JP2006134611A - Manufacturing device and manufacturing method of junction - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a manufacturing device and a manufacturing method of a junction having high productivity capable of preventing warp of the junction. <P>SOLUTION: The manufacturing device of junction manufacturing a junction of catalyst layer and electrolyte film or that of diffusion layer and a catalyst layer carrying electrolyte layer comprises a heating/pressing means forming the junction by continuously transferring a transfer layer on a base material by heating and pressing a carrying base material, carrying a plurality of transfer layers which are either the catalyst layers or the diffusion layers on one face, and a base material composed of a layer to be transported which is either the electrolyte film or the catalyst layer carrying electrolyte layer, in a state that the transfer layer is made to contact with the layer to be transferred; and a cooling/pressing means continuously cooling and pressing the junction. The heating/pressing means and the cooling/pressing means are the junction manufacturing device contacting with respective transfer layers in a manner of face contact or a plurality of line contacts. <P>COPYRIGHT: (C)2006,JPO&NCIPI

Description

  The present invention relates to a joined body manufacturing apparatus and a joined body manufacturing method, and more specifically, a joined body manufacturing apparatus for manufacturing a joined body of a catalyst layer and an electrolyte membrane, or a joined body of an electrolyte membrane having a catalyst layer and a diffusion layer. And a joined body manufacturing method.

  As one of the countermeasures for environmental problems and resource problems, an electrochemical reaction using an oxidizing gas such as oxygen or air and a reducing gas such as hydrogen or methane (fuel gas) or a liquid fuel such as methanol as raw materials Fuel cells that generate electricity by converting chemical energy into electrical energy have attracted attention. The fuel cell is provided with a fuel electrode (anode catalyst layer) on one side of the electrolyte membrane and an air electrode (cathode catalyst layer) on the other side of the electrolyte membrane with the electrolyte membrane sandwiched between them. Further, a diffusion layer is further provided, and a battery is formed by sandwiching these layers between separators provided with a path for supplying raw materials, and power is generated by supplying raw materials such as hydrogen and oxygen to each catalyst layer.

  Fuel cells have been studied in various ways as a clean energy source due to the abundance of raw material gas and liquid fuel used for power generation and the fact that the substance discharged from the power generation principle is water. ing.

  As a joined body manufacturing apparatus and manufacturing method for manufacturing a joined body of a catalyst layer and an electrolyte membrane used in such a fuel cell or the like, or a joined body of an electrolyte membrane having a catalyst layer and a diffusion layer, for example, a patent Document 1 proposes a method in which a catalyst layer of a catalyst-carrying film is transferred onto an electrolyte membrane by a hot press or a hot roller and integrated to form a catalyst layer-electrolyte assembly.

  In Patent Document 2, a catalyst-carrying film and a preheated electrolyte membrane are hot-pressed by a heating and pressing roller to transfer a catalyst layer, and then cooled by a cooling roller and peeled off by a peeling roller. A body manufacturing apparatus has been proposed.

Japanese Patent Laid-Open No. 10-64574 JP 2001-196070 A

  However, in the transfer by hot pressing as in the method described in Patent Document 1, the catalyst layer supporting film and the electrolyte membrane are pressed one by one to transfer the catalyst layer, and then one by one in the state as it is. Since it is necessary to cool, it takes a long time and productivity is poor.

  Moreover, in the transfer by the hot roller (heating and pressing roller) described in Patent Document 1 and Patent Document 2, the contact between the catalyst layer carrying film and the electrolyte membrane and the hot roller is a line contact, and the catalyst layer carrying film In addition, heat cannot be uniformly applied to the entire electrolyte membrane. In addition, warpage of the joined body may occur in the cooling process after heating and pressing by the hot roller. Even when a cooling step using a cooling roller is provided after heating and pressing as in Patent Document 2, the contact between the catalyst layer-supporting film and the electrolyte membrane and the cooling roller is a line contact, and the catalyst layer-supporting film and the entire electrolyte membrane are Since it is not cooled uniformly, warping of the joined body may occur. The same problem also occurs in the manufacture of a joined body of a catalyst layer-supported electrolyte membrane and a diffusion layer.

  In the present invention, the transfer by heating and pressurization of the catalyst layer to the electrolyte membrane using the catalyst layer-supporting film, or the transfer by heating and pressurization of the diffusion layer to the catalyst layer-supporting electrolyte membrane using the diffusion layer support film, It is the joined body manufacturing apparatus and joined body manufacturing method which can prevent generation | occurrence | production of the curvature of the obtained joined body.

