US20140017590A1 - Electrolyte membrane-electrode assembly for fuel cells, and method for producing same - Google Patents

Electrolyte membrane-electrode assembly for fuel cells, and method for producing same Download PDF

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Publication number
US20140017590A1
US20140017590A1 US14/008,193 US201214008193A US2014017590A1 US 20140017590 A1 US20140017590 A1 US 20140017590A1 US 201214008193 A US201214008193 A US 201214008193A US 2014017590 A1 US2014017590 A1 US 2014017590A1
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US
United States
Prior art keywords
electrode
resin
frame member
resin frame
gas diffusion
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Abandoned
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US14/008,193
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English (en)
Inventor
Masashi Sugishita
Daisuke Okonogi
Yoshihito Kimura
Yukihito Tanaka
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Honda Motor Co Ltd
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Honda Motor Co Ltd
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Filing date
Publication date
Application filed by Honda Motor Co Ltd filed Critical Honda Motor Co Ltd
Assigned to HONDA MOTOR CO., LTD. reassignment HONDA MOTOR CO., LTD. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: KIMURA, YOSHIHITO, OKONOGI, DAISUKE, SUGISHITA, MASASHI, TANAKA, YUKIHITO
Publication of US20140017590A1 publication Critical patent/US20140017590A1/en
Priority to US15/857,807 priority Critical patent/US10658683B2/en
Abandoned legal-status Critical Current

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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
    • H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0276—Sealing means characterised by their form
    • 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
    • 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
    • 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
    • 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
    • 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
    • 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 membrane electrode assembly (electrolyte membrane-electrode assembly for fuel cells), and a method of producing the fuel cell membrane electrode assembly.
  • the fuel cell membrane electrode assembly includes a solid polymer electrolyte membrane and a first electrode and a second electrode provided on both sides of the solid polymer electrolyte membrane.
  • Each of the first electrode and the second electrode includes an electrode catalyst layer and a gas diffusion layer.
  • the outer size of the first electrode is smaller than the outer size of the second electrode.
  • a solid polymer electrolyte fuel cell employs a solid polymer electrolyte membrane.
  • the solid polymer electrolyte membrane is a polymer ion exchange membrane.
  • the fuel cell includes a membrane electrode assembly (MEA) where an anode and a cathode are provided on both sides of the solid polymer electrolyte membrane.
  • Each of the anode and the cathode includes a catalyst layer (electrode catalyst layer) and a gas diffusion layer (porous carbon).
  • the membrane electrode assembly is sandwiched between separators (bipolar plates).
  • a predetermined number of the fuel cells are stacked together to form a fuel cell stack.
  • the fuel cell stack is mounted in a fuel cell electric vehicle as an in-vehicle fuel cell stack.
  • the membrane electrode assembly has structure where components of the MEA have different sizes, i.e., the surface size (surface area) of one of diffusion layers is smaller than the surface size (surface area) of the solid polymer electrolyte membrane, and the surface size of the other of the gas diffusion layers is the same as the surface size of the solid polymer electrolyte membrane (a stepped-type MEA).
  • a membrane electrode assembly disclosed in Japanese Laid-Open Patent Publication No. 2007-066766 (hereinafter referred to as conventional technique) includes an electrolyte membrane 1 , a cathode catalyst layer 2 a provided on one side of the electrolyte membrane 1 , an anode catalyst layer 2 b provided on the other surface of the electrolyte membrane 1 , and gas diffusion layers 3 a , 3 b provided on both sides of the electrolyte membrane 1 .
  • the surface area of the gas diffusion layer 3 b of the anode is equal to the surface area of the electrolyte membrane 1 , and larger than the surface area of the gas diffusion layer 3 a of the cathode.
  • a gasket structure body 4 is provided in an edge area of the membrane electrode assembly (MEA), and the outer end of the electrolyte membrane 1 adjacent to the gas diffusion layer 3 a is joined to the gasket structure body 4 through an adhesive layer 5 .
  • the MEA and the gasket structure body 4 are fixed to the outer marginal portion of the electrolyte membrane 1 exposed to the outside from the gas diffusion layer 3 a , through the adhesive layer 5 only. Therefore, the strength of joining the MEA and the gasket structure body 4 is low, and the desired strength cannot be obtained.
  • the present invention has been made to solve the problem of this type, and an object of the present invention is to provide a fuel cell membrane electrode assembly and a method of producing the fuel cell membrane electrode assembly in which it is possible to firmly and easily join a resin frame member around a solid polymer electrolyte membrane, and suitably suppress deformation of the resin frame member.
  • the present invention relates to a fuel cell membrane electrode assembly, and a method of producing the fuel cell membrane electrode assembly.
  • the fuel cell membrane electrode assembly includes a solid polymer electrolyte membrane and a first electrode and a second electrode provided on both sides of the solid polymer electrolyte membrane.
  • Each of the first electrode and the second electrode includes an electrode catalyst layer and a gas diffusion layer.
  • An outer size of the first electrode is smaller than an outer size of the second electrode.
  • the membrane electrode assembly includes a resin frame member provided around the solid polymer electrolyte membrane and an impregnation portion for joining the resin frame member and at least one of an outer marginal portion of the first electrode and an outer marginal portion of the second electrode together.
