EP1579524A2 - Katalysatorhaltiges gasverteilersubstrat für brennstoffzellen sowie verfahren zu dessen herstellung - Google Patents
Katalysatorhaltiges gasverteilersubstrat für brennstoffzellen sowie verfahren zu dessen herstellungInfo
- Publication number
- EP1579524A2 EP1579524A2 EP03789404A EP03789404A EP1579524A2 EP 1579524 A2 EP1579524 A2 EP 1579524A2 EP 03789404 A EP03789404 A EP 03789404A EP 03789404 A EP03789404 A EP 03789404A EP 1579524 A2 EP1579524 A2 EP 1579524A2
- Authority
- EP
- European Patent Office
- Prior art keywords
- catalyst
- containing gas
- gas distributor
- diffusion layer
- substrate
- Prior art date
- Legal status (The legal status 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 status listed.)
- Withdrawn
Links
Classifications
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
- H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
- H01M4/926—Metals of platinum group supported on carriers, e.g. powder carriers on carbon or graphite
-
- 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
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
-
- 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
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
- H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
- H01M8/0668—Removal of carbon monoxide or carbon dioxide
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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
- H01M8/10—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
- H01M8/1007—Fuel cells with solid electrolytes with both reactants being gaseous or vaporised
-
- 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
- H01M8/1009—Fuel cells with solid electrolytes with one of the reactants being liquid, solid or liquid-charged
- H01M8/1011—Direct alcohol fuel cells [DAFC], e.g. direct methanol fuel cells [DMFC]
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
- H01M2300/0082—Organic polymers
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- 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 catalyst-containing gas distributor substrate for " fuel cells, in particular low-temperature fuel cells (such as PEMFC or DMFC), which have an ion-conducting polymer as the electrolyte.
- the gas distributor substrate is used on the anode side of the fuel cell and contains catalyst components which remove or remove carbon monoxide (CO), for example
- CO carbon monoxide
- a product can be used in membrane electrode assemblies (MEEs) for low-temperature fuel cells, for example PEM fuel cells, which are operated with CO-containing reformate gas but can also be used for direct methanol fuel cells (DMFC).
- MEEs membrane electrode assemblies
- Fuel cells convert a fuel and an oxidizing agent locally separated from each other on two electrodes into electricity, heat and water. Hydrogen, methanol or a hydrogen-rich gas can be used as fuel, oxygen or air as oxidizing agent.
- the process of energy conversion in the fuel cell is characterized by a high level of pollution-free and particularly high efficiency. For this reason, fuel cells are becoming increasingly important for alternative drive concepts, home energy supply systems and portable applications.
- the membrane fuel cells for example the polymer electrolyte fuel cell (English: PEMFC) and the Direlrt methanol fuel cell (English: DMFC), are suitable for many mobile and stationary applications due to their low operating temperatures, their compact design and their power density.
- PEMFC polymer electrolyte fuel cell
- DMFC Direlrt methanol fuel cell
- PEM fuel cells are constructed in a stacked arrangement ("stack") from many fuel cell units. These are electrically connected in series to increase the operating voltage.
- Each fuel cell unit contains a 5-layer membrane electrode unit ("MEE") which is between bipolar plates, also called separator plates, is arranged for gas supply and power conduction.
- MEE 5-layer membrane electrode unit
- Such a 5- Layered membrane electrode unit is in turn constructed from a polymer electrolyte membrane, which is provided with an electrode layer on each side (3-layer, catalyst-coated membrane, CCM).
- One of the electrode layers is designed as an anode for the oxidation of hydrogen and the second electrode layer as a cathode for the reduction of oxygen.
- the polymer electrolyte membrane consists of proton-conducting polymers.
- the anode and cathode of the CCM contain electrocatalysts that catalytically support the respective reaction (oxidation of hydrogen or reduction of oxygen).
- the metals of the platinum group of the periodic table of the elements are preferably used as catalytically active components. So-called supported catalysts are used in the majority.
- gas diffusion layers So-called gas diffusion layers (GDLs or "backings") are then attached to the two sides of the CCM, so that the five-layer membrane electrode assembly is thereby obtained.
- the gas distributor substrates usually consist of carbon fiber paper or carbon fiber fabric and enable one good access of the reaction gases to the reaction layers and good drainage of the cell flow and the water that forms.
- Typical hydrogen-containing fuel gases which are generated by reforming hydrocarbons such as natural gas, methane, petroleum, gasoline or alcohols, contain up to 2-3 vol.% Carbon monoxide (CO) depending on the cleaning process.