  Moreover, this invention is a bonded body manufacturing apparatus and a bonded body manufacturing method with high productivity.

  The present invention is a joined body manufacturing apparatus for manufacturing a joined body of a catalyst layer and an electrolyte membrane or a joined body of a diffusion layer and a catalyst layer-supporting electrolyte membrane, and a plurality of the catalyst layers and the diffusion layers. A transfer substrate and a transfer layer, and a transfer substrate and a transfer layer that is one of the electrolyte membrane and the catalyst layer-supported electrolyte membrane. Heating and pressurizing means for heating and pressurizing in contact with each other to continuously transfer the transfer layer to the substrate to form a joined body; and cooling and pressurizing means for continuously cooling and pressurizing the joined body. The heating and pressing unit and the cooling and pressing unit are in surface contact or multiple line contact with each of the transfer layers.

  Moreover, in the joined body manufacturing apparatus, at least one of the heating and pressing unit and the cooling and pressing unit includes a heat conductive elastic body, and the heat conductive elastic body may be in surface contact or in multiple line contact. preferable.

  Moreover, in the joined body manufacturing apparatus, it is preferable that at least one of the heating and pressing unit and the cooling and pressing unit includes a metal material, and the metal material is in surface contact or multiple line contact.

  In the joined body manufacturing apparatus, it is preferable that at least one of the heating and pressing unit and the cooling and pressing unit is an endless track system.

  In the joined body manufacturing apparatus, it is preferable that at least one of the heating and pressing unit and the cooling and pressing unit includes a plurality of rollers, and the plurality of rollers are in contact with each other by a plurality of lines.

  In the joined body manufacturing apparatus, it is preferable that the plate made of the thermally conductive elastic body is in surface contact.

  In the joined body manufacturing apparatus, it is preferable that a belt made of the heat conductive elastic body is in surface contact.

  Moreover, in the joined body manufacturing apparatus, it is preferable that the thermal conductive elastic body is subjected to pressure deformation and brought into surface contact.

  Furthermore, the present invention is a joined body manufacturing method for manufacturing a joined body of a catalyst layer and an electrolyte membrane or a joined body of a diffusion layer and a catalyst layer-supported electrolyte membrane, wherein either the catalyst layer or the diffusion layer is used. The transfer substrate and the transfer layer are formed by supporting a transfer substrate having a plurality of transfer layers supported on one surface and a transfer substrate that is one of the electrolyte membrane and the catalyst layer-supporting electrolyte membrane. And a heating and pressurizing step of continuously transferring and transferring the transfer layer to the substrate to form a joined body, and cooling and pressurizing for continuously cooling and pressurizing the joined body. In the heating and pressing step and the cooling and pressing step, the heating and pressing and the cooling and pressing are performed by surface contact or multi-line contact with respect to each transfer layer.

  In the present invention, in the transfer by heating and pressurization to the electrolyte membrane of the catalyst layer using the catalyst layer-supporting film, or in the transfer by heating and pressurization to the catalyst layer-supporting electrolyte membrane of the diffusion layer using the diffusion layer support film, Bonded body manufacturing apparatus and bonded body capable of preventing warpage of the obtained bonded body by performing surface pressure or multiple line contact with one surface of each catalyst layer or each diffusion layer and heating and pressurizing and cooling and pressing. A body manufacturing method can be provided.

  Moreover, in this invention, the joining body manufacturing apparatus and joining body manufacturing method with high productivity can be provided by carrying out heating pressurization and cooling pressurization continuously.

  Hereinafter, a bonded body manufacturing apparatus and a bonded body manufacturing method according to an embodiment of the present invention will be described.

  A joined body manufacturing apparatus according to an embodiment of the present invention is a joined body manufacturing apparatus that manufactures a joined body of a catalyst layer and an electrolyte membrane or a joined body of a diffusion layer and a catalyst layer-supported electrolyte membrane. A transfer substrate and a substrate to be transferred, each of which includes a substrate having a plurality of transfer layers that are one of the layers supported on one surface, and a substrate having a transfer layer that is one of the electrolyte membrane and the catalyst layer-supported electrolyte membrane. A heating and pressurizing means for continuously transferring and transferring the transfer layer to the substrate to form a joined body, and a cooling and pressurizing means for continuously cooling and pressurizing the joined body. The heating and pressing means and the cooling and pressing means are in surface contact or multiple line contact with each transfer layer.