  • the production method includes the steps of forming the first electrode and the second electrode on both sides of the solid polymer electrolyte membrane, forming a resin frame member, and overlapping an outer marginal portion of the first electrode and an inner marginal portion of the resin frame member with each other and heating the overlapped portions of the first electrode and the resin frame member to impregnate only the outer marginal portion of the first electrode with the inner marginal portion of the resin frame member and join the resin frame member around the solid polymer electrolyte membrane.
  • the production method includes the steps of overlapping an outer marginal portion of the gas diffusion layer of the first electrode and an inner marginal portion of the resin frame member with each other and heating the overlapped portions of the first electrode and the resin frame member to impregnate only the outer marginal portion of the first electrode with the inner marginal portion of the resin frame member and join the resin frame member to the first electrode, forming the electrode catalyst layers on both surfaces of the solid polymer electrolyte membrane, and combining the gas diffusion layer of the first electrode joined to the resin frame member and the gas diffusion layer of the second electrode on both sides of the solid polymer electrolyte membrane into one piece.
  • the production method includes the steps of overlapping an outer marginal portion of the gas diffusion layer of the first electrode and an inner marginal portion of the resin frame member with each other and heating the overlapped portions of the first electrode and the resin frame member to impregnate only the outer marginal portion of the first electrode with the inner marginal portion of the resin frame member and join the resin frame member to the first electrode, forming the electrode catalyst layer on the gas diffusion layer of the second electrode and forming the electrode catalyst layer of the first electrode on one side of the solid polymer electrolyte membrane, and combining the first electrode joined to the resin frame member and the second electrode on both sides of the solid polymer electrolyte membrane into one piece.
  • the impregnation portion joining the resin frame member and the at least one of the outer marginal portion of the first electrode and the outer marginal portion of the second electrode together is provided.
  • the joining strength for joining the resin frame member to at least one of the first electrode and the second electrode is improved suitably, and it is possible to suppress occurrence of peeling or the like as much as possible.
  • the resin frame member is joined only to the first electrode. Therefore, the portion of the resin frame member where heat contraction occurs is reduced, and it becomes possible to suppress occurrence of warpage or the like of the resin frame member. Thus, it is possible to firmly and easily join the resin frame member around the solid polymer electrolyte membrane, and suitably suppress deformation of the resin frame member.
  • the outer ends of the gas diffusion layers of the first electrode and the second electrode and the resin frame member are impregnated with resin to form the resin impregnation portion integrally.
  • the joining strength for joining the resin frame member to the first electrode and the second electrode is improved suitably, and it is possible to suppress occurrence of peeling or the like as much as possible.
  • the outer end of the gas diffusion of the second electrode and the resin frame member are impregnated with resin to form the resin impregnation portion integrally. Therefore, the portion of the resin frame member where heat contraction occurs is reduced, and it becomes possible to suppress occurrence of warpage or the like of the resin frame member. Further, since the resin impregnation portion is provided only at the second electrode having the large size, as the resin member, resin mixed with a glass filler is adopted, and it becomes possible to use resin having high melting temperature.
  • FIG. 1 is an exploded perspective view showing main components of a solid polymer electrolyte fuel cell including a membrane electrode assembly according to a first embodiment of the present invention
  • FIG. 2 is a cross sectional view showing the fuel cell, taken along a line II-II in FIG. 1 ;
  • FIG. 3 is a front view showing a cathode of the membrane electrode assembly
  • FIG. 4 is a partial cross sectional view showing an MEA having different sizes of components in a production method according to the first embodiment of the present invention
  • FIG. 5 is a view showing a resin frame member
  • FIG. 6 is a view showing a process of joining the MEA and the resin frame member
  • FIG. 7 is a diagram showing steps of a production method according to a second embodiment of the present invention.
  • FIG. 8 is a diagram showing steps of a production method according to a third embodiment of the present invention.
  • FIG. 9 is a cross sectional view showing a solid polymer electrolyte fuel cell including a membrane electrode assembly according to a fourth embodiment of the present invention.
  • FIG. 10 is a front view showing a cathode of the membrane electrode assembly
  • FIG. 11 is a front view showing an anode of the membrane electrode assembly
  • FIG. 12 is a view showing a method of producing the membrane electrode assembly
  • FIG. 13 is a view showing a comparative example of the membrane electrode assembly
  • FIG. 14 is a cross sectional view showing main components of a membrane electrode assembly according to a fifth embodiment of the present invention.
  • FIG. 15 is a cross sectional view showing main components of a membrane electrode assembly according to a sixth embodiment of the present invention.
  • FIG. 16 is a cross sectional view showing main components of a membrane electrode assembly according to a seventh embodiment of the present invention.
  • FIG. 17 is a cross sectional view showing a solid polymer electrolyte fuel cell including a membrane electrode assembly according to an eighth embodiment of the present invention.
  • FIG. 18 is a view showing a method of producing the membrane electrode assembly.
  • FIG. 19 is a view showing a membrane electrode assembly disclosed in Japanese Laid-Open Patent Publication No. 2007-066766.
  • a solid polymer electrolyte fuel cell 12 including a membrane electrode assembly 10 according to a first embodiment of the present invention is formed by sandwiching the membrane electrode assembly 10 between a first separator 14 and a second separator 16 .
