WO2011083548A1 - 電極-膜-枠接合体及びその製造方法、並びに燃料電池 - Google Patents
電極-膜-枠接合体及びその製造方法、並びに燃料電池 Download PDFInfo
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- WO2011083548A1 WO2011083548A1 PCT/JP2010/007548 JP2010007548W WO2011083548A1 WO 2011083548 A1 WO2011083548 A1 WO 2011083548A1 JP 2010007548 W JP2010007548 W JP 2010007548W WO 2011083548 A1 WO2011083548 A1 WO 2011083548A1
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- membrane
- catalyst layer
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- electrolyte membrane
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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
- H01M8/002—Shape, form of a fuel cell
- H01M8/006—Flat
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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
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
- H01M8/0263—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant having meandering or serpentine paths
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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
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0267—Collectors; Separators, e.g. bipolar separators; Interconnectors having heating or cooling means, e.g. heaters or coolant flow channels
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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
- H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
- H01M8/0273—Sealing or supporting means around electrodes, matrices or membranes with sealing or supporting means in the form of a frame
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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
- H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
- H01M8/028—Sealing means characterised by their material
- H01M8/0284—Organic resins; Organic polymers
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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
- H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
- H01M8/0286—Processes for forming seals
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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
- H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
- H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
- H01M8/242—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes comprising framed electrodes or intermediary frame-like gaskets
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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
- H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
- H01M8/2465—Details of groupings of fuel cells
- H01M8/2483—Details of groupings of fuel cells characterised by internal manifolds
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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
- H01M2008/1095—Fuel cells with polymeric electrolytes
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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
Definitions
- the present invention relates to a fuel cell used as a driving source for a moving body such as an automobile, a distributed power generation system, a household cogeneration system, and the like, and more particularly to an electrode-membrane-frame assembly provided in the fuel cell and its manufacture. Regarding the method.
- a fuel cell for example, a polymer electrolyte fuel cell
- a fuel cell is an apparatus that generates electric power and heat simultaneously by electrochemically reacting a fuel gas containing hydrogen and an oxidant gas containing oxygen such as air. It is.
- a fuel cell is generally configured by stacking a plurality of cells and pressurizing them with a fastening member such as a bolt.
- One cell is configured by sandwiching a membrane electrode assembly (hereinafter referred to as MEA: Membrane-Electrode-Assembly) between a pair of plate-like conductive separators.
- MEA Membrane-Electrode-Assembly
- the peripheral edge of the MEA is held by a frame.
- the MEA including the frame is referred to as an electrode-membrane-frame assembly.
- FIG. 26A to FIG. 26C are schematic explanatory views showing the manufacturing process of the conventional electrode-membrane-frame assembly in an enlarged manner of the joint portion between the MEA and the frame.
- a primary molded body 102A constituting a part of the frame body 102 is injection-molded by pouring molten thermoplastic resin into a mold T100A.
- the MEA 101 is disposed on the primary molded body 102A.
- the MEA 101 includes a polymer electrolyte membrane 111 and a pair of electrode layers 112 disposed on both surfaces of the polymer electrolyte membrane 111.
- Each electrode layer 112 is generally composed of a catalyst layer 113 mainly composed of carbon powder carrying a metal catalyst, and a porous and conductive gas diffusion layer 114 disposed on the catalyst layer 113. ing.
- a secondary molded body 102B constituting the other part of the frame body 102 is injection molded by pouring molten thermoplastic resin into the mold T100B.
- the primary molded body 102A and the secondary molded body 102B are integrated to form the frame body 102, and the electrode-membrane-frame assembly is manufactured.
- the secondary molded body 102B of the frame body 102 is formed by injection molding.
- the temperature of the thermoplastic resin when it is poured into the mold is, for example, a high temperature of 200 degrees or more.
- the catalyst layer 113 is normally comprised with the porous member which has as a main component the carbon powder which carry
- the high-temperature thermoplastic resin When the high-temperature thermoplastic resin is in direct contact with the catalyst layer 113, the high-temperature thermoplastic resin reaches the polymer electrolyte membrane 111 through the catalyst layer 113, and the polymer electrolyte membrane 111 is deteriorated by the heat of the thermoplastic resin (the film thickness of Reduction, strength reduction, etc.).
- the injection pressure of the thermoplastic resin into the mold generally needs to be, for example, 10 times or more the fastening pressure of the cell in order to ensure sufficient molding accuracy.
- the high pressure thermoplastic resin when injection molding the secondary molded body 102B, when a high-pressure thermoplastic resin is in direct contact with the polymer electrolyte membrane 111, the polymer electrolyte membrane 111 may be deteriorated by the pressure of the thermoplastic resin.
- the high pressure thermoplastic resin when the high pressure thermoplastic resin is in direct contact with the catalyst layer 113, the high pressure thermoplastic resin may reach the polymer electrolyte membrane 111 through the catalyst layer 113, and the polymer electrolyte membrane 111 may be deteriorated by the pressure of the thermoplastic resin.
- the power generation unit refers to a portion where the pair of gas diffusion layers 114 and 114 overlap each other when viewed from the thickness direction of the polymer electrolyte membrane 111.
- an object of the present invention is to solve the above-mentioned problems, and to suppress degradation of the polymer electrolyte membrane, an electrode-membrane-frame assembly, a method for producing the same, and the electrode-membrane-frame assembly. It is providing a fuel cell provided with.
- the present invention is configured as follows.
- a frame body is provided at a peripheral portion of a membrane electrode assembly having a second catalyst layer disposed on the second main surface of the electrolyte membrane and a second gas diffusion layer disposed on the main surface of the second catalyst layer.
- a method for producing a formed electrode-membrane-frame assembly comprising: The manufacturing method includes: When viewed from the thickness direction of the electrolyte membrane, the first main surface of the electrolyte membrane is such that the peripheral edge portion of the electrolyte membrane and at least the inner edge portion of the first molded body having a pre-shaped frame shape overlap each other. Arranging the first molded body on the side; When viewed from the thickness direction of the electrolyte membrane, the second main surface of the electrolyte membrane so that the peripheral edge portion of the electrolyte membrane and at least the inner edge portion of the second molded body having a pre-shaped frame shape overlap each other.
- the peripheral surface of the second catalyst layer is exposed so that a part of the main surface of the peripheral portion of the second catalyst layer is exposed.
- the third molded body is overlapped with a part of the peripheral edge of the exposed second catalyst layer as seen from the thickness direction of the electrolyte membrane.
- a part of the resin material constituting the third molded body is mixed in a part of the peripheral edge of the exposed second catalyst layer.
- the fourth aspect of the present invention in the step of disposing the first molded body, on the peripheral portion of the first catalyst layer such that a part of the main surface of the peripheral portion of the first catalyst layer is exposed.
- the first molded body is disposed on
- the third molded body is overlapped with a part of the peripheral edge portion of the exposed first catalyst layer.
- a part of the resin material constituting the third molded body is mixed in a part of the peripheral edge of the exposed first catalyst layer.
- the membrane electrode assembly when the membrane electrode assembly is viewed from the thickness direction of the electrolyte membrane, at least one of the peripheral portion of the first catalyst layer and the peripheral portion of the second catalyst layer is the The method for producing an electrode-membrane-frame assembly according to any one of the first to fifth embodiments, which is disposed on the inner side of the peripheral edge of the electrolyte membrane, is provided.
- the peripheral portion of the first catalyst layer is disposed outside the peripheral portion of the first gas diffusion layer when viewed from the thickness direction of the electrolyte membrane.
- the peripheral portion of the second catalyst layer is disposed outside the peripheral portion of the second gas diffusion layer,
- the first molded body is arranged such that a peripheral edge portion of the first catalyst layer and at least an inner edge portion of the first molded body overlap each other when viewed from the thickness direction of the electrolyte membrane.
- the second molded body is arranged such that a peripheral edge portion of the second catalyst layer and at least an inner edge portion of the second molded body overlap each other when viewed from the thickness direction of the electrolyte membrane.
- the manufacturing method comprises: Before the step of arranging the first molded body, the step of arranging the second molded body, and the step of forming the frame body, Disposing the first gas diffusion layer on the main surface of the first catalyst layer; Disposing the second gas diffusion layer on the main surface of the second catalyst layer; Including In the step of arranging the first molded body, the first molded body is disposed outside the peripheral edge of the first gas diffusion layer as viewed from the thickness direction of the electrolyte membrane, Any one of the first to seventh aspects, wherein, in the step of arranging the second molded body, the second molded body is disposed outside the peripheral edge of the second gas diffusion layer when viewed from the thickness direction of the electrolyte membrane.
- a method for producing the electrode-membrane-frame assembly according to one is provided.
- the manufacturing method comprises: After the step of arranging the first molded body, the step of arranging the second molded body, and the step of forming the frame body, Disposing the first gas diffusion layer on the main surface of the first catalyst layer; Disposing the second gas diffusion layer on the main surface of the second catalyst layer; Including In the step of disposing the first molded body, the first gas diffusion layer is disposed inside the inner edge of the first molded body as viewed from the thickness direction of the electrolyte membrane, Any one of the first to seventh aspects, wherein, in the step of arranging the second molded body, the second gas diffusion layer is disposed inside the inner edge of the second molded body as viewed from the thickness direction of the electrolyte membrane.
- a method for producing the electrode-membrane-frame assembly according to one is provided.
- injection molding is performed so that a part of the resin material constituting the third molded body is mixed in the peripheral portion of the second gas diffusion layer.
- the first molded body is disposed with a gap from the first gas diffusion layer
- the second molded body is disposed with a gap from the second gas diffusion layer
- the method for producing an electrode-membrane-frame assembly according to the eighth or ninth aspect further includes a step of disposing an elastic body in the gap after the step of forming the frame.
- the first molded body and the second molded body are integrally molded so that a part of them is connected before being connected by the third molded body.
- a method for producing the electrode-membrane-frame assembly according to the first aspect is provided.
- a formed electrode-membrane-frame assembly comprising: The frame is Having a first molded body, a second molded body, and a third molded body;
- the first molded body has a frame-like shape, and the electrolyte membrane so that a peripheral edge portion of the electrolyte membrane and at least an inner edge portion of the first molded body overlap each other when viewed from the thickness direction of the electrolyte membrane.
- Arranged on the first main surface side of The second molded body has a frame shape, and the electrolyte membrane so that a peripheral edge portion of the electrolyte membrane and at least an inner edge portion of the second molded body overlap each other when viewed from the thickness direction of the electrolyte membrane.
- Arranged on the second main surface side of The third molded body is disposed between the first molded body and the second molded body so as to integrally connect the first molded body and the second molded body.
- the frame body includes at least one of the peripheral portions of the first catalyst layer and the second catalyst layer and the third portion as viewed from the thickness direction of the electrolyte membrane.
- the electrode-membrane-frame assembly according to the twelfth aspect is provided, wherein the electrode-membrane-frame assembly is disposed so as to overlap a part of the molded body.
