WO2022002932A1 - Couche de diffusion gazeuse destinée à une pile à combustible et dotée de propriétés variables le long de l'étendue d'une surface - Google Patents

Couche de diffusion gazeuse destinée à une pile à combustible et dotée de propriétés variables le long de l'étendue d'une surface Download PDF

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Publication number
WO2022002932A1
WO2022002932A1 PCT/EP2021/067839 EP2021067839W WO2022002932A1 WO 2022002932 A1 WO2022002932 A1 WO 2022002932A1 EP 2021067839 W EP2021067839 W EP 2021067839W WO 2022002932 A1 WO2022002932 A1 WO 2022002932A1
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WO
WIPO (PCT)
Prior art keywords
gas diffusion
layer
diffusion layer
fuel cell
extent
Prior art date
Application number
PCT/EP2021/067839
Other languages
German (de)
English (en)
Inventor
Harald Bauer
Original Assignee
Robert Bosch Gmbh
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 Robert Bosch Gmbh filed Critical Robert Bosch Gmbh
Priority to EP21740438.3A priority Critical patent/EP4176477A1/fr
Publication of WO2022002932A1 publication Critical patent/WO2022002932A1/fr

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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
    • 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
    • H01M4/92—Metals of platinum group
    • H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
    • H01M4/926—Metals of platinum group supported on carriers, e.g. powder carriers on carbon or graphite
    • 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
    • H01M8/0234—Carbonaceous material
    • 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 present invention relates to a gas diffusion layer for a fuel cell, a fuel cell with such a gas diffusion layer and a method for producing a gas diffusion layer.
  • PEM fuel cell stacks usually comprise a plurality of stacked fuel cells, each of which has a hydrophilic membrane with a catalyst layer on both sides and adjoining hydrophobized gas diffusion layers which are in contact with a flow field for distributing educts. Due to the gas diffusion layers, the membrane can, on the one hand, have a certain humidity and, on the other hand, gaseous starting materials can reach the catalyst layer of the membrane in the opposite direction.
  • hydrogen reacts with oxygen and an electrical voltage is provided at the electrodes of the fuel cells. This creates water at the cathode. If not all of the water vapor is removed, water can condense under unfavorable conditions.
  • the fuel cell in question could be flooded locally as a result and the educts can no longer come into contact with the catalyst, at least locally, due to the water barrier created as a result.
  • the performance of the cell is reduced locally and thus the overall performance of the system is reduced.
  • Such flooded areas could be zones or starting points for degradation effects, such as corrosion.
  • gas diffusion layers made of a dense hydrophobic particulate layer can be arranged on a carbon fiber fleece and placed between the flow field and the membrane with its catalyst layer, so that gas and water vapor are always allowed through and still sufficient liquid water is held on the membrane, with additional required or excess liquid water is passed through.
  • the gas diffusion layers can also be used as a gas diffusion electrode for diverting the generated current.
  • Educts that are fed to the membrane via the flow fields and via the gas diffusion layer always require a certain pressure to overcome the flow resistance along the entire flow path.
  • the local pressure over the membrane is not constant over the area even with constant operating parameters.
  • a method is known for producing gas diffusion layers, in particular the particulate hydrophobic layer, in which integrally optimized properties are to be set. Either statistically uniform properties (e.g. cracks, pores, holes) are set in the area, or a gradient profile perpendicular to the area is provided.
  • a gas diffusion layer or a gas diffusion electrode must, on the one hand, hold a certain amount of liquid water on the membrane and, on the other hand, remove the excess water produced in the fuel cell process and allow the gaseous reactants to reach the membrane. This can be done with a porous structure.
  • the object of the invention is therefore to propose a gas diffusion layer with which local condensation can be avoided, but at the same time the desired moisture content of the membrane is maintained and the supply of the starting materials is not hindered.
  • a gas diffusion layer for a fuel cell is proposed, the gas diffusion layer having a flat extent and a layer thickness measured perpendicular to the flat extent, and the gas diffusion layer having predetermined physical properties that include at least one permeability and one hydrophobicity. According to the invention, it is provided that at least one of the physical properties changes from an initial value in an initial area to an end value in an end area spaced therefrom in at least one direction along the two-dimensional extent.
