen- den Pulvern, die für die Ausbildung der elektrischen Kontaktierung eingesetzt werden können, erreicht werden.This can be achieved through a fine grinding of the powders that can be used for the formation of the electrical contact can be achieved.
Werden beispielsweise Oxide als Ausgangspulver für die metallische Komponente eingesetzt, so kann eine gegenüber der Partikelgröße der Ausgangspulver verringerte Partikelgröße eines durch Reduktion erhaltenen reinen Metalls bzw. einer entsprechenden Metall- legierung innerhalb der Kontaktierung erreicht werden.If, for example, oxides are used as the starting powder for the metallic component, a particle size of a pure metal or a corresponding metal alloy obtained by reduction compared to the particle size of the starting powder can be achieved within the contact.
Die an bzw. zwischen die zu kontaktierenden elektrisch leitenden Elementen ausgebildete Kontaktierung sollte eine Dicke von 2 bis 500 μm aufweisen, um den gewünschten Langzeitschutz bei gleichzeitiger ausreichend hoher elektrischer Leitfähigkeit gewährleisten zu können.The contacting formed on or between the electrically conductive elements to be contacted should have a thickness of 2 to 500 μm in order to be able to guarantee the desired long-term protection while at the same time having a sufficiently high electrical conductivity.
So kann die elektrische Kontaktierung zumindest auf einer Oberfläche eines metallischen Netzwerkes, das zwischen einer Anode und dem dieser zugeordneten Interkonnektor in einer Hochtemperaturbrennstoffzelle angeordnet ist, ausgebildet sein.For example, the electrical contact can be formed on at least one surface of a metallic network which is arranged between an anode and the interconnector assigned to it in a high-temperature fuel cell.
Ein solches metallisches Netzwerk, das wie beim Stand der Technik auch aus Nickel gebildet worden sein kann, sollte zumindest an der Oberfläche, die mit der Anode in Kontakt steht, mit einer erfindungsgemäßen Kontaktierung versehen worden sein.Such a metallic network, which, as in the prior art, can also have been formed from nickel, should have been provided with a contact according to the invention at least on the surface which is in contact with the anode.
Eine erfindungsgemäße Kontaktierung kann aber auch flächig auf der entsprechenden Oberfläche der Anode und/oder der in das Innere der Brennstoffzelle wei- senden Oberfläche des Interkonnektors ausgebildet worden sein. Für die Herstellung einer erfindungsgemäßen elektrischen Kontaktierung für Hochtemperaturbrennstoffzellen kann so vorgegangen werden, dass an elektrisch leitend miteinander zu verbindenden aber auch zwischen solchen elektrisch leitenden Elementen ein Gemisch, das aus einer metallischen und einer keramischen Komponente gebildet ist, aufgebracht wird.However, contacting according to the invention can also have been formed over a large area on the corresponding surface of the anode and / or on the surface of the interconnector facing the interior of the fuel cell. For the production of an electrical contact according to the invention for high-temperature fuel cells, a procedure can be followed such that a mixture which is formed from a metallic and a ceramic component is applied to elements which are to be electrically connected to one another but also between such electrically conductive elements.
Im Anschluss an diesen Auftrag erfolgen eine Wärmebehandlung und eine Zufuhr eines Reduktionsmittels, wobei die Zufuhr des Reduktionsmittels zeitversetzt nach Erreichen einer bestimmten vorgebbaren Mindest- temperatur erfolgen kann.This order is followed by heat treatment and a supply of a reducing agent, the supply of the reducing agent being able to take place after a certain predetermined temperature has been reached.
Dadurch wird eine zumindest teilweise Reduktion eines Metalloxides, das Bestandteil der metallischen Komponente in der Kontaktierung ist, zu dem entsprechenden reinen Metall oder einer Metalllegierung sowie eine Aushärtung der Kontaktierung erreicht.This results in an at least partial reduction of a metal oxide, which is a component of the metallic component in the contact, to the corresponding pure metal or a metal alloy, and a hardening of the contact.
Gleichzeitig können gegebenenfalls im Ausgangsgemisch enthaltene Binderbestandteile ausgetrieben werden.Simultaneously, binder components contained in the starting mixture can be driven out.
