WO2001093354A2 - Systeme de pile a combustible et procede permettant de le produire - Google Patents

Systeme de pile a combustible et procede permettant de le produire Download PDF

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Publication number
WO2001093354A2
WO2001093354A2 PCT/EP2001/006175 EP0106175W WO0193354A2 WO 2001093354 A2 WO2001093354 A2 WO 2001093354A2 EP 0106175 W EP0106175 W EP 0106175W WO 0193354 A2 WO0193354 A2 WO 0193354A2
Authority
WO
WIPO (PCT)
Prior art keywords
fuel cell
layer
gas diffusion
arrangement according
membrane
Prior art date
Application number
PCT/EP2001/006175
Other languages
German (de)
English (en)
Other versions
WO2001093354A3 (fr
Inventor
Arthur Koschany
Original Assignee
Manhattan Scientifics, Inc.
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 Manhattan Scientifics, Inc. filed Critical Manhattan Scientifics, Inc.
Priority to AU2001267500A priority Critical patent/AU2001267500A1/en
Publication of WO2001093354A2 publication Critical patent/WO2001093354A2/fr
Publication of WO2001093354A3 publication Critical patent/WO2001093354A3/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
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • 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
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2250/00—Fuel cells for particular applications; Specific features of fuel cell system
    • H01M2250/20—Fuel cells in motive systems, e.g. vehicle, ship, plane
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0082—Organic polymers
    • 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]
    • 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T90/00—Enabling technologies or technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02T90/40—Application of hydrogen technology to transportation, e.g. using fuel cells