  • a core of the invention is therefore not to keep the determining physical properties of the gas diffusion layer with regard to the accumulating water constant in the area of the respective fuel cells, i.e. in the cell plane perpendicular to a stacking direction. They therefore change essentially with the pressure profile along the flow field, so that, despite the pressure differences, the functionality of the gas diffusion layer, in particular for the retention capacity of liquid water and the permeability of gaseous educts, is almost the same everywhere.
  • the gas diffusion layer can thus be loaded equally everywhere in order to achieve high performance and low degradation with high power density in a stacked system.
  • the physical properties include at least the permeability and the hydrophobicity.
  • the hydrophobicity can have a comparatively low value where there is still no water. In an area opposite this, in which the greatest amount of water can be expected, it makes sense to select a higher hydrophobicity.
  • the hydrophobicity can be achieved, for example, by a content of water-repellent material incorporated therein that changes along the extent of the surface. This material can include, for example, PTFE.
  • the use of the hydrophobic material can prevent or reduce the excess water.
  • the permeability which can be controlled, for example, by the porosity of the gas diffusion layer, can also allow adaptation to the pressure curve.
  • a lower permeability can be provided than in an area with low pressure.
  • a uniform volume flow can be achieved over the entire surface of the gas diffusion layer.
  • an applied microporous layer its thickness can be influenced, which among other things also leads to a changing local depth of penetration into the carrier layer.
  • the microporous layer could be applied locally differently by means of multi-layer printing.
  • the electrical contact resistance, the electrical volume resistance, the wetting angle and the hydrophobicity can be adjusted, for example by using different local densities or contents of a hydrophobizing material.
  • the microporous layer could be printed onto the carrier layer, with different pore shapes and thus variable properties being able to be produced by printing different areas with different contents of hydrophobing material, uneven drying, different masses or the like.
  • the porosity can also be adjusted by means of a variable drilling pattern.
  • the gas diffusion layer has a carrier layer made of a fiber fleece, in which at least one of the hydrophobicity, layer thickness and fiber density changes along the two-dimensional extent.
  • the fiber fleece can have carbon fibers.
  • the hydrophobicity can be achieved through the use of a hydrophobic material that can be integrated into the carrier layer. Influencing the layer thickness and the fiber density allow the permeability to be adjusted via the two-dimensional expansion of the gas diffusion layer.
  • the carrier layer could have a base layer on which several sections of nonwovens with different fiber densities are applied next to one another, so that as a result, a fiber density profile can be realized overall.
  • the local thickness and the local fiber density can control the permeability.
  • a local content of a hydrophobizing material changes in or on the carrier layer along the two-dimensional extent.
  • the hydrophobic material such as PTFE, leads to a contact angle of more than 90 ° with respect to water, so that a water-repellent effect is achieved.
  • the local PTFE content or the lack of water-repellent material can be adjusted via the local variation of the properties of the carrier layer.
  • the gas diffusion layer has a microporous layer in which at least one of the hydrophobicity, layer thickness and porosity changes along the two-dimensional extent.
  • a microporous layer can be applied to an aforementioned carrier layer or provided as a separate layer.
  • the microporous layer can comprise one or more layers of carbon allotropes.
  • the hydrophobic properties of the microporous layer can also be influenced by the selection of the carbon allotropes.
  • the microporous layer could also be arranged on the carrier layer and at least partially penetrate into the carrier layer. Consequently, the gas diffusion layer has several layers which form a coherent mechanical unit.
  • the adaptation of the physical properties can be achieved by combining different measures.
  • the carrier layer could have a changing permeability, while for example the microporous layer can have different particle sizes or particle densities over the two-dimensional extent, so that the porosity changes.
  • the carrier layer and / or the microporous layer can each be interspersed with a hydrophobizing material, its density or the local content also being able to change over the two-dimensional extent.