- a part of the resin material constituting the third molded body is a part of the main surface of the peripheral part of the first catalyst layer and the main part of the peripheral part of the second catalyst layer. Are mixed in at least one part of the surface, The material constituting the first molded body is not mixed on the main surface of the peripheral edge of the first catalyst layer,
- the electrode-membrane-frame assembly according to the thirteenth or fourteenth aspect is provided, wherein the material constituting the second molded body is not mixed in the main surface of the peripheral portion of the second catalyst layer.
- the sixteenth aspect of the present invention when viewed from the thickness direction of the electrolyte membrane, at least one of the peripheral portion of the first catalyst layer and the peripheral portion of the second catalyst layer is more than the peripheral portion of the electrolyte membrane.
- the electrode-membrane-frame assembly according to any one of the thirteenth to fifteenth embodiments is provided.
- the peripheral portion of the first catalyst layer when viewed from the thickness direction of the electrolyte membrane, is disposed outside the peripheral portion of the first gas diffusion layer, and the second catalyst layer A peripheral portion is disposed outside a peripheral portion of the second gas diffusion layer;
- the frame is When viewed from the thickness direction of the electrolyte membrane, the first molded body is disposed such that a peripheral edge portion of the first catalyst layer and at least an inner edge portion of the first molded body overlap each other.
- the second molded body is disposed so that the peripheral edge of the second catalyst layer and at least the inner edge of the second molded body overlap each other when viewed from the thickness direction of the electrolyte membrane.
- the first molded body is disposed outside the peripheral edge of the first gas diffusion layer as seen from the thickness direction of the electrolyte membrane
- the electrode-membrane according to any one of the thirteenth to seventeenth aspects, wherein the second molded body is disposed outside the peripheral edge of the second gas diffusion layer as viewed from the thickness direction of the electrolyte membrane. -Provide a frame assembly.
- At least one of the first and second molded bodies is arranged with a gap from at least one of the first and second gas diffusion layers, and the gap and the gap
- An electrode-membrane-frame assembly according to an eighteenth aspect is provided, wherein an elastic body is disposed so as to cover at least one of the first and second molded bodies adjacent to the first and second molded bodies.
- a part of the resin material constituting the elastic body is mixed in at least one peripheral edge of the first and second gas diffusion layers adjacent to the gap.
- the electrode-membrane-frame assembly according to the thirteenth aspect, wherein the first molded body and the second molded body are made of resin materials having different hardness.
- either one of the first and second molded bodies is made of a thermoplastic resin
- Either one of the first and second molded bodies is composed of a thermoplastic elastomer.
- the electrode-membrane-frame assembly according to the twenty-first aspect is provided.
- At least one of the first and second molded bodies is composed of a multilayer structure including a thermoplastic resin layer and a thermoplastic elastomer layer.
- the electrode-membrane-frame assembly described is provided.
- the electrode-membrane-frame assembly according to the twenty-third aspect, wherein the thermoplastic elastomer layer is configured to come into contact with a peripheral edge of the first or second catalyst layer.
- a fuel cell comprising the electrode-membrane-frame assembly according to any one of the 13th to 24th aspects.
- a first molded body that has been molded in advance is disposed on the first main surface side of the peripheral portion of the electrolyte membrane, and a second portion of the peripheral portion of the electrolyte membrane is disposed.
- a second molded body molded in advance is arranged on the main surface side.
- the third molded body does not directly contact the inner region of the main surface of the electrolyte membrane located inside the outer edge portion of the second molded body as viewed from the thickness direction of the electrolyte membrane. That is, high temperature and high pressure thermoplastic resin is prevented from coming into direct contact with the catalyst layer in the vicinity of the power generation unit. Thereby, deterioration of a polymer electrolyte membrane can be suppressed and the fall of electric power generation performance can be suppressed.
- the first molded body and the second molded body are integrated by injection molding the third molded body.
- the adhesion between the frame and the MEA can be improved.
- the frame body is constituted by three molded bodies, and the first molded body and the second molded body are integrally connected by the third molded body. Therefore, the necessity of injection-molding the first molded body and the second molded body can be eliminated. Thereby, deterioration of the polymer electrolyte membrane can be suppressed.
- FIG. 1 is a perspective view schematically showing a part of the structure of a fuel cell having an electrode-membrane-frame assembly according to a first embodiment of the present invention
- FIG. 2 is a partially exploded view of the cell stacking section taken along line II-II in FIG.
- FIG. 3 is a plan view schematically showing the configuration of the electrode-membrane-frame assembly of FIG. 4 is a cross-sectional view taken along line IV-IV in FIG.
- FIG. 5 is a plan view showing a surface structure on the anode separator side of the electrode-membrane-frame assembly of FIG.
- FIG. 1 is a perspective view schematically showing a part of the structure of a fuel cell having an electrode-membrane-frame assembly according to a first embodiment of the present invention
- FIG. 2 is a partially exploded view of the cell stacking section taken along line II-II in FIG.
- FIG. 3 is a plan view schematically showing the configuration of the electrode-membrane-frame assembly
- FIG. 6 is a plan view showing a surface structure on the cathode separator side of the electrode-membrane-frame assembly of FIG.
- FIG. 7A is a schematic cross-sectional view showing the manufacturing process of the electrode-membrane-frame assembly of FIG. 1 by enlarging the joint portion between the peripheral portion of the MEA and the frame
- FIG. 7B is a schematic cross-sectional view showing a step following FIG. 7A
- FIG. 7C is a schematic cross-sectional view showing a step following FIG. 7B.
- FIG. 8A is a schematic cross-sectional view showing a manufacturing process different from the manufacturing process of the electrode-membrane-frame assembly shown in FIGS.
- FIG. 8B is a schematic cross-sectional view showing a step following FIG. 8A.
- FIG. 8C is a schematic cross-sectional view showing a step following FIG. 8B.
- FIG. 8D is a schematic cross-sectional view showing a step following FIG. 8C.
- FIG. 9 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a second embodiment of the present invention in an enlarged manner at a joint portion between the peripheral portion of the MEA and the frame, FIG.
- FIG. 10 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a third embodiment of the present invention by enlarging a joint portion between the peripheral portion of the MEA and the frame
- FIG. 11 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a fourth embodiment of the present invention by enlarging a joint portion between the peripheral portion of the MEA and the frame
- FIG. 12 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a fifth embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame
- FIG. 11 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a fourth embodiment of the present invention by enlarging a joint portion between the peripheral portion of the MEA and the frame
- FIG. 12 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a fifth embodiment of the
- FIG. 13 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a sixth embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame
- FIG. 14 is a schematic cross-sectional view showing a state in which the first catalyst layer and the second catalyst layer are short-circuited
- FIG. 15 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a seventh embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame
- FIG. 16 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to an eighth embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame
- FIG. 17 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a ninth embodiment of the present invention by enlarging a joint portion between the peripheral portion of the MEA and the frame
- FIG. 18 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a tenth embodiment of the present invention by enlarging a joint portion between the peripheral portion of the MEA and the frame
- FIG. 19 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to an eleventh embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame
- FIG. 20 is a plan view schematically showing the configuration of the electrode-membrane-frame assembly according to the twelfth embodiment of the present invention.
- 21 is a cross-sectional view taken along line VI-VI in FIG.
- FIG. 22A is a schematic cross-sectional view showing a manufacturing process of an electrode-membrane-frame assembly according to a twelfth embodiment of the present invention by enlarging a joint portion between the peripheral portion of the MEA and the frame
- FIG. 22B is a schematic cross-sectional view showing a step following FIG. 22A.
- FIG. 22C is a schematic cross-sectional view showing a step following FIG. 22B.
- FIG. 23 is a plan view schematically showing a configuration of an electrode-membrane-frame assembly according to a thirteenth embodiment of the present invention.
- 24 is a sectional view taken along line VIII-VIII in FIG.
- FIG. 25 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a fourteenth embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame, FIG.
- FIG. 26A is a schematic explanatory view showing a manufacturing process of a conventional electrode-membrane-frame assembly in which a joint portion between the MEA and the frame is enlarged
- FIG. 26B is a schematic cross-sectional view showing a step following FIG. 26A
- FIG. 26C is a schematic cross-sectional view showing a step following FIG. 26B
- FIG. 27 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to the fifteenth aspect of the present invention, in which the joint between the peripheral portion of the MEA and the frame is enlarged
- FIG. 28 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to the sixteenth aspect of the present invention, in which the joint portion between the peripheral portion of the MEA and the frame is enlarged.
- FIG. 1 is a perspective view schematically showing a part of the structure of a fuel cell having an electrode-membrane-frame assembly according to the first embodiment.
- FIG. 2 is a partially exploded view of the cell stacking section taken along the line II-II in FIG. 3 is a plan view schematically showing the configuration of the electrode-membrane-frame assembly of FIG. 1, and
- FIG. 4 is a cross-sectional view taken along the line IV-IV of FIG.
- FIG. 5 is a plan view showing the surface structure on the anode separator side of the electrode-membrane-frame assembly of FIG. 1
- FIG. 6 is a plan view showing the surface structure on the cathode palator side.
- the fuel cell according to the first embodiment is a polymer that generates electric power and heat simultaneously by electrochemically reacting a fuel gas containing hydrogen and an oxidant gas containing oxygen such as air. This is an electrolyte fuel cell.
- the present invention is not limited to the polymer electrolyte fuel cell, and can be applied to various fuel cells.
- the fuel cell is configured by laminating a plurality (for example, 60) of cells (unit cell modules) 10 which are basic unit configurations.
- a current collector plate, an insulating plate, and an end plate are attached to both ends of the stacked cells 10 group, and fastening bolts are inserted through the bolt holes 4 and fixed with nuts.
- a predetermined fastening force for example, 10 kN.
- the cell 10 is configured by sandwiching the electrode-membrane-frame assembly 1 between an anode separator 2 and a cathode separator 3 which are a pair of conductive separators.
- the electrode-membrane-frame assembly 1 includes a membrane electrode assembly 5 (hereinafter referred to as MEA) and a frame body 6 formed so as to seal and hold the peripheral edge portion 5E of the MEA 5.
- MEA membrane electrode assembly 5
- frame body 6 formed so as to seal and hold the peripheral edge portion 5E of the MEA 5.
- the MEA 5 includes a polymer electrolyte membrane 5A that selectively transports hydrogen ions, and a pair of first and second electrode layers 5D1 and 5D2 formed on both surfaces of the electrolyte membrane 5A (that is, Anode electrode layer and cathode electrode layer).
- the first electrode layer 5D1 has a two-layer structure including a first catalyst layer 5B1 and a first gas diffusion layer 5C1.
- the second electrode layer 5D2 has a two-layer structure of a second catalyst layer 5B2 and a second gas diffusion layer 5C2.
