WO2000026982A2 - Unite membrane-electrode pour pile a combustible a membrane electrolytique polymere, et son procede de production - Google Patents

Unite membrane-electrode pour pile a combustible a membrane electrolytique polymere, et son procede de production Download PDF

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Publication number
WO2000026982A2
WO2000026982A2 PCT/DE1999/003319 DE9903319W WO0026982A2 WO 2000026982 A2 WO2000026982 A2 WO 2000026982A2 DE 9903319 W DE9903319 W DE 9903319W WO 0026982 A2 WO0026982 A2 WO 0026982A2
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WO
WIPO (PCT)
Prior art keywords
membrane
catalyst
catalyst powder
electrode
powder
Prior art date
Application number
PCT/DE1999/003319
Other languages
German (de)
English (en)
Other versions
WO2000026982A3 (fr
Inventor
Klaus Dennerlein
Ulrich Gebhardt
Original Assignee
Siemens Aktiengesellschaft
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 Siemens Aktiengesellschaft filed Critical Siemens Aktiengesellschaft
Publication of WO2000026982A2 publication Critical patent/WO2000026982A2/fr
Publication of WO2000026982A3 publication Critical patent/WO2000026982A3/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]
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
    • C25B9/23—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms comprising ion-exchange membranes in or on which electrode material is embedded
    • 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
    • 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

Definitions

  • the invention relates to a membrane-electrode unit for a PEM fuel cell, in which the active electrode catalyst layer is pressed directly onto the membrane as a dry powder.
  • the invention also relates to a cost-effective and mass-production method for this membrane electrode assembly (ME).
  • ME are known in which the catalyst is applied as a paste or ink, ie with the addition of an additive such as a leveling aid, directly to the membrane by spraying, rolling or by means of screen printing.
  • an additive such as a leveling aid
  • a disadvantage of these MEs is that the additive later affects the activity of the electrode catalyst layer and increases its internal resistance, in particular if it has not been removed without residue.
  • an additive always causes the membrane to swell and thus interferes with its dimensional stability.
  • ME are also known in which the catalyst is applied to a gas conducting layer between the membrane and the active electrode catalyst layer. A not inconsiderable proportion of electrode catalyst is deposited in the pores of the gas conducting layer, which is then no longer catalytically active.
  • the MEs known to date therefore have a high proportion of catalyst, which remains surface-ineffective in the electrochemical cell, because it is either embedded in the pores of the gas conducting layer or is enclosed in an additive (i.e. a processing aid).
  • the "working section” denotes the production of an intermediate product
  • the "working step” eg drying of the applied layer
  • the object of the invention is therefore to optimize the utilization or surface effectiveness of the catalytic converter on the ME and its electrochemical connection and to provide a simple (ie comprising only one working section), inexpensive and mass-production process for producing an ME with optimized catalytic converter utilization .
  • a membrane-electrode unit comprising a membrane with an active electrode catalyst layer on both sides, in which the active electrode catalyst layer is free of additives and is applied directly to the membrane.
  • the invention also relates to a process for the continuous production of a membrane electrode assembly, comprising the following steps:
  • the reduction in internal resistance can be estimated to be approximately 15% by using the invention in the manufacture of the ME.
  • the internal resistance in the ME conventionally produced with this membrane is approximately 130 m ⁇ * cm 2 and is reduced accordingly when the invention is applied to approximately 110 m ⁇ * cm 2 .
  • One embodiment of the process is that in a continuous process, one side of the membrane is first coated with catalyst, then the membrane strip is turned over deflection rollers before the other side is coated with catalyst.
  • the catalyst is advantageously shaken onto the membrane band with a sieve.
  • the geometric dimensions of the cathode and / or anode are realized by the contour of the screen, such as, for example, angular, in particular rectangular or square.
  • fractionation of the catalyst is possible using an additional sieve.
  • an ME with a layer structure with regard to volume concentration and / or porosity of the electrode catalyst can be realized.
  • the porosity can be varied depending on the requirements by the pore structure, pore size and / or volume concentration.
  • a catalyst support can be applied to the ME after manufacture.
  • the membrane band is kept moist during processing. This can e.g. using spray devices and / or water films.
  • the advantage here is that the wet membrane has a constant shape, which it also has when operating in the electrochemical cell. Dimensional stability is therefore provided and no volume changes due to swelling or drying (as is the case with the known processes which undergo numerous tempering and / or drying steps during production) need to be taken into account.
  • the catalyst for example the Pt catalyst
  • hydrophobic catalysts such as teflon based and / or nafionized Pt catalysts are used.
  • the membrane band 1 comes under the first sieve 2, in which there is possibly pretreated, dry catalyst powder. Depending on the dwell time and vibrating intensity, a predetermined amount of the dry catalyst powder is applied through the sieve 2 to the membrane belt. After the catalyst powder has been applied, the electrode catalyst layer is produced on the membrane belt 1 by the press 3. The membrane band 1 with the finished electrode catalyst layer 4 is then turned over the deflection rollers 5 and 6, so that the other, still unoccupied side of the membrane band 1 comes to rest under the second sieve 7. There may be another Pretreated and dry catalyst powder, applied to the membrane 1 in an amount that can be adjusted by the dwell time and the shaking intensity. The press 8 again creates a finished electrode catalyst layer on the membrane band 1. At the end of the method, a finished ME is only punched out of the membrane band 1 with the punch 9.
  • the invention describes a simple tape production from ME.
  • an optimal electrolytic connection of the catalyst to the membrane is achieved, which results in a reduction in the internal resistance of the ME in the electrochemical cell.

