EP1055018A1 - Asymmetric electrodes for direct-feed fuel cells - Google Patents
Asymmetric electrodes for direct-feed fuel cellsInfo
- Publication number
- EP1055018A1 EP1055018A1 EP99906802A EP99906802A EP1055018A1 EP 1055018 A1 EP1055018 A1 EP 1055018A1 EP 99906802 A EP99906802 A EP 99906802A EP 99906802 A EP99906802 A EP 99906802A EP 1055018 A1 EP1055018 A1 EP 1055018A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- electrode
- catalyst
- membrane
- backing substrate
- electrode backing
- 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- Withdrawn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
-
- 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
- H01M4/8605—Porous electrodes
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
- C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
- C25B9/23—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms comprising ion-exchange membranes in or on which electrode material is embedded
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
-
- 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
-
- 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
- This disclosure generally relates to organic fuel cells for use in the generation of electrical energy and in particular liquid direct-feed organic fuel cells and the manufacturing thereof .
- Fuel cells are electrochemical cells in which a free energy change resulting from a fuel oxidation reaction is converted into electrical energy. Fuel cells use renewable fuels such as methanol ; typical products from the electrochemical reactions include carbon dioxide and water. Fuel cells may be an attractive alternative to the combustion of fossil fuels.
- JPL Jet Propulsion Laboratory
- FIG. 1 illustrates a typical structure of a JPL fuel cell with an anode 110, a solid electrolyte membrane 120, and a cathode 130 enclosed in housing 140.
- An anode 110 is formed on a first surface 145 of the solid electrolyte membrane 120 with a first catalyst for electro-oxidation.
- Cathode 130 is formed on a second surface 150 thereof opposing the first surface 145 with a second catalyst for electro-reduction.
- the anode 110, the solid electrolyte membrane 120, and the cathode 130 are bonded to form a single multi-layer composite structure 160, referred to herein as a membrane electrode assembly (MEA) .
- An electrical load 170 is connected to the anode 110 and cathode 130 for electrical power output .
- MEA membrane electrode assembly
- a fuel pump 180 is provided for pumping an organic fuel and water solution into an anode chamber 190 of housing 140.
- the organic fuel and water mixture is withdrawn through an outlet port 1100 and is recirculated.
- Carbon dioxide formed in the anode chamber 190 is vented through a port 1120 within fuel tank 1130.
- An oxygen or air compressor 1140 is provided to feed oxygen or air into a cathode chamber 1150 within housing 140.
- anode chamber 190 Prior to use, anode chamber 190 is filled with the organic fuel and water mixture and cathode chamber 1150 is filled with air or oxygen.
- the organic fuel is circulated past anode 110 while oxygen or air is pumped into cathode chamber 1150 and circulated past cathode 130.
- an electrical load 170 is connected between anode 110 and cathode 130, electro- oxidation of the organic fuel occurs at anode 110 and electro-reduction of oxygen occurs at cathode 130.
- Electrons generated by electro-oxidation at anode 110 are conducted through the external load 170 and are captured at cathode 130.
- Hydrogen ions or protons generated at anode 110 are transported directly across the solid electrolyte membrane 120 to cathode 130.
- a flow of current is sustained by a flow of ions through the cell and electrons through the external load 170.
- anode 110, cathode 130 and solid electrolyte membrane 120 form a single composite layered structure 160.
- solid electrolyte membrane 120 is formed from NAFION(TM), a perfluorinated proton-exchange membrane material.
- NAFION(TM) is a co-polymer of tetrafluoroethylene and perfluorovinylether sulfonic acid. Other membrane materials can also be used.
- Anode 110 includes a catalyst material applied to an electrode backing substrate.
- the preferred catalyst used for the anode is platinum-ruthenium.
- the loading of the catalyst is preferably in the range of 0.5 - 4.0 mg/cm 2 . More efficient electro-oxidation is realized at higher loading levels.
- TORAY(TM) paper is used as the electrode backing substrate.
