JP5101185B2 - Membrane-membrane reinforcing member assembly, membrane-catalyst layer assembly, membrane-electrode assembly, and polymer electrolyte fuel cell - Google Patents

Description

The present invention, membrane - membrane reinforcing member assembly, the membrane - catalyst layer assembly, a membrane - electrode assembly, and relates to a polymer electrolyte fuel cells.

  A polymer electrolyte fuel cell is one in which a fuel gas such as hydrogen and an oxidizing gas such as air are electrochemically reacted by a gas diffusion layer electrode having a catalyst layer such as platinum, and generates electricity and heat simultaneously. It is. The structure is a mixture of a carbon powder carrying a platinum-based metal catalyst on both sides of a polymer electrolyte membrane that selectively transports hydrogen ions, and a mixture of a hydrogen ion conductive polymer electrolyte. A catalyst layer is formed. Next, a gas diffusion layer is formed on the outer surface of the catalyst layer by using, for example, carbon paper that has both air permeability and electronic conductivity, such as water repellent treatment. The catalyst layer and the gas diffusion layer are collectively referred to as a gas diffusion electrode.

  Next, a gas sealant or gasket is placed around the electrode with a polymer electrolyte membrane in order to prevent the fuel gas supplying the fuel from leaking outside or mixing the fuel gas and oxidant gas with each other. To do. This sealant or gasket is integrated with the electrode and the polymer electrolyte membrane, and this is called MEA (membrane-electrode assembly). On the outside of the MEA, a conductive separator for mechanically fixing the MEA and electrically connecting adjacent MEAs to each other in series is disposed. In the portion of the separator that comes into contact with the MEA, a reaction gas is supplied to the electrode surface, and a gas flow path for carrying away the generated gas and surplus gas is formed. The gas flow path can be provided separately from the separator, but a system in which a groove is provided on the surface of the separator to form a gas flow path is common.

  Many fuel cells have a stacked structure in which a large number of unit cells having the above-described structure are stacked. During operation of the fuel cell, heat is generated with the generation of electric power. In a laminated battery, by providing a cooling water channel or the like for every 1 to 3 cells of a single cell, the generated thermal energy can be used in the form of hot water or the like while keeping the battery temperature constant.

  When the stack is manufactured, the polymer electrolyte membrane is sandwiched between electrodes and a separator, and is tightened with end plates and bolts. The polymer electrolyte membrane needs to have sufficient strength so that it can withstand the tightening pressure and so that physical damage due to wear or the like does not occur during long-term use. On the other hand, for reasons such as improving proton conductivity, it is necessary to make the polymer electrolyte membrane as thin as possible. For these reasons, various studies have been made to increase the strength of the polymer electrolyte without increasing the thickness.

For example, Patent Document 1 proposes a polymer electrolyte fuel cell intended to prevent damage to the polymer electrolyte membrane by attaching a frame-shaped protective membrane to the peripheral portion of the polymer electrolyte membrane (for example, FIG. 1 of Patent Document 1). Hereinafter, the structure of the polymer electrolyte fuel cell will be described with reference to the drawings. FIG. 13 is an exploded perspective view of a main part for explaining the positional relationship between a solid polymer electrolyte membrane and a fluororesin sheet (protective membrane) in the polymer electrolyte fuel cell described in Patent Document 1. . As shown in FIG. 13, in the polymer electrolyte fuel cell of Patent Document 1, a fluororesin sheet (protective membrane) is formed so as to cover all of the peripheral portion of the main surface of the solid polymer electrolyte membrane 1000 having a substantially rectangular shape. ) 220 and a fluororesin sheet (protective film) 240 are disposed on each of the front main surface and the back main surface of the solid polymer electrolyte membrane 1000.
Japanese Patent Laid-Open No. 5-21077

  However, since the polymer electrolyte fuel cell in the above-described prior art does not have a configuration (structure) that can be easily mass-produced at low cost, particularly in the joined part of the polymer electrolyte membrane and the protective membrane, There was still room for improvement when it was intended to further reduce the cost of the polymer electrolyte fuel cell and to further improve productivity (intended for efficient mass production).

  The present invention has been made in view of the above viewpoints, and has a configuration capable of ensuring sufficient durability and having a configuration suitable for cost reduction and mass production of a polymer electrolyte fuel cell. An object is to provide a member assembly and a method for manufacturing the same. Another object of the present invention is to provide a membrane-catalyst layer assembly comprising the membrane-membrane reinforcing member assembly of the present invention, and further having a catalyst layer disposed thereon, and a method for producing the same. Furthermore, an object of the present invention is to provide a membrane-electrode assembly having the membrane-catalyst layer assembly of the present invention described above, and further having a gas diffusion layer disposed thereon, and a method for producing the same. Another object of the present invention is to provide a polymer electrolyte fuel cell comprising the membrane-electrode assembly of the present invention.

  The reason why the polymer electrolyte fuel cell in the above-described prior art does not have a configuration that can be easily mass-produced at low cost, particularly in the joined portion of the polymer electrolyte membrane and the protective membrane, is as follows. It demonstrates more concretely using.

  FIG. 14 is an explanatory view showing an example of a manufacturing method generally assumed when the polymer electrolyte fuel cell described in Patent Document 1 is intended to be mass-produced using a known manufacturing technique of a thin film laminate. It is. For example, when mass-producing the polymer electrolyte fuel cell described in Patent Document 1, first, as shown in FIG. 14, a tape-shaped solid polymer electrolyte membrane 260 is manufactured and wound to roll 262. Then, a tape-shaped protective film 250 (a tape-shaped film in which the protective film 220 shown in FIG. 14 is continuously formed) is manufactured, and this is wound to form a roll 252. Next, a laminate having a tape-shaped protective film 250 laminated on at least one of the main surfaces of the tape-shaped solid polymer electrolyte membrane 260 is manufactured using an apparatus having a manufacturing mechanism configured as shown in FIG. . For example, the tape-shaped protective film 250 and the tape-shaped solid polymer electrolyte membrane 260 are pulled out from the roll 252 and the roll 262, respectively, and sandwiched between a pair of rollers 290 and wound as a laminate, The roll is 280. In some cases, the heat treatment, the pressure treatment, and the pressure heat treatment may be performed during the integration between the rollers 290. Immediately before the integration, the tape-shaped protective film 250 and the tape-shaped solid polymer electrolyte are provided. An adhesive may be applied to at least one main surface (adhesion surface) of the film 260.

  When the roll 280 is manufactured, tension is applied to the protective film 250 in a direction D10 in which the protective film 250 travels (longitudinal direction of the tape-shaped protective film 250). At this time, the protective film 250 is a very thin film (for example, 50 μm or less), and the opening 222 is formed inside the main surface. The vertical portion R200 comes to be lifted. Accordingly, there is a high possibility that the portion of R200 is wrinkled between the roller 290 and the roll 252 when the protective film 250 is pressed by the roller 290. Further, there is a high possibility that the R200 portion of the protective film 250 is peeled off from the solid polymer electrolyte membrane 260 due to the tension between the roller 290 and the roll 280.

  For the above reasons, in the polymer electrolyte fuel cell having the conventional configuration shown in FIG. 13, from the viewpoint of reliably manufacturing without producing defective products, it takes time and complexity to manufacture MEAs one by one. It was only possible to adopt the method. That is, it is only possible to employ a complicated and expensive manufacturing method in which the protective films 220 and 240 are positioned and attached to the solid electrolyte membrane 1000 one by one by a batch method.

In order to solve such a problem, the present invention provides a polymer electrolyte membrane having a pair of first main surface and second main surface facing each other and having a substantially rectangular shape,
It is arranged in a portion along a pair of opposite sides of the four sides of the first main surface, has a main surface smaller than the first main surface, and exhibits a film-like shape that can be wound. A pair of first membrane reinforcing members for reinforcing the polymer electrolyte membrane;
It is arranged in a portion along a pair of opposite sides of the four sides of the second main surface, has a main surface smaller than the second main surface, and exhibits a film-like shape that can be wound. A pair of second membrane reinforcing members for reinforcing the polymer electrolyte membrane;
Have
The one set of sides of the first main surface where the pair of first membrane reinforcing members are arranged, and the one set of sides of the second main surface where the pair of second membrane reinforcing members are arranged And are almost orthogonal,
The pair of first membrane reinforcing members and the pair of second membrane reinforcing members are alternately arranged on the first main surface and the second main surface along the four sides of the polymer electrolyte membrane as a whole. Extending so as to exist and arranged so as to sandwich the four corner portions of the polymer electrolyte membrane ,
The first membrane reinforcing member and the second membrane reinforcing member are polyethylene naphthalate, polytetrafluoroethylene, polyethylene terephthalate, fluoroethylene-propylene copolymer, tetrafluoroethylene-perfluoroalkoxyethylene copolymer, polyethylene, polypropylene. And at least one synthetic resin selected from the group consisting of polyetheramide, polyetherimide, polyetheretherketone, polyethersulfone, polyphenylene sulfide, polyarylate, polysulfide, polyimide, and polyimideamide. The membrane-membrane reinforcing member assembly is provided.

  As described above, the membrane-membrane reinforcing member assembly of the present invention has a pair of reinforcing members only on one set of sides facing each other among the four sides of the main surface (first main surface or second main surface). (The 1st film | membrane reinforcement member or the 2nd film | membrane reinforcement member) has the structure arrange | positioned. Therefore, there is no R200 portion in the protective film 250 of the fuel cell described above with reference to FIG. Therefore, the membrane-membrane reinforcing member assembly of the present invention is obtained by laminating a tape-like reinforcing member (first membrane reinforcing member or second membrane reinforcing member) on a tape-like polymer electrolyte membrane, and the polymer electrolyte membrane and It is possible to easily apply a known mass production technique for a thin film laminate, such as manufacturing a roll made of a laminate of reinforcing members. Therefore, the membrane-membrane reinforcing member assembly of the present invention is a complicated and expensive manufacturing method in which the protective film is positioned and attached to the solid electrolyte membrane one by one by the batch method described above. Therefore, mass production can be easily performed at low cost. In the membrane-membrane reinforcing member assembly of the present invention, as described above, the pair of first membrane reinforcing members and the pair of second membrane reinforcing members are arranged on the four sides of the polymer electrolyte membrane as a whole. The polymer electrolyte membrane is arranged so as to extend along the four corners of the polymer electrolyte membrane. Thereby, the membrane-membrane reinforcing member assembly of the present invention has sufficient mechanical strength that can sufficiently prevent damage to the polymer electrolyte membrane. That is, in the membrane-membrane reinforcing member assembly of the present invention, sufficient durability is ensured by the pair of first membrane reinforcing members and the pair of second membrane reinforcing members.