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

Abstract

L'invention concerne une unité membrane-électrode destinée à une pile à combustible à membrane électrolytique polymère, dans laquelle la couche de catalyseur d'électrode active est appliquée par pression directement sur la membrane, sous la forme d'une poudre sèche. L'invention concerne en outre un procédé économique permettant la fabrication en masse d'une telle unité membrane-électrode, selon lequel la poudre de catalyseur sèche est appliquée simplement sur la bande membranaire à l'aide d'un tamis, puis travaillée, sans additif, avec une presse pour former une couche de catalyseur d'électrode.
PCT/DE1999/003319 1998-10-30 1999-10-15 Unite membrane-electrode pour pile a combustible a membrane electrolytique polymere, et son procede de production WO2000026982A2 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE19850119.6 1998-10-30
DE19850119 1998-10-30

Publications (2)

Publication Number Publication Date
WO2000026982A2 true WO2000026982A2 (fr) 2000-05-11
WO2000026982A3 WO2000026982A3 (fr) 2000-09-21

Family

ID=7886197

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/DE1999/003319 WO2000026982A2 (fr) 1998-10-30 1999-10-15 Unite membrane-electrode pour pile a combustible a membrane electrolytique polymere, et son procede de production

Country Status (1)

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WO (1) WO2000026982A2 (fr)