- the first gas diffusion layer 5C1 has a smaller outer size than the first catalyst layer 5B1, and is disposed on the main surface of the first catalyst layer 5B1 so that the peripheral edge of the first catalyst layer 5B1 is exposed. Accordingly, the peripheral edge portion of the first catalyst layer 5B1 is located outside the peripheral edge portion of the first gas diffusion layer 5C1 when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the second gas diffusion layer 5C2 has a smaller outer size than the second catalyst layer 5B2, and is disposed on the main surface of the second catalyst layer 5B2 so that the peripheral edge of the second catalyst layer 5B2 is exposed. Thereby, the peripheral edge portion of the second catalyst layer 5B2 is located outside the peripheral edge portion of the second gas diffusion layer 5C2 when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the polymer electrolyte membrane 5A is composed of a solid polymer material exhibiting proton conductivity, for example, a perfluorosulfonic acid membrane (Nafion membrane manufactured by DuPont).
- the first and second catalyst layers 5B1 and 5B2 are porous members mainly composed of carbon powder supporting a platinum group metal catalyst, for example, and are formed on the surface of the polymer electrolyte membrane 5A.
- the first and second gas diffusion layers 5C1 and 5C2 have both air permeability and electronic conductivity of fuel gas or oxidant gas, and are formed on the surfaces of the first and second catalyst layers 5B1 and 5B2.
- first and second gas diffusion layers 5C1 and 5C2 for example, a porous member composed mainly of conductive particles and a polymer resin can be used without using carbon fiber as a base material.
- a conductive base material having a porous structure manufactured using carbon woven fabric or carbon non-woven fabric to give gas permeability. can be used.
- a water repellent polymer exemplified by a fluororesin may be dispersed in the first gas diffusion layer 5C1 and / or the second gas diffusion layer 5C2.
- a water repellent carbon layer composed of a water repellent polymer and carbon powder may be provided on the main surface of the two catalyst layer 5B2.
- the frame body 6 is composed of three frame-shaped members including a first molded body 61, a second molded body 62, and a third molded body 63.
- the 1st molded object 61 is arrange
- the second molded body 62 is disposed on the peripheral edge of the second catalyst layer 5B2 in proximity to the second gas diffusion layer 5C2. That is, the second molded body 62 is disposed outside the peripheral edge portion of the second gas diffusion layer 5C2 when viewed from the thickness direction of the polymer electrolyte membrane 5A. Accordingly, at least the inner edge portion of the second molded body 62 is positioned so as to overlap the peripheral edge portion of the second catalyst layer 5B2 when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the third molded body 63 is configured to integrally connect the first molded body 61 and the second molded body 62 around the peripheral edge of the MEA 5.
- the first molded body 61, the second molded body 62, and the third molded body 63 are formed by injection molding using a thermoplastic resin that is an example of a resin material.
- the first molded body 61 and the second molded body 62 are injection-molded in advance before being arranged on the first catalyst layer 5B1 or the second catalyst layer 5B2. For this reason, a part of thermoplastic resin which comprises the 1st and 2nd molded objects 61 and 62 is not mixed in the 1st catalyst layer 5B1 and 2nd catalyst layer 5B2 which are porous.
- the third molded body 63 is viewed from the thickness direction of the polymer electrolyte membrane 5A after the first and second molded bodies 61 and 62 are arranged on the first and second catalyst layers 5B1 and 5B2.
- the third molded body 63 and the second catalyst layer 5B2 are injection molded so as to overlap with a part of the peripheral edge.
- a part of the thermoplastic resin constituting the third molded body 63 melts at the time of injection molding and flows into the porous second catalyst layer 5B2, whereby a part of the peripheral edge of the second catalyst layer 5B2 To be mixed.
- This third molded body 63 (due to the anchor effect) improves the adhesion between the frame body 6 and the MEA 5.
- the contact width W1 in the surface direction between the third molded body 63 and the second catalyst layer 5B2 is preferably 1 mm or more.
- the second molded body 62 is disposed on the peripheral edge of the second catalyst layer 5B2 so that the entire circumference of the main surface of the peripheral edge of the second catalyst layer 5B2 is exposed, and viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the third molded body 63 is preferably injection-molded so that a part of the third molded body 63 overlaps the entire periphery of the exposed peripheral edge of the second catalyst layer 5B2. With this configuration, a part of the thermoplastic resin constituting the third molded body 63 can be mixed in the entire periphery of the peripheral portion of the second catalyst layer 5B2, and the frame extends over the entire periphery of the peripheral portion of the second catalyst layer 5B2.
- the adhesion between the body 6 and the MEA 5 can be increased. Moreover, it can suppress that fuel gas and oxidant gas leak between 1st catalyst layer 5B1 and 2nd catalyst layer 5B2 through the peripheral part of 2nd catalyst layer 5B2.
- thermoplastic resin used for the injection molding of the first and second molded bodies 61 and 62 is chemically clean and stable below the operating temperature of the fuel cell, and has an appropriate elastic modulus and a relatively high load deflection. It is preferable that it has temperature.
- the compression modulus of the thermoplastic resin is preferably at least 2,000 MPa or more.
- the elastic modulus refers to a compressive elastic modulus measured by a compressive elastic modulus measurement method defined in JIS-K7181.
- the deflection temperature under load of the thermoplastic resin is preferably 120 ° C. or higher.
- thermoplastic resin used for the first and second molded bodies 61 and 62 is preferably a crystalline resin rather than an amorphous resin from the viewpoint of chemical stability, and among them, the mechanical strength is high and A resin having high heat resistance is preferable.
- thermoplastic resin a so-called super engineering plastic grade, for example, polyphenylene sulfide (PPS), polyether ether ketone (PEEK), liquid crystal polymer (LCP), polyether nitrile (PEN) and the like are preferable.
- PPS polyphenylene sulfide
- PEEK polyether ether ketone
- LCP liquid crystal polymer
- PEN polyether nitrile
- thermoplastic resin Even a resin material that is widely used, for example, polypropylene (GFPP) filled with glass filler has an elastic modulus several times that of unfilled polypropylene (compression elastic modulus 1,000 to 1,500 MPa). Since it has a deflection temperature near 150 ° C., it can be suitably used as the thermoplastic resin.
- GFPP polypropylene
- the 3rd molded object 63 can use the resin material similar to the above-mentioned 1st and 2nd molded object 61,62.
- the joining force is stronger when joining the same quality materials than when joining different materials, it is easy to injection-mold the third molded body 63 and connect the frame bodies integrally.
- the third molded body 63 may be made of a material having a lower compression elastic modulus than the first molded body 61 and the second molded body 62.
- the mechanical stress applied to the polymer electrolyte membrane 5A at the time of handling can be reduced by connecting the first molded body 61 and the second molded body 62 with a material having a low compression modulus, for example, the polymer electrolyte Mechanical deterioration of the film 5A can be suppressed.
- a suitable material of the 3rd molded object 63 the material similar to the thermoplastic resin or thermoplastic elastomer used for the gasket 7 mentioned later can be used, for example, the polypropylene by which the glass filler is not filled is used. be able to.
- a groove 6A is formed on both main surfaces of the frame 6, and a gasket 7 is fitted in the groove 6A.
- the electrode-membrane-frame assembly 1 is sandwiched between an anode separator 2 and a cathode separator 3 via a gasket 7.
- the gasket 7 is made of an elastic body, and is deformed by pressing the anode separator 2 and the cathode separator 3 toward the electrode-membrane-frame assembly 1 when the cell 10 is fastened, and seals the periphery of the MEA 5.
- a specific configuration of the gasket 7 will be described in detail later.
- the anode separator 2 and the cathode separator 3 are generally formed in a flat plate shape.
- the shape of the electrode-membrane-frame assembly 1 ie, the inner surface
- the steps 25 and 35 are formed so as to correspond to the steps due to the difference in thickness. That is, the inner surfaces of the anode separator 2 and the cathode separator 3 are formed so that the central portion protrudes in a trapezoidal shape.
- the anode separator 2 and the cathode separator 3 are made of a gas impermeable conductive material.
- a material obtained by cutting a resin-impregnated carbon material into a predetermined shape or a material obtained by molding a mixture of carbon powder and a resin material can be used.
- the anode separator 2, the cathode separator 3, and the frame 6 are provided with fuel gas manifold holes 12, 22, and 32, which are a pair of through holes through which the fuel gas flows. Further, as shown in FIG. 1, the anode separator 2, the cathode separator 3 and the frame 6 are provided with oxidant gas manifold holes 13, 23 and 33, respectively, which are a pair of through holes through which the oxidant gas flows. It has been. In a state where the anode separator 2, the cathode separator 3, and the frame 6 are fastened as the cell 10, the fuel gas manifold holes 12, 22, and 32 are connected to form a fuel gas manifold. Similarly, when the anode separator 2, the cathode separator 3, and the frame 6 are fastened as the cell 10, the oxidant gas manifold holes 13, 23, and 33 are connected to form an oxidant gas manifold.
- the anode separator 2, the cathode separator 3, and the frame 6 have cooling medium manifold holes that are two pairs of through holes through which a cooling medium (for example, pure water or ethylene glycol) flows. 14, 24 and 34 are provided.
- a cooling medium for example, pure water or ethylene glycol
- the anode separator 2, the cathode separator 3, and the frame 6 are provided with four bolt holes 4 in the vicinity of each corner. A fastening bolt is inserted into each bolt hole 4, and a cell is fastened by a nut being coupled to the fastening bolt.
- a fuel gas passage groove 21 is provided on the inner main surface of the anode separator 2 (surface on the electrode-membrane-frame assembly 1 side) so as to connect the pair of fuel gas manifold holes 22 and 22.
- the fuel gas channel groove 21 includes a first gas diffusion layer contact portion 21A formed on a surface that contacts the first gas diffusion layer 5C1 in the assembled state of the cell 10, and the contact portion 21A and the fuel gas manifold hole 22. And a communication part (communication channel groove) 21B that connects the two.
- the fuel gas flows from the fuel gas manifold 22 on the supply side into the first gas diffusion layer contact portion 21A through the connection portion 21B on the supply side, and comes into contact with the first gas diffusion layer 5C1.
- surplus gas and reaction product components of the fuel gas that have passed through the first gas diffusion layer contact portion 21A are discharged to the discharge-side fuel gas manifold 22 through the discharge-side connection portion 21B.
- a one-dot broken line indicates a position where the fuel gas channel groove 21 contacts or faces the frame body 6 in the assembled state of the cell 10.
- an oxidant gas flow channel groove 31 is provided on the inner main surface of the cathode separator 3 (surface on the electrode-membrane-frame assembly 1 side) so as to connect the pair of oxidant gas manifold holes 33 and 33. It has been.
- the oxidant gas channel groove 31 includes a second gas diffusion layer contact portion 31A formed on the surface that contacts the second gas diffusion layer 5C2 in the assembled state of the cell 10, and the contact portion 31A and the oxidant gas manifold.
- a communication portion (communication channel groove) 31B that connects the hole 33 is provided.
- the oxidant gas flows from the supply side oxidant gas manifold 32 into the second gas diffusion layer contact portion 31A through the supply side connection portion 31B and comes into contact with the second gas diffusion layer 5C2. Yes. Further, surplus gas and reaction product of the oxidant gas that has passed through the second gas diffusion layer contact part 31A are discharged to the discharge-side oxidant gas manifold 32 through the discharge-side connection part 31B. Yes.