  Therefore, the membrane-membrane reinforcing member assembly of the present invention is mass-produced in which a pair of first membrane reinforcing members and a pair of second membrane reinforcing members are arranged via a polymer electrolyte membrane as described above. Therefore, if a polymer electrolyte fuel cell is configured using the membrane-membrane reinforcing member assembly of the present invention, sufficient durability can be ensured while the polymer electrolyte fuel cell is further improved. Cost reduction and further improvement in productivity can be easily achieved.

  Furthermore, the membrane-membrane reinforcing member assembly of the present invention has the first membrane reinforcing member (or the second membrane) only on one set of sides facing each other among the four sides of the first main surface (or the second main surface). 14 is a material more than the polymer electrolyte fuel cell described in Patent Document 1 having a configuration in which the protective films 220 and 240 shown in FIG. 14 are arranged on all the peripheral portions of the main surface. Cost can be reduced.

The present invention also includes the membrane-membrane reinforcing member assembly of the present invention described above,
A first catalyst layer disposed in at least a part of a region of the first main surface of the polymer electrolyte of the membrane-membrane reinforcing member assembly where the first membrane reinforcing member is not disposed;
A second catalyst layer disposed in at least part of a region where the second membrane reinforcing member is not disposed in the second main surface of the polymer electrolyte of the membrane-membrane reinforcing member assembly;
A membrane-catalyst layer assembly is provided.

  As described above, since the membrane-catalyst layer assembly of the present invention has a configuration including the membrane-membrane reinforcing member assembly of the present invention, a polymer using the membrane-catalyst layer assembly of the present invention is used. If the electrolyte fuel cell is configured, it is possible to easily further reduce the cost of the polymer electrolyte fuel cell and further improve the productivity.

Furthermore, the present invention relates to the membrane-catalyst layer assembly of the present invention described above,
A first gas diffusion layer arranged to cover the first catalyst layer of the membrane-catalyst layer assembly;
A second gas diffusion layer arranged to cover the second catalyst layer of the membrane-catalyst layer assembly;
A membrane-electrode assembly is provided.

  As described above, since the membrane-electrode assembly of the present invention has a configuration including the membrane-membrane reinforcing member assembly of the present invention and the membrane-catalyst layer assembly, the membrane-electrode of the present invention. If a polymer electrolyte fuel cell is configured using the joined body, further cost reduction and further improvement in productivity of the polymer electrolyte fuel cell can be easily achieved.

The present invention also provides the membrane-electrode assembly of the present invention described above and the first gas diffusion layer on the peripheral portion of the main surface of the membrane-electrode assembly where the first gas diffusion layer is formed. A frame-shaped first gasket arranged so as to surround, and a groove-like flow path of one reaction gas is formed on one main surface, and the one main surface is the first gas diffusion of the membrane-electrode assembly A plate-like first separator disposed so as to contact the layer and the first gasket, and the second gas at a peripheral portion of the main surface on which the second gas diffusion layer of the membrane-electrode assembly is formed. A frame-shaped second gasket arranged so as to surround the diffusion layer, and a groove-like flow path for the other reaction gas is formed on one main surface, and the one main surface is the first of the membrane-electrode assembly. and comprises 2 and the second separator arranged plate-shaped so as to contact with the gas diffusion layer and the second gasket, the Providing a polymer electrolyte fuel cell.

  As described above, the polymer electrolyte fuel cell of the present invention has a configuration comprising the membrane-membrane reinforcing member assembly of the present invention, the membrane-catalyst layer assembly, and the membrane-electrode assembly of the present invention. Therefore, according to the polymer electrolyte fuel cell of the present invention, further cost reduction and further productivity improvement can be easily achieved.

According to the present invention, it can ensure sufficient durability, and cost reduction of the polymer electrolyte fuel cell, and has a configuration suitable for mass production, film - can provide a membrane reinforcing member assembly.

Further, according to the present invention, the membrane-membrane reinforcing member assembly of the present invention described above is provided, and a catalyst layer is further disposed, which is suitable for cost reduction and mass production of a polymer electrolyte fuel cell. film - it is possible to provide a catalyst layer assembly.

Furthermore, according to the present invention, the membrane-catalyst layer assembly of the present invention described above is provided, and a gas diffusion layer is further disposed, which is suitable for cost reduction and mass production of a polymer electrolyte fuel cell. it is possible to provide an electrode assembly - film.

Further, according to the present invention, films of the present invention described above - can provide includes a electrode assembly, cost reduction, and polymer electrolyte fuel cells suitable for mass production.

The best mode for carrying out the present invention will be described below with reference to the drawings. In addition, the same code | symbol is attached | subjected to the same or an equivalent part, and the overlapping description may be abbreviate | omitted.
[First Embodiment]
FIG. 1 is a perspective view showing an example of the basic configuration of the first embodiment of the membrane-membrane reinforcing member assembly of the present invention. FIG. 2 shows a basic configuration of a membrane-catalyst layer assembly (first embodiment of the membrane-catalyst layer assembly of the present invention) in which a catalyst layer is further arranged on the membrane-membrane reinforcing member assembly 1 shown in FIG. It is a perspective view which shows an example. 3 shows the basic configuration of the membrane-electrode assembly (the first embodiment of the membrane-electrode assembly of the present invention) in which a gas diffusion layer is further arranged on the membrane-catalyst layer assembly 2 shown in FIG. It is a perspective view which shows an example. FIG. 4 shows an example of the basic configuration of a polymer electrolyte fuel cell (the first embodiment of the polymer electrolyte fuel cell of the present invention) provided with the membrane-electrode assembly 3 shown in FIG. It is sectional drawing which shows a part.

  First, the membrane-membrane reinforcing member assembly 1 according to the first embodiment shown in FIG. 1 will be described.

  As shown in FIG. 1, the membrane-membrane reinforcing member assembly 1 includes a first membrane reinforcing member 22 and 24 and a second membrane reinforcing member 26 and 28 as a whole along four sides of the polymer electrolyte membrane 10. And is arranged so as to sandwich the four corners of the polymer electrolyte membrane 10 (hereinafter, referred to as “in a cross-beam pattern”).

  That is, as shown in FIG. 1, the membrane-membrane reinforcing member assembly 1 includes a polymer electrolyte membrane having a pair of first main surface F1 and second main surface F2 that face each other and have a substantially rectangular shape. 10 and four sides of the first main surface F1 are disposed along a pair of opposing sides, and have a main surface smaller than the first main surface F1 and have a film-like shape. A pair of first membrane reinforcing members 22 and 24 and a main surface that is disposed along a pair of opposing sides of the four sides of the second main surface F2 and that is smaller than the second main surface F2. And a pair of second membrane reinforcing members 26 and 28 having a film-like shape.

  The membrane-membrane reinforcing member assembly 1 according to the first embodiment includes a pair of reinforcing members (the first membrane reinforcing member 22 and the first membrane reinforcing member 22) on only one set of opposing sides of the four sides of the first main surface F1. 24) is arranged. Further, the membrane-membrane reinforcing member assembly 1 includes a pair of opposing sides among the four sides of the second main surface F2 (the first membrane reinforcing members 22 and 24 among the four sides of the second main surface F2). A pair of reinforcing members (second membrane reinforcing members 26 and 28) is disposed only on a pair of sides that are substantially orthogonal to a pair of sides of the first main surface F1 on which is disposed. Yes.

  Therefore, there is no R200 portion in the protective film 250 of the fuel cell described above with reference to FIG. Therefore, the membrane-membrane reinforcing member assembly 1 includes a tape-like polymer electrolyte membrane 140 and a tape-like reinforcing member (first membrane reinforcing members 142A and 142B, etc.) as will be described later with reference to FIGS. Thus, it is possible to easily apply a known mass production technique for a thin film laminate, such as producing a laminate 143 of a polymer electrolyte membrane and a reinforcing member.

  Therefore, the membrane-membrane reinforcing member assembly 1 is a batch type method in which the solid electrolyte membrane 10 is provided with reinforcing members (first membrane reinforcing members 22 and 24 or second membrane reinforcing members 26 and 28) one by one. It is not necessary to employ a complicated and expensive manufacturing method that requires time and positioning and can be easily mass-produced at low cost.

  In addition, as described above, the membrane-membrane reinforcing member assembly 1 includes the first membrane reinforcing members 22 and 24 and the second membrane reinforcing members 26 and 28 as a whole along the four sides of the polymer electrolyte membrane 10. And is arranged so as to sandwich the four corners of the polymer electrolyte membrane 10 (in a cross-beam pattern). Thereby, the membrane-membrane reinforcing member assembly 1 has a sufficient mechanical strength that can sufficiently prevent the polymer electrolyte membrane 10 from being damaged.

  As described above, the membrane-membrane reinforcing member assembly 1 has a structure suitable for mass production in which the first membrane reinforcing members 22 and 24 and the second membrane reinforcing members 26 and 28 are arranged via the polymer electrolyte membrane 10. Therefore, if a polymer electrolyte fuel cell is configured using the membrane-membrane reinforcing member assembly 1, further cost reduction of the polymer electrolyte fuel cell can be achieved while ensuring sufficient durability, and Further improvement in productivity can be easily achieved.

  In the membrane-membrane reinforcing member assembly 1 shown in FIG. 1, the outer edges of the first membrane reinforcing members 22 and 24 coincide with the outer edge of the polymer electrolyte membrane 10, and the second membrane reinforcing member. Although the embodiment in which the outer edges of the polymer electrolyte membrane 10 coincide with each other has been described, the first membrane reinforcing members 22 and 24 and the second membrane reinforcing members 26 and 28 as a whole are polymer electrolyte membranes. 10, and the arrangement positions of the first membrane reinforcing members 22 and 24 and the second membrane reinforcing members 26 and 28 on the polymer electrolyte membrane 10 are limited to this mode. Is not to be done.