  • the properties of the carrier layer are preferably largely constant and the determining properties such as hydrophobicity and permeability are essentially set by the microporous layer.
  • the properties of both layers are superimposed on the gas diffusion layer from the carrier layer and the microporous layer.
  • the microporous layer can accordingly generate the essential, pressure-dependent adaptations of the gas diffusion layer even with a constant structure of the carrier layer.
  • microporous layer has a penetration depth that changes along the two-dimensional extent. This also allows at least the permeability and hydrophobicity to be set.
  • the gas diffusion layer can consequently have a plurality of sections in which the corresponding physical properties are in each case constant. This can simplify production. However, it is also conceivable that the properties change continuously over the area. An even better adaptation to the pressure curve to be expected could thus be achieved.
  • a simplified approach to generating a gas diffusion layer can be used in which the fuel cell in question is thought to be subdivided into several small fuel cells, each of which has a gas diffusion layer with constant properties. The division could be made into 2, 3, 4, 5, 6, 7, 8, 9, 10 or more individual imaginary fuel cells.
  • the change in the at least one physical property preferably takes place continuously.
  • the invention further relates to a fuel cell with a membrane which is surrounded by two gas diffusion layers according to one of the preceding claims, which are in fluid connection with the flow fields surrounding the gas diffusion layers.
  • the at least one of the physical properties changes as a function of a change in pressure in each case along a flow channel of the flow fields.
  • the pressure change ie in particular the pressure drop, meander-shaped, spiral-shaped, in strips or in some other way over the flow field.
  • the properties of the gas diffusion layer are adapted to this.
  • the starting area is a region of highest pressure from which the flow channel extends to an end region as a region of lowest pressure. The pressure changes along the distance covered and the intended properties of the gas diffusion layer change accordingly.
  • a single web can be produced, for example, by means of film extrusion or compression of the mass with a rolling mill or film drawing, as is the case with lithium-ion battery anodes (carbon particles + binder polymer), which have this profile of properties.
  • a fluidizing agent can be used for the production, or a solvent for a binder polymer or the like dissolved therein.
  • FIG. 1 shows a schematic representation of a fuel cell stack
  • FIG. 2 shows a plan view of a flow field
  • the fuel cell stack 2 in a simplified, schematic sectional illustration.
  • the fuel cell stack 2 is delimited at opposite ends by an end plate 4.
  • An electrical voltage is provided at the end plates 4.
  • a plurality of fuel cells 6 are arranged between the end plates 4, each of which is designed as a membrane electrode assembly (MEA). These have a membrane 8 to which electrodes on both sides 10 connect, each of which has a gas diffusion layer 12 and a catalyst layer 14.
  • the gas diffusion layer 12 could comprise a carrier layer 16 in the form of a carbon fiber fleece with a microporous layer 18 arranged thereon.
  • the carrier layer 16 could have a uniform thickness in a plane parallel to the membrane 8.
  • the microporous layer 18 can partially penetrate into the carrier layer 16. It has, for example, particles from a carbon allotrope, such as graphite.
  • the gas diffusion layer 12 has a layer thickness d which is preferably constant.
  • Bipolar plates 20 are arranged between the individual fuel cells 6, each of which has a flow field 22 on both sides with a series of flow channels 24 which are provided for supplying starting materials and removing reaction products.
  • the flow channels 22 are in fluid connection with the respective membrane 8 via the respective gas diffusion layer 12.
  • the flow field 22 is shown with an exemplary meandering flow channel 24.
  • the explanations relating to the gas diffusion layer 12 are also possible for other shapes of the flow channel 24. These could be designed as a comb distributor, with a band structure, a spiral structure or as a counter-rotating gas distributor.
  • An educt is introduced into the flow field 22 in a first area 26 arranged at the top of the plane of the drawing the second region 28 arranged at the bottom of the plane of the drawing leave the flow field 22.
  • a sufficient initial pressure in the first region 26 is necessary.
  • a certain flow resistance is to be expected.
  • the local pressure of the educt drops continuously from the first area 26 to the second area 28.
