WO2023078819A2 - Assemblage membrane-électrodes pour cellule électrochimique et procédé de fabrication d'un assemblage membrane-électrodes - Google Patents

Assemblage membrane-électrodes pour cellule électrochimique et procédé de fabrication d'un assemblage membrane-électrodes Download PDF

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Publication number
WO2023078819A2
WO2023078819A2 PCT/EP2022/080327 EP2022080327W WO2023078819A2 WO 2023078819 A2 WO2023078819 A2 WO 2023078819A2 EP 2022080327 W EP2022080327 W EP 2022080327W WO 2023078819 A2 WO2023078819 A2 WO 2023078819A2
Authority
WO
WIPO (PCT)
Prior art keywords
membrane
recesses
electrode
frame structure
film
Prior art date
Application number
PCT/EP2022/080327
Other languages
German (de)
English (en)
Other versions
WO2023078819A3 (fr
Inventor
Patrick Schwamm
Juergen Herold
Florian Dirscherl
Robert Landvogt
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
Publication of WO2023078819A2 publication Critical patent/WO2023078819A2/fr
Publication of WO2023078819A3 publication Critical patent/WO2023078819A3/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
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
    • 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
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0273—Sealing or supporting means around electrodes, matrices or membranes with sealing or supporting means in the form of a frame
    • 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
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0286—Processes for forming seals
    • 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
    • H01M2008/1095—Fuel cells with polymeric electrolytes