Vorteilhafterweise können die Wärmebehandlung und die Reduktion in situ innerhalb der Hochtemperaturbrennstoffzelle durchgeführt werden, wobei der jeweilige Brennstoff als Reduktionsmittel fungieren kann.The heat treatment and the reduction can advantageously be carried out in situ within the high-temperature fuel cell, the respective fuel being able to act as a reducing agent.
Infolge der Wärmebehandlung kann auch ein haftfester Diffusionsverbund an den Grenzflächen der miteinander zu kontaktierenden elektrisch leitenden Elemente ausgebildet werden.As a result of the heat treatment, an adhesive diffusion bond can also be formed at the interfaces of the electrically conductive elements to be contacted.
Wie bereits angedeutet, können sowohl die metallische Komponente als auch die keramische Komponente in Pul- verform eingesetzt werden, wobei es günstig ist, diese gemeinsam mit einem Binder und gegebenenf lls einem geeigneten Lösungsmittel, wie z.B. Wasser und einem organischen Lösungsmittel miteinander zu vermischen, so dass eine pastδse Konsistenz eingestellt werden kann.As already indicated, both the metallic component and the ceramic component can be deformed are used, it being favorable to mix them together with a binder and, if appropriate, a suitable solvent, such as water and an organic solvent, so that a pasty consistency can be set.
In dieser pastδsen Form kann das Gemisch aufgebracht werden.The mixture can be applied in this pasty form.
Dabei kann ein Auftrag durch an sich bekannte Siebdruck-Technik oder durch Aufrollen erfolgen.An order can be made by screen printing technology known per se or by rolling up.
Ein Gemisch mit entsprechend geeigneter Konsistenz kann aber auch im Nasspulverspritzverfahren aufgebracht werden .A mixture with a suitable consistency can also be applied using the wet powder spray method.
Mit der erfindungsgemäßen Lösung kann ein dauerhafter und effektiver Schutz des Nickel vor einer Oxidation auch bei den innerhalb der Brennstoffzelle bei deren Betrieb herrschenden erhöhten Temperaturen und unter Einwirkung des jeweiligen Brennstoffes erreicht und eine Erhöhung des elektrischen Widerstandes vermieden werden.With the solution according to the invention, permanent and effective protection of the nickel against oxidation can be achieved even at the elevated temperatures prevailing within the fuel cell during its operation and under the influence of the respective fuel, and an increase in the electrical resistance can be avoided.
Des Weiteren kann die katalytische Aktivität einer Hochtemperaturbrennstoffzelle durch eine entsprechend erreichbare Vergrößerung der aktiven Anodenfläche verbessert werden.Furthermore, the catalytic activity of a high-temperature fuel cell can be improved by a correspondingly achievable increase in the active anode area.
Die erfindungsgemäße elektrische Kontaktierung ist aber auch bei den häufig vorkommenden Redox-Zyklen chemisch und thermisch beständig, was eine dauerhaft ausreichend hohe elektrische Leitfähigkeit mit ge- währleistet. Wie bereits angedeutet, kann durch den erreichbaren Diffusionsverbund eine erhöhte Haftfestigkeit der Kontaktierung erreicht werden.However, the electrical contacting according to the invention is also chemically and thermally resistant in the frequently occurring redox cycles, which also ensures a sufficiently high electrical conductivity in the long term. As already indicated, an increased adhesive strength of the contact can be achieved through the diffusion bond that can be achieved.
Nachfolgend soll die Erfindung beispielhaft näher erläutert werden.The invention will be explained in more detail below by way of example.
Dabei zeigen:Show:
Figur 1 in schematischer Form eine Schnittdarstellung durch eine Hochtemperaturbrennstoffzelle mit einer zwischen einem metallischen Netzwerk und der Anode der Brennstoffzelle ausgebildeten elektrischen Kontaktierung und1 shows a schematic representation of a section through a high-temperature fuel cell with an electrical contact formed between a metallic network and the anode of the fuel cell and
Figur 2 in schematischer Form und Vergrößerung die zwischen metallischem Netzwerk und Anode ausgebildete elektrische Kontaktierung in einem Beispiel.Figure 2 in a schematic form and enlargement of the electrical contact formed between the metallic network and anode in one example.