- the one-dot broken line indicates a position where the oxidant gas flow channel 31 abuts or faces in the assembled state of the cell 10.
- the fuel gas flowing through the fuel gas passage groove 21 contacts the first gas diffusion layer 5C1, and the oxidant gas flowing through the oxidant gas passage groove 31 enters the second gas diffusion layer 5C2.
- the contact causes a fuel cell electrochemical reaction. Thereby, electric power and heat are generated simultaneously.
- cooling medium flow channel grooves 50 are respectively formed on the outer main surfaces (back surfaces) of the anode separator 2 and the cathode separator 3.
- the cooling medium passage groove 50 is formed so as to connect the two pairs of cooling medium manifold holes 24 and 34. That is, the cooling medium is configured to branch from the cooling medium manifold on the supply side to the cooling medium flow channel groove 50 and to flow to the cooling medium manifold on the discharge side.
- the cell 10 can be maintained at a predetermined temperature suitable for the electrochemical reaction by utilizing the heat transfer capability of the cooling medium.
- channel can be formed by cutting process and a shaping
- the fuel gas manifold, the oxidant gas manifold, and the cooling medium manifold are not limited to the above-described configuration, and various modifications can be made.
- each manifold may have a so-called external manifold structure.
- illustration of each hole is abbreviate
- the gasket 7 surrounds the pair of fuel gas manifold holes 12, the pair of oxidant gas manifold holes 13, and the two pairs of cooling medium manifold holes 14, and the first and second gas diffusion layers 5 ⁇ / b> C ⁇ b> 1 of the MEA 5.
- An annular portion 7A surrounding 5C2 is provided. As shown in FIG. 5, on the anode separator 2 side, the annular portion 7A is formed so as to integrally surround the fuel gas manifold hole 12 and the MEA 5 except for the position corresponding to the connecting portion 21B of the fuel gas flow channel groove 21. Is formed. Further, as shown in FIG.
- the oxidant gas manifold hole 13 and the MEA 5 are integrally surrounded except for the position corresponding to the connecting portion 31B of the oxidant gas flow channel 31.
- An annular portion 7A is formed. This prevents the fuel gas and the oxidant gas from flowing out of the fuel gas flow channel 21 and the oxidant gas flow channel 31.
- a rib 7 ⁇ / b> B is formed on the top surface of the annular portion 7 ⁇ / b> A of the gasket 7.
- the rib 7B is pressed against the anode separator 2 or the cathode separator 3 when the cell 10 is assembled.
- the fastening force of the cell 10 is concentrated on the rib 7B, and the manifold holes 12, 13, 14 and the periphery of the MEA 5 are more reliably sealed. That is, the gasket 7 can be more reliably sealed by the rib 7B.
- the fluid passing through the manifold holes 12, 13, and 14 is prevented from leaking from the manifold holes 12, 13, and 14 and has a high pressure.
- the ribs 7B and 7B located closest to the first and second gas diffusion layers 5C1 and 5C2 are located closer to the first and second gas diffusion layers 5C1 and 5C2 than the outer edge of the polymer electrolyte membrane 5A. It is preferable. With such a configuration, the ribs 7B and 7B facing each other sandwich the peripheral portion 5E of the MEA 5 via the frame 6 by the fastening force in the assembled state of the cell 10, and the peripheral portion 5E of the MEA 5 and the frame 6 The adhesion and bonding strength can be enhanced.
- the gasket 7 is made of a thermoplastic resin or a thermoplastic elastomer which is an example of a resin material.
- the thermoplastic resin or thermoplastic elastomer is preferably chemically stable (particularly not hydrolyzed) below the operating temperature of the fuel cell, and preferably has hot water resistance.
- the compression modulus of the gasket 7 is preferably 200 MPa or less, for example.
- Suitable materials for the gasket 7 are polyethylene, polypropylene (PP), ethylene-propylene-diene copolymer (EPDM), polybutylene, polystyrene, polyvinyl chloride, polyvinylidene chloride, polyvinyl alcohol, Polyacrylamide, polyamide, polycarbonate, polyacetal, polyurethane, silicone, fluororesin, polybutylene terephthalate, polyethylene terephthalate, polyethylene naphthalate, syndiotactic polystyrene, polyphenylene sulfide, polyether ether ketone, polyether ketone, liquid crystal polymer, polyether Nitrile, modified polyphenylene ether, polysulfone, polyethersulfone, polyarylate, polyamideimide, Li polyetherimide, and is at least one selected from the group consisting of a thermoplastic polyimide.
- PP polypropylene
- EPDM ethylene-propylene-diene copolymer
- Santoprene 8101-55 manufactured by Advanced Elastomer System
- PP and EPDM polyolefin-based thermoplastic elastomer having PP and EPDM
- a general seal member 9 such as a squeezed packing made of a heat-resistant material is disposed around each manifold hole on the outer main surface (back surface) of the anode separator 2 and the cathode separator 3. This prevents the fuel gas, the oxidant gas, and the cooling medium from flowing out from the connecting portions of the manifold holes 22, 23, 24, 32, 33, 34 between the cells 10, 10 adjacent to each other.
- FIG. 7A to 7C are schematic cross-sectional views showing each manufacturing process of the electrode-membrane-frame assembly 1 by enlarging the joint portion between the peripheral edge portion 5E of the MEA 5 and the frame body 6.
- FIG. 1st molded object 61 and the 2nd molded object 62 shall be injection-molded previously, and MEA5 shall be produced previously.
- the first molded body 61 is disposed on the peripheral edge of the first catalyst layer 5B1 in the vicinity of the first gas diffusion layer 5C1 of the MEA5. That is, the first molded body 61 is disposed outside the peripheral edge portion of the first gas diffusion layer 5C1 when viewed from the thickness direction of the polymer electrolyte membrane 5A. Accordingly, at least the inner edge portion of the first molded body 61 is positioned so as to overlap with the peripheral edge portion of the first catalyst layer 5B1 when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the second molded body 62 is disposed on the peripheral edge of the second catalyst layer 5B2 in the vicinity of the second gas diffusion layer 5C2 of the MEA 5. That is, as viewed from the thickness direction of the polymer electrolyte membrane 5A, the second molded body 62 is disposed outside the peripheral edge portion of the second gas diffusion layer 5C2. At this time, the second molded body 62 is arranged so that a part of the main surface of the peripheral edge of the second catalyst layer 5B2 is exposed. Accordingly, at least the inner edge portion of the second molded body 62 is positioned so as to overlap the peripheral edge portion of the second catalyst layer 5B2 when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the first molded body 61 and the second molded body 62 are sandwiched between the pair of molds T1 around the peripheral edge 5E of the MEA 5, and the first formed in the pair of molds T1.
- the molten thermoplastic resin is poured into the gap between the first molded body 61 and the second molded body 62, and the third molded body 63 is injection molded.
- a part of 3rd molded object 63 overlaps with a part of peripheral part of 2nd catalyst layer 5B2 seeing from the thickness direction of 5 A of polymer electrolyte membranes.
- a part of the molten thermoplastic resin is mixed in a part of the main surface of the peripheral edge of the second catalyst layer 5B2.
- the first molded body 61 formed in advance is disposed on the peripheral edge of the first catalyst layer 5B1 in the vicinity of the first gas diffusion layer 5C1, and in the vicinity of the second gas diffusion layer 5C2. Then, the second molded body 62 molded in advance is arranged on the peripheral edge of the second catalyst layer 5B2. Further, the third molded body 63 has a (second) main surface of the polymer electrolyte membrane 5A located inside the outer edge 62-1 of the second molded body 62 when viewed from the thickness direction of the polymer electrolyte membrane 5A. So that it does not touch the inner area directly.
- the power generation unit refers to a portion where the first gas diffusion layer 5C1 and the second gas diffusion layer 5C2 overlap each other when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the first molded body 61 and the second molded body 62 are integrated by injection molding of the third molded body 63, so that the frame 6 and the MEA 5 are integrated. Adhesion can be improved.
- the frame body 6 is constituted by three molded bodies (first to third molded bodies 61, 62, 63), and the first molded body 61 and the second molded body 63 are formed by the third molded body 63. Since the molded body 62 is integrally connected, the necessity of injection molding the first molded body 61 and the second molded body 62 can be eliminated. Thereby, deterioration of the polymer electrolyte membrane 5A can be suppressed.
- the first molded body 61 and the second molded body 62 are made of the same resin material. However, they may be made of different materials so as to have different hardnesses.
- the first molded body 61 may be made of a hard material (for example, a thermoplastic resin), and the second molded body 62 may be made of a soft material (for example, a thermoplastic elastomer).
- the first molded body 61 is a hard member, the shape of the electrode-membrane-frame assembly 1 can be maintained (maintained). In other words, the electrode-membrane-frame assembly 1 can be prevented from being bent or bent.
- the second molded body 62 is a soft member (elastic body)
- the fastening pressure applied to the polymer electrolyte membrane 5A when the cell 10 is fastened can be relieved, and mechanical degradation of the polymer electrolyte membrane 5A can be reduced. Can be suppressed.
- the first molded body 61 and / or the second molded body 62 may have a multilayer structure including a thermoplastic resin layer and a thermoplastic elastomer layer.
- the joining property with the third molded body 63 can be enhanced by the thermoplastic resin layer, and the fastening pressure applied to the MEA 5 when the cell 10 is fastened can be relieved by the thermoplastic elastomer layer.
- the thermoplastic elastomer layer is configured to contact the first catalyst layer 5B1 and / or the second catalyst layer 5B2.
- the first molded body 61 is disposed on the anode side, and the second molded body 62 is disposed on the cathode side.
- the first molded body 61 is disposed on the cathode side, and the second The molded body 62 may be disposed on the anode side.
- the peripheral edge portion of the first catalyst layer 5B1 when viewed from the thickness direction of the polymer electrolyte membrane 5A, the peripheral edge portion of the first catalyst layer 5B1 is disposed outside the peripheral edge portion of the first gas diffusion layer 5C1 over the entire periphery, and the second catalyst layer The periphery of 5B2 is arranged outside the periphery of the second gas diffusion layer 5C2 over the entire periphery.
- the inner edge of the first frame 61 and the polymer electrolyte membrane 5A are not in direct contact with each other in the vicinity of the periphery of the first gas diffusion layer 5C1, and the periphery of the second gas diffusion layer 5C2.
- a part of the peripheral edge of the first catalyst layer 5B1 may be disposed on the inner side of the peripheral edge of the first gas diffusion layer 5C1 as long as the above-described effect is achieved.
- a part of the peripheral edge of the layer 5B2 may be disposed inside the peripheral edge of the second gas diffusion layer 5C2.
- the present invention when viewed from the thickness direction of the polymer electrolyte membrane 5A, at least the inner edge portion of the first molded body 61 is disposed so as to overlap the peripheral edge portion of the first catalyst layer 5B1.
