JP2005063780A - Electrolyte membrane. electrolyte membrane complex, manufacturing method of electrolyte membrane complex, electrolyte membrane/electrode assembly for fuel cell, manufacturing method of electrolyte membrane/electrode assembly for fuel cell, and fuel cell - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide an electrolyte membrane for manufacturing an electrode having an intended pattern with high quality and with productivity of high efficiency. <P>SOLUTION: Masking members (12, 13) having holes (12a, 13a) hollowed out in an intended shape of an electrode are stuck by themselves or through a fine adhesive on at least one surface of the electrolyte film (11) for a fuel cell before sticking the electrode. <P>COPYRIGHT: (C)2005,JPO&NCIPI

Description

  The present invention relates to an electrolyte membrane, an electrolyte membrane composite, a method of manufacturing an electrolyte membrane composite, an electrolyte membrane / electrode assembly (MEA) for a fuel cell, a method of manufacturing an electrolyte membrane / electrode assembly (MEA) for a fuel cell, and a fuel cell. About. Specifically, the present invention relates to an electrolyte membrane and an electrode of a solid polymer electrolyte membrane fuel cell (PEFC).

  Conventionally, the electrode formation of a polymer electrolyte fuel cell is carried out by applying a liquid electrode ink directly on an electrolyte membrane and drying it to form an electrode, or by applying a release treatment to a fluorine-based film or a polyester-based film. After the ink is applied and dried, the electrode is formed by heating and pressurizing and transferring to the electrolyte membrane, generally the liquid electrode ink is dried on one side of a gas diffusion layer called carbon paper, and the electrolyte membrane or There is a method of thermocompression bonding to an electrolyte membrane in which an electrode is formed in advance in a desired thickness (for example, see Patent Document 1). On the other hand, a method of applying a powdered electrode material made of a mixture of a carbon carrying a catalyst platinum or the like and an electrolyte solution instead of a liquid electrode ink to an electrolyte membrane or the like has been attempted as a measure for future total VOC.

Japanese National Patent Publication No. 9-501535 Japanese Patent Laid-Open No. 4-135670 JP-A-4-176363 JP-A-4-210273 Japanese Patent Laid-Open No. 5-76819 (refer to FIG. 3 in particular) DuPont, Product Information, "DuPont Nafion PFSA Membranes NR-111 and NR-112", NAE201 (Nov2002)

As a method for producing an electrolyte membrane / electrode assembly for a fuel cell, there is a method in which liquid electrode ink is directly applied to the electrolyte membrane. This method is good because when the liquid electrode ink is applied directly to the electrolyte membrane so that cracks and pinholes do not occur in the coating film, the cost and cost can be reduced because the adhesion and performance aspects and processes can be reduced. Has been.
However, when the liquid electrode ink is directly applied to the electrolyte membrane, there are the following two problems.

  The first problem is that the electrolyte membrane instantaneously wets or swells when it comes into contact with water or alcohol solvent, which is the solvent of the liquid electrode ink, or moisture in the air, and the electrolyte membrane is left as it is. Then, it will be deformed as soon as it does not stop the prototype.

The second problem is that the wet film thickness of the liquid electrode ink to be applied to the electrolyte membrane is large. The solid content contained in the liquid electrode ink is about 5 to 15 percent. The dry weight of the electrolyte membrane / electrode assembly for a fuel cell varies depending on the content of a catalyst such as platinum, but is generally in the range of about 0.5 to 6 mg / cm ² , and more often about 0. it is in the range of 8~3mg / cm ^2. When the wet film thickness of the liquid electrode ink is converted from these, the electrode ink has a wet film thickness of approximately 50 to 600 μm. Even in a general painting operation, when a paint having such a large wet film thickness is applied on a substrate, it is a collection of bubbles such as dripping, cracking, blistering of a blistering phenomenon, and microbubbles. Therefore, removing the armpit phenomenon accompanied by pinholes is a difficult task.

  As a measure for solving the above problem, the concentration of the electrode ink is increased before the electrode ink reaches the electrolyte membrane, that is, as much solvent as possible is required until the electrode ink reaches the electrolyte membrane. Volatilization from electrode ink. For this purpose, instead of using conventional methods such as roll coating, die coating with slot nozzles, curtain coating, and screen printing, which are typical examples of liquid film coating, the electrode ink is made into droplets and as fine particles as possible in the atmosphere. It is important to select a spray method that is applied while increasing contact with the substrate. However, in the spray method, since the liquid is applied in the form of particles, the particles are likely to scatter and it is impossible to form an electrode pattern having a desired sharp outline. Therefore, the use of the masking member was an absolute condition.

For example, if the methods described in Patent Document 2, Patent Document 3 and Patent Document 4 are used, it is simple as an automatic masking method in the general coating field, but in the application of electrode ink, it adheres to the masking member on the line. It was necessary to remove the dried electrode ink with a solvent. Because of the catalyst, there was a danger of ignition when heated and contact with the solvent. A large amount of waste liquid or waste containing electrode ink generated in these operations is sent to a catalyst manufacturer or the like, and platinum is reused. Unnecessary cleaning solvent is used and the solvent cost is high, and the cost for the operator to clean the masking member after the operation is also generated. Since the solvent is handled as a dangerous substance and the catalyst has the above-mentioned problems, the transportation means is also expensive.
When spraying electrode ink or / and powdered electrode material on the electrolyte membrane, the masking member floats and the electrode ink or / and powdered electrode material is placed in the gap between the masking member and the electrolyte membrane. There is also the problem of being soaked. In such a case, there arises a problem that an electrode having a desired pattern cannot be formed accurately.

  The present invention has been made in view of the above-described problems. An electrolyte membrane, an electrolyte membrane composite, and an electrolyte membrane composite for manufacturing an electrode having a desired pattern with high quality and high productivity. It is an object to provide a manufacturing method, an electrolyte membrane / electrode assembly for a fuel cell, a manufacturing method of an electrolyte membrane / electrode assembly for a fuel cell, and a fuel cell.

In order to solve the above-described problems, the present invention employs the following electrolyte membrane.
That is, the electrolyte membrane was formed by laminating a masking member having holes perforated in a desired electrode shape on at least one surface of the electrolyte membrane for a fuel cell before application of an electrode.
By setting it as such a structure, a clearance gap cannot be made between electrolyte membrane and a masking member, and the electrode of a desired shape can be formed accurately.
In addition, it is not necessary to separately load the masking member into the coating apparatus, and an electrode having a desired shape (pattern) can be accurately manufactured only by loading the electrolyte membrane according to the present invention into the coating apparatus.
Furthermore, according to the present invention, the electrode ink that adheres to the masking member and is dried is wound up together with the masking member, so that the wound-up masking member is transported to the catalyst manufacturer and platinum is reused. Therefore, a cleaning solvent and a cleaning process for cleaning the masking member can be eliminated.

You may laminate | stack the masking member which has the hole hollowed in the substantially similar desired electrode shape on both surfaces of an electrolyte membrane.
The masking member may be attached to the electrolyte membrane through self-adhesion or a slight adhesive.
The electrolyte membrane and / or the masking member may be a web, and the electrolyte membrane may be a roll stock.
The electrolyte membrane may be cut into a sheet.
A gas barrier sheet or web may be laminated on at least one masking member.
The thickness of the masking member may be substantially the same as or thicker than the thickness of the electrode formed in the subsequent process.
The electrolyte membrane may be wrapped with a gas barrier packaging material.

Further, the fuel cell electrolyte membrane / electrode assembly of the present invention is obtained by applying or filling electrode ink or / and powdered electrode material to the electrolyte membrane through the holes of the masking member of the fuel cell electrolyte membrane described above, and then masking. It was manufactured by peeling off the member.
By using an electrolyte membrane for fuel cells on which a masking member was laminated, an electrolyte membrane / electrode assembly for fuel cells formed with high productivity and high accuracy could be obtained.
The electrode ink or / and the powdered electrode material may be fixed to the electrolyte membrane.
In particular, the electrode ink or / and the powdered electrode material may be fixed to the electrolyte membrane by drying, heating or / and pressing.
A fuel cell may be manufactured using the fuel cell electrolyte membrane / electrode assembly described above.