Definitions

  • the invention relates to a fuel cell arrangement comprising at least one polymer electrolyte membrane (PEM) fuel cell with a polymer electrolyte membrane arranged between a cathode and an anode catalyst layer, gas diffusion layers arranged on both sides thereof and at least one closing layer adjacent to at least one of the gas diffusion layers, and on one A process for their manufacture, and specifically relates to high power density PEM fuel cells that are functional without external mechanical compression devices and are manufactured by lamination processes.
  • PEM polymer electrolyte membrane
  • the central component of a PEM fuel cell is a polymer electrolyte membrane (PEM). It has the task that is typical of fuel cells
  • Reactants e.g. B. hydrogen or methanol as fuel and air or pure
  • Membrane (anode) free of electrons and H + ions.
  • the cathode the electrons passed through an external circuit are combined with the H + ions traveling through the membrane and the oxidizing agent (e.g. oxygen from the air) to form the reaction product (e.g. water).
  • the reaction product e.g. water
  • the area of the clamping plates here is similar in size to the total active area of the cell arrangement.
  • the invention is intended to create fuel power assemblies with a high power density without the use of mechanical compression devices, for which purpose simple and inexpensive lamination processes are preferably used to produce such fuel cell assemblies.
  • the membrane, the catalyst layers, the gas diffusion layers and the at least one end layer of the fuel cell are mechanically solid and electrically conductive or electrochemically active over the entire surface by ion-conducting chemical binders, in particular polymers and / or thermo - And / or thermosets, are connected to one another without the arrangement or the cell comprising a mechanical device compressing them, or in that during the manufacture of the cell the membrane, the catalyst layers, the gas diffusion layers and the end layer (s) of the Fuel cells are mechanically solid and electrically conductive or electrochemically active by means of ion-conducting polymers and / or thermoplastics and / or thermosets.
  • the greatest advantages of the invention arise in the application fertilizer on planar arrangements of single and double cells.
  • connection of layers namely a polymer electrolyte membrane with two gas diffusion electrodes, by applying heat and pressure is known per se, e.g. B. from EP 0 935 304 A.
  • FIG. 1 shows a cross section through a single fuel cell.
  • 2 shows a plan view of a planar arrangement of three fuel cells on a common substrate;
  • Fig. 3 shows a cross section through a double fuel cell.
  • a substrate 1 in a stack-like structure from bottom to top, consists of a substrate 1, an anode arranged on the substrate 1.
  • the current arrester 2 to which a carbon composite layer 3 is further connected and this in turn is connected to an anode gas diffusion layer 4.
  • This layer 4 carries on its upper side in the drawing a catalyst 5 which lies directly against a membrane 6, the opposite side of which is covered by a layer 7 of a catalyst 7 on the cathode side.
  • This layer is followed by a cathodic gas diffusion layer 8 on the side facing away from the membrane, on which narrow conductor tracks 9, possibly also only wires, are applied as current conductors.
  • the anode gas diffusion layer 4 forms a gas space, which is sealed with the aid of a seal 10 and is supplied with combustible gas via a hydrogen inlet 11 Reaction products are discharged again via an outlet 12.
  • the substrate 1, the anode current collector 2 and the carbon composite layer 3 together form a termination layer 13.
  • the termination layer may also consist only of the layers 2 and 3, or even only the current conductor 2.
  • Cells of the type shown in FIG. 1 can, for example, be arranged side by side in a planar manner on the substrate 1 on which the anode current conductors 2 are arranged with separating spaces 14.
  • the connections of the individual parts of the anode current collector 2 are shown at 15; they are each connected to a star point of the cathode current conductor 9 for the purpose of connecting the three cells in series.
  • the two current draw poles are marked with "+" and "-".
  • the individual cells have no through bolts or the like for pressing, but are glued together using suitable binders. By appropriately choosing these binders, the compressive strength of the arrangement is maintained despite a certain excess pressure in the anode gas diffusion layer 4.
  • the cells can also be assembled as a stack, for example as a double cell according to FIG. 3, which is mirrored on the substrate 1. Such cells are also constructed without mechanical pressing means.
  • the hydrogen pressures typically used are 10 4 to 2 • 10 5 Pa (0.1 - 2 bar).
  • the described sequence of mechanically connected (laminated) layers can be used analogously for all common cell arrangements such as bipolar stacks, monopolar stacks, single cells and quasi monopolar double cells. For a special arrangement useless layers such.
  • B. the substrate 1 for the inner cells of a bipolar stack can also be omitted.
  • the end layer has different functions in different cell arrangements.
  • the requirements for gas tightness and conductivity parallel to the layer level are different. All requirements can be met by the finishing layer according to the invention, in particular according to Example 1.
  • channel structures for gas routing in the gas diffusion and / or closing layer are not explicitly discussed with the exception of example 1.
  • the end layer 13 comprises a material with an electrical conductivity parallel and perpendicular to the cell plane, which is sufficient to transport the electrical current produced during operation to the contact point 15 without a substantial drop in voltage.
  • a continuous or slotted one is preferred
  • Non-precious metal foil e.g. copper
  • a conductive, dense protective layer e.g. copper
  • the lamination method described in Example 1 is preferably used, which is based on a conductive, preformed layer material, as is known from WO 00/10174.
  • a metal foil can be fixed on a substrate that is as rigid as possible and has a low density. Glass or carbon fiber reinforced epoxy resin plates have particularly good properties. The easiest way is to use a continuous or partially copper-coated electronic board, which is available at very low cost due to mass production.
  • the membrane 6, the catalyst layers 5, 7 and the gas diffusion layers 4, 8 can be connected by hot pressing using an auxiliary polymer, preferably in a single operation to form the so-called membrane electrode assembly (MEA).
  • MEA membrane electrode assembly
  • the temperatures of up to 180 ° C (preferably up to 140 ° C) and pressures up to 5 • 10 7 Pa (500 bar, preferably up to 250 bar) place high demands on the materials used.
  • unfilled commercially available carbon fiber papers from Toray, Japan
  • Suitable very pressure stable gas diffusion layers are known from US Pat. No. 5,998,057.
  • auxiliary polymers find Nafion TM (Dupont), PTFE, THV TM (Dyneon) and non-fluorinated thermoplastics such as. B. PE, PP and PS use.
  • a suitable application of several of these polymers increases the adhesive force compared to the prior art and makes a significant contribution to the present invention.
  • the polymers can be added in the form of powder, nonwovens, films, suspensions or solutions before the hot pressing of the gas diffusion and the catalyst layer. By applying the elevated temperature and pressure, these polymers melt or soften and combine
  • the conductive mechanical connection of the final layer and the MEA takes place, for. B. by applying a curable resin such as epoxy, furan or phenolic resin on the surface of the anode and / or on the surface of the final layer facing the anode. Curing is preferably carried out under pressure at elevated temperature.
  • a curable resin such as epoxy, furan or phenolic resin
  • a microporous, conductive layer e.g. B. be applied from carbon black, which absorbs the liquid resin during the curing process. Due to the larger capillary forces in the fine-pored layer, the resin penetrates the electrode only slightly.
  • the hot pressing of the final layer and the MEA with a thermoplastic material positioned in between in the form of a film or a nonwoven leads to a firm, conductive connection.
  • Membrane edge performed with the end plate.
  • An adhesive seal with cold- or hot-curing silicones according to WO 00/02279 is preferably applied.
  • an adhesive seal without a free membrane edge can also be used with particular preference.
  • Example 4 contains a detailed description of one of the methods.
  • the cathode current arrester shown in Fig.l only partially covers the cathode so that the oxygen in the air can diffuse to the catalyst. It preferably consists of a metal foil (for example copper) which is coated on one or both sides either with a noble metal or by the process in Example 1 (finishing layer).
  • the current conductor is laminated to the cathode or the MEA analogously to the method for connecting the anode to the end layer.
  • the cathode current arrester can also be in the form of a grid or slotted
  • Metal foil is inserted between two cathodic gas diffusion layers during the reinforcement process mentioned above and then laminated in by means of an increase in pressure and temperature.
  • a carbon fiber fleece (3 mg / cm 2 ) with a dispersion of expanded, ground graphite, conductive carbon black and PTFE is impregnated one or more times by rolling in and dried after each impregnation step.
  • the mass fraction of graphite based on the brought carbon materials is 10 to 100%, preferably 40 to 75%.
  • the proportion of PTFE in the total solids introduced is about 3 to 10%.
  • the total mass per unit area of the impregnated nonwoven is 6 to 25 mg / cm 2 , preferably 8 to 14 mg / cm 2 .
  • This still porous layer material is covered with a solution of synthetic resin, e.g. B.
  • Epoxy resin, soaked in acetone and the solvents are evaporated.
  • the proportion of synthetic resin in the solution is 10 to 90%, and preferably 40 to 60%.
  • One or more of these nonwovens containing synthetic resin are placed on a copper foil or an electronic circuit board with exposed conductor tracks or a free but closed copper surface and, if necessary, increased
  • the conductor tracks on the electronic board can be designed in such a way that channels for guiding the reaction gases, in particular hydrogen, are formed. After coating, this channel structure is essentially retained.
  • a mechanically firmly connected and electrochemically active MEA is created.
  • the above numerical data are only examples and can be subjected to large variations.
  • other thermoplastics such as polyethylene can be used instead of polypropylene. In this case, the processing temperature can be significantly reduced.
  • a firm connection is also created if the gas diffusion layer, an additional layer on this gas diffusion layer or the catalyst layer contain powdered thermoplastics.
  • the side of the end layer 13 facing the anode is covered with a sion of conductive carbon black, expanded graphite and PTFE in the 1: 1 mixed dispersion liquids isopropanol and water sprayed one or more times with intermediate drying.
  • the PTFE content is typically 3 to 10%.
  • the mass ratio of graphite and conductive carbon black can be varied within wide limits.
  • the dry mass of the spray layer is approximately 0.5 to 3 mg / cm 2 .
  • PTFE only serves as an auxiliary binder for the layer during processing.
  • a diluted synthetic resin e.g. epoxy resin
  • Example 1 A diluted synthetic resin (e.g. epoxy resin) as used in Example 1 is sprayed onto the previously described layer in a suitable amount. The solvents are then evaporated off. The sealing area of the later cell should be left out during both spraying processes.
  • an adhesive bead made of thermosetting silicone is applied to the end layer on the circumference of the anode.
  • the MEA is positioned exactly, placed on the final layer and hot pressed with it until the plastics have fully or partially cured.
  • Typical pressures are in the range of 10 6 to 3 • 10 7 Pa (10 to 300 bar), the temperature depends on the requirements for curing epoxy resin and silicone.
  • the end product of this process step is a gas-tight, mechanically firm composite of MEA and final layer on the anode side.
  • the cathode current arrester can be laminated afterwards.
  • FIG. 3 A planar double cell according to FIG. 3 of basically known per se
  • Type (eg WO 95/17772) with connected anode spaces and two opposite cathodes is preferred with the help of a double-sided with metal coated electronic board built.
  • the continuous or interrupted metal layers of the board are coated as described in Example 1 with a composite of polymers with different carbon materials. A double final layer is thus created.
  • Membrane-electrode units with current arresters are attached and sealed on both sides of this layer using one of the methods mentioned above.
  • a hydrogen inflow and outflow hole connects and supplies the two anode compartments.
  • the top and bottom of this planar arrangement consist of cathodes. Since the metal layers of the two anodes are electrically insulated, the two cells can be connected in series, providing one for many

