JP2009026536A - Electrolyte membrane-electrode assembly for solid polymer fuel cell and manufacturing method thereof, catalyst transfer film used for this, and solid polymer fuel cell - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide an electrolyte membrane-electrode assembly for a solid polymer fuel cell in which one layer consisting of a proton conductive material is arranged between an electrolyte membrane and a catalyst layer and formation of a proton conductive path is secured to obtain an effect to prevent deterioration of power generation performance, to provide a manufacturing method thereof, to provide a catalyst transfer film used for the electrolyte membrane-electrode assembly, and to provide a solid polymer fuel cell. <P>SOLUTION: The electrolyte membrane-electrode assembly (33) has at least a catalyst layer (22) and a porous electrode layer (27) laminated on both surfaces of an electrolyte membrane (24). The electrolyte membrane (24) is constructed of a proton conductive material enveloping a filler, and at least a part of the filler is exposed from the electrolyte membrane (24), a proton conductive material layer (23) exists between the electrolyte membrane (24) and at least one of the catalyst layer (22), moreover, the filler and the proton conductive material layer (23) are in direct contact. <P>COPYRIGHT: (C)2009,JPO&INPIT

Description

  The present invention relates to an electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell, a method for producing the same, a catalyst transfer film used therefor, and a polymer electrolyte fuel cell.

  A polymer electrolyte fuel cell is made up of a solid polymer membrane with proton conductivity as an electrolyte, and a fuel electrode and an air electrode are joined to both sides of this membrane. Hydrogen is supplied to the fuel electrode and oxygen or air is supplied to the air electrode. This is a system that generates electricity through an electrochemical reaction. The following reactions occur at each electrode.

Fuel electrode: H ₂ → 2H ⁺ + 2e ⁻
Air electrode: (1/2) O ₂ + 2H ⁺ + 2e ⁻ → H ₂ O
Total reaction: H ₂ + (1/2) O ₂ → H ₂ O
As can be seen from these reaction equations, only water is generated during power generation. Fuel cells are attracting attention as one of the next generation clean energy systems.

  The polymer electrolyte fuel cell can generate electric power even when methanol is supplied as a fuel. In this case, the polymer electrolyte fuel cell is particularly called a direct methanol fuel cell. The following reactions occur at each electrode.

Fuel electrode: CH ₃ OH + H ₂ O → 6H ⁺ + 6e ⁻ + CO ₂
Air electrode: (3/2) O ₂ + 6H ⁺ + 6e ⁻ → 3H ₂ O
All reactions: CH ₃ OH + (3/2) O ₂ → 2H ₂ O + CO ₂
A polymer electrolyte fuel cell has a structure in which a proton conductive polymer electrolyte membrane is used as an electrolyte membrane, a catalyst layer is arranged on both sides thereof, an electrode base material is arranged on both sides thereof, and this is further sandwiched between separators. is doing. The one in which the catalyst layers are arranged on both surfaces of the electrolyte membrane (that is, the layer configuration of catalyst layer / electrolyte membrane / catalyst layer) is called an electrolyte membrane-catalyst layer assembly (abbreviation: CCM), An electrode base material disposed on both surfaces of the electrolyte membrane-catalyst layer assembly (ie, electrode base material / catalyst layer / electrolyte membrane / catalyst layer / electrode base material layer structure) is an electrolyte membrane-electrode joint. It is called a body (abbreviation: MEA).

  Examples of proton conductive polymer electrolyte membranes include, for example, perfluorosulfonic acid-based fluorine ion exchange resins, and more specifically, perfluorocarbon sulfonic acid-based ones in which C—H bonds of hydrocarbon-based ion exchange membranes are substituted with fluorine. Examples include polymers (PFS polymers). By introducing a fluorine atom having high electronegativity, it is chemically very stable, the dissociation degree of the sulfonic acid group is high, and high ion conductivity can be realized. Specific examples of such a proton conductive polymer electrolyte membrane include “Nafion” (registered trademark) manufactured by DuPont, “Flemion” (registered trademark) manufactured by Asahi Glass Co., Ltd., and “Aciplex” manufactured by Asahi Kasei Corporation. "(Registered trademark)", "Gore Select" (registered trademark) manufactured by Gore, and the like.