- the present invention is not limited to this.
- at least the inner edge portion of the first molded body 61 is on one main surface side of the polymer electrolyte membrane 5A so as to overlap the peripheral edge portion of the polymer electrolyte membrane 5A. You may arrange.
- At least the inner edge portion of the second molded body 62 is disposed so as to overlap with the peripheral edge portion of the second catalyst layer 5B2. It is not limited. For example, when viewed from the thickness direction of the polymer electrolyte membrane 5A, at least the inner edge portion of the second molded body 62 is on the other main surface side of the polymer electrolyte membrane 5A so as to overlap the peripheral edge portion of the polymer electrolyte membrane 5A. You may arrange.
- thermoplastic resin does not directly contact the polymer electrolyte membrane 5A in the vicinity of the power generation unit, deterioration of the polymer electrolyte membrane 5A can be suppressed.
- the peripheral edge portion of the first catalyst layer 5B1 when viewed from the thickness direction of the polymer electrolyte membrane 5A, the peripheral edge portion of the first catalyst layer 5B1 is disposed outside the peripheral edge portion of the first gas diffusion layer 5C1 over the entire circumference, and the second Although the peripheral portion of the catalyst layer 5B2 is arranged outside the peripheral portion of the second gas diffusion layer 5C2 over the entire periphery, the present invention is not limited to this.
- the peripheral edge portion of the first catalyst layer 5B1 may be disposed inside the peripheral edge portion of the first gas diffusion layer 5C1, and the first catalyst layer 5B1 and the first gas diffusion layer 5C1 have the same size. There may be.
- the peripheral edge portion of the second catalyst layer 5B2 may be disposed inside the peripheral edge portion of the second gas diffusion layer 5C2, and the second catalyst layer 5B2 and the second gas diffusion layer 5C2 have the same size. There may be. Even with such a configuration, since the high-temperature and high-pressure thermoplastic resin does not directly contact the polymer electrolyte membrane 5A in the vicinity of the power generation unit, deterioration of the polymer electrolyte membrane 5A can be suppressed.
- the peripheral portion of the first gas diffusion layer 5C1 and the peripheral portion of the second gas diffusion layer 5C2 coincide with each other when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the invention is not limited to this.
- the peripheral edge portion of the first gas diffusion layer 5C1 and the peripheral edge portion of the second gas diffusion layer 5C2 may be shifted from each other in the surface direction of the polymer electrolyte membrane 5A.
- the MEA 5 is manufactured in advance when the electrode-membrane-frame assembly 1 is manufactured.
- the electrode-membrane-frame assembly 1 can be manufactured as shown in FIGS. 8A to 8D.
- 8A to 8D are schematic cross-sectional views showing the respective manufacturing steps of the electrode-membrane-frame assembly 1 by enlarging the joint portion between the peripheral portion 5E of the MEA 5 and the frame body 6.
- FIG. the 1st molded object 61 and the 2nd molded object 62 shall be injection-molded previously.
- the first molded body 61 is disposed on the peripheral edge of the first catalyst layer 5B1 of the MEA 5. Accordingly, at least the inner edge portion of the first molded body 61 is positioned so as to overlap with the peripheral edge portion of the first catalyst layer 5B1 when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the second molded body 62 is disposed on the peripheral edge of the second catalyst layer 5B2 of the MEA 5. Accordingly, at least the inner edge portion of the second molded body 62 is positioned so as to overlap the peripheral edge portion of the second catalyst layer 5B2 when viewed from the thickness direction of the polymer electrolyte membrane 5A. At this time, the second molded body 62 is arranged so that a part of the main surface of the peripheral edge of the second catalyst layer 5B2 is exposed.
- the first molded body 61 and the second molded body 62 are sandwiched between the pair of molds T1 around the peripheral edge 5E of the MEA 5, and are formed in the pair of molds T1.
- the molten thermoplastic resin is poured into the gap between the first molded body 61 and the second molded body 62, and the third molded body 63 is injection molded.
- a part of 3rd molded object 63 overlaps with a part of peripheral part of 2nd catalyst layer 5B2 seeing from the thickness direction of 5 A of polymer electrolyte membranes.
- a part of the molten thermoplastic resin is mixed in a part of the main surface of the peripheral edge of the second catalyst layer 5B2.
- the first gas diffusion layer 5 ⁇ / b> C ⁇ b> 1 is disposed on the inner side of the inner edge of the first molded body 61, and the second gas diffusion is disposed on the inner side of the inner edge of the second molded body 62.
- Layer 5C2 is disposed.
- FIG. 9 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a second embodiment of the present invention, in which the joint portion between the peripheral portion of the MEA and the frame is enlarged.
- the electrode-membrane-frame assembly 1A according to the second embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that the third molded body 63a is a peripheral portion of the second catalyst layer 5B2. It is the point which is not in contact with the main surface of the.
- the electrode-membrane-frame assembly according to the first embodiment. 1 can suppress the deterioration of the polymer electrolyte membrane 5A.
- the peripheral edge portion of the first catalyst layer 5B1 when viewed from the thickness direction of the polymer electrolyte membrane 5A, the peripheral edge portion of the first catalyst layer 5B1 is disposed outside the peripheral edge portion of the first gas diffusion layer 5C1 over the entire circumference, and the second Although the peripheral portion of the catalyst layer 5B2 is arranged outside the peripheral portion of the second gas diffusion layer 5C2 over the entire periphery, the present invention is not limited to this.
- the peripheral edge portion of the first catalyst layer 5B1 may be disposed inside the peripheral edge portion of the first gas diffusion layer 5C1, and the first catalyst layer 5B1 and the first gas diffusion layer 5C1 have the same size. There may be.
- the peripheral edge portion of the second catalyst layer 5B2 may be disposed inside the peripheral edge portion of the second gas diffusion layer 5C2, and the second catalyst layer 5B2 and the second gas diffusion layer 5C2 have the same size. It may be. Even with such a configuration, since the high-temperature and high-pressure thermoplastic resin does not directly contact the polymer electrolyte membrane 5A in the vicinity of the power generation unit, deterioration of the polymer electrolyte membrane 5A can be suppressed.
- FIG. 10 is an enlarged schematic cross-sectional view showing an electrode-membrane-frame assembly according to a third embodiment of the present invention, in which an interface between the peripheral portion of the MEA and the frame is enlarged.
- the electrode-membrane-frame assembly 1B according to the third embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that the third molded body 63b is the same as the second embodiment. Is not in contact with the main surface of the peripheral edge of the second catalyst layer 5B2.
- the third molded body 63b to be injection-molded is not in contact with the main surface of the peripheral edge of the polymer electrolyte membrane 5A. It is possible to suppress the deterioration of the polymer electrolyte membrane 5A more than the electrode-membrane-frame assembly 1 according to the above.
- FIG. 11 is an enlarged schematic cross-sectional view showing an electrode-membrane-frame assembly according to a fourth embodiment of the present invention, in which an interface between the peripheral portion of the MEA and the frame is enlarged.
- the electrode-membrane-frame assembly 1C according to the fourth embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that the third molded body 63c is a peripheral portion of the second catalyst layer 5B2.
- the third molded body 63c is formed so as to wrap around the first catalyst layer 5B1 side and to contact a part of the main surface of the peripheral portion of the first catalyst layer 5B1. It is.
- thermoplastic resin constituting the third molded body 63c to be injection-molded is melted at the time of injection molding and flows into the porous first catalyst layer 5B1, whereby the first It is made to mix in a part of peripheral part of catalyst layer 5B1.
- the third molded body 63c due to the anchor effect, the adhesion between the frame body 6 and the MEA 5 is improved as in the first embodiment.
- the first molded body 61 is disposed on the peripheral edge of the first catalyst layer 5B1 so that the entire circumference of the main surface of the peripheral edge of the first catalyst layer 5B1 is exposed, and viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the third molded body 63 is preferably injection-molded so that a part of the third molded body 63 overlaps the entire periphery of the exposed peripheral edge portion of the first catalyst layer 5B1. With this configuration, a part of the thermoplastic resin constituting the third molded body 63c can be mixed in the entire periphery of the peripheral edge of the first catalyst layer 5B1, and over the entire periphery of the peripheral edge of the first catalyst layer 5B1.
- the adhesion between the frame 6 and the MEA 5 can be improved. Moreover, it can suppress that fuel gas and oxidant gas leak between 1st catalyst layer 5B1 and 2nd catalyst layer 5B2 through the peripheral part of 1st catalyst layer 5B1 by this.
- FIG. 12 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a fifth embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame.
- the electrode-membrane-frame assembly 1D according to the fifth embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that the third molded body 63d rotates toward the first catalyst layer 5B1. It is a point formed so that it may touch and a part of main surface of the peripheral part of 1st catalyst layer 5B1.
- the frame body 6 and the MEA 5 are in close contact with each other.
- the sex can be further improved.
- FIG. 13 is an enlarged schematic cross-sectional view showing an electrode-membrane-frame assembly according to a sixth embodiment of the present invention, in which an interface between the peripheral portion of the MEA and the frame is enlarged.
- the electrode-membrane-frame assembly 1E according to the sixth embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that a polymer is seen from the thickness direction of the polymer electrolyte membrane 5A. This is that the peripheral edge of the first catalyst layer 5B1 is formed on the inner side than the peripheral edge of the electrolyte membrane 5A.
- the first catalyst layer 5B1 and the second catalyst layer 5B2 are provided on the entire main surfaces of the polymer electrolyte membrane 5A.
- Such a structure can be realized, for example, by forming a catalyst layer on both main surfaces of a large size polymer electrolyte membrane and then cutting the polymer electrolyte membrane to a desired size.
- the first catalyst layer 5B1 and the second catalyst layer 5B2 may be short-circuited as shown in FIG.
- the first catalyst layer 5B1 is not formed on the entire surface of the polymer electrolyte membrane 5A, and the periphery of the polymer electrolyte membrane 5A is viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the peripheral portion of the first catalyst layer 5B1 is arranged on the inner side than the portion. Thereby, a short circuit failure between the first catalyst layer 5B1 and the second catalyst layer 5B2 can be prevented.
- the first catalyst layer 5B1 is not formed on the entire surface of the polymer electrolyte membrane 5A, and the first catalyst layer 5B1 is first formed from the peripheral portion of the polymer electrolyte membrane 5A when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the peripheral portion of the catalyst layer 5B1 is arranged on the inner side, the present invention is not limited to this.
- the second catalyst layer 5B2 is not formed on the entire surface of the polymer electrolyte membrane 5A, and the polymer is seen from the thickness direction of the polymer electrolyte membrane 5A. You may comprise so that the peripheral part of 2nd catalyst layer 5B2 may be arrange
- FIG. 15 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a seventh embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame.
- the electrode-membrane-frame assembly 1F according to the seventh embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that a polymer is seen from the thickness direction of the polymer electrolyte membrane 5A. This is that the peripheral portions of the first catalyst layer 5B1 and the second catalyst layer 5B2 are formed on the inner side from the peripheral portion of the electrolyte membrane 5A. Further, the third molded body 63f is provided so as to go around to the first catalyst layer 5B1 side.
