JP2006185762A - Method of manufacturing membrane and catalyst layer junction for polymer electrolyte fuel cell, method of manufacturing polymer electrolyte fuel cell, and device of manufacturing membrane and catalyst layer junction for polymer electrolyte fuel cell - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a membrane and catalyst layer junction which is suitable for mass production of a fuel cell and does not deteriorate power generation efficiency per usage amount of a catalyst, a method of manufacturing a polymer electrolyte fuel cell using it, and a device of manufacturing the membrane and catalyst junction. <P>SOLUTION: This is the method of manufacturing the membrane and catalyst layer junction for the polymer electrolyte fuel cell in which catalyst layers 3 are respectively formed on both sides of an electrolyte membrane 1, and comprises a first process in which a long electrolyte membrane 1 is prepared, a second process in which a transfer film 2 formed with the catalyst layer 3 is prepared on a base material film 5, a third process in which the transfer film 2 is arranged on at least one face of the electrolyte membrane 1 so that the catalyst layer 3 of the transfer film 2 may face the electrolyte membrane 1, and a fourth process in which the catalyst layer 3 of the transfer film 2 is intermittently transferred at desired spacing on at least one face of the electrode membrane 1. <P>COPYRIGHT: (C)2006,JPO&NCIPI

Description

  TECHNICAL FIELD The present invention relates to a method for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell, a method for producing a polymer electrolyte fuel cell, and a device for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell. It is.

  A fuel cell is a cell in which electrodes are arranged on both sides of an electrolyte and generates electricity by an electrochemical reaction between hydrogen and oxygen, and only water is generated during power generation. Thus, unlike the conventional internal combustion engine, it is expected to spread as a next-generation clean energy system because it does not generate environmental load gas such as carbon dioxide. In particular, the polymer electrolyte fuel cell has a low operating temperature and low electrolyte resistance. In addition, it uses a highly active catalyst, so it can obtain high output even in a small size. Is expected.

  A polymer electrolyte fuel cell uses a hydrogen ion (proton) conductive polymer membrane as an electrolyte membrane, a catalyst layer is arranged on both sides thereof, an electrode substrate is then arranged on both sides, and this is further sandwiched between separators. It has a structure. A catalyst layer disposed on both sides of an electrolyte membrane (that is, a catalyst layer / electrolyte membrane / catalyst layer structure) is called a membrane / catalyst layer assembly, and an electrode substrate is further disposed on both sides of the membrane. The obtained structure (namely, electrode base material / catalyst layer / electrolyte membrane / catalyst layer / electrode base material layer structure) is called a membrane electrode assembly (MEA: MEMBRANE ELECTRODE ASSEMBLY).

  Conventionally, as a method for producing a membrane / electrode assembly, for example, two electrode base materials having a catalyst layer formed by applying a printing method or a spray method on one side are used, and the catalyst layer surface of the electrode base material is an electrolyte membrane. A catalyst layer is formed by applying a printing method or a spray method on both surfaces of the electrolyte membrane (Patent Documents 1 and 2, etc.) by placing the electrodes in contact with both surfaces and applying heat pressing, and an electrode substrate on each catalyst layer surface. There is known a method of arranging and touching with heat (such as Patent Document 3).

  However, these methods have various drawbacks. For example, in the former method, when the catalyst layer is formed on the electrode base material by applying a printing method or a spray method, the catalyst layer enters the porous electrode base material. It becomes difficult and it becomes difficult to form a catalyst layer uniformly on an electrode base material. Furthermore, this method may block holes on the surface of the electrode base material or inside, and may impede gas flow performance. As a result, the performance of the fuel cell using the obtained membrane-electrode assembly may be deteriorated.

  In the latter method, a catalyst layer is formed by printing or spraying a solution obtained by dissolving or dispersing the constituent components of the catalyst layer in an organic solvent on both surfaces of the electrolyte membrane, but the electrolyte membrane is swollen and deformed by the organic solvent. It may be difficult to maintain the shape of the electrolyte membrane. For this reason, it may be difficult to adjust the thickness of the catalyst layer, or it may be difficult to uniformly form the catalyst layer on the electrolyte membrane. As a result, the obtained membrane / electrode assembly may not be able to produce a fuel cell with uniform performance.

  In addition, both of these manufacturing methods are suitable for small-scale production, but are not suitable for mass production accompanying the expected increase in demand for polymer electrolyte fuel cells.