  • the first separator 14 and the second separator 16 are made of metal plates such as steel plates, stainless steel plates, aluminum plates, plated steel sheets, or metal plates having anti-corrosive surfaces by surface treatment.
  • carbon members may be used as the first separator 14 and the second separator 16 .
  • the membrane electrode assembly 10 includes a solid polymer electrolyte membrane 18 , and an anode (second electrode) 20 and a cathode (first electrode) 22 sandwiching the solid polymer electrolyte membrane 18 .
  • the solid polymer electrolyte membrane 18 is formed by impregnating a thin membrane of perfluorosulfonic acid with water, for example.
  • a fluorine based electrolyte may be used as the solid polymer electrolyte membrane 18 .
  • an HC (hydrocarbon) based electrolyte may be used as the solid polymer electrolyte membrane 18 .
  • the surface size (surface area) of the cathode 22 is smaller than the surface sizes (surface areas) of the solid polymer electrolyte membrane 18 and the anode 20 . It should be noted that the surface size of the cathode 22 may be equal to or larger than the surface size of the anode 20 .
  • the anode 20 is provided on one surface 18 a of the solid polymer electrolyte membrane 18 and the cathode 22 is provided on the other surface 18 b of the solid polymer electrolyte membrane 18 such that a frame shaped outer portion of the solid polymer electrolyte membrane 18 is exposed.
  • the anode 20 includes an electrode catalyst layer 20 a joined to the surface 18 a of the solid polymer electrolyte membrane 18 and a gas diffusion layer 20 c stacked on the electrode catalyst layer 20 a through an intermediate layer (underlying layer) 20 b .
  • the cathode 22 includes an electrode catalyst layer 22 a joined to the surface 18 b of the solid polymer electrolyte membrane 18 and a gas diffusion layer 22 c stacked on the electrode catalyst layer 22 a through an intermediate layer (underlying layer) 22 b.
  • Each of the electrode catalyst layers 20 a , 22 a is formed by carbon black supporting platinum particles as catalyst particles.
  • polymer electrolyte As an ion conductive binder, polymer electrolyte is used. Catalyst paste formed by mixing the catalyst particles uniformly in the solution of this polymer electrolyte is printed, applied (coated) or transferred on both surfaces 18 a , 18 b of the solid polymer electrolyte membrane 18 to form the electrode catalyst layers 20 a , 22 a.
  • Carbon black and FEP (fluorinated ethylene-propylene copolymer) particles and carbon nanotube are prepared in a form of paste, and coated on the gas diffusion layer 20 c , 22 c to form the intermediate layers 20 b , 22 b .
  • the gas diffusion layers 20 c , 22 c are made of carbon papers or the like, and the surface size of the gas diffusion layer 20 c is larger that the surface size of the gas diffusion layer 22 c.
  • the membrane electrode assembly 10 includes a resin frame member 24 formed around the solid polymer electrolyte membrane 18 , and joined only to the cathode 22 of the solid polymer electrolyte membrane 18 .
  • the resin frame member 24 is made of PPS (poly phenylene sulfide), PPA (polyphthalamide), etc., and includes an impregnation portion 26 for impregnation of only the outer marginal portion of the cathode 22 with the inner marginal portion of the resin frame member 24 .
  • an oxygen-containing gas supply passage 30 a for supplying an oxygen-containing gas, a coolant supply passage 32 a for supplying a coolant, and a fuel gas discharge passage 34 b for discharging a fuel gas such as a hydrogen-containing gas are arranged in a vertical direction indicated by an arrow C.
  • the oxygen-containing gas supply passage 30 a , the coolant supply passage 32 a , and the fuel gas discharge passage 34 b extend through the fuel cell 12 in a stacking direction indicated by an arrow A.
  • a fuel gas supply passage 34 a for supplying the fuel gas, a coolant discharge passage 32 b for discharging the coolant, and an oxygen-containing gas discharge passage 30 b for discharging the oxygen-containing gas are arranged in the direction indicated by the arrow C.
  • the fuel gas supply passage 34 a , the coolant discharge passage 32 b , and the oxygen-containing gas discharge passage 30 b extend through the fuel cell 12 in the direction indicated by the arrow A.
  • the second separator 16 has an oxygen-containing gas flow field 36 on its surface 16 a facing the membrane electrode assembly 10 .
  • the oxygen-containing gas flow field 36 is connected to the oxygen-containing gas supply passage 30 a and the oxygen-containing gas discharge passage 30 b.
  • the first separator 14 has a fuel gas flow field 38 on its surface 14 a facing the membrane electrode assembly 10 .
  • the fuel gas flow field 38 is connected to the fuel gas supply passage 34 a and the fuel gas discharge passage 34 b .
  • a coolant flow field 40 is formed between a surface 14 b of the first separator 14 and a surface 16 b of the second separator 16 .
  • the coolant flow field 40 is connected to the coolant supply passage 32 a and the coolant discharge passage 32 b.
  • a first seal member 42 is formed integrally with the surfaces 14 a , 14 b of the first separator 14 , around the outer end of the first separator 14 .
  • a second seal member 44 is formed integrally with the surfaces 16 a , 16 b of the second separator 16 , around the outer end of the second separator 16 .
  • the first seal member 42 includes a first ridge seal 42 a which contacts the resin frame member 24 of the membrane electrode assembly 10 , and a second ridge seal 42 b interposed between the first separator 14 and the second separator 16 .
