JP6515648B2 - Catalyst layer transfer substrate, method of manufacturing membrane electrode assembly, and membrane electrode assembly - Google Patents

Description

  The present invention relates to a catalyst layer transfer substrate used for producing a membrane electrode assembly provided in a polymer electrolyte fuel cell, a method for producing a membrane electrode assembly using the catalyst layer transfer substrate, and a membrane electrode assembly About.

  A polymer electrolyte fuel cell is a fuel cell using a polymer membrane having proton conductivity as an electrolyte. FIG. 11 is a cross-sectional view showing an example of the structure of a polymer electrolyte fuel cell.

  As shown in FIG. 11, the polymer electrolyte membrane 110 has a cathode contact surface 110a, which is one side, and an anode contact surface 110b, which is a side opposite to the cathode contact surface 110a. The electrode catalyst layer 120C is in contact with the cathode contact surface 110a, and the electrode catalyst layer 120C and the porous diffusion layer 130C are stacked in this order. The electrode catalyst layer 120A is in contact with the anode contact surface 110b, and the electrode catalyst layer 120A and the porous diffusion layer 130A are stacked in this order. The electrode catalyst layer 120C constitutes an air electrode which is a cathode, and the electrode catalyst layer 120A constitutes a fuel electrode which is an anode.

  A gasket layer 140C is disposed on the cathode contact surface 110a on the outer peripheral edge of the electrode catalyst layer 120C and outside the outer peripheral edge of the porous diffusion layer 130C. A gasket layer 140A is disposed on the anode contact surface 110b on the outer peripheral edge of the electrode catalyst layer 120A and on the outer side than the outer peripheral edge of the porous diffusion layer 130A. The gasket layers 140C and 140A are attached to the polymer electrolyte membrane 110. The membrane electrode assembly 100 includes a polymer electrolyte membrane 110, electrode catalyst layers 120C and 120A, porous diffusion layers 130C and 130A, and gasket layers 140C and 140A, and the pair of separators 150C and 150A are membrane electrode junctions. The body 100 is held.

  An oxidant gas containing oxygen is supplied to the electrode catalyst layer 120C on the cathode side from a gas flow passage 160C formed in the separator 150C. A fuel gas containing hydrogen is supplied to the electrode catalyst layer 120A on the anode side from a gas flow passage 160A formed in the separator 150A. Then, an electromotive force is generated between the cathode and the anode by advancing the electrode reaction between the oxidant gas and the fuel gas in the presence of the catalyst. During this time, the gasket layers 140C and 140A prevent the gas supplied to the electrode catalyst layers 120C and 120A from leaking from the polymer electrolyte fuel cell.

  As a method of forming the electrode catalyst layers 120C and 120A in the manufacturing process of the membrane electrode assembly 100, a liquid or paste mixture in which a catalyst and an electrolyte are mixed is printed on the surface of the polymer electrolyte membrane 110. And the method of forming the electrode catalyst layers 120C and 120A by the method and the spray method, and the method of forming the electrode catalyst layers 120C and 120A by applying the mixture on the surface of the porous diffusion layers 130C and 130A. Be Even when the electrode catalyst layers 120C and 120A are formed on the surface of the polymer electrolyte membrane 110, and even if the electrode catalyst layers 120C and 120A are formed on the surfaces of the porous diffusion layers 130C and 130A, the electrode catalyst layer 120C , 120A, the polymer electrolyte membrane 110 and the porous diffusion layers 130C, 130A are joined by hot pressing or the like (see, for example, Patent Documents 1 to 3).

  On the other hand, as another method of forming the electrode catalyst layers 120C and 120A, the above mixture is applied on a base different from the polymer electrolyte membrane 110 and the porous diffusion layers 130C and 130A to form the electrode catalyst layers 120C and 120A. There is a method of transferring the formed electrode catalyst layers 120C and 120A from the substrate to the polymer electrolyte membrane 110 by a hot press or a heat roll (see, for example, Patent Document 4). In such a method, the film thickness of the electrode catalyst layers 120C and 120A can be easily controlled, and the uniformity of the electrode catalyst layers 120C and 120A can be easily improved, so that the cell performance can be improved. It is excellent at high production efficiency.

Unexamined-Japanese-Patent No. 06-203849 Japanese Patent Application Laid-Open No. 08-88011 Japanese Patent Application Publication No. 08-106915 JP 10-64574 A

  In the method of disposing the electrode catalyst layers 120C and 120A on the surface of the polymer electrolyte membrane 110 by transfer from the base material, after the electrode catalyst layers 120C and 120A are disposed on the surface of the polymer electrolyte membrane 110, the polymer Gasket layers 140C and 140A are disposed around the electrode catalyst layers 120C and 120A on the surface of the electrolyte membrane 110, respectively.

  However, since it is difficult to precisely match the dimensions of the gasket layers 140C and 140A with the dimensions of the electrode catalyst layers 120C and 120A, when the gasket layers 140C and 140A and the polymer electrolyte membrane 110 are bonded, A gap may be formed between the electrode catalyst layer 120C and the gasket layer 140C, and between the electrode catalyst layer 120A and the gasket layer 140A. The portion facing the gap is a portion exposed to the separator 150C or the separator 150A, and is directly exposed to the oxidant gas or the fuel gas. Further, since the exposed portion is not held by any of the electrode catalyst layers 120C and 120A and the gasket layers 140C and 140A, stress associated with swelling or contraction of the polymer electrolyte membrane 110 during power generation concentrates on the exposed portion. Do. As described above, the exposed portion of the polymer electrolyte membrane 110 is one of the factors promoting the degradation of the polymer electrolyte membrane 110.

  The present invention provides a catalyst layer transfer substrate capable of suppressing exposure of a polymer electrolyte membrane from between an electrode catalyst layer and a gasket layer, a method of manufacturing a membrane electrode assembly, and a membrane electrode assembly. The purpose is

  A catalyst layer transfer substrate for solving the above problems comprises a substrate layer having a first surface and a second surface opposite to the first surface, and a frame shape disposed on the first surface A multilayer structure layer having a plurality of layers, the multilayer structure layer defining, on the first surface, an opening in which a material for forming an electrode catalyst layer is embedded, the multilayer structure layer being a first junction It has a structure in which the layer, the second bonding layer, the gasket layer, and the third bonding layer are arranged in this order from the side closer to the first surface, and it is necessary to peel the second bonding layer from the gasket layer The force is smaller than the force required to peel the first bonding layer from the base layer, and smaller than the force required to peel the third bonding layer from the gasket layer.

  According to the above configuration, the opening in which the electrode catalyst layer is formed is partitioned by the multilayer structure layer including the gasket layer, so that the electrode catalyst layer is formed in the opening, thereby forming the electrode catalyst layer Sometimes the dimensions of the gasket layer and the electrode catalyst layer are matched. Then, by performing transfer using this catalyst layer transfer substrate, the electrode catalyst layer and the gasket layer are simultaneously transferred to the polymer electrolyte membrane, so that a gap is formed between the electrode catalyst layer and the gasket layer. As a result, exposure of the polymer electrolyte membrane can be suppressed.

Then, peeling of the second bonding layer from the gasket layer is easier than peeling of the first bonding layer from the base material layer and peeling of the third bonding layer from the gasket layer, so that the base material after transfer is transferred. At the time of layer peeling, peeling at the interface between the second bonding layer and the gasket layer is smoothly realized. In particular, since the bonding layer disposed between the base material layer and the gasket layer is two layers, the adhesion of the bonding layer to the base material layer and the gasket as compared with the case where such a bonding layer is one layer. The degree of freedom in adjusting the adhesion of the bonding layer to the layer is increased. As a result, when adjusting the adhesive force, the restriction imposed by the material of the base layer and the material of the gasket layer is reduced, and even when various materials are used as such materials, the base layer can be easily made from the gasket layer. A peelable catalyst layer transfer substrate can be realized.
In the above configuration, a reinforcing layer that suppresses deformation of the base material layer due to temperature change is disposed on the second surface of the base material layer.

  According to the above configuration, even if the temperature of the catalyst layer transfer base material is largely changed due to the drying process or the like at the time of forming the electrode catalyst layer, the occurrence of warpage in the base material layer can be suppressed. As a result, the workability in the manufacturing process of the membrane electrode assembly using the catalyst layer transfer substrate is improved. In addition, since a layer different from the base material layer is disposed on the front and back of the base material layer, the rigidity of the catalyst layer transfer base material is enhanced, which also improves the workability.

  In the above configuration, the peel strength of the first bonding layer with respect to the base material layer is larger than the peel strength of the second bonding layer with respect to the gasket layer, and the difference in the peel strength of these is 0.01 N / 25 mm or more. And it is preferable that it is less than 10 N / 25 mm.

  According to the above configuration, when peeling the base material layer after transfer, the base material layer can be easily peeled off at the interface between the second bonding layer and the gasket layer, together with the first bonding layer and the second bonding layer. .

  In the above configuration, the peel strength of the third bonding layer with respect to the gasket layer is greater than the peel strength of the second bonding layer with respect to the gasket layer, and the difference in the peel strength is 0.01 N / 25 mm or more, and And preferably less than 10 N / 25 mm.

According to the above configuration, when peeling the base material layer after transfer, the base material layer can be easily peeled off at the interface between the second bonding layer and the gasket layer, together with the first bonding layer and the second bonding layer. .
In the said structure, it is preferable that the peeling strength of the said 1st joining layer with respect to the said base material layer is 0.02 N / 25 mm or more and less than 10 N / 25 mm.