  For example, the first membrane reinforcing member 22 may be disposed on the polymer electrolyte membrane 10 such that the outer edge of the polymer electrolyte membrane 10 protrudes outside the outer edge of the first membrane reinforcing member 22. Further, for example, the first membrane reinforcing member 22 may be disposed on the polymer electrolyte membrane 10 such that the outer edge of the first membrane reinforcing member 22 protrudes outside the outer edge of the polymer electrolyte membrane 10. Furthermore, the arrangement position of the first membrane reinforcing member 24 on the polymer electrolyte membrane 10, the arrangement position of the second membrane reinforcing member 26 on the polymer electrolyte membrane 10, and the second position on the polymer electrolyte membrane 10. The arrangement position of the membrane reinforcing member 28 may be the same as the arrangement position of the first membrane reinforcing member 22 on the polymer electrolyte membrane 10.

  Next, each component of the membrane-membrane reinforcing member assembly 1 will be described.

  The membrane-membrane reinforcing member assembly of the present invention has the first membrane reinforcing member (or the second membrane reinforcing member) only on one set of sides facing each other among the four sides of the first main surface (or the second main surface). 14), the material cost is lower than that of the polymer electrolyte fuel cell described in Patent Document 1 having the configuration in which the protective films 220 and 240 shown in FIG. 14 are arranged on all the peripheral portions of the main surface. Can be reduced.

  The polymer electrolyte membrane 10 has proton conductivity. Preferred examples of the polymer electrolyte membrane 10 include those having sulfonic acid groups, carboxylic acid groups, phosphonic acid groups, and sulfonimide groups as cation exchange groups. From the viewpoint of proton conductivity, the polymer electrolyte membrane 10 preferably has a sulfonic acid group.

  The resin constituting the polymer electrolyte membrane having a sulfonic acid group is preferably a dry resin having an ion exchange capacity of 0.5 to 1.5 meq / g. It is preferable that the ion exchange capacity of the polymer electrolyte membrane is 0.5 meq / g dry resin or more because an increase in the resistance value of the polymer electrolyte membrane during power generation can be more sufficiently reduced, and the ion exchange capacity is 1.5 meq / g. It is preferable that it is less than g dry resin since the water content of the polymer electrolyte membrane does not increase, it becomes difficult to swell, and the pores in the catalyst layer are not likely to be clogged. From the same viewpoint as described above, the ion exchange capacity is particularly preferably 0.8 to 1.2 meq / g dry resin.

As the polymer _{electrolyte, CF 2 = CF- (OCF 2} CFX) m-Op- (CF 2) a perfluorovinyl compound represented by the n-SO ₃ H (m is an integer of 0 to 3, n is 1 represents an integer of 1 to 12, p represents 0 or 1, and X represents a fluorine atom or a trifluoromethyl group.) And a copolymer comprising a polymer unit based on tetrafluoroethylene It is preferable.

Preferable examples of the fluorovinyl compound include compounds represented by the following formulas (4) to (6). However, in the following formula, q is an integer of 1 to 8, r is an integer of 1 to 8, and t is 1 to 8.
An integer of 3 is shown.

_{CF 2 = CFO (CF 2)} q-SO 3 H ··· (4)
_{CF 2 = CFOCF 2 CF (CF} 3) O (CF 2) r-SO 3 H ··· (5)
_{CF 2 = CF (OCF 2 CF} (CF 3)) tO (CF 2) 2 -SO 3 H ··· (6)
The 1st membrane reinforcement member 22 and the 1st membrane reinforcement member 24 are arrange | positioned in the part along a pair of edge | sides which mutually oppose among 4 sides of the 1st main surface F1 of the polymer electrolyte membrane 10. FIG. Moreover, the 1st membrane reinforcement member 22 and the 1st membrane reinforcement member 24 have the substantially rectangular main surfaces F22 and F24 smaller than the 1st main surface F1. When the first membrane reinforcing member 22 and the first membrane reinforcing member 24 are arranged on the polymer electrolyte membrane 10, the fastening pressure when the polymer electrolyte fuel cell 4 (see FIG. 4 described later) is configured. The polymer electrolyte membrane 10 is sufficiently prevented from being damaged due to such as.

  The 2nd membrane reinforcement member 26 and the 2nd membrane reinforcement member 28 are arrange | positioned in the part along a pair of mutually opposing edge | side of 4 sides of the 2nd main surface F2 of the polymer electrolyte membrane 10. FIG. Moreover, the 2nd film | membrane reinforcement member 26 and the 1st film | membrane reinforcement member 28 have the substantially rectangular main surfaces F26 and F28 smaller than the 2nd main surface F2. The second membrane reinforcing member 26 and the second membrane reinforcing member 28 are disposed on the polymer electrolyte membrane 10, so that when the polymer electrolyte fuel cell 4 is configured, a polymer is applied due to a fastening pressure. Damage to the electrolyte membrane 10 is sufficiently prevented.

  In the membrane-membrane reinforcing member assembly 1 shown in FIG. 1, a pair of first membrane reinforcing members 22 and 24 and a pair of second membrane reinforcing members 26 and 28 are interposed via the polymer electrolyte membrane 10. They are arranged so as to form a cross girder. The positional relationship between the first membrane reinforcing members 22 and 24 and the second membrane reinforcing members 26 and 28 will be described more specifically. The membrane-membrane reinforcing member assembly 1 is viewed from the normal direction of the first main surface. In this case, the first membrane reinforcing members 22 and 24 and the second membrane reinforcing members 26 and 28 are the longitudinal direction (long side direction) of the main surface F22 of the first membrane reinforcing member 22 and the main membrane of the first membrane reinforcing member 24. The longitudinal direction (long side direction) of the surface F24, the longitudinal direction (long side direction) of F26 of the main surface of the second membrane reinforcing member 26, and the longitudinal direction (long side direction) of the main surface F28 of the second membrane reinforcing member 28. Are disposed so as to be substantially perpendicular to each other (arranged so that the polymer electrolyte membranes 10 are substantially perpendicular to each other with the polymer electrolyte membranes 10 disposed therebetween).

  In addition, as a material constituting the first membrane reinforcing member 22 and the first membrane reinforcing member 24, or the second membrane reinforcing member 26 and the second membrane reinforcing member 28, polyethylene naphthalate, polytetra Fluoroethylene, polyethylene terephthalate, fluoroethylene-propylene copolymer, tetrafluoroethylene-perfluoroalkoxyethylene copolymer, polyethylene, polypropylene, polyether amide, polyether imide, polyether ether ketone, polyether sulfone, polyphenylene sulfide, It is preferably at least one synthetic resin selected from the group consisting of polyarylate, polysulfide, polyimide, and polyimideamide.

  Furthermore, the thickness of the first membrane reinforcing member 22, the thickness of the first membrane reinforcing member 24, the thickness of the second membrane reinforcing member 26, and the thickness of the second membrane reinforcing member 28 obtain the effects of the present invention. The thickness of the first membrane reinforcing member 22 is preferably equal to the thickness of the first membrane reinforcing member 24 from the viewpoint of more reliably obtaining the effects of the present invention. From the same viewpoint, the thickness of the second membrane reinforcing member 26 and the thickness of the second membrane reinforcing member 28 are preferably equal.

  Next, the membrane-catalyst layer assembly 2 of the first embodiment shown in FIG. 2 will be described.

  In the membrane-catalyst layer assembly 2, the first catalyst layer 31 is disposed substantially at the center of the first main surface F1, and the second catalyst layer 32 (see FIG. 4) is disposed substantially at the center of the second main surface F2. Except for this, it has the same configuration as the membrane-membrane reinforcing member assembly 1 shown in FIG.

  From the viewpoint of ease of manufacture, the thickness of the first catalyst layer 31 is preferably equal to or less than the thickness of the first membrane reinforcing member 22 and the thickness of the first membrane reinforcing member 24, and more preferably equal. From the same viewpoint, the thickness of the second catalyst layer 32 is preferably equal to or less than the thicknesses of the second membrane reinforcing member 26 and the second membrane reinforcing member 28, and more preferably equal.

  The structure of the 1st catalyst layer 31 and the structure of the 2nd catalyst layer 32 will not be specifically limited if the effect of this invention is acquired, It is the same as that of the catalyst layer of the gas diffusion electrode mounted in the well-known fuel cell. You may have the structure of. Moreover, the structure of the 1st catalyst layer 31 and the structure of the 2nd catalyst layer 32 may be the same, and may differ.

  For example, the configuration of the first catalyst layer 31 and the configuration of the second catalyst layer 32 include a configuration including conductive carbon particles carrying an electrode catalyst and a polymer electrolyte having cation (hydrogen ion) conductivity. You may have, and you may have the structure which further contains water-repellent materials, such as polytetrafluoroethylene. In addition, as a polymer electrolyte, the same kind as the constituent material of the polymer electrolyte membrane 10 mentioned above may be used, and a different kind may be used. As a polymer electrolyte, what was described as a constituent material of the polymer electrolyte membrane 10 can be used.

  The electrode catalyst is made of metal particles (for example, metal particles made of a noble metal) and is used by being supported on conductive carbon particles (powder). The metal particles are not particularly limited and various metals can be used, but from the viewpoint of electrode reaction activity, platinum, gold, silver, ruthenium, rhodium, palladium, osmium, iridium, chromium, iron, titanium, manganese It is preferably at least one selected from the group consisting of cobalt, nickel, molybdenum, tungsten, aluminum, silicon, zinc and tin. Among these, platinum and an alloy of platinum are preferable, and an alloy of platinum and ruthenium is particularly preferable in the anode because the activity of the catalyst is stabilized.

  The electrode catalyst particles more preferably have an average particle size of 1 to 5 nm. An electrode catalyst having an average particle diameter of 1 nm or more is preferable because it is easy to prepare industrially, and if it is 5 nm or less, the activity per mass of the electrode catalyst is more easily secured, thereby reducing the cost of the fuel cell. Connection is preferable.