  • the second seal member 44 is a flat surface seal. Instead of providing the second ridge seal 42 b , the second seal member 44 may have a ridge seal (not shown).
  • Each of the first seal member 42 and the second seal members 44 is made of seal material, cushion material, or packing material such as an EPDM (ethylene propylene diene monomer) rubber, an NBR (nitrile butadiene rubber), a fluoro rubber, a silicone rubber, a fluorosilicone rubber, a butyl rubber, a natural rubber, a styrene rubber, a chloroprene rubber, or an acrylic rubber.
  • EPDM ethylene propylene diene monomer
  • NBR nitrile butadiene rubber
  • fluoro rubber a silicone rubber
  • fluorosilicone rubber a butyl rubber
  • natural rubber a styrene rubber
  • chloroprene rubber a chloroprene rubber
  • acrylic rubber acrylic rubber
  • the first separator 14 has supply holes 46 connecting the fuel gas supply passage 34 a to the fuel gas flow field 38 , and discharge holes 48 connecting the fuel gas flow field 38 to the fuel gas discharge passage 34 b.
  • an MEA 50 having different sizes of components is produced. Specifically, the electrode catalyst layers 20 a , 22 a are coated on both surfaces 18 a , 18 b of the solid polymer electrolyte membrane 18 , and the intermediate layers 20 b , 22 b each comprising a mixture of water-repellent agent and carbon particles are coated on the gas diffusion layers 20 c , 22 c.
  • the gas diffusion layer 20 c is placed on a side adjacent to the surface 18 a of the solid polymer electrolyte membrane 18 , i.e., the gas diffusion layer 20 c is placed such that the intermediate layer 20 b faces the electrode catalyst layer 20 a .
  • the gas diffusion layer 22 c is placed on a side adjacent to the surface 18 b of the solid polymer electrolyte membrane 18 , i.e., the gas diffusion layer 22 c is placed such that the intermediate layer 22 b faces the electrode catalyst layer 22 a .
  • the resin frame member 24 is formed by an injection molding machine (not shown) beforehand.
  • the dimension (width) H 1 of the resin frame member 24 and the dimension (thickness) H 1 of the MEA 50 are the same.
  • the resin frame member 24 has an inner extension 24 a at its inner marginal portion.
  • the thickness H 2 of the inner extension 24 a and the thickness H 2 of the cathode 22 of the MEA 50 are the same.
  • the extension length L of the inner extension 24 a is the sum of the distance from the front end of the solid polymer electrolyte membrane 18 of the MEA 50 to the front end of the cathode 22 and the length of the impregnation portion 26 .
  • the MEA 50 is placed on a base table 52 such that the anode 20 is positioned on the lower side.
  • the front end of the inner extension 24 a of the resin frame member 24 is overlapped with the outer marginal portion of the cathode 22 of the MEA 50 .
  • a glass plate 54 is placed on the resin frame member 24 .
  • a load F is applied to the resin frame member 24 through the glass plate 54 , toward the base table 52 , and a laser beam Lb is radiated from a laser machine 56 through the glass plate 54 to the overlapped portions (an area where the outer marginal portion of the cathode 22 and the inner marginal portion of the resin frame member 24 are overlapped with each other).
  • the inner extension 24 a of the resin frame member 24 as the inner marginal portion is locally heated in a concentrated manner, and melted.
  • the gas diffusion layer 22 c of the cathode 22 is impregnated with the melted resin of the inner extension 24 a of the resin frame member 24 . Therefore, as shown in FIG. 2 , the resin frame member 24 is joined to the cathode 22 by the impregnation portion 26 where only the outer marginal portion of the cathode 22 is impregnated with the melted resin of the inner marginal portion of the resin frame member 24 . In this manner, the membrane electrode assembly 10 is produced.
  • the joining strength for joining the resin frame member 24 to the cathode 22 is improved suitably, and it is possible to suppress occurrence of peeling or the like as much as possible.
  • the resin frame member 24 is joined only to the cathode 22 , the portion of the resin frame member 24 where heat contraction occurs is reduced, and it becomes possible to suppress occurrence of warpage or the like of the resin frame member 24 .
  • the heating treatment is applied only to the overlapped portions in a concentrated manner by laser heating using the laser machine 56 . Therefore, since the resin frame member 24 is heated only locally, the time required for melting is reduced. Accordingly, cost reduction is achieved, and deformation is reduced as much as possible. It should be noted that infrared welding, impulse welding or the like may be adopted instead of laser welding using the laser machine 56 .
  • an oxygen-containing gas is supplied to the oxygen-containing gas supply passage 30 a , and a fuel gas such as a hydrogen-containing gas is supplied to the fuel gas supply passage 34 a . Further, coolant such as pure water, ethylene glycol, or oil is supplied to the coolant supply passage 32 a.
  • the oxygen-containing gas flows from the oxygen-containing gas supply passage 30 a to the oxygen-containing gas flow field 36 of the second separator 16 .
  • the oxygen-containing gas moves in the direction indicated by the arrow B, and the oxygen-containing gas is supplied to the cathode 22 of the membrane electrode assembly 10 .
  • the fuel gas flows from the fuel gas supply passage 34 a through the supply holes 46 into the fuel gas flow field 38 of the first separator 14 .