  According to the above configuration, the adhesion between the base material layer and the first bonding layer is enhanced, so the adhesion between the base material layer and the multilayer structure layer is enhanced. As a result, it is possible to suppress the formation of a gap between the base layer and the multilayer structure layer. Therefore, when forming the electrode catalyst layer, the material for forming the electrode catalyst layer is between the base layer and the multilayer structure layer. Entry into the gap between

  In the above configuration, the device further includes an electrode catalyst layer disposed in the opening, and the thickness of the multilayer structure layer is larger than the thickness of the electrode catalyst layer, and the thickness of the multilayer structure layer and the thickness of the electrode catalyst layer Is preferably 100 μm or less.

  According to the above configuration, since the difference between the thickness of the multilayer structure layer and the thickness of the electrode catalyst layer is not too large, the difference in level between the end of the multilayer structure layer and the edge of the electrode catalyst layer has less influence on transfer. The transfer between the electrode catalyst layer and the gasket layer can be favorably performed.

In the above configuration, the thickness of the gasket layer is preferably 1 μm or more and 100 μm or less.
According to the above configuration, the function as the gasket is suitably exhibited. In addition, the depth of the opening in which the electrode catalyst layer is formed can be easily secured in a range suitable for film formation and transfer of the electrode catalyst layer.

  In a method of manufacturing a membrane electrode assembly that solves the above-mentioned problems, the first surface of the base material layer having a first surface and a second surface opposite to the first surface is provided on the first surface of the base layer. A multilayer structure layer which defines an opening on the surface, a first bonding layer of the multilayer structure layer, a second bonding layer, a gasket layer, and a third bonding layer are arranged in this order from the side closer to the first surface An electrode catalyst layer is formed into a film in the opening by the step of arranging so as to line up, and coating of ink, and a catalyst layer transfer substrate having the substrate layer, the multilayer structure layer, and the electrode catalyst layer is formed. And pressing the catalyst layer transfer substrate against the polymer electrolyte membrane having a contact surface, and pressing the electrode catalyst layer and the third bonding layer in the multilayer structure layer on the contact surface, Adhesion of the first bonding layer to the base layer, and the adhesion of the first bonding layer to the gasket layer. The adhesion of the bonding layer is greater than the adhesive strength of the second bonding layer with respect to the gasket layer.

  According to the above method, when forming the electrode catalyst layer, the dimensions of the gasket layer and the electrode catalyst layer are matched, and the electrode catalyst layer and the gasket layer are simultaneously transferred to the polymer electrolyte membrane. Therefore, a gap is formed between the electrode catalyst layer and the gasket layer, and the exposure of the polymer electrolyte membrane can be suppressed.

  In addition, since peeling of the second bonding layer from the gasket layer is easier than peeling of the first bonding layer from the base material layer and peeling of the third bonding layer from the gasket layer, the membrane / electrode assembly When it is necessary to peel off the base material layer to produce a polymer electrolyte fuel cell using it, the peeling at the interface between the second bonding layer and the gasket layer is smoothly realized. In particular, since the bonding layer disposed between the base material layer and the gasket layer is two layers, the adhesion of the bonding layer to the base material layer and the gasket as compared with the case where such a bonding layer is one layer. The degree of freedom in adjusting the adhesion of the bonding layer to the layer is increased. As a result, when adjusting the adhesive force, the restriction imposed by the material of the base layer and the material of the gasket layer is reduced, and even when various materials are used as such materials, the base layer can be easily made from the gasket layer. It can be made peelable.

  In the method, the electrode catalyst layer and the gasket layer transferred from the catalyst layer transfer substrate to the contact surface of the polymer electrolyte membrane, the base material layer, the first bonding layer, and the second It is preferable to further include the step of peeling the bonding layer.

  According to the above method, since the base material layer can be easily peeled off at the interface between the second bonding layer and the gasket layer together with the first bonding layer and the second bonding layer, it is suitable for a polymer electrolyte fuel cell The membrane electrode assembly used in

  A membrane electrode assembly that solves the above problems is a polymer electrolyte membrane having a contact surface, an electrode catalyst layer located on the contact surface, and a surface direction of the contact surface located around the electrode catalyst layer, and A gasket layer in contact with the peripheral end face of the electrode catalyst layer; a base material layer covering the electrode catalyst layer and the gasket layer; and a base material layer disposed between the gasket layer and the base material layer. And a second bonding layer disposed between the gasket layer and the base material layer and in contact with the gasket layer and the first bonding layer, the polymer electrolyte membrane, and the gasket layer. And a third bonding layer disposed between and in contact with the polymer electrolyte membrane and the gasket layer, and a force required to peel the second bonding layer from the gasket layer is the third base layer from the base layer. 1Peel the bonding layer Less than the force required to, and less than the force required to peel the third bonding layer from said gasket layer.

  The membrane electrode assembly is manufactured using the catalyst layer transfer substrate. Therefore, in the membrane electrode assembly, exposure of the polymer electrolyte membrane between the electrode catalyst layer and the gasket layer is suppressed. Furthermore, since the base material layer functions as a protective layer of the electrode catalyst layer, for example, the membrane electrode assembly is transported to a place different from the production place of the membrane electrode assembly and used for producing a polymer electrolyte fuel cell When it is possible, etc., the electrode catalyst layer can be protected without separately providing a protective sheet. Therefore, the process of applying the protective sheet is not necessary, and the members used are also reduced.

  According to the present invention, exposure of the polymer electrolyte membrane between the electrode catalyst layer and the gasket layer can be suppressed.

It is sectional drawing which shows the cross-section of the catalyst layer transfer base material in one Embodiment. It is a top view which shows the planar structure of the catalyst layer transfer base material in one Embodiment. In the manufacturing method of the membrane electrode assembly of one Embodiment, it is a figure which shows the arrangement | positioning process of a multilayer structure layer and a reinforcement layer. In the manufacturing method of the membrane electrode assembly of one Embodiment, it is a figure which shows the film-forming process of an electrode catalyst layer. In the manufacturing method of the membrane electrode assembly of one Embodiment, it is a figure which shows the transfer process of an electrode catalyst layer and a gasket layer. In the manufacturing method of the membrane electrode assembly of one Embodiment, it is a figure which shows the peeling process of a base material layer. It is sectional drawing which shows the cross-section of the membrane electrode assembly manufactured by the manufacturing method of the membrane electrode assembly of one Embodiment. It is sectional drawing which shows a part of cross-section of the membrane electrode assembly manufactured by the manufacturing method of the membrane electrode assembly of one Embodiment, Comprising: The figure which expands and shows the part A enclosed with an alternate long and short dash line in FIG. It is. FIG. 1 is a perspective view showing a perspective view of a polymer electrolyte fuel cell provided with a membrane electrode assembly manufactured by the method of manufacturing a membrane electrode assembly of one embodiment. It is sectional drawing which shows the cross-section of the membrane electrode assembly of a modification. FIG. 6 is a cross-sectional view showing a cross-sectional structure of a polymer electrolyte fuel cell in a conventional example.

  A catalyst layer transfer substrate, a method of manufacturing a membrane electrode assembly, and one embodiment of a membrane electrode assembly will be described with reference to FIGS. 1 to 9.

[Composition of catalyst layer transfer substrate]
The structure of the catalyst layer transfer substrate will be described with reference to FIGS. 1 and 2.
As shown in FIG. 1, the catalyst layer transfer base material 10C includes a base material layer 11C, a reinforcing layer 12C, and a multilayer structure layer 15C having a frame shape. The reinforcing layer 12C is composed of a support layer 14C and a reinforcing bonding layer 13C, and the multilayer structure layer 15C includes the first bonding layer 16C, the second bonding layer 17C, the gasket layer 18C, and the third bonding layer 19C. It is configured.

The base material layer 11C has a first surface 11a and a second surface 11b which is a surface opposite to the first surface 11a. The multilayer structure layer 15C is disposed on the side of the first surface 11a with respect to the base layer 11C, and the reinforcing layer 12C is disposed on the side of the second surface 11b with respect to the base layer 11C.
Specifically, the reinforcing bonding layer 13C covers the entire second surface 11b, and the supporting layer 14C is bonded to the base layer 11C by the reinforcing bonding layer 13C.

  Further, the first bonding layer 16C is in contact with the first surface 11a in a region surrounding the central portion of the first surface 11a along the outer edge of the first surface 11a, and the first bonding layer 16C and the second bonding layer 17C. The gasket layer 18C and the third bonding layer 19C are arranged in this order from the side closer to the first surface 11a. That is, the second bonding layer 17C is in contact with the first bonding layer 16C, and the gasket layer 18C is bonded to the base layer 11C by the two bonding layers 16C and 17C. The surface of the gasket layer 18C opposite to the surface in contact with the second bonding layer 17C is covered with the third bonding layer 19C. The surface of the third bonding layer 19C opposite to the surface in contact with the gasket layer 18C is covered with the covering layer 20C. The covering layer 20C covers the third bonding layer 19C at the time of formation of the electrode catalyst layer, and is peeled from the third bonding layer 19C at the time of transfer of the electrode catalyst layer.

  The force required to peel the second bonding layer 17C from the gasket layer 18C is smaller than the force required to peel the first bonding layer 16C from the base material layer 11C, and the gasket layer 18C to the third bonding layer 19C. Less than the force required to peel the

As shown in FIG. 2, the base material layer 11C has a substantially rectangular outer shape, and the multilayer structure layer 15C and the covering layer 20C have an annular shape along the outer edge of the base material layer 11C, that is, a rectangular frame shape have. On the first surface 11a of the base layer 11C, a substantially rectangular opening in which a material for forming an electrode catalyst layer is embedded by the inner peripheral edge of the multilayer structure layer 15C and the covering layer 20C in the surface direction of the base layer 11C. 21C is divided.
The reinforcing layer 12C has a substantially rectangular outer shape, and the outer dimensions of the reinforcing layer 12C substantially match the outer dimensions of the base layer 11C.