- a short circuit failure between the first catalyst layer 5B1 and the second catalyst layer 5B2 can be prevented more reliably.
- FIG. 16 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to an eighth embodiment of the present invention by enlarging the joint between the peripheral edge of the MEA and the frame.
- the electrode-membrane-frame assembly 1G according to the eighth embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that a polymer is seen from the thickness direction of the polymer electrolyte membrane 5A.
- the peripheral edge of the first catalyst layer 5B1 is arranged on the inner side than the peripheral edge of the electrolyte membrane 5A, and the peripheral edge of the first catalyst layer 5B1 and the inner edge of the first molded body 61 are not overlapped. Is a point.
- a short circuit failure between the first catalyst layer 5B1 and the second catalyst layer 5B2 can be prevented more reliably. Moreover, since the peripheral part of 1st catalyst layer 5B1 and the inner edge part of the 1st molded object 61 do not overlap, the quantity of 1st catalyst layer 5B1 which does not contribute effectively to electric power generation can be reduced.
- FIG. 17 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a ninth embodiment of the present invention by enlarging the joint portion between the peripheral edge of the MEA and the frame.
- the electrode-membrane-frame assembly 1H according to the ninth embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that a polymer is seen from the thickness direction of the polymer electrolyte membrane 5A.
- the peripheral edge of the second catalyst layer 5B2 is disposed on the inner side than the peripheral edge of the electrolyte membrane 5A, and the peripheral edge of the second catalyst layer 5B2 and the inner edge of the second molded body 62 are not overlapped. Is a point.
- a short circuit failure between the first catalyst layer 5B1 and the second catalyst layer 5B2 can be prevented more reliably. Moreover, since the peripheral part of 2nd catalyst layer 5B2 and the inner edge part of the 2nd molded object 62 do not overlap, the quantity of 2nd catalyst layer 5B2 which does not contribute effectively to electric power generation can be reduced.
- FIG. 18 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a tenth embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame.
- the electrode-membrane-frame assembly 1I according to the tenth embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that the first is seen from the thickness direction of the polymer electrolyte membrane 5A.
- the peripheral portion of the gas diffusion layer 5C1 is disposed outside the peripheral portion of the second gas diffusion layer 5C2, and the peripheral portion of the first gas diffusion layer 5C1 and the inner edge portion of the second molded body 62 are arranged to overlap each other. It is a point.
- the same effect as in the first embodiment can be obtained.
- the peripheral edge portion of the first gas diffusion layer 5C1 and the inner edge portion of the second molded body 62 are arranged so as to overlap each other when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the handling properties (breakage prevention, deformation prevention, etc.) of the electrode-membrane-frame assembly 1I can be improved.
- the member which has a thick part and a thin part like the 1st molded object 61 is injection-molded, if the length of a thin part is long, the difficulty of a manufacturing process will become high. For this reason, as shown in FIG. 18, it is preferable to make the length of the thin part of the 1st molded object 61a in the surface direction shorter than the 1st molded object 61 of the said 1st Embodiment.
- FIG. 19 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to an eleventh embodiment of the present invention by enlarging the joint between the peripheral edge of the MEA and the frame.
- the electrode-membrane-frame assembly 1J according to the eleventh embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that the second point is the second as seen from the thickness direction of the polymer electrolyte membrane 5A.
- the peripheral portion of the gas diffusion layer 5C2 is disposed outside the peripheral portion of the first gas diffusion layer 5C1, and the peripheral portion of the second gas diffusion layer 5C2 and the inner edge portion of the first molded body 61b overlap each other. It is a point.
- the same effect as in the first embodiment can be obtained.
- the peripheral edge portion of the second gas diffusion layer 5C2 and the inner edge portion of the first molded body 61a are arranged so as to overlap each other when viewed from the thickness direction of the polymer electrolyte membrane 5A.
- the handling properties (breakage prevention, deformation prevention, etc.) of the electrode-membrane-frame assembly 1I can be improved.
- FIG. 20 is a plan view schematically showing the configuration of the electrode-membrane-frame assembly according to the twelfth embodiment of the present invention.
- 21 is a cross-sectional view taken along the line VI-VI in FIG.
- the electrode-membrane-frame assembly 1K according to the twelfth embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that the first molded body 61c is the same size as the second molded body 62.
- the third molded body 63k is formed so as to connect them.
- the first molded body 61c is formed in the same size as the second molded body 62, they can be produced with one type of mold, and the manufacturing cost can be reduced. Can be achieved.
- the electrode-membrane-frame assembly 1K according to the twelfth embodiment can be manufactured as follows. 22A to 22C are schematic cross-sectional views showing each manufacturing process of the electrode-membrane-frame assembly 1K by enlarging the joint portion between the peripheral portion 5E of the MEA 5 and the frame body 6.
- the 1st molded object 61c and the 2nd molded object 62 shall be injection-molded previously, and MEA5 shall be produced previously.
- the first molded body 61c is disposed on the peripheral portion of the first catalyst layer 5B1 in the vicinity of the first gas diffusion layer 5C1 of the MEA 5.
- the 1st molded object 61c is arrange
- the second molded body 62 is disposed on the peripheral edge of the second catalyst layer 5B2 in the vicinity of the second gas diffusion layer 5C2 of the MEA 5.
- the 2nd molded object 62 is arrange
- FIG. 23 is a plan view schematically showing the configuration of the electrode-membrane-frame assembly according to the thirteenth embodiment of the present invention.
- 24 is a cross-sectional view taken along line VIII-VIII in FIG.
- the electrode-membrane-frame assembly 1L according to the thirteenth embodiment differs from the electrode-membrane-frame assembly 1K according to the thirteenth embodiment in that a part of the first molded body 61c and the second molded body 62 are used. Is partly connected before the third molded body 63l is injection molded. That is, in the thirteenth embodiment, the first molded body 61c and the second molded body 62 are integrally molded.
- the first molded body 61c and the second molded body 62 are integrally molded, the number of manufacturing steps can be reduced.
- FIG. 25 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a fourteenth embodiment of the present invention by enlarging the joint between the peripheral edge of the MEA and the frame.
- the electrode-membrane-frame assembly 1M according to the fourteenth embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that the frame 6 has first and second gas diffusion layers 5C1, 5C2 is provided with a gap, and extending portions 7C1 and 7C2, which are examples of elastic bodies extending from the gaskets 7 and 7 so as to close the gap, are provided.
- the entire gasket 7 including the extending portions 7C1 and 7C2 is formed in such a manner that the high-temperature and high-pressure thermoplastic resin does not directly contact the polymer electrolyte membrane 5A near the power generation portion.
- the gasket 7 is made of an elastic body that has been injection-molded in advance.
- the frame 6 of the electrode-membrane-frame assembly 1 and the MEA 5 A gap 40 is formed between the vicinity of the joining portion and the anode separator 2 and the cathode separator 3.
- the fuel gas and the oxidant gas mainly undergo an electrochemical reaction between the first and second electrode layers 5D1 and 5D2 that face each other, but the gap 40 serves as a shortcut passage, and the fuel gas and the oxidant gas are the first.
- the second electrode layers 5D1 and 5D2 may not be sufficiently supplied.
- the extending portions 7C1 and 7C2 are extended from the gasket 7 so as to close the gap 40. Thereby, the fuel gas and the oxidant gas can be sufficiently supplied to the first and second electrode layers 5D1 and 5D2.
- FIG. 27 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a sixteenth embodiment of the present invention by enlarging the joint portion between the peripheral portion of the MEA and the frame.
- the electrode-membrane-frame assembly 1N according to the fifteenth embodiment is different from the electrode-membrane-frame assembly 1M according to the fourteenth embodiment in that the gap 40 is blocked by the extending portions 7C1 and 7C2.
- the gap 40 is closed by the elastic body 71.
- the elastic body 71 is formed in such a manner that a high-temperature and high-pressure thermoplastic resin does not directly contact the polymer electrolyte membrane 5A near the power generation unit.
- the elastic body 71 is injection-molded in advance before being disposed between the first gas diffusion layer 5C1 and the first molded body 61 and between the second gas diffusion layer 5C2 and the second molded body 621. ing. Thereby, the same effect as the 14th embodiment that fuel gas and oxidant gas can fully be supplied to the 1st and 2nd electrode layers 5D1 and 5D2 can be acquired.
- FIG. 28 is a schematic cross-sectional view showing an electrode-membrane-frame assembly according to a sixteenth embodiment of the present invention by enlarging the joint between the peripheral edge of the MEA and the frame.
- the electrode-membrane-frame assembly 1P according to the sixteenth embodiment is different from the electrode-membrane-frame assembly 1 according to the first embodiment in that a part of the resin material constituting the third molded body 63p is used. This is a point that covers all or part of the second molded body 62. Even with such a configuration, the same effects as those of the first embodiment can be obtained.
- the third molded body 63p can be firmly fixed. Moreover, even if there is a gap between the second gas diffusion layer 5C2 and the second molded body 62, the third molded body 63p can suppress the occurrence of defects such as shortcuts. Furthermore, since the high-temperature and high-pressure thermoplastic resin is not in direct contact with the polymer electrolyte membrane 5A in the vicinity of the power generation unit, the deterioration of the polymer electrolyte membrane 5A can be suppressed, and the decrease in power generation performance can be suppressed. Can do.
- the electrode-membrane-frame assembly and the manufacturing method thereof according to the present invention can suppress the deterioration of the polymer electrolyte membrane, so that, for example, mobile bodies such as automobiles, distributed power generation systems, home cogeneration systems, etc. It is useful for a fuel cell used as a drive source.