  • the fuel gas flows along the fuel gas flow field 38 in the direction indicated by the arrow B, and the fuel gas is supplied to the anode 20 of the membrane electrode assembly 10 .
  • the oxygen-containing gas supplied to the cathode 22 and the fuel gas supplied to the anode 20 are partially consumed in the electrochemical reactions in the electrode catalyst layers for generating electricity.
  • the oxygen-containing gas partially consumed at the cathode 22 flows along the oxygen-containing gas discharge passage 30 b , and the oxygen-containing gas is discharged in the direction indicated by the arrow A.
  • the fuel gas partially consumed at the anode 20 flows through the discharge holes 48 .
  • the fuel gas flow along the fuel gas discharge passage 34 b , and the fuel gas is discharged in the direction indicated by the arrow A.
  • the coolant supplied to the coolant supply passage 32 a flows into the coolant flow field 40 between the first separator 14 and the second separator 16 . Then, the coolant flows in the direction indicated by the arrow B. After the coolant cools the membrane electrode assembly 10 , the coolant is discharged into the coolant discharge passage 32 b.
  • FIG. 7 is a diagram showing steps of a method of producing the membrane electrode assembly 10 according to a second embodiment of the present invention.
  • the intermediate layer 20 b is coated on the gas diffusion layer of the anode (S 1 ), and the intermediate layer 22 b is coated on the gas diffusion layer 22 c of the cathode (S 2 ).
  • the resin frame member 24 formed by injection molding beforehand is joined to the gas diffusion layer 22 c (S 3 ).
  • the process of joining the gas diffusion layer 22 c of the cathode 22 to the resin frame member 24 is substantially the same as in the case of the first embodiment.
  • the gas diffusion layer 22 c and the resin frame member 24 are joined together by placing the gas diffusion layer 22 c on the base table 52 shown in FIG. 6 . In this manner, the resin frame member 24 and the gas diffusion layer 22 c of the cathode 22 are combined into one piece by the impregnation portion 26 .
  • the electrode catalyst layers 20 a , 22 a are coated on both surfaces 18 a , 18 b of the solid polymer electrolyte membrane 18 (S 4 ). Further, the gas diffusion layer 20 c of the anode and the gas diffusion layer 22 c joined to the resin frame member 24 are placed on both surfaces 18 a , 18 b of the solid polymer electrolyte membrane 18 , respectively. These components are subjected to hot pressing treatment to produce the membrane electrode assembly 10 (S 5 ).
  • FIG. 8 is a diagram showing steps of a method of producing a membrane electrode assembly 10 according to a third embodiment of the present invention.
  • the electrode catalyst layer 20 a is coated on the intermediate layer 20 b of the gas diffusion layer 20 c (S 12 ).
  • the resin frame member 24 is joined to the gas diffusion layer 22 c (S 14 ). The process of joining the gas diffusion layer 22 c to the resin frame member 24 is the same as in the cases of the first and second embodiments.
  • the electrode catalyst layer 22 a of the cathode is coated on the surface 18 b of the solid polymer electrolyte membrane 18 (S 15 ). Then, the gas diffusion layer 20 c of the anode and the gas diffusion layer 22 c of the cathode joined to the resin frame member 24 are placed on both surfaces 18 a , 18 b of the solid polymer electrolyte membrane 18 , respectively. These components are subjected to hot pressing treatment to produce the membrane electrode assembly 10 (S 16 ).
  • FIG. 9 is a cross sectional view showing a solid polymer electrolyte fuel cell 62 including a membrane electrode assembly 60 according to a fourth embodiment of the present invention.
  • the constituent elements of the solid polymer electrolyte fuel cell 62 that are identical to those of the solid polymer electrolyte fuel cell 12 including the membrane electrode assembly 10 according to the first embodiment are labeled with the same reference numerals, and descriptions thereof will be omitted.
  • the constituent elements that are identical to those of the solid polymer electrolyte fuel cell 12 including the membrane electrode assembly 10 according to the first embodiment are labeled with the same reference numerals, and descriptions thereof will be omitted.
  • the anode 20 includes an electrode catalyst layer 20 a joined to the surface 18 a of the solid polymer electrolyte membrane 18 and a gas diffusion layer 20 c stacked on the electrode catalyst layer 20 a .
  • the cathode 22 includes an electrode catalyst layer 22 a joined to the surface 18 b of the solid polymer electrolyte membrane 18 and a gas diffusion layer 22 c stacked on the electrode catalyst layer 22 a .
  • the electrode catalyst layer 20 a and the gas diffusion layer 20 c may be provided through an intermediate layer (underlying layer).
  • the electrode catalyst layer 22 a and the gas diffusion layer 22 c may be provided through an intermediate layer (underlying layer).
  • the resin frame member 24 and the gas diffusion layer 22 c of the cathode 22 are combined into one piece by a first resin impregnation portion 26 a
  • the resin frame member 24 and the gas diffusion layer 20 c of the anode 20 are combined into one piece by a second resin impregnation portion 26 b.
  • the first resin impregnation portion 26 a is formed over the entire circumference of the gas diffusion layer 22 c of the cathode 22 .
  • the width L 1 on the long side of the first resin impregnation portion 26 a (side extending in the direction indicated by the arrow B) is larger than the width L 2 on the short side of the first resin impregnation portion 26 a (side extending in the direction indicated by the arrow C) (L 1 >L 2 ).