As a method without the above drawbacks, a method is known in which a catalyst layer is transferred to an electrolyte membrane from a transfer sheet having a catalyst layer formed on a substrate (Patent Document 4). The membrane / electrode assembly is produced by joining an electrode substrate to the catalyst layer of the membrane / catalyst layer assembly obtained by this transfer method.
Japanese Examined Patent Publication No. 62-61118 Japanese Patent Publication No.62-61119 Japanese Examined Patent Publication No. 2-48632 Japanese Patent Laid-Open No. 10-64574

  However, since the catalyst layer is continuously transferred to the entire electrolyte membrane in the above transfer method, there is a catalyst layer in a portion that does not contribute to the battery reaction, such as a portion that fits into the gasket when assembling the cell. As a result, there is a disadvantage that the power generation efficiency per the amount of catalyst such as expensive platinum is reduced.

  Therefore, the present invention is suitable for mass production of fuel cells and does not reduce the power generation efficiency per catalyst usage, and a membrane / catalyst layer assembly, and a method for producing a solid polymer fuel cell using the same, It is an object of the present invention to provide an apparatus for producing the membrane / catalyst layer assembly.

  As a means for solving the above-mentioned problems, a method for producing a membrane / catalyst layer assembly according to the present invention comprises a membrane / catalyst layer assembly for a polymer electrolyte fuel cell in which catalyst layers are respectively formed on both surfaces of an electrolyte membrane. In the manufacturing method, a first step of preparing the long electrolyte membrane, a second step of preparing a transfer film in which the catalyst layer is formed on a long base film, and a catalyst of the transfer film A third step of disposing the transfer film on at least one surface of the electrolyte membrane so that the layer faces the electrolyte membrane; and a catalyst layer of the transfer film with a desired interval on at least one surface of the electrolyte membrane. And a fourth step of intermittently transferring.

  In the fourth step, the long electrolyte membrane is continuously fed in the length direction, the long transfer film is intermittently fed in the same direction as the electrolyte membrane, and a heat roll is transferred to the transfer film. By sandwiching the electrolyte membrane and the transfer film in conjunction with the feeding, the catalyst layer can be intermittently transferred to at least one surface of the electrolyte membrane at a desired interval.

  Alternatively, the long electrolyte membrane is continuously fed in the length direction, the long transfer film is intermittently fed in the same direction as the electrolyte membrane, and the seal bar is interlocked with the feed of the transfer film. By sandwiching the electrolyte membrane and the transfer film, the catalyst layer can be transferred intermittently at a desired interval to at least one surface of the electrolyte membrane.

  Alternatively, the long electrolyte membrane and transfer film are intermittently sent in the length direction, and a thermal stamper sandwiches the electrolyte membrane and transfer film in conjunction with intermittent stop of the electrolyte membrane and transfer film, The catalyst layer may be transferred intermittently at a desired interval to at least one surface of the electrolyte membrane.

  Furthermore, while the thermal head sandwiches the electrolyte membrane and the transfer film at a constant pressure, the long electrolyte membrane is continuously sent in the length direction, and the long transfer film is intermittently fed. The catalyst layer is intermittently transferred at a desired interval to at least one surface of the electrolyte membrane by feeding in the same direction as the electrolyte membrane and raising the temperature of the thermal head in conjunction with the feed of the transfer film. You can also do it.

  Further, as a means for solving the above-mentioned problems, the method for producing a polymer electrolyte fuel cell according to the present invention comprises a membrane / electrode assembly comprising a catalyst layer and an electrode substrate on both sides of an electrolyte membrane, and the membrane. In a method for producing a polymer electrolyte fuel cell comprising a pair of separators that sandwich an electrode assembly, a first step of preparing the long electrolyte membrane, and the catalyst on a long base film A second step of preparing a transfer film having a layer formed thereon; and a third step of disposing the transfer film on at least one surface of the electrolyte membrane so that a catalyst layer of the transfer film faces the electrolyte membrane. A fourth step of intermittently transferring the catalyst layer of the transfer film to at least one surface of the electrolyte membrane at a desired interval, and a fifth step of laminating and forming the electrode base material on the catalyst layer And the separate And having a sixth step of sandwiching the membrane electrode assembly by.

  Further, as means for solving the above-mentioned problems, the first apparatus for producing a membrane / catalyst layer assembly according to the present invention comprises a membrane for a polymer electrolyte fuel cell in which catalyst layers are formed on both surfaces of an electrolyte membrane, respectively. In the catalyst layer assembly manufacturing apparatus, the catalyst layer is formed on the long base film on at least one surface side of the electrolyte membrane, and the electrolyte membrane feeding section that sends the long electrolyte membrane in the length direction A transfer film feeding unit that feeds the transferred transfer film in the same direction as the electrolyte membrane, and a pair of heat rolls installed so as to sandwich the electrolyte membrane and the transfer film. The transfer film feed unit is intermittent feed drive, and the pair of heat rolls are configured to sandwich the electrolyte membrane and the transfer film in conjunction with the feed of the transfer film feed unit. And butterflies.