  In this specification, a case where a roller and a heated pressure member or a cooled pressure member are in contact with each other with a line or an extremely narrow width as in the conventional roller system is referred to as “line contact”, as in this embodiment. The case where the contact portion of the heating / pressurizing unit or the cooling / pressurizing unit and the heated / pressurized member or the cooled / pressurized member contact with each other with a certain width or more is referred to as “surface contact”. Further, a plurality of “line contact” by a roller or the like is performed on one heated pressure member or a cooled pressure member, and the heating pressure member or the cooling pressure member and the heated pressure member or the cooled pressure member are heated. Is called “multiple line contact”.

  FIG. 1 shows an example of the configuration of a joined body manufacturing apparatus 1 according to an embodiment of the present invention. The joined body manufacturing apparatus 1 includes a base material supply roller 10, support base material supply rollers 12A and 12B, guide rollers 14A and 14B, heating and pressing units 16A and 16B, cooling and pressing units 18A and 18B, and a joined body winding roller 20. And film take-up rollers 22A and 22B.

  In the joined body manufacturing apparatus 1, a supporting substrate supply roller 12 </ b> A that supplies a supporting substrate having a transfer layer supported on one surface is provided above a substrate supplying roller 10 that supplies a substrate composed of a transfer layer. A supporting base material supply roller 12 </ b> B is disposed below the material supply roller 10. A guide roller 14A is disposed on the right side of the base material supply roller 10, and further, heating and pressurizing units 16A and 16B are provided on the right side from the base material supplied from the base material supply roller 10 and the supporting base material supply rollers 12A and 12B. It arrange | positions so that a base material and a support base material may be pinched | interposed respectively up and down with respect to the surface of the support base material supplied. Further, on the right side, the cooling and pressurizing portions 18A and 18B are respectively located above and below the surface of the base material supplied from the base material supply roller 10 and the surface of the support base material supplied from the support base material supply rollers 12A and 12B. Between the substrate and the supporting substrate. A guide roller 14B is disposed on the right side of the cooling and pressurizing portions 18A and 18B, and a joined body winding roller 20 for winding the joined body obtained on the right side thereof is disposed. Further, a film take-up roller 22 </ b> A for taking up the carrier substrate from which the transfer layer has been peeled is disposed above the joined body take-up roller 20, and a film take-up roller 22 </ b> B is disposed below the joined body take-up roller 20.

  Next, an operation of manufacturing a joined body by the joined body manufacturing apparatus 1 according to the present embodiment will be described with reference to FIG. The base material supply roller 10 unwinds and supplies the electrolyte membrane 24 which is a base material made of a transfer layer. As shown in FIG. 2, the supporting substrate supply roller 12 </ b> A has a catalyst layer supporting film 26 </ b> A in which a fuel electrode (anode catalyst layer) 28 that is a transfer layer is supported on one surface by a film 32 that is a supporting substrate. The material supply roller 12B unwinds and supplies the catalyst layer carrying film 26B, in which the air electrode (cathode catalyst layer) 30 as the transfer layer is carried on one surface of the film 32 as the carrying base. The electrolyte membrane 24 and the catalyst layer supporting films 26A and 26B aligned with each other through the guide roller 14A are divided into catalyst layers (transfer layers) 28 and 30 and an electrolyte membrane 24 (transfer target layer) by the heating and pressurizing portions 16A and 16B. It is heated and pressurized in the contact state and joined. Thereafter, the joined joined body is cooled and pressurized by the cooling and pressurizing portions 18A and 18B, and after passing through the guide roller 14B, the film 32 is peeled off and taken up by the film take-up rollers 22A and 22B, respectively. The joined body, that is, the electrolyte membrane 24 on which the catalyst layers 28 and 30 are formed on the surface is wound up by the roller 20.

  In this way, the fuel electrode 28 is continuously transferred to one surface of the electrolyte membrane 24 and the air electrode 30 is transferred to the other surface so as to face each other with the electrolyte membrane 24 interposed therebetween, thereby forming a joined body.

  As shown in FIG. 3, the heating and pressing units 16A and 16B include a metal plate 34, a heat conductive elastic body 36, a roller 38, a heating unit 40, and the like. A plurality of metal plates 34 having a plate-like thermally conductive elastic body 36 on the surface thereof are provided along the outer periphery of one or more, preferably a plurality of cylindrical, columnar, etc. rollers 38. , Endless orbit). The surface of the roller 38 is heated by the heating unit 40 provided inside the roller 38, and the heat conductive elastic body 36 is heated through the metal plate 34. As shown in FIGS. 1 and 3, the metal plate 34 having the heat conductive elastic body 36 constituting the caterpillar on the surface, the electrolyte membrane 24, and the catalyst layer supporting films 26A and 26B are conveyed so as to be pressed, The heated thermally conductive elastic body 36 is in surface contact with the catalyst layers 28 and 30 of the catalyst layer supporting films 26A and 26B through the film 32 to heat and press one surface of the catalyst layers 28 and 30. Thus, the electrolyte membrane 24 and the catalyst layers 28 and 30 are joined. Thereby, heating and pressurization can be performed uniformly over the entire surfaces of the catalyst layers 28 and 30, and warpage of the joined body can be prevented. Moreover, it can heat and press continuously by using a caterpillar system.

