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WO2001078174A1 - Fuel cell with a diffusion layer - Google Patents

Fuel cell with a diffusion layer Download PDF

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Publication number
WO2001078174A1
WO2001078174A1 PCT/DE2001/001077 DE0101077W WO0178174A1 WO 2001078174 A1 WO2001078174 A1 WO 2001078174A1 DE 0101077 W DE0101077 W DE 0101077W WO 0178174 A1 WO0178174 A1 WO 0178174A1
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Prior art keywords
diffusion layer
fuel cell
fuel
anode
methanol
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Ceased
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PCT/DE2001/001077
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German (de)
French (fr)
Inventor
Hendrik Dohle
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Forschungszentrum Juelich GmbH
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Forschungszentrum Juelich GmbH
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Publication of WO2001078174A1 publication Critical patent/WO2001078174A1/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • 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
    • H01M8/1009—Fuel cells with solid electrolytes with one of the reactants being liquid, solid or liquid-charged
    • 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 fuel cell with a diffusion layer, in which a direct electrochemical conversion of a fuel into electricity takes place, in particular a low-temperature fuel cell.
  • DMFC direct methanol fuel cell
  • Such a fuel cell has an anode compartment with an anode, an electrolyte membrane and a cathode compartment with a cathode.
  • the cathode becomes an oxidizing agent, e.g. B. air and the anode is a fuel through the anode compartment, for. B. hydrogen or methanol.
  • the cathode and anode of a fuel cell generally have a continuous porosity so that the two operating media, oxidizing agent and fuel, can be fed to the active areas of the electrodes.
  • the electrodes typically have a catalyst layer in which the actual electrochemically catalyzed processes take place.
  • the supplied fuel is depleted on the anode side, in the case of a methanol fuel cell a methanol / water mixture, during operation along the anode.
  • the following disadvantages occur.
  • the high concentration of methanol at the inlet of the anode space causes an increased permeation of the methanol through the electrolyte membrane and thus leads to the formation of a mixed potential on the cathode side. This regularly has a negative impact on fuel efficiency.
  • the low methanol concentrations at the outlet of the anode compartment can lead to diffusion overvoltages. This also has a negative impact on the efficiency of the fuel cell.
  • the object of the invention is to create a fuel cell which reduces the above-mentioned disadvantages of the varying fuel concentrations along the anode during operation and regularly achieves an improved efficiency.
  • the methanol fuel cell according to the invention comprises an anode space with an anode, a diffusion layer being arranged on the anode.
  • the diffusion layer of the fuel cell according to the invention has different diffusivities for the
  • Different diffusivity for the fuel means that the particle flow of the fuel from the free anode space through the diffusion layer to the electrode takes on different values.
  • this is achieved by a diffusion layer with different thickness. It was found within the scope of the invention that this changes the distance the fuel travels through the porous material of the diffusion layer. If the layer thickness of the porous material is increased, the path length also increases. The particle flow decreases accordingly.
  • the concentration of the fuel can be influenced directly at the anodic catalyst layer by varying the diffusivity of the diffusion layer.
  • the thickness of the diffusion layer decreases continuously from the fuel inlet side to the fuel outlet side.
  • the high initial concentrations in the free anode space at the fuel inlet are buffered or reduced by a thick diffusion layer directly at the anode.
  • the low content of fuel on the fuel outlet side is led to the anode almost unchanged by a thin diffusion layer there.
  • Such a diffusion layer regularly results in a more uniform concentration profile directly at the anode, in contrast to that in the free anode space.
  • a methanol fuel cell according to the invention is produced as a low-temperature fuel cell with a diffusion layer that has different diffusivities as follows.
  • the diffusion layer is applied to an electrical conductor that is in the form of a graphite fabric.
  • a mixture of 15% PTFE and 85% activated carbon (eg XC 72) is weighed out, mixed, diluted with a water / isopropanol mixture and thus produced a sprayable form.
  • the sprayable mixture is then sprayed onto the current conductor, the coverage usually varying from approximately 4 to 12 mg / cm 2 .
  • This diffusion layer for a methanol fuel cell comprises porous material and is permeable to methanol, water and CO 2 .
  • the fuel reaches the anode from the free anode space through the diffusion layer, where it can react on the catalyst layer.
  • the resulting reaction products, water and CO 2 can diffuse back into the anode compartment through the diffusion layer.
  • a suitable diffusion layer typically comprises PTFE and activated carbon, where the PTFE can be present in the form of fine-grain powder or as a suspension when the diffusion layer is produced.
  • a different diffusivity in the diffusion layer alternatively results from different porosities or also from different compositions within the diffusion layer. The proportion of PTFE in the mixture has a significant influence on the diffusivity of the diffusion layer.