  Further, as means for solving the above-mentioned problems, the second apparatus for producing a membrane / catalyst layer assembly according to the present invention comprises a membrane for a polymer electrolyte fuel cell in which catalyst layers are formed on both surfaces of an electrolyte membrane, respectively. In the catalyst layer assembly manufacturing apparatus, the catalyst layer is formed on the long base film on at least one surface side of the electrolyte membrane, and the electrolyte membrane feeding section that sends the long electrolyte membrane in the length direction A transfer film feeding section that feeds the transferred transfer film in the same direction as the electrolyte membrane, and a pair of seal bars that can be sandwiched between the electrolyte membrane and the transfer film, and the electrolyte membrane feeding section is continuously fed The transfer film feeding section is intermittently driven, and the pair of seal bars are configured to sandwich the electrolyte membrane and the transfer film in conjunction with the feeding of the transfer film feeding section. The features.

  Moreover, as a means for solving the above-mentioned problem, the third apparatus for producing a membrane / catalyst layer assembly according to the present invention comprises a membrane for a polymer electrolyte fuel cell in which catalyst layers are formed on both surfaces of an electrolyte membrane, respectively. In the catalyst layer assembly manufacturing apparatus, the catalyst layer is formed on the long base film on at least one surface side of the electrolyte membrane, and the electrolyte membrane feeding section that sends the long electrolyte membrane in the length direction A transfer film feeding section for feeding the transferred transfer film in the same direction as the electrolyte membrane, and a pair of thermal stampers installed so as to sandwich the electrolyte membrane and the transfer film, the electrolyte membrane feeding section and the transfer film feeding And the pair of thermal stampers sandwich the electrolyte membrane and the transfer film in conjunction with the intermittent stop of the electrolyte membrane and the transfer film, so that the catalyst layer is electrolyzed. Characterized in that it is configured to intermittently transfer at a desired interval on at least one surface of the film.

  Further, as a means for solving the above-mentioned problems, a fourth apparatus for producing a membrane / catalyst layer assembly according to the present invention comprises a membrane for a polymer electrolyte fuel cell in which catalyst layers are respectively formed on both surfaces of an electrolyte membrane. In the catalyst layer assembly manufacturing apparatus, the catalyst layer is formed on the long base film on at least one surface side of the electrolyte membrane, and the electrolyte membrane feeding section that sends the long electrolyte membrane in the length direction A transfer film feeding section for feeding the transferred transfer film in the same direction as the electrolyte membrane, and a pair of thermal heads sandwiching the electrolyte membrane and the transfer film with a constant pressure. Drive, wherein the transfer film feed section is intermittent feed drive, and the temperature of the pair of thermal heads rises in conjunction with the feed of the transfer film feed section. At this time, the pair of thermal heads has a plurality of heating elements at the tip portions in contact with the electrolyte membrane or the transfer film, and raises the temperature of the heating elements selected from the plurality of heating elements. May be a feature.

  According to the present invention, the catalyst layer is formed by transferring the catalyst layer intermittently at a desired interval on at least one surface of the electrolyte membrane. Therefore, a portion where the catalyst layer between the catalyst layers is not transferred is fitted to a gasket or the like. Thus, the amount of the catalyst layer in which a relatively expensive material is used can be reduced.

  In addition, by transferring the catalyst layer to at least one surface of the electrolyte membrane with a thermal stamper, the shape of the transfer surface of the thermal stamper is changed to a desired shape, so that the shape of the catalyst layer transferred to the electrolyte membrane can be changed to a desired shape. It can be a shape.

  Furthermore, by using a thermal head having a heating element capable of raising and lowering the temperature at the tip to transfer the catalyst layer to at least one surface of the electrolyte membrane, the pressure of the thermal head on the electrolyte membrane and the transfer film is always applied. The catalyst layer can be intermittently formed at a desired interval on at least one surface of the electrolyte membrane while being kept constant. In addition, by having a plurality of heating elements and raising or lowering the temperature of only the desired heating element among the plurality of heating elements, only the catalyst layer corresponding to the heating element whose temperature has been raised is transferred to the electrolyte membrane. The catalyst layers having different shapes can be transferred to the electrolyte membrane in the same manufacturing process without exchanging the hot press machine or the transfer film.