The electrolyte membrane composite of the present invention comprises an electrolyte membrane and a masking member provided with a plurality of holes, and the masking member is detachably attached to one surface of the electrolyte membrane.
The hole may be formed in the shape of the fuel electrode of the fuel cell.
The electrolyte membrane composite may further include a gas barrier sheet.
The electrolyte membrane composite may further include a masking member that is detachably attached to the other surface of the electrolyte membrane.
The gas barrier sheet is preferably attached to the masking member or the electrolyte membrane so as to be peeled off.
The masking member and the gas barrier sheet may be made of a self-adhesive material, and may be attached to the electrolyte membrane in a peelable manner without using an adhesive.
The electrolyte membrane composite may be wound into a roll stock.
The roll stock of the electrolyte membrane composite is preferably wrapped in a gas barrier packaging material.

The method for producing an electrolyte membrane composite comprising an electrolyte membrane and a masking member according to the present invention comprises a step of forming a hole having a desired shape in the masking member, and a step of bonding the masking member and the electrolyte membrane thereafter.
Further, another method for producing an electrolyte membrane composite comprising an electrolyte membrane and a masking member according to the present invention includes a step of bonding the masking member and the electrolyte membrane, and then a step of opening a hole of a desired shape in the masking member. It consists of.

A method of manufacturing an electrolyte membrane / electrode assembly for a fuel cell according to the present invention includes a step of rotatably installing a roll stock of an electrolyte membrane composite comprising an electrolyte membrane and a masking member provided with a plurality of holes, Drawing the electrolyte membrane composite from the substrate, applying the electrode ink or powdered electrode material to the electrolyte membrane through the plurality of holes in the masking member while transporting the electrolyte membrane composite, or laminating them, and It consists of the process of making it adhere to an electrolyte membrane, and the process of peeling a masking member from an electrolyte membrane. In particular, when a powdered electrode material is used, it is preferable to employ a thermocompression bonding method for fixing to the electrolyte membrane.
Another method for producing an electrolyte membrane / electrode assembly for a fuel cell according to the present invention is a roll stock of an electrolyte membrane composite comprising an electrolyte membrane, a masking member provided with a plurality of holes, and a gas barrier sheet. A step of pulling out the electrolyte membrane composite from the roll stock, a step of peeling off the gas barrier sheet, and an electrode ink on the electrolyte membrane through the plurality of holes of the masking member while transporting the electrolyte membrane composite. Or it consists of the process of apply | coating a powder-form electrode material or laminating them, the process of adhering them to an electrolyte membrane, and the process of peeling a masking member from an electrolyte membrane.
Furthermore, another method for manufacturing an electrolyte membrane / electrode assembly for a fuel cell according to the present invention is a first method in which an electrolyte membrane and a plurality of holes are provided on the first surface of the electrolyte membrane. A step of rotatably installing a roll stock of an electrolyte membrane composite comprising a masking member and a second masking member attached to the second surface of the electrolyte membrane and provided with a plurality of holes; A step of drawing out the membrane composite, and a step of applying an electrode ink or a powdered electrode material to the first surface of the electrolyte membrane through a plurality of holes of the first masking member while transporting the electrolyte membrane composite, or laminating them A step of fixing them to the electrolyte membrane, a step of peeling the first masking member from the electrolyte membrane, a step of inverting the electrolyte membrane and the second masking member, and an electrolyte membrane And applying the electrode ink or powdered electrode material to the second surface of the electrolyte membrane through the plurality of holes of the second masking member while conveying the second masking member, or laminating them, and applying them to the electrolyte membrane It comprises a step of fixing and a step of peeling the second masking member from the electrolyte membrane.
Furthermore, a method of manufacturing an electrolyte membrane / electrode assembly for a fuel cell according to the present invention includes a step of installing a sheet of an electrolyte membrane composite comprising an electrolyte membrane and a masking member provided with at least one hole; Applying or filling an electrode ink or / and powdered electrode material into the electrolyte membrane through at least one hole of the masking member, or laminating them; fixing the mask material to the electrolyte membrane; And a step of peeling from the film.
Furthermore, another method of manufacturing the fuel cell electrolyte membrane / electrode assembly according to the present invention is to provide a powdered electrode material through a plurality of holes in the first masking member and the second masking member laminated on both sides of the electrolyte membrane. The filling or coating process, the pressure bonding with a roll or the like, the process of increasing the bulk density by vibration, deaeration under vacuum, or a combination thereof, and the process is repeated as necessary. It consists of a process, a process of heating or / and press-bonding to the electrolyte membrane when the desired film thickness is reached, and a process of peeling the first and second masking members from the electrolyte film.
The method for producing an electrolyte membrane / electrode assembly for a fuel cell may include a step of cutting the electrolyte membrane.

The electrolyte membrane / electrode assembly for a fuel cell according to the present invention is manufactured by the above-described method for manufacturing an electrolyte membrane / electrode assembly for a fuel cell.
A fuel cell may be manufactured using the fuel cell electrolyte membrane / electrode assembly described above.

According to the present invention, electrode ink or powdered electrode material can be accurately applied to the electrolyte membrane in a desired pattern to increase the productivity of fuel cell electrode formation, which is particularly useful.
According to the present invention, there is no gap between the electrolyte membrane and the masking member, and an electrode having a desired shape can be accurately formed.
In addition, it is not necessary to separately load the masking member into the coating apparatus, and an electrode having a desired shape (pattern) can be accurately manufactured only by loading the electrolyte membrane according to the present invention into the coating apparatus.
Furthermore, according to the present invention, the electrode ink that adheres to the masking member and is dried is wound up together with the masking member, so that the wound-up masking member is transported to the catalyst manufacturer and platinum is reused. Therefore, a cleaning solvent and a cleaning process for cleaning the masking member can be eliminated.

  Hereinafter, the present invention will be described based on preferred embodiments with reference to the drawings. However, the dimensions, materials, shapes, relative arrangements, and the like of the components described in the following embodiments are not intended to limit the scope of the present invention only to those unless otherwise specified. Absent.

(Electrolyte membrane composite)
FIG. 1 is a perspective view of an electrolyte membrane composite 1 according to the present invention. FIG. 2 is an exploded view of the electrolyte membrane composite 1.

The electrolyte membrane composite 1 includes an electrolyte membrane 11, a masking member 12 attached to the first surface 11 a of the electrolyte membrane 11, and a masking member 13 attached to the second surface 11 b of the electrolyte membrane 11. The electrolyte membrane 11 has a property of passing only ions without passing electrons, and is used in a polymer electrolyte fuel cell. The electrolyte membrane 11 is a solid polymer electrolyte membrane, for example, an electrolyte membrane using a perfluorosulfonic acid polymer, “NAFION” (registered trademark) of DuPont, USA, an electrolyte membrane using an aromatic hydrocarbon engineering plastic, Examples include an electrolyte membrane using carbon-based fullerene (C ₆₀ ) as a constituent material, and an electrolyte membrane in which an electrolyte is formed in countless small holes provided in a polyester film. The masking members 12 and 13 are a sheet-like member, a film-like member, or a web made of paper, plastic, preferably a polyvinyl chloride material. Although the materials for the electrolyte membrane and the masking member have been exemplified, the present invention is not construed as being limited to these materials.

  The masking members 12 and 13 are provided with a plurality of holes 12a and 13a having a predetermined shape. The plurality of holes 12a and 13a are provided to form a fuel electrode of the fuel cell. In other words, the predetermined shape may correspond to the shape of the fuel electrode. The thickness of the masking members 12 and 13 is approximately the same as or greater than the thickness of the fuel electrode. This is because if the thickness of the masking members 12 and 13 is thinner than the thickness of the fuel electrode, the applied electrode ink leaks from the hole and it becomes difficult to form the fuel electrode.