[Method of producing membrane electrode assembly]
With reference to FIGS. 3-6, the manufacturing method of the membrane electrode assembly using the above-mentioned catalyst layer transfer base material is demonstrated.
As shown in FIG. 3, the multilayer structure layer 15C to which the covering layer 20C is attached is disposed on the first surface 11a of the substrate layer 11C, and the reinforcing layer 12C is disposed on the second surface 11b of the substrate layer 11C. As a result, the catalyst layer transfer substrate 10C is formed.

  When the multilayer structure layer 15C and the covering layer 20C are disposed on the first surface 11a, first, a laminate of the multilayer structure layer 15C and the covering layer 20C is formed, and the opening 21C is formed in the laminate. . Thereafter, the first bonding layer 16C, the second bonding layer 17C, the gasket layer 18C, and the third bonding layer 19C are in contact with the base layer 11C and the first bonding layer 16C. The layered product of multilayer structure layer 15C and covering layer 20C is arranged on the 1st field 11a of base material layer 11C so that it may be arranged in this order from the near one.

  The reinforcing layer 12C is disposed on the second surface 11b after the multilayer structure layer 15C and the covering layer 20C are disposed on the first surface 11a of the base layer 11C. The reinforcing layer 12C may be disposed on the second surface 11b before the multilayer structure layer 15C and the covering layer 20C are disposed on the first surface 11a.

  The base material layer 11C can transfer a sheet formed of a material capable of transferring the electrode catalyst layer formed on the surface of the base material layer 11C, or can transfer the electrode catalyst layer formed on the surface of the base material layer 11C. It is a sheet on which surface treatment was performed.

Examples of the material of the base layer 11C include ethylene tetrafluoroethylene copolymer (ETFE), tetrafluoroethylene-hexafluoropropylene copolymer (FEP), tetrafluoroperfluoroalkyl vinyl ether copolymer (PFA), and poly Fluorine-based resins such as tetrafluoroethylene (PTFE) or polyethylene terephthalate (PET), polyethylene naphthalate (PEN), syndiotactic polystyrene (SPS), polytetrafluoroethylene (PTFE), polyimide (PI), etc. are used. Be Moreover, a silicone treatment etc. are mentioned as surface treatment.
The thickness of the base layer 11C is preferably about 1 μm to 100 μm, and is appropriately selected according to the material so that the strength and the heat resistance can be appropriately secured.

  As the first bonding layer 16C, the second bonding layer 17C, and the third bonding layer 19C, an adhesive layer which does not require solidification at the time of bonding of an object may be used, or an adhesive layer which needs solidification at the time of bonding of an object may be used. Good. As materials of the bonding layers 16C, 17C, 19C, for example, an adhesive or an adhesive such as an epoxy resin type, an acrylic resin type, a urethane resin type, a silicone resin type, and a rubber type can be used. As materials for forming the bonding layers 16C, 17C, and 19C, a material capable of exerting the adhesive force required for each bonding layer is selected for each bonding layer. In the present embodiment, the terms adhesion and adhesive force are also used in the bonding of objects with an adhesive.

  The first bonding layer 16C and the second bonding layer 17C are preferably formed of different materials, and the second bonding layer 17C and the third bonding layer 19C are preferably formed of different materials. The first bonding layer 16C and the third bonding layer 19C may be formed of the same material or may be formed of different materials.

  As a formation material of each of the first bonding layer 16C and the second bonding layer 17C, the adhesion of the first bonding layer 16C to the second bonding layer 17C, that is, between the first bonding layer 16C and the second bonding layer 17C The adhesion acting on the base layer 11C is at least greater than the adhesion of the second joint layer 17C to the gasket layer 18C, preferably, the adhesion of the first joint layer 16C to the base layer 11C, and A material is selected which is sufficiently larger than the adhesion and the adhesion of the third bonding layer 19C to the gasket layer 18C. Further, as a material for forming the third bonding layer 19C, the adhesion of the third bonding layer 19C to the polymer electrolyte membrane is at least larger than the adhesion of the second bonding layer 17C to the gasket layer 18C, and preferably, the substrate Select a material that is sufficiently larger than the adhesion of the first bonding layer 16C to the layer 11C, the adhesion of the second bonding layer 17C to the gasket layer 18C, and the adhesion of the third bonding layer 19C to the gasket layer 18C. Be done.

  The adhesion of the first bonding layer 16C to the base layer 11C is larger than the adhesion of the second bonding layer 17C to the gasket layer 18C. Furthermore, each of the adhesion of the first bonding layer 16C to the base material layer 11C and the adhesion of the second bonding layer 17C to the gasket layer 18C was measured at a peeling rate of 300 mm / min using a tensile tester at 180 °. When it expresses as peeling strength (JIS-K-6854-2: 1999), it is preferable that the difference of these peeling strength is 0.01 N / 25 mm or more and less than 10 N / 25 mm. When the base material layer 11C is peeled off after the transfer of the electrode catalyst layer, if the peel strength difference is in the above range, the second bonding layer 17C is easily peeled off at the interface with the gasket layer 18C.

  Further, the adhesion of the third bonding layer 19C to the gasket layer 18C is larger than the adhesion of the second bonding layer 17C to the gasket layer 18C. Furthermore, 180 ° peeling measured for each of the adhesion of the third bonding layer 19C to the gasket layer 18C and the adhesion of the second bonding layer 17C to the gasket layer 18C using a tensile tester at a peeling speed of 300 mm / min. When expressed as strength (JIS-K-6854-2: 1999), it is preferable that the difference in peel strength between them is 0.01 N / 25 mm or more and less than 10 N / 25 mm. When the base material layer 11C is peeled off after the transfer of the electrode catalyst layer, if the peel strength difference is in the above range, the second bonding layer 17C is easily peeled off at the interface with the gasket layer 18C.

  Moreover, when the adhesive force of the first bonding layer 16C to the base material layer 11C is expressed as 180 ° peel strength (JIS-K-6854-2: 1999) measured at a peel rate of 300 mm / min using a tensile tester. It is preferable that it is 0.02 N / 25 mm or more and less than 10 N / 25 mm. When the peel strength is in the above range, the adhesion between the base material layer 11C and the first bonding layer 16C is high, so the adhesion between the base material layer 11C and the multilayer structure layer 15C is enhanced. As a result, since the formation of a gap between the base material layer 11C and the multilayer structure layer 15C is suppressed, the catalyst ink is formed in the gap between the base material layer 11C and the multilayer structure layer 15C when the electrode catalyst layer is formed. Entry is suppressed, and the linearity of the outer peripheral edge of the electrode catalyst layer is improved.

The thickness of each of the bonding layers 16C, 17C, and 19C is not particularly limited, but is preferably 0.1 μm to 40 μm. When the thickness of each of the bonding layers 16C, 17C, and 19C is 0.1 μm or more, it is possible to suppress the occurrence of coating unevenness of the material when forming the bonding layer.
The peel strength between the bonding layers can be set by appropriately selecting a pressure-sensitive adhesive and an adhesive having different adhesion (adhesive force) so that a difference in peel strength occurs between the bonding layers.

The gasket layer 18C is formed of a resin that is generally used for polymer electrolyte fuel cells among thermoplastic resins. For example, as a material of the gasket layer 18C, polyethylene terephthalate (PET), polyethylene naphthalate (PEN), syndiotactic polystyrene (SPS), polytetrafluoroethylene (PTFE), polyimide (PI) or the like is used.
The thickness of the gasket layer 18C is preferably 1 μm or more and 100 μm or less, and is appropriately selected according to the material so that the strength and the heat resistance can be appropriately secured.

  The material of the support layer 14C and the reinforcing bonding layer 13C in the reinforcing layer 12C is not particularly limited, and a material which generally flows may be used. For example, as a material of the support layer 14C, polyethylene terephthalate (PET), polyethylene naphthalate (PEN), syndiotactic polystyrene (SPS), polytetrafluoroethylene (PTFE), polyimide (PI) or the like is used, and reinforcement bonding is performed. As a material of the layer 13C, epoxy resin, acrylic resin, urethane resin, silicone resin, rubber or the like is used.

  The thickness of the reinforcing layer 12C is not particularly limited, but the thickness of the support layer 14C is preferably about 1 μm to 100 μm, and particularly preferably the same thickness as the gasket layer 18C. When the thickness of the support layer 14C and the thickness of the gasket layer 18C are equal to each other, warpage of the base material layer 11C due to a temperature change at the time of forming the electrode catalyst layer is suitably suppressed.

The material of the coating layer 20C is not particularly limited, and generally used resins may be used. For example, as a material of the covering layer 20C, polyethylene (PE), polypropylene (PP), polyethylene terephthalate (PET), polyvinyl chloride (PVC), polycarbonate (PC), polyethylene naphthalate (PEN), syndiotactic polystyrene ( SPS), polytetrafluoroethylene (PTFE), polyimide (PI) and the like are used. For example, a separate film attached to the third bonding layer 19C may be used as the covering layer 20C.
The thickness of the covering layer 20C is not particularly limited, but is preferably about 1 μm to 40 μm.