In Figur 1 ist in schematischer Form ein Schnitt durch eine Hochtemperaturbrennstoffzelle dargestellt.A section through a high-temperature fuel cell is shown in schematic form in FIG.
Bei diesem Beispiel ist eine bipolare Platte als ein Interkonnektor 6 kathodenseitig angeordnet .In this example, a bipolar plate is arranged on the cathode side as an interconnector 6.
Daran anschließend ist eine Elektrodeneinheit mit einer Kathode 3', einem Festelektrolyten 2 und der Ano- de 3 vorhanden.Then there is an electrode unit with a cathode 3 ', a solid electrolyte 2 and the anode 3.
Auf der dem Interkonnektor 6 gegenüberliegenden Seite der Brennstoffzelle ist ein weiterer Interkonnektor 5 angeordnet, bei dem in schematischer Form Kanäle für die Zuführung eines geeigneten Brennstoffes für den Betrieb der Brennstoffzelle durch eine entsprechende Strukturierung ausgebildet worden sind.A further interconnector 5 is arranged on the side of the fuel cell opposite the interconnector 6, in which channels for the supply of a suitable fuel for the operation of the fuel cell by a corresponding one in schematic form Structuring have been trained.
Auf der in das Innere der Hochtemperaturbrennstoffzelle weisenden Oberfläche des Interkonnektors 5, der ebenfalls als bipolare Platte ausgebildet sein kann, ist ein metallisches Netzwerk 4 aus Nickel aufgelegt worden. Die Verbindung des metallischen Netzwerkes 4 mit dem Interkonnektor 5 kann Punktweise durch Schweißen hergestellt worden sein.A metallic network 4 made of nickel has been placed on the surface of the interconnector 5 which faces the interior of the high-temperature fuel cell and which can also be designed as a bipolar plate. The connection of the metallic network 4 to the interconnector 5 may have been made point by point by welding.
Auf der in Richtung auf die Anode 3 weisenden Oberfläche des metallischen Netzwerkes 4 wurde die elektrische Kontaktierung 1 ausgebildet.The electrical contact 1 was formed on the surface of the metallic network 4 pointing in the direction of the anode 3.
Hierzu wurde ein Kompositgemisch aus Nickeloxid undFor this purpose, a composite mixture of nickel oxide and
Magnesiumoxid als metallische Komponente mit Yttriumoxid stabilisiertem Zirkonoxid aufgebracht, wie es im allgemeinen Teil der Beschreibung bereits erläutert worden ist.Magnesium oxide applied as a metallic component with yttrium oxide stabilized zirconium oxide, as has already been explained in the general part of the description.
In Figur 1 ist weiterhin ein Gaskanal zwischen Kathode 3 ' und Interkonnektor 6 für die Zufuhr des für den Betrieb der Brennstoffzelle erforderlichen Oxidati- onsmittels (Sauerstoff oder Luft) gezeigt.FIG. 1 also shows a gas channel between cathode 3 'and interconnector 6 for supplying the oxidizing agent (oxygen or air) required for operating the fuel cell.
Die in Richtung auf das Innere der Hochtemperaturbrennstoffzelle weisende Oberfläche des Interkonnektors 5 wurde vorab mit einer Nickelschutzschicht versehen.The surface of the interconnector 5 pointing in the direction of the interior of the high-temperature fuel cell was previously provided with a protective nickel layer.