These perfluorocarbon sulfonic acid-based polymers exhibit high performance as an electrolyte membrane as described above, but have a problem of high cost. In addition, there is a problem that remarkable deterioration is observed at a high temperature range of 80 ° C. or higher, and proton conductivity is remarkably lowered by drying of the electrolyte membrane. Furthermore, since it swells due to water content and shows a large dimensional change, there also arises a problem that the catalyst layer formed on the electrolyte membrane is peeled off after repeated start / stop (humidification / drying). In order to make up for these drawbacks, proposals have been made to embed fillers such as polymer fibers and inorganic particles in the polymer electrolyte membrane to increase water retention under high temperature conditions and to suppress dimensional changes. (For example, Patent Documents 1 and 2).
JP 2003-157862 A JP-A-6-1111827

However, if a part of the filler is exposed on the surface of the electrolyte membrane, the proton conduction path is broken at the junction with the catalyst layer, which causes a decrease in power generation performance. An electrolyte membrane-electrode junction for a polymer electrolyte fuel cell in which a layer made of a proton conductive material is disposed between the membrane and the catalyst layer to ensure the formation of a proton conduction path and to suppress the deterioration of power generation performance. And a catalyst transfer film used therefor, and a polymer electrolyte fuel cell.

  The electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell of the present invention is an electrolyte membrane-electrode assembly in which at least a catalyst layer and a porous electrode layer are laminated on both surfaces of the electrolyte membrane, the electrolyte membrane Is composed of a proton conductive material containing a filler, at least a part of the filler is exposed from the electrolyte membrane, and a proton conductive material layer exists between at least one of the electrolyte membrane and the catalyst layer. The filler and the proton conductive material layer are in direct contact with each other.

  The catalyst transfer film of the present invention is characterized in that a catalyst layer composed of catalyst particles and an electrolyte binder is formed on a base film, and a proton conductive material layer is further formed thereon.

  The polymer electrolyte fuel cell of the present invention incorporates any one of the above electrolyte membrane-electrode assemblies for polymer electrolyte fuel cells.

  In the method for producing an electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell of the present invention, a catalyst layer comprising catalyst particles and an electrolyte binder is formed on a base film, and a proton conductive material layer is further formed thereon. The step of arranging the proton conductive material layer side of the formed catalyst transfer film toward the electrolyte membrane, the step of hot pressing the catalyst transfer film-electrolyte membrane-catalyst transfer film laminate, and the heat pressing The step of peeling the base film from the catalyst transfer film-electrolyte membrane-catalyst transfer film laminate to obtain an electrolyte membrane-catalyst layer assembly, and a pair of electrode groups on both surfaces of the electrolyte membrane-catalyst layer assembly Placing the material.

  In another method for producing an electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell according to the present invention, a catalyst layer comprising catalyst particles and an electrolyte binder is formed on an electrode substrate, and a proton conductive material is further formed thereon. A step of disposing the proton conductive material layer side of the gas diffusion electrode formed with the layer toward the electrolyte membrane, and a step of hot pressing the gas diffusion electrode-electrolyte membrane-gas diffusion electrode laminate.

  The present invention is for a polymer electrolyte fuel cell in which a layer made of a proton conductive material is disposed between an electrolyte membrane and a catalyst layer, the formation of a proton conduction path is ensured, and the effect of suppressing a decrease in power generation performance is obtained. An electrolyte membrane-electrode assembly and a production method thereof, a catalyst transfer film used therefor, and a polymer electrolyte fuel cell can be provided.

  In the present invention, the electrolyte membrane is composed of a proton conductive material containing a filler.

