CN1294762A - Membrane-electrode unit for fuel cell - Google Patents

Membrane-electrode unit for fuel cell Download PDF

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Publication number
CN1294762A
CN1294762A CN99804275A CN99804275A CN1294762A CN 1294762 A CN1294762 A CN 1294762A CN 99804275 A CN99804275 A CN 99804275A CN 99804275 A CN99804275 A CN 99804275A CN 1294762 A CN1294762 A CN 1294762A
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China
Prior art keywords
nonwoven fabrics
membrane
electrode unit
microfibre
fuel cell
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Pending
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CN99804275A
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Chinese (zh)
Inventor
U·斯蒂明
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Carl Freudenberg KG
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Carl Freudenberg KG
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Publication of CN1294762A publication Critical patent/CN1294762A/en
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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)
  • Crystallography & Structural Chemistry (AREA)
  • Composite Materials (AREA)
  • Fuel Cell (AREA)
  • Inert Electrodes (AREA)

Abstract

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. The proton conductor consists of a microfibre-fleece material which has been impregnated with an electrolyte to the point of saturation. The fleece material is chemically inert in relation to the electrolyte at temperatures of up to +200 DEG C and in oxidizing and reducing conditions and weighs 20 to 200 g/m<2>. The thickness of the fleece is less than 1 mm and the pore volume is 65 to 92 %.