- CO Carbon monoxide
- the carbon monoxide components in turn poison the Pt or PtRu anode catalyst and thus lead to one
- EP 0 736 921 B1 describes an electrode which contains two different catalytic components.
- the first catalytic component is active for gas phase reaction sites, while the second catalytic component is active at electrochemical reaction sites.
- Both catalytic components are applied to the gas distributor substrate as a double layer (“bi-layer”) and are in mutual relationship
- WO 00/36679 describes a gas distribution substrate (“backing”) for a PEM anode
- Gas phase active catalyst and electrocatalyst are both formed as thin layers and as such are not
- EP 0 985 241 describes an integral PEM fuel cell stack which has an anode which is designed as a three-layer anode. This has a CO oxidation-selective catalyst layer on the side facing away from the membrane and an electrochemically active layer on the side facing the membrane.
- a low-temperature (PEM) fuel cell which likewise contains a gas diffusion layer with a CO oxidation catalyst.
- the CO oxidation catalyst is in a mixture of conductive material (eg carbon black) and water-repellent material (eg PTFE) processed into a porous film and applied to the gas diffusion layer.
- the residence time of the CO-containing fuel gas on the catalyst material is reduced. This leads to only a partial conversion and thus to incomplete CO oxidation.
- the gas-phase-active catalysts are used in the form of prefabricated supported catalysts (for example Ru on carbon black, Pt on aluminum oxide) and then processed further in a mixture with carbon black, Teflon and possibly other components. In many cases, the active catalyst surface is blocked by these additional components. This means that the active catalyst surface is not used optimally, which in turn means that the last residues of CO (e.g. fractions below 100 ppm) are not removed. This means that CO poisoning of the electrocatalysts continues to take place on the anode of the fuel cell stack.
- the invention relates to a catalyst-containing gas diffusion layer for
- the catalyst-containing gas distributor substrate in the catalyst-containing gas distributor substrate according to the invention, a good utilization of the catalyst or the catalyst surface 0 and thus a high activity and selectivity in the removal of carbon monoxide (either by CO oxidation or by methanization) and in the oxidation of methanol (in the DMFC). Furthermore, the method according to the invention for producing such gas distributor substrates is characterized by a low level of complexity. It is practical and can be easily integrated into a continuous manufacturing process, which 5 reduces manufacturing costs.
- the catalyst-containing gas diffusion layer according to the invention contains a catalytically active component; which is evenly distributed over the entire volume of the gas distributor substrate. It can be generated in a process in which precursors are soluble like water
- a gas diffusion layer is impregnated or impregnated with an aqueous solution of a precursor (e.g. with an easily decomposable metal compound). This potion process can
- the gas diffusion layer is placed in a tub that contains a solution of the metal compound, then removed and dried. The process is
- occupancy quantities are in
- the catalyst component is uniformly distributed over the entire volume of the substrate and preferably the catalytically active particles are fixed on the support material. This ensures optimal distribution of the particles in the substrate as well as very good accessibility of the reactants
- the impregnation or impregnation process can be carried out continuously in suitable devices, for example from roll to roll.
- the gas distribution substrate can be used as an endless, flexible belt and can be guided through various stations, consisting, for example, of hydrophobization, impregnation / impregnation with precursor solution, drying, coating with a compensating layer and tempering.
- the impregnation or impregnation with the precursor compound can thus be easily incorporated into a continuous manufacturing process for gas distributor substrates. It causes low additional costs, but at the same time leads to a higher quality product.
- the tempering that can be used to decompose the precursors and at which the
- 35 catalyst particles are formed, one usually leads at temperatures from 200 to
- 900 ° C preferably 200 to 600 ° C through. It can be in an air atmosphere, but also under Shielding gas (for example nitrogen, argon or mixtures thereof) or reducing gases (for example nitrogen / hydrogen mixtures or forming gas).
- Shielding gas for example nitrogen, argon or mixtures thereof
- reducing gases for example nitrogen / hydrogen mixtures or forming gas.
- Continuous belt furnaces, muffle furnaces, chamber furnaces and combinations thereof can be used.
- Ru, PfRu or Pt alloys with base metals are preferred.
- Gold-containing catalysts such as Au, Au / titanium oxide or .Au / iron oxide can also be used.
- Supported silver-containing catalysts for example Ag / titanium oxide can also be used.
- For the methanation of CO according to Eq. (2) are suitable, for example, catalysts based on nickel and / or ruthenium.