  • the second resin impregnation portion 26 b is formed over the entire circumference of the gas diffusion layer 20 c of the anode 20 .
  • the width L 3 on the long side of the second resin impregnation portion 26 b (side extending in the direction indicated by the arrow B) is larger than the width L 4 on the short side of the second resin impregnation portion 26 b (side extending in the direction indicated by the arrow C) (L 3 >L 4 ).
  • the second resin impregnation portion 26 b is terminated at a position spaced outward of a first inner circumferential portion 24 c of the resin frame member 24 adjacent to the cathode 22 by the distance H. That is, the second resin impregnation portion 26 b is not provided at a position overlapped with the cathode 22 in the stacking direction.
  • an MEA 64 having different sizes of components (stepped-type MEA) of the membrane electrode assembly 60 is produced.
  • the electrode catalyst layers 20 a , 22 a are coated on both surfaces 18 a , 18 b of the solid polymer electrolyte membrane 18 .
  • the gas diffusion layer 20 c is placed adjacent to the surface 18 a of the solid polymer electrolyte membrane 18 , i.e., on the electrode catalyst layer 20 a
  • the gas diffusion layer 22 c is placed adjacent to the surface 18 b of the solid polymer electrolyte membrane 18 , i.e., on the electrode catalyst layer 22 a .
  • These components are stacked together, and subjected to hot pressing treatment to produce the MEA 64 .
  • the resin frame member 24 is formed beforehand by an injection molding machine (not shown).
  • the resin frame member 24 is positioned in alignment with the MEA 64 .
  • the resin frame member 24 has the first inner circumferential portion 24 c and a second inner circumferential portion 24 d .
  • the end of the cathode 22 is positioned at the first inner circumferential portion 24 c
  • the end of the anode 20 is positioned at the second inner circumferential portion 24 d.
  • a first resin member 26 aa forming the first resin impregnation portion 26 a is prepared at the cathode 22
  • a second resin member 26 bb forming the second resin impregnation portion 26 b is prepared at the anode 20 .
  • Each of the first resin member 26 aa and the second resin member 26 bb has a frame shape, and is made of the same material as the resin frame member 24 , for example.
  • the resin frame member 24 uses resin material enforced by mixing a filler with the resin material.
  • the first resin member 26 aa and the second resin member 26 bb may be made of resin material which is not mixed with any filler.
  • the MEA 64 and the resin frame member 24 can be joined together.
  • the first resin member 26 aa and the second resin member 26 bb are placed over the MEA 64 and the resin frame member 24 and a load is applied to the MEA 64 and the resin frame member 24 through the first resin member 26 aa and the second resin member 26 bb , the first resin member 26 aa and the second resin member 26 bb are heated.
  • a heating method any of laser welding, infrared welding, and impulse welding, etc. is adopted.
  • the first resin member 26 aa and the second resin member 26 bb are melted by heating.
  • Both of the gas diffusion layer 22 c of the cathode 22 and the resin frame member 24 are impregnated with the melted resin of the first resin member 26 aa
  • both of the gas diffusion layer 20 c of the anode 20 and the resin frame member 24 are impregnated with the melted resin of the second resin member 26 bb.
  • the first resin impregnation portion 26 a is formed over the gas diffusion layer 22 c of the cathode 22 and the resin frame member 24
  • the second resin impregnation portion 26 b is formed over the gas diffusion layer 20 c of the anode 20 and the resin frame member 24 to produce the membrane electrode assembly 60 .
  • the outer ends of the gas diffusion layers 22 c , 20 c of the cathode 22 and the anode 20 and the resin frame member 24 are impregnated with resin, respectively, and formed integrally with the first resin impregnation portion 26 a and the second resin impregnation portion 26 b.
  • the joining strength for joining the resin frame member 24 to the cathode 22 and the anode 20 is improved suitably, and it is possible to suppress occurrence of peeling or the like as much as possible.
  • the width L 1 on the long side of the first resin impregnation portion 26 a is larger than the width L 2 on the short side of the first resin impregnation portion 26 a (L 1 >L 2 ) (see FIG. 10 ).
  • the width L 3 on the long side of the second resin impregnation portion 26 b is larger than the width L 4 on the short side of the second resin impregnation portion 26 b (L 3 >L 4 ) (see FIG. 11 ).
  • the second resin impregnation portion 26 b is terminated at a position spaced outward of the first inner circumferential portion 24 c of the resin frame member 24 adjacent to the cathode 22 , by the distance H.
  • the distance H In the range of the distance H, since the electrode catalyst layer 22 a of the cathode 22 facing the anode 20 is not present, abnormal reaction does not occur.
  • the gas diffusion layer 22 c of the cathode 22 and the resin frame member 24 are combined into one piece by a first resin impregnation portion 27 a .
  • the gas diffusion layer 20 c of the anode 20 and the resin frame member 24 are combined into one piece by a second resin impregnation portion 27 b .
  • the second resin impregnation portion 27 b extends inward of the end of the first resin impregnation portion 27 a by the distance Ha.
  • the electrode catalyst layer 22 a of the cathode 22 is present in the range of the distance Ha where the second resin impregnation portion 27 b is provided.