  Embodiments of a method for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell, a method for producing a polymer electrolyte fuel cell, and a device for producing a membrane / catalyst layer assembly according to the present invention will now be described with reference to the accompanying drawings. explain. FIG. 1 is a perspective view schematically showing a production apparatus for a membrane / catalyst layer assembly according to the present embodiment. FIG. 2 is a front view of the production apparatus in a transfer state (a) and a non-transfer state (b). FIG. As shown in FIGS. 1 and 2, the manufacturing apparatus includes a hot roll 7 (hot press machine), an electrolyte membrane feed unit 35 having an electrolyte membrane supply roll 31 and a membrane / catalyst layer assembly winding roll 32, And a pair of transfer film feeding sections 36 having a transfer film supply roll 33 and a base film take-up roll 34. First, the electrolyte membrane supply roll 31 has a long electrolyte membrane 1, and the transfer film supply roll 33 has a long transfer film 2 in which a catalyst layer 3 is coated on a base film 5. The electrolyte membrane 1 and the transfer film 2 are wound around a membrane / catalyst layer assembly winding roll 32 and a base film winding roll 34, respectively. At this time, the transfer film 2 is disposed on both surfaces of the electrolyte membrane 1 so that the catalyst layer 3 faces the electrolyte membrane 1. Then, the electrolyte membrane 1 and the transfer film 2 arranged in this way can be sandwiched from the back surface (base film 5 side) of each transfer film 2, that is, the pair of heat rolls 7 is provided with the electrolyte membrane 1 and the transfer film 2. It is arranged so that it can approach and separate from the center.

  Next, materials for the electrolyte membrane 1 and the transfer film 2 will be described. The electrolyte membrane 1 is formed, for example, by applying a solution containing a hydrogen ion conductive polymer electrolyte on a substrate and drying it. Examples of the hydrogen ion conductive polymer electrolyte include a perfluorosulfonic acid-based fluorine ion exchange resin, more specifically, a perfluorocarbonsulfonic acid-based resin in which the C—H bond of a hydrocarbon ion-exchange membrane is substituted with fluorine. Examples include polymers (PFS polymers). By introducing a fluorine atom having high electronegativity, it is chemically very stable, the dissociation degree of the sulfonic acid group is high, and high ion conductivity can be realized. Specific examples of such a hydrogen ion conductive polymer electrolyte include “Nafion” (registered trademark) manufactured by DuPont, “Flemion” (registered trademark) manufactured by Asahi Glass Co., Ltd., and “Aciplex” manufactured by Asahi Kasei Corporation. ”(Registered trademark),“ Gore Select ”(registered trademark) manufactured by Gore, and the like. The concentration of the hydrogen ion conductive polymer electrolyte contained in the hydrogen ion conductive polymer electrolyte-containing solution is usually about 5 to 60% by weight, preferably about 20 to 40% by weight. In addition, the film thickness of the electrolyte membrane 1 is about 20-250 micrometers normally, Preferably it is about 20-80 micrometers.

  The transfer film 2 is prepared by mixing and dispersing carbon particles carrying catalyst particles and a hydrogen ion conductive polymer electrolyte in an appropriate solvent to prepare a catalyst paste, and a catalyst layer to be formed is desired. The catalyst paste is preferably coated on the base film 5 through a release layer as necessary according to a known method so as to have a film thickness. The method of applying the catalyst paste is not particularly limited, and for example, general methods such as screen printing, gravure printing, knife coater, bar coater, spray, dip coater, spin coater, roll coater, die coater, curtain coater, etc. Applicable. Examples of the catalyst particles include platinum and platinum compounds. Examples of the platinum compound include an alloy of platinum and at least one metal selected from the group consisting of ruthenium, palladium, nickel, molybdenum, iridium, iron and the like. In general, the catalyst particles contained in the cathode catalyst layer are platinum, and the catalyst particles contained in the anode catalyst layer are an alloy of the metal and platinum. Moreover, as a hydrogen ion conductive polymer electrolyte, the same material as what is used for the electrolyte membrane 1 mentioned above can be used. Examples of the solvent include various alcohols, various ethers, various dialkyl sulfoxides, water, or a mixture thereof. Of these, alcohols are preferable. Examples of alcohols include monohydric alcohols having 1 to 4 carbon atoms such as methanol, ethanol, n-propanol, isopropanol, n-butanol, and tert-butanol, and various polyhydric alcohols.

  Examples of the base film 5 include polyimide, polyethylene terephthalate, polyparvanic acid aramid, polyamide (nylon), polysulfone, polyethersulfone, polyphenylene sulfide, polyether ether ketone, polyetherimide, polyarylate, polyethylene naphthalate. Examples thereof include polymer films such as phthalate.

  Further, heat resistance of ethylene tetrafluoroethylene copolymer (ETFE), tetrafluoroethylene-hexafluoropropylene copolymer (FEP), tetrafluoroperfluoroalkyl vinyl ether copolymer (PFA), polytetrafluoroethylene (PTFE), etc. Fluorine resin can also be used.

  Furthermore, the base film 5 may be a coated paper such as art paper, coated paper, lightweight coated paper, non-coated paper such as notebook paper, copy paper, etc. in addition to the polymer film.

  The thickness of the base film 5 is usually about 6 to 100 μm, preferably about 6 to 50 μm, more preferably about 10 to 30 μm from the viewpoints of handleability and economy.