  The masking members 12 and 13 are attached to the electrolyte membrane 11 so that they can be peeled off from the electrolyte membrane 11. The masking members 12 and 13 are made of a slight adhesive approved by the electrolyte membrane supplier so that the electrolyte membrane 11 is not damaged when being peeled off, and the electrolyte membrane 11 is not contaminated. It is good to affix on the electrolyte membrane 11. FIG. Alternatively, the masking members 12 and 13 may be a film coated with a pressure sensitive adhesive such as a cellophane tape, and may be attached to the electrolyte membrane 11. Alternatively, the masking members 12 and 13 may be self-adhesive films having a property of adhering without using an adhesive, and the self-adhesive films may be attached to the electrolyte membrane 11. Usually, a hole having a desired pattern may be punched through a form supplied from an electrolyte membrane supplier, for example, a backing film or a cover sheet laminated on both sides of DuPont's Nafion (registered trademark). The Nafion backing film and cover sheet are described in Non-Patent Document 1.

(Storage method)
When the electrolyte membrane 11 is exposed to the outside air, it absorbs moisture and swells. Therefore, it is desirable to store the electrolyte membrane 11 while blocking it from the outside air.
FIG. 3 is a diagram showing a state in which the electrolyte membrane composite 1 wound in a roll shape is wrapped with the packaging material 20. By sealing the roll stock of the electrolyte membrane composite 1 with the packaging material 20, the electrolyte membrane 11 can be stored from outside air. The packaging material 20 is preferably a water vapor barrier material film.

FIG. 4 is a diagram showing a gas barrier sheet 14 attached to one surface of the electrolyte membrane composite 1. The gas barrier sheet 14 is stuck on the masking member 12 so as to be peeled off with a slight adhesive. When the gas barrier sheet 14 is made of a self-adhesive material, the gas barrier sheet 14 can be attached to the masking member 12 without using an adhesive.
As shown in FIG. 5, the electrolyte membrane composite 1 is surrounded by the gas barrier sheet 14 by winding the electrolyte membrane composite 1 so that the gas barrier sheet 14 is outside. Thereby, even if it does not package with a gas shielding material, it can be set as the roll stock of the electrolyte membrane composite 1 by which gas shielding was carried out. Furthermore, if it is wrapped with the gas shielding packaging material 20, the gas shielding performance can be improved.

  The gas barrier sheet 14 may be attached to both surfaces of the electrolyte membrane composite 1. That is, the gas barrier sheet 14 may be attached to each of the masking members 12 and 13.

(Manufacturing method of electrolyte membrane / electrode assembly for fuel cell)
FIG. 6 is a schematic configuration diagram of a coating apparatus 30 that applies electrode ink to the electrolyte membrane composite 1.
A fuel electrode (anode) is formed on one surface of the electrolyte membrane 11, and an air electrode (cathode) is formed on the other surface.
The coating device 30 includes a first coating device 31 and a second coating device 32. The first coating device 31 is disposed above the second coating device 32. Since the first coating device 31 and the second coating device 32 have substantially the same configuration, the first coating device 31 will be described, and the same components will be described using the same reference numerals for the second coating device 32. Is omitted.

The first coating device 31 includes a driving roller 34, a driven roller 36, a screen belt (circulation moving body) 38 stretched around the driving roller 34 and the driven roller 36, a vacuum suction and heating device 40, and electrode ink. And a nozzle 42 for application. When the driving roller 34 rotates in the clockwise direction indicated by the arrow A, the screen belt 38 rotates in the clockwise direction indicated by the arrow B.
In the second coating device 32, the drive roller 34 rotates in the counterclockwise direction indicated by the arrow C, whereby the screen belt 38 rotates in the counterclockwise direction indicated by the arrow D.

  An underlay web 44 is disposed on the screen belt 38. The underlay web 44 is made of a breathable material such as paper. The underlay web 44 is pulled out from the take-up mandrel 46 in the direction indicated by arrow E, adsorbed by the screen belt 38, conveyed in the direction indicated by arrow B, and taken up by the take-up mandrel 48. Similarly, in the second coating device 32, the underlay web 44 is pulled out from the take-up mandrel 46 in the direction indicated by arrow F, adsorbed to the screen belt 38, and conveyed in the direction indicated by arrow D, and the take-up mandrel 48. Rolled up.

  The roll stock 50 of the electrolyte membrane composite 1 is rotatably mounted on the winding mandrel 52 of the coating device 30. From the winding mandrel 52, the electrolyte membrane complex 1 is drawn in the direction indicated by the arrow G. The electrolyte membrane composite 1 is adsorbed on the underlying web 44 and conveyed in the direction indicated by the arrow B by the screen belt 38.

  When the gas barrier sheet 14 is attached to the electrolyte membrane composite 1, the gas barrier sheet 14 is wound around the winding mandrel 56 via the guide roller 54. As a result, the gas barrier sheet 14 is peeled from the electrolyte membrane composite 1. When the gas barrier sheet 14 is attached to the electrolyte membrane composite 1, the roll stock 50 of the electrolyte membrane composite 1 is reversed in the first coating device 31 without using the underlay web 44. The gas barrier sheet 14 may be adsorbed to the screen belt 38. That is, the gas barrier sheet 14 can be used in place of the underlay web 44. Thereby, the mechanism of the winding mandrel 46, 48, 56 can be omitted, and the cost of the apparatus and the member can be reduced.

  The electrolyte membrane composite 1 and the underlying web 44 are adsorbed and heated by the screen belt 38 by the vacuum adsorption and heating device 40. The nozzle 42 applies electrode ink toward the hole 12 a of the masking member 12 of the electrolyte membrane composite 1. Since the hole 12a is formed in a desired shape, a fuel electrode having a desired shape can be easily formed on the first surface 11a of the electrolyte membrane 11. In the present invention, since the masking members 12 and 13 are already bonded to the electrolyte membrane composite 1, it is not necessary to prepare a separate masking member, and the manufacturing process can be simplified.

When the nozzle 42 is a slot nozzle, the width of the underlying web 44 may be substantially the same as the width of the electrolyte membrane composite 1. In the present invention, the type of the nozzle 42 or the applicator is not particularly limited. However, the spray nozzle may be applied by a liquid film, or by a roll, screen, slot nozzle, or the like that is a contact-type application method via liquid. Good. There is a problem that the electrolyte membrane swells due to the solvent of the electrode ink. Therefore, it is important to volatilize as much solvent as possible from the electrode ink before the electrode ink reaches the electrolyte membrane. For this purpose, it is preferable to apply the electrode ink to fine particles with a spray nozzle while increasing contact with the atmosphere. However, since the spray nozzle is applied by forming a liquid into particles, the particles are likely to be scattered. Therefore, when the nozzle 42 is a spray nozzle, it is better to make the width of the underlay web 44 wider than the width of the electrolyte membrane composite 1. The electrode ink discharged from the nozzles 42 may be slightly scattered and spread on the underlay web 44. Such scattered electrode ink adheres to the underlay web 44. The underlay web 44 is wound around a winding mandrel 48.
Thus, the scattered electrode ink can be collected by using the underlay web 44. Therefore, it is possible to provide a coating device that is favorable in terms of environmental hygiene. Moreover, since the electrode ink contains platinum, expensive platinum can be recovered and reused.

The upper masking member 12 of the electrolyte membrane composite 1 is wound around the upper winding mandrel 60 via the guide roller 58. As a result, the masking member 12 is peeled from the electrolyte membrane composite 1. Note that the masking member 12 may proceed downstream without being peeled off and may be wound up in the final step.
The electrode ink applied to the electrolyte membrane 11 is fixed to the electrolyte membrane 11 by drying. Alternatively, the electrode ink may be fixed to the electrolyte membrane 11 by drying through a vacuum chamber, heating with hot air, or heating through a heating roller. Note that the fixing step may be performed in the final step.