Cited By (25)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1406328A1 (fr) * 2001-07-06 2004-04-07 Honda Giken Kogyo Kabushiki Kaisha Appareil d'ajustage et procede de couplage d'un ensemble membrane/electrode, appareil de transport associe
WO2004034498A2 (fr) 2002-10-04 2004-04-22 Pemeas Gmbh Membrane polymere conductrice de protons recouverte d'une couche catalytique et contenant des polyazoles, et son utilisation dans des piles a combustible
WO2006008158A2 (fr) 2004-07-21 2006-01-26 Pemeas Gmbh Unites membrane-electrode et piles a combustible a longevite accrue
US7455888B2 (en) 2004-02-19 2008-11-25 Toyota Jidosha Kabushiki Kaishi Method and apparatus for forming catalyst layer on substrate constituting membrane electrode assembly
EP2131433A1 (fr) 2008-06-05 2009-12-09 Reinz-Dichtungs-Gmbh Cellule électrochimique et procédé de sa fabrication
US7727651B2 (en) 2002-08-02 2010-06-01 Basf Fuel Cell Gmbh Proton-conducting polymer membrane comprising polymers containing phosphonic acid groups and its use in fuel cells
WO2010099948A1 (fr) 2009-03-06 2010-09-10 Basf Se Unités à membrane-électrode améliorées
EP2237356A1 (fr) 2004-02-21 2010-10-06 BASF Fuel Cell GmbH Unité d'électrodes à membrane dotée d'une puissance élevée et son application dans des cellules combustibles
WO2011003884A1 (fr) 2009-07-07 2011-01-13 Basf Se Encre renfermant des particules de polymère, électrode et unité mea correspondantes
WO2011006623A1 (fr) 2009-07-16 2011-01-20 Basf Se Procédé pour faire fonctionner une pile à combustible
WO2011006625A1 (fr) 2009-07-16 2011-01-20 Basf Se Procédé permettant de faire fonctionner une pile à combustible, et pile à combustible correspondante
WO2011006624A2 (fr) 2009-07-16 2011-01-20 Basf Se Procédé pour faire fonctionner une pile à combustible et pile à combustible associée
US7883818B2 (en) 2002-08-29 2011-02-08 Basf Fuel Cell Gmbh Process for producing proton-conducting polymer membranes, improved polymer membranes and the use thereof in fuel cells
WO2011054503A1 (fr) 2009-11-06 2011-05-12 Basf Se Ensemble d'électrodes à membrane et piles à combustible avec performances accrues
US8012647B2 (en) 2004-08-05 2011-09-06 Basf Fuel Cell Gmbh Membrane-electrode unit and fuel elements with increased service life
US8066784B2 (en) 2004-07-15 2011-11-29 Basf Fuel Cell Gmbh Method for the production of membrane/electrode units
WO2011154811A1 (fr) 2010-06-08 2011-12-15 Rensselaer Polytechnic Institute Procédé de production de cellule électrochimique
US8206870B2 (en) 2004-08-05 2012-06-26 Basf Fuel Cell Gmbh Long-life membrane electrode assemblies with gasket and frame
WO2013037591A1 (fr) * 2011-09-15 2013-03-21 Siemens Aktiengesellschaft Procédé de production à sec d'une unité membrane-électrodes, unité membrane-électrodes et ensemble de laminage
US8815467B2 (en) 2010-12-02 2014-08-26 Basf Se Membrane electrode assembly and fuel cells with improved lifetime
EP2843743A1 (fr) 2013-09-02 2015-03-04 Basf Se Unités d'électrodes à membrane pour piles à combustible à haute température avec une stabilité améliorée
EP2869382A1 (fr) 2013-10-30 2015-05-06 Basf Se Ensembles électrode à membrane améliorée
US9048478B2 (en) 2010-04-22 2015-06-02 Basf Se Polymer electrolyte membrane based on polyazole
US9825320B2 (en) 2013-04-16 2017-11-21 Basf Se Process for the manufacture of membrane electrode units
JP2019139856A (ja) * 2018-02-06 2019-08-22 トヨタ自動車株式会社 膜電極ガス拡散層接合体の裁断装置

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US3134697A (en) * 1959-11-03 1964-05-26 Gen Electric Fuel cell
US3134696A (en) * 1959-11-03 1964-05-26 Gen Electric Fuel battery
GB1163149A (en) * 1965-12-06 1969-09-04 Tno Fuel Cell.
US4272353A (en) * 1980-02-29 1981-06-09 General Electric Company Method of making solid polymer electrolyte catalytic electrodes and electrodes made thereby
DE3036066A1 (de) * 1980-09-25 1982-05-06 Hoechst Ag, 6000 Frankfurt Verfahren zur herstellung eines elektroden-membran-verbundsystems
DE19509749A1 (de) * 1995-03-17 1996-10-02 Deutsche Forsch Luft Raumfahrt Verfahren zur Herstellung eines Verbundes aus Elektrodenmaterial, Katalysatormaterial und einer Festelektrolytmembran
WO1997023916A2 (fr) * 1995-12-22 1997-07-03 Hoechst Research & Technology Deutschland Gmbh & Co. Kg Composites et leur production en continu
WO1997023919A1 (fr) * 1995-12-22 1997-07-03 Hoechst Research & Technology Deutschland Gmbh & Co.Kg Procede de production en continu de composites membrane-electrode
EP0926753A2 (fr) * 1997-12-23 1999-06-30 Deutsches Zentrum für Luft- und Raumfahrt e.V. Méthode de fabrication de couches fonctionelles pour piles à combustible
BE1011693A3 (nl) * 1998-01-07 1999-12-07 Zevco Belgium Besloten Vennoot Werkwijze voor het vervaardigen van een pem-enkelcel.