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

Abstract

A fuel cell, wherein the diffusion layer used for the distribution of fuel to the anodic catalyst layer exhibits various diffusivities created advantageously by decreasing the thickness of said layer in the direction of the fuel flow. The inventive diffusion layer provides a regular, more uniform fuel concentration profile directly at the anode as opposed to that in the free anode region. The diffusion layer can be used advantageously in a methanol fuel cell.

Description

e s c h r e i b u n g e s c h r e i b u n g

Brennstoffzelle mit DiffusionsschichtFuel cell with diffusion layer

Die Erfindung betrifft eine Brennstoffzelle mit einer Diffusionsschicht, in der eine direkte elektrochemische Umsetzung eines Brennstoffs in Elektrizität stattfindet, insbesondere eine Niedertemperatur-Brennstoffzelle .The invention relates to a fuel cell with a diffusion layer, in which a direct electrochemical conversion of a fuel into electricity takes place, in particular a low-temperature fuel cell.

Ein typisches Beispiel für eine solche Niedertemperatur-Brennstoffzelle ist die Direkt-Methanol-Brennstoff- zelle (DMFC), bei der Methanol bei niedriger Temperatur direkt verströmt wird.A typical example of such a low-temperature fuel cell is the direct methanol fuel cell (DMFC), in which methanol is emitted directly at a low temperature.

Eine derartige Brennstoffzelle weist einen Anodenraum mit einer Anode, eine Elektrolytmembran und einen Kathodenraum mit einer Kathode auf. Der Kathode wird durch den Kathodenraum ein Oxidationsmittel, z. B. Luft und der Anode wird durch den Anodenraum ein Brennstoff, z. B. Wasserstoff oder Methanol zugeführt. Kathode und Anode einer Brennstoffzelle weisen in der Regel eine durchgehende Porosität auf, damit die beiden Betriebsmittel Oxidationsmittel und Brennstoff den aktiven Be- reichen der Elektroden zugeführt werden können. Ferner weisen die Elektroden typischerweise eine Katalysatorschicht auf, in der die eigentlichen elektrochemisch katalysierten Vorgänge stattfinden. Durch die oben beschriebene Konstruktion bedingt wird anodenseitig der zugefuhrte Brennstoff, im Fall einer Methanol-Brennstoffzelle ein Methanol/Wassergemisch, wahrend des Betriebs entlang der Anode abgereichert . Das bedeutet, daß der Brennstoff mit einem hohen Methanolgehalt in den Anodenraum eingeleitet wird und sich m Stromungsrichtung entlang der Anode abreichert. Anschließend tritt er mit einem geringen Methanolgehalt wieder aus dem Anodenraum aus. Bei den bisherigen Kon- struktionen einer Methanol-Brennstof zelle treten dabei folgende Nachteile auf. Die hohe Methanolkonzentration am Einlaß des Anodenraums bewirkt eine erhöhte Permea- tion des Methanols durch die Elektrolytmembran und fuhrt dadurch auf der Kathodenseite zur Bildung eines Mischpotentials. Dies wirkt sich regelmäßig negativ auf die Brennstoffeffizienz aus. Dem gegenüber können die geringen Methanolkonzentrationen am Auslaß des Anodenraums zu Diffusionsuberspannungen fuhren. Auch dies wirkt sich negativ auf den Wirkungsgrad der Brennstoff- zelle aus.Such a fuel cell has an anode compartment with an anode, an electrolyte membrane and a cathode compartment with a cathode. The cathode becomes an oxidizing agent, e.g. B. air and the anode is a fuel through the anode compartment, for. B. hydrogen or methanol. The cathode and anode of a fuel cell generally have a continuous porosity so that the two operating media, oxidizing agent and fuel, can be fed to the active areas of the electrodes. Furthermore, the electrodes typically have a catalyst layer in which the actual electrochemically catalyzed processes take place. Due to the construction described above, the supplied fuel is depleted on the anode side, in the case of a methanol fuel cell a methanol / water mixture, during operation along the anode. This means that the fuel with a high methanol content is introduced into the anode compartment and is depleted in the direction of flow along the anode. It then emerges from the anode compartment with a low methanol content. In the previous designs of a methanol fuel cell, the following disadvantages occur. The high concentration of methanol at the inlet of the anode space causes an increased permeation of the methanol through the electrolyte membrane and thus leads to the formation of a mixed potential on the cathode side. This regularly has a negative impact on fuel efficiency. In contrast, the low methanol concentrations at the outlet of the anode compartment can lead to diffusion overvoltages. This also has a negative impact on the efficiency of the fuel cell.