The conductive carbon particles preferably have a specific surface area of 50 to 1500 m ² / g. A specific surface area of 50 m ² / g or more is preferable because it is easy to increase the loading ratio of the electrode catalyst and the output characteristics of the obtained first catalyst layer 31 and second catalyst layer 32 can be more sufficiently secured. When the specific surface area is 1500 m ² / g or less, sufficiently large pores can be secured more easily and coating with a polymer electrolyte becomes easier, and the first catalyst layer 31 and the second catalyst layer This is preferable because the output characteristics of 32 can be more sufficiently secured. From the same viewpoint as described above, the specific surface area is particularly preferably 200 to 900 m ² / g.

  The conductive carbon particles preferably have an average particle size of 0.1 to 1.0 μm. When the thickness is 0.1 μm or more, gas diffusibility in the first catalyst layer 31 and the second catalyst layer 32 is more easily secured, and flooding can be prevented more reliably. In addition, when the average particle diameter of the conductive carbon particles is 1.0 μm or less, it becomes easy to easily make the electrode catalyst covered with the polymer electrolyte in a good state, and the electrode catalyst covered area with the polymer electrolyte is more increased. Since it becomes easy to ensure enough, it becomes easy to ensure sufficient electrode performance more and is preferable.

  The 1st catalyst layer 31 and the 2nd catalyst layer 32 can be formed using the manufacturing method of the catalyst layer of the gas diffusion electrode of a well-known fuel cell, for example. For example, a liquid (for forming a catalyst layer) containing at least a constituent material of the first catalyst layer 31 and the second catalyst layer 32 (for example, conductive carbon particles carrying an electrode catalyst and a polymer electrolyte) and a dispersion medium. Ink) can be prepared and used.

  Next, the membrane-electrode assembly 3 according to the first embodiment shown in FIG. 3 will be described.

  In the membrane-electrode assembly 3, a first gas diffusion layer 41 having a substantially rectangular main surface F5 is disposed so as to cover the first catalyst layer 31, and further, a substantially rectangular shape is formed so as to cover the second catalyst layer 32. The membrane-catalyst layer assembly 2 has the same configuration as the membrane-catalyst layer assembly 2 shown in FIG. 2 except that the second gas diffusion layer 42 having the main surface F6 having the shape is arranged.

  The area of the main surface F5 of the first gas diffusion layer is preferably equal to or larger than the area of the main surface F3 of the first catalyst layer, and more preferably larger than the area of the main surface F3 of the first catalyst layer. Furthermore, the area of the main surface F6 of the second gas diffusion layer is preferably equal to or larger than the area of the main surface F4 of the second catalyst layer, and more preferably larger than the area of the main surface F4 of the second catalyst layer.

  Furthermore, the area of the main surface F5 of the first gas diffusion layer is larger than the area of the main surface F3 of the first catalyst layer, and the area of the main surface F6 of the second gas diffusion layer is the main surface F4 of the second catalyst layer. Of the four sides of the substantially rectangular main surface F5, which is a pair of sides facing each other, and is disposed at a position closest to the first membrane reinforcing member 22 and the first membrane reinforcing member 24. End portions of the first gas diffusion layer including a set of sides are placed on the main surface F22 of the first membrane reinforcing member 22 and the main surface F24 of the first membrane reinforcing member 24. Is preferred. In addition, one set of sides of the four sides of the substantially rectangular main surface F6 facing each other, the set of sides arranged closest to the second membrane reinforcing member 26 and the second membrane reinforcing member 28 It is preferable that the edge part of the 2nd gas diffusion layer containing is in the state mounted on the main surface F26 of the 2nd film | membrane reinforcement member 26, and the main surface F28 of the 2nd film | membrane reinforcement member 28. FIG. By arranging the first gas diffusion layer 41 and the second gas diffusion layer 42 as described above, when the membrane-electrode assembly 3 is fastened, the end of the gas diffusion layer 41 and the end of the gas diffusion layer 42 are In addition, high durability can be obtained more reliably without directly contacting the polymer electrolyte membrane 10.

  The configuration of the first gas diffusion layer 41 and the configuration of the second gas diffusion layer 42 are not particularly limited as long as the effects of the present invention can be obtained, and the gas diffusion of a gas diffusion electrode mounted on a known fuel cell is performed. You may have the structure similar to a layer. Further, the configuration of the first gas diffusion layer 41 and the configuration of the second gas diffusion layer 42 may be the same or different.

  For example, the first gas diffusion layer 41 and the second gas diffusion layer 42 are produced using high surface area carbon fine powder, pore former, carbon paper, carbon cloth, or the like in order to provide gas permeability. Alternatively, a conductive substrate having a porous structure may be used. Further, from the viewpoint of obtaining sufficient drainage, a water repellent polymer typified by a fluororesin may be dispersed in the first gas diffusion layer and the second gas diffusion layer 42. Furthermore, from the viewpoint of obtaining sufficient electron conductivity, the first gas diffusion layer 41 and the second gas diffusion layer 42 may be made of an electron conductive material such as carbon fiber, metal fiber, or carbon fine powder.

  Further, between the first gas diffusion layer 41 and the first catalyst layer 31 and between the second gas diffusion layer 42 and the second catalyst layer 32, a water repellent polymer and carbon powder are used. A water repellent carbon layer may be provided. Thereby, water management in the membrane-electrode assembly (retention of water necessary for maintaining good characteristics of the membrane-electrode assembly and quick drainage of unnecessary water) can be performed more easily and reliably. it can.

  Next, the fuel cell 4 of the first embodiment shown in FIG. 4 will be described.

  The polymer electrolyte fuel cell 4 mainly includes the membrane-electrode assembly 3 shown in FIG. 3, a gasket 60 and a gasket 62, and a separator 50 and a separator 52.

  The gasket 60 and the gasket 62 are disposed around the membrane-electrode assembly 3 in order to prevent leakage and mixing of the fuel gas and the oxidant gas supplied to the membrane-electrode assembly 3 to the outside.

  A pair of separator 50 and separator 52 for mechanically fixing the membrane-electrode assembly 3 are disposed outside the membrane-electrode assembly 3. On the inner surface of the separator 50 that contacts the first gas diffusion layer 41 of the membrane-electrode assembly 3 (the main surface F5 on the outer side of the first gas diffusion layer 41), oxidant gas or fuel gas is applied to the membrane-electrode assembly. 3 and a gas flow path 78 is formed for carrying a gas containing the electrode reaction product and unreacted reaction gas from the reaction field to the outside of the membrane-electrode assembly 3. Further, the inner surface of the separator 52 that is in contact with the second gas diffusion layer 42 of the membrane-electrode assembly 3 (the main surface F6 outside the second gas diffusion layer 42) is supplied to the membrane-electrode assembly 3, In addition, a gas flow path 78 is formed for carrying the electrode reaction product and a gas containing unreacted reaction gas from the reaction field to the outside of the membrane-electrode assembly 3.

  Although the gas flow path 78 can be provided separately from the separator 50 and the separator 52, in the fuel cell 4 of FIG. 4, the inner surface of the separator 50 (the surface in contact with the outer main surface F <b> 5 of the first gas diffusion layer 41) and A configuration having a gas flow path 78 formed of a groove provided on the inner surface of the separator 52 (the surface in contact with the outer main surface F6 of the second gas diffusion layer 42) is employed.

  Further, the separator 50 may have a configuration in which a cooling water flow path (not shown) including a groove provided by cutting or the like is formed on the outer surface opposite to the membrane-electrode assembly 3. . Further, the separator 52 may also have a configuration in which a cooling water flow path (not shown) including a groove provided by cutting or the like is formed on the outer surface on the side opposite to the membrane-electrode assembly 3. .

In this way, the membrane-electrode assembly 3 is fixed between the pair of separators 50 and 52, and for example, fuel gas is supplied to the gas flow path 78 of the separator 50 and oxidized to the gas flow path 78 of the separator 52. By supplying the agent gas, an electromotive force of about 0.7 to 0.8 V can be generated in one fuel cell 4 when a practical current density of several tens to several hundred mA / cm ² is applied. However, normally, when a polymer electrolyte fuel cell is used as a power source, a voltage of several volts to several hundred volts is required, so in practice, the required number of fuel cells 4 are connected in series, It is used as a so-called stack (not shown). For example, a stacked body in which a plurality of fuel cells 4 are stacked is disposed between two end plates that are opposed to each other, and used as a stack that is fastened.

  Next, an example of a manufacturing method of the membrane-membrane reinforcing member assembly 1 shown in FIG. 1, the membrane-catalyst layer assembly 2 shown in FIG. 2, and the membrane-electrode assembly 3 shown in FIG. Preferred embodiments of the method for producing the membrane-membrane reinforcing member assembly, preferred embodiments of the method for producing the membrane-catalyst layer assembly of the present invention, and preferred embodiments of the method for producing the membrane-electrode assembly of the present invention ) Will be described with reference to the drawings.

  5 shows a series of steps for manufacturing the membrane-membrane reinforcing member assembly 1 shown in FIG. 1, the membrane-catalyst layer assembly 2 shown in FIG. 2, and the membrane-electrode assembly 3 shown in FIG. It is explanatory drawing which shows a part of FIG.

  The membrane-membrane reinforcing member assembly 1 shown in FIG. 1, the membrane-catalyst layer assembly 2 shown in FIG. 2, and the membrane-electrode assembly 3 shown in FIG. 3 are a series of first steps P1 shown in FIG. Through the second process P2, the third process P3, the fourth process P4, and the fifth process P5, mass production can be easily performed at low cost.

  First, using a known thin film manufacturing technique, a polymer electrolyte roll 122 around which a tape-shaped polymer electrolyte membrane 140 (a member that becomes the polymer electrolyte membrane 10 of FIG. 1 after cutting) is wound, and a tape-shaped membrane A membrane reinforcing member roll 120A wound with a reinforcing member 142A (member that becomes the first membrane reinforcing member 22 in FIG. 1 after cutting) and a tape-like membrane reinforcing member 142B (after cutting, the first membrane reinforcing member in FIG. 1) 24) and a membrane reinforcing member roll 120B wound with a member.

  Next, the membrane reinforcing member 142A and the membrane reinforcing member 142B are joined to the side end portion of the polymer electrolyte membrane 140 (first process P1). The first process P1 will be described with reference to the drawings. FIG. 6 is an explanatory diagram for explaining the operation of the first step P1 in FIG.

