AU738679B2 - Membrane-electrode unit for a fuel cell - Google Patents

Membrane-electrode unit for a fuel cell Download PDF

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Publication number
AU738679B2
AU738679B2 AU37040/99A AU3704099A AU738679B2 AU 738679 B2 AU738679 B2 AU 738679B2 AU 37040/99 A AU37040/99 A AU 37040/99A AU 3704099 A AU3704099 A AU 3704099A AU 738679 B2 AU738679 B2 AU 738679B2
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Prior art keywords
electrode unit
membrane electrode
fleece material
per
microfibre
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AU3704099A (en
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Ulrich Stimming
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Carl Freudenberg KG
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Carl Freudenberg KG
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Assigned to CARL FREUDENBERG KG reassignment CARL FREUDENBERG KG Request to Amend Deed and Register Assignors: FIRMA CARL FREUDENBERG
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    • 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
    • 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
    • H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
    • H01M8/1018—Polymeric electrolyte materials
    • H01M8/1067—Polymeric electrolyte materials characterised by their physical properties, e.g. porosity, ionic conductivity or thickness
    • 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
    • H01M8/0289—Means for holding the electrolyte
    • 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
    • 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
    • H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
    • H01M8/1018—Polymeric electrolyte materials
    • H01M8/102—Polymeric electrolyte materials characterised by the chemical structure of the main chain of the ion-conducting polymer
    • H01M8/1023—Polymeric electrolyte materials characterised by the chemical structure of the main chain of the ion-conducting polymer having only carbon, e.g. polyarylenes, polystyrenes or polybutadiene-styrenes
    • 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
    • H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
    • H01M8/1018—Polymeric electrolyte materials
    • H01M8/1039—Polymeric electrolyte materials halogenated, e.g. sulfonated polyvinylidene fluorides
    • 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
    • H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
    • H01M8/1018—Polymeric electrolyte materials
    • H01M8/1041—Polymer electrolyte composites, mixtures or blends
    • H01M8/1046—Mixtures of at least one polymer and at least one additive
    • H01M8/1048—Ion-conducting additives, e.g. ion-conducting particles, heteropolyacids, metal phosphate or polybenzimidazole with phosphoric acid
    • 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
    • H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
    • H01M8/1018—Polymeric electrolyte materials
    • H01M8/1058—Polymeric electrolyte materials characterised by a porous support having no ion-conducting properties
    • H01M8/106—Polymeric electrolyte materials characterised by a porous support having no ion-conducting properties characterised by the chemical composition of the porous support
    • 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
    • H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
    • H01M8/1018—Polymeric electrolyte materials
    • H01M8/1058—Polymeric electrolyte materials characterised by a porous support having no ion-conducting properties
    • H01M8/1062—Polymeric electrolyte materials characterised by a porous support having no ion-conducting properties characterised by the physical properties of the porous support, e.g. its porosity or thickness
    • 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