The proton conductive material constituting the electrolyte membrane is a general proton conductive material used for fuel cells, such as a fluorine-based proton conductive polymer material, a hydrocarbon-based proton conductive material, and an inorganic proton conductive material. Material, organic-inorganic hybrid proton conductive material, ionic liquid, and a mixture thereof. Examples of the fluorine-based proton conductive polymer material include Nafion (trade name), Flemion (trade name), and Aciplex (trade name). Hydrocarbon proton conductive materials are phosphoric acid impregnated polybenzimidazole (PBI), alkylsulfonic acid impregnated polybenzimidazole (PBI), sulfonated 4-phenoxybenzoyl-1,4-phenylene (SPPBP), sulfonated polyether ether Examples include ketones (SPEEK) and styrene-ethylene / butylene / ethylene block copolymers. Examples of inorganic proton conductive materials include metal hydrated oxides such as tungsten oxide and tin oxide hydrate, multi-component silica such as SiO ₂ —H ₃ PO ₄ and SiO ₂ —TiO ₂ —P ₂ O ₅ , TiO 2. Metal phosphate compounds such as _2- H ₃ PO ₄ , heteropoly acid complexes such as phosphotungstic acid and phosphomolybdic acid, inorganic substances such as CsHSO ₄ , CsH ₂ PO ₄ , Sn _X In _(1-X) P ₂ O ₇ Examples thereof include oxyacid salts. Organic-inorganic hybrid materials include hybrid materials made of polyether polymers such as silica and polyethylene oxide (PEO), polypropylene oxide (PPO), or polytetramethylene oxide (PTMO), and solids such as tungstophosphoric acid. An example to which an acid is added is given. Examples of the ionic liquid include 1-ethyl-3-methylimidazolium bis (trifluoromethylsulfonyl) imide (EMI-TFSI), 1-ethyl-3-methylimidazolium triflate (EMI-Tf), 1-ethyl- An example is 3-methylimidazolium fluorohydrogenate (EMIm (HF) nF).

  The filler is included for the purpose of improving mechanical strength, dimensional stability, heat resistance, chemical stability, water retention and the like with respect to the electrolyte membrane. For example, polymer fibrils and inorganic particle materials are included. Used. Examples of the polymer fibrils include polytetrafluoroethylene, polyimide, polyethylene terephthalate, polyamide (nylon), polysulfone, polyethersulfone, polyphenylene sulfide, polyetheretherketone, polyetherimide, polyarylate, polyethylene naphthalate, Ethylene tetrafluoroethylene copolymer (ETFE), tetrafluoroethylene-hexafluoropropylene copolymer (FEP), tetrafluoroperfluoroalkyl vinyl ether copolymer (PFA), polytetrafluoroethylene (PTFE), etc. it can. Examples of the inorganic particle material include silica, alumina, zirconia, titania, magnesia, molybdenum oxide, tungsten oxide, zinc oxide, tin oxide, barium titanate, aluminum titanate, silicon carbide, and silicon nitride. Further, the inorganic particle material may be added with a different metal element for the purpose of improving the mechanical strength. For example, as for zirconia, partially stabilized zirconia to which yttrium is added (referred to as “YSZ”) can be cited as an example. The inorganic particle material may be a laminated body of spherical particles, a porous body, or a self-organized structure of scaly particles.

  Hereinafter, embodiments of an electrolyte membrane for a polymer electrolyte fuel cell and a method for producing the same according to the present invention will be described with reference to the drawings.

  1A to 1D are schematic cross-sectional views of an electrolyte membrane containing a filler in a comparative example. The filler represents the polymer fibril 2 in FIG. 1A, the inorganic particle material 3 in FIG. 1B, and the scaly particle material 4 in FIG. 1C. 1 is a proton conductive material. A part of the fillers 2 to 4 are exposed on the surfaces of these electrolyte membranes 10 as indicated by a plurality of arrows, and as shown on the left side of FIG. There is a risk of performance degradation due to the interruption of the proton conduction path indicated by the arrow. In FIG. 1D, 1 is a proton conductive material, 5 is a filler (support), 7 is catalyst particles, and 8 is an electrolyte binder. The disconnection of the proton conduction path means, for example, a state where the electrolyte binder 8 and the proton conductive material 1 are not in contact with each other due to the presence of the filler 5 having poor proton conductivity between the electrolyte binder 8 and the proton conductive material 1. Point to.