Nach dem Auftrag des die bereits erwähnte metallische Komponente und die keramische Komponente enthaltenden Gemisches auf die Oberfläche des metallischen Netzwerkes 4, hier mit einer Schichtdicke von 300 μm und anschließender Montage der Brennstoffzelle, wurde diese normal in Betrieb genommen, so dass bei gleich- zeitiger Erwärmung, also einer quasi Wärmebehandlung das Nickeloxidausgangspulver vollständig zu metallischem Nickel reduziert worden ist. Gleichzeitig wurde mit dem Magnesiumoxid ein haftfester Diffusionsverbund zwischen Anode 3, metallischem Netzwerk 4 und der elektrischen Kontaktierung 1 sowie auch mit dem die keramische Komponente bildenden stabilisierten Zirkonoxid an den jeweiligen Grenzflächen ausgebildet.After the mixture containing the aforementioned metallic component and the ceramic component had been applied to the surface of the metallic network 4, here with a layer thickness of 300 μm and subsequent assembly of the fuel cell, it was put into operation normally, so that early heating, i.e. a quasi heat treatment, the nickel oxide starting powder has been completely reduced to metallic nickel. At the same time, an adherent, diffusion bond was formed with the magnesium oxide between the anode 3, the metallic network 4 and the electrical contact 1 and also with the stabilized zirconium oxide forming the ceramic component at the respective interfaces.
So kann bei ausreichend hoher elektrischer Leitfähigkeit zwischen metallischem Netzwerk 4 und Anode 3 und dementsprechend auch zum Interkonnektor 5 eine ausreichend hohe elektrische Leitfähigkeit bei gleich- zeitig sicherem Schutz vor einer unerwünschten insbesondere die elektrische Leitfähigkeit reduzierenden Oxidschichtbildung innerhalb dieses kritischen Bereiches erreicht werden. Thus, with a sufficiently high electrical conductivity between the metallic network 4 and the anode 3 and, accordingly, also to the interconnector 5, a sufficiently high electrical conductivity can be achieved within this critical range, while at the same time providing reliable protection against undesired oxide layer formation, which in particular reduces the electrical conductivity.

Claims

Patentansprüche claims
1. Elektrische Kontaktierung für Hochtemperaturbrennstoffzellen, die als Komposit aus einer metallischen Komponente und einer keramischen Komponente gebildet ist.1. Electrical contacting for high-temperature fuel cells, which is formed as a composite of a metallic component and a ceramic component.
2. Kontaktierung nach Anspruch 1, dadurch gekennzeichnet, dass die metallische Komponente mit mindestens einem Metalloxid gebildet ist.2. Contact according to claim 1, characterized in that the metallic component is formed with at least one metal oxide.
3. Kontaktierung nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass die keramische Kom- ponente für Sauerstoffionen leitend ist.3. Contact according to claim 1 or 2, characterized in that the ceramic component is conductive for oxygen ions.
4. Kontaktierung nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass in der metallischen Komponente Nickel, Kupfer oder eine Legierung dieser Elemente enthalten ist .4. Contacting according to one of the preceding claims, characterized in that the metallic component contains nickel, copper or an alloy of these elements.
5. Kontaktierung nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass in der metallischen Komponente NiO, CuO und/oder MgO enthalten ist/sind.5. Contacting according to one of the preceding claims, characterized in that NiO, CuO and / or MgO is / are contained in the metallic component.
6. Kontaktierung nach einem der vorhergehenden An- Sprüche, dadurch gekennzeichnet, dass in der keramischen Komponente Zr02 und/oder Ce02 enthalten ist/sind.6. Contacting according to one of the preceding claims, characterized in that Zr0 2 and / or Ce0 2 is / are contained in the ceramic component.
7. Kontaktierung nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die metal- lische Komponente mit 80 bis 100 Masse-% und die keramische Komponente mit 0 bis 20 Masse-% enthalten ist. 7. Contacting according to one of the preceding claims, characterized in that the metallic component with 80 to 100 mass% and the ceramic component with 0 to 20 mass% is included.
8. Kontaktierung nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass stabilisiertes Zr02 enthalten ist .8. Contacting according to one of the preceding claims, characterized in that stabilized Zr0 2 is included.
9. Kontaktierung nach einem der vorhergehenden An- Sprüche, dadurch gekennzeichnet, dass dotiertes Ce02 enthalten ist .9. Contacting according to one of the preceding claims, characterized in that doped Ce0 2 is included.
10. Kontaktierung nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die metallische Komponente in hochdispergierter Form ent- halten ist.10. Contacting according to one of the preceding claims, characterized in that the metallic component is contained in highly dispersed form.
11. Kontaktierung nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass sie eine Dicke von 2 bis 500 μm aufweist.11. Contact according to one of the preceding claims, characterized in that it has a thickness of 2 to 500 microns.