Aufgabe der Erfindung ist es, eine Brennstoffzelle zu schaffen, die die oben genannten Nachteile der variierenden Brennstoffkonzentrationen entlang der Anode wah- rend des Betriebs verringert und regelmäßig einen verbesserten Wirkungsgrad erzielt.The object of the invention is to create a fuel cell which reduces the above-mentioned disadvantages of the varying fuel concentrations along the anode during operation and regularly achieves an improved efficiency.

Die Aufgabe wird gelost durch eine Brennstoffzelle nach Anspruch 1. Vorteilhafte Ausgestaltungen ergeDen sich aus den darauf ruckbezogenen Ansprüchen. Dazu umfaßt die erfindungsgemäße Methanol-Brennstoffzelle einen Anodenraum mit einer Anode, wobei auf der Anode eine Diffusionsschicht angeordnet ist.The object is achieved by a fuel cell according to claim 1. Advantageous refinements emerge from the claims which refer to it jerkily. For this purpose, the methanol fuel cell according to the invention comprises an anode space with an anode, a diffusion layer being arranged on the anode.

Die Diffusionsschicht der erfindungsgemaßen Brennstoff- zelle weist unterschiedliche Diffusivitaten für denThe diffusion layer of the fuel cell according to the invention has different diffusivities for the

Brennstoff auf. Diese treten insbesondere entlang der Elektrode, vorzugsweise in Richtung von Brennstoffein- laßseite zur Brennstoffauslaßseite auf. Unter unterschiedlicher Diffusivitat für den Brennstoff ist zu verstehen, daß der Teilchenstrom des Brennstoffes aus dem freien Anodenraum durch die Diffusionsschicht zur Elektrode unterschiedliche Werte annimmt. In einer vorteilhaften Ausgestaltung der Erfindung wird dies durch eine Diffusionsschicht mit unterschiedlicher Dicke rea- lisiert. Im Rahmen der Erfindung wurde gefunden, daß sich dadurch die Weglange, die der Brennstoff durch das poröse Material der Diffusionsschicht zurücklegt, ändert. Wird die Schichtdicke des porösen Materials erhöht, erhöht sich auch die Weglange. Der Teilchenstrom nimmt entsprechend ab.Fuel on. These occur in particular along the electrode, preferably in the direction from the fuel inlet side to the fuel outlet side. Different diffusivity for the fuel means that the particle flow of the fuel from the free anode space through the diffusion layer to the electrode takes on different values. In an advantageous embodiment of the invention, this is achieved by a diffusion layer with different thickness. It was found within the scope of the invention that this changes the distance the fuel travels through the porous material of the diffusion layer. If the layer thickness of the porous material is increased, the path length also increases. The particle flow decreases accordingly.

Durch die Variation der Diffusivitat der Diffusionsschicht kann die Konzentration des Brennstoffes direkt an der anodischen Katalysatorschicht beeinflußt werden.The concentration of the fuel can be influenced directly at the anodic catalyst layer by varying the diffusivity of the diffusion layer.