The electrolyte membrane 11 and the masking member 13 are guided to the second coating device 32 by a guide roller 62 disposed below. At this time, the conveying direction of the electrolyte membrane 11 and the masking member 13 is reversed from the direction indicated by the arrow H to the direction indicated by the arrow I by the guide roller 62, whereby the masking member 13 is on the upper side.
The electrolyte membrane 11 and the masking member 13 are guided by the guide roller 64, adsorbed on the underlying web 44 of the second coating device 32, and conveyed in the direction indicated by the arrow D by the screen belt 38. The first surface 11a of the electrolyte membrane 11 on which the fuel electrode is formed by the first coating device 31 faces downward, the first surface 11a contacts the underlay web 44, and the masking member 13 faces upward.

  The electrolyte membrane 11, the masking member 13, and the underlying web 44 are adsorbed and heated by the screen belt 38 by the vacuum adsorption and heating device 40. The nozzle 42 applies electrode ink toward the hole 13 a of the masking member 13. Since the hole 13a is formed in a desired shape, a fuel electrode having a desired shape can be easily formed on the second surface 11b of the electrolyte membrane 11.

The masking member 13 is wound around the upper winding mandrel 68 via the guide roller 66. As a result, the masking member 13 is peeled off from the electrolyte membrane 11.
The electrode ink applied to the electrolyte membrane 11 is fixed to the electrolyte membrane 11 by drying. Alternatively, the electrode ink may be fixed to the electrolyte membrane 11 by drying through a vacuum chamber, heating with hot air, or heating through a heating roller.

The electrolyte membrane 11 is wound around the winding mandrel 70. Alternatively, the electrolyte membrane 11 is conveyed to a cutting device (not shown) and cut into a desired size to form a fuel cell electrolyte membrane / electrode assembly. Thus, an electrolyte membrane / electrode assembly for a fuel cell in which the fuel electrode (anode) and the air electrode (cathode) are formed on the electrolyte membrane 11 is obtained.
A fuel cell is manufactured using the electrolyte membrane / electrode assembly (MEA) for a fuel cell thus manufactured.

  In Example 1, although the example which affixed the masking member on both surfaces of the electrolyte membrane was shown, in the following Example 2, the example which affixed the masking member only on the single side | surface of the electrolyte membrane is shown.

(Electrolyte membrane composite)
FIG. 7 is a perspective view of the electrolyte membrane composite 101 according to the present invention. FIG. 8 is an exploded view of the electrolyte membrane composite 101.
The electrolyte membrane composite 101 includes an electrolyte membrane 111 and a masking member 112 attached to the first surface 111a of the electrolyte membrane 111. The masking member 112 is provided with a plurality of holes 112a having a predetermined shape. The plurality of holes 112a are provided to form a fuel electrode of the fuel cell. The thickness of the masking member 112 is approximately the same as or greater than the thickness of the fuel electrode.

  The masking member 112 is attached to the electrolyte membrane 111 so that it can be peeled off from the electrolyte membrane 111. The masking member 112 is attached to the electrolyte membrane 111 with a slight adhesive so that the electrolyte membrane 111 is not damaged when being peeled off. Alternatively, the masking member 112 may be a self-adhesive film having a property of adhering without using an adhesive, and the self-adhesive film may be attached to the electrolyte membrane 111.

(Storage method)
Similarly to Example 1 shown in FIG. 3, the electrolyte membrane composite 101 is rolled into a roll stock, and the roll stock is wrapped in a gas barrier packaging material, and the electrolyte membrane composite 101 is stored. The electrolyte membrane composite 101 may be wound so that the masking member 112 is on the outside.

  As another storage method, the gas barrier sheet 114 may be attached to one surface of the electrolyte membrane composite 101. FIG. 9 is a diagram illustrating a gas barrier sheet 114 attached to the second surface 111 b of the electrolyte membrane 111 of the electrolyte membrane composite 101. The gas barrier sheet 114 is attached to the electrolyte membrane 111 so as to be peeled off with a slight adhesive. Instead of the slightly adhesive, an adhesive may be used, or a function such as Velcro (registered trademark) may be applied to the surface for pasting. When the gas barrier sheet 114 is made of a self-adhesive material, the gas barrier sheet 114 can be attached to the electrolyte membrane 111 without using an adhesive or the like. FIG. 10 is a diagram showing a gas barrier sheet 114 attached to the masking member 112 of the electrolyte membrane composite 101.

  The gas barrier sheets 114 may be attached to both surfaces of the electrolyte membrane composite 101, respectively. That is, the gas barrier sheet 114 may be attached to each of the electrolyte membrane 111 and the masking member 112.

  Similarly to Example 1 shown in FIG. 5, the electrolyte membrane composite 101 is surrounded by the gas barrier sheet 114 by winding the electrolyte membrane composite 101 so that the gas barrier sheet 114 is outside. Thereby, even if it does not package with a gas shielding material, it can be set as the roll stock of the electrolyte membrane composite 101 by which gas shielding was carried out. Furthermore, if it is packaged with a packaging material of a gas shielding material, the gas shielding performance can be improved.

(Manufacturing method of electrolyte membrane / electrode assembly for fuel cell)
FIGS. 11 and 12 are schematic configuration diagrams of a coating apparatus 130 that applies electrode ink to the electrolyte membrane composite 101.
An electrode is formed on one surface of the electrolyte membrane 11.
The coating device 130 applies a driving roller 134, a driven roller 136, a screen belt (circulation moving body) 138 stretched around the driving roller 134 and the driven roller 136, a vacuum suction and heating device 140, and electrode ink. Nozzle 142. When the driving roller 134 rotates in the clockwise direction indicated by the arrow A, the screen belt 138 rotates in the clockwise direction indicated by the arrow B.

  An underlay web 144 is disposed on the screen belt 138. The underlay web 144 is made of a breathable material such as paper. The underlay web 144 is pulled out from the take-up mandrel 146 in the direction indicated by arrow E, adsorbed by the screen belt 138, conveyed in the direction indicated by arrow B, and taken up by the take-up mandrel 148.

  The roll stock 150 of the electrolyte membrane composite 101 is rotatably mounted on the winding mandrel 152 of the coating device 130. When the gas barrier sheet 114 is not attached to the electrolyte membrane composite 101, the electrolyte is obtained by rotating the roll stock 150 of the electrolyte membrane composite 101 in the clockwise direction indicated by the arrow J as shown in FIG. The roll stock 150 is mounted on the take-up mandrel 152 so that the membrane composite 101 is pulled out. From the winding mandrel 152, the electrolyte membrane complex 101 is drawn in the direction indicated by the arrow G. The electrolyte membrane composite 101 is adsorbed on the underlying web 144 and conveyed in the direction indicated by the arrow B by the screen belt 138.

  Here, when the gas barrier sheet 114 is attached to the masking member 112 of the electrolyte membrane composite 101, the roll stock 150 of the electrolyte membrane composite 101 is rotated clockwise as indicated by an arrow J as shown in FIG. The roll stock 150 is mounted on the winding mandrel 152 so that the electrolyte membrane composite 101 is pulled out by rotating in the direction. This is because the electrolyte membrane composite 101 is wound so that the gas barrier sheet 114 is outside the roll stock 150. That is, the roll stock 150 is mounted on the coating apparatus 130 so that the gas barrier sheet 114, the masking member 112, and the electrolyte membrane 111 are arranged in this order from the top. Then, the gas barrier sheet 114 is wound around the upper winding mandrel 156 via the guide roller 154. As a result, the gas barrier sheet 114 is peeled upward from the electrolyte membrane composite 101.

  On the other hand, when the gas barrier sheet 114 is attached to the electrolyte membrane 111 of the electrolyte membrane composite 101, the roll stock 150 of the electrolyte membrane composite 101 is rotated counterclockwise as indicated by an arrow K as shown in FIG. The roll stock 150 is mounted on the winding mandrel 152 so that the electrolyte membrane composite 101 is pulled out by rotating in the direction. This is because the electrolyte membrane composite 101 is wound so that the gas barrier sheet 114 is outside the roll stock 150. That is, the roll stock 150 is mounted on the coating apparatus 130 so that the masking member 112, the electrolyte membrane 111, and the gas barrier sheet 114 are arranged in this order from the top. Then, the gas barrier sheet 114 is wound around the lower winding mandrel 182 via the guide roller 180. As a result, the gas barrier sheet 114 is peeled downward from the electrolyte membrane composite 101.