  As shown in FIGS. 5 and 6, the membrane reinforcing member 142A is pulled out from the roll 120A, the membrane reinforcing member 142B is pulled out from the roll 120B, the polymer electrolyte membrane 140 is pulled out from the roll 122, and these are paired with a pair of rollers 124 and 126. The membrane reinforcing member 142A and the membrane reinforcing member 142B are guided so as to be placed on the side end portions of the polymer electrolyte membrane 140 in a thermocompression bonding machine (not shown). As shown in FIG. 6, the polymer electrolyte membrane 140, the membrane reinforcing member 142A, and the membrane reinforcing member 142B are polymer electrolyte membrane 140 in the process of moving in the traveling direction D1 between the rollers 124 and 126 in the thermocompression bonding machine. The membrane reinforcing member 142A and the membrane reinforcing member 142B are joined to each other at the side end portions thereof to form a tape-like membrane-membrane reinforcing member laminate 141. Here, the width between the roll 120 </ b> A and the roll 120 </ b> B is adjusted to correspond to the size of the first catalyst layer 31.

  In the first step P1, there is no R200 portion (a portion that tends to float when tension is applied, or that is substantially perpendicular to the direction of tension) in the protective film 250 of the fuel cell described above with reference to FIG. The polymer electrolyte membrane 140, the membrane reinforcing member 142A, and the membrane reinforcing member 142B are formed in the process of moving in the traveling direction D1 between the roller 124 and the roller 126 in the thermocompression bonding machine. Generation | occurrence | production of position shift and peeling of the film | membrane reinforcement member 142B can fully be suppressed.

  Next, a membrane reinforcing member 136A (a member that becomes the second membrane reinforcing member 26 in FIG. 1 after cutting) and a membrane reinforcing member 136B (after the cutting, the second membrane reinforcing member 28 in FIG. 1) are formed on the back surface of the laminate 141. Members) (second step P2). The second process P2 will be described with reference to the drawings. FIG. 7 is an explanatory diagram for explaining the operation of the second step P2 in FIG.

  As shown in FIGS. 5 and 7, the laminated body 141 obtained in the first step P <b> 1 further advances to the area of the second step P <b> 2 in the traveling direction D <b> 1 by driving the roller 128 and the roller 130 and temporarily stops. As shown in FIG. 7, in the area where the second step P2 is performed, a base material-reinforcing member laminate in which a tape-like membrane reinforcing member 136A is laminated on a tape-like base material 137A on the back surface of the laminate 141. A roll 134A around which a body 135A is wound and a roll 134B around which a base material-reinforcing member laminate 135B in which a tape-like membrane reinforcing member 136B is laminated on a tape-like base material 137B are arranged. Yes.

  More specifically, in the roll 134A, the traveling direction D2 of the laminated body 135A drawn from the roll 134A and the traveling direction D1 of the laminated body 141 are substantially perpendicular, and the tape-shaped membrane reinforcing member 136A is the laminated body 141. It arrange | positions so that the back surface (surface in which the membrane reinforcement member 142A and the membrane reinforcement member 142B are not arrange | positioned) of this polymer electrolyte membrane 140 may be contacted. Further, in the roll 134B, the traveling direction D3 of the laminated body 135B drawn from the roll 134B and the traveling direction D1 of the laminated body 141 are substantially perpendicular, and the tape-shaped membrane reinforcing member 136B is a polymer electrolyte membrane of the laminated body 141. It arrange | positions so that the back surface (surface in which membrane reinforcement member 142A and membrane reinforcement member 142B are not arrange | positioned) 140 may be contacted.

  In this area, at the same time as the laminated body 141 is stopped, the base membrane-membrane reinforcing member laminate 135A drawn from the roll 134A and the base membrane-membrane reinforcing member laminate 135B drawn from the roll 134B are used as the membrane reinforcing member. 136A and the membrane reinforcing member 136B are stopped so as to contact the back surface of the polymer electrolyte membrane 140. Next, the pressing means (not shown) prevents the positional displacement of the contact portion between the polymer electrolyte membrane 140 and the membrane reinforcing member 136A and the contact portion between the polymer electrolyte membrane 140 and the membrane reinforcing member 136B. The material film-membrane reinforcing member laminate 135A, the base film-membrane reinforcing member laminate 135B, and the laminate 141 are fixed.

  Next, by two cutters (not shown), according to the width of the laminated body 141 (the portion of the membrane reinforcing member 136A that contacts the polymer electrolyte membrane 140 and the portion of the membrane reinforcing member 136B that contacts the polymer electrolyte membrane 140) The membrane reinforcing member 136A of the base material-membrane reinforcing member laminate 135A and the membrane reinforcing member 136B of the base membrane-membrane reinforcing member laminate 135B are cut. At this time, the cutting depth of the two cutters is a depth at which the base material 137A in the base material membrane-membrane reinforcing member laminate 135A and the base material 137B in the base material membrane-membrane reinforcing member laminate 135B are not cut. It is adjusted to. Further, the base material 137A and the base material 137B also have sufficient mechanical strength (hardness, flexibility) that is not cut by the two cutters. In this way, a laminate 143 in which the second membrane reinforcing member 26 and the second membrane reinforcing member 28 are joined to the back surface of the laminate 141 is obtained. Here, the width between the rolls 134 </ b> A and 134 </ b> B is adjusted to correspond to the size of the second catalyst layer 32. In addition, it is good also as a structure cut | disconnected by one cutter instead of two cutters.

  Further, in the second step P2, a process for sufficiently integrating 136A and 136B with the polymer electrolyte membrane 140 is performed. For example, when cutting with two cutters, a heat treatment may be further performed by a pressing means, and a process of fusing 136A and 136B to the polymer electrolyte membrane 140 may be performed. Further, for example, a pretreatment may be performed in which an adhesive is applied to the surfaces (parts to be contact surfaces) of 136A and 136B before being brought into contact with the polymer electrolyte membrane 140. When this pretreatment is performed, the above-described fusion process may be performed, or only the pressurizing process by the pressing unit may be performed without performing the fusion process. Furthermore, it is preferable that the adhesive does not deteriorate the battery characteristics. For example, a polymer electrolyte material of the same type or different type from the polymer electrolyte membrane 140 (however, having an affinity that can be sufficiently integrated with the polymer electrolyte membrane 140) (for example, the constituent material of the polymer electrolyte membrane 10 previously) A liquid in which a dispersion medium or a solvent is contained) may be used.

  In the second step P1, there is no portion of R200 (a portion that tends to float when tension is applied and is substantially perpendicular to the direction of tension) in the protective film 250 of the fuel cell described above with reference to FIG. More specifically, the second membrane reinforcing member 26 and the second membrane reinforcing member 28 joined to the back surface of the multilayer body 141 in the second step P1 are portions that are substantially perpendicular to the direction in which the tension is applied, but are adjacent to each other. Unlike the R200 portion, the matching second membrane reinforcing member 26 and second membrane reinforcing member 28 are not directly coupled to each other, and are unlikely to rise even when tension is applied. Therefore, also in the second step P1, in the process of proceeding in the traveling direction D1, it is possible to sufficiently suppress the occurrence of displacement and peeling of the second membrane reinforcing member 26 and the second membrane reinforcing member 28 with respect to the polymer electrolyte membrane 140. it can. The portion of R200 shown in FIG. 14 is easily lifted because adjacent R200 portions are directly coupled as part of the same protective film 250.

  Next, after the formation of the laminated body 143, the main surface F1A of the polymer electrolyte membrane 140 on the side where the membrane reinforcing member 142A and the membrane reinforcing member 142B of the laminated body 143 are formed (after cutting, the first main surface in FIG. The catalyst layer 190 (the one that becomes the first catalyst layer 31 in FIG. 2 after cutting) is formed on the surface that becomes F1 (third step P3). The third step P3 will be described with reference to the drawings. FIG. 8 is an explanatory diagram for explaining the operation of the third step P3 in FIG.

  As shown in FIGS. 5 and 8, the laminate 143 obtained in the second step P <b> 2 further advances to the area of the third step P <b> 3 by driving the roller 128 and the roller 130, and temporarily stops. As shown in FIG. 8, in the area where the third step P3 is performed, the laminated body 143 stopped in this area is supported from the back surface (the surface opposite to the main surface F1A of the polymer electrolyte membrane 140). A mask 186 for forming the catalyst layer 190 is disposed between the supporting means (for example, a supporting base) that is not used and the membrane reinforcing member 142A and the membrane reinforcing member 142B on the main surface F1A of the polymer electrolyte membrane 140.

  The mask 186 is provided with an opening 186A. The shape and area of the opening 186A are set so as to correspond to the shape and area of the catalyst layer 190. Further, a catalyst layer forming device 130C is disposed above the area of the third step. A catalyst layer 190 is formed on the main surface F1A of the polymer electrolyte membrane 140 corresponding to the opening 186A of the mask 186A by coating or spraying the catalyst layer forming ink on the catalyst layer forming apparatus 130C. Mechanism is provided. As this mechanism, a mechanism that is employed for forming a catalyst layer of a gas diffusion layer of a known fuel cell can be employed. For example, a mechanism designed based on a spray method, a spin coating method, a doctor blade method, a die coating method, or a screen printing method can be employed.

  Next, an example of the work flow of the third step P3 will be described in detail. First, the laminate 143 stopped in the area of the third step P3 is fixed so as to be sandwiched between the mask 186A and a support base (not shown). Next, the catalyst layer forming apparatus 130C is operated, and the polymer electrolyte membrane 140 corresponding to the opening 186A of the mask 186A is coated or sprayed from above the opening 186A of the mask 186, for example. A catalyst layer 190 is formed on the main surface F1A of the substrate, and a laminate 144 on which the catalyst layer 190 is formed is obtained. Next, after the formation of the catalyst layer 190, the mask 186A and the support base (not shown) are separated from the stacked body 144. Next, by driving the roller 128 and the roller 130, the stacked body 144 moves along the traveling direction D1.

  Next, after the formation of the laminated body 144, the main surface of the laminated body 144 on the side where the catalyst layer 190 of the polymer electrolyte membrane 140 is not formed (the surface that becomes the second main surface F2 in FIG. 2), a catalyst layer (which becomes the second catalyst layer 32 in FIG. 4 after cutting, hereinafter referred to as the second catalyst layer 32 for convenience of description) is formed (fourth step P4). The fourth step P4 will be described with reference to FIG.