  As shown in FIG. 4, the catalyst ink is applied to the inside of the opening 21C and dried to expose the multilayer structure layer 15C and the covering layer 20C in the first surface 11a of the substrate layer 11C. The electrode catalyst layer 22C is formed on the portion. The covering layer 20C may be peeled off before the transfer of the electrode catalyst layer 22C after the formation of the electrode catalyst layer 22C, and after the formation of the electrode catalyst layer 22C, the covering layer 20C is applied to the catalyst layer transfer substrate 10C. The cover layer 20C may be handled in a peeled state.

When the base material layer 11C and the gasket layer 18C are made of materials different from each other, the base material layer after cooling is caused by the temperature change that occurs when the catalyst ink coated in the opening 21C passes through the drying process. Warpage due to stress may occur in 11C. On the other hand, in the present embodiment, since the reinforcing layer 12C for suppressing the deformation of the base material layer 11C due to the temperature change is disposed on the second surface 11b of the base material layer 11C, the warpage of the base material layer 11C is reduced. Thus, the workability in the production of the membrane electrode assembly is improved.
The catalyst ink contains a polymer electrolyte, a catalyst substance, and an ink solvent.

  As the polymer electrolyte contained in the catalyst ink, for example, a polymer material having proton conductivity such as a fluorine-based polymer electrolyte or a hydrocarbon-based polymer electrolyte is used. As the fluorine-based polymer electrolyte, for example, NAFION (registered trademark) manufactured by DuPont, FLEMION (registered trademark) manufactured by Asahi Glass Co., Ltd., ACIPLEX (registered trademark) manufactured by Asahi Kasei Corporation, GORE-SELECT (registered trademark) manufactured by Gore And the like. Among these materials, in order to increase the output voltage of the polymer electrolyte fuel cell, it is preferable to use NAFION (registered trademark) manufactured by DuPont. Examples of hydrocarbon-based polymer electrolytes include electrolytes such as sulfonated polyether ketone, sulfonated polyether sulfone, sulfonated polyether ether sulfone, sulfonated polysulfide, sulfonated polyphenylene, and the like.

  As a catalyst substance, for example, platinum (Pt), ruthenium (Ru), rhodium (Rh), molybdenum (Mo), chromium (Cr), cobalt (Co), iron (Fe) and the like are used. In particular, platinum is preferably used as the catalyst substance. The catalyst substance is preferably supported on carbon particles as a conductive carrier, but a single catalyst substance may be used. As a carbon particle, carbon black etc. are used, for example.

  The ink solvent is a solvent that does not erode the catalyst substance-supporting carbon body, which is a carbon particle carrying a catalyst substance, and the polymer electrolyte, and the polymer electrolyte is dissolved in a fluid state, or It is preferable to use a solvent that disperses a polymer electrolyte as a gel. Such an ink solvent preferably contains a volatile organic solvent, and examples of the organic solvent contained in the ink solvent include methanol, ethanol, 1-propanol, 2-propanol, 1-butanol, 2-butanol, and the like. Alcohols such as isobutyl alcohol, tert-butyl alcohol, pentanol, acetone, methyl ethyl ketone, pentanone, methyl isobutyl ketone, heptanone, cyclohexanone, cyclohexanone, methyl cyclohexanone, acetonyl acetone, ketone solvents such as diisobutyl ketone, tetrahydrofuran, dioxane, diethylene glycol Ether solvents such as dimethyl ether, anisole, methoxytoluene, dibutyl ether, and dimethylformamide, dimethylacetamide, N-methyl pylori Emissions, ethylene glycol, diethylene glycol, diacetone alcohol, polar solvents such as 1-methoxy-2-propanol. In addition, two or more of the organic solvents may be mixed and used as an ink solvent.

  When a lower alcohol is used as the organic solvent, it is preferable that the ink solvent be a mixed solvent of an organic solvent and water in order to increase the ignition temperature of the ink solvent. Also, in order to increase the affinity between the polymer electrolyte and the ink solvent, the ink solvent contains water to such an extent that the polymer electrolyte is separated from the ink solvent to cause white turbidity or the polymer electrolyte does not gel. Is preferred.

  The solid content of the polymer electrolyte and the catalyst substance-supporting carbon body in the catalyst ink is preferably 1% by mass or more and 50% by mass or less. When the solid content in the catalyst ink is 50% by mass or less, the viscosity of the catalyst ink does not become too high, so that the surface of the electrode catalyst layer 22C to be formed is unlikely to be cracked. On the other hand, if the solid content is 1% by mass or more, the viscosity of the catalyst ink does not become too low, so the film forming speed of the electrode catalyst layer 22C is appropriately secured, and the productivity of the electrode catalyst layer 22C is reduced. Can be suppressed.

  Even in the case of a catalyst ink in which the content of the polymer electrolyte and the catalyst substance-supporting carbon body are equal to each other, the viscosity of the catalyst ink becomes higher as the proportion of carbon particles in the solid content becomes larger. The lower the viscosity, the lower the viscosity of the catalyst ink. Therefore, the concentration of the carbon particles in the solid content contained in the catalyst ink is preferably 10% by mass or more and 80% by mass or less.

  In addition, adjustment of the solid content in the catalyst ink, adjustment of the concentration of carbon particles in the solid content, and the addition of a dispersant to the catalyst ink during dispersion processing of the solid content in the ink solvent besides these It is also possible to adjust the viscosity of the catalyst ink to a predetermined value. The mass ratio of the polymer electrolyte to the catalyst substance-supporting carbon body is preferably 0.04% by mass or more and 3.00% by mass or less.

  As a method of applying the catalyst ink to the base layer 11C, a coating method such as a doctor blade method, a dipping method, a screen printing method, a roll coating method, or a spray method is used. Among these coating methods, it is preferable to use a spray method such as a pressure spray method, an ultrasonic spray method or an electrostatic spray method. According to these methods, since aggregation of the catalyst ink hardly occurs when the coated catalyst ink is dried, it is possible to obtain a homogeneous electrode catalyst layer 22C having a high porosity.

  In the catalyst ink coating process, when the ink temperature of the catalyst ink is 10 ° C. or more, the viscosity of the catalyst ink does not become too high, so the uniformity of the electrode catalyst layer 22C to be formed into a film is enhanced. In addition, when the ink temperature is 50 ° C. or less, volatilization of the ink solvent during coating of the catalyst ink can be suppressed. The thickness of the electrode catalyst layer 22C is not particularly limited, but is preferably about 1 μm to 30 μm.

  The thickness of the electrode catalyst layer 22C is smaller than the thickness of the multilayer structure layer 15C, and the difference between the thickness of the multilayer structure layer 15C and the thickness of the electrode catalyst layer 22C is preferably 100 μm or less.

  As shown in FIG. 5, in the production of the membrane electrode assembly, a catalyst layer transfer substrate 10A having the same configuration as the catalyst layer transfer substrate 10C is further formed. That is, the catalyst layer transfer base material 10A includes the base material layer 11A, the reinforcing layer 12A including the support layer 14A and the reinforcing bonding layer 13A, the first bonding layer 16A, the second bonding layer 17A, the gasket layer 18A, and , And a multilayer structure layer 15C composed of the third bonding layer 19A. The base layer 11A has the same configuration as the base layer 11C, the support layer 14A has the same configuration as the support layer 14C, and the reinforcing bonding layer 13A has the same configuration as the reinforcing bonding layer 13C. The first bonding layer 16A has the same configuration as the first bonding layer 16C, the second bonding layer 17A has the same configuration as the second bonding layer 17C, and the gasket layer 18A has the same configuration as the gasket layer 18C. The third bonding layer 19A has the same configuration as the third bonding layer 19C.

Then, as in the electrode catalyst layer 22C, the catalyst ink described above is applied and dried inside the openings 21A of the catalyst layer transfer substrate 10A, whereby the electrode catalyst layer 22A is formed.
The catalyst layer transfer substrate 10C in which the electrode catalyst layer 22C is formed and the catalyst layer transfer substrate 10A in which the electrode catalyst layer 22A is formed are disposed with the polymer electrolyte membrane 30 interposed therebetween.

  The polymer electrolyte membrane 30 is a polymer membrane having proton conductivity. As a material of the polymer electrolyte membrane 30, for example, a fluorine-based polymer electrolyte or a hydrocarbon-based polymer electrolyte is used. As the fluorine-based polymer electrolyte, for example, NAFION (registered trademark) manufactured by DuPont, FLEMION (registered trademark) manufactured by Asahi Glass Co., Ltd., ACIPLEX (registered trademark) manufactured by Asahi Kasei Corporation, GORE-SELECT (registered trademark) manufactured by Gore Is used. In particular, in order to increase the output voltage of the polymer electrolyte fuel cell, NAFION (registered trademark) manufactured by DuPont is preferably used.

  As the hydrocarbon-based polymer electrolyte membrane, an electrolyte membrane of sulfonated polyether ketone, sulfonated polyether sulfone, sulfonated polyether ether sulfone, sulfonated polysulfide, sulfonated polyphenylene or the like is used. In order to enhance the adhesion between the electrode catalyst layers 22C and 22A and the polymer electrolyte membrane 30, the polymer electrolyte contained in the electrode catalyst layers 22C and 22A and the polymer electrolyte constituting the polymer electrolyte membrane 30 are the same. It is preferable that they are the same material.

  The polymer electrolyte membrane 30 has a cathode contact surface 30a and an anode contact surface 30b opposite to the cathode contact surface 30a. The electrode catalyst layer 22C and the third bonding layer 19C have a cathode contact surface 30a. The electrode catalyst layer 22A and the third bonding layer 19A face the anode contact surface 30b.