  The electrolyte membrane composite 101 and the underlying web 144 are adsorbed and heated by the screen belt 138 by the vacuum adsorption and heating device 140. The nozzle 142 applies electrode ink to the electrolyte membrane 111 through the hole 112 a of the masking member 112 of the electrolyte membrane composite 101. Since the hole 112 a is formed in a desired shape, a fuel electrode having a desired shape can be easily formed on the first surface 111 a of the electrolyte membrane 111. In the present invention, since the masking member 112 is already bonded to the electrolyte membrane composite 101, it is not necessary to prepare a separate masking member, and the manufacturing process can be simplified. In addition, since the masking member 112 is self-adhered or attached to the electrolyte membrane 111 with a slight adhesive, the masking member 112 does not float. Therefore, it is possible to prevent the electrode shape from being infiltrated between the masking member 112 and the electrolyte membrane 111 and causing the electrode shape to become defective.

The masking member 112 is wound around the upper winding mandrel 160 via the guide roller 158. As a result, the masking member 112 is peeled from the electrolyte membrane 111. Note that the masking member 112 may be peeled off in the final step.
The electrode ink applied to the electrolyte membrane 111 is fixed to the electrolyte membrane 111 by drying. Alternatively, the electrode ink may be fixed to the electrolyte membrane 111 by drying through a vacuum chamber, heating with hot air, or heating through a heating roller. Note that the fixing step may be performed in the final step.
The electrolyte membrane 111 is wound around the winding mandrel 170. Alternatively, the electrolyte membrane 111 is conveyed to a cutting device (not shown) and cut into a desired size to form a fuel cell electrolyte membrane / electrode assembly.
A fuel cell is manufactured using the electrolyte membrane / electrode assembly (MEA) for a fuel cell thus manufactured.

(Method for producing electrolyte membrane composite)
FIG. 13 is a diagram for explaining a method for producing an electrolyte membrane composite.
In FIG. 13, a hole 212 a having a desired shape is punched with a punching punch 220 while the masking member 212 is pulled out from the roll 210 of the masking member. The fine adhesive 235 is applied to the masking member 212 from which the hole 212a has been punched by removing the hole 212a with the slot nozzle 230. The electrolyte membrane 211 is pulled out from the roll 240 of the electrolyte membrane, and the electrolyte membrane 211 and the masking member 212 are bonded together with a pair of pressing rolls 250. In this way, the electrolyte membrane composite 201 is manufactured.
Note that when the masking member 212 is made of a self-adhesive material, an adhesive application step by the slot nozzle 230 is not necessary.

FIG. 14 is a diagram for explaining another method for producing an electrolyte membrane composite.
In FIG. 14, while the electrolyte membrane 311 is pulled out from the electrolyte membrane roll 340, the fine adhesive 335 is applied with the slot nozzle 330 except for the portion 315 corresponding to the desired shape. The masking member 312 is pulled out from the roll 310 of the masking member, and the electrolyte membrane 311 and the masking member 312 are bonded together with a pair of pressing rolls 350. The masking member 312 is punched into a desired shape by the punching punch 320 corresponding to the portion where the slight adhesive is not applied. At this time, the punching punch 320 is adjusted so that the electrolyte membrane 311 is not punched. When the masking member 312 is wound around the small-diameter roller 360 having a large curvature, the punched piece 312b is separated by a self-separating action, and the scraped piece 370 is scooped up and peeled off. In this way, the electrolyte membrane composite 301 is manufactured.

(Manufacturing method of electrolyte membrane / electrode assembly for fuel cell)
In Example 1 and Example 2, an electrode ink was applied to the electrolyte membrane to produce a fuel cell electrolyte membrane / electrode assembly. In Example 4, a fuel cell electrolyte membrane / electrode assembly (MEA) is manufactured using a powdered electrode material.

FIG. 15 is a schematic cross-sectional view of a filling device for applying or filling a powdered electrode material to an electrolyte membrane composite in order to manufacture an electrolyte membrane / electrode assembly (MEA) for a fuel cell.
The filling device 500 includes a container 502 that stores a powdered electrode material, and a pair of brush rollers 504 and 505 provided in the container 502.
The electrolyte membrane complex 610 composed of the electrolyte membrane 601 and the masking members 602 and 603 attached to both surfaces of the electrolyte membrane 601 is conveyed vertically upward as indicated by an arrow X through the opening 502a of the container 502. The masking members 602 and 603 are formed with holes 602a and 603a having desired shapes.
When the electrolyte membrane 601 passes through the container 502, the powdered electrode material is applied or filled into the holes 602a and 603a of the masking members 602 and 603 by the brush rollers 504 and 505. Thereby, an electrode having a desired shape can be formed on the electrolyte membrane 601.
In this embodiment, the brush rollers 504 and 505 are used as application (or filling) means. However, the present invention may be pushed by a normal roller instead of the brush roller. Alternatively, a powdered electrode material may be adsorbed to the electrolyte membrane 601 through the holes 602a and 603a of the masking members 602 and 603 by using an electrostatic force by using a rubber roller or a resin roller. Furthermore, the type and method of coating and filling are not limited, such as coating with a powder spray gun for general coating instead of filling, coating with a squeegee in the rotary screen method, or applying static electricity to them.

  The filling device 500 may be provided with a squeegee 506 on the downstream side in the conveying direction indicated by the arrow X of the brush rollers 504 and 505. The squeegee 506 acts as a leveling member that removes the powdered electrode material adhering to the surfaces of the masking members 602 and 603 and smoothes the powdered electrode material filled in the holes 602a and 603a. By providing the squeegee 506, excess electrode material can be scraped off. The squeegee 506 is not limited to the plate-like member shown in FIG. 15, but may be a roll-like member or a brush-like member.

  The filling device 500 may be provided with a pressing roller 508 on the downstream side of the conveying direction indicated by the arrow X of the brush rollers 504 and 505. The pressing roller 508 presses the electrolyte membrane composite 610 in order to increase the bulk density of the powdered electrode material P filled in the holes 602a and 603a. Since the powdered electrode material P contains air, the bulk density of the powdered electrode material filled in the holes 602a and 603a with the brush rollers 504 and 505 is low. Therefore, the bulk density is increased to a predetermined density by pressing the powdered electrode material P filled in the holes 602a and 603a by the pressing roller 508.

Incidentally, instead of the squeegee 506 and the pressing roller 508, a pressing and vacuum recovery device 550 as shown in FIG. 16 may be provided. The pressing and vacuum recovery device 550 includes a pressing and driving roller 552, a tension roller 554, a driven roller 556, and a belt 558 stretched between these rollers 552, 554 and 556. The belt 558 is driven in the direction indicated by the arrow Y by the pressing and driving roller 552.
FIG. 17 is a plan view of the belt 558. FIG. 18 is a side view of the belt 558. The belt 558 has holes 558 a having a shape complementary to the holes 602 a and 603 a having desired shapes of the masking members 602 and 603. That is, the belt 558 connects the corresponding portions 558b corresponding to the holes 602a and 603a, both end portions 558c, the first connecting portion 558d connecting the corresponding portions 558b and both end portions 558c, and the adjacent corresponding portions 558b. It consists of two connection parts 558e. The belt 558 moves in the direction indicated by the arrow Y in synchronization with the electrolyte membrane complex 610 so that the corresponding portion 558b coincides with the holes 602a and 603a of the masking members 602 and 603. When the corresponding portion 558b is in contact with the powdered electrode material filled in the holes 602a and 603a, the both end portions 558c, the first connection portion 558d, and the second connection portion 558e of the belt 558 are connected to the masking member 602, A gap is formed away from the surface of 603. A vacuum chamber 560 is provided on the opposite side of the belt 558 facing the masking members 602 and 603. The vacuum chamber 560 sucks the excess powdered electrode material Ps adhering to the surfaces of the masking members 602 and 603 with a vacuum force and collects the material in a collection container (not shown). At this time, since the powdered electrode material P filled in the holes 602a and 603a of the masking members 602 and 603 is covered with the corresponding portion 558b of the belt 558, it is not sucked out by the vacuum force. The pressing and driving roller 552 presses the belt 558 against the electrolyte membrane composite 610, whereby the powdered electrode material P filled in the holes 602a and 603a is pressed, and the powdered electrode material P is The density can be increased.