  In order to prevent performance degradation due to the disconnection of the proton conduction path at the time of joining with the catalyst layer 9 as shown on the left side of FIG. As shown in an example of the invention, an electrolyte membrane 10 in which proton conductive material layers 11, 11a, and 11b are formed on the surface of an electrolyte membrane 10 including fillers 2 to 4 is used. The filler represents the polymer fibril 2 in FIG. 2A, the inorganic particle material 3 in FIG. 2B, and the scaly particle material 4 in FIG. 2C. A proton conductive material layer 11 is formed on the surfaces of these electrolyte membranes 10 and the filler exposed in FIGS. 1A to 1D is covered. In this case, at the time of joining with the catalyst layer 9, the proton conduction path indicated by the two-way arrow is not interrupted, and the performance is not deteriorated (FIG. 2D).

The proton conductive material layer is selected from the group consisting of a fluorine-based proton conductive polymer material, a hydrocarbon proton conductive material, an inorganic proton conductive material, an organic-inorganic hybrid proton conductive material, and a mixture thereof. It is preferable. Examples of the fluorine-based proton conductive polymer material include Nafion (trade name), Flemion (trade name), and Aciplex (trade name). Hydrocarbon proton conductive materials are phosphoric acid impregnated polybenzimidazole (PBI), alkylsulfonic acid impregnated polybenzimidazole (PBI), sulfonated 4-phenoxybenzoyl-1,4-phenylene (SPPBP), sulfonated polyether ether Examples include ketones (SPEEK) and styrene-ethylene / butylene / ethylene block copolymers. Examples of inorganic proton conductive materials include metal hydrated oxides such as tungsten oxide and tin oxide hydrate, multi-component silica such as SiO ₂ —H ₃ PO ₄ and SiO ₂ —TiO ₂ —P ₂ O ₅ , TiO 2. Metal phosphate compounds such as _2- H ₃ PO ₄ , heteropoly acid complexes such as phosphotungstic acid and phosphomolybdic acid, inorganic substances such as CsHSO ₄ , CsH ₂ PO ₄ , Sn _X In _(1-X) P ₂ O ₇ Examples thereof include oxyacid salts. Organic-inorganic hybrid materials include hybrid materials made of polyether polymers such as silica and polyethylene oxide (PEO), polypropylene oxide (PPO), or polytetramethylene oxide (PTMO), and solids such as tungstophosphoric acid. An example to which an acid is added is given.

  In the coating of the proton conductive material layer on the electrolyte membrane, a known method such as knife coating, gravure coating, bar coating, or screen printing can be used. Further, the coating treatment may be performed on a single sheet, or a long film having an arbitrary length may be formed by continuously coating a long electrolyte film.

  The proton conductive material layer has a thickness of 0.01 to 10.00 μm. When the thickness of the proton conductive material layer exceeds about 10.00 μm, the membrane resistance increases, and there is a concern about the decrease in power generation performance. On the other hand, if the thickness of the proton conductive material layer is less than about 0.01 μm, the filler exposed from the electrolyte membrane is not sufficiently covered, and the power generation performance due to the cutting of the proton conduction path is lowered. Thus, in order to cover the filler exposed from the electrolyte membrane and form a sufficient proton conduction path, the thickness of the proton conductive material layer covering the electrolyte membrane needs to be in an appropriate region. .

  FIG. 3 is a schematic view showing a cross section of an electrolyte membrane-catalyst layer assembly using the electrolyte membrane of the present invention shown in FIG. As shown in FIG. 3, catalyst layers 13 and 13 'made of catalyst particles and an electrolyte binder are formed on both surfaces of the electrolyte membrane 12, respectively.