  • the final pressure at the end of the flow channel 24 in the second region 28 is then more or less clearly below the initial pressure. Due to the concise pressure profile, excessive condensation could occur locally on the membrane 8, where the pressure and temperature are below a saturated steam curve. In order to avoid this, so that a free flow of educts to the membrane is possible, the same pressure would have to be set everywhere at a constant temperature within a fuel cell via the two-dimensional extension of the flow field 22. Due to the flow resistance, this is only conceivable for very small fuel cells with a generous flow field under laboratory conditions.
  • the gas diffusion layer 12 is designed in such a way that the physical properties of the gas diffusion layer that determine the water balance and permeability are not constant in the area of the respective fuel cells, but are adapted to the pressure profile of the flow field 22. They change with the pressure profile along the flow channel 24. Where a lot of water could condense out, it is advantageous to set the hydrophobicity of the gas diffusion layer 12 to be particularly high. In places where little or no water could condense out, a lower level of water repellency would make sense. In locations with high pressure, the gas diffusion layer 12 could be less gas-permeable, i.e. permeable, than in locations with lower pressure. Overall, the retention capacity of liquid water and the permeability of gaseous starting materials can then be approximately the same everywhere along the gas diffusion layer 12, despite the pressure differences.
  • FIG. 3 A simplified example of a gas diffusion layer 12a is shown in FIG. 3.
  • the areal extent can be seen here, through which flow paths 30 lie in a direction vertical to the areal extent.
  • the flow paths 30 could be visible as perforation openings, for example.
  • the gas diffusion layer 12a can overall have a porous surface, so that the illustration in FIG. 3 is to be understood schematically.
  • gas diffusion layers made of a solid material, which are provided with individual bores 30, could also be used.
  • the gas diffusion layer 12a has a higher density of flow paths 30 at the upper end in the plane of the drawing, which consequently results in a higher density Porosity or a higher permeability leads.
  • the density of flow paths 30 is significantly lower.
  • the permeability changes either steadily, ie continuously, or in stages.
  • the lower end can be placed on the first region 26 of the flow field 22.
  • This area of the gas diffusion layer 12a is called the starting area 27 here.
  • the upper end which here represents an end area 29, should, however, be placed on the second area 28.
  • the permeability can largely follow inversely proportional to the pressure in the flow channel 24, so that an at least largely uniform volume flow is established over the entire flow channel 24 through the gas diffusion layer 12 to the membrane 8.
  • the course can run in strips from the starting area 27 to the end area 29. In finer gradations, the course could also be set in a meandering shape or at least continuously in one plane direction.
  • variable permeability could also be achieved by a changing depth of penetration of the microporous layer 18 shown in FIG. 1 into the carrier layer 16, as indicated in FIG. 4 with a gas diffusion layer 12b.
  • the depth of penetration of the microporous layer 18 is greater at the upper end in the plane of the drawing than at the lower end. It is conceivable that the thickness of the microporous layer increases with the depth of penetration, so that the gas diffusion layer 12b overall has a constant thickness. With a higher penetration depth, the permeability could be reduced. In the case of the greater penetration depth, the starting area 27 is formed. In the case of the lower penetration depth, the end region 29.
  • FIG. 5 shows a gas diffusion layer 12c into which a hydrophobing material 32 is integrated, for example PTFE.
  • the density or the content of the hydrophobic material 32 changes here along the two-dimensional extent. With the higher density or the higher content, a higher water entry could be countered, so that the density or the content of the hydrophobic material 32 can be selected largely inversely proportional to the pressure curve.
  • the starting area 27 is consequently with the lower content of the hydrophobizing material, the end area 29 with the higher content of the hydrophobizing material 32.
  • a production is also possible that geometrically combines the fiber layer (carbon backbone) and the PTFE particle layer (MPL) with respect to a web and, in total, has the same property profile of previously known gas diffusion layers.
  • This path can also be provided with the property gradient described here.
  • a gas diffusion layer is produced in the same way as a battery carbon anode by coating it with solvent on a base, drying it and then detaching it from the base, then pressing it together as a free-standing web.
  • These layers can contain fibers.
  • not only PTFE is processed, but other binder polymers can be used, which affects the variation in the PTFE content and thus the setting of the