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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)

Abstract

Jusqu'à présent, on utilisait pour des piles à combustible à membrane à électrolyte polymérique connues des dispositifs de compression mécanique, servant la plupart du temps à agir à l'encontre d'agents réactifs amenés avec surpression. Le poids et le volume élevés de ces dispositifs et les frais ainsi induits, constituent un obstacle majeur à l'utilisation de piles à combustible. Selon l'invention, les couches sont maintenues sans dispositifs mécaniques, par des liants chimiques. L'invention permet par conséquent de pallier tous les inconvénients mentionnés ci-dessus, au moyen de processus de laminage simples et économiques, par élimination des dispositifs de compression mécanique. Les processus de laminage selon l'invention s'utilisent notamment dans le cadre de l'utilisation de piles à combustible à membrane à électrolyte polymérique, dans le domaine mobile, comme dans une configuration planaire de piles individuelles où il se trouve une pluralité de piles simples ou doubles adjacentes sur une surface plane ou cintrée.
PCT/EP2001/006175 2000-05-31 2001-05-31 Systeme de pile a combustible et procede permettant de le produire WO2001093354A2 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU2001267500A AU2001267500A1 (en) 2000-05-31 2001-05-31 Polymer-electrolyte membrane (pem) fuel cell system and method for the production thereof