  FIG. 4 is a cross-sectional view of the electrolyte membrane-electrode assembly in one embodiment of the present invention. A fuel electrode 15 composed of a catalyst layer 13 and an electrode base material 14 is disposed on the electrolyte membrane 12, and an air electrode 17 composed of a catalyst layer 13 ′ and an electrode base material 16 is disposed under the electrolyte membrane 12. ing. And a single cell (fuel cell) is comprised by arrange | positioning the separator with a rib and a collector (not shown) further on both these outer sides. Protons flow from the fuel electrode 15 through the electrolyte membrane 12 to the air electrode 17. Further, electrons flow from the fuel electrode 15 to the air electrode 17 via an external circuit. As a result, electricity flows between the fuel electrode 15 and the air electrode 17.

  5A to 5D are cross-sectional views of the catalyst transfer film 20 in one embodiment of the present invention. As shown in FIG. 5A, a catalyst layer 22 made of catalyst particles and an electrolyte binder is formed on a transfer substrate 21, and a proton conductive material layer 23 is arranged on the catalyst layer 22. As shown in FIG. 5B, the catalyst transfer film 20 is overlaid on at least one surface of the electrolyte membrane 24 encapsulating the filler so that the proton conductive material layer 23 is in contact with the electrolyte membrane 24, and hot pressing (for example, 135 To 150 ° C., 3 to 6 MPa), the catalyst layers 22 and 22 are bonded onto the electrolyte membrane 24, and then the transfer base materials 21 and 21 are peeled to form the electrolyte membrane-catalyst layer assembly 30. Form (FIG. 5C). Furthermore, the electrolyte membrane-electrode assembly 31 is obtained by disposing the electrode base materials 25 and 26 on both surfaces of the electrolyte membrane-catalyst layer assembly 30 (FIG. 5D).

  6A-B are cross-sectional views of the gas diffusion electrode 32 in one embodiment of the present invention. A catalyst layer 22 composed of catalyst particles and an electrolyte binder is formed on a conductive electrode substrate 27, and a proton conductive material layer 23 is disposed on the catalyst layer 22 (FIG. 6A). A pair of the gas diffusion electrodes 32 are overlapped on both surfaces of the electrolyte membrane 24 containing the filler so that the proton conductive material layer 23 is in contact with the electrolyte membrane 24, and hot pressing (for example, 135 to 150 ° C., 3 to 6 MPa). As a result, the catalyst layer 22 is bonded onto the electrolyte membrane 24 to obtain an electrolyte membrane-electrode assembly 33 (FIG. 6B). In the gas diffusion electrode 32, a porous layer made of a carbon material called a planarization layer or a diffusion layer may be formed between the electrode base material 27 and the catalyst layer 22.

  The transfer substrate is not only a polymer film such as polyimide, polyethylene terephthalate, polytetrafluoroethylene (PTFE), but also coated paper such as art paper, coated paper, lightweight coated paper, notebook paper, copy paper, etc. The non-coated paper may be used. These are examples of transfer base materials, and are limited to these as long as they can form a coating film on the catalyst layer by coating and drying and can peel the catalyst layer in the thermal transfer step. Not what you want.

  The catalyst particles are fine particles composed of material particles having a catalytic action and a conductive carrier. The material particles having the catalytic action are particularly limited as long as the material has a fuel oxidizing ability or a reducing agent reducing ability. It is not a thing. For example, platinum or a platinum compound is used as the material having the catalytic action. Examples of the platinum compound include an alloy of platinum and at least one metal selected from the group consisting of ruthenium, palladium, nickel, molybdenum, tungsten, iridium, cobalt, iron and the like.

  As the conductive carrier, carbon materials such as acetylene black, furnace black and activated carbon are mainly used. The catalyst particles may be a black catalyst that does not use the conductive carrier.

  The electrode base material is known, and various electrode base materials constituting a fuel electrode and an air electrode can be used, so that fuel gas, fuel liquid and oxidant gas as fuel can be efficiently supplied to the catalyst layer. A porous conductive material is used. For example, porous carbon materials such as carbon paper, carbon cloth, and carbon fiber nonwoven fabric are used.