Description

The membrane-electrode unit that is used for fuel cell
The present invention relates to be used for the membrane-electrode unit of fuel cell, it comprises that one randomly randomly uses the proton conductor of negative electrode, between anode and negative electrode of catalyst-coated with the anode, of catalyst-coated.
A kind of like this unit is known.It causes separating of ion and electric channel when reacting gas that comprises hydrogen and oxygen or liquid component reaction in fuel cell, to realize the direct conversion of chemical energy to electric energy.
The character of fuel cells of different types and type of action are described in K.-D.Kreuer and J.Maier's " science rich and varied " (Spektrum der Wissenschaft) (Juli1995), 92-96.
Electrode must be fabulous electronic conductor (the about 0.1 Ω cm of resistance -l).It should be with the required reaction of electrolyte surface catalysis.Electrolyte must have high ionic conductivity and have alap electron conduction simultaneously.In addition, it must be impermeable as far as possible for output gas.Between all materials and and participate between the reactor should be chemically inert,, also not allow undesirable chemical combination each other at the strong oxidizing condition on the negative electrode and under the strong reducing condition on the anode.
For more monocell is connected into battery pile, must give the solid constituent that is contained in the monocell with enough mechanical bearing capacitys.In addition, the material of battery component and technology cost, life-span and Environmental compatibility also play an important role.
For 80-90 ℃ operating temperature, under the situation of fuel cell, the protonically conductive polymer film achieves the goal.This polymer film combines gives molecule and proton with the liquid properties of free migration and stable in shape solid performance.Perfluorinate ionomer based on the polytetrafluoroethylene with sulfonation perfluoroalkyl vinyl ether side chain has nearly ideally satisfied this requirement.This material is made up of hydrophobic and hydrophilic segment, and they have been decomposed to form gel under the situation of water but the film of dimensionally stable existing.The hydrophobic main chain of this polymer is very resistance to oxidation and reduction, even and also give the skeleton of film with dimensionally stable under solvent swelling state.The sulfonic acid side chain that contains hydrophilic, similar liquids of swelling makes fabulous proton conductive become possibility in water.The aperture of several nanometers is corresponding to the size of a little several hydrone.The existence of water makes the high proton animal migration in passage and hole become possibility.
Described as the document of being quoted, the shortcoming of this cation-exchanger is to cost an arm and a leg, because preparation technology expends very much.In addition, its discarded or recovery can cause ecological problem.
In service at fuel cell, these films are easy to drying, especially by air flow battery input burning oxygen, but based on the character of proton stream, when hydrone is delivered to negative electrode by anode.
Be limited to 90-100 ℃ on the thermal stability of known film or its sulfonic acid group, under higher temperature, morphosis begins collapse.
Therefore as the film of independence, known perfluorinate ionomeric membrane is not suitable for higher temperature, so that be not suitable for following application:
A) under surpassing 130 ℃ temperature, use hydrogen from the methyl alcohol that transforms act as a fuel (this method be described in U.Benz's etc. " science rich and varied " (Juli 1995) 97-104 in).
B) surpass 130 ℃, be used for direct oxidation methyl alcohol on anode under 150-200 ℃ the temperature usually.
Task of the present invention is, a kind of membrane-electrode unit that is used for fuel cell is provided, and it is except the favorable characteristics of above-mentioned perfluorinate ionomeric membrane, and it also has following performance:
1. with respect to the prior art polymers film, manufacturing cost reduces.
2. harmful substance reduces when discarded
3. help reducing the effect of catalyst poison until 200 ℃ temperature stability, from the applicability that the hydrogen of the methyl alcohol that transforms acts as a fuel, the inside of methyl alcohol transforms or the direct oxidation of methyl alcohol.
This task of the present invention is achieved by the membrane-electrode unit of claim 1.Provided advantageous embodiment in the dependent claims.
According to the present invention, proton conductor is made of the microfibre nonwoven fabrics, this nonwoven fabrics with electrolyte dipping until saturated, at this, this nonwoven fabrics is until+200 ℃ temperature and be chemically inert for electrolyte under oxidation and reducing condition.Wherein the weight of this nonwoven fabrics is 20-200g/m 2Nonwoven thickness is 1mm to the maximum and pore volume is 65-92%.
The average pore radius of this microfibre nonwoven fabrics should be 20nm to 10 μ m.
For theme of the present invention, the nonwoven fabrics skeleton of microfibre nonwoven fabrics is guaranteed the mechanical stability of film, so that electrolyte no longer must be realized this task.With respect to the expense of being made respective two-dimensional independence film by the perfluorinate ionomer, the material cost of film can reduce up to 90% thus.
The microfibre nonwoven fabrics can be filled with the perfluorinate ionomer, and wherein this perfluorinate ionomer can be the polytetrafluoroethylene with sulfonation perfluoroalkyl vinyl ether side chain.Scheme can be used the aqueous sulfuric acid of 1-5 molar concentration or flood the microfibre nonwoven fabrics with SPA as an alternative.Might use the basic zirconium phosphate and the ammonium dihydrogen phosphate of hydration in addition.
Following embodiment can illustrate that with regard to the power (ionic conductivity) of fuel cell, the present invention can mention in the same breath with the straight polymer film that is made of the perfluorinate ionomer, and need not to use expensive so far material.
In an embodiment, shared following basic material:
Nonwoven cloth material: polysulfone fibre with square-section (wide 6-13 μ m, high 1.7-2.4 μ m)
The engineering properties of polysulfone material: melting range: 343-399 ℃.
Tensile strength: 70MPa
Extension at break: 50-100%
E-modulus: 2.4GPa
Flexure temperature under the 1.8MPa load: 174 ℃
The manufacturing of fiber: in electrostatic field, the solution of polysulfones in carrene is carried out spinning.Can for example use the device of DE-OS 2620399 for this reason.On the weaving yarn guide of linear continuous motion, collect fiber.
The nonwoven fabrics performance:
Weight: 150g/m 2
Thickness (compression): 0.05mm
Thickness (flooding): 0.18mm with electrolyte
Average pore radius under the uncompressed state: 8 μ m
Average pore radius under the compressive state: 4 μ m
Pore volume: 83%
Therefore the temperature stability of film of the present invention if there is not other reason to hinder, basically by the nonwoven cloth material decision, and only just stops at about 174 ℃ for pure fiber material polysulfones.Because the mutual mechanical bond of fiber in the nonwoven fabrics, mechanical stability even bring up to temperature until 250 ℃.Therefore the high-temperature operation of fuel cell becomes possibility, and this can reduce the poisoning of anode catalyst greatly.
Embodiment 1
In the frit of 16mm diameter, layer overlay liquid Nafion on the microfibre nonwoven fabrics (the commercial perfluorinate ionomer that a kind of Firma DuPont produces).By applying the pore structure that slight negative pressure makes liquid phase enter nonwoven fabrics, with the film of dipping like this in drying cupboard in 60 ℃ of dried to remove solvent.Can hold it in the distilled water until further processing.
Embodiment 2-4:
Be similar to the aqueous sulfuric acid dipping microfibre nonwoven fabrics of 3 kinds of different molar concentrations of embodiment 1 usefulness, but wherein sulfuric acid be heated to about 70 ℃ for reducing viscosity.Also nonwoven fabrics a few minutes can be boiled in being heated to 70 ℃ acid and other result can be do not obtained.
Should in corresponding steeping medium, preserve the film that so obtains.
Use is according to the ratio conductivity of in March, 1979 film that makes by this way that DIN 53779 method detects
Embodiment Measure temperature ℃ Specific conductivity S/cm
????????1 ??????23 ????0．016
????????2 ????1MH 2SO 4 ??????18 ????0．031
????????3 ????3MH 2SO 4 ??????18 ????0．041
????????4 ????5MH 2SO 4 ??????18 ????0．080
5 comparative examples ??????25 ????0．070
(Nafion-117, the thickness of the prior art that DuPont) makes are the respective measurement values of the self-contained polymer film of 125 μ m by the perfluorinate ionomer in embodiment 5 representatives in the table.
Value than conductivity S/cm clearlys show, uses the present invention to compare the film of considerably cheaper, simple in structure and mechanically stable with pure Nafion, can realize having the fuel cell operation with the prior art corresponding power.For the application that surpasses 100 ℃ temperature, can use SPA as ion conductor.
Compare with the swelling Nafion film that 125 μ m are thick, being used for nonwoven fabrics embodiment 1-4, that flood with electrolyte is that its twice is thick.
The power of fuel cell (it is by long-pending the providing of voltage and current intensity) not only can be by higher acid concentration, and promptly higher specific conductivity S/cm reaches, and can reach by using thin nonwoven fabrics to reduce diffusional resistance.
Show to illustrative the current/voltage curve that corresponds respectively to embodiment 1,3 and 5 under the room temperature in the drawings.This figure shows, compares with prior art (embodiment 5), has obtained similar curve distribution by film of the present invention.The effect that reaches the higher power of battery by higher acid concentration or thin nonwoven cloth material above-mentioned is showed to moving of coordinate positive direction by curve in the figure.
Based on the high temperature stability of nonwoven fabrics,, also can use SPA as electrolyte in the application that surpasses under 100 ℃ the temperature.