As shown in FIG. 5, the laminated body 144 obtained in the third step P3 is further advanced to the area of the fourth step P4 in the traveling direction D1 by driving the roller 128 and the roller 130, and is temporarily stopped. Here, as shown in FIG. 5, the laminated body 144 is folded back at the roller 128, and the main surface F1B (not shown) on the side where the catalyst layer 190 of the polymer electrolyte membrane 140 is not formed faces upward. The main surface F1A on the side where the catalyst layer 190 of the polymer electrolyte membrane 140 is formed is inverted so as to face downward.
In the area where the fourth step P4 is performed, a support 144 (not shown) that supports the laminated body 144 stopped in this area from its back surface (main surface F1A of the polymer electrolyte membrane 140), and a polymer A mask (not shown) for forming the second catalyst layer 32 is disposed between the second membrane reinforcing member 26 and the second membrane reinforcing member 28 on the main surface F1B of the electrolyte membrane 140.

  This mask is provided with an opening (not shown) similar to the opening 186A of the mask 186 described above. The shape and area of the opening are set so as to correspond to the shape and area of the second catalyst layer 32. Furthermore, as shown in FIG. 5, a catalyst layer forming apparatus 130B having the same mechanism as the catalyst layer forming apparatus 130C described above is disposed above the area of the fourth step.

  Next, the work flow of the fourth step P4 is the same as that of the third step P3 described above. By the fourth step P4, a laminate 145 in which the second catalyst layer 32 is further formed on the laminate 144 is obtained. Next, by driving the roller 128 and the roller 130, the stacked body 145 moves along the traveling direction D1.

  Next, as shown in FIG. 5, the laminate 145 is introduced into a cutting apparatus having a cutting mechanism 132, and is cut at a preset size to obtain the membrane-catalyst layer assembly 2 shown in FIG. 5 process P5).

  It should be noted that the catalyst layer 190 and the second catalyst layer 32 are adjusted in their component composition and degree of drying so as to have appropriate flexibility, and the polymer electrolyte membrane 140 is also folded when the roller 128 and the roller 130 are folded. Measures are taken to prevent it from peeling off. Further, each time the catalyst layer 190 and the second catalyst layer 32 are formed on the polymer electrolyte membrane 140, a drying process (for example, at least one of a heating process, a blowing process, and a deaeration process) is appropriately performed. Also good.

  Next, the first gas diffusion layer 41 and the second gas diffusion layer 42 are bonded to the membrane-catalyst layer assembly 2 to obtain the membrane-electrode assembly 3 shown in FIG. More specifically, a first gas diffusion layer 41 and a second gas diffusion layer 42 having appropriate sizes corresponding to the size of the membrane-catalyst layer assembly 2 obtained after cutting the laminate 145 are prepared. Alternatively, the first gas diffusion layer 41 and the second gas diffusion layer 42 may be bonded to the membrane-catalyst layer assembly 2.

  In addition, a gas diffusion layer winding roll (not shown) in which a tape-like gas diffusion layer (for example, carbon cloth) is wound is prepared, and a bonding mechanism similar to the first step shown in FIG. The tape-like gas diffusion layer drawn out from the gas diffusion layer winding roll is integrated with the belt-like laminate 145 obtained after the fourth step P4 using the apparatus having the same, and then the same cutting as in the fifth step P5 Work may be performed to form the membrane electrode assembly 3 continuously. In this case, when the water repellent carbon layer is further formed, the water repellent carbon layer having the same mechanism as the catalyst layer forming apparatus 130C used in the third step P3 except that the water repellent carbon layer forming ink is used. A forming apparatus (not shown) may be used. In this case, the water-repellent carbon layer forming device may be disposed at a position where the water-repellent carbon layer forming ink can be applied or sprayed on the band-shaped laminate 145 or the tape-like gas diffusion layer before bonding. In the case of forming the water-repellent carbon layer, a tape-shaped gas diffusion layer roll which is continuously formed in advance at the position where the water-repellent carbon layer is set may be used.

  Note that the manufacturing process may be designed so that the operation of the second step P2 described above is performed after the operation of the third step P3. Further, the work of the third process P3 may be continuously performed after the work of the second process P2 is completed in the area of the second process P2.

  Next, the membrane-membrane reinforcing member assembly 1 shown in FIG. 1, the membrane-catalyst layer assembly 2 shown in FIG. 2, and another example of the manufacturing method of the membrane-electrode assembly 3 shown in FIG. Will be described.

  FIG. 9 is an explanatory diagram for explaining a method of manufacturing a membrane-membrane reinforcing member laminate that is a constituent member of the membrane-membrane reinforcing member assembly 1. FIG. 10 is an explanatory diagram for explaining an operation of joining two membrane-membrane reinforcing member laminates.

  First, as shown in FIG. 9, three or more tape-like membrane reinforcing members (members that become the second membrane reinforcing members 26 and 28 in FIG. 1 after cutting) 100, 102, 104, 106. A membrane-membrane reinforcing member laminate 100A having a configuration in which one main surface of the membrane 110 is arranged at regular intervals so as to be substantially parallel to each other is created. The membrane-membrane reinforcing member laminate 100A can be produced, for example, by the same method as the first step described above with reference to FIG. The interval between two adjacent ones of the three or more tape-like membrane reinforcing members 100, 102, 104, 106... Corresponds to the size of the catalyst layer (second catalyst layer 32) to be formed later. It is adjusted to.

  Next, the membrane-membrane reinforcing member laminate 100A is cut from a direction substantially perpendicular to the longitudinal direction of the tape-like membrane reinforcing member 100 (for example, in FIG. 9, a cutting line cut from such a direction is indicated by a dotted line 110A, 110B, 110C). As a result, a plurality of tape-like membrane-membrane reinforcing member laminates 108B are obtained. As shown in FIG. 9, a plurality of membrane reinforcing members (members that become the second membrane reinforcing members 26 and 28 in FIG. 1 after cutting) in the tape-like membrane-membrane reinforcing member laminate 108B are in the longitudinal direction. Are arranged so as to be substantially perpendicular to the longitudinal direction of the tape-shaped membrane-membrane reinforcing member laminate 108B of the main body. Next, the tape-like membrane-membrane reinforcing member laminate 108B thus obtained is wound into a roll (not shown).

  On the other hand, in the same manner as in the first step shown in FIG. 6, the membrane-bonded membrane-bonding member 142A and membrane-reinforcing member 142B are placed on the side ends of the tape-shaped polymer electrolyte membrane 140A. A membrane reinforcing member laminate 108A (see FIG. 10) is produced. Then, the obtained membrane-membrane reinforcing member laminate 108A is wound into a roll (not shown). The width of the membrane-membrane reinforcing member laminate 108A (width in the short direction) and the width of the membrane-membrane reinforcing member laminate 108B (width in the short direction) are adjusted so as to coincide with each other.

  Next, as shown in FIG. 10, the membrane-membrane reinforcing member laminate 108A and the membrane-membrane reinforcing member laminate 108B are joined. More specifically, the membrane-membrane reinforcing member laminate 108A and the membrane-membrane reinforcing member laminate 108B are pulled out from the respective rolls, and these are thermocompression bonding machines (not shown) having a pair of rollers 170 and rollers 172. It is guided so as to overlap. At this time, the back surface of the polymer electrolyte membrane 140A of the membrane-membrane reinforcing member laminate 108A (the surface on the side where the membrane reinforcing member is not disposed) and the back surface of the polymer electrolyte membrane 140A of the membrane-membrane reinforcing member laminate 108B (The surface on the side where the membrane reinforcing member is not disposed) is joined. Further, at this time, when the membrane-membrane reinforcing member laminate 108A and the membrane-membrane reinforcing member laminate 108B are viewed from the normal direction of the main surface of the membrane-membrane reinforcing member laminate 108A, the membrane-membrane reinforcing member laminate 108A. The membrane-membrane reinforcing member laminate 108B is overlapped so that a part of the membrane-membrane reinforcing member laminate 108B protrudes and cannot be seen.

  As shown in FIG. 10, the membrane-membrane reinforcing member laminate 108 </ b> A and the membrane-membrane reinforcing member laminate 108 are in the state described above in the process of moving in the traveling direction D <b> 1 between the roller 170 and the roller 172 in the thermocompression bonding machine. To form a tape-like membrane-membrane reinforcing member laminate 141.

  After the tape-shaped membrane-membrane reinforcing member laminate 141 is manufactured, for example, the membrane-catalyst layer assembly 2 shown in FIG. 2 and the membrane shown in FIG. The electrode assembly 3 can be manufactured.

Furthermore, the method for producing the polymer electrolyte fuel cell 4 shown in FIG. 4 using the membrane-electrode assembly 3 is not particularly limited, and a known polymer electrolyte fuel cell manufacturing technique can be employed. .
[Second Embodiment]
Next, a second embodiment of the membrane-membrane reinforcing member assembly of the present invention will be described with reference to the drawings. FIG. 11 is a perspective view showing an example of the basic configuration of the second embodiment of the membrane-membrane reinforcing member assembly of the present invention.

  The membrane-membrane reinforcing member assembly 1A of the second embodiment shown in FIG. 11 has the membrane-membrane reinforcing member assembly of FIG. 1 shown in the first embodiment except that a polymer electrolyte membrane 10A described later is mounted. It has the same configuration as the body 1.

  Next, the polymer electrolyte membrane 10A will be described. As shown in FIG. 11, in the polymer electrolyte membrane-inner reinforcing membrane complex 10A, an inner reinforcing membrane 80 is disposed between the first polymer electrolyte membrane 11 and the second polymer electrolyte membrane 12 that are arranged to face each other. The film has a three-layer structure. The first polymer electrolyte membrane 11 and the second polymer electrolyte membrane 12 are membranes having the same configuration as the polymer electrolyte membrane 10 shown in FIG. Next, the internal reinforcing film 80 shown in FIG. 11 will be described in detail with reference to FIG. FIG. 12 is an enlarged front view of an essential part showing an example of a basic configuration of the internal reinforcing membrane 80 provided in the membrane-membrane reinforcing member assembly 1A shown in FIG.

