WO1999060650A1 - Membran-elektroden-einheit für eine brennstoffzelle - Google Patents
Membran-elektroden-einheit für eine brennstoffzelle Download PDFInfo
- Publication number
- WO1999060650A1 WO1999060650A1 PCT/EP1999/002233 EP9902233W WO9960650A1 WO 1999060650 A1 WO1999060650 A1 WO 1999060650A1 EP 9902233 W EP9902233 W EP 9902233W WO 9960650 A1 WO9960650 A1 WO 9960650A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- membrane
- nonwoven fabric
- membrane electrode
- electrode unit
- electrolyte
- Prior art date
Links
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
-
- 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
Definitions
- the invention relates to a membrane electrode assembly for a fuel cell, comprising an anode optionally coated with a catalyst, a cathode optionally coated with a catalyst, and a proton conductor located between the anode and cathode.
- Such a unit causes a separation of the ionic and electrical path in the reaction of hydrogen and oxygen-containing reaction gases or flow components in a fuel cell for the direct conversion of chemical into electrical energy.
- the electrodes must be very good electron conductors (electrical resistance around 0.1 ⁇ cm "1 ). Together with the electrolyte surface, they should catalyze the required reaction.
- the electrolyte must have a high ionic conductivity have the lowest possible electronic conductivity. It must also be as impermeable as possible to the starting gases. All materials should be chemically inert with each other and with the reactants, so they must not enter into undesirable compounds with one another under the strongly oxidizing conditions on the cathode and the strongly reducing conditions on the anode.
- the solid components contained in the individual cells must have sufficient mechanical strength. Furthermore, material and process costs, lifespan and environmental compatibility of the cell components play an important role.
- Proton-conducting polymer membranes have become established in fuel cells for operating temperatures of 80 to 90 ° C. They combine the ability of liquids to give the molecules and protons free mobility and that of solids to be dimensionally stable. These requirements are almost ideally met by a perfluorinated ionomer membrane based on polytetrafluoroethylene with sulfonated perfluorovinyl ether side chains. This material consists of hydrophobic and hydrophilic areas that separate in the presence of water to form a gel-like but dimensionally stable membrane. The hydrophobic main chain of the polymer is very resistant to oxidation and reduction and gives the membrane a dimensionally stable structure even when swollen.
- the hydrophilic, liquid-like sulfonic acid-containing side chains swollen in water enable very good proton conductivity.
- the pore size of a few nanometers corresponds to the dimensions of a few water molecules.
- the presence of water enables high proton mobility in the channels and pores.
- such membranes tend to dry out, especially when the combustion oxygen is supplied to the cell by means of an air flow, but also because of the property of the proton flow, to transport water molecules from the anode to the cathode.
- the upper end of the thermal stability of the known film or its sulfonic acid groups is 90 to 100 ° C; the morphological structure begins to collapse at higher temperatures.
- the known perfluorinated ionomer membrane therefore closes at higher operating temperatures as an independent film, so that it is unsuitable for the following applications:
- the object of the invention is to provide a membrane-electrode unit for a fuel cell, which complements the advantageous properties of the perfluorinated ionomer membrane with the following properties:
- the proton conductor is formed by a microfiber nonwoven which is saturated with an electrolyte until saturated; wherein the nonwoven fabric is chemically inert to the electrolyte at temperatures up to +200 ° C and under oxidizing and reducing conditions, the nonwoven fabric weight being: 20 to 200 g / m 2 ; where the nonwoven thickness is at most 1 mm and where the pore volume is: 65 to 92%.
- the average pore radius of the microfiber nonwoven should be 20 nm to 10 ⁇ m.
- the nonwoven structure of the microfiber nonwoven ensures the mechanical stability of the membrane, so that the electrolyte no longer has to fulfill this task.
- the material costs for the membrane can be reduced by up to 90%, compared e.g. B. with the expenses for the production of a correspondingly dimensioned, independent membrane made of perfluorinated ionomer.
- the microfiber nonwoven fabric can be filled with perfluorinated ionomer, the perfluorinated ionomer being a polytetrafluoroethylene with sulfonated perfluorovinyle- ther side chains can be.
- perfluorinated ionomer being a polytetrafluoroethylene with sulfonated perfluorovinyle- ther side chains can be.
- Nonwoven material Polysulfone fibers with a rectangular cross-section (width 6 to 13 ⁇ m, height 1, 7 to 2.4 ⁇ m).
- Production of the fibers spinning a solution of polysulfone in methylene chloride in an electrostatic field.
- a device according to DE-OS 26 20 399 can be used.
- the fibers are collected on a linear, continuously moving, textile carrier.