- the operating temperatures of the cell should preferably be slightly above the normal temperatures of the PEM fuel cell when using gas distribution substrates with a methanation catalyst. At operating temperatures of over 90 ° C, an increase in the methanation activity of the catalyst is achieved and, at the same time, the CO poisoning of the Pt-containing anode catalyst is suppressed.
- the precursors for the catalytically active components are water-soluble, easily decomposable metal compounds, preferably compounds from the group of amine nitrates, nitrates, carbonates, carboxylates, hydrooxycarboxylates, acetates, lactates, butanoates, oxalates, formates, octanoates, or ethylhexanoates, which are used in the Decompose the desired catalyst particles.
- Preferred catalytic articles include metals, in particular noble metals such as Pt, Pd, Ru. Rh, Au, Ag, Ir, Os. and / or their oxides, and / or their mixtures or alloys with base metals, but also base metals such as Ti, Fe. Co, Mn, Cr or Ni. Corrosion greens are used to avoid halogen- or chlorine-containing precursors if possible.
- organometallic complexes of the metals, so-called resinates can also be used, for example.
- Suitable noble metal compounds are the Pt precursors platinum (II) nitrate, platinum (II) lactate, platinum (II) amine nitrate, ethylammonium platinum hexahydrate, platinum acetate etc.
- suitable Ru precursors are ruthenium (III) nitrosyl nitrate or ruthenium (III) acetate.
- Au-containing precursors are gold resinates such as Au polymer esters (from FERRO GmbH, Frankfurt) or gold-containing complex salts. Analog complexes of the other noble metals can of course also be used.
- Precursors for base metals that can be used alone or in combination with the noble metal precursors are, for example, cobalt (II) nitrate, manganese (II) oxalate, chromium (III) nitrate, nickel (II) nitrate, iron (II) -carbonate and comparable compounds other elements such as the base metals listed above.
- cobalt (II) nitrate manganese (II) oxalate
- chromium (III) nitrate chromium
- nickel (II) nitrate nickel
- iron (II) -carbonate iron
- halogen-containing precursors are avoided for reasons of corrosion.
- additional components can be added to the noble metal and base metal precursors described, which act as cocatalysts, as support materials or as precursors thereof.
- these are high-surface precious metal tubes, fine metal powders, carbon blacks, pyrogenic oxides such as, for example, silica (“Aerosil” from Degussa), pyrogenic titanium oxides and comparable materials.
- pyrogenic oxides such as, for example, silica (“Aerosil” from Degussa)
- pyrogenic titanium oxides such as, for example, silica (“Aerosil” from Degussa)
- other inorganic components that can be converted into oxidic materials during pyrolysis or temperature treatment Examples of these are organic silicon esters, organosilanes, organotitanates, organostannates, aluminates, borates and similar compounds.
- the precursor compounds are processed into a preparation that is suitable for the respective application process on the gas distributor substrate.
- a correspondingly low-viscosity solution is produced for the application in the immersion or impregnation process.
- This can contain auxiliaries such as surfactants, wetting agents, binders, thickeners, anti-settling agents or organic solvents to improve the processing properties.
- auxiliaries such as surfactants, wetting agents, binders, thickeners, anti-settling agents or organic solvents to improve the processing properties.
- the viscosity of the solutions is modified accordingly. Means and ways of doing this are known to the skilled worker.
- Porous carbon fiber substrates can be used as starting materials for the production of the catalyst-containing gas diffusion layer according to the invention.
- Porous carbon fiber substrates carbon fiber paper or carbon fiber fabric
- These materials usually have a porosity of 60 to 90% and an average pore diameter of 20 to 50 ⁇ m.
- substrate materials that differ in structure, manufacturing process and properties. Examples of such porous materials are Toray paper,
- metal mesh fine, is also used as the starting material for gas distributor substrates
- Metal nets conductive coated plastic fabrics, conductive coated textile fabrics, coated glass fibers and similar materials can be used. Basically, they can
- the catalyst-containing gas diffusion layer according to the invention can be with or without
- Equalization layer must be equipped.
- a layer on that side of the gas distributor substrate is used as a compensating layer (so-called “microlayer”) understood, which is in contact with the electrode layer in the fuel cell.
- the leveling layer usually contains a mixture of a hydrophobic polymer such as PTFE and finely divided carbon blacks.
- the compensation layer is usually applied by screen printing, its thickness is, for example, from 5 to 100 ⁇ m.
- a complete membrane electrode assembly (“MEE") of a PEM or DMFC fuel cell contains a catalyst-coated polymer electrolyte membrane (“CCM”) with gas distributor substrates attached on both sides.