Definitions

  • Membrane-electrode assembly for an electrochemical cell and method of making a membrane-electrode assembly
  • the present invention relates to a membrane-electrode assembly for an electrochemical cell, in particular for a fuel cell, and a method for producing such a membrane-electrode assembly.
  • Fuel cells are electrochemical energy converters in which, for example, hydrogen and oxygen are converted into water, electrical energy and heat.
  • Fuel cells or fuel cell stacks are made up of multipart cells which have membrane electrode units and bipolar plates arranged alternately one above the other.
  • the bipolar plates serve to supply the electrodes with educts and to cool the fuel cell stack.
  • the bipolar plates have a distribution structure that guides fluids containing educt along the electrodes;
  • a bipolar plate usually consists of two distributor plates.
  • the distributor structures serve to guide a cooling fluid along the other distributor structures or within the bipolar plate.
  • the distribution structures are usually designed as channels, through which the different fluids can be conducted.
  • a special type of fuel cell is the polymer electrolyte membrane fuel cell (PEM-FC).
  • PEM-FC polymer electrolyte membrane fuel cell
  • the PEM-FC also includes gas diffusion layers (GDL) in the active area, which delimit the polymer electrolyte membrane (PEM) and the two porous electrodes with a catalyst layer on both sides.
  • GDL gas diffusion layers
  • the PEM, the two electrodes with the catalyst layer and optionally also the two GDLs can form a so-called membrane-electrode unit (MEA) in the active area of the PEM-FC.
  • MEA membrane-electrode unit
  • Two opposing bipolar plates (halves) delimit the MEA on both sides.
  • a fuel cell stack is made up of MEA and bipolar plates arranged alternately one above the other.
  • the fuel in particular hydrogen
  • the oxidizing agent in particular air/oxygen
  • the MEA can be enclosed in a frame-like opening of two foils arranged one on top of the other.
  • the two films of this frame structure are usually made of the same material, for example polyethylene naphthalate (PEN).
  • PEN polyethylene naphthalate
  • the two films formed from the same material can dispensably have redundant properties, for example electrical insulating ability (electrically insulating) and/or oxygen impermeability of each of the two films.
  • PEM electrolytic cells have a similar structure.
  • DE 10 2005 058370 A1 discloses a fuel cell which has two bipolar plates, a membrane-electrode unit being arranged between the bipolar plates and a diffusion layer being arranged between the membrane-electrode unit and the bipolar plates.
  • the membrane-electrode unit is arranged on a carrier frame or a frame structure.
  • DE 101 40 684 A1 discloses a membrane-electrode unit for a fuel cell, containing a layered arrangement of an anode electrode, a cathode electrode and a membrane arranged between them, with a polymer material on a top and bottom side of the layered arrangement is applied. Air pockets can occur in the frame structure of the membrane-electrode unit, which impairs the function and the tolerances of the membrane-electrode unit.
  • the object of the present invention is to avoid these air inclusions and thereby increase the robustness of the electrochemical cell.
  • the membrane-electrode unit includes a membrane, two electrode layers and a frame structure.
  • the frame structure includes a foil and a further foil which are glued to one another by means of an adhesive.
  • the film has a large number of recesses.
  • the recesses only weaken the strength of the foil in a negligible manner, so that the strength of the frame structure is nevertheless maintained. Furthermore, this structure allows the two films to be joined over a large area; a flat unrolling under pressure - to minimize the air bubbles - is no longer necessary.
  • the membrane-electrode unit preferably comprises a flat membrane, in particular a polymer electrolyte membrane (PEM).
  • the membrane-electrode unit preferably comprises two porous electrode layers, each with a catalyst paste, the electrode layers being arranged on the membrane and delimiting it on both sides.
  • the membrane-electrode assembly can include two diffusion layers. In particular, these can delimit the MEA-3 on both sides.
  • the film is preferably bonded directly to the other film in a bonding area by means of the adhesive.
  • the recesses are only in that Bonding area arranged. Laying the two films on top of each other, with the adhesive layer in between, is particularly prone to trapping air bubbles. It is precisely in this bonding area that the recesses are then particularly effective for outgassing the enclosed air.
  • the film covers the electrode layer in an overlapping area.
  • the recesses are then at least partially arranged in the overlapping area. This is particularly advantageous when the adhesive is also present in the overlapping area, because the adhesive in turn increases the risk of trapped air in the overlapping area.
  • the further film has no recesses. This ensures the tightness of the frame structure because the further film fulfills the function of tightness, although the tightness of the first film is impaired due to the recesses.
  • the invention also relates to a method for producing a membrane-electrode unit according to one of the above statements.
  • the membrane-electrode unit has a membrane, two electrode layers and a frame structure.
  • the frame structure includes a foil and another foil. The process is characterized by the following process steps:
  • the recesses are preferably introduced by a spiked roller or by a laser.
  • the spiked roller By means of the spiked roller, the recesses can be made in the film quickly and cheaply using a rolling process. With a laser, the positioning of the recesses can be varied as desired.
  • the two films are placed on top of each other over a large area.
  • the two foils are not positioned relative to one another under pressure by means of a rolling process.
  • the rolling process was necessary to remove trapped air bubbles as best as possible avoid.
  • the positioning accuracy of the two foils relative to each other is now improved by laying them flat or holistically on top of each other.
  • the electrochemical cell can be, for example, a fuel cell, an electrolytic cell or a battery cell.
  • the fuel cell and the electrolytic cell are in particular a PEM-FC (polymer electrolyte membrane fuel cell) or PEM-EC.
  • a cell stack comprises, in particular, a multiplicity of electrochemical cells arranged one above the other.
  • FIG. 2 Vertical section of a membrane-electrode assembly, only the essential areas being shown,
  • FIG. 3 shows a schematic of the frame structure of a membrane-electrode assembly with an enclosed air bubble, only the essential areas being shown,
  • FIG. 4 vertical section of a membrane electrode assembly according to the invention, only the essential areas being shown,
  • FIG. 5 shows a schematic of the frame structure of a membrane electrode assembly according to the invention without an enclosed air bubble, only the essential areas being shown,
  • FIG. 6 Top view of two flat membrane-electrode units, only the essential areas being shown.
  • FIG. 1 shows schematically a known from the prior art electrochemical cell 100 in the form of a fuel cell, with only the essential areas are shown.
  • the fuel cell 100 has a membrane 2, in particular a polymer electrolyte membrane.
  • a cathode space 100a is formed on one side of the membrane 2 and an anode space 100b on the other side.