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

Description

Applicant: Carl Freudenberg, 69469 Weinheim 15 March 1999 Ho/sta Membrane electrode unit for a fuel cell Description Technical field The invention relates to a membrane electrode unit for a fuel cell comprising an optionally catalyst-coated anode, an optionally catalyst-coated cathode and a proton conductor located between said anode and said cathode.
Current state-of-the-art A unit of this kind is well-known. It's function is to separate the ionic and electrical paths in the reaction between the reaction gases or fluid components containing hydrogen and oxygen in a fuel cell for the purpose of directly converting chemical into electrical energy.
The nature and functioning of various types of fuel cells has been described by K.-D.
Kreuer and J. Maier in "Spektrum der Wissenschaft" (July 1995), 92-96.
The electrodes must be very good electron conductors (electrical resistance around 0.1 Q Their purpose together with the electrolyte surface is to catalyse the desired reactions. The electrolyte must have a high ionic conductivity whilst having the lowest possible electron conductivity. Furthermore, it must be as impermeable as possible to the product gases. All materials should be chemically inert with respect to one another and the reaction components, that is, they should not form any undesired compounds in the strongly oxidising conditions at the cathode or the strongly reducing conditions at the anode.
To be able to interconnect several single cells into cell stacks, the solid components present within the single cells should have sufficient mechanical strength to do so.
Furthermore, material and process costs, service life and environmental compatibility of the cell components also play an important role.
For operating temperatures of 80 to 90'C, proton conducting polymer membranes have proven the most successful for fuel cells. They combine the fluid-like ability to provide free mobility for the molecules and protons with the solid-like ability to remain inherently stable. These requirements are met almost ideally by a perfluorinated ionomer membrane based on polytetrafluoroethylene with sulfonated perfluoro vinylether side chains. This material comprises both hydrophobic and hydrophilic regions which in the presence of water separate out to form a gel-like but nevertheless inherently stable membrane. The hydrophobic backbone chain of the polymer is very resistant to oxidation and reduction and provides the membrane with an inherently stable framework even in the swelled state. It is the swelled hydrophilic, liquid-like, sulphonic acid containing side chains in the water that provide the very good proton conductivity. The pore size of a few nanometers corresponds to the dimension of just a few water molecules. The presence of water facilitates the high mobility of the protons in the channels and pores.
The disadvantage of this cation exchanger, as already described in the cited literature source, is its high price as a result of the expensive manufacturing process required.
Furthermore, its disposal or recycling poses ecological problems.
When operating these fuel cells such membranes have a tendency to dry out, in particular when the combustion oxygen is fed to the cell by means of an air current but also because of the particular property of the proton current to transport water molecules from the anode to the cathode.
The upper limit of the thermal stability of the known foil or its sulphonic acid groups is about 90 to 100 at higher temperatures the morphological structure begins to break down.
The known perfluorinated ionomer membrane therefore deteriorates as an independent foil at higher operating temperatures thus making it unsuitable for the following applications: a) when hydrogen from reformed methanol is used as the fuel at temperatures above 130 °C (this process is described by U. Benz et al,. "Spektrum der Wissenschaft" (July 1995) 97-104); b) when used at temperatures above 130 typically 150 200 for direct oxidation of methanol at the anode.
Description of the invention The task of the present invention is to make available a membrane electrode unit for a fuel cell that complements the previously described advantageous properties of perfluorinated ionomer membranes with the following properties: 1. Reduction in production costs compared to the state-of-the-art polymer membrane P:WPDOCS\RE1\RpiX751958.doc-26MV7/ -4- 2. Reduction in pollutant when disposing of the unit.
3. Temperature resistance up to 200 0 C in the interests of reducing the effect of catalyst poisons, being able to use hydrogen from reformed methanol as a fuel, the internal reforming of methanol or direct oxidation of methanol.
The present invention seeks to solve this task for a membrane electrode unit as per the preamble by means of providing a membrane electrode unit for a fuel cell comprising an optionally catalyst-coated anode, an optionally catalyst-coated cathode and a proton conductor located between said anode and said cathode, characterised in that the proton conductor consists of a microfibre fleece material which has been impregnated with an electrolyte to the point of saturation; wherein the fleece material is chemically inert in relation to the electrolyte at temperatures of up to +200 0 C and in oxidising and reducing conditions and weighs 20 to 200g/m 2 wherein the thickness of the fleece is less than 1mm and the pore volume is 65 to 92%.
The present invention also seeks to provide that the microfibre fleece material has a median pore radius between 20nm and 10 pim.
S 20 The present invention also seeks to provide that the microfibre fleece material has been impregnated with hydrated zirconium phosophate or ammonium dihydrogen phosphate.
The present invention seeks to provide that, the fleece supporting structure of the microfibre fleece material provides the mechanical stability of the membrane so that the 25 electrolyte no longer needs to fulfill this task. This can reduce the material costs for the .o membrane by up to 90%, compared for example to the costs required to manufacture an equivalently dimensioned, independent membrane made of perfluorinated ionomer.