  • shortage of hydrogen occurs at the anode 20 in the range of the distance Ha, and abnormal reaction tends to occur at the cathode 22 .
  • FIG. 14 is a cross sectional view showing main components of a membrane electrode assembly 70 according to a fifth embodiment of the present invention.
  • the membrane electrode assembly 70 includes a resin frame member 72 joined to the cathode 22 and the anode 20 .
  • a first resin protrusion 74 a and a second resin protrusion 74 b are formed integrally with the resin frame member 72 for combining the resin frame member 72 and the gas diffusion layer 22 c of the cathode 22 into one piece, and combining the resin frame member 72 and the gas diffusion layer 20 c of the anode 20 into one piece.
  • the first resin protrusion 74 a is formed in a frame shape around the first inner circumferential portion 24 c
  • the second resin protrusion 74 b is formed in a frame shape around the second inner circumferential portion 24 d .
  • the first resin protrusion 74 a has an inclined surface 74 as as an end surface opposite to the first inner circumferential portion 24 c , and the inclined surface 74 as is inclined in a direction spaced from the resin frame member 72 .
  • the second resin protrusion 74 b has an inclined surface 74 bs as an end surface opposite to the second inner circumferential portion 24 d , and the inclined surface 74 bs is inclined in a direction spaced from the resin frame member 72 .
  • the first resin protrusion 74 a and the second resin protrusion 74 b are heated by a heating machine (not shown), and melted.
  • a heating machine not shown
  • the gas diffusion layers 22 c , 20 c are impregnated with the melted resin of the first resin protrusion 74 a and the second resin protrusion 74 b .
  • the first resin impregnation portion 26 a and the second resin impregnation portion 26 b are formed.
  • FIG. 15 is a cross sectional view showing main components of a membrane electrode assembly 80 according to a sixth embodiment of the present invention.
  • the membrane electrode assembly 80 includes a resin frame member 82 joined to the cathode 22 and the anode 20 .
  • the resin frame member 82 includes a first resin member 84 a and a second resin member 84 b for combining the resin frame member 82 and the gas diffusion layer 22 c of the cathode 22 into one piece, and combining the resin frame member 82 and the gas diffusion layer 20 c of the anode 20 into one piece.
  • the first resin member 84 a and the second resin member 84 b are formed integrally with the resin frame member 82 by insert molding beforehand.
  • the first resin member 84 a and the second resin member 84 b are heated by a heating machine (not shown), and melted.
  • a heating machine not shown
  • the gas diffusion layers 22 c , 20 c are impregnated with the melted resin of the first resin member 84 a and the second resin member 84 b .
  • the first resin impregnation portion 26 a and the second resin impregnation portion 26 b are formed.
  • FIG. 16 is a cross sectional view showing a membrane electrode assembly 90 according to a seventh embodiment of the present invention.
  • the membrane electrode assembly 90 includes a resin frame member 92 joined to the cathode 22 and the anode 20 .
  • a first resin protrusion 94 a and a second resin protrusion 94 b are provided integrally with the resin frame member 92 for combining the resin frame member 92 and the gas diffusion layer 22 c of the cathode 22 into one piece, and combining the resin frame member 92 and the gas diffusion layer 20 c of the anode 20 into one piece.
  • the first resin protrusion 94 a is formed in a frame shape around the first inner circumferential portion 24 c
  • the second resin protrusion 94 b is formed in a frame shape around the second inner circumferential portion 24 d.
  • Each of the first resin protrusion 94 a and the second resin protrusion 94 b has a rectangular shape in cross section.
  • the first resin protrusion 94 a and the second resin protrusion 94 b are formed by eliminating the inclined surfaces 74 as , 74 bs of the first resin protrusion 74 a and the second resin protrusion 74 b in the membrane electrode assembly 70 according to the fifth embodiment.
  • the first resin protrusion 94 a and the second resin protrusion 94 b are heated by a heating machine (not shown), and melted.
  • the gas diffusion layers 22 c , 20 c are impregnated with the melted resin of the first resin protrusion 94 a and the second resin protrusion 94 b .
  • the first resin impregnation portion 26 a and the second resin impregnation portion 26 b are formed.
  • FIG. 17 is a cross sectional view showing a solid polymer electrolyte fuel cell 102 including a membrane electrode assembly 100 according to an eighth embodiment of the present invention.
  • the resin frame member 24 and the gas diffusion layer 20 c of the anode 20 are combined into one piece by a resin impregnation portion 104 . That is, the resin frame member 24 is joined only to the anode 20 which is larger than the cathode 22 .
  • an MEA 106 having different sizes of components (stepped-type MEA) of the membrane electrode assembly 100 is produced.
  • a resin member 104 a for forming the resin impregnation portion 104 is prepared.
  • the resin member 104 a has a frame shape, and uses resin material enforced by mixing a glass filler with the resin material.
  • the resin member 104 a is heated.
  • the heated resin member 104 a is melted to form the resin impregnation portion 104 over the gas diffusion layer 20 c of the anode 20 and the resin frame member 24 .
  • the membrane electrode assembly 100 is produced.
  • the glass filler when the resin member 104 a is heated, and melted, the glass filler does not enter the gas diffusion layer 20 c . Therefore, the resin member 104 a does not directly contact the solid polymer electrolyte membrane 18 .