  Therefore, the base film 5 is preferably a polymer film that is inexpensive and easily available, and more preferably polyethylene terephthalate.

  And after apply | coating a catalyst paste to the base film 5, the transfer film 2 is formed by drying at predetermined temperature and time. A drying temperature is about 40-100 degreeC normally, Preferably it is about 60-80 degreeC. Although depending on the drying temperature, the drying time is usually about 5 minutes to 2 hours, preferably about 10 minutes to 1 hour.

  Next, a method for producing a membrane / catalyst layer assembly and a method for producing a polymer electrolyte fuel cell using the production apparatus will be described with reference to FIGS. First, as shown in FIGS. 1 and 2, the long electrolyte membrane 1 and the transfer film 2 set on the electrolyte membrane supply roll 31 and the transfer film supply roll 33 are sent in the same length direction, and the membrane / catalyst layer It is wound around the joined body winding roll 32 and the base film winding roll 34. The pair of heat rolls 7 intermittently pressurize at a predetermined pressure from the back surfaces (base film 5 side) of both transfer films 2, whereby the catalyst layer 3 of the transfer film 2 is intermittently formed on both surfaces of the electrolyte membrane 1. Transcribed. At this time, the electrolyte membrane feed unit 35 is a continuous feed drive, and always feeds the electrolyte membrane 1 continuously at a constant speed, while the transfer film feed unit 36 is an intermittent feed drive, The film 2 is intermittently fed, and the pair of heat rolls 7 sandwich the electrolyte membrane 1 and the transfer film 2 in conjunction with the feed of the transfer film 2 of the transfer film feed unit 36 and pressurize them with a predetermined pressure. FIG. 3A shows a correspondence relationship between the pressurized state of the heat roll 7, the feeding state of the electrolyte membrane feeding unit 35, and the transfer film feeding unit 36. The horizontal axis represents time, and the vertical axis represents ON / OFF of the pressurized state or the feeding state. FIGS. 3B and 3C show the positional relationship of the catalyst layer 3 on the electrolyte membrane 1 formed by this correspondence and the state of the transfer film 2 after transfer. As is clear from these figures, when the heating roller 7 is in the ON state, the transfer film feeding unit 36 is also in the ON state, and the electrolyte membrane feeding unit 35 is always in the ON state. At this time, the catalyst layer 3 of the transfer film 2 is transferred onto the electrolyte membrane 1, and the membrane / catalyst layer assembly 9 is manufactured (see FIG. 2A). In addition, when the pressurization state of the heat roll 7 is OFF, the transfer state of the transfer film feed unit 36 is also OFF, and only the feed state of the electrolyte membrane feed unit 35 is ON. It is formed (see FIG. 2B).

  As described above, the catalyst layers 3 are intermittently transferred to both surfaces of the electrolyte membrane 1 to form the spaces S between the catalyst layers 3, whereby a plurality of membrane / catalyst layer assemblies 9 are manufactured. The membrane / catalyst layer assembly 9 manufactured in this way is wound around the membrane / catalyst layer assembly winding roll 32. Moreover, the base film 5 is peeled off from the catalyst layer 3 after the transfer, wound up by the base film winding roll 34, and collected. The temperature of the hot roll 7 is preferably 80 to 200 ° C, more preferably 100 to 150 ° C, and the pressure is preferably 0.5 to 20 MPa, more preferably 1 to 10 MPa. Further, the feeding speed of the electrolyte membrane 1 and the transfer film 2 is preferably 0.001 to 10 m / min, and more preferably 0.01 to 1 m / min.

  Then, the plurality of membrane / catalyst layer assemblies 9 manufactured in this way are cut out for each membrane / catalyst layer assembly 9 as shown in FIG. 3, the electrode base material 15 is laminated and formed, and the membrane / electrode assembly 17 is formed. Then, the membrane / electrode assembly 19 is sandwiched by the separator 21 via the gasket 19 so that the gasket 19 fits in the gap S, and the fuel cell 23 is manufactured. In the above example, each membrane / catalyst layer assembly 9 is cut out for each membrane / electrode assembly 17 to form the membrane / electrode assembly 17, and the membrane / electrode assembly 17 is sandwiched by the separator 21 via the gasket 19. Although the fuel cell 23 is formed by cutting out the membrane / catalyst layer assembly 9 for each desired unit, the fuel cells 23 may be cut out to form one fuel cell 23.