- This porous carbon backing paper is first pre-processed to improve its water resistant characteristics to reduce fuel crossover.
- the pre-processing uses a DUPONT(TM) "TEFLON (TM) 30" suspension of about 60% solids. "TEFLON (TM) 30” is added to approximately 17.1 grams of water.
- the paper is dipped and then sintered in a furnace oven at approximately 350°C for one hour. A processed paper will increase its weight by about 5% over the course of this process.
- the paper is weighed to determine if sufficient absorption has occurred and/or if further paper processing is needed. This coated substrate forms the eventual electrode.
- Cathode 130 is a gas diffusion electrode wherein - platinum catalyst is the preferred catalyst material .
- the catalyst material is applied on an electrode backing substrate.
- the loading of the catalyst onto the electrode backing substrate is preferably in the range of 0.5-4.0 mg/cm 2 . With better performance at 4.0 mg/cm 2 .
- the catalyst material and the electrode backing substrate contain 10-50 weight percent TEFLON (TM) to provide hydrophobicity, creating a three-phase boundary and to achieve efficient removal of water produced by electro-reduction of oxygen.
- a fuel and water mixture containing no acidic or alkaline electrolyte in the concen- tration range of 0.5 - 3.0 mole/liter is circulated past anode 110 within anode chamber 190.
- flow rates in the range of 10 - 500 ml/min. are used.
- Carbon dioxide produced by the above reaction is withdrawn along with the fuel and water solution through outlet port 1100 and separated from the solution in a gas-liquid separator.
- the fuel and water solution is then re-circulated into the cell by fuel pump 180.
- the liquid fuel which is dissolved in water may pass through catalyst gate structures in the solid electrolyte membrane 120 and may combine with oxygen on the surface of the cathode electrocatalyst .
- This process is described by equation 3 for the example of methanol.
- Fuel crossover lowers the operating potential of the oxygen electrode, cathode 130, and results in consumption of fuel without producing useful electrical energy. In general, fuel crossover is a parasitic reaction that lowers efficiency. Fuel crossover reduces performance and generates heat in the fuel cell . Reduction of the rate of fuel crossover is desirable. The rate of fuel crossover is proportional to the permeability of the fuel through the solid electrolyte membrane and increases with increasing fuel concentration and temperature .
- the inventors disclose processes which aid in reduction of undesirable fuel and water diffusion from the anode to the cathode. These processes reduce fuel crossover by closing catalyst gate structures at the electrode-membrane interface.
- One process, multi-layer catalyst application reduces fuel crossover by applying the catalyst material in multiple layers, forming a multi -layer catalyst formation on the electrode with the densest layer of catalyst near the electrode-membrane interface.
- the densest catalyst layer serves as a "pore plugger" which closes catalyst gate structures.
- Another process, inert pore blocker application reduces fuel crossover by applying an inert pore blocker layer on top of the catalyst formation at the electrode- membrane interface.
- This final layer of inert pore plugging material is preferably made of fine carbon particles .
- MEA membrane electrode assembly
- Utilization of the above processes during MEA fabrication can improve fuel cell performance. Fuel crossover can be reduced from 42% to 25%.
- FIG. 1 illustrates a direct liquid feed fuel cell
- FIG. 2 shows a membrane electrode assembly (MEA) fabricated by multi-layer catalyst application
- FIG. 3 shows a MEA fabricated by inert pore blocker application.
- Catalyst gate structures allow fuel to enter the MEA to react with the anode catalyst and gas to enter the MEA to react with the cathode catalyst .
- Pore structures are provided by the electrode backing substrate .
- the electrode backing substrate is preferably a porous carbon backing paper.
- pore structures are generally undesirable at the interface between the electrodes and the membrane, referred to herein as the electrode-membrane interface.
- the pore structures at the interface promote undesirable fuel crossover from the anode to the cathode through the solid electrolyte membrane.
- Membrane electrode assemblies (MEA) wherein the pore structures on the electrode are closed at the electrode-membrane interface are disclosed.