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JPH1064574A (ja) * 1996-08-26 1998-03-06 Fuji Electric Co Ltd 固体高分子電解質型燃料電池の製造方法

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US3134697A (en) * 1959-11-03 1964-05-26 Gen Electric Fuel cell
US3134696A (en) * 1959-11-03 1964-05-26 Gen Electric Fuel battery
GB1163149A (en) * 1965-12-06 1969-09-04 Tno Fuel Cell.
US4272353A (en) * 1980-02-29 1981-06-09 General Electric Company Method of making solid polymer electrolyte catalytic electrodes and electrodes made thereby
DE3036066A1 (de) * 1980-09-25 1982-05-06 Hoechst Ag, 6000 Frankfurt Verfahren zur herstellung eines elektroden-membran-verbundsystems
DE19509749A1 (de) * 1995-03-17 1996-10-02 Deutsche Forsch Luft Raumfahrt Verfahren zur Herstellung eines Verbundes aus Elektrodenmaterial, Katalysatormaterial und einer Festelektrolytmembran
WO1997023916A2 (fr) * 1995-12-22 1997-07-03 Hoechst Research & Technology Deutschland Gmbh & Co. Kg Composites et leur production en continu
WO1997023919A1 (fr) * 1995-12-22 1997-07-03 Hoechst Research & Technology Deutschland Gmbh & Co.Kg Procede de production en continu de composites membrane-electrode
EP0926753A2 (fr) * 1997-12-23 1999-06-30 Deutsches Zentrum für Luft- und Raumfahrt e.V. Méthode de fabrication de couches fonctionelles pour piles à combustible
BE1011693A3 (nl) * 1998-01-07 1999-12-07 Zevco Belgium Besloten Vennoot Werkwijze voor het vervaardigen van een pem-enkelcel.