  As described above, the long electrolyte membrane 1 is continuously fed at a constant speed, and the press of the heat roll 7 is intermittently performed from the back surface of the transfer film 2, so that the catalyst layer 3 is spaced on the electrolyte membrane 1. A plurality of membrane / catalyst layer assemblies 9 are manufactured by intermittently transferring the material with S removed. This space | interval S can be made into the site | parts which do not contribute to battery reaction, such as the site | part fitted to a gasket. Further, since the transfer film 2 is fed only when the pressurization state of the heat roll 7 is ON, and when the pressurization state of the heat roll 7 is OFF, the transfer state of the transfer film 2 is turned OFF, FIG. ), The catalyst layer 3 on the transfer film 2 is entirely transferred to the electrolyte membrane 1, and the non-transfer site 11 is not formed between the transfer sites 13, so that a relatively expensive material is used. The amount of catalyst layer 3 used can be reduced, and the cost can be reduced.

  As mentioned above, although one Embodiment of this invention was described, this invention is not limited to this, A various change is possible unless it deviates from the meaning. For example, the hot pressing can be performed not by the pair of heat rolls 7 but by a pair of seal bars used for sealing processing such as heat sealing. Moreover, in the said embodiment, although the transfer film 2 is arrange | positioned 1 each on the upper and lower sides of the electrolyte membrane 1, respectively, as shown in FIG. It is also possible to change the number of films 2. By doing so, the membrane / catalyst layer assembly 9 can be more efficiently manufactured. In addition, although an example in which the transfer film 2 has two rows has been described, it is of course possible to transfer using three or more rows of transfer films 2 in parallel. Furthermore, a plurality of rows of catalyst layers 3 are transferred at a constant interval by using a single row of transfer film 2 and a plurality of heat rolls 7 installed in the width direction, etc., and a plurality of rows of membrane / catalyst layer assemblies 9 are transferred. It is also possible to form In the above embodiment, the catalyst layer 3 is transferred to both surfaces of the electrolyte membrane 1, but the catalyst layer 3 may be transferred only to one surface of the electrolyte membrane 1.

  Further, as shown in FIG. 5, the hot pressing can be performed not by the pair of heat rolls 7 but by the pair of heat stampers 71. In this method, when the catalyst layer 3 is transferred onto the electrolyte membrane 1, the feeding state of the electrolyte membrane feeding unit 35 and the transfer film feeding unit 36 is OFF, that is, the stopped state, and the pressurizing state of the thermal stamper 71 is set to ON. (FIG. 5A). And when forming the space | interval S, the pressurization state of the heat stamper 71 becomes OFF, and the electrolyte membrane sending part 35 sends the electrolyte membrane 1 in the length direction by the desired space S. At this time, the feeding state of the transfer film feeding portion 36 is OFF, that is, stopped (FIG. 5B). After the electrolyte membrane 1 has been sent by the interval S, the electrolyte membrane feed unit 35 and the transfer film feed unit 36 are turned off after the electrolyte membrane 1 and the transfer film 2 have been fed by the amount of the catalyst layer 3, Thus, the pressurization state of the thermal stamper 7 is turned ON, and the catalyst layer 3 is transferred to the electrolyte membrane 1 again. As another method, the catalyst layer 3 is transferred onto the electrolyte membrane 1 by turning off the feeding state of the electrolyte membrane feeding unit 35 and the transfer film feeding unit 36 and turning on the pressing state of the thermal stamper 71. Thereafter, in order to form the interval S, the pressurization state of the thermal stamper 71 is turned OFF, the feeding speed of the electrolyte membrane feeding section 35 is made faster than the feeding speed of the transfer film feeding section 36, and the electrolyte membrane feeding section 35 is The electrolyte membrane 1 is fed in the length direction by the distance S and the catalyst layer 3, and the transfer film feed unit 36 feeds the transfer film 2 by the amount of the catalyst layer 3. After that, with the feeding state of the electrolyte membrane feeding unit 35 and the transfer film feeding unit 36 turned off and stationary again, the pressure state of the thermal stamper 71 is turned on, and the catalyst layer 3 of the transfer film 2 is placed on the electrolyte membrane 1. The catalyst layer 3 can be intermittently transferred to the electrolyte membrane 1 with an interval S.

  When the transfer is performed by the heat stamper 71 instead of the heat roll 7 in this way, the shape of the catalyst layer 3 can also be changed to a desired shape only by changing the shape of the heat stamper 71 to a desired shape.