  Then, in a state where the polymer electrolyte membrane 30 is sandwiched between the two catalyst layer transfer substrates 10C and 10A, these members are heated and pressurized. Thus, the electrode catalyst layer 22C and the third bonding layer 19C are pressure-bonded to the cathode contact surface 30a of the polymer electrolyte membrane 30. Further, the electrode catalyst layer 22A and the third bonding layer 19A are crimped to the anode contact surface 30b of the polymer electrolyte membrane 30.

  As shown in FIG. 6, after the electrode catalyst layers 22C and 22A and the third bonding layers 19C and 19A are pressure-bonded to the polymer electrolyte membrane 30, the base layers 11C and 11A and the reinforcing layers 12C and 12A are peeled off. Ru. At this time, the first bonding layer 16C and the second bonding layer 17C are peeled off together with the base material layer 11C in a state where the second bonding layer 17C is bonded to the first bonding layer 16C bonded to the base material layer 11C. . That is, the second bonding layer 17C is peeled off at the interface with the gasket layer 18C. Similarly, the first bonding layer 16A and the second bonding layer 17A are peeled off together with the base material layer 11A in a state where the second bonding layer 17A is bonded to the first bonding layer 16A bonded to the base material layer 11A. . That is, the second bonding layer 17A is peeled off at the interface with the gasket layer 18A.

  The adhesion of the first bonding layer 16C, 16A to the base layer 11C, 11A and the adhesion of the third bonding layer 19C, 19A to the gasket layer 18C, 18A are the second bonding layer 17C, to the gasket layer 18C, 18A. By being larger than the adhesive force of 17A, peeling at the interface between the second bonding layer 17C, 17A and the gasket layer 18C, 18A is smoothly realized.

  Thereby, the electrode catalyst layers 22C and 22A, the third bonding layers 19C and 19A, and the gasket layers 18C and 18A are transferred to the polymer electrolyte membrane 30, and a membrane electrode assembly is formed. In a state where the electrode catalyst layers 22C and 22A, the third bonding layers 19C and 19A, and the gasket layers 18C and 18A are transferred to the polymer electrolyte membrane 30, the thickness of the electrode catalyst layers 22C and 22A is the same as that of the third bonding layers 19C and 19C. The thickness may be substantially the same as the total thickness of 19A and the gasket layers 18C and 18A, or may be smaller than the total thickness of the third bonding layers 19C and 19A and the gasket layers 18C and 18A. When the thickness of the electrode catalyst layers 22C and 22A is smaller than the total thickness of the third bonding layers 19C and 19A and the gasket layers 18C and 18A, the base material layer 11C laminated on the electrode catalyst layers 22C and 22A. , 11A, the electrode catalyst layers 22C, 22A are transferred to the polymer electrolyte membrane 30.

  The transfer of each member to the cathode contact surface 30a of the polymer electrolyte membrane 30 and the transfer of each member to the anode contact surface 30b of the polymer electrolyte membrane 30 may be performed simultaneously, or one row at a time. It may be

[Configuration of membrane electrode assembly]
The detailed configuration of the membrane electrode assembly manufactured by the above-described manufacturing method will be described.
As shown in FIG. 7, the membrane electrode assembly 35 includes the polymer electrolyte membrane 30, the pair of electrode catalyst layers 22 C and 22 A, the pair of gasket layers 18 C and 18 A, the gasket layer 18 C and the polymer electrolyte membrane 30. And a third bonding layer 19A for bonding the gasket layer 18A and the polymer electrolyte membrane 30 to each other.
The cathode contact surface 30a is located opposite to the anode contact surface 30b, and the cathode contact surface 30a and the anode contact surface 30b are located substantially in parallel.

  An electrode catalyst layer 22C, a third bonding layer 19C, and a gasket layer 18C are disposed at a position facing the cathode contact surface 30a. The electrode catalyst layer 22C constitutes a cathode of a polymer electrolyte fuel cell. An electrode catalyst layer 22A, a third bonding layer 19A, and a gasket layer 18A are disposed at a position facing the anode contact surface 30b. The electrode catalyst layer 22A constitutes an anode of a polymer electrolyte fuel cell.

  The electrode catalyst layer 22C and the third bonding layer 19C are in surface contact with the cathode contact surface 30a, and the third bonding layer 19C and the gasket layer 18C are on the outer periphery of the electrode catalyst layer 22C on the surface of the cathode contact surface 30a. And is in contact with the electrode catalyst layer 22C. The electrode catalyst layer 22A and the third bonding layer 19A are in surface contact with the anode contact surface 30b, and the third bonding layer 19A and the gasket layer 18A are on the outer periphery of the electrode catalyst layer 22A on the surface of the anode contact surface 30b. And is in contact with the electrode catalyst layer 22A. That is, in the surface direction of the contact surfaces 30a and 30b, the gasket layers 18C and 18A are located around the electrode catalyst layers 22C and 22A and are in contact with the peripheral end surfaces of the electrode catalyst layers 22C and 22A.

  In such a configuration, the third bonding layers 19C and 19A are sandwiched between the gasket layers 18C and 18A and the polymer electrolyte membrane 30 to be in contact with these members, and the gasket layers 18C and 18A and the polymer electrolyte membrane 30 are third Bonding by the bonding layers 19C and 19A enhances the adhesion between the gasket layers 18C and 18A and the polymer electrolyte membrane 30.

  The positions of the two members of each set of the electrode catalyst layer 22C and the electrode catalyst layer 22A, the third bonding layer 19C and the third bonding layer 19A, and the gasket layer 18C and the gasket layer 18A are as follows: It is preferable that the polymer electrolyte membrane 30 be sandwiched between them in plane symmetry.

  As shown in FIG. 8, in the portion where the electrode catalyst layer 22C and the third bonding layer 19C are in contact with each other, the third bonding layer 19C is embedded in the electrode catalyst layer 22C. That is, the third bonding layer 19C protrudes to the electrode catalyst layer 22C side which is the inner side than the inner peripheral edge of the gasket layer 18C when viewed from the opposite direction which is the direction facing the cathode contact surface 30a.

  In general, the electrode catalyst layer 22C and the third bonding layer 19C have lower rigidity than the gasket layer 18C. In addition, the electrode catalyst layer 22C has lower rigidity than the third bonding layer 19C. Therefore, due to the pressure applied during pressure bonding, the inner peripheral edge of the third bonding layer 19C is crushed by the gasket layer 18C and sinks into the outer peripheral edge of the electrode catalyst layer 22C in contact with the inner peripheral edge of the third bonding layer 19C. That is, when transferring the electrode catalyst layer 22C, the third bonding layer 19C, and the gasket layer 18C, these members are both pressed against the polymer electrolyte membrane 30, and as a result, the third bonding layer 19C is embedded in the electrode catalyst layer 22C. It is formed.

Since the third bonding layer 19C is pressed from both the gasket layer 18C and the polymer electrolyte membrane 30, an intermediate position in the thickness direction of the third bonding layer 19C in the inner peripheral edge of the third bonding layer 19C is in the thickness direction. It is easier for the electrode catalyst layer 22C to sink in than the both ends.
Similarly, in a portion where the electrode catalyst layer 22A and the third bonding layer 19A are in contact with each other, a structure in which the third bonding layer 19A is embedded in the electrode catalyst layer 22A is formed.

  The membrane electrode assembly 35 may include a porous diffusion layer superimposed on each of the electrode catalyst layers 22C and 22A. The porous diffusion layer includes a base formed of a material having gas diffusivity and conductivity, and as a material of the base, for example, a porous carbon material such as carbon cloth, carbon paper, or non-woven fabric is used. The porous diffusion layer is pressure-bonded to the electrode catalyst layers 22C and 22A by being superposed on the electrode catalyst layers 22C and 22A and being heated and pressurized after the transfer of the electrode catalyst layers 22C and 22A.

[Composition of a polymer electrolyte fuel cell]
The configuration of a polymer electrolyte fuel cell provided with the above-described membrane electrode assembly will be described with reference to FIG.
As shown in FIG. 9, the polymer electrolyte fuel cell 40 includes a membrane electrode assembly 35 including a pair of porous diffusion layers 23C and 23A, and a pair of separators 41C and 41A. The membrane electrode assembly 35 is sandwiched between the separator 41C and the separator 41A. In the separator 41C, a gas flow channel 42C is recessed on the surface facing the membrane electrode assembly 35, and a cooling water flow channel 43C is recessed on the surface on the opposite side of the membrane electrode assembly 35. ing. In the separator 41A, the gas flow channel 42A is recessed on the surface facing the membrane electrode assembly 35, and the cooling water flow channel 43A is recessed on the surface on the opposite side of the membrane electrode assembly 35. ing.

  The separators 41C and 41A are assembled to the membrane electrode assembly 35, and further, a mechanism for supplying an oxidant gas and a fuel gas, and the like are provided, whereby a solid polymer fuel cell 40 of a single cell is manufactured. The polymer electrolyte fuel cell 40 is used in a single cell state or in a state where a plurality of polymer electrolyte fuel cells 40 are combined.

  When the polymer electrolyte fuel cell 40 is used, an oxidant gas is caused to flow through the gas flow path 42C of the separator 41C on the cathode side, and a fuel gas is caused to flow through the gas flow path 42A of the separator 41A on the anode side. Further, the cooling water flows in 43C and 43A of the cooling water flow path of each of the separators 41C and 41A. Then, a gas is supplied from the gas flow channel 42C to the cathode, and a gas is supplied from the gas flow channel 42A to the anode, whereby an electrode reaction involving proton conduction in the polymer electrolyte membrane 30 progresses. , And an electromotive force is generated between the cathode and the anode.