P:\WPDOCS\RET'speci\7519580.doc-26A07/01 -4a- The microfibre fleece material can be filled with perfluorinated ionomer where the perfluorinated ionomer could be a polytetrafluoroethylene with sulphonated perfluoro vinylether side chains. A possible alternative would be to impregnate the microfibre fleece material with one to 5 molar, aqueous sulphuric acid or with concentrated *oo phosphoric acid. Furthermore, it would also be possible to use hydrated zirconium phosphate and and ammonium dihydrogen phosphate.
The following examples serve to illustrate that the invention, in respect to the power output of the fuel cell (ionic conductivity), compares favourably with a pure polymer membrane made of perfluorinated ionomer without the need to use the costly materials required up to now.
Implementation of the invention All examples use the same base materials which will now be described: Fleece material: polysulphone fibres with a rectangular cross-section (width 6 to 13 .tm, height 1.7 to 2.4 gm).
Mechanical properties of the polysulphone material: melting range: 343 to 399 °C Tensile strength: 70 MPa Fracture strain: 50 to 100% E modulus: 2.4 GPa Bending temperature at a load of 1.8 MPa: 174 °C Production of the fibres: spinning from a solution of polysulphone in methylene chloride in an electrostatic field. This could for example be done using a device as per DE-OS 26 20 399. The fibres are collected on a linear, continuously moving, textile carrier.
Fleece properties: Weight: 150 g/m 2 Thickness (compressed): 0.05 mm i.
6 Thickness (impregnated with electrolyte): 0.18 mm Median pore radius in the uncompressed state: 8 Lm Median pore radius in the compressed state: 4 gm Pore volume: 83 The temperature resistance of the membrane in accordance with the invention, other things being equal, is essentially determined by the fleece material and thus breaks down at about 174 *C for pure polysulphone fibre material. As a consequence of the mechanical linkage of the fibres in the fleece material the mechanical stability can be extended even to temperatures of 250 This allows the fuel cell to be operated at high temperatures which can significantly reduce the amount of contamination of the anode catalyst.
Example 1: The microfibre fleece material was covered with a layer of liquid Nafion, a commercial perfluorinated ionomer from the DuPont company, in a 16 mm diameter fritted glass. By applying a light partial vacuum, the liquid phase was drawn into the pore structure of the fleece material. To remove all solvent, the membrane impregnated in this manner was treated at 60 'C in a drying chamber. The membrane can then be stored in distilled water until further processing.
Examples 2 to 4: The microfibre fleece material was impregnated with three different molar, aqueous sulphuric acid solutions analogous to example 1 however to reduce the viscosity, the sulphuric acid was heated to about 70 0 C. The fleece material can be boiled in the oC hot acid for several minutes without affecting the results.
It is advantageous to store the membrane obtained in this way in the actual impregnation medium used.
Using the method described in DIN 53 779, dated March 1979, the following specific conductivities were obtained for the membranes prepared in this way: Example measurement temperature oC specific conductivity S/cm 1 23 0.016 2 18 0.031 1M H 2 S04 3 18 0.041 3M H 2 S04 4 18 0.080
H
2 S0 4 25 0.070 (reference) Example 5 in the table represents a reference example for corresponding measurements on a 125 pm thick, state-of-the-art self-supporting polymer membrane made of perfluorinated ionomer (Nafion-117, DuPont).
1 1"4 8 The specific conductivity values (S/cm) clearly show that the membrane in accordance with the invention, which is considerably less expensive, of simpler construction and mechanically more robust than pure Nafion, can be used to operate a fuel cell at the typical power output for a state-of-the-art fuel cell. If used at temperatures above 100 0 C, concentrated phosphoric acid would be suitable as the ion conductor.
In comparison to other swollen Nafion membranes of for example 125 jAm thickness, the fleece material impregnated with electrolyte used in examples 1 to 4 is twice as thick.
The power output of the fuel cell, which is given by the product of the voltage and the current intensity, can not only be achieved by using higher acid concentrations, i.e.
higher specific conductivities S/cm, but also by decreasing the diffusion resistance by using thinner fleece material.
To illustrate this, Figure 1 shows the respective current/voltage curves at room temperature corresponding to the the examples 1, 3 and 5. It can be seen that, compared to the state-of-the-art membrane (example a comparable curve can be obtained for the membrane in accordance with the invention. The above described effects, of achieving a higher cell output by increasing the acid concentration or by using a thinner fleece material, would have the effect of shifting the curve in the positive direction on the Y axis on this graph.
Due to the high temperature resistance of the fleece, concentrated phosphoric acid could be used as the electrolyte for applications at temperatures above 100°C.
Documen135-25/07/D 8a- Throughout this specification and the claims which follow, unless the context requires otherwise, the word "comprise", and variations such as "comprises" or "comprising", will be understood to imply the inclusion of a stated integer or step or group of integers or steps but not the exclusion of any other integer or step or group of integers or steps.
The reference to any prior art in this specification is not, and should not be taken as, an acknowledgement or any form of suggestion that that prior art forms part of the common general knowledge in Australia.
ooee o*• *gig *•oo