- Nonwoven properties Weight: 150 g / m 2 thickness (compressed): 0.05 mm Thickness (impregnated with electrolyte): 0.18 mm Mean pore radii in the uncompressed state: 8 ⁇ m Mean pore radii in the compressed state: 4 ⁇ m pore volume: 83%
- the temperature resistance of the membrane according to the invention is, unless there are other reasons to the contrary, essentially determined by the nonwoven material and consequently only ends at about 174 ° C. for the pure fiber material polysulfone.
- the mechanical stability also increases up to temperatures of 250 ° C. This enables high-temperature operation of the fuel cell, which can significantly reduce the poisoning of the anode catalyst.
- microfiber nonwoven is overlaid with liquid Nafion, a commercially available, perfluorinated ionomer from DuPont, in a glass frit with a diameter of 16 mm.
- liquid Nafion a commercially available, perfluorinated ionomer from DuPont
- the liquid phase is drawn into the pore structure of the nonwoven.
- the membrane soaked is treated in a drying cabinet at 60 ° C. Storage until further processing is then possible in distilled water.
- microfiber nonwoven fabric is impregnated with three different molar, aqueous sulfuric acid solutions analogously to Example 1, but the sulfuric acid is heated to about 70 ° C. to reduce the viscosity. Without obtaining any other result, the nonwoven fabric can also be boiled for a few minutes in the acid heated to 70 ° C.
- the membrane thus obtained is expediently stored in the corresponding impregnation medium.
- Example 5 in the table represents a comparative example for corresponding measurements on a 125 ⁇ m thick, self-supporting polymer membrane of the prior art made of perfluorinated ionomer (Naf ⁇ on-117, DuPont).
- the values for the specific conductivity S / cm clearly show that the operation of a fuel cell with the state of the art is possible with the membrane according to the invention, which is considerably less expensive, structurally simple and mechanically more resistant than pure Nafion.
- Concentrated phosphoric acid can be used as an ion conductor for use at temperatures above 100 ° C.
- the nonwovens soaked with electrolyte used in Examples 1 to 4 are twice as thick.
- the figure shows the corresponding current / voltage curves at room temperature, which correspond to Examples 1, 3 and 5. It follows that, compared with the prior art (Example 5), comparable curves are achieved through the membranes according to the invention.
- the above-mentioned effects of higher cell output due to higher acid concentration or thinner nonwoven materials would have an effect in this representation by shifting the curves in the positive direction of the ordinate.
- concentrated phosphoric acid can also be used as electrolytes for applications at temperatures above 100 ° C.
Landscapes
- 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)
Abstract
Description
Claims
Priority Applications (5)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
BR9910535-7A BR9910535A (pt) | 1998-05-18 | 1999-04-01 | Unidade de eletrodo de membrana para uma célula de combustìvel |
AU37040/99A AU738679B2 (en) | 1998-05-18 | 1999-04-01 | Membrane-electrode unit for a fuel cell |
CA002327520A CA2327520A1 (en) | 1998-05-18 | 1999-04-01 | Membrane-electrode unit for a fuel cell |
JP2000550170A JP2002516472A (ja) | 1998-05-18 | 1999-04-01 | 燃料電池用膜電極ユニット |
EP99919173A EP1088361A1 (de) | 1998-05-18 | 1999-04-01 | Membran-elektroden-einheit für eine brennstoffzelle |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE19821978A DE19821978C2 (de) | 1998-05-18 | 1998-05-18 | Membran-Elektroden-Einheit für eine Brennstoffzelle |
DE19821978.4 | 1998-05-18 |
Publications (1)
Publication Number | Publication Date |
---|---|
WO1999060650A1 true WO1999060650A1 (de) | 1999-11-25 |
Family
ID=7867976
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/EP1999/002233 WO1999060650A1 (de) | 1998-05-18 | 1999-04-01 | Membran-elektroden-einheit für eine brennstoffzelle |
Country Status (10)
Country | Link |
---|---|
EP (1) | EP1088361A1 (de) |
JP (1) | JP2002516472A (de) |
KR (1) | KR100392921B1 (de) |
CN (1) | CN1294762A (de) |
AU (1) | AU738679B2 (de) |
BR (1) | BR9910535A (de) |
CA (1) | CA2327520A1 (de) |