[Effect]
The effect | action of the manufacturing method of the membrane electrode assembly using the catalyst layer transfer base material of this embodiment is demonstrated.
In the above-described manufacturing method, the electrode catalyst layers 22C and 22A are formed on the catalyst layer transfer substrates 10C and 10A in a state where the gasket layers 18C and 18A are disposed on the substrate layers 11C and 11A. Then, the catalyst layer transfer substrate 10C in which the electrode catalyst layer 22C is formed and the catalyst layer transfer substrate 10A in which the electrode catalyst layer 22A is formed are pressed against the polymer electrolyte membrane 30, thereby the electrode catalyst layer 22C, 22A and the gasket layers 18C and 18A are transferred to the polymer electrolyte membrane 30.

  According to such a manufacturing method, the electrode catalyst layers 22C and 22A are formed on the surfaces of the base material layers 11C and 11A on which the gasket layers 18C and 18A are disposed. Therefore, when the electrode catalyst layers 22C and 22A are formed, The dimensions of the inner peripheral edge of the gasket layer 18C, 18A and the outer peripheral edge of the electrode catalyst layer 22C, 22A are matched. The electrode catalyst layer 22C and the gasket layer 18C are simultaneously transferred to the cathode contact surface 30a of the polymer electrolyte membrane 30, and the electrode catalyst layer 22A and the gasket layer 18A are on the anode contact surface 30b of the polymer electrolyte membrane 30. It is simultaneously transcribed. Therefore, the formation of a gap between the electrode catalyst layer 22C and the gasket layer 18C or between the electrode catalyst layer 22A and the gasket layer 18A can be suppressed. As a result, exposure of the polymer electrolyte membrane 30 between the electrode catalyst layers 22C and 22A and the gasket layers 18C and 18A can be suppressed.

  Further, since the first bonding layers 16C and 16A and the second bonding layers 17C and 17A are peeled off together with the base layers 11C and 11A, the membrane electrodes are transferred when the electrode catalyst layers 22C and 22A and the gasket layers 18C and 18A are transferred. Unnecessary members are not disposed on the polymer electrolyte membrane 30 in the joined body 35.

  Here, in the present embodiment, the relative relationship of the adhesive force in each bonding layer is determined as follows. That is, the force required to peel the second bonding layers 17C and 17A from the gasket layers 18C and 18A is smaller than the force required to peel the first bonding layers 16C and 16A from the base material layers 11C and 11A, and The force required to peel the third bonding layers 19C and 19A from the gasket layers 18C and 18A is smaller than the force required to peel the third bonding layers 19C and 19A. Thereby, peeling at the interface between the second bonding layers 17C and 17A and the gasket layers 18C and 18A is smoothly realized.

  In particular, by forming two bonding layers disposed between the base material layers 11C and 11A and the gasket layers 18C and 18A, the base material layer 11C, in comparison with the case where the number of such bonding layers is one, The range of adjustment of the adhesion of the bonding layer to 11A and the adhesion of the bonding layer to the gasket layers 18C and 18A is broadened. As a result, when adjusting the adhesive force, the restriction imposed by the material of the base material layers 11C and 11A and the material of the gasket layers 18C and 18A is reduced, and even when various materials are used as such materials, the base material layer Catalyst layer transfer substrates 10C and 10A can be realized that can easily separate 11C and 11A from the gasket layers 18C and 18A.

  Moreover, it is possible to utilize the separate film stuck on the 3rd joining layer 19C as covering layer 20C, and it is possible to utilize a separate film similarly as a covering layer also about the 3rd joining layer 19A. The covering layer 20C functions as a mask for forming the electrode catalyst layer 22C and as a cover for suppressing the exposure of the adhesive, so that members necessary for forming the electrode catalyst layers 22C and 22A can be reduced.

  Also, conventionally, a structure has been proposed in which the gasket layer is disposed on the surface of the electrode catalyst layer to suppress the exposure of the polymer electrolyte membrane from between the electrode catalyst layer and the gasket layer. Compared with such a structure, in the membrane electrode assembly 35 of the present embodiment, the electrode catalyst layers 22C and 22A and the gasket layers 18C and 18A do not overlap when viewed from the opposite direction, so that the diffusion of gas is hindered and the electrodes It can be suppressed that the catalyst layers 22C and 22A do not contribute to power generation. As a result, even when expensive platinum group noble metals are used for the electrode catalyst layers 22C and 22A, the increase in cost required for manufacturing the membrane electrode assembly 35 can be suppressed. In addition, the thickness of the membrane electrode assembly does not vary due to the presence of the overlapping portion and the non-overlapping portion of the electrode catalyst layer and the gasket layer in the opposite direction.

As described above, according to the catalyst layer transfer base material of the present embodiment, the method of manufacturing a membrane electrode assembly, and the membrane electrode assembly, the following effects can be obtained.
(1) In the catalyst layer transfer substrate 10C, 10A, the openings 21C, 21A in which the electrode catalyst layers 22C, 22A are formed are divided by the multilayer structure layers 15C, 15A including the gasket layers 18C, 18A. By forming the electrode catalyst layers 22C and 22A in the openings 21C and 21A, the dimensions of the gasket layers 18C and 18A and the electrode catalyst layers 22C and 22A can be matched when forming the electrode catalyst layers 22C and 22A. Then, by performing transfer using the catalyst layer transfer base materials 10C and 10A, the electrode catalyst layers 22C and 22A and the gasket layers 18C and 18A are simultaneously transferred to the polymer electrolyte membrane 30, so that the electrode catalyst layer 22C is obtained. 22A and the gasket layers 18C and 18A, the exposure of the polymer electrolyte membrane 30 is suppressed.

  The peeling of the second bonding layers 17C and 17A from the gasket layers 18C and 18A is the peeling of the first bonding layers 16C and 16A from the base material layers 11C and 11A, and the third bonding from the gasket layers 18C and 18A. Since it is easier than the peeling of the layers 19C and 19A, the peeling at the interface between the second bonding layers 17C and 17A and the gasket layers 18C and 18A is smoothly realized when peeling the base material layers 11C and 11A after transfer. Ru. In particular, since the bonding layer disposed between the base material layers 11C and 11A and the gasket layers 18C and 18A is two layers, the base material layers 11C and 11A are compared with the case where the bonding layer is one layer. And the degree of freedom in adjusting the adhesion of the bonding layer to the gasket layers 18C and 18A. As a result, even when various materials are used as the base material layers 11C and 11A and the gasket layers 18C and 18A, a catalyst layer transfer base material capable of easily peeling the base material layers 11C and 11A from the gasket layers 18C and 18A. 10C, 10A can be realized.

  (2) Since the reinforcing layers 12C and 12A are disposed on the second surface of the substrate layers 11C and 11A, the catalyst layer transfer substrate 10C and 10C can be formed by a drying process or the like at the time of forming the electrode catalyst layers 22C and 22A. Even when the temperature of 10A changes significantly, the occurrence of warpage in the base material layers 11C and 11A can be suppressed. As a result, the workability in the manufacturing process of the membrane electrode assembly 35 using the catalyst layer transfer substrates 10C and 10A is improved. In addition, since another layer different from the base material layers 11C and 11A is disposed on the front and back of the base material layers 11C and 11A, the rigidity of the catalyst layer transfer base materials 10C and 10A is enhanced, which also improves the workability. .

  (3) The difference between the peel strength of the first bonding layers 16C and 16A with respect to the base material layers 11C and 11A and the peel strength of the second bonding layers 17C and 17A with respect to the gasket layers 18C and 18A is 0.01 N / 25 mm or more. And since it is less than 10 N / 25 mm, when peeling off the base material layers 11C and 11A after transfer, the base material layers 11C and 11A together with the first bonding layers 16C and 16A and the second bonding layers 17C and 17A It can be easily peeled off at the interface between the bonding layers 17C and 17A and the gasket layers 18C and 18A.

  (4) The difference between the peel strength of the third bonding layers 19C and 19A with respect to the gasket layers 18C and 18A and the peel strength of the second bonding layers 17C and 17A with respect to the gasket layers 18C and 18A is 0.01 N / 25 mm or more, , Less than 10 N / 25 mm, so when peeling off the base material layers 11C and 11A after transfer, the second bonding is performed together with the first bonding layers 16C and 16A and the second bonding layers 17C and 17A. It can be easily peeled off at the interface between the layers 17C, 17A and the gasket layers 18C, 18A.

  (5) The peel strength of the first bonding layers 16C and 16A with respect to the substrate layers 11C and 11A is 0.02 N / 25 mm or more and less than 10 N / 25 mm, so the substrate layers 11C and 11A and the multilayer structure layer 15C , Adhesion with 15A is enhanced. As a result, since the formation of a gap between the base layers 11C and 11A and the multilayer structure layers 15C and 15A is suppressed, the catalyst ink is multilayered with the base layers 11C and 11A when the electrode catalyst layers 22C and 22A are formed. It can be suppressed from entering the gap between the structural layers 15C and 15A.

  (6) The thickness of the multilayer structure layers 15C and 15A is larger than the thickness of the electrode catalyst layers 22C and 22A, and the difference between these thicknesses is 100 μm or less. Therefore, since the difference between the thickness of the multilayer structure layers 15C and 15A and the thickness of the electrode catalyst layers 22C and 22A is not too large, the difference between the end of the multilayer structure layers 15C and 15A and the edge of the electrode catalyst layers 22C and 22A Thus, the influence exerted on the transfer is reduced, and the transfer between the electrode catalyst layers 22C and 22A and the gasket layers 18C and 18A can be performed well.