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE10027069.7 2000-05-31
DE10027069 2000-05-31

Publications (2)

Publication Number Publication Date
WO2001093354A2 true WO2001093354A2 (fr) 2001-12-06
WO2001093354A3 WO2001093354A3 (fr) 2002-11-28

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WO (1) WO2001093354A2 (fr)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2005045974A1 (fr) * 2003-10-31 2005-05-19 Hewlett-Packard Development Company L.P. Joint d'ensemble pile a combustible pour confinement de combustible
US8609297B2 (en) 2003-07-29 2013-12-17 Industrial Technology Research Institute Flat fuel cell assembly and fabrication thereof
DE112004000171B4 (de) * 2003-02-05 2014-05-08 General Motors Corp. Korrosionsbeständige Anschlussplatten für Brennstoffzellen
WO2021239859A1 (fr) * 2020-05-29 2021-12-02 Sgl Carbon Se Agent de revêtement

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
AT393045B (de) * 1989-08-08 1991-07-25 Peter Dipl Ing Dr Schuetz Plattenfoermige duennschicht-h2/o2-brennstoffzelle und verfahren zu ihrer herstellung
EP0499935A1 (fr) * 1991-02-16 1992-08-26 ABBPATENT GmbH Assemblage de piles à combustible à électrolyte solide
GB2323700A (en) * 1997-03-29 1998-09-30 Ballard Power Systems Electrochemical cells
DE19823880A1 (de) * 1997-06-03 1998-12-10 Motorola Inc Bipolarplatte für Brennstoffzellenanordnung
US5945232A (en) * 1998-04-03 1999-08-31 Plug Power, L.L.C. PEM-type fuel cell assembly having multiple parallel fuel cell sub-stacks employing shared fluid plate assemblies and shared membrane electrode assemblies
WO2000002279A2 (fr) * 1998-06-30 2000-01-13 Manhattan Scientifics, Inc. Ensemble etanche aux gaz forme d'une plaque bipolaire et d'une unite membrane-electrodes de piles a combustible a membrane d'electrolyte polymere

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH08185875A (ja) * 1994-12-28 1996-07-16 Tokyo Gas Co Ltd 固体高分子型燃料電池のシ−ル方法

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
AT393045B (de) * 1989-08-08 1991-07-25 Peter Dipl Ing Dr Schuetz Plattenfoermige duennschicht-h2/o2-brennstoffzelle und verfahren zu ihrer herstellung
EP0499935A1 (fr) * 1991-02-16 1992-08-26 ABBPATENT GmbH Assemblage de piles à combustible à électrolyte solide
GB2323700A (en) * 1997-03-29 1998-09-30 Ballard Power Systems Electrochemical cells
DE19823880A1 (de) * 1997-06-03 1998-12-10 Motorola Inc Bipolarplatte für Brennstoffzellenanordnung
US5945232A (en) * 1998-04-03 1999-08-31 Plug Power, L.L.C. PEM-type fuel cell assembly having multiple parallel fuel cell sub-stacks employing shared fluid plate assemblies and shared membrane electrode assemblies
WO2000002279A2 (fr) * 1998-06-30 2000-01-13 Manhattan Scientifics, Inc. Ensemble etanche aux gaz forme d'une plaque bipolaire et d'une unite membrane-electrodes de piles a combustible a membrane d'electrolyte polymere

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
PATENT ABSTRACTS OF JAPAN vol. 1996, no. 11, 29. November 1996 (1996-11-29) -& JP 08 185875 A (TOKYO GAS CO LTD), 16. Juli 1996 (1996-07-16) *

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE112004000171B4 (de) * 2003-02-05 2014-05-08 General Motors Corp. Korrosionsbeständige Anschlussplatten für Brennstoffzellen
US8609297B2 (en) 2003-07-29 2013-12-17 Industrial Technology Research Institute Flat fuel cell assembly and fabrication thereof
DE102004033606B4 (de) * 2003-07-29 2015-09-24 Industrial Technology Research Institute Verfahren zur Herstellung einer Brennstoffzelle, Brennstoffzelle sowie flache Brennstoffzellenanordnung
WO2005045974A1 (fr) * 2003-10-31 2005-05-19 Hewlett-Packard Development Company L.P. Joint d'ensemble pile a combustible pour confinement de combustible
WO2021239859A1 (fr) * 2020-05-29 2021-12-02 Sgl Carbon Se Agent de revêtement

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Publication number Publication date
AU2001267500A1 (en) 2001-12-11
WO2001093354A3 (fr) 2002-11-28

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