  Hereinafter, the present invention will be described more specifically with reference to examples.

(1) Preparation of electrolyte membrane As a filler, a flaky silica particle material (a flaky silica water slurry (■ Sun Lovely LFS (trade name): HN-050, solid content of about 14% by weight) manufactured by Asahi Glass Stech Co., Ltd.) is protonated. "Nafion" as a conductive material (DuPont, 5 wt% Nafion (trade name) solution)
Was used. The composition was prepared so that the scaly silica was 10% by weight and Nfion was 90% by weight in terms of dry weight. The flaky silica water slurry and the Nafion solution were mixed, and a uniform dispersion was prepared by repeating stirring with a magnetic stirrer and ultrasonic stirring. The resulting dispersion was stirred with a magnetic stirrer while heating at 50-80 ° C., and the viscosity was adjusted while evaporating the dispersion. The obtained high-viscosity dispersion was cast on a polytetrafluoroethylene (PTFE) substrate, and allowed to stand and dried in a drying oven at about 100 ° C. to form an electrolyte membrane. The obtained electrolyte membrane had a thickness of about 110 μm.

(2) Preparation of catalyst transfer film Catalyst (for fuel electrode: Tanaka Kikinzoku Pt-Ru / C (TEC62E58), air electrode: Tanaka Kikinzoku Pt / C (TEC10E50E)) and electrolyte binder (DuPont, 5% by weight) “Nafion” (trade name) solution) was mixed and stirred with isopropyl alcohol as a dispersion medium to prepare a catalyst ink. A polyethylene terephthalate film (E3120, manufactured by Toyobo Co., Ltd.) was used as a transfer substrate, and the catalyst ink was applied and dried to obtain a catalyst transfer film. Further, a Nafion solution whose viscosity was adjusted by heating at 50 ° C. was applied and dried on the catalyst layer of the catalyst transfer film to form a proton conductive material layer.

(3) Power generation performance evaluation (hydrogen fuel)
The electrolyte membrane produced in the above (1) and the pair of catalyst transfer films produced in the above (2) are stacked in such a direction that the proton conductive material layer is in contact with the electrolyte membrane, and hot pressing (temperature: 135 to 150 ° C., The catalyst layer was transferred and formed on the electrolyte membrane with a pressure of 4-6 MPa), and the transfer substrate was peeled and removed to obtain an electrolyte membrane-catalyst layer assembly. Further, the electrolyte membrane-catalyst layer assembly was sandwiched between a pair of gas diffusion layers (manufactured by Toray Industries, Inc., carbon paper) to form an electrolyte membrane-electrode assembly. The electrolyte membrane-electrode assembly was sandwiched between a separator having a flow path for supplying fuel and an oxidant and a current collector to constitute a single cell. The anode electrode was 1.0 mg-Pt-Ru / cm ² , and the cathode electrode was 0.5 mg-Pt / cm ² .

  Hydrogen gas (0.1 NLM, dew point 80 ° C.) as the fuel and air (0.5 NLM, dew point 70 ° C.) as the oxidant are supplied to the fuel electrode and the air electrode, respectively, and hydrogen of the above electrolyte membrane-electrode assembly at 80 ° C. The power generation performance of the fuel cell was evaluated. The obtained open electromotive force was about 1.01V. The “NLM” refers to normal liter per minute. The cell resistance measured with a digital low resistance meter was about 50 mΩ.

As a comparative example, power generation performance evaluation of a hydrogen fuel cell using an electrolyte membrane-electrode assembly produced in the same manner as described above was performed using a catalyst transfer film having no proton conductive material layer. The thickness of the electrolyte membrane was about 110 μm, the anode electrode was 1.0 mg-Pt-Ru / cm ² , and the cathode electrode was 0.5 mg-Pt / cm ² . As a result, the open electromotive force showed a value equivalent to 1.01 V, while the cell resistance was about 65 mΩ. These results indicate that the formation of a proton conduction path is improved by disposing a proton conductive material layer at the interface between the electrolyte membrane and the catalyst layer in the examples.