  (7) Since the thickness of the gasket layers 18C and 18A is 1 μm or more and 100 μm or less, the function as a gasket in the polymer electrolyte fuel cell is suitably exhibited. Further, the depths of the openings 21C and 21A in which the electrode catalyst layers 22C and 22A are formed can be easily secured in a range suitable for film formation and transfer of the electrode catalyst layers 22C and 22A.

  (8) The inner peripheral edge of the third bonding layer 19C, 19A sinks into the outer peripheral edge of the electrode catalyst layers 22C, 22A due to the pressure applied during transfer of the electrode catalyst layers 22C, 22A and the gasket layers 18C, 18A. It is appropriately suppressed that a gap is formed between the electrode catalyst layers 22C and 22A and the gasket layers 18C and 18A.

(Modification)
The above embodiment can be modified as follows.
-As shown in FIG. 10, the base layers 11C and 11A, the first bonding layers 16C and 16A, the second bonding layers 17C and 17A, and the reinforcing layers 12C and 12A are not peeled off, and these layers are You may use as a protective layer for protecting each layer which comprises an electrode assembly from the exterior. For example, when the membrane electrode assembly is transported to a place different from the production site of the membrane electrode assembly and used for the production of a polymer electrolyte fuel cell, the electrode catalyst layers 22C and 22A are transported during transport of the membrane electrode assembly. It is necessary to apply a protective sheet for protecting the electrode catalyst layers 22C and 22A. Here, if the base layers 11C and 11A, the first bonding layers 16C and 16A, the second bonding layers 17C and 17A, and the reinforcing layers 12C and 12A are used as a protective layer without peeling off, a process of applying a protective sheet Is unnecessary, and the parts used are also reduced. In addition, when the protective sheet is peeled off, it is also suppressed that a part of the adhesive layer of the protective sheet remains on the electrode catalyst layers 22C and 22A.

  In this case, the membrane electrode assembly 36 is added to the polymer electrolyte membrane 30, the electrode catalyst layers 22C and 22A, the third bonding layers 19C and 19A, and the gasket layers 18C and 18A which function as constituent members of a polymer electrolyte fuel cell. The base material layers 11C and 11A, the first bonding layers 16C and 16A, the second bonding layers 17C and 17A, and the reinforcing layers 12C and 12A. The base layers 11C and 11A cover the electrode catalyst layers 22C and 22A and the gasket layers 18C and 18A, and the first bonding layers 16C and 16A are disposed between the gasket layers 18C and 18A and the base layers 11C and 11A. And the second bonding layer 17C, 17A is disposed between the gasket layer 18C, 18A and the base material layer 11C, 11A to form the gasket layer 18C, 18A and the first bonding layer 16C. , 16A. The base layers 11C and 11A, the first bonding layers 16C and 16A, the second bonding layers 17C and 17A, and the reinforcing layers 12C and 12A are peeled off during the production of the polymer electrolyte fuel cell.

-The member which comprises catalyst layer transfer base material 10C, 10A may contain electrode catalyst layer 22C, 22A, and does not need to be contained. That is, the layered body before the formation of the electrode catalyst layer 22C, 22A may be used as the catalyst layer transfer base 10C, 10A, or the layered body after the formation of the electrode catalyst layer 22C, 22A may be the electrode catalyst layer 22C, 22A may be included as the catalyst layer transfer substrate 10C or 10A. The point is that the members constituting the catalyst layer transfer substrates 10C and 10A may include only a part or all of the members to be transferred to the polymer electrolyte membrane 30.
The reinforcing layers 12C and 12A may be omitted from the catalyst layer transfer substrates 10C and 10A. Also by such a configuration, the effect of the above (1) can be obtained.

  -In the membrane electrode assembly 35, 36, the shape of the electrode catalyst layer 22C, 22A and the shape of the gasket layer 18C, 18A viewed from the opposite direction, ie, the catalyst layer transfer substrate 10C, 10A, the substrate layer 11C, The shape of the openings 21C and 21A and the shape of the multilayer structure layers 15C and 15A viewed from the direction opposite to the first surface of 11A may be a triangular shape or a polygonal shape having five or more sides. The shape may be circular or elliptical. Further, the inner peripheral edge of the gasket layers 18C, 18A may be inclined with respect to the opposing direction. For example, the inner peripheral edge of the gasket layer 18C may have a reverse tapered shape as viewed from the base layer 11C side such that the cross-sectional area of the opening 21C becomes smaller toward the portion closer to the base layer 11C. That is, the inner side surface of the multilayer structure layer 15C that partitions the opening 21C has a frustum cylindrical shape, and the electrode catalyst layer 22C fills the bottom of the opening 21C having such a shape. In this case, in the membrane electrode assemblies 35 and 36, the inner peripheral edge of the gasket layer 18C has a forward tapered shape as viewed from the polymer electrolyte membrane 30 side. According to such a manufacturing method, the electrode catalyst layers 22C and 22A and the gasket layers 18C and 18A are separately formed on the surface of the polymer electrolyte membrane 30 as in the conventional manner. It can also be formed in a shape that is difficult to form depending on the manufacturing method placed in

The catalyst layer transfer substrate described above and the method of producing a membrane electrode assembly using the catalyst layer transfer substrate will be described using specific examples and comparative examples.
Example 1
A laminate of the bonding layer and the gasket layer was formed using a pressure-sensitive adhesive sheet in which separate films were disposed on both sides, and the laminate was bonded to the base material layer. As the first bonding layer, an acrylic pressure-sensitive adhesive having a thickness of 10 μm is used. As the second bonding layer, an acrylic pressure-sensitive adhesive having a thickness of 10 μm is used. As the third bonding layer, a thickness is An acrylic adhesive having a thickness of 10 μm was used. In addition, a PTFE (polytetrafluoroethylene) sheet having a thickness of 50 μm was used as the base material layer, and a PET (polyethylene terephthalate) film having a thickness of 25 μm was used as the gasket layer.

  The peel strength of the first bonding layer with respect to the base material layer is larger than the peel strength of the second bonding layer with respect to the gasket layer, and the difference between these peel strengths was 0.2 N / 25 mm. In addition, the peel strength of the third bonding layer to the gasket layer is larger than the peel strength of the second bonding layer to the gasket layer, and the difference between the peel strengths was 1.4 N / 25 mm. Peeling strength was determined by measuring 180 ° peeling strength at a peeling speed of 300 mm / min according to JIS-K-6854-2: 1999 using a tensile tester (manufactured by A & D Co .: STA-1225).

A separate film attached to one surface of the third bonding layer was used as a covering layer, and a 5 cm ² square opening was formed in the laminate of the bonding layer and the gasket layer. The reinforcement layer was arrange | positioned on the surface on the opposite side of the base material layer to which the laminated body was bonded. As the reinforcing layer, PET with a bonding layer having a thickness of 25 μm was used.

  Subsequently, the catalyst ink was applied to the base material layer through the openings by the doctor blade method, and the applied catalyst ink was dried for 5 minutes in an air atmosphere at a temperature of 80 ° C. to form an electrode catalyst layer. Thereby, the catalyst layer transfer base material of Example 1 was obtained.

  Two catalysts using NAFION® 212 (manufactured by DuPont) as the polymer electrolyte membrane, so that each of the two catalyst layer transfer substrates faces each of the two contact surfaces of the polymer electrolyte membrane A layer transfer substrate and a polymer electrolyte membrane were disposed. Thereafter, the polymer electrolyte membrane sandwiched between these two catalyst layer transfer substrates is heated to 130 ° C. and held under pressure for 10 minutes, and the electrode catalyst layer and the gasket layer are transferred to the polymer electrolyte membrane. By doing this, the membrane electrode assembly of Example 1 was obtained. In the peeling process of the base material layer after transfer, the base material layer could be peeled off at the interface between the second bonding layer and the gasket layer together with the first bonding layer and the second bonding layer.

Example 2
A catalyst layer transfer substrate of Example 2 was obtained in the same manner as in Example 1 except for the peel strength of the bonding layer. The peel strength of the first bonding layer with respect to the base material layer is larger than the peel strength of the second bonding layer with respect to the gasket layer, and the difference between these peel strengths is 0.1 N / 25 mm. In addition, the peel strength of the third bonding layer to the gasket layer is larger than the peel strength of the second bonding layer to the gasket layer, and the difference between the peel strengths was 3.5 N / 25 mm.

  A membrane / electrode assembly of Example 2 was obtained in the same manner as in Example 1 using the catalyst layer transfer base material of Example 2. In the peeling step of the base material layer after transfer of the electrode catalyst layer and the gasket layer, the base material layer could be peeled off at the interface between the second bonding layer and the gasket layer together with the first bonding layer and the second bonding layer.

[Example 3]
A catalyst layer transfer substrate of Example 3 was obtained in the same manner as in Example 1 except for the peeling strength of the bonding layer. The peel strength of the first bonding layer with respect to the base material layer is larger than the peel strength of the second bonding layer with respect to the gasket layer, and the difference between these peel strengths was set to 8.5 N / 25 mm. Further, the peel strength of the third bonding layer to the gasket layer is larger than the peel strength of the second bonding layer to the gasket layer, and the difference in the peel strength between them was 6.2 N / 25 mm.

  A membrane / electrode assembly of Example 3 was obtained in the same manner as in Example 1 using the catalyst layer transfer base material of Example 3. In the peeling step of the base material layer after transfer of the electrode catalyst layer and the gasket layer, the base material layer could be peeled off at the interface between the second bonding layer and the gasket layer together with the first bonding layer and the second bonding layer.