  Furthermore, as shown in FIG. 6, hot pressing can be performed by a thermal head 72 instead of the hot roll 7. The thermal head 72 has a structure in which a plurality of heating elements capable of rapidly raising and lowering the temperature are arranged one-dimensionally on the tip side of the thermal head 72 that contacts the electrolyte membrane 1 or the transfer film 2. In the transfer method using the thermal head 72, first, the pair of thermal heads 72 are sandwiched from the back surfaces of the two transfer films 2 and pressed with the predetermined pressure. Then, the temperature of each heating element of the thermal head 72 is raised to the above predetermined temperature, and the electrolyte membrane feeding unit 35 and the transfer film feeding unit 36 send the electrolyte membrane 1 and the transfer film 2 in the length direction. The catalyst layer 3 of the transfer film 2 is transferred. Then, the temperature of each heating element of the thermal head 72 is lowered, the feeding state of the transfer film feeding unit 36 is turned off, the feeding state of the electrolyte membrane feeding unit 35 is turned on, and the desired interval S is fed. This process is repeated to produce a plurality of membrane / catalyst layer assemblies 9. At the time of this transfer, by raising only the temperature of the selected heating element among the plurality of heating elements, it becomes possible to transfer the catalyst layer 3 only at the portion corresponding to the heating element whose temperature is rising. . By doing so, it is possible to easily manufacture membrane / catalyst layer assemblies having different shapes in the same manufacturing process without exchanging a hot press or a transfer film. Of course, you may raise the temperature of all the some heat generating bodies.

  Furthermore, as another transfer method using the thermal head 72, when the catalyst layer 3 of the transfer film 2 is transferred to the electrolyte membrane 1, the electrolyte membrane feed portion 35 and the transfer film feed portion 36 are the electrolyte membrane 1 and the transfer film as described above. 2 is transferred in the length direction, and the thermal head 72 is fixed to perform transfer. However, the feeding state of the electrolyte membrane feeding unit 35 and the transfer film feeding unit 36 is turned off, and the heating element of the thermal head 72 is pressurized and heated. The transfer can also be performed by moving the thermal head 72.

1 is a perspective view showing an embodiment of an apparatus for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell according to the present invention. It is the front view (a) in the transfer state of FIG. 1, and the front view (b) in a non-transfer state. The figure (a) showing the correspondence of the pressurization state of the hot roll in this embodiment, the electrolyte membrane, and the transfer state of the transfer film, and the positional relationship of the catalyst layer on the electrolyte membrane formed by the correspondence It is the top view (b) represented, and the top view (c) showing the state of the transfer film after transcription | transfer. It is the top view (a) showing the state of the transfer film after transfer in other embodiments, and the top view (b) showing the positional relationship of the catalyst layer on an electrolyte membrane. It is the front view (a) in the transfer state which shows other embodiment of the manufacturing apparatus of the membrane / catalyst layer assembly for solid polymer fuel cells concerning the present invention, and the front view (b) in the non-transfer state. It is a front view which shows other embodiment of the manufacturing apparatus of the membrane / catalyst layer assembly for solid polymer fuel cells concerning the present invention. 1 is a front cross-sectional view showing a polymer electrolyte fuel cell produced by an embodiment of a method for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell according to the present invention.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Electrolyte membrane 2 Transfer film 3 Catalyst layer 5 Base film 7 Heat roll 9 Membrane / catalyst layer assembly 15 Electrode base material 17 Membrane / electrode assembly 21 Separator 23 Polymer electrolyte fuel cell 35 Electrolyte membrane feed part 36 Transfer film Feeder 71 Thermal stamper 72 Thermal head S Spacing

Claims (11)