  The filling device 500 may be provided with a vibration device 570 in a container 502 that contains a powdered electrode material. When the brush rollers 504 and 505 apply or fill the powdered electrode material into the holes 602a and 603a of the masking members 602 and 603, the vibrating device 570 vibrates the container 502, thereby filling the holes 602a and 603a. The bulk density of the powdered electrode material can be increased.

The filling device 500 is provided with a vacuum chamber 580 for applying or filling a powdered electrode material into the holes 602a and 603a of the masking members 602 and 603 under vacuum. The vacuum chamber 580 includes at least brush rolls 504 and 505. The vacuum chamber 580 may include a container 502. The vacuum chamber 580 may include a squeegee 506. The vacuum chamber 580 may further include a pressing roller 508. The vacuum chamber 580 is connected to a vacuum pump 586 via a recovery chamber 582 and a filter 584. The vacuum chamber 580 can collect the powdered electrode material scattered around in the filling process of the powdered electrode material.
The vacuum degree of the vacuum chamber is not particularly questioned. For example, in a vacuum chamber having a vacuum degree of 1 to 40 kPa that can be produced by a relatively inexpensive vacuum pump, the powder electrode material is filled with a high bulk density. In addition, since the oxygen concentration can be kept extremely low, it is extremely effective for materials that are easily ignited or easily ignited, such as electrode materials.

  If necessary, the filling apparatus 500 may repeatedly perform the filling process using the brush rolls 504 and 505. Alternatively, the leveling process using the squeegee 506 and the filling process may be repeated. Alternatively, the pressing process by the pressing roller 508, the leveling process, and the filling process may be repeated.

The electrolyte membrane composite 610 that has come out of the filling device 500 is sent to a fixing portion (not shown). In the fixing portion, the powdered electrode material is heated and pressure-bonded by a heating pressure roller and fixed to the electrolyte membrane 601. This fixing process is performed after the masking members 602 and 603 are peeled off. Alternatively, the fixing step may be performed before the masking members 602 and 603 are peeled off. In this way, an electrolyte membrane / electrode assembly (MEA) for a fuel cell is manufactured.
A fuel cell is manufactured using the electrolyte membrane / electrode assembly (MEA) for a fuel cell thus manufactured.
In the fourth embodiment, the fixing portion (not shown) is arranged outside the vacuum chamber 580, but the fixing portion may be arranged inside the vacuum chamber 580.

(Manufacturing method of electrolyte membrane / electrode assembly for fuel cell)
In Example 4, a fuel cell electrolyte membrane / electrode assembly (MEA) was manufactured by applying or filling a powdered electrode material to an electrolyte membrane composite having a masking member laminated thereon. In Example 5, an electrolyte membrane / electrode assembly (MEA) for a fuel cell is manufactured by applying or filling a powdered electrode material to an electrolyte membrane on which no masking member is laminated.

FIG. 19 is a schematic cross-sectional view of a filling apparatus for applying or filling a powdered electrode material to an electrolyte membrane in order to manufacture an electrolyte membrane / electrode assembly (MEA) for a fuel cell.
The filling device 700 includes a container 702 that stores a powdered electrode material, a pair of brush rollers 704 and 705 provided in the container 702, and a masking device 750.
The masking member 750 includes a pressing and driving roller 752, a tension roller 754, driven rollers 756 and 757, and a masking belt 758 stretched between these rollers 752, 754, 756, and 757. Masking belt 758 is driven in the direction indicated by arrow N by pressing and driving roller 752. The masking belt 758 has a hole 758a cut out to form a fuel electrode (anode) and an air electrode (cathode).

The electrolyte membrane 801 is sandwiched between two masking belts 758, and is conveyed vertically upward indicated by an arrow M through the opening 702a of the container 702. When the electrolyte membrane 801 sandwiched between the two masking belts 758 passes through the container 702, the powdered electrode material is applied or filled into the holes 758a of the masking belt 758 by the brush rollers 704 and 705. Thus, an electrode having a desired shape can be formed on the electrolyte membrane 801.
In this embodiment, the brush rollers 704 and 705 are used as the application (or filling) means, but the present invention may be pushed by a normal roller instead of the brush roller. Alternatively, a powdered electrode material may be adsorbed to the electrolyte membrane 801 through the hole 758a of the masking belt 758 by using an electrostatic force by using a rubber roller or a resin roller.
Furthermore, the method and type of application and filling are not limited, such as application with a powder spray gun for general coating instead of filling, application with a squeegee of the rotary screen method, or application of static electricity to them.

  The filling device 700 may be provided with a squeegee 706 on the downstream side in the conveying direction indicated by the arrow M of the brush rollers 704 and 705. The squeegee 706 acts as a leveling member that removes the powdered electrode material adhering to the surface of the masking belt 758 or smoothes the powdered electrode material filled in the hole 758a. By providing the squeegee 706, excess electrode material can be scraped off. Note that the squeegee 706 is not limited to the plate-like member shown in FIG. 19, but may be a roll-like member or a brush-like member.

  The pressing and driving roller 752 presses the masking belt 758 against the electrolyte membrane 801, whereby the powdered electrode material P filled in the hole 758a is pressed, and the bulk density of the powdered electrode material P is reduced. Can be increased.

  The filling device 700 may be provided with a vibration device 770 in a container 702 that stores a powdered electrode material. When the brush rollers 704 and 705 apply the powdered electrode material to the hole 758a of the masking belt 758, that is, fill the hole 758a, the vibration device 770 vibrates the container 702, thereby determining whether the powdered electrode material filled in the hole 758a. The density can be increased.

On the downstream side of the pressing and driving roller 752, the masking belt 758 is separated from the electrolyte membrane 801. On the electrolyte membrane 801, a powdered electrode material P having a desired shape is attached. The powdered electrode material P is heated and pressed by a pair of heating pressure rollers 775 and is fixed to the electrolyte membrane 801. In this way, an electrolyte membrane / electrode assembly (MEA) for a fuel cell is manufactured.
A fuel cell is manufactured using the electrolyte membrane / electrode assembly (MEA) for a fuel cell thus manufactured.

  The filling device 700 is provided with a vacuum chamber 780 for applying or filling a powdered electrode material into the hole 758a of the masking belt 758 under vacuum. In the vacuum chamber 780, brush rolls 704 and 705, a container 702, a squeegee 706, a masking device 750, and a heating pressure roller 775 are provided. The heating pressure roller 775 may be provided outside the vacuum chamber 780. The vacuum chamber 780 is connected to a vacuum pump 786 via a recovery chamber 782 and a filter 784. The vacuum chamber 780 can collect the powdered electrode material scattered around in the filling process of the powdered electrode material.

  If necessary, the filling device 700 may repeatedly perform the filling process using the brush rolls 704 and 705. Alternatively, the leveling process using the squeegee 706 and the filling process may be repeated. Further, a pressure roller (not shown) may be added on the downstream side of the squeegee 706. The pressing process with the pressing roller, the leveling process, and the filling process may be repeated.

(Manufacturing method of electrolyte membrane / electrode assembly for fuel cell)
In Example 6, an electrolyte membrane / electrode assembly (MEA) for a fuel cell is manufactured by applying or filling a powdered electrode material to an electrolyte membrane on which no masking member is laminated.