Claims (8)

1. Membrane electrode unit for a fuel cell comprising an optionally catalyst-coated anode, an optionally catalyst-coated cathode and a proton conductor located between said anode and said cathode, characterised in that the proton conductor consists of a microfibre fleece material which has been impregnated with an electrolyte to the point of saturation; wherein the fleece material is chemically inert in relation to the electrolyte at temperatures of up to +200 °C and in oxidising and reducing conditions and weighs 20 to 200 g/m 2 wherein the thickness of the fleece is less than 1 mm and the pore volume is 65 to 92
2. Membrane electrode unit as per claim 1 characterised in that the microfibre fleece material has a median pore radius between 20 nm and 10 .tm.
3. Membrane electrode unit as per claims 1 or 2 characterised in that the microfibre fleece material is filled with perfluorinated ionomer.
4. Membrane electrode unit as per claim 3 characterised in that the perfluorinated ionomer is a polytetrafluoroethylene with sulphonated perfluoro vinylether side chains.
Membrane electrode unit as per claims 1 or 2 characterised in that the microfibre fleece material has been impregnated with a one to 5 molar, aqueous sulphuric acid solution.
6. Membrane electrode unit as per claims 1 or 2 characterised in that the microfibre fleece material has been impregnated with concentrated phosphoric acid.
7. Membrane electrode unit as per claims 1 or 2 characterised in that the microfibre fleece material has been impregnated with hydrated zirconium phosophate or ammonium dihydrogen phosphate. Doaim-05-3325/07A01 10
8. Membrane electrode unit for fuel cell, substantially as herein disclosed with reference to the accompanying figures. DATED this 25 1h day of July, 2001 FIRMA CARL FREUDENBERG By Their Patent Attorneys DAVIES COLLISON CAVE
AU37040/99A 1998-05-18 1999-04-01 Membrane-electrode unit for a fuel cell Ceased AU738679B2 (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE19821978 1998-05-18
DE19821978A DE19821978C2 (en) 1998-05-18 1998-05-18 Membrane electrode unit for a fuel cell
PCT/EP1999/002233 WO1999060650A1 (en) 1998-05-18 1999-04-01 Membrane-electrode unit for a fuel cell

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AU3704099A AU3704099A (en) 1999-12-06
AU738679B2 true AU738679B2 (en) 2001-09-27

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EP (1) EP1088361A1 (en)
JP (1) JP2002516472A (en)
KR (1) KR100392921B1 (en)
CN (1) CN1294762A (en)
AU (1) AU738679B2 (en)
BR (1) BR9910535A (en)
CA (1) CA2327520A1 (en)
DE (1) DE19821978C2 (en)
WO (1) WO1999060650A1 (en)
ZA (1) ZA200001232B (en)

Families Citing this family (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10101315A1 (en) * 2001-01-12 2002-07-25 Ulrich Stimming Fuel cell with proton-conducting solid electrolyte for operation in the temperature range 200-600 ° C
DE10208275A1 (en) * 2002-02-26 2003-09-04 Creavis Tech & Innovation Gmbh Flexible electrolyte membrane based on a carrier comprising polymer fibers, process for their production and the use thereof
AU2003248105A1 (en) * 2002-07-26 2004-02-16 Asahi Glass Company, Limited Polymer film, process for producing the same, and united membrane electrode assembly for solid polymer type fuel cell
JP4815759B2 (en) * 2003-06-30 2011-11-16 住友化学株式会社 Polymer electrolyte composite membrane, production method thereof and use thereof
CN100454623C (en) * 2004-04-28 2009-01-21 日产自动车株式会社 Membrane-electrode assembly for fuel cell and fuel cell using same
US9640805B2 (en) * 2005-10-17 2017-05-02 GM Global Technology Operations LLC Coating process for fuel cell components
DE102006036019A1 (en) * 2006-08-02 2008-02-07 Pemeas Gmbh Membrane electrode assembly and fuel cells with increased performance

Family Cites Families (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CA1002588A (en) * 1973-04-04 1976-12-28 Alfred D. Nelson Membrane of micro-fibers for fuel cells
DE2620399C3 (en) * 1976-05-08 1980-11-13 Fa. Carl Freudenberg, 6940 Weinheim Device for electrostatic spraying
JPS6337134A (en) * 1986-08-01 1988-02-17 Tokuyama Soda Co Ltd Fluorine-containing ion exchange membrane
ES2139376T3 (en) * 1995-07-27 2000-02-01 Aventis Res & Tech Gmbh & Co POLYMER ELECTROLYTES AND PROCEDURE FOR ITS PRODUCTION.
US5672438A (en) * 1995-10-10 1997-09-30 E. I. Du Pont De Nemours And Company Membrane and electrode assembly employing exclusion membrane for direct methanol fuel cell

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DE19821978C2 (en) 2002-06-06
EP1088361A1 (en) 2001-04-04
CN1294762A (en) 2001-05-09
BR9910535A (en) 2001-01-16
KR20010071286A (en) 2001-07-28
CA2327520A1 (en) 1999-11-25
DE19821978A1 (en) 1999-11-25
JP2002516472A (en) 2002-06-04
AU3704099A (en) 1999-12-06
ZA200001232B (en) 2002-05-13
KR100392921B1 (en) 2003-07-28
WO1999060650A1 (en) 1999-11-25

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