In einer vorteilhaften Ausgestaltung nimmt die Dicke der Diffusionsschicht von der Brennstoffeinlaßseite zur Brennstoffauslaßseite kontinuierlich ab. Die hohen Anfangskonzentrationen im freien Anodenraum am Brennstoffeinlaß werden durch eine dicke Diffusionsschicht direkt an der Anode abgepuffert, bzw. redu- ziert. Gleichzeitig wird der geringe Gehalt an Brennstoff an der Brennstoffauslaßseite durch eine dünne Diffusionsschicht dort nahezu unverändert an die Anode gefuhrt . Durch eine solche Diffusionsschicht wird regelmäßig ein gleichförmigeres Konzentrationsprofil direkt an der Anode im Gegensatz zu dem im freien Anodenraum erzielt.In an advantageous embodiment, the thickness of the diffusion layer decreases continuously from the fuel inlet side to the fuel outlet side. The high initial concentrations in the free anode space at the fuel inlet are buffered or reduced by a thick diffusion layer directly at the anode. At the same time, the low content of fuel on the fuel outlet side is led to the anode almost unchanged by a thin diffusion layer there. Such a diffusion layer regularly results in a more uniform concentration profile directly at the anode, in contrast to that in the free anode space.

In einem Ausfuhrungsbeispiel wird eine erfindungsgemaße Methanol-Brennstoffzelle als Niedertemperatur-Brennstoffzelle mit einer Diffusionsschicht, die unterschiedliche Diffusivitaten aufweist, wie folgt hergestellt. Dabei wird die Diffusionsschicht auf einen Stromleiter, der in Form eines Graphitgewebes vorliegt, aufgebracht. Eine Mischung aus 15 % PTFE und 85 % Aktivkohle (z. B. XC 72) wird ausgewogen, gemischt, mit einem Wasser/Iso- propanol Gemisch verdünnt und so eine spritzfahige Form erzeugt. Die spritzfahige Mischung wird anschließend auf den Stromleiter aufgesprüht, wobei die Belegung üblicherweise von ca. 4 bis 12 mg/cm2 variiert.In an exemplary embodiment, a methanol fuel cell according to the invention is produced as a low-temperature fuel cell with a diffusion layer that has different diffusivities as follows. The diffusion layer is applied to an electrical conductor that is in the form of a graphite fabric. A mixture of 15% PTFE and 85% activated carbon (eg XC 72) is weighed out, mixed, diluted with a water / isopropanol mixture and thus produced a sprayable form. The sprayable mixture is then sprayed onto the current conductor, the coverage usually varying from approximately 4 to 12 mg / cm 2 .

Diese Diffusionsschicht für eine Methanol-Brennstoff- zelle umfaßt poröses Material und ist durchlassig für Methanol, Wasser und C02. Der Brennstoff gelangt aus dem freien Anodenraum durch die Diffusionsschicht an die Anode, wo er an der Katalysatorschicht reagieren kann. Die entstehenden Reaktionsprodukte, Wasser und CO2, können durch die Diffusionsschicht zurück in den Anodenraum diffundieren. Eine geeignete Diffusionsschicht umfaßt typischerweise PTFE und Aktivkohle, wobei das PTFE bei der Herstellung der Diffusionsschicht in Form von feinkornigem Pulver oder auch als Suspen- sion vorliegen kann. Eine unterschiedliche Diffusivitat in der Diffusionsschicht ergibt sich alternativ auch durch unterschiedliche Porositäten oder auch durch unterschiedliche Zusammensetzungen innerhalb der Diffusionsschicht . So hat der Anteil an PTFE m der Mischung einen deutlichen Einfluß auf die Diffusivitat der Diffusionsschicht .This diffusion layer for a methanol fuel cell comprises porous material and is permeable to methanol, water and CO 2 . The fuel reaches the anode from the free anode space through the diffusion layer, where it can react on the catalyst layer. The resulting reaction products, water and CO 2 , can diffuse back into the anode compartment through the diffusion layer. A suitable diffusion layer typically comprises PTFE and activated carbon, where the PTFE can be present in the form of fine-grain powder or as a suspension when the diffusion layer is produced. A different diffusivity in the diffusion layer alternatively results from different porosities or also from different compositions within the diffusion layer. The proportion of PTFE in the mixture has a significant influence on the diffusivity of the diffusion layer.

Möglich ist aber auch jegliche Kombination dieser drei Alternativen, so beispielsweise unterschiedliche Zusam- mensetzungen kombiniert mit unterschiedlichen Schichtdicken . However, any combination of these three alternatives is also possible, for example different compositions combined with different layer thicknesses.