  • An electrode layer 3, a diffusion layer 5 and a distributor plate 7 are arranged in the cathode chamber 100a, pointing outwards from the membrane 2--ie in the normal direction or stacking direction z.
  • an electrode layer 4, a diffusion layer 6 and a distributor plate 8 are arranged in the anode chamber 100b, pointing outwards from the membrane 2.
  • the membrane 2 and the two electrode layers 3, 4 form a membrane-electrode assembly 1.
  • the two diffusion layers 5, 6 are also part of the membrane-electrode assembly 1.
  • the distributor plates 7, 8 have ducts 11 for the supply of gas--for example air in the cathode space 100a and hydrogen in the anode space 100b--to the diffusion layers 5,6.
  • the diffusion layers 5, 6 typically consist of a carbon fiber fleece on the channel side--ie towards the distributor plates 7, 8--and on the electrode side--ie towards the electrode layers 3, 4--of a microporous particle layer.
  • the distributor plates 7 , 8 have the channels 11 and thus implicitly also the webs 12 adjoining the channels 11 .
  • the undersides of these webs 12 consequently form a contact surface 13 of the respective distributor plate 7, 8 with the underlying diffusion layer 5, 6.
  • the cathode-side distributor plate 7 and the anode-side distributor plate 8 differ from one another;
  • the cathode-side distributor plate 7 of an electrochemical cell 100 and the anode-side distributor plate 8 of the adjacent electrochemical cell are firmly connected, for example by welded joints, and are thus combined to form a bipolar plate.
  • FIG. 2 shows, in a vertical section, the membrane electrode assembly 1 of an electrochemical cell 100, in particular a fuel cell, in one Marginal area, with only the essential areas being shown.
  • the membrane-electrode assembly 1 has the flat membrane 2, for example a polymer electrolyte membrane (PEM), and the two porous electrode layers 3 and 4, each with a catalyst layer or a catalyst paste 31, 41, the electrode layers 3 and 4 with their catalyst pastes 31, 41 are each arranged on one side or surface of the membrane 2.
  • the electrochemical cell 100 has the two diffusion layers 5 and 6, which can also belong to the membrane-electrode arrangement 1, depending on the design.
  • the membrane electrode assembly 1 is surrounded on its periphery by the frame structure 16, which is also referred to as a subgasket.
  • the frame structure 16 is used for rigidity and tightness of the membrane electrode assembly 1 and is a non-active area of the electrochemical cell 100.
  • the frame structure 16 is particularly U-shaped or Y-shaped in section, with a first leg of the U-shaped frame section being formed by a film 161 made of a first material W1 and a second leg of the U-shaped frame section being formed by a further film 162 is formed from a second material W2.
  • the foil 161 and the further foil 162 are glued together by means of an adhesive 163 made of a third material W3.
  • the first material W1 and the second material W2 are often identical and are made of a thermoplastic polymer, for example PEN (polyethylene naphthalate).
  • the two diffusion layers 5 and 6 overlap the frame structure 16 in an edge area 22.
  • the electrode layers 3, 4 are covered by the frame structure 16; this is a non-active area of the electrochemical cell 100.
  • the frame structure 16 also encompass the two diffusion layers 5, 6.
  • the diffusion layers 5, 6 are each in contact with an electrode layer 3, 4, so that the electrochemical reaction that is characteristic of the electrochemical cell 100 can take place here.
  • the Electrode layers 3, 4 each have a catalyst paste 31, 41 in which catalysts, usually catalyst particles, are embedded.
  • the catalyst paste 31, 41 is usually a very expensive part of the electrochemical cell 100.
  • the following components of the membrane-electrode assembly 1 are arranged from the inside to the outside in the non-active overlapping area 22:
  • foils 161, 162 pre-coated with adhesive 163 are preferably used.
  • This composite is "sticky", i.e. the foils 161, 162 are fixed to one another after the first contact with one another, repositioning or shifting is no longer possible.
  • FIG. 1 schematically shows the inclusion of an air bubble 170 between the two films 161, 162 coated with adhesive 163 in the adhesive area 23. Even lamination under pressure cannot ensure that the included air bubbles 170 are squeezed out of the frame structure 16.
  • at least one of the two films 161, 162 now has a large number of recesses 164, which are used to allow the air bubbles 170 trapped during the bonding process to escape from the frame structure 16 through the recesses 164. This can already happen when the frame structure 16 is joined, but it also works later when the two films 161, 162 are laminated or sealed.
  • FIG. 4 shows a vertical section of a membrane-electrode unit 1, which is similar to the embodiment according to FIG.
  • the recesses 164 are formed in the film 161 and are arranged both in the overlapping area 22 and in the bonding area 23 .
  • the recesses 164 can also be arranged in only one of these two areas.
  • Figure 5 shows the gluing of the two foils 161, 162 in the gluing area 23, analogously to Figure 3.
  • the foil 161 now has a large number of perforations or recesses 164 which, during lamination, allow the air bubbles 170 to escape from the space between allow the two films 161, 162.
  • the tightness of the frame structure 16 is ensured by the additional film 162, which is preferably non-perforated. Air inclusions are prevented by the recesses 164 or air bubbles 170 located between the foils 161, 162 can escape through the perforation.
  • the joining of the two foils 161, 162 no longer has to be done by unrolling, but can also be done flatly, the two foils 161, 162 can be placed one on top of the other with the adhesive 163 interposed.
  • the Recesses 164 allow the trapped air to escape even when joining over a large area.
  • the mechanical strength of the frame structure 16 and the symmetry of the structure are nevertheless retained. Unrolling - as was previously necessary - is no longer necessary, the associated handling errors and material fluctuations, which previously led to air pockets, no longer have to be taken into account.
  • the focus when assembling the membrane electrode assembly 1 can be placed on the positioning accuracy.
  • the lamination of the frame structure 16 can be decoupled from this.
  • the perforation or the plurality of recesses 164 can be introduced over the entire surface, as can be seen in FIG. 6a. There, both the overlapping area 22 and the adhesive area 23 have the recesses outlined with a large number of circles. This has advantages, for example, because this variant can simply be delivered as rolled goods.
  • the holes it is also conceivable for the holes to be arranged over a partial area, oriented towards defined areas of the assembly group, preferably only in the partial area of the bonding area 23, as shown in FIG. 6b.
  • the recesses 164 can be introduced using various methods, e.g. mechanically using a spiked roller or thermally using a laser and other methods.
  • the recesses 164 can also be introduced at different points in the process chain. This can already take place during the production of the foils 161, 162, but also only as a sub-process during the production of the membrane-electrode unit 1. This can take place before or after the two foils 161, 162 are joined. When perforating after joining, it is preferably ensured that the further film 162 is not perforated in order to be able to guarantee the impermeability requirement for the frame structure 16 .