- MEA Metal steps in fabricating MEA include: 1) Pre- treating the solid electrolyte membrane with softening and swelling agents; 2) Application of the catalyst material onto the electrode backing substrate; 3) Application of a "pore-plugging" layer; 4) Assembly of MEA by hot press bonding. Each step is described in detail herein.
- the catalyst material is made from mixing a catalyst metal powder with a water-repelling material.
- the anode catalyst metal powder is bimetallic having separate platinum particles and separate ruthenium particles which are uniformly mixed.
- One embodiment uses approximately 60% platinum, 40% ruthenium.
- the catalyst material includes a dilute polytetrafluoroethylene, e.g. TEFLON (TM) 30, suspension of 12 weight percent solids having 1 gram of TEFLON (TM) 30 concentrate to 4 grams of de-ionized water. 300 mg of de-ionized water is added to 350 mg of the 12 weight percent TEFLON (TM) solution. 144 mg of catalyst metal powder is mixed into this solution. The catalyst metal power and TEFLON (TM) mixture is sonicated for 4 minutes. The catalyst material is then applied onto one side of a 2-inch by 2-inch piece of plain TGPH-90 or 060 paper which is manufactured by Toray Inc. The catalyst material applied onto the electrode backing substrate forms the electrode.
- TM dilute polytetrafluoroethylene
- the cathode uses a preferred catalyst material including platinum catalyst and TEFLON (TM) prepared similarly to the catalyst material for the anode.
- the catalyst material is applied to a 5 weight percent tefIonized electrode backing substrate, preferably a porous carbon backing paper. TefIonized electrode backing substrate reduces fuel crossover.
- TEFLON binds the catalyst material onto the electrode. Sintering burns off surfactants. Sintering also improves TEFLON (TM)'s hydrophobicity. Exposure to high temperatures improves TEFLON (TM) ' s bonding ability thereby preventing catalyst migration during hot press bonding .
- an ionomer solution is applied onto the electrode.
- a solution of perflurosulfonic acid, NAFION(TM) is used.
- NAFION(TM) improves ion conduction resulting in better performance. Since NAFION(TM) can not tolerate the sintering process, NAFION(TM) is applied afterwards.
- the pore structures at the electrode-membrane interface are modified by application of an asymmetric layer of catalyst at the interface .
- the asymmetric layer is formed by a plurality of varying density. For example, starting with the initial catalyst layer application onto the electrode backing substrate, each successive layers of catalyst applied is denser than the layer before. The last catalyst layer applied is the densest.
- Each application follows the steps disclosed above where the electrode is sintered after the catalyst material is applied, then cooled before the ionomer is applied onto the electrode backing substrate.
- the resulting product is an electrode with an asymmetric, non-isotropic distribution of electrode components, namely, varying densities of catalyst layers.
- Both the anode and the cathode are fabricated to have this multi-layer catalyst formation as shown in FIG. 2.
- the membrane electrode assembly 160 When fully assembled using the multi-layer catalyst application, the membrane electrode assembly 160 has a solid electrolyte membrane 120 with two surfaces.
- the first membrane surface 145 is in contact with the densest catalyst layer 220 of a multi-layer catalyst formation 210 of the anode 110.
- the densest catalysl layer 220 is at the electrode-membrane interface 230 between the anode 110 and the membrane 120.
- the anode 2 0 comprises a multi-layer catalyst formation 210 coated on an electrode backing substrate 240.
- the second membrane surface 150 positioned on the opposite side of the first membrane surface 145, is in contact with the densest catalyst layer 260 of a multi- layer catalyst formation 250 of the cathode 130.
- the densest catalyst layer 260 is at the electrode-membrane interface 270 between the cathode 130 and the membrane 120.
- the cathode 130 comprises the multi-layer catalyst formation 250 coated on the electrode backing substrate 280.