Claims

P a t e n t a n s p r ü c h eP a t e n t a n s r u c h e 1) Brennstoffzelle umfassend einen Anodenraum mit einer Anode, sowie einer auf der Anode angeordneten1) Fuel cell comprising an anode compartment with an anode and one arranged on the anode Dif fusionsschicht , dadurch ge kennze ichnet , daß die Dif fusionsschicht unterschiedliche Dif fu- sivitaten aufweist.Diffusion layer, characterized in that the diffusion layer has different diffusions. Brennstoffzelle nach vorhergehendem Anspruch, dadurch gekennzeichnet, daß die Diffusionsschicht eine variierende Dicke aufweist .Fuel cell according to the preceding claim, characterized in that the diffusion layer has a varying thickness. Brennstoffzelle nach einem der vorhergehendenFuel cell according to one of the preceding Ansprüche, dadurch gekennzeichnet, daß die Dicke der Diffusionsschicht um wenigstensClaims, characterized in that the thickness of the diffusion layer by at least 10 % variiert.10% varies. Brennstoffzelle nach einem der vorhergehendemFuel cell according to one of the preceding Ansprüche, dadurch gekennzeichnet , daß die Dicke der Dif fusionsschicht entlang derClaims, characterized in that the thickness of the diffusion layer along the Anode variiert.Anode varies. Brennstoffzelle nach einem der vorhergehendemFuel cell according to one of the preceding Ansprüche, dadurch gekennzeichnet , daß die Dicke der Dif fusionsschicht entlang der Stromungsrichtung des Brennstoffs an der Anode abnimmt .Claims, characterized in that the thickness of the diffusion layer along the Flow direction of the fuel at the anode decreases. 6 ) Brennstoffzelle nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, daß die Diffusionsschicht unterschiedliche Porositäten aufweist.6) Fuel cell according to one of the preceding claims, characterized in that the diffusion layer has different porosities. 7) Brennstoffzelle nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, daß die Diffusionsschicht unterschiedliche Zusammensetzungen innerhalb der Diffusionsschicht auf- weist.7) Fuel cell according to one of the preceding claims, characterized in that the diffusion layer has different compositions within the diffusion layer. 8) Methanol-Brennstoffzelle als Brennstoffzelle nach einem der vorhergehenden Ansprüche. 8) methanol fuel cell as a fuel cell according to one of the preceding claims.
PCT/DE2001/001077 2000-04-05 2001-03-17 Fuel cell with a diffusion layer Ceased WO2001078174A1 (en)

Applications Claiming Priority (2)

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DE10016820A DE10016820A1 (en) 2000-04-05 2000-04-05 Fuel cell with diffusion layer
DE10016820.5 2000-04-05

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS60189868A (en) * 1984-03-12 1985-09-27 Fuji Electric Corp Res & Dev Ltd Reaction fluid feed structure to fuel cell electrode layer
WO1996035003A1 (en) * 1995-05-01 1996-11-07 E.I. Du Pont De Nemours And Company Electrochemical cell having a self-regulating gas diffusion layer
US5840438A (en) * 1995-08-25 1998-11-24 Ballard Power Systems Inc. Electrochemical fuel cell with an electrode substrate having an in-plane nonuniform structure for control of reactant and product transport
DE19838814A1 (en) * 1997-08-28 1999-03-04 Fuji Electric Co Ltd Fuel cell with gas stream path for addition of water

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS60189868A (en) * 1984-03-12 1985-09-27 Fuji Electric Corp Res & Dev Ltd Reaction fluid feed structure to fuel cell electrode layer
WO1996035003A1 (en) * 1995-05-01 1996-11-07 E.I. Du Pont De Nemours And Company Electrochemical cell having a self-regulating gas diffusion layer
US5840438A (en) * 1995-08-25 1998-11-24 Ballard Power Systems Inc. Electrochemical fuel cell with an electrode substrate having an in-plane nonuniform structure for control of reactant and product transport
DE19838814A1 (en) * 1997-08-28 1999-03-04 Fuji Electric Co Ltd Fuel cell with gas stream path for addition of water

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
PATENT ABSTRACTS OF JAPAN vol. 010, no. 032 (E - 379) 7 February 1986 (1986-02-07) *

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