- the gas distributor substrate according to the invention is preferably used on the anode side of the membrane electrode unit.
- the membrane electrode assemblies thus produced can be used as fuel gas due to the improved tolerance to carbon monoxide for the use of CO-containing hydrogen mixtures.
- Such fuel gases are often produced by reforming hydrocarbons such as natural gas, methane or gasoline and are used in the stationary use of the fuel cell.
- the catalyst-containing gas diffusion layer according to the invention can also be used in MEEs for direct methanol fuel cells (DMFC).
- DMFC direct methanol fuel cells
- it causes better oxidation of the methanol on the anode side and improves the performance of the DMFC cell.
- Figure 1 Schematic representation of the inventive kata 'lysator inconveniencen gas diffusion layer with compensation layer
- Figure 1 shows a schematic cross section through an inventive catalyst-containing gas diffusion layer.
- (11) denotes the porous substrate material.
- the catalyst particles (12) are fixed to the surface of the substrate and are evenly distributed over the entire volume of the substrate. They are therefore optimally accessible, for example for a fuel gas contaminated with CO.
- Figure 2 Complete 5-layer membrane electrode assembly with a catalyst-containing gas distribution substrate according to the invention on the anode side.
- FIG. 2 shows a schematic cross section through a complete 5-layer MEU with a gas distributor substrate (21) according to the invention containing catalyst particles (22) on the anode side.
- the gas distributor substrate (21) is in contact with a three-layer catalyst-coated ionomer membrane, consisting of an anode catalyst layer (23a), Ionomer membrane (23) and cathode catalyst layer (23b).
- An uncatalyzed gas diffusion layer (24) is attached to the cathode side.
- the two gas distributor substrates do not have a compensation layer.
- a hy 'drophobiertes Kohlefase ⁇ apier serves the area as a starting material 50 cm 2 (dimensions of about 7x7 cm) with a thickness of 200 microns (Sigracet 10, Fa. SGL Carbon).
- the Teflon content is approx. 8% by weight.
- the substrate is immersed in a large dish with ruthenium (III) acetate solution (5% by weight Ru in water, OMG, Hanau). After complete wetting, the substrate is removed from the immersion bath using tweezers. It is allowed to drain for a short time and then dried in a drying cabinet at 100 ° C. for 15 minutes.
- the mixture is then allowed to cool and the amount of Ru acetate absorbed is determined gravimetrically.
- the dipping process is repeated three times until a loading of 0.85 mg -Ru acetate / cm 2 is obtained.
- the gas distributor substrate is then tempered for 30 minutes in an oven at 200 ° C. under forming gas (95% by volume nitrogen, 5% by volume hydrogen). After the substrate has cooled, the Ru content of the substrate is 0.48 mg Ru / cm 2 .
- the Ru particles are evenly distributed in the substrate and fixed on the substrate surface. They have an average particle size of 5 nm, measured by means of transmission electron spectroscopy (TEM).
- a leveling layer made of carbon black / PFTE is applied by screen printing, dried and annealed at 390 ° C. for 10 minutes.
- the layer thickness of the compensation layer is approx. 20 ⁇ m.
- the substrate is combined as a pre-anode with a catalyst-coated membrane (CCM) and combined to form a membrane electrode assembly (MEE).
- CCM catalyst-coated membrane
- MEE membrane electrode assembly
- a CC-coated membrane of type 6 C is used as CCM (loading anode 0.2 mg Pt / cm 2 ; loading cathode 0.4 mg Pt / cm 2 , membrane EW 1100 with 50 micron thickness, from OMG, Hanau).
- a hydrophobized carbon fiber paper with a compensating layer (standard, from SGL, type Sigracet 10) is used on the cathode side.
- the MEE is tested in a PEM fuel cell in hydrogen / air and reformate / air operation and shows very good results, especially in reformate / air operation with a content of 100 ppm CO (see Table 1).
- the tolerance towards CO is significantly improved. This shows that the catalyst-containing gas diffusion layer according to the invention has a very good effectiveness.
- a hydrophobicized carbon fiber paper with an area of 50 cm 2 (dimensions approx. 7x7 cm) and a thickness of 200 ⁇ m (Sigracet 10, SGL Carbon) is used as the starting material.
- the Teflon content is approx. 8% by weight.
- the impregnation with precursor solution is carried out as described in Example 1.
- the dipping process is repeated twice until a loading of 0.5 mg Ru acetate / cm 2 is obtained.