- FIG. 3 An MEA fabricated by inert pore blocker application is shown in FIG. 3. Catalyst materials are applied onto the electrode backing substrate 240 of the anode 110 and the electrode backing substrate 280 of the cathode 130. The resulting catalyst formation 310 of the anode 110 and catalyst formation 330 of the cathode 130 are allowed to dry.
- Pore structures are then blocked by applying a final layer of inert material preferably made of very fine particles on top of the catalyst formation at the electrode-membrane interface. These particles make up the inert pore blocker layer; the particles will penetrate and plug the pore structures at the electrode- membrane interface. Inert materials used in the preferred embodiment are very fine carbon particles.
- the resulting product is an electrode with an asymmetric, non-isotropic distribution of electrode components, namely, a catalyst formation and an inert pore blocker layer.
- the membrane electrode assembly 160 When fully assembled using the inert pore blocker application, the membrane electrode assembly 160 has a solid electrolyte membrane 120 with two surfaces.
- the first membrane surface 145 is in contact with the catalyst formation 310 face of the anode 110.
- the inert pore blocker layer 320 is at the anod -membrane interface 230.
- the anode 110 comprises the inert pore blocker layer 320, the catalyst formation 310, and the electrode backing substrate 240.
- the second membrane surface 150 positioned on the opposite side of the first membrane surface 145, is in contact with the catalyst formation 330 face of the cathode 130.
- the inert pore blocker layer 340 is at the cathode-membrane interface 270.
- the cathode 130 comprises the inert pore blocker layer 340, the catalyst formation 330, and the electrode backing substrate 280.
- the pre-treated membrane is sandwiched between the catalyst coated anode and cathode supports and held in a press for 10 minutes under a pressure that can vary from 500 psi- 1500 psi .
- a pressure that can vary from 500 psi- 1500 psi .
- the preferred pressures are close to 500 psi. With thicker papers the optimum pressures are as high as 1250 psi.
- heating is commenced.
- the heat is slowly ramped up to about 145°C.
- the slow ramping up should take place over 25-30 minutes, with the last 5 minutes of heating being a time of temperature stabilization.
- the heat is switched off, but the pressure is maintained.
- the press is then rapidly cooled using circulating water while the pressure is maintained. On cooling to about 60°C, the membrane electrode assembly is removed from the press and stored in water in a sealed plastic bag.
Abstract
Description
Claims
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US2164098A | 1998-02-10 | 1998-02-10 | |
US21640 | 1998-02-10 | ||
PCT/US1999/002677 WO1999040237A1 (en) | 1998-02-10 | 1999-02-08 | Asymmetric electrodes for direct-feed fuel cells |
Publications (2)
Publication Number | Publication Date |
---|---|
EP1055018A1 true EP1055018A1 (en) | 2000-11-29 |
EP1055018A4 EP1055018A4 (en) | 2004-08-11 |
Family
ID=21805330
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP99906802A Withdrawn EP1055018A4 (en) | 1998-02-10 | 1999-02-08 | Asymmetric electrodes for direct-feed fuel cells |
Country Status (3)
Country | Link |
---|---|
EP (1) | EP1055018A4 (en) |
AU (1) | AU2662699A (en) |
WO (1) | WO1999040237A1 (en) |
Families Citing this family (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US6500571B2 (en) | 1998-08-19 | 2002-12-31 | Powerzyme, Inc. | Enzymatic fuel cell |
EP1601035A1 (en) * | 1999-09-21 | 2005-11-30 | Matsushita Electric Industrial Co., Ltd. | Polymer electrolyte fuel cell and method for producing the same |