FIG. 20 is a schematic cross-sectional view of a coating apparatus for applying a powdered electrode material to an electrolyte membrane in order to manufacture a fuel cell electrolyte membrane / electrode assembly (MEA).
The coating apparatus 900 is preferably a coating apparatus shown in FIG.
The coating device 900 includes a hopper 902 that contains a powdered electrode material, a rotating brush 904 disposed in the hopper 902, a hollow roll 906 in which a hole 906a having a desired electrode shape is hollowed out, and an inner side of the hollow roll 906. And a slit 910 for compressed gas disposed inside the screen 908. The screen 908 has an eye smaller than the particle size of the powdered electrode material. The outer shape of the screen 908 is substantially equal to the inner diameter of the hollow roll 906, and the screen 908 is attached to the hollow roll 906 and rotates together in the direction indicated by the arrow S.

  The powdered electrode material P in the hopper 902 is filled into a hole 906 a provided in the hollow roll 906 by the rotating brush 904. The powdered electrode material P is stably filled by the suction V from the suction port 902a of the hopper 902. The powdered electrode material sucked from the suction port 902a may be returned to the hopper 902 and circulated.

The hollow roll 906 in which the hole 906a is filled with the powdered electrode material P rotates in the direction indicated by the arrow S. The electrolyte membrane 951 is transported in the direction indicated by the arrow S1. The hollow roll 906 is disposed to face the electrolyte membrane 951 being conveyed. A compressed gas slit nozzle 910 is provided on the opposite side of the hollow roll 906 facing the electrolyte membrane 951. When the powdered electrode material P filled in the hole 906a reaches the compressed gas slit nozzle 910, the powdered electrode material P is applied to the electrolyte membrane 951 by the compressed gas ejected from the compressed gas slit nozzle 910. The Since the hole 906a is formed in a desired electrode shape, the powdered electrode material P applied on the electrolyte membrane 951 has a desired electrode shape. The electrolyte membrane 951 is conveyed in the direction indicated by the arrow S1, and is sandwiched between a pair of downstream heating pressure rollers 912 to be applied with heat and pressure, and the powdered electrode material P is fixed to the electrolyte membrane 951. Is done. In this way, an electrolyte membrane / electrode assembly (MEA) for a fuel cell is manufactured.
A fuel cell is manufactured using the electrolyte membrane / electrode assembly (MEA) for a fuel cell thus manufactured.

  The coating apparatus 900 may be provided with a low pressure chamber 920. If a recovery device is provided in the low-pressure chamber 920, the powdered electrode material scattered around can be recovered by performing the coating operation in the low-pressure chamber 920.

(Manufacturing method of electrolyte membrane / electrode assembly for fuel cell)
Example 7 is a combination of application or filling of electrode ink and application or filling of powdered electrode material.
FIG. 21 is a diagram showing an example in which electrode ink EI and powdered electrode material P are laminated and applied. The electrolyte membrane composite 1001 includes an electrolyte membrane 1002 and a masking member 1003 laminated on the electrolyte membrane 1002. The masking member 1003 is formed with a hole 1003a hollowed into a desired electrode shape.
The hole 1003a is filled with the electrode ink EI by the above-described filling device, then filled with the powdered electrode material P, and then filled with the electrode ink EI, whereby the electrode ink EI and the powdered electrode material are filled. An electrode made of a laminate with P can be easily produced.
It should be noted that the type of electrode ink, powdered electrode material, order of lamination, and means for lamination are not particularly limited, and include a method of applying them while mixing them.

  In the present invention, the electrolyte membrane has been described. However, the present invention is masked with a hole on one side such as PTFE used as a gas diffusion layer (GDL) or indirect transfer film, or PET or PP treated so as to be easily peeled off. A method of laminating members and applying electrode ink or the like can also be applied. That is, what replaced the electrolyte membrane of the present invention with a gas diffusion layer or an indirect transfer film also belongs to the scope of the present invention.

As described above, according to the present invention, an electrolyte membrane, an electrolyte membrane composite, a method for producing an electrolyte membrane composite, and a fuel cell electrolyte for producing an electrode having a desired pattern with high quality and high productivity A membrane / electrode assembly and a method for producing an electrolyte membrane / electrode assembly for a fuel cell can be provided.
According to the present invention, there is no gap between the electrolyte membrane and the masking member, and an electrode having a desired shape can be accurately formed.
In addition, it is not necessary to separately load the masking member into the coating apparatus, and an electrode having a desired shape (pattern) can be accurately manufactured only by loading the electrolyte membrane according to the present invention into the coating apparatus.
Furthermore, according to the present invention, the dried electrode ink or / and the powdered electrode material attached to the masking member are wound together with the masking member, so that the wound masking member is transported to the catalyst manufacturer. Platinum is reused. Therefore, a cleaning solvent and a cleaning process for cleaning the masking member can be eliminated.

  The present invention is not limited to the embodiments described above, and can be implemented in various other forms without departing from the features thereof. For this reason, the above-described embodiment is merely an example in all respects and should not be interpreted in a limited manner. The scope of the present invention is shown by the scope of claims, and is not restricted by the text of the specification. Further, all modifications and changes belonging to the equivalent scope of the claims are within the scope of the present invention.

The perspective view of the electrolyte membrane composite 1 by this invention. FIG. 3 is an exploded view of the electrolyte membrane composite 1. The figure which shows the state in which the electrolyte membrane composite 1 wound by roll shape is wrapped with the packaging material 20. FIG. The figure which shows what stuck the gas barrier sheet | seat 14 on the one surface of the electrolyte membrane composite 1. FIG. The figure which shows the state which wound the electrolyte membrane composite 1 so that the gas barrier property sheet | seat 14 may become an outer side. The schematic block diagram of the coating device 30 which apply | coats electrode ink to the electrolyte membrane composite 1. FIG. The perspective view of the electrolyte membrane composite_body | complex 101 by this invention. The exploded view of the electrolyte membrane composite 101. FIG. The figure which shows what adhered the gas barrier sheet | seat 114 to the 2nd surface 111b of the electrolyte membrane 111 of the electrolyte membrane composite 101. FIG. The figure which shows what adhered the gas barrier property sheet | seat 114 to the masking member 112 of the electrolyte membrane composite 101. FIG. The schematic block diagram of the coating device 130 which apply | coats electrode ink to the electrolyte membrane composite 101. FIG. The schematic block diagram of the coating device 130 which apply | coats electrode ink to the electrolyte membrane composite 101. FIG. The figure explaining the manufacturing method of electrolyte membrane composite. The figure explaining another manufacturing method of an electrolyte membrane composite. The schematic sectional drawing of the apparatus which apply | coats, ie, fills with powdered electrode material to electrolyte membrane composite. The figure which shows the press and vacuum collection | recovery apparatus 550. FIG. The top view of the belt 558. FIG. The side view of the belt 558. FIG. The schematic sectional drawing of the filling apparatus which apply | coats, ie, fills with powdered electrode material to an electrolyte membrane. The schematic sectional drawing of the coating device which apply | coats a powdered electrode material to an electrolyte membrane. The figure which shows the example which laminated | stacked and apply | coated the electrode ink EI and the powdery electrode material P. FIG.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1,101 Electrolyte membrane composite 11, 111 Electrolyte membrane 12, 13, 112 Masking member 12a, 13a, 112a Hole 14, 114 Gas barrier sheet 30, 130 Coating apparatus 50, 150 Roll stock 500, 700, 900 Filling apparatus P Powder Electrode material

Claims (41)