Example 4
A catalyst layer transfer substrate of Example 4 was obtained in the same manner as in Example 1 except for the peel strength of the bonding layer. The peel strength of the first bonding layer with respect to the base material layer is larger than the peel strength of the second bonding layer with respect to the gasket layer, and the difference between these peel strengths was set to 0.05 N / 25 mm. In addition, the peel strength of the third bonding layer to the gasket layer is larger than the peel strength of the second bonding layer to the gasket layer, and the difference between the peel strengths of these was set to 0.07 N / 25 mm.

  A membrane / electrode assembly of Example 4 was obtained in the same manner as in Example 1 using the catalyst layer transfer base material of Example 4. In the peeling step of the base material layer after transfer of the electrode catalyst layer and the gasket layer, the base material layer could be peeled off at the interface between the second bonding layer and the gasket layer together with the first bonding layer and the second bonding layer.

[Example 5]
A catalyst layer transfer substrate of Example 5 was obtained in the same manner as in Example 1 except for the peel strength of the bonding layer. The peel strength of the first bonding layer with respect to the base material layer is larger than the peel strength of the second bonding layer with respect to the gasket layer, and the difference between these peel strengths is 0.1 N / 25 mm. In addition, the peel strength of the third bonding layer to the gasket layer is larger than the peel strength of the second bonding layer to the gasket layer, and the difference between the peel strengths of these was 3.7 N / 25 mm.

  A membrane / electrode assembly of Example 5 was obtained in the same manner as in Example 1 using the catalyst layer transfer base material of Example 5. In the peeling step of the base material layer after transfer of the electrode catalyst layer and the gasket layer, the base material layer could be peeled off at the interface between the second bonding layer and the gasket layer together with the first bonding layer and the second bonding layer.

Comparative Example 1
A catalyst layer transfer base material of Comparative Example 1 was obtained in the same manner as Example 1 except for the peeling strength of the bonding layer. The peel strength of the first bonding layer with respect to the base material layer is smaller than the peel strength of the second bonding layer with respect to the gasket layer, and the difference between these peel strengths was 1.5 N / 25 mm. In addition, the peel strength of the third bonding layer to the gasket layer is larger than the peel strength of the second bonding layer to the gasket layer, and the difference in the peel strength between them is 0.1 N / 25 mm.

  A membrane / electrode assembly of Comparative Example 1 was obtained in the same manner as in Example 1 using the catalyst layer transfer base material of Comparative Example 1. In the peeling step of the base material layer after transfer of the electrode catalyst layer and the gasket layer, peeling occurred at the interface between the first bonding layer and the base layer, and peeling at the interface between the second bonding layer and the gasket layer was not possible.

Comparative Example 2
A catalyst layer transfer base material of Comparative Example 2 was obtained in the same manner as Example 1 except for the peeling strength of the bonding layer. The peel strength of the first bonding layer with respect to the base material layer is smaller than the peel strength of the second bonding layer with respect to the gasket layer, and the difference between these peel strengths was 1.5 N / 25 mm. In addition, the peel strength of the third bonding layer to the gasket layer is smaller than the peel strength of the second bonding layer to the gasket layer, and the difference in the peel strength between them was 0.7 N / 25 mm.

  A membrane / electrode assembly of Comparative Example 2 was obtained in the same manner as in Example 1 using the catalyst layer transfer base material of Comparative Example 2. In the peeling step of the base material layer after transfer of the electrode catalyst layer and the gasket layer, peeling occurred at the interface between the first bonding layer and the base layer, and peeling at the interface between the second bonding layer and the gasket layer was not possible.

From the above examples and comparative examples, in the configuration in which the adhesion of the first bonding layer to the base material layer and the adhesion of the third bonding layer to the gasket layer are larger than the adhesion of the second bonding layer to the gasket layer. It has been shown that the base material layer can be peeled off at the interface between the second bonding layer and the gasket layer, together with the first bonding layer and the second bonding layer.
(Supplementary note)
Means for solving the above problems include the following appendices as technical ideas derived from the above embodiment and the above modification.

(Supplementary Note 1) A membrane / electrode assembly manufactured using the above-mentioned catalyst layer transfer substrate, which is a polymer electrolyte membrane having a contact surface, an electrode catalyst layer located on the contact surface, and a surface of the contact surface. A gasket layer located in the periphery of the electrode catalyst layer in the direction, and a bonding layer located in the periphery of the electrode catalyst layer at the contact surface and sandwiched between the polymer electrolyte membrane and the gasket layer; A membrane electrode assembly in which an inner peripheral edge of the bonding layer is embedded in an outer peripheral edge of the electrode catalyst layer.
(Supplementary Note 2) A polymer electrolyte fuel cell comprising the membrane electrode assembly according to supplementary note 1 and a pair of separators sandwiching the membrane electrode assembly.

  The membrane electrode assembly or the polymer electrolyte fuel cell of the above-described configuration is manufactured using the manufacturing method described in the above embodiment. Therefore, in the membrane electrode assembly, exposure of the polymer electrolyte membrane between the electrode catalyst layer and the gasket layer is suppressed.

  10C, 10A: catalyst layer transfer base material, 11C, 11A: base material layer, 11a: first surface, 11b: second surface, 12C, 12A: reinforcing layer, 13C, 13A: reinforcing bonding layer, 14C, 14A: support Layers 15C, 15A: multilayer structure layer 16C, 16A: first bonding layer, 17C, 17A: second bonding layer, 18C, 18A: gasket layer, 19C, 19A: third bonding layer, 20C: covering layer, 21C 21A: opening 22C 22A: electrode catalyst layer 23C: 23A porous diffusion layer 30: polymer electrolyte membrane 30a: cathode contact surface 30b: anode contact surface 35: 36: membrane electrode assembly 40 Solid polymer fuel cell, 41C, 41A Separator.

Claims (10)

A base material layer having a first surface and a second surface which is a surface opposite to the first surface;
A multilayer structure layer having a frame shape disposed on the first surface, wherein the multilayer structure layer defines, on the first surface, an opening in which a material for forming an electrode catalyst layer is embedded.
Equipped with
The multilayer structure layer has a structure in which a first bonding layer, a second bonding layer, a gasket layer, and a third bonding layer are arranged in this order from the side closer to the first surface.
The force required to peel the second bonding layer from the gasket layer is smaller than the force required to peel the first bonding layer from the base layer, and from the gasket layer to the third bonding layer Catalyst layer transfer substrate smaller than the force required to peel off. The catalyst layer transfer substrate according to claim 1, wherein a reinforcing layer that suppresses deformation of the substrate layer due to a temperature change is disposed on the second surface of the substrate layer. The peel strength of the first bonding layer with respect to the base layer is greater than the peel strength of the second bonding layer with respect to the gasket layer, and the difference in the peel strength is at least 0.01 N / 25 mm and 10 N / The catalyst layer transfer substrate according to claim 1, which is less than 25 mm. The peel strength of the third bonding layer with respect to the gasket layer is larger than the peel strength of the second bonding layer with respect to the gasket layer, and the difference in peel strength between them is 0.01 N / 25 mm or more and 10 N / 25 mm. It is less than the catalyst layer transfer base material as described in any one of Claims 1-3. The catalyst layer transfer base material according to any one of claims 1 to 4, wherein the peel strength of the first bonding layer to the base material layer is 0.02 N / 25 mm or more and less than 10 N / 25 mm. The electrocatalyst layer is further disposed in the opening,
The thickness of the multilayer structure layer is larger than the thickness of the electrode catalyst layer, and the difference between the thickness of the multilayer structure layer and the thickness of the electrode catalyst layer is 100 μm or less. The catalyst layer transfer base material as described in 4. The catalyst layer transfer substrate according to any one of claims 1 to 6, wherein a thickness of the gasket layer is 1 μm or more and 100 μm or less. In the first surface of the base material layer having a first surface and a second surface opposite to the first surface, there is provided a multilayer structure layer which defines an opening on the first surface, Arranging the first bonding layer of the structural layer, the second bonding layer, the gasket layer, and the third bonding layer in this order from the side closer to the first surface;
Forming an electrode catalyst layer in the opening by coating the ink to form a catalyst layer transfer substrate having the substrate layer, the multilayer structure layer, and the electrode catalyst layer;
Pressing the catalyst layer transfer substrate against a polymer electrolyte membrane having a contact surface, and pressing the electrode catalyst layer and the third bonding layer in the multilayer structure layer on the contact surface;
Including
The adhesion of the first bonding layer to the base layer and the adhesion of the third bonding layer to the gasket layer are greater than the adhesion of the second bonding layer to the gasket layer. Production method. The base layer, the first bonding layer, and the second bonding layer are peeled off from the electrode catalyst layer and the gasket layer transferred from the catalyst layer transfer substrate to the contact surface of the polymer electrolyte membrane. The method for producing a membrane electrode assembly according to claim 8, further comprising the step of: A polymer electrolyte membrane having a contact surface,
An electrode catalyst layer located on the contact surface;
A gasket layer positioned around the electrode catalyst layer in a surface direction of the contact surface and in contact with a circumferential end surface of the electrode catalyst layer;
A base layer covering the electrode catalyst layer and the gasket layer;
A first bonding layer disposed between the gasket layer and the base layer and in contact with the base layer;
A second bonding layer disposed between the gasket layer and the base material layer and in contact with the gasket layer and the first bonding layer;
A third bonding layer disposed between the polymer electrolyte membrane and the gasket layer and in contact with the polymer electrolyte membrane and the gasket layer;
Equipped with
The force required to peel the second bonding layer from the gasket layer is smaller than the force required to peel the first bonding layer from the base layer, and from the gasket layer to the third bonding layer Membrane electrode assembly smaller than the force required to peel off.

Images