  • the resin member 104 a it become possible to adopt resin mixed with a glass filler, and use resin having high melting temperature.
  • the resin used for the resin member 104 a can be adopted from a wide variety of selection advantageously.

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  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Fuel Cell (AREA)
US14/008,193 2011-04-01 2012-03-23 Electrolyte membrane-electrode assembly for fuel cells, and method for producing same Abandoned US20140017590A1 (en)

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WO2017055815A1 (en) * 2015-09-30 2017-04-06 Intelligent Energy Limited Fuel cell sub-assembly
US10637077B2 (en) 2018-03-02 2020-04-28 Honda Motor Co., Ltd. Frame equipped membrane electrode assembly and fuel cell
US10665873B2 (en) 2015-10-21 2020-05-26 Honda Motor Co., Ltd. Resin frame equipped membrane electrode assembly for fuel cell and method of producing the same
US10727504B2 (en) 2016-11-17 2020-07-28 Honda Motor Co., Ltd. Method of operating fuel cell
US11018366B2 (en) 2019-01-18 2021-05-25 Honda Motor Co., Ltd. Method of producing frame equipped membrane electrode assembly, the frame equipped membrane electrode and fuel cell
US20210226241A1 (en) * 2020-01-17 2021-07-22 Toyota Jidosha Kabushiki Kaisha Fuel cell and method of manufacturing fuel cell
US11121384B2 (en) 2019-07-30 2021-09-14 Honda Motor Co., Ltd. Frame equipped membrane electrode assembly and fuel cell
US11196058B2 (en) 2019-07-30 2021-12-07 Honda Motor Co., Ltd. Frame equipped membrane electrode assembly, method of producing the frame equipped membrane electrode assembly, and fuel cell
US11374240B2 (en) 2019-09-30 2022-06-28 Toyota Jidosha Kabushiki Kaisha Fuel-cell unit cell
US11437632B2 (en) 2019-09-30 2022-09-06 Toyota Jidosha Kabushiki Kaisha Fuel-cell unit cell
US11600831B2 (en) 2019-09-30 2023-03-07 Toyota Jidosha Kabushiki Kaisha Fuel-cell unit cell

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JP6100225B2 (ja) * 2014-11-20 2017-03-22 本田技研工業株式会社 燃料電池用樹脂枠付き電解質膜・電極構造体
JP6442393B2 (ja) * 2015-10-22 2018-12-19 本田技研工業株式会社 燃料電池用樹脂枠付き電解質膜・電極構造体
JP6843730B2 (ja) * 2016-11-17 2021-03-17 本田技研工業株式会社 燃料電池及びその運転方法
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US20160190610A1 (en) * 2013-08-08 2016-06-30 Nissan Motor Co., Ltd. Membrane electrode assembly with frame, fuel cell single cell, and fuel cell stack
WO2017055815A1 (en) * 2015-09-30 2017-04-06 Intelligent Energy Limited Fuel cell sub-assembly
US11056694B2 (en) 2015-09-30 2021-07-06 Intelligent Energy Limited Fuel cell sub-assembly
US10665873B2 (en) 2015-10-21 2020-05-26 Honda Motor Co., Ltd. Resin frame equipped membrane electrode assembly for fuel cell and method of producing the same
US11094947B2 (en) 2015-10-21 2021-08-17 Honda Motor Co., Ltd. Resin frame equipped membrane electrode assembly for fuel cell and method of producing the same
US10727504B2 (en) 2016-11-17 2020-07-28 Honda Motor Co., Ltd. Method of operating fuel cell
US10637077B2 (en) 2018-03-02 2020-04-28 Honda Motor Co., Ltd. Frame equipped membrane electrode assembly and fuel cell
US11018366B2 (en) 2019-01-18 2021-05-25 Honda Motor Co., Ltd. Method of producing frame equipped membrane electrode assembly, the frame equipped membrane electrode and fuel cell
US11121384B2 (en) 2019-07-30 2021-09-14 Honda Motor Co., Ltd. Frame equipped membrane electrode assembly and fuel cell
US11196058B2 (en) 2019-07-30 2021-12-07 Honda Motor Co., Ltd. Frame equipped membrane electrode assembly, method of producing the frame equipped membrane electrode assembly, and fuel cell
US11374240B2 (en) 2019-09-30 2022-06-28 Toyota Jidosha Kabushiki Kaisha Fuel-cell unit cell
US11437632B2 (en) 2019-09-30 2022-09-06 Toyota Jidosha Kabushiki Kaisha Fuel-cell unit cell
US11600831B2 (en) 2019-09-30 2023-03-07 Toyota Jidosha Kabushiki Kaisha Fuel-cell unit cell
US20210226241A1 (en) * 2020-01-17 2021-07-22 Toyota Jidosha Kabushiki Kaisha Fuel cell and method of manufacturing fuel cell
US11588167B2 (en) * 2020-01-17 2023-02-21 Toyota Jidosha Kabushiki Kaisha Fuel cell and method of manufacturing fuel cell

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DE112012001547T5 (de) 2013-12-24
CN103443981A (zh) 2013-12-11
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WO2012137609A1 (ja) 2012-10-11
US10658683B2 (en) 2020-05-19
CN103443981B (zh) 2016-08-17
US20180145359A1 (en) 2018-05-24

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