  A fuel cell electrolyte membrane prior to application of an electrode, wherein a masking member having a hole hollowed in a desired electrode shape is laminated on at least one surface of the electrolyte membrane.   2. The electrolyte membrane for a fuel cell according to claim 1, wherein masking members each having a hole formed in a substantially similar desired electrode shape are laminated on both surfaces of the electrolyte membrane.   3. The fuel membrane electrolyte membrane according to claim 1, wherein the masking member is attached to the electrolyte membrane via self-adhesion or a slight adhesive. 4.   4. The electrolyte membrane for fuel cells according to claim 1, wherein the electrolyte membrane and / or the masking member is a web, and the electrolyte membrane is a roll stock.   4. The electrolyte membrane for a fuel cell according to claim 1, wherein the electrolyte membrane is cut into a sheet.   6. The fuel cell electrolyte membrane according to claim 1, wherein a gas barrier sheet or web is laminated on at least one masking member.   7. The fuel membrane electrolyte membrane according to claim 1, wherein the thickness of the masking member is substantially the same as or thicker than the thickness of the electrode formed in the subsequent step.   8. The electrolyte membrane for a fuel cell according to claim 1, wherein the electrolyte membrane is wrapped with a gas barrier packaging material. An electrolyte membrane / electrode assembly for a fuel cell,
A fuel cell electrolyte membrane according to any one of claims 1 to 8, which is manufactured by applying or filling an electrode ink or / and a powdered electrode material into a fuel cell electrolyte membrane through a hole in the masking member and peeling off the masking member. Electrolyte membrane / electrode assembly for fuel cells.   10. The fuel cell electrolyte membrane according to claim 9, wherein the electrode ink or / and the powdered electrode material applied or filled in the fuel cell electrolyte membrane are fixed to the fuel cell electrolyte membrane. Electrode assembly.   12. The fuel cell electrolyte membrane / electrode assembly according to claim 11, wherein the electrode ink or / and the powdered electrode material are fixed to the fuel cell electrolyte membrane by drying, heating or / and pressing. .   A fuel cell using the electrolyte membrane / electrode assembly for a fuel cell according to claim 9. An electrolyte membrane composite,
An electrolyte membrane;
Consisting of a masking member provided with a plurality of holes,
The electrolyte membrane composite, wherein the masking member is detachably attached to one surface of the electrolyte membrane.   14. The electrolyte membrane composite according to claim 13, wherein the hole is formed in the shape of a fuel electrode of a fuel cell.   The electrolyte membrane composite according to claim 13 or 14, further comprising a masking member that is detachably attached to the other surface of the electrolyte membrane.   The electrolyte membrane composite according to any one of claims 13 to 15, further comprising a gas barrier sheet.   The electrolyte membrane composite according to claim 16, wherein the gas barrier sheet is attached to the masking member so as to be peeled off.   The electrolyte membrane composite according to claim 16 or 17, wherein the gas barrier sheet is detachably attached to the electrolyte membrane.   The electrolyte membrane composite according to claim 13, wherein the masking member is made of a self-adhesive material.   20. The electrolyte membrane composite according to claim 16, wherein the gas barrier sheet is made of a self-adhesive material.   The electrolyte membrane composite according to any one of claims 13 to 20, wherein the electrolyte membrane composite is wound into a roll stock.   21. The electrolyte membrane composite according to any one of claims 13 to 20, wherein the electrolyte membrane composite is cut into a sheet to be provided with at least one hole.   The electrolyte membrane composite according to any one of claims 13 to 22, wherein the electrolyte membrane composite is wrapped in a gas barrier packaging material. A method for producing an electrolyte membrane composite comprising an electrolyte membrane and a masking member,
A step of making a hole of a desired shape in the masking member;
Thereafter, the method comprises a step of bonding the masking member and the electrolyte membrane together. A method for producing an electrolyte membrane composite comprising an electrolyte membrane and a masking member,
A step of bonding the masking member and the electrolyte membrane;
Thereafter, a step of opening a hole of a desired shape in the masking member. A method of manufacturing an electrolyte membrane / electrode assembly for a fuel cell, comprising:
A step of rotatably installing a roll stock of an electrolyte membrane composite comprising an electrolyte membrane and a masking member provided with a plurality of holes;
Extracting the electrolyte membrane composite from the roll stock;
Applying or filling an electrode ink or / and powdered electrode material to the electrolyte membrane through a plurality of holes in the masking member while conveying the electrolyte membrane composite;
And a step of peeling the masking member from the electrolyte membrane. A method of manufacturing an electrolyte membrane / electrode assembly for a fuel cell, comprising:
A step of rotatably installing a roll stock of an electrolyte membrane composite comprising an electrolyte membrane, a masking member provided with a plurality of holes, and a gas barrier sheet;
Extracting the electrolyte membrane composite from the roll stock;
Removing the gas barrier sheet; and
Applying or filling an electrode ink or / and powdered electrode material to the electrolyte membrane through a plurality of holes in the masking member while conveying the electrolyte membrane composite;
And a step of peeling the masking member from the electrolyte membrane. A method of manufacturing an electrolyte membrane / electrode assembly for a fuel cell, comprising:
An electrolyte membrane, a first masking member attached to the first surface of the electrolyte membrane and provided with a plurality of holes, and a second masking member attached to the second surface of the electrolyte membrane and provided with a plurality of holes A step of rotatably installing a roll stock of an electrolyte membrane composite comprising a masking member;
Extracting the electrolyte membrane composite from the roll stock;
Applying or filling electrode ink or / and powdered electrode material on the first surface of the electrolyte membrane through the plurality of holes of the first masking member while conveying the electrolyte membrane composite;
Removing the first masking member from the electrolyte membrane;
Reversing the electrolyte membrane and the second masking member;
Applying or filling electrode ink or / and powdered electrode material on the second surface of the electrolyte membrane through the plurality of holes of the second masking member while conveying the electrolyte membrane and the second masking member;
And a step of peeling the second masking member from the electrolyte membrane. A method of manufacturing an electrolyte membrane / electrode assembly for a fuel cell, comprising:
A step of installing a sheet of electrolyte membrane composite comprising an electrolyte membrane and a masking member provided with at least one hole;
Applying or filling the electrolyte membrane with electrode ink or / and powdered electrode material through at least one hole of the masking member;
And a step of peeling the masking member from the electrolyte membrane.   30. The method according to claim 26, further comprising the step of fixing an electrode ink or / and a powdered electrode material to the electrolyte membrane. A method of manufacturing an electrolyte membrane / electrode assembly for a fuel cell, comprising:
An electrolyte membrane, a first masking member attached to the first surface of the electrolyte membrane and provided with a plurality of holes, and a second masking member attached to the second surface of the electrolyte membrane and provided with a plurality of holes A method comprising filling or / and applying a powdered electrode material through a hole in the first masking member and the second masking member while transporting an electrolyte membrane composite comprising a masking member.   32. The method of claim 31, further comprising increasing the density of the powdered electrode material filled or / and applied to the holes of the first masking member and the second masking member.   The method according to claim 32, comprising the step of repeating the filling or / and applying step and the step of increasing the density of the powdered electrode material.   The method according to any one of claims 31 to 33, further comprising a step of heating or / and pressing the powdered electrode material and a step of peeling off the first and second masking members.   The method according to any one of claims 31 to 34, wherein the step of filling or / and applying at least the powdered electrode material is performed under vacuum.   36. The method according to any one of claims 31 to 35, further comprising a step of cutting the electrolyte membrane. An electrolyte membrane / electrode assembly for a fuel cell,
37. An electrolyte membrane / electrode assembly for a fuel cell produced by the method according to claim 31 to 36.   A fuel cell, wherein the fuel cell electrolyte membrane / electrode assembly according to claim 37 is used.   A method of manufacturing an electrolyte membrane / electrode assembly for a fuel cell, wherein a masking member having a hole hollowed out in an electrode shape is laminated on a gas diffusion layer or / and an indirect transfer film for electrode, and electrode ink or / and A method comprising: applying or filling a powdered electrode material; removing a masking member; and transferring or thermocompression bonding to an electrolyte membrane.   40. The method according to claim 39, comprising the steps of forming an anode electrode and a cathode electrode on the gas diffusion layer for both electrodes and / or the indirect transfer film for electrodes, and simultaneously transferring or press-bonding to the electrolyte membrane. An electrolyte membrane / electrode assembly for a fuel cell,
An electrolyte membrane / electrode assembly for a fuel cell produced by the method according to claim 39 or 40.

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