Claims (7)

1. the membrane-electrode unit that is used for fuel cell, comprise an optional anode, the optional proton conductor of negative electrode, between anode and negative electrode with catalyst-coated with catalyst-coated, it is characterized in that, proton conductor is made of the microfibre nonwoven fabrics, this nonwoven fabrics floods until saturated with electrolyte, at this, this nonwoven fabrics is until+200 ℃ temperature and be chemically inert for electrolyte under oxidation and reducing condition, and wherein the weight of this nonwoven fabrics is 20-200g/m 2Nonwoven thickness is 65-92% less than 1mm and pore volume.
2. according to the membrane-electrode unit of claim 1, it is characterized in that the average pore radius of this microfibre nonwoven fabrics is 20nm to 10 μ m.
3. according to the membrane-electrode unit of claim 1 or 2, it is characterized in that this microfibre nonwoven fabrics is filled with the perfluorinate ionomer.
4. according to the membrane-electrode unit of claim 3, it is characterized in that described perfluorinate ionomer is the polytetrafluoroethylene with sulfonation perfluoroalkyl vinyl ether side chain.
5. according to the membrane-electrode unit of claim 1 or 2, it is characterized in that this microfibre nonwoven fabrics floods with the aqueous sulfuric acid of 1-5 molar concentration.
6. according to the membrane-electrode unit of claim 1 or 2, it is characterized in that this microfibre nonwoven fabrics floods with SPA.
7. according to the membrane-electrode unit of claim 1 or 2, it is characterized in that this microfibre nonwoven fabrics is with hydration basic zirconium phosphate or ammonium dihydrogen phosphate dipping.
CN99804275A 1998-05-18 1999-04-01 Membrane-electrode unit for fuel cell Pending CN1294762A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE19821978.4 1998-05-18
DE19821978A DE19821978C2 (en) 1998-05-18 1998-05-18 Membrane electrode unit for a fuel cell

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CN1294762A true CN1294762A (en) 2001-05-09

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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)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
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
CN101030643B (en) * 2005-10-17 2011-05-11 通用汽车环球科技运作公司 Coating process for fuel cell components

Families Citing this family (5)

* 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
JP4613614B2 (en) * 2002-07-26 2011-01-19 旭硝子株式会社 POLYMER MEMBRANE, METHOD FOR PRODUCING THE SAME, AND MEMBRANE ELECTRODE ASSEMBLY FOR SOLID POLYMER 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
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
CA2227835C (en) * 1995-07-27 2008-07-15 Hoechst Research & Technology Deutschland Gmbh & Co. Kg Polymeric electrolytes and process for their preparation
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

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
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
CN101030643B (en) * 2005-10-17 2011-05-11 通用汽车环球科技运作公司 Coating process for fuel cell components

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CA2327520A1 (en) 1999-11-25
ZA200001232B (en) 2002-05-13
BR9910535A (en) 2001-01-16
KR20010071286A (en) 2001-07-28
KR100392921B1 (en) 2003-07-28
EP1088361A1 (en) 2001-04-04
DE19821978C2 (en) 2002-06-06
DE19821978A1 (en) 1999-11-25
WO1999060650A1 (en) 1999-11-25
JP2002516472A (en) 2002-06-04
AU738679B2 (en) 2001-09-27
AU3704099A (en) 1999-12-06

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