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Abstract
Description
次いで、図26Bに示すように、一次成形体102A上にMEA101を配置する。
本発明の第1態様によれば、高分子電解質膜の第1の主面に配置された第1触媒層と、前記第1触媒層の主面に配置された第1ガス拡散層と、前記電解質膜の第2の主面に配置された第2触媒層と、前記第2触媒層の主面に配置された第2ガス拡散層と、を有する膜電極接合体の周縁部に枠体が形成された電極-膜-枠接合体の製造方法であって、
前記製造方法は、
前記電解質膜の厚み方向から見て、前記電解質膜の周縁部と予め成形された額縁状の形状を有する第1成形体の少なくとも内縁部とが重なるように、前記電解質膜の第1の主面側に前記第1成形体を配置する工程と、
前記電解質膜の厚み方向から見て、前記電解質膜の周縁部と予め成形された額縁状の形状を有する第2成形体の少なくとも内縁部とが重なるように、前記電解質膜の第2の主面側に前記第2成形体を配置する工程と、
前記第1成形体を配置する工程及び前記第2成形体を配置する工程の後、前記電解質膜の厚み方向から見て前記第2成形体の外縁部よりも内側に位置する前記電解質膜の第2の主面の内側領域に直接接することなく、前記第1成形体及び前記第2成形体を一体的に接続するように前記第1成形体と前記第2成形体との間に第3成形体を射出成形することにより、前記第1成形体と前記第2成形体と前記第3成形体とを含む前記枠体を形成する工程と、
を含む、電極-膜-枠接合体の製造方法を提供する。
前記枠体を形成する工程において、前記電解質膜の厚み方向から見て、前記第3成形体の一部が前記露出する第2触媒層の周縁部の一部とが重なるように、前記第3成形体を射出成形する、第1態様に記載の電極-膜-枠接合体の製造方法を提供する。
前記枠体を形成する工程において、前記電解質膜の厚み方向から見て、前記第3成形体の一部と前記露出する第1触媒層の周縁部の一部とが重なるように、前記第3成形体を射出成形する、第2態様に記載の電極-膜-枠接合体の製造方法を提供する。
前記第1成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第1触媒層の周縁部と前記第1成形体の少なくとも内縁部とが重なるように、前記第1成形体を配置し、
前記第2成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第2触媒層の周縁部と前記第2成形体の少なくとも内縁部とが重なるように、前記第2成形体を配置する、第1~5態様のいずれか1つに記載の電極-膜-枠接合体の製造方法を提供する。
前記第1成形体を配置する工程、第2成形体を配置する工程、及び前記枠体を形成する工程の前に、
前記第1触媒層の主面に前記第1ガス拡散層を配置する工程と、
前記第2触媒層の主面に前記第2ガス拡散層を配置する工程と、
を含み、
前記第1成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第1ガス拡散層の周縁部より外側に前記第1成形体を配置し、
前記第2成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第2ガス拡散層の周縁部より外側に前記第2成形体を配置する、第1~7態様のいずれか1つに記載の電極-膜-枠接合体の製造方法を提供する。
前記第1成形体を配置する工程、第2成形体を配置する工程、及び前記枠体を形成する工程の後に、
前記第1触媒層の主面に前記第1ガス拡散層を配置する工程と、
前記第2触媒層の主面に前記第2ガス拡散層を配置する工程と、
を含み、
前記第1成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第1成形体の内縁部より内側に前記第1ガス拡散層を配置し、
前記第2成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第2成形体の内縁部より内側に前記第2ガス拡散層を配置する、第1~7態様のいずれか1つに記載の電極-膜-枠接合体の製造方法を提供する。
前記第2成形体は、前記第2ガス拡散層と隙間を空けて配置され、
前記枠体を形成する工程の後、前記隙間に弾性体を配置する工程をさらに含む、第8又は9態様に記載の電極-膜-枠接合体の製造方法を提供する。
前記枠体は、
第1成形体と第2成形体と第3成形体とを有し、
前記第1成形体は、額縁状の形状を有し、前記電解質膜の厚み方向から見て、前記電解質膜の周縁部と少なくとも前記第1成形体の内縁部とが重なるように、前記電解質膜の第1の主面側に配置され、
前記第2成形体は、額縁状の形状を有し、前記電解質膜の厚み方向から見て、前記電解質膜の周縁部と少なくとも前記第2成形体の内縁部とが重なるように、前記電解質膜の第2の主面側に配置され、
前記第3成形体は、前記第1成形体と前記第2成形体とを一体的に接続するように、前記第1成形体と前記第2成形体との間に配置されている、
電極-膜-枠接合体を提供する。
前記第1成形体を構成する材料は、前記第1触媒層の周縁部の主面に混在しておらず、
前記第2成形体を構成する材料は、前記第2触媒層の周縁部の主面に混在していない、第13又は14態様に記載の電極-膜-枠接合体を提供する。
前記枠体は、
前記電解質膜の厚み方向から見て、前記第1触媒層の周縁部と前記第1成形体の少なくとも内縁部とが重なるように、前記第1成形体が配置され、
前記電解質膜の厚み方向から見て、前記第2触媒層の周縁部と前記第2成形体の少なくとも内縁部とが重なるように、前記第2成形体が配置されている、第13~16態様のいずれか1つに記載の電極-膜-枠接合体の製造方法を提供する。
前記第2成形体は、前記電解質膜の厚み方向から見て、前記第2ガス拡散層の周縁部より外側に配置されている、第13~17態様のいずれか1つに記載の電極-膜-枠接合体を提供する。
前記第1及び第2成形体のいずれか他方は、熱可塑性エラストマーで構成されている、
第21態様に記載の電極-膜-枠接合体を提供する。
以下、本発明の実施の形態について、図面を参照しながら説明する。
図1~図5を用いて、本発明の第1実施形態にかかる電極-膜-枠接合体を有する燃料電池の構造を説明する。図1は、本第1実施形態にかかる電極-膜-枠接合体を有する燃料電池の構造を、一部を分解して模式的に示す斜視図である。図2は、図1のII-II線断面におけるセルの積層断面を、一部を分解して示す図である。図3は、図1の電極-膜-枠接合体の構成を模式的に示す平面図であり、図4は、図3のIV-IV線断面図である。図5は、図1の電極-膜-枠接合体のアノードセパレータ側の表面構造を示す平面図であり、図6は、カソードパレータ側の表面構造を示す平面図である。
また、第3成形体63は、第1成形体61及び第2成形体62よりも圧縮弾性率の低い材料で構成されていてもよい。この場合、第1成形体61及び第2成形体62を圧縮弾性率の低い材料で接続することにより、例えば、ハンドリング時に高分子電解質膜5Aにかかる機械的なストレスを低減できるため、高分子電解質膜5Aの機械的劣化を抑制できる。第3成形体63の好適な材料としては、例えば、後述するガスケット7に用いられる熱可塑性樹脂又は熱可塑性エラストマーと同様の材料を用いることができ、例えば、ガラスフィラーが充填されていないポリプロピレンを用いることができる。
以上により、図4に示す電極-膜-枠接合体1が製造される。
以上により、図4に示す電極-膜-枠接合体1が製造される。
図9は、本発明の第2実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第2実施形態にかかる電極-膜-枠接合体1Aが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、第3成形体63aが第2触媒層5B2の周縁部の主面と接触していない点である。
図10は、本発明の第3実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第3実施形態にかかる電極-膜-枠接合体1Bが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、前記第2実施形態と同様に、第3成形体63bが第2触媒層5B2の周縁部の主面と接触していない点である。
図11は、本発明の第4実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第4実施形態にかかる電極-膜-枠接合体1Cが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、第3成形体63cが第2触媒層5B2の周縁部の主面と接触しておらず、第3成形体63cが第1触媒層5B1側に回り込んで第1触媒層5B1の周縁部の主面の一部と接触するように形成されている点である。
図12は、本発明の第5実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第5実施形態にかかる電極-膜-枠接合体1Dが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、第3成形体63dが第1触媒層5B1側に回り込んで第1触媒層5B1の周縁部の主面の一部と接触するように形成されている点である。
図13は、本発明の第6実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第6実施形態にかかる電極-膜-枠接合体1Eが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、高分子電解質膜5Aの厚み方向から見て、高分子電解質膜5Aの周縁部より第1触媒層5B1の周縁部が内側に形成されている点である。
図15は、本発明の第7実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第7実施形態にかかる電極-膜-枠接合体1Fが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、高分子電解質膜5Aの厚み方向から見て、高分子電解質膜5Aの周縁部より第1触媒層5B1及び第2触媒層5B2の周縁部が内側に形成されている点である。また、第3成形体63fが第1触媒層5B1側に回り込むように設けられている。
図16は、本発明の第8実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第8実施形態にかかる電極-膜-枠接合体1Gが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、高分子電解質膜5Aの厚み方向から見て、高分子電解質膜5Aの周縁部より第1触媒層5B1の周縁部が内側に配置され、かつ、第1触媒層5B1の周縁部と第1成形体61の内縁部とが重ならないように形成されている点である。
図17は、本発明の第9実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第9実施形態にかかる電極-膜-枠接合体1Hが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、高分子電解質膜5Aの厚み方向から見て、高分子電解質膜5Aの周縁部より第2触媒層5B2の周縁部が内側に配置され、かつ、第2触媒層5B2の周縁部と第2成形体62の内縁部とが重ならないように形成されている点である。また、第1触媒層5B1の周縁部の主面の一部が露出するように形成し、第3成形体63hが第1触媒層5B1側に回り込むように形成されている。
図18は、本発明の第10実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第10実施形態にかかる電極-膜-枠接合体1Iが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、高分子電解質膜5Aの厚み方向から見て、第1ガス拡散層5C1の周縁部が第2ガス拡散層5C2の周縁部より外側に配置され、かつ、第1ガス拡散層5C1の周縁部と第2成形体62の内縁部とが重なるように配置されている点である。
図19は、本発明の第11実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第11実施形態にかかる電極-膜-枠接合体1Jが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、高分子電解質膜5Aの厚み方向から見て、第2ガス拡散層5C2の周縁部が第1ガス拡散層5C1の周縁部より外側に配置され、かつ、第2ガス拡散層5C2の周縁部と第1成形体61bの内縁部とが重なるように配置されている点である。
図20は、本発明の第12実施形態にかかる電極-膜-枠接合体の構成を模式的に示す平面図である。図21は、図20のVI-VI線断面図である。本第12実施形態にかかる電極-膜-枠接合体1Kが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、第1成形体61cが第2成形体62と同じ大きさに形成され、それらをつなぐように第3成形体63kが形成されている点である。
以上により、図21に示す電極-膜-枠接合体1Kが製造される。