- the gas distributor substrate is then tempered for 30 minutes in an oven at 250 ° C. under forming gas (95% by volume nitrogen, 5% by volume hydrogen). After the substrate has cooled, the Ru content of the substrate is 0.28 mg Ru / cm 2 .
- the Ru particles are evenly distributed in the substrate and fixed on the substrate surface. They have an average particle size of 4 nm (measured with TEM).
- the substrate is combined as a pre-anode with a catalyst-coated membrane (CCM) and, as described in Example 1, combined to form a membrane electrode unit (MEE).
- CCM catalyst-coated membrane
- MEE membrane electrode unit
- This example describes the production of an Au / Ti0 2 -containing gas distribution substrate without a compensation layer.
- a hydrophobized carbon fiber paper with an area of 50 cm 2 (dimensions approx. 7x7 cm) and a thickness of 200 ⁇ m (Sigracet 10, SGL Carbon) is again used as the starting material.
- the Teflon content is approx. 8% by weight.
- a water-containing precursor solution is produced containing Au polymer ester HF 3401 (from FERRO, Frankfurt) and titanium oxide (type P25, from Degussa, Frankfurt).
- the Au content of the solution is 5% by weight of Au, the proportion of titanium oxide is 0.1% by weight.
- the impregnation is carried out as described in Example 1. The diving process is repeated three times.
- the gas distributor substrate is annealed for 30 min in an oven at 250 ° C. under forming gas.
- the Au content of the substrate is approximately 0.1 mg Au / cm 2 .
- the Au particles are evenly distributed in the substrate in combination with the titanium oxide.
- the substrate is combined as a pre-anode with a catalyst-coated membrane (CCM) and joined to form a membrane electrode assembly (MEE) 5.
- CCM catalyst-coated membrane
- MEE membrane electrode assembly
- a hydrophobicized carbon fiber paper with an area of 50 cm 2 (dimensions approx. 7x7 cm) and a thickness of 200 ⁇ m (Sigracet 10, SGL Carbon) is used as the starting material.
- the Teflon content is approx. 8 " % by weight.
- the catalyst-free substrate is added
- a hydrophobicized carbon fiber paper with an area of 50 cm 2 (dimensions approx. 7x7 cm) and a thickness of 200 ⁇ m (Sigracet 10, SGL Carbon) is used as the starting material.
- the Teflon content is approx. 8% by weight. After the weight has been determined using a laboratory balance, the substrate is placed in a large bowl with 6 parts of ruthenium (III) acetate.
- the Ru content of the substrate is approximately 0.65 mg Ru / cm 2 and the platinum content is approximately 0.35 mg Pt / cm 2 .
- the Pt and Ru particles are evenly distributed over the entire volume of the substrate.
- the substrate is combined as a pre-anode with a catalyst-coated membrane (CCM, type R22 anode loading 0.3 mg Pt / cm 2 and 0.15 mg Ru / cm 2 , cathode loading 0.4 mg Pt / cm 2 ; OMG, Hanau) and, as described in Example 1, combined to form a membrane electrode assembly (MEE).
- CCM catalyst-coated membrane
- MEE membrane electrode assembly
- This is installed in a " Direlct-methanol fuel cell (DMFC) with an active cell area of 50 cm 2.
- DMFC Direlct-methanol fuel cell
- a 2-molar methanol / water solution is used for the measurement, the cell temperature is 60 ° C. Air in the A very high power density (peak power density) of over 80
- a fuel gas mixture of 60% by volume H 2 , 15% by volume N 2 and 25% by volume C0 2 is used as the anode gas.
- 100 ppm CO with an "airbleed" of 1% by volume or 3% by volume of air is added to the fuel gas.
- This fuel gas mixture simulates a reformate gas which can be obtained by reforming methane or hydrocarbons by means of steam reforming and subsequent purification stages Air is used as the cathode gas.
- the cell temperature is 75 ° C.
- the pressure of the working gases is 3 bar (absolute).
- the stoichiometry of the gases is 1.5 (anode gas) and 2.0 (cathode gas).
- the MEEs are in a cell with 50 cm 2 of active area according to OMG standard conditions
- Table 1 The results for Examples 1, 2 and 3 and for Comparative Example VB 1 are summarized in Table 1.