  The present invention is not limited to the above embodiment. The above-described embodiment is an exemplification, and the present invention has substantially the same configuration as the technical idea described in the claims of the present invention, and any device that exhibits the same function and effect is the present invention. It is included in the technical scope of the invention.

1A to 1D are schematic cross-sectional views of an electrolyte membrane containing a filler in a comparative example. 2A to 2D are schematic cross-sectional views of an electrolyte membrane on which a proton conductive material layer is formed according to an embodiment of the present invention. FIG. 3 is a schematic view showing a cross section of an electrolyte membrane-catalyst layer assembly using the electrolyte membrane of the present invention shown in FIG. FIG. 4 is a cross-sectional view of the electrolyte membrane-electrode assembly in one embodiment of the present invention. 5A to 5D are cross-sectional views of the catalyst transfer film 20 in one embodiment of the present invention. 6A-B are cross-sectional views of the gas diffusion electrode 32 in one embodiment of the present invention.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Proton conductive material 2 Polymer fibril 3 Inorganic particle material 4 Scale-like particle material 5 Filler (support)
7 Catalyst Particles 8 Electrolyte Binder 9, 13, 13 ′, 22 Catalyst Layer 10, 12, 24 Electrolyte Membrane 11, 11a, 11b, 23 Proton Conductive Material Layer 14, 16, 25, 26, 27 Electrode Base 15 Fuel Electrode 17 Air electrode 20 Catalyst transfer film 21 Transfer substrate 30 Electrolyte membrane-catalyst layer assembly 31, 33 Electrolyte membrane-electrode assembly 32 Gas diffusion electrode

Claims (8)

An electrolyte membrane-electrode assembly in which at least a catalyst layer and a porous electrode layer are laminated on both surfaces of the electrolyte membrane,
The electrolyte membrane is composed of a proton conductive material containing a filler, and at least a part of the filler is exposed from the electrolyte membrane,
A proton conductive material layer exists between at least one of the electrolyte membrane and the catalyst layer,
The electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell, wherein the filler and the proton conductive material layer are in direct contact with each other.   The electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell according to claim 1, wherein the filler is a scaly particle material.   The electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell according to claim 1, wherein the filler is a polymer fibril or an inorganic particle material.   4. The electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell according to claim 1, wherein a thickness of the proton conductive material layer is in a range of 0.01 to 10.00 μm. A catalyst transfer film for use in the electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell according to any one of claims 1 to 4,
A catalyst transfer film, wherein a catalyst layer comprising catalyst particles and an electrolyte binder is formed on a base film, and a proton conductive material layer is further formed thereon.   A polymer electrolyte fuel cell incorporating the electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell according to any one of claims 1 to 4. A catalyst layer composed of catalyst particles and an electrolyte binder is formed on the base film, and the proton conductive material layer side of the catalyst transfer film on which the proton conductive material layer is further formed is arranged facing the electrolyte membrane. And a process of
Heat-pressing the catalyst transfer film-electrolyte membrane-catalyst transfer film laminate; and
Peeling the base film from the heat-pressed catalyst transfer film-electrolyte membrane-catalyst transfer film laminate to obtain an electrolyte membrane-catalyst layer assembly;
A method for producing an electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell, comprising a step of disposing a pair of electrode substrates on both surfaces of the electrolyte membrane-catalyst layer assembly. A catalyst layer composed of catalyst particles and an electrolyte binder is formed on the electrode substrate, and the proton conductive material layer side of the gas diffusion electrode on which the proton conductive material layer is formed is arranged facing the electrolyte membrane. And a process of
A process for producing an electrolyte membrane-electrode assembly for a polymer electrolyte fuel cell, comprising a step of hot pressing the gas diffusion electrode-electrolyte membrane-gas diffusion electrode laminate.

Images