図23は、本発明の第13実施形態にかかる電極-膜-枠接合体の構成を模式的に示す平面図である。図24は、図23のVIII-VIII線断面図である。本第13実施形態にかかる電極-膜-枠接合体1Lが前記第13実施形態にかかる電極-膜-枠接合体1Kと異なる点は、第1成形体61cの一部と第2成形体62の一部とが、第3成形体63lを射出成形する前に一体的に接続されている点である。すなわち、本第13実施形態においては、第1成形体61cと第2成形体62とが一体成形されている。
図25は、本発明の第14実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第14実施形態にかかる電極-膜-枠接合体1Mが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、枠体6が第1及び第2ガス拡散層5C1,5C2との間に隙間を空けて設けられ、当該隙間を塞ぐようにガスケット7,7から延伸した弾性体の一例である延伸部7C1,7C2が設けられている点である。本第14実施形態において、延伸部7C1,7C2を含むガスケット7全体は、発電部の近くにおいて、高温及び高圧の熱可塑性樹脂が高分子電解質膜5Aに直接接触することが無いような方法で形成されている。例えば、ガスケット7は、予め射出成形された弾性体で構成されている。
図27は、本発明の第16実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第15実施形態にかかる電極-膜-枠接合体1Nが前記第14実施形態にかかる電極-膜-枠接合体1Mと異なる点は、延伸部7C1,7C2により隙間40を塞ぐことに代えて、弾性体71により隙間40を塞ぐようにした点である。
図28は、本発明の第16実施形態にかかる電極-膜-枠接合体を、MEAの周縁部と枠体との接合部分を拡大して示す模式断面図である。本第16実施形態にかかる電極-膜-枠接合体1Pが前記第1実施形態にかかる電極-膜-枠接合体1と異なる点は、第3成形体63pを構成する樹脂材料の一部が第2成形体62の全部または一部を覆っている点である。このような構成によっても、前記第1実施形態と同様の効果を得ることができる。
Claims (25)
- 高分子電解質膜の第1の主面に配置された第1触媒層と、前記第1触媒層の主面に配置された第1ガス拡散層と、前記電解質膜の第2の主面に配置された第2触媒層と、前記第2触媒層の主面に配置された第2ガス拡散層と、を有する膜電極接合体の周縁部に枠体が形成された電極-膜-枠接合体の製造方法であって、
前記製造方法は、
前記電解質膜の厚み方向から見て、前記電解質膜の周縁部と予め成形された額縁状の形状を有する第1成形体の少なくとも内縁部とが重なるように、前記電解質膜の第1の主面側に前記第1成形体を配置する工程と、
前記電解質膜の厚み方向から見て、前記電解質膜の周縁部と予め成形された額縁状の形状を有する第2成形体の少なくとも内縁部とが重なるように、前記電解質膜の第2の主面側に前記第2成形体を配置する工程と、
前記第1成形体を配置する工程及び前記第2成形体を配置する工程の後、前記電解質膜の厚み方向から見て前記第2成形体の外縁部よりも内側に位置する前記電解質膜の第2の主面の内側領域に直接接することなく、前記第1成形体及び前記第2成形体を一体的に接続するように、前記第1成形体と前記第2成形体との間に第3成形体を射出成形することにより、前記第1成形体と前記第2成形体と前記第3成形体とを含む前記枠体を形成する工程と、
を含む、電極-膜-枠接合体の製造方法。 - 前記第2成形体を配置する工程において、前記第2触媒層の周縁部の主面の一部が露出するように前記第2触媒層の周縁部上に前記第2成形体を配置し、
前記枠体を形成する工程において、前記電解質膜の厚み方向から見て、前記第3成形体の一部と前記露出する第2触媒層の周縁部の一部とが重なるように、前記第3成形体を射出成形する、請求項1に記載の電極-膜-枠接合体の製造方法。 - 前記枠体を形成する工程において、前記第3成形体を構成する樹脂材料の一部が前記露出する第2触媒層の周縁部の一部に混在するように、前記第3成形体を射出成形する、請求項2に記載の電極-膜-枠接合体の製造方法。
- 前記第1成形体を配置する工程において、前記第1触媒層の周縁部の主面の一部が露出するように、前記第1触媒層の周縁部上に前記第1成形体を配置し、
前記枠体を形成する工程において、前記電解質膜の厚み方向から見て、前記第3成形体の一部と前記露出する第1触媒層の周縁部の一部とが重なるように、前記第3成形体を射出成形する、請求項2に記載の電極-膜-枠接合体の製造方法。 - 前記枠体を形成する工程において、前記第3成形体を構成する樹脂材料の一部が前記露出する第1触媒層の周縁部の一部に混在するように、前記第3成形体を射出成形する、請求項4に記載の電極-膜-枠接合体の製造方法。
- 前記膜電極接合体は、前記電解質膜の厚み方向から見て、前記第1触媒層の周縁部及び前記第2触媒層の周縁部のうち少なくとも一方が、前記電解質膜の周縁部より内側に配置されている、請求項1~5のいずれか1つに記載の電極-膜-枠接合体の製造方法。
- 前記膜電極接合体は、
前記電解質膜の厚み方向から見て、前記第1触媒層の周縁部が前記第1ガス拡散層の周縁部より外側に配置され、前記第2触媒層の周縁部が前記第2ガス拡散層の周縁部より外側に配置され、
前記第1成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第1触媒層の周縁部と前記第1成形体の少なくとも内縁部とが重なるように、前記第1成形体を配置し、
前記第2成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第2触媒層の周縁部と前記第2成形体の少なくとも内縁部とが重なるように、前記第2成形体を配置する、請求項1~5のいずれか1つに記載の電極-膜-枠接合体の製造方法。 - 前記製造方法は、
前記第1成形体を配置する工程、前記第2成形体を配置する工程、及び前記枠体を形成する工程の前に、
前記第1触媒層の主面に前記第1ガス拡散層を配置する工程と、
前記第2触媒層の主面に前記第2ガス拡散層を配置する工程と、
を含み、
前記第1成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第1ガス拡散層の周縁部より外側に前記第1成形体を配置し、
前記第2成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第2ガス拡散層の周縁部より外側に前記第2成形体を配置する、請求項1~7のいずれか1つに記載の電極-膜-枠接合体の製造方法。 - 前記製造方法は、
前記第1成形体を配置する工程、前記第2成形体を配置する工程、及び前記枠体を形成する工程の後に、
前記第1触媒層の主面に前記第1ガス拡散層を配置する工程と、
前記第2触媒層の主面に前記第2ガス拡散層を配置する工程と、
を含み、
前記第1成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第1成形体の内縁部より内側に前記第1ガス拡散層を配置し、
前記第2成形体を配置する工程において、前記電解質膜の厚み方向から見て、前記第2成形体の内縁部より内側に前記第2ガス拡散層を配置する、請求項1~7のいずれか1つに記載の電極-膜-枠接合体の製造方法。 - 前記枠体を形成する工程においては、前記第3成形体を構成する樹脂材料の一部が前記第2ガス拡散層の周縁部に混在するように射出成形される、請求項8又は9に記載の電極-膜-枠接合体の製造方法。
- 前記第1成形体は、前記第1ガス拡散層と隙間を空けて配置され、
前記第2成形体は、前記第2ガス拡散層と隙間を空けて配置され、
前記枠体を形成する工程の後、前記隙間に弾性体を配置する工程をさらに含む、請求項8~10のいずれか1つに記載の電極-膜-枠接合体の製造方法。 - 前記第1成形体と前記第2成形体とは、前記第3成形体により接続される前に、それらの一部が接続されるように一体成形されている、請求項1に記載の電極-膜-枠接合体の製造方法。
- 高分子電解質膜の第1の主面に配置された第1触媒層と、前記第1触媒層の主面に配置された第1ガス拡散層と、前記電解質膜の第2の主面に配置された第2触媒層と、前記第2触媒層の主面に配置された第2ガス拡散層と、を有する膜電極接合体の周縁部に枠体が形成された電極-膜-枠接合体であって、
前記枠体は、
第1成形体と第2成形体と第3成形体とを有し、
前記第1成形体は、額縁状の形状を有し、前記電解質膜の厚み方向から見て、前記電解質膜の周縁部と少なくとも前記第1成形体の内縁部とが重なるように、前記電解質膜の第1の主面側に配置され、
前記第2成形体は、額縁状の形状を有し、前記電解質膜の厚み方向から見て、前記電解質膜の周縁部と少なくとも前記第2成形体の内縁部とが重なるように、前記電解質膜の第2の主面側に配置され、
前記第3成形体は、前記第1成形体と前記第2成形体とを一体的に接続するように、前記第1成形体と前記第2成形体との間に配置されている、
電極-膜-枠接合体。 - 前記枠体は、前記電解質膜の厚み方向から見て、前記第1触媒層及び前記第2触媒層の周縁部の一部のうち少なくとも一方と前記第3成形体の一部とが重なるように配置されている、請求項13に記載の電極-膜-枠接合体。
- 前記第3成形体を構成する樹脂材料の一部は、前記第1触媒層の周縁部の主面の一部及び第2触媒層の周縁部の主面の一部のうち少なくとも一方に混在しており、
前記第1成形体を構成する材料は、前記第1触媒層の周縁部の主面に混在しておらず、
前記第2成形体を構成する材料は、前記第2触媒層の周縁部の主面に混在していない、請求項13又は14に記載の電極-膜-枠接合体。 - 前記電解質膜の厚み方向から見て、前記第1触媒層の周縁部及び前記第2触媒層の周縁部のうち少なくとも一方が、前記電解質膜の周縁部より内側に配置されている、請求項13~15のいずれか1つに記載の電極-膜-枠接合体。
- 前記電解質膜の厚み方向から見て、前記第1触媒層の周縁部が前記第1ガス拡散層の周縁部より外側に配置され、前記第2触媒層の周縁部が前記第2ガス拡散層の周縁部より外側に配置され、
前記枠体は、
前記電解質膜の厚み方向から見て、前記第1触媒層の周縁部と前記第1成形体の少なくとも内縁部とが重なるように、前記第1成形体が配置され、
前記電解質膜の厚み方向から見て、前記第2触媒層の周縁部と前記第2成形体の少なくとも内縁部とが重なるように、前記第2成形体が配置されている、請求項13~16のいずれか1つに記載の電極-膜-枠接合体。 - 前記第1成形体は、前記電解質膜の厚み方向から見て、前記第1ガス拡散層の周縁部より外側に配置され、
前記第2成形体は、前記電解質膜の厚み方向から見て、前記第2ガス拡散層の周縁部より外側に配置されている、請求項13~17のいずれか1つに記載の電極-膜-枠接合体。 - 前記第1及び第2成形体のうち少なくとも一方は、前記第1及び第2ガス拡散層のうち少なくとも一方と隙間を空けて配置され、当該隙間と当該隙間に隣接する前記第1及び第2成形体のうち少なくとも一方とを覆うように弾性体が配置されている、請求項18に記載の電極-膜-枠接合体。
- 前記弾性体は、前記弾性体を構成する樹脂材料の一部が、前記隙間に隣接する第1及び第2ガス拡散層のうち少なくとも一方の周縁部に混在している、請求項19に記載の電極-膜-枠接合体。
- 前記第1成形体と第2成形体とは、硬度が異なる樹脂材料で構成されている、請求項13に記載の電極-膜-枠接合体。
- 前記第1及び第2成形体のいずれか一方は、熱可塑性樹脂で構成され、
前記第1及び第2成形体のいずれか他方は、熱可塑性エラストマーで構成されている、
請求項21に記載の電極-膜-枠接合体。 - 前記第1及び第2成形体のうち少なくとも一方は、熱可塑性樹脂層と熱可塑性エラストマー層とを含む複層構造で構成されている、請求項13に記載の電極-膜-枠接合体。
- 前記熱可塑性エラストマー層が前記第1又は第2触媒層の周縁部と接触するように構成されている、請求項23に記載の電極-膜-枠接合体。
- 請求項13~24のいずれか1つに記載の電極-膜-枠接合体を備える燃料電池。
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Also Published As
Publication number | Publication date |
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CN102365778B (zh) | 2014-11-05 |
EP2523244B1 (en) | 2018-08-01 |
EP2523244A1 (en) | 2012-11-14 |
US20110311898A1 (en) | 2011-12-22 |
CN102365778A (zh) | 2012-02-29 |
US10044047B2 (en) | 2018-08-07 |
JPWO2011083548A1 (ja) | 2013-05-13 |
JP4890665B2 (ja) | 2012-03-07 |
EP2523244A4 (en) | 2016-09-07 |
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