  The guide roller 14A rotates to synchronize with the conveying speed of the electrolyte membrane 24 due to the rotation of the caterpillar in the heating and pressurizing units 16A and 16B, and tension is applied to the electrolyte membrane 24 when heated and pressurized by the heating and pressurizing units 16A and 16B. To prevent it from working. By doing so, deformation of the electrolyte membrane 24 during heating and pressing can be suppressed.

  In the heating and pressurizing portions 16A and 16B, the area of one contact portion (here, one heat conductive elastic body 36) when contacting the transfer layer in a pressable manner is one catalyst layer 28 and 30 to be transferred. As long as it is at least the area. Thereby, it is possible to uniformly heat and press the entire surfaces of the catalyst layers 28 and 30 to be transferred. Moreover, if this contact area is more than the area which can heat-press with respect to the whole surface of the some catalyst layers 28 and 30, productivity can be improved further.

  The metal plate 34 and the roller 38 are not particularly limited as long as the metal plate 34 and the roller 38 are metal materials having high heat capacity and heat conductivity such as steel and stainless steel.

  The heat conductive elastic body 36 is not particularly limited as long as it is an elastic body having high heat capacity, heat conductivity, and heat resistance. In addition, if the elasticity of the elastic body is too high or too low, heat cannot be applied uniformly and bonding is not sufficiently performed. Therefore, it is preferable to select an elastic body having an appropriate elasticity. Preferred examples of the elastic body include resins such as polyethylene, various natural rubbers, various synthetic rubbers, and rubbers obtained by vulcanizing them. In addition, a filler or the like may be added as necessary to adjust mechanical strength, elasticity, and the like.

  The heating unit 40 is not particularly limited as long as it can heat the roller 38, but various heaters, various heating media, and the like can be used. In order to uniformly heat the metal plate 34, the heat conductive elastic body 36, and the roller 38, the heating unit 40 preferably uses a heat medium such as steam or various oils. In this case, a heat medium such as steam and various oils can be supplied from the outside.

  As shown in FIG. 4, the cooling and pressurizing units 18A and 18B include a metal plate 42, a heat conductive elastic body 44, a roller 46, a cooling unit 48, and the like. A plurality of metal plates 42 having a plate-like thermally conductive elastic body 44 on the surface thereof are provided along the outer periphery of one or more, preferably a plurality of cylindrical, columnar, etc. rollers 46. ). The surface of the roller 46 is cooled by the cooling unit 48 provided inside the roller 46, and the heat conductive elastic body 44 is cooled through the metal plate 42. As shown in FIGS. 1 and 4, the metal plate 42 having the heat conductive elastic body 44 constituting the caterpillar on the surface and the joined body are conveyed so as to be pressed, and each of the cooled heat conductive elastic bodies 44 is cooled. The joined body is cooled by surface-contacting the catalyst layers 28 and 30 via the film 32 and cooling and pressurizing one surface of each of the catalyst layers 28 and 30. Thereby, cooling and pressurization can be performed uniformly while keeping the physical constraints on the entire surfaces of the catalyst layers 28 and 30 (while pressure is applied), and warpage of the joined body can be prevented. Further, the cooling and pressurization can be continuously performed by using the caterpillar system.

  Further, in the cooling and pressurizing portions 18A and 18B, the area of one contact portion (here, one heat conductive elastic body 44) when contacting the joined body so as to be pressed is one catalyst layer 28 to be cooled. And an area of 30 or more. Thereby, it is possible to uniformly cool and pressurize the entire surfaces of the catalyst layers 28 and 30 to be cooled. Further, if the contact area is equal to or larger than the area where the entire surface of the plurality of catalyst layers 28 and 30 can be cooled and pressurized, the productivity can be further improved.

  As the metal plate 42, the heat conductive elastic body 44, and the roller 46, the same materials as the metal plate 34, the heat conductive elastic body 36, and the roller 38 of the heating and pressurizing units 16A and 16B can be used.