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Title
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Cited By (34)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1406328A4 (fr) * 2001-07-06 2007-01-03 Honda Motor Co Ltd Appareil d'ajustage et procede de couplage d'un ensemble membrane/electrode, appareil de transport associe
EP1406328A1 (fr) * 2001-07-06 2004-04-07 Honda Giken Kogyo Kabushiki Kaisha Appareil d'ajustage et procede de couplage d'un ensemble membrane/electrode, appareil de transport associe
US7727651B2 (en) 2002-08-02 2010-06-01 Basf Fuel Cell Gmbh Proton-conducting polymer membrane comprising polymers containing phosphonic acid groups and its use in fuel cells
US7883818B2 (en) 2002-08-29 2011-02-08 Basf Fuel Cell Gmbh Process for producing proton-conducting polymer membranes, improved polymer membranes and the use thereof in fuel cells
US7661542B2 (en) 2002-10-04 2010-02-16 Basf Fuel Cell Gmbh Proton-conducting polymer membrane that contains polyazoles and is coated with a catalyst layer, and application therof in fuel cells
WO2004034498A2 (fr) 2002-10-04 2004-04-22 Pemeas Gmbh Membrane polymere conductrice de protons recouverte d'une couche catalytique et contenant des polyazoles, et son utilisation dans des piles a combustible
DE112005000257B4 (de) * 2004-02-19 2010-06-02 Toyota Jidosha Kabushiki Kaisha, Toyota-shi Verfahren und Vorrichtung zur Ausbildung einer Katalysatorschicht auf einem Substrat, welches eine Membran-Elektrodenanordnung bildet
US7455888B2 (en) 2004-02-19 2008-11-25 Toyota Jidosha Kabushiki Kaishi Method and apparatus for forming catalyst layer on substrate constituting membrane electrode assembly
EP2237356A1 (fr) 2004-02-21 2010-10-06 BASF Fuel Cell GmbH Unité d'électrodes à membrane dotée d'une puissance élevée et son application dans des cellules combustibles
US8177863B2 (en) 2004-07-15 2012-05-15 Basf Fuel Cell Gmbh Method for the production of membrane/electrode units
US8066784B2 (en) 2004-07-15 2011-11-29 Basf Fuel Cell Gmbh Method for the production of membrane/electrode units
WO2006008158A2 (fr) 2004-07-21 2006-01-26 Pemeas Gmbh Unites membrane-electrode et piles a combustible a longevite accrue
US8012647B2 (en) 2004-08-05 2011-09-06 Basf Fuel Cell Gmbh Membrane-electrode unit and fuel elements with increased service life
US8206870B2 (en) 2004-08-05 2012-06-26 Basf Fuel Cell Gmbh Long-life membrane electrode assemblies with gasket and frame
EP2131433A1 (fr) 2008-06-05 2009-12-09 Reinz-Dichtungs-Gmbh Cellule électrochimique et procédé de sa fabrication
WO2010099948A1 (fr) 2009-03-06 2010-09-10 Basf Se Unités à membrane-électrode améliorées
EP2228857A1 (fr) 2009-03-06 2010-09-15 Basf Se Unités d'électrodes à membrane améliorées
WO2011003884A1 (fr) 2009-07-07 2011-01-13 Basf Se Encre renfermant des particules de polymère, électrode et unité mea correspondantes
WO2011006623A1 (fr) 2009-07-16 2011-01-20 Basf Se Procédé pour faire fonctionner une pile à combustible
WO2011006624A2 (fr) 2009-07-16 2011-01-20 Basf Se Procédé pour faire fonctionner une pile à combustible et pile à combustible associée
WO2011006625A1 (fr) 2009-07-16 2011-01-20 Basf Se Procédé permettant de faire fonctionner une pile à combustible, et pile à combustible correspondante
WO2011054503A1 (fr) 2009-11-06 2011-05-12 Basf Se Ensemble d'électrodes à membrane et piles à combustible avec performances accrues
US9048478B2 (en) 2010-04-22 2015-06-02 Basf Se Polymer electrolyte membrane based on polyazole
WO2011154811A1 (fr) 2010-06-08 2011-12-15 Rensselaer Polytechnic Institute Procédé de production de cellule électrochimique
US9537166B2 (en) 2010-06-08 2017-01-03 Rensselaer Polytechnic Institute Method for the production of an electrochemical cell
US8815467B2 (en) 2010-12-02 2014-08-26 Basf Se Membrane electrode assembly and fuel cells with improved lifetime
US9365020B2 (en) 2011-09-15 2016-06-14 Siemens Aktiengesellschaft Method for the dry production of a membrane electrode unit, membrane electrode unit, and roller arrangement
WO2013037591A1 (fr) * 2011-09-15 2013-03-21 Siemens Aktiengesellschaft Procédé de production à sec d'une unité membrane-électrodes, unité membrane-électrodes et ensemble de laminage
US9825320B2 (en) 2013-04-16 2017-11-21 Basf Se Process for the manufacture of membrane electrode units
EP2843743A1 (fr) 2013-09-02 2015-03-04 Basf Se Unités d'électrodes à membrane pour piles à combustible à haute température avec une stabilité améliorée
US9997791B2 (en) 2013-09-02 2018-06-12 Basf Se Membrane electrode units for high temperature fuel cells with improved stability
EP2869382A1 (fr) 2013-10-30 2015-05-06 Basf Se Ensembles électrode à membrane améliorée
US9537168B2 (en) 2013-10-30 2017-01-03 Basf Se Membrane electrode assemblies
JP2019139856A (ja) * 2018-02-06 2019-08-22 トヨタ自動車株式会社 膜電極ガス拡散層接合体の裁断装置

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