Abstract

L'invention concerne un assemblage membrane-électrodes (1) pour une cellule électrochimique (100). L'assemblage membrane-électrodes (1) comporte une membrane (2), deux couches d'électrode (3, 4) et une structure formant cadre (16). La structure formant cadre (16) comprend une feuille (161) et une autre feuille (162), lesquelles sont collées l'une à l'autre au moyen d'un adhésif (163). La feuille (161) comporte une pluralité d'évidements (164).
PCT/EP2022/080327 2021-11-03 2022-10-31 Assemblage membrane-électrodes pour cellule électrochimique et procédé de fabrication d'un assemblage membrane-électrodes WO2023078819A2 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102021212401.1 2021-11-03
DE102021212401.1A DE102021212401A1 (de) 2021-11-03 2021-11-03 Membran-Elektroden-Einheit für eine elektrochemische Zelle und Verfahren zum Herstellen einer Membran-Elektroden-Einheit

Publications (2)

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WO2023078819A2 true WO2023078819A2 (fr) 2023-05-11
WO2023078819A3 WO2023078819A3 (fr) 2023-11-16

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PCT/EP2022/080327 WO2023078819A2 (fr) 2021-11-03 2022-10-31 Assemblage membrane-électrodes pour cellule électrochimique et procédé de fabrication d'un assemblage membrane-électrodes

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WO (1) WO2023078819A2 (fr)

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10140684A1 (de) 2001-08-24 2003-03-06 Daimler Chrysler Ag Dichtungsaufbau für eine MEA und Verfahren zur Herstellung des Dichtungsaufbaus
DE102005058370A1 (de) 2005-12-06 2007-06-14 Harro Höfliger Verpackungsmaschinen GmbH Brennstoffzelle, Verfahren zur Herstellung derselben und Vorrichtung zum Ausführen des Herstellverfahrens einer Brennstoffzelle

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20110177423A1 (en) * 2010-01-21 2011-07-21 Anton Nachtmann Five-Layer Membrane Electrode Assembly with Attached Border and Method of Making Same
EP2874219B1 (fr) * 2012-07-10 2016-11-30 Nissan Motor Co., Ltd. Ensemble électrode à membrane
DE102020216093A1 (de) * 2020-12-17 2022-06-23 Robert Bosch Gesellschaft mit beschränkter Haftung Membran-Elektroden-Einheit für eine elektrochemische Zelle und Verfahren zur Herstellung einer Membran-Elektroden-Einheit
FR3132394B3 (fr) * 2022-07-25 2024-03-22 Symbio France Assemblage membrane-électrode de pile à combustible, procédé de fabrication d’un tel assemblage et pile à combustible comprenant au moins un tel assemblage

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10140684A1 (de) 2001-08-24 2003-03-06 Daimler Chrysler Ag Dichtungsaufbau für eine MEA und Verfahren zur Herstellung des Dichtungsaufbaus
DE102005058370A1 (de) 2005-12-06 2007-06-14 Harro Höfliger Verpackungsmaschinen GmbH Brennstoffzelle, Verfahren zur Herstellung derselben und Vorrichtung zum Ausführen des Herstellverfahrens einer Brennstoffzelle

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Publication number Publication date
WO2023078819A3 (fr) 2023-11-16
DE102021212401A1 (de) 2023-05-04

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