12. Kontaktierung nach einem der vorhergehenden An- Sprüche, dadurch gekennzeichnet, dass die Kontaktierung (1) an der Oberfläche eines metallischen Netzwerkes (4) , das zwischen einer Anode und einem Interkonnektor (5) einer Hochtemperaturbrennstoffzelle angeordnet ist, ausgebildet ist.12. Contacting according to one of the preceding claims, characterized in that the contacting (1) is formed on the surface of a metallic network (4) which is arranged between an anode and an interconnector (5) of a high-temperature fuel cell.
13. Kontaktierung nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die Kontaktierung (1) flächig auf der Oberfläche der Anode (3) und/oder eines Interkonnektors (5) ei- ner Hochtemperaturbrennstoffzelle ausgebildet ist . 13. Contact according to one of the preceding claims, characterized in that the contact (1) is formed flat on the surface of the anode (3) and / or an interconnector (5) of a high-temperature fuel cell.
14. Verfahren zur Herstellung einer elektrischen Kontaktierung für Hochtemperaturbrennstoffzellen bei dem, an/zwischen elektrisch leitenden Elementen, bei dem eine metallische und eine kera- mische Komponente enthaltendes Gemisch aufgebracht , anschließend eine Wärmebehandlung bei Zufuhr eines Reduktionsmittels bei gleichzeitiger Aushär- tung der Kontaktierung (1) durchgeführt und durch eine zumindest teilweise Reduktion eines Metalloxides zu reinem Metall oder einer Metall- legierung erreicht werden.14. Method for producing an electrical contact for high-temperature fuel cells in the case of, on / between electrically conductive elements, in which a mixture containing a metallic and a ceramic component is applied, followed by a heat treatment with the addition of a reducing agent with simultaneous hardening of the contact (1 ) and can be achieved by at least partially reducing a metal oxide to pure metal or a metal alloy.
15. Verfahren nach Anspruch 14, dadurch gekennzeichnet, dass die Wärmebehandlung und Reduktion in situ innerhalb der Hochtemperaturbrennstoffzelle durchgeführt werden.15. The method according to claim 14, characterized in that the heat treatment and reduction are carried out in situ within the high-temperature fuel cell.
16. Verfahren nach Anspruch 14 oder 15, dadurch gekennzeichnet, dass bei der Wärmebehandlung an den Grenzflächen der miteinander zu kontaktierenden elektrisch leitenden Elemente ein haftfester Diffusionsverbund ausgebildet wird.16. The method according to claim 14 or 15, characterized in that an adhesive diffusion bond is formed during the heat treatment at the interfaces of the electrically conductive elements to be contacted.
17. Verfahren nach einem der Ansprüche 14 bis 16, dadurch gekennzeichnet, dass ein Gemisch bestehend aus pulverfδrmiger metallischer Komponente und keramischer Komponente mit einem Binder aufgetragen wird.17. The method according to any one of claims 14 to 16, characterized in that a mixture consisting of powdery metallic component and ceramic component is applied with a binder.
18. Verfahren nach einem der Ansprüche 14 bis 17, dadurch gekennzeichnet, dass das Gemisch in pastöser Form aufgetragen wird. 18. The method according to any one of claims 14 to 17, characterized in that the mixture is applied in pasty form.
9. Verfahren nach einem der Ansprüche 14 bis 18, dadurch gekennzeichnet, dass das Gemisch durch ein Nasspulverspritzverfahren, durch Siebdruck oder durch Aufrollen aufgetragen wird. 9. The method according to any one of claims 14 to 18, characterized in that the mixture is applied by a wet powder spraying process, by screen printing or by rolling up.
EP04762750A 2003-09-08 2004-08-30 Electric contact for high-temperature fuel cells and methods for the production of said contact Withdrawn EP1665429A2 (en)

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DE10342161A DE10342161A1 (en) 2003-09-08 2003-09-08 Electrical contacting for high-temperature fuel cells and method for producing such a contact
PCT/DE2004/001964 WO2005027246A2 (en) 2003-09-08 2004-08-30 Electric contact for high-temperature fuel cells and methods for the production of said contact

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