DE (1) | DE19821978C2 (de) |
WO (1) | WO1999060650A1 (de) |
ZA (1) | ZA200001232B (de) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2003073545A2 (de) * | 2002-02-26 | 2003-09-04 | Creavis Gesellschaft Für Technologie Und Innovation Mbh | Flexible elektrolytmembran auf basis eines polymerfasern umfassenden trägers, verfahren zu deren herstellung und die verwendung derselben |
Families Citing this family (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE10101315A1 (de) * | 2001-01-12 | 2002-07-25 | Ulrich Stimming | Brennstoffzelle mit protonenleitendem Festelektrolyt für den Betrieb im Temperaturbereich 200-600 DEG C |
CN1308381C (zh) * | 2002-07-26 | 2007-04-04 | 旭硝子株式会社 | 高分子膜、其制造方法及固体高分子型燃料电池用膜电极接合体 |
JP4815759B2 (ja) * | 2003-06-30 | 2011-11-16 | 住友化学株式会社 | 高分子電解質複合膜、その製造方法及びその用途 |
CN100454623C (zh) * | 2004-04-28 | 2009-01-21 | 日产自动车株式会社 | 燃料电池用膜-电极接合体以及使用其的燃料电池 |
US9640805B2 (en) * | 2005-10-17 | 2017-05-02 | GM Global Technology Operations LLC | Coating process for fuel cell components |
DE102006036019A1 (de) * | 2006-08-02 | 2008-02-07 | Pemeas Gmbh | Membran-Elektroden-Einheit und Brennstoffzellen mit erhöhter Leistung |
Citations (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE2416520A1 (de) * | 1973-04-04 | 1974-10-24 | Minnesota Mining & Mfg | Matrixaufbau fuer brennstoffzellen |
JPS6337134A (ja) * | 1986-08-01 | 1988-02-17 | Tokuyama Soda Co Ltd | 含フツ素系イオン交換膜 |
WO1997005191A1 (de) * | 1995-07-27 | 1997-02-13 | Hoechst Research & Technology Deutschland Gmbh & Co. Kg | Polymerelektrolyte und verfahren zu deren herstellung |
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 |
Family Cites Families (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE2620399C3 (de) * | 1976-05-08 | 1980-11-13 | Fa. Carl Freudenberg, 6940 Weinheim | Vorrichtung zum elektrostatischen Versprühen |
-
1998
- 1998-05-18 DE DE19821978A patent/DE19821978C2/de not_active Expired - Fee Related
-
1999
- 1999-04-01 JP JP2000550170A patent/JP2002516472A/ja active Pending
- 1999-04-01 EP EP99919173A patent/EP1088361A1/de not_active Withdrawn
- 1999-04-01 BR BR9910535-7A patent/BR9910535A/pt not_active IP Right Cessation
- 1999-04-01 WO PCT/EP1999/002233 patent/WO1999060650A1/de not_active Application Discontinuation
- 1999-04-01 CN CN99804275A patent/CN1294762A/zh active Pending
- 1999-04-01 KR KR10-2000-7012939A patent/KR100392921B1/ko not_active IP Right Cessation
- 1999-04-01 CA CA002327520A patent/CA2327520A1/en not_active Abandoned
- 1999-04-01 AU AU37040/99A patent/AU738679B2/en not_active Ceased
-
2001
- 2001-02-13 ZA ZA200001232A patent/ZA200001232B/xx unknown
Patent Citations (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE2416520A1 (de) * | 1973-04-04 | 1974-10-24 | Minnesota Mining & Mfg | Matrixaufbau fuer brennstoffzellen |
JPS6337134A (ja) * | 1986-08-01 | 1988-02-17 | Tokuyama Soda Co Ltd | 含フツ素系イオン交換膜 |
WO1997005191A1 (de) * | 1995-07-27 | 1997-02-13 | Hoechst Research & Technology Deutschland Gmbh & Co. Kg | Polymerelektrolyte und verfahren zu deren herstellung |
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 |
Non-Patent Citations (1)
Title |
---|
DATABASE WPI Section Ch Week 8813, Derwent World Patents Index; Class A18, AN 88-087250, XP002113869 * |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2003073545A2 (de) * | 2002-02-26 | 2003-09-04 | Creavis Gesellschaft Für Technologie Und Innovation Mbh | Flexible elektrolytmembran auf basis eines polymerfasern umfassenden trägers, verfahren zu deren herstellung und die verwendung derselben |
WO2003073545A3 (de) * | 2002-02-26 | 2005-01-06 | Creavis Tech & Innovation Gmbh | Flexible elektrolytmembran auf basis eines polymerfasern umfassenden trägers, verfahren zu deren herstellung und die verwendung derselben |
Also Published As
Publication number | Publication date |
---|---|
AU3704099A (en) | 1999-12-06 |
AU738679B2 (en) | 2001-09-27 |
ZA200001232B (en) | 2002-05-13 |
KR100392921B1 (ko) | 2003-07-28 |
BR9910535A (pt) | 2001-01-16 |
DE19821978C2 (de) | 2002-06-06 |
KR20010071286A (ko) | 2001-07-28 |
EP1088361A1 (de) | 2001-04-04 |
JP2002516472A (ja) | 2002-06-04 |
CA2327520A1 (en) | 1999-11-25 |
DE19821978A1 (de) | 1999-11-25 |
CN1294762A (zh) | 2001-05-09 |
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