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

Abstract

L'invention concerne une couche de diffusion gazeuse destinée à une pile à combustible, la couche de diffusion gazeuse présentant une étendue surfacique et une épaisseur de couche perpendiculaire à l'étendue surfacique, et la couche de diffusion gazeuse possédant des caractéristiques physiques prédéfinies qui comprennent au moins une perméabilité et hydrophobicité. L'invention prévoit qu'au moins une caractéristique physique d'une valeur initiale dans une zone initiale se transforme en une valeur finale dans une zone finale dans au moins une direction le long de l'étendue surfacique.
PCT/EP2021/067839 2020-07-02 2021-06-29 Couche de diffusion gazeuse destinée à une pile à combustible et dotée de propriétés variables le long de l'étendue d'une surface WO2022002932A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP21740438.3A EP4176477A1 (fr) 2020-07-02 2021-06-29 Couche de diffusion gazeuse destinée à une pile à combustible et dotée de propriétés variables le long de l'étendue d'une surface

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102020208276.6A DE102020208276A1 (de) 2020-07-02 2020-07-02 Gasdiffusionslage für eine Brennstoffzelle mit entlang einer Flächenerstreckung variablen Eigenschaften
DE102020208276.6 2020-07-02

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WO2022002932A1 true WO2022002932A1 (fr) 2022-01-06

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DE (1) DE102020208276A1 (fr)
WO (1) WO2022002932A1 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP4358196A1 (fr) 2022-10-18 2024-04-24 Carl Freudenberg KG Couche de diffusion gazeuse à faible déformabilité plastique et à haute qualité de surface et son procédé de fabrication
EP4358197A1 (fr) 2022-10-18 2024-04-24 Carl Freudenberg KG Couche de diffusion gazeuse pour piles à combustible à gradient de propriété et à faible formabilité plastique et son procédé de production

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102021210461A1 (de) 2021-09-21 2023-03-23 Robert Bosch Gesellschaft mit beschränkter Haftung Gasdiffusionsschicht für eine Brennstoffzelle

Citations (2)

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Publication number Priority date Publication date Assignee Title
US20050233203A1 (en) * 2004-03-15 2005-10-20 Hampden-Smith Mark J Modified carbon products, their use in fluid/gas diffusion layers and similar devices and methods relating to the same
EP2680352A2 (fr) * 2012-06-29 2014-01-01 JNTC Co., Ltd. Substrat de carbone pour couche de diffusion de gaz, couche de diffusion de gaz l'utilisant et électrode pour pile à combustible comprenant ladite couche

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JPH11154523A (ja) 1997-11-19 1999-06-08 Fuji Electric Co Ltd 固体高分子電解質型燃料電池の単セルおよびスタック
DE102018200687A1 (de) 2018-01-17 2019-07-18 Audi Ag Kaskadierter Brennstoffzellenstapel und Brennstoffzellensystem

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20050233203A1 (en) * 2004-03-15 2005-10-20 Hampden-Smith Mark J Modified carbon products, their use in fluid/gas diffusion layers and similar devices and methods relating to the same
EP2680352A2 (fr) * 2012-06-29 2014-01-01 JNTC Co., Ltd. Substrat de carbone pour couche de diffusion de gaz, couche de diffusion de gaz l'utilisant et électrode pour pile à combustible comprenant ladite couche

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP4358196A1 (fr) 2022-10-18 2024-04-24 Carl Freudenberg KG Couche de diffusion gazeuse à faible déformabilité plastique et à haute qualité de surface et son procédé de fabrication
EP4358197A1 (fr) 2022-10-18 2024-04-24 Carl Freudenberg KG Couche de diffusion gazeuse pour piles à combustible à gradient de propriété et à faible formabilité plastique et son procédé de production
WO2024083602A1 (fr) 2022-10-18 2024-04-25 Carl Freudenberg Kg Couche de diffusion gazeuse pour piles à combustible à gradient de propriétés et à faible déformabilité plastique et procédé de production correspondant
WO2024083601A1 (fr) 2022-10-18 2024-04-25 Carl Freudenberg Kg Couche de diffusion gazeuse ayant une faible déformabilité plastique et une qualité de surface élevée et son procédé de fabrication

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