  The internal reinforcing film 80 is made of a resin film and has a plurality of openings (through holes) 82 penetrating in the thickness direction as shown in FIG. The opening 82 is filled with a polymer electrolyte having the same or different component as the polymer electrolyte membrane 11 and the polymer electrolyte membrane 12. The ratio (opening degree) of the area of the opening 82 to the main surface of the internal reinforcing film 80 is preferably 50% to 90%. When the opening degree is 50% or more, sufficient ionic conductivity can be easily obtained. On the other hand, when the opening degree is 90% or less, sufficient mechanical strength of the internal reinforcing film 80 can be easily obtained.

  Further, the inner reinforcing membrane 80 may be a stretched porous film (not shown: for example, “Gore Select (II)” manufactured by Japan Gore Tech Step Co., Ltd.). Thus, the opening 82 of the inner reinforcing membrane 80 may be very fine pores (for example, the pore diameter is several tens of μm). Even in this case, the openness (porosity) is preferably 50% to 90% for the same reason as described above.

  As the resin constituting the internal reinforcing film 80, polytetrafluoroethylene, fluoroethylene-propylene copolymer, tetrafluoroethylene-perfluoroalkoxyethylene copolymer are used from the viewpoint of chemical stability and mechanical stability. Selected from the group consisting of polyethylene, polypropylene, polyether amide, polyether imide, polyether ether ketone, polyether sulfone, polyphenylene sulfide, polyarylate, polysulfide, polyimide, polyethylene naphthalate, polyethylene terephthalate, and polyimide amide It is preferably at least one synthetic resin.

  The internal reinforcing membrane 80 is configured such that the above-described opening is obtained by containing at least one of fibrous reinforcing particles and spherical reinforcing particles in the polymer electrolyte membrane 10 described above. It is good also as a structure which provided the part. Examples of the constituent material of the reinforcing body particles include a resin constituting the internal reinforcing film 80.

The manufacturing method of the polymer electrolyte membrane 10A is not particularly limited, and can be manufactured using a known thin film manufacturing technique. The membrane-membrane reinforcing member assembly 1A can be manufactured by the same method as the membrane-membrane reinforcing member assembly 1 described above except that the polymer electrolyte membrane 10A is used.
[Third Embodiment]
The third embodiment of the present invention is to manually perform the second step P2 shown in FIG. 7 in the method for manufacturing the membrane-membrane reinforcing member assembly 1 of the first embodiment. That is, in the present embodiment, in FIG. 7, the other main surface of the laminate 141 formed by attaching the membrane reinforcing member 142 </ b> A and the membrane reinforcing member 142 </ b> B to the side end portion of one main surface of the polymer electrolyte membrane 140, The tape-like membrane reinforcing member 136A and the tape-like membrane reinforcing member 136B are manually cut and pasted to a predetermined length. Others are the same as in the first embodiment. Moreover, it can replace with the polymer electrolyte membrane 10 of 1st Embodiment, and can also use 10 A of polymer electrolyte membrane-internal reinforcement membrane composites of 2nd Embodiment.

  According to this embodiment, at least the laminate 141, the membrane-catalyst layer assembly 2, and the membrane-electrode assembly 3 can be mass-produced, and the manufacturing cost can be reduced as compared with the conventional case. Can do.

EXAMPLES Hereinafter, although an Example and a comparative example are given and this invention is demonstrated in more detail, this invention is not limited to a following example at all.
Example 1
In this example, first, a membrane-membrane reinforcing member assembly of the present invention having the structure shown in FIG. 1 was produced.

  The first membrane reinforcing members 22 and 24 and the second membrane reinforcing members 26 and 28 are provided on both sides of the polymer electrolyte membrane 10 (a commercially available polymer electrolyte membrane made of perfluorocarbon sulfonic acid, 150 mm × 150 mm, thickness: 40 μm). These are arranged at the same positions as shown in FIG.

  The first membrane reinforcing members 22 and 24 and the second membrane reinforcing members 26 and 28 were tape-shaped thin films (thickness: 20 μm) made of PEN (polyethylene naphthalate).

  Next, the membrane-catalyst layer assembly of the present invention having the structure shown in FIG. 2 was produced using the membrane-membrane reinforcing member assembly obtained as described above.

  A catalyst-supporting carbon (TEC10E50E manufactured by Tanaka Kikinzoku Kogyo Co., Ltd., 50% by mass of Pt) obtained by supporting platinum particles as an electrode catalyst on carbon powder, and a polymer electrolyte solution having hydrogen ion conductivity (Asahi Glass ( Flemion) was dispersed in a mixed dispersion medium (mass ratio 1: 1) of ethanol and water to prepare a cathode forming ink.

  Further, a catalyst-supporting carbon (TEC61E54 manufactured by Tanaka Kikinzoku Kogyo Co., Ltd.) in which platinum ruthenium alloy (platinum: ruthenium = 1: 1.5 molar ratio (substance ratio)) particles as an electrode catalyst are supported on carbon powder. 50% by mass of Pt—Ru alloy) and a polymer electrolyte solution having hydrogen ion conductivity (Flemion manufactured by Asahi Glass Co., Ltd.) in a mixed dispersion medium (mass ratio 1: 1) of ethanol and water. An ink for forming an anode catalyst layer was prepared by dispersing.

The obtained cathode catalyst layer forming ink was applied to one side of the above-mentioned polymer electrolyte membrane by a spray method to form a cathode catalyst layer having a platinum loading of 0.6 mg / cm ² and dimensions of 140 mm × 140 mm. It was formed so as to be arranged at a position similar to the position shown in FIG.

Furthermore, the obtained ink for forming an anode catalyst layer was applied to the surface of the polymer electrolyte membrane opposite to the surface on which the cathode catalyst layer was formed by a spray method, so that the platinum loading was 0.35 mg / cm ^2. The anode catalyst layer having a size of 140 mm × 140 mm was formed so as to be arranged at the same position as that shown in FIG.

  By forming the anode catalyst layer and the cathode catalyst layer in this way, a membrane-catalyst layer assembly was formed.

  Next, using the membrane-catalyst layer assembly obtained as described above, a membrane-electrode assembly having the structure shown in FIG. 3 was produced.

  In order to form a gas diffusion layer, carbon paper having a size of 200 mm × 200 mm and a thickness of 100 μm was impregnated with an aqueous dispersion containing a fluororesin, and then dried to impart water repellency to the carbon cloth (repellency). Water treatment).

  Subsequently, a water repellent carbon layer was formed on one surface (entire surface) of the carbon paper after the water repellent treatment. Conductive carbon powder (Denka Black (trade name) manufactured by Denki Kagaku Kogyo Co., Ltd.) and an aqueous solution (D-1 manufactured by Daikin Industries, Ltd.) in which fine powder of polytetrafluoroethylene (PTFE) is dispersed. By mixing, an ink for forming a water-repellent carbon layer was prepared. This water repellent carbon layer forming ink was applied to one surface of the carbon paper after the water repellent treatment by a doctor blade method to form a water repellent carbon layer. At this time, a part of the water-repellent carbon layer was embedded in the carbon paper.

  Thereafter, the carbon paper after the water repellent treatment and the formation of the water repellent carbon layer was fired at 350 ° C., which is a temperature equal to or higher than the melting point of PTFE, for 30 minutes. Finally, the central portion of the carbon paper was cut with a punching die to obtain a gas diffusion layer with dimensions of 142.5 mm × 142.5 mm.

Next, the membrane-catalyst layer assembly is composed of two gas diffusion layers so that the central portion of the water-repellent carbon layer of the gas diffusion layer obtained as described above is in contact with the cathode catalyst layer and the anode catalyst layer. Each of the two gas diffusion layers is arranged at the same position as shown in FIG. 3 by sandwiching and thermocompressing the whole with a hot press machine (120 ° C., 30 minutes, 10 kgf / cm ² ). Thus, the membrane-electrode assembly of the present invention was obtained.

  Finally, using the membrane-electrode assembly of the present invention obtained as described above, a polymer electrolyte fuel cell of the present invention (unit cell 1) having the structure shown in FIG. 4 was produced.

The membrane electrode assembly is sandwiched between a separator plate having a gas flow path for supplying fuel gas and a cooling water flow path and a separator plate having a gas flow path for supplying oxidant gas and a cooling water flow path. Between the cathode and the anode, a fluororubber gasket was arranged to obtain a single cell (polymer electrolyte fuel cell of the present invention) having an effective electrode area (effective electrode area of the anode or cathode) of 196 cm ² . .
<< Comparative Example 1 >>
Instead of the first membrane reinforcing members 22 and 24 and the second membrane reinforcing members 26 and 28, the frame-shaped protective film 220 and protective film 240 shown in FIG. 13 (here, both are made of the same PEN as in Example 1). A membrane-reinforcing member assembly, a membrane-catalyst layer assembly, a membrane-electrode assembly, and a unit cell (unit cell 2) were prepared in the same manner as in Example 1 except that the above were disposed.
[Evaluation test]
(1) Aging process (activation process)
The unit cell 1 and the unit cell 2 obtained in Example 1 and Comparative Example 1 are controlled to 64 ° C., hydrogen gas is supplied as a fuel gas to the anode-side gas flow channel, and air is supplied to the cathode-side gas channel. Each supplied. At this time, the hydrogen gas utilization rate was set to 70%, the air utilization rate was set to 55%, and the dew points of hydrogen gas and air were each humidified so as to be about 64 ° C., and then supplied to the unit cell. Then, aging was performed by operating the cell at a current density of 0.2 A / cm ² for 12 hours.
(2) Battery output characteristic evaluation test 1
About the single cell of Example 1 and Comparative Example 1, the rated durability test performed on the conditions close | similar to the actual driving | operation of a fuel cell was done.

In the rated durability test, the current density was 0.16 A / cm ² , and the mixed gas of hydrogen and carbon dioxide (volume ratio 3: 1) was set so that the hydrogen gas utilization rate would be 75% in the gas flow path on the anode side. ) Was operated under the same conditions as the above aging, and the output voltage after 12 hours was recorded.
(3) Battery output characteristic evaluation test 2
For the single cells of Example 1 and Comparative Example 1, accelerated durability tests were performed in which the deterioration of the membrane electrode assembly was accelerated and the life could be judged in a shorter time.