US20020068213A1 (en) * | 2000-12-01 | 2002-06-06 | Honeywell International, Inc. Law Dept. Ab2 | Multiple layer electrode for improved performance |
US7727663B2 (en) * | 2001-07-18 | 2010-06-01 | Tel-Aviv University Future Technology Development L.P. | Fuel cell with proton conducting membrane and with improved water and fuel management |
FR2838870B1 (en) * | 2002-04-23 | 2004-05-28 | Commissariat Energie Atomique | FUEL CELL BASE COMPONENT LIMITING THE ELECTROLYTE CROSSING BY METHANOL |
US7790304B2 (en) | 2005-09-13 | 2010-09-07 | 3M Innovative Properties Company | Catalyst layers to enhance uniformity of current density in membrane electrode assemblies |
GB0613951D0 (en) * | 2006-07-14 | 2006-08-23 | Johnson Matthey Plc | Membrane electrode assembly for direct mathanol fuel cell |
KR101020900B1 (en) * | 2008-04-11 | 2011-03-09 | 광주과학기술원 | Membrane Electrode Assembly for Direct Liquid Fuel Cell and Manufacturing Method Thereof |
Citations (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3423247A (en) * | 1963-06-07 | 1969-01-21 | Union Carbide Corp | Porous conductive electrode having at least two zones |
EP0631337A2 (en) * | 1993-06-18 | 1994-12-28 | Tanaka Kikinzoku Kogyo K.K. | Solid polymer electrolyte composition |
WO1996029752A1 (en) * | 1995-03-20 | 1996-09-26 | E.I. Du Pont De Nemours And Company | Membranes containing inorganic fillers and membrane and electrode assemblies and electrochemical cells employing same |
US5599638A (en) * | 1993-10-12 | 1997-02-04 | California Institute Of Technology | Aqueous liquid feed organic fuel cell using solid polymer electrolyte membrane |
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 |
WO1997040924A1 (en) * | 1996-04-30 | 1997-11-06 | W.L. Gore & Associates, Inc. | Integral ion-exchange composite membranes |
WO1997050141A1 (en) * | 1996-06-26 | 1997-12-31 | Siemens Aktiengesellschaft | Anode for a direct methanol fuel cell |
Family Cites Families (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US5336384A (en) * | 1991-11-14 | 1994-08-09 | The Dow Chemical Company | Membrane-electrode structure for electrochemical cells |
-
1999
- 1999-02-08 WO PCT/US1999/002677 patent/WO1999040237A1/en active Application Filing
- 1999-02-08 EP EP99906802A patent/EP1055018A4/en not_active Withdrawn
- 1999-02-08 AU AU26626/99A patent/AU2662699A/en not_active Abandoned
Patent Citations (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3423247A (en) * | 1963-06-07 | 1969-01-21 | Union Carbide Corp | Porous conductive electrode having at least two zones |
EP0631337A2 (en) * | 1993-06-18 | 1994-12-28 | Tanaka Kikinzoku Kogyo K.K. | Solid polymer electrolyte composition |
US5599638A (en) * | 1993-10-12 | 1997-02-04 | California Institute Of Technology | Aqueous liquid feed organic fuel cell using solid polymer electrolyte membrane |
WO1996029752A1 (en) * | 1995-03-20 | 1996-09-26 | E.I. Du Pont De Nemours And Company | Membranes containing inorganic fillers and membrane and electrode assemblies and electrochemical cells employing same |
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 |
WO1997040924A1 (en) * | 1996-04-30 | 1997-11-06 | W.L. Gore & Associates, Inc. | Integral ion-exchange composite membranes |
WO1997050141A1 (en) * | 1996-06-26 | 1997-12-31 | Siemens Aktiengesellschaft | Anode for a direct methanol fuel cell |
Non-Patent Citations (2)
Title |
---|
REN X ET AL: "METHANOL CROSS-OVER IN DIRECT METHANOL FUEL CELLS" ELECTROCHEMICAL SOCIETY PROCEEDINGS, ELECTROCHEMICAL SOCIETY, PENNINGTON, NJ, US, vol. 95-23, 1995, pages 284-298, XP002045798 ISSN: 0161-6374 * |
See also references of WO9940237A1 * |
Also Published As
Publication number | Publication date |
---|---|
WO1999040237A1 (en) | 1999-08-12 |
AU2662699A (en) | 1999-08-23 |
WO1999040237A9 (en) | 1999-10-21 |
EP1055018A4 (en) | 2004-08-11 |
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