In the method for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell in which catalyst layers are formed on both sides of the electrolyte membrane,
A first step of preparing a long electrolyte membrane;
A second step of preparing a transfer film in which the catalyst layer is formed on a long base film;
A third step of disposing the transfer film on at least one surface of the electrolyte membrane such that the catalyst layer of the transfer film faces the electrolyte membrane;
And a fourth step of intermittently transferring the catalyst layer of the transfer film to at least one surface of the electrolyte membrane at a desired interval.   In the fourth step, the long electrolyte membrane is continuously fed in the length direction, the long transfer film is intermittently fed in the same direction as the electrolyte membrane, and a hot roll feeds the transfer film. 2. The membrane according to claim 1, wherein the catalyst layer is intermittently transferred at a desired interval to at least one surface of the electrolyte membrane by sandwiching the electrolyte membrane and the transfer film in conjunction with each other. -Manufacturing method of catalyst layer assembly.   In the fourth step, the long electrolyte membrane is continuously fed in the length direction, the long transfer film is intermittently fed in the same direction as the electrolyte membrane, and a seal bar feeds the transfer film. 2. The membrane according to claim 1, wherein the catalyst layer is intermittently transferred at a desired interval to at least one surface of the electrolyte membrane by sandwiching the electrolyte membrane and the transfer film in conjunction with each other. -Manufacturing method of catalyst layer assembly.   In the fourth step, the long electrolyte membrane and transfer film are intermittently sent in the length direction, and a thermal stamper sandwiches the electrolyte membrane and transfer film in conjunction with intermittent stop of the electrolyte membrane and transfer film. 2. The method for producing a membrane / catalyst layer assembly according to claim 1, wherein the catalyst layer is intermittently transferred to at least one surface of the electrolyte membrane at a desired interval.   In the fourth step, while the thermal head sandwiches the electrolyte membrane and the transfer film with a constant pressure, the long electrolyte membrane is continuously sent in the length direction, and the long transfer film Are intermittently fed in the same direction as the electrolyte membrane, and the temperature of the thermal head is raised in conjunction with the feed of the transfer film, so that the catalyst layer is spaced at least on one surface of the electrolyte membrane. The method for producing a membrane / catalyst layer assembly according to claim 1, wherein the transfer is performed intermittently. In a method for producing a polymer electrolyte fuel cell comprising a membrane / electrode assembly comprising a catalyst layer and an electrode substrate on each side of an electrolyte membrane, and a pair of separators sandwiching the membrane / electrode assembly,
A first step of preparing a long electrolyte membrane;
A second step of preparing a transfer film in which the catalyst layer is formed on a long base film;
A third step of disposing the transfer film on at least one surface of the electrolyte membrane such that the catalyst layer of the transfer film faces the electrolyte membrane;
A fourth step of intermittently transferring the catalyst layer of the transfer film to at least one surface of the electrolyte membrane at a desired interval;
A fifth step of laminating and forming the electrode base material on the catalyst layer;
And a sixth step of sandwiching the membrane-electrode assembly by the separator. A method for producing a polymer electrolyte fuel cell, comprising: In an apparatus for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell in which catalyst layers are formed on both surfaces of an electrolyte membrane,
An electrolyte membrane feed section for feeding the long electrolyte membrane in the length direction;
A transfer film feeding section for feeding a transfer film in which the catalyst layer is formed on a long base film in the same direction as the electrolyte membrane on at least one surface side of the electrolyte membrane;
A pair of heat rolls installed so as to be able to sandwich the electrolyte membrane and the transfer film,
The electrolyte membrane feed unit is a continuous feed drive, the transfer film feed unit is an intermittent feed drive, and the pair of heat rolls sandwich the electrolyte membrane and the transfer film in conjunction with the feed of the transfer film feed unit. An apparatus for producing a membrane / catalyst layer assembly, characterized in that it is configured to be attached. In an apparatus for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell in which catalyst layers are formed on both surfaces of an electrolyte membrane,
An electrolyte membrane feed section for feeding the long electrolyte membrane in the length direction;
A transfer film feeding section for feeding a transfer film in which the catalyst layer is formed on a long base film in the same direction as the electrolyte membrane on at least one surface side of the electrolyte membrane;
A pair of seal bars installed so as to be able to sandwich the electrolyte membrane and the transfer film,
The electrolyte membrane feed unit is a continuous feed drive, the transfer film feed unit is an intermittent feed drive, and the pair of seal bars sandwich the electrolyte membrane and the transfer film in conjunction with the feed of the transfer film feed unit. An apparatus for producing a membrane / catalyst layer assembly, characterized in that it is configured to be attached. In an apparatus for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell in which catalyst layers are formed on both surfaces of an electrolyte membrane,
An electrolyte membrane feed section for feeding the long electrolyte membrane in the length direction;
A transfer film feeding section for feeding a transfer film in which the catalyst layer is formed on a long base film in the same direction as the electrolyte membrane on at least one surface side of the electrolyte membrane;
A pair of thermal stampers installed so as to be able to sandwich the electrolyte membrane and the transfer film,
The electrolyte membrane feeding unit and the transfer film feeding unit are intermittently fed, and the pair of thermal stampers sandwich the electrolyte membrane and the transfer film in conjunction with the intermittent stop of the electrolyte membrane and the transfer film, whereby the catalyst An apparatus for producing a membrane / catalyst layer assembly, wherein the layer is intermittently transferred to at least one surface of the electrolyte membrane at a desired interval. In an apparatus for producing a membrane / catalyst layer assembly for a polymer electrolyte fuel cell in which a catalyst layer is formed on each side of an electrolyte membrane,
An electrolyte membrane feed section for feeding the long electrolyte membrane in the length direction;
A transfer film feeding section for feeding a transfer film in which the catalyst layer is formed on a long base film in the same direction as the electrolyte membrane on at least one surface side of the electrolyte membrane;
A pair of thermal heads sandwiching the electrolyte membrane and the transfer film at a constant pressure,
The electrolyte membrane feed unit is a continuous feed drive, the transfer film feed unit is an intermittent feed drive, and the temperature of the pair of thermal heads rises in conjunction with the feed of the transfer film feed unit. An apparatus for producing a membrane / catalyst layer assembly.   The pair of thermal heads includes a plurality of heating elements at a tip portion in contact with the electrolyte membrane or the transfer film, and raises the temperature of the heating element selected from the plurality of heating elements. The apparatus for producing a membrane / catalyst layer assembly according to claim 5.

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