  In the accelerated durability test, the unit cell 1 and the unit cell 2 obtained in Example 1 and Comparative Example 1 were controlled at 90 ° C. under the same conditions as the battery output characteristic evaluation test 1 (rated durability test). Each cell was operated and the output voltage after 12 hours was recorded. In addition, the 90 degreeC control of the cell 1 and the cell 2 was performed using the heater for heating.

表１に示した結果から明らかなように、実施例１は、比較例１と同等の電池出力特性を有することが確認できた。

As is clear from the results shown in Table 1, it was confirmed that Example 1 had the same battery output characteristics as Comparative Example 1.

  As mentioned above, although embodiment of this invention was described in detail, this invention is not limited to the said embodiment.

  For example, in the embodiment of the present invention described above, the outer peripheral edge (edge) of the membrane reinforcing member (for example, the first membrane reinforcing members 22 and 24 shown in FIG. 1) is the polymer electrolyte membrane (for example, FIG. 1). (Polymer electrolyte membrane 10) shown in FIG. 5 is aligned with the peripheral edge (edge) (when viewed from the substantially normal direction of the main surface of the polymer electrolyte membrane, the outer edge of the membrane reinforcing member and the polymer electrolyte) The embodiment in which the edges of the membranes overlap and the edges of the polymer electrolyte membrane protrude and cannot be seen has been described. However, the present invention is not limited to this, and in the present invention, for example, the present invention The edge of the membrane reinforcing member may be entirely or partially protruded from the edge of the polymer electrolyte membrane as long as the above effect is obtained. All than the edge of the member It may have or partially protruding Configurations.

  The membrane-reinforcing member assembly, membrane-catalyst layer assembly, and membrane-electrode assembly of the present invention are useful as parts of a polymer electrolyte fuel cell capable of mass production.

  The polymer electrolyte fuel cell of the present invention is expected to be suitably used as a main power source or auxiliary power source for a moving body such as an automobile, a distributed (on-site) power generation system (home cogeneration system), and the like. The

It is a perspective view which shows an example of the basic composition of 1st Embodiment of the membrane-membrane reinforcement member assembly of the present invention. 1 is a perspective view showing an example of a basic configuration of a membrane-catalyst layer assembly (first embodiment of the membrane-catalyst layer assembly of the present invention) in which a catalyst layer is further arranged on the membrane-membrane reinforcing member assembly 1 shown in FIG. FIG. FIG. 3 is a perspective view showing an example of a basic configuration of a membrane-electrode assembly (first embodiment of the membrane-electrode assembly of the present invention) in which a gas diffusion layer is further arranged on the membrane-catalyst layer assembly 2 shown in FIG. 2. is there. FIG. 4 is a cross-sectional view showing an example (unit cell portion) of a basic configuration of a fuel cell (first embodiment of the polymer electrolyte fuel cell of the present invention) including the membrane-electrode assembly 3 shown in FIG. 3. Part of a series of steps for manufacturing the membrane-membrane reinforcing member assembly 1 shown in FIG. 1, the membrane-catalyst layer assembly 2 shown in FIG. 2, and the membrane-electrode assembly 3 shown in FIG. It is explanatory drawing shown roughly. It is explanatory drawing for demonstrating the operation | work of the 1st process P1 in FIG. It is explanatory drawing for demonstrating the operation | work of the 2nd process P2 in FIG. It is explanatory drawing for demonstrating the operation | work of the 3rd process P3 in FIG. It is explanatory drawing for demonstrating the manufacturing method of the membrane-membrane reinforcement member laminated body used as the structural member of the membrane-membrane reinforcement member assembly 1. FIG. It is explanatory drawing for demonstrating the operation | work which joins a membrane-membrane reinforcement member laminated body. It is a perspective view which shows an example of the basic composition of 2nd Embodiment of the membrane-membrane reinforcement member assembly of this invention. FIG. 12 is an enlarged front view of an essential part showing an example of a basic configuration of an internal reinforcing membrane 80 provided in the membrane-membrane reinforcing member assembly 1A shown in FIG. 3 is an exploded perspective view of a main part for explaining the positional relationship between a solid polymer electrolyte membrane and a fluororesin sheet (protective membrane) in a polymer electrolyte fuel cell described in Patent Document 1. FIG. It is explanatory drawing which shows an example of the manufacturing method generally assumed when it intends to mass-produce the polymer electrolyte fuel cell of patent document 1 using the manufacturing technique of a well-known thin film laminated body.

Explanation of symbols

    DESCRIPTION OF SYMBOLS 1, 1A ... Membrane-membrane reinforcement member assembly, 2, Membrane-catalyst layer assembly, 3 ... Membrane-electrode assembly, 4 ... Fuel cell, 10 ... Polymer electrolyte membrane, 10A ... Polymer electrolyte-inner reinforcing membrane composite, 11 ... first polymer electrolyte membrane, 12 ... second polymer electrolyte membrane, 22, 24 ... first membrane reinforcing member, 26, 28 ... 2nd membrane reinforcement member, 31 ... 1st catalyst layer, 32 ... 2nd catalyst layer, 41 ... 1st gas diffusion layer, 42 ... 2nd gas diffusion layer, 50, 52 ... Separator, 60, 62 ... Gasket, 70, 72, 74, 76 ... Gap, 78 ... Gas flow path, 80 ... Internal reinforcing membrane, 82 ... Opening, 120A, 120B, 122, 134A, 134B ... rolls, 124, 126 ... thermocompression bonding machines, 128, 130 ... rollers, 130B, 13 C ... Catalyst layer coating machine, 132 ... Cutting machine, 135A, 135B ... Base material-membrane reinforcing member laminate, 136A, 136B ... Membrane reinforcing member, 137A, 137B ... Base material 138 ... membrane reinforcing member cut surface, 140 ... polymer electrolyte membrane, 141 ... membrane-membrane reinforcing member laminate, 142A, 142B ... membrane reinforcing members, 143, 144, 145 ... Laminate, 186 ... Mask, 186A ... Opening, 190 ... Catalyst layer, D1, D2, D3 ... Traveling direction, F1 ... First main surface, F2 ... Second main Surface, F3 ... main surface of the first catalyst layer, F4 ... main surface of the second catalyst layer, F5 ... main surface of the first gas diffusion layer, F6 ... main surface of the second gas diffusion layer Surface, F1A, F22, F24, F26, F28 ... main surface, P1 ... first step, P2 ... second step, P3 ... third step, P4 ... fourth step, P ... fifth step.

Claims (6)

A polymer electrolyte membrane having a pair of first main surface and second main surface facing each other and having a substantially rectangular shape;
It is arranged in a portion along a pair of opposite sides of the four sides of the first main surface, has a main surface smaller than the first main surface, and exhibits a film-like shape that can be wound. A pair of first membrane reinforcing members for reinforcing the polymer electrolyte membrane;
It is arranged in a portion along a pair of opposite sides of the four sides of the second main surface, has a main surface smaller than the second main surface, and exhibits a film-like shape that can be wound. A pair of second membrane reinforcing members for reinforcing the polymer electrolyte membrane;
Have
The one set of sides of the first main surface where the pair of first membrane reinforcing members are arranged, and the one set of sides of the second main surface where the pair of second membrane reinforcing members are arranged And are almost orthogonal,
The pair of first membrane reinforcing members and the pair of second membrane reinforcing members are alternately arranged on the first main surface and the second main surface along the four sides of the polymer electrolyte membrane as a whole. Extending so as to exist and arranged so as to sandwich the four corner portions of the polymer electrolyte membrane ,
The first membrane reinforcing member and the second membrane reinforcing member are polyethylene naphthalate, polytetrafluoroethylene, polyethylene terephthalate, fluoroethylene-propylene copolymer, tetrafluoroethylene-perfluoroalkoxyethylene copolymer, polyethylene, polypropylene. And at least one synthetic resin selected from the group consisting of polyetheramide, polyetherimide, polyetheretherketone, polyethersulfone, polyphenylene sulfide, polyarylate, polysulfide, polyimide, and polyimideamide. A membrane-membrane reinforcing member assembly.   The membrane-membrane reinforcing member assembly according to claim 1, further comprising an internal reinforcing membrane disposed in the polymer electrolyte membrane and having a through hole serving as an ion conduction path. The membrane-membrane reinforcing member assembly according to claim 1 or 2 ,
A first catalyst layer disposed in at least a part of a region of the first main surface of the polymer electrolyte membrane of the membrane-membrane reinforcing member assembly where the first membrane reinforcing member is not disposed;
A second catalyst layer disposed in at least a part of a region of the second main surface of the polymer electrolyte membrane of the membrane-membrane reinforcing member assembly where the second membrane reinforcing member is not disposed; A membrane-catalyst layer assembly comprising: The membrane-catalyst layer assembly according to claim 3 ,
A first gas diffusion layer arranged to cover the first catalyst layer of the membrane-catalyst layer assembly;
And a second gas diffusion layer disposed so as to cover the second catalyst layer of the membrane-catalyst layer assembly. The first gas diffusion layer is disposed so as to cover the first catalyst layer and at least a part of the first membrane reinforcing member,
The membrane-electrode assembly according to claim 4 , wherein the second gas diffusion layer is disposed so as to cover the second catalyst layer and at least a part of the second membrane reinforcing member. The membrane-electrode assembly according to claim 4 or 5 and a peripheral portion of a main surface of the membrane-electrode assembly where the first gas diffusion layer is formed are disposed so as to surround the first gas diffusion layer. A frame-shaped first gasket, and a groove-like flow path of one reaction gas is formed on one main surface, and the one main surface is the first gas diffusion layer of the membrane-electrode assembly and the first A plate-like first separator disposed so as to be in contact with the gasket and a peripheral portion of a main surface of the membrane-electrode assembly on which the second gas diffusion layer is formed so as to surround the second gas diffusion layer A frame-shaped second gasket disposed on the first main surface, and a groove-like flow path for the other reactive gas on one main surface, the one main surface being the second gas diffusion layer of the membrane-electrode assembly A plate-like second separator disposed so as to come into contact with the second gasket, and polymer electrolysis Fuel cell.

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