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Materials Engineering (AREA)
- Inert Electrodes (AREA)
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Abstract
Description
Claims
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP03789404A EP1579524A2 (de) | 2002-12-30 | 2003-12-23 | Katalysatorhaltiges gasverteilersubstrat für brennstoffzellen sowie verfahren zu dessen herstellung |
Applications Claiming Priority (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP02029084 | 2002-12-30 | ||
EP02029084A EP1435672A1 (de) | 2002-12-30 | 2002-12-30 | Katalysatorhaltiges Gasverteilersubstrat für Brennstoffzellen sowie Verfahren zu dessen Herstellung |
EP03789404A EP1579524A2 (de) | 2002-12-30 | 2003-12-23 | Katalysatorhaltiges gasverteilersubstrat für brennstoffzellen sowie verfahren zu dessen herstellung |
PCT/EP2003/014839 WO2004059770A2 (de) | 2002-12-30 | 2003-12-23 | Katalysatorhaltiges gasverteilersubstrat für brennstoffzellen sowie verfahren zu dessen herstellung |
Publications (1)
Publication Number | Publication Date |
---|---|
EP1579524A2 true EP1579524A2 (de) | 2005-09-28 |
Family
ID=32479734
Family Applications (2)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP02029084A Withdrawn EP1435672A1 (de) | 2002-12-30 | 2002-12-30 | Katalysatorhaltiges Gasverteilersubstrat für Brennstoffzellen sowie Verfahren zu dessen Herstellung |
EP03789404A Withdrawn EP1579524A2 (de) | 2002-12-30 | 2003-12-23 | Katalysatorhaltiges gasverteilersubstrat für brennstoffzellen sowie verfahren zu dessen herstellung |
Family Applications Before (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP02029084A Withdrawn EP1435672A1 (de) | 2002-12-30 | 2002-12-30 | Katalysatorhaltiges Gasverteilersubstrat für Brennstoffzellen sowie Verfahren zu dessen Herstellung |
Country Status (7)
Country | Link |
---|---|
US (1) | US20060177727A1 (de) |
EP (2) | EP1435672A1 (de) |
JP (1) | JP5134763B2 (de) |
KR (1) | KR20050084512A (de) |
AU (1) | AU2003293990A1 (de) |
CA (1) | CA2511920C (de) |
WO (1) | WO2004059770A2 (de) |
Families Citing this family (20)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE112004000288T5 (de) * | 2003-02-13 | 2006-09-14 | E.I. Dupont De Nemours And Co., Wilmington | Elektrokatalysatoren und Verfahren zur Herstellung |
TWI301001B (en) * | 2004-05-25 | 2008-09-11 | Lg Chemical Ltd | Ruthenium-rhodium alloy electrode catalyst and fuel cell comprising the same |
DE102005001290A1 (de) * | 2005-01-11 | 2006-07-20 | Basf Ag | Vorrichtung und Verfahren zur Entfernung von Kohlenmonoxid aus einem wasserstoffhaltigen Gasstrom |
US7608334B2 (en) * | 2005-03-29 | 2009-10-27 | 3M Innovative Properties Company | Oxidatively stable microlayers of gas diffusion layers |
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2002
- 2002-12-30 EP EP02029084A patent/EP1435672A1/de not_active Withdrawn
-
2003
- 2003-12-23 KR KR1020057012296A patent/KR20050084512A/ko not_active Application Discontinuation
- 2003-12-23 AU AU2003293990A patent/AU2003293990A1/en not_active Abandoned
- 2003-12-23 CA CA2511920A patent/CA2511920C/en not_active Expired - Fee Related
- 2003-12-23 US US10/541,173 patent/US20060177727A1/en not_active Abandoned
- 2003-12-23 JP JP2004563200A patent/JP5134763B2/ja not_active Expired - Fee Related
- 2003-12-23 WO PCT/EP2003/014839 patent/WO2004059770A2/de active Application Filing
- 2003-12-23 EP EP03789404A patent/EP1579524A2/de not_active Withdrawn
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Title |
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See references of WO2004059770A2 * |
Also Published As
Publication number | Publication date |
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JP2006512724A (ja) | 2006-04-13 |
EP1435672A1 (de) | 2004-07-07 |
CA2511920C (en) | 2013-06-25 |
US20060177727A1 (en) | 2006-08-10 |
CA2511920A1 (en) | 2004-07-15 |
AU2003293990A1 (en) | 2004-07-22 |
WO2004059770A3 (de) | 2004-08-19 |
KR20050084512A (ko) | 2005-08-26 |
JP5134763B2 (ja) | 2013-01-30 |
WO2004059770A2 (de) | 2004-07-15 |
AU2003293990A8 (en) | 2004-07-22 |
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