  The cooling unit 48 is not particularly limited as long as it can cool the roller 46, but various cooling devices, various refrigerants, and the like can be used. In order to uniformly heat the metal plate 42, the heat conductive elastic body 44, and the roller 46, the cooling unit 48 may use water; mixed water such as water / alcohol or water / ethylene glycol; or a refrigerant such as air. preferable. In this case, refrigerants such as water, mixed water, and air can be supplied from the outside.

The electrolyte membrane 24 is not particularly limited as long as it is a material having high ion conductivity such as proton (H ⁺ ) or oxygen ion (O ²⁻ ), and examples thereof include a solid polymer electrolyte membrane and a stabilized zirconia membrane. However, a solid polymer electrolyte membrane such as perfluorosulfonic acid is preferably used. Specifically, Goreselect (registered trademark) of Japan Gore-Tex Corporation, Nafion (registered trademark) of Du Pont (Du Pont), Aciplex (registered trademark) of Asahi Kasei Co., Ltd. Perfluorosulfonic acid solid polymer electrolyte membranes such as Flemion (registered trademark) of Asahi Glass Co., Ltd. can be used. The film thickness of the electrolyte membrane 28 is, for example, in the range of 10 μm to 200 μm, preferably 30 μm to 50 μm.

  As the fuel electrode 28 constituting the catalyst layer supporting film 26A, for example, a catalyst such as carbon in which platinum (Pt) or the like is supported together with another metal such as ruthenium (Ru) is used. The film thickness of the fuel electrode 28 is, for example, in the range of 1 μm to 100 μm, preferably 1 μm to 20 μm.

  As the air electrode 30 constituting the catalyst layer carrying film 26B, for example, a catalyst such as carbon carrying platinum (Pt) or the like is used. The film thickness of the air electrode 30 is, for example, 1 μm to 100 μm, preferably 1 μm to 20 μm.

  The catalyst layer (fuel electrode 28 and air electrode 30) is formed on one or both sides of a film 32 made of a resin such as polytetrafluoroethylene (PTFE) by, for example, a spray method, a printing method, a transfer method, etc. The catalyst layer supporting films 26A and 26B can be obtained. The film thickness of the film 32 is, for example, in the range of 10 μm to 1000 μm, preferably 50 μm to 200 μm.

  In the above description, the example in which the catalyst layers (the fuel electrode 28 and the air electrode 30) are provided on both surfaces of the electrolyte membrane 24 to form a joined body has been described, but at least one of the fuel electrode 28 and the air electrode 30 on one surface of the electrolyte membrane 24. You may comprise the conjugate | zygote manufacturing apparatus 1 which concerns on this embodiment so that this may be provided.

  In the above description, the manufacturing apparatus and the manufacturing method for forming the catalyst layers (the fuel electrode 28 and the air electrode 30) on both surfaces of the electrolyte membrane 24 have been described, but at least one of the fuel electrode 28 and the air electrode 30 is present. Even when the diffusion layer 52 is formed on the catalyst layers 28 and 30 of the catalyst layer-supported electrolyte membrane 50 formed on one side or both sides of the electrolyte membrane 24, the joined body manufacturing apparatus and the joined body manufacturing method according to the present embodiment. Can be used.

  In this case, as shown in FIG. 5, the base material supply roller 10 unwinds and supplies the catalyst layer-supported electrolyte membrane 50 that is a base material made of the transfer layer. As shown in FIG. 2, the supporting substrate supply roller 12A is a diffusion layer supporting film 54A in which a diffusion layer 52A as a transfer layer is supported on a film 68 as a supporting substrate. Then, the diffusion layer carrying film 54B, in which the diffusion layer 52B as the transfer layer is carried on one surface of the film 68 as the carrying substrate, is unwound and supplied. The catalyst layer-supporting electrolyte membrane 50 and the diffusion layer-supporting films 54A and 54B, which are aligned via the guide roller 14A, are diffused (transfer layers) 52A and 52B and the catalyst layer-supporting electrolyte membrane 50 (by the heating and pressurizing portions 16A and 16B. The layer to be transferred) is heated and pressed in contact with the layer to be transferred. Thereafter, the joined joined body is cooled and pressurized by the cooling and pressurizing portions 18A and 18B, and after passing through the guide roller 14B, the film 68 is peeled off and taken up by the film take-up rollers 22A and 22B, respectively. The electrolyte membrane in which the diffusion layer 52 is formed on the joined body, that is, the fuel electrode 28 and the air electrode 30 is wound up by the roller 20.

  In this way, the diffusion layer 52 continuously faces the fuel electrode 28 on one surface of the electrolyte membrane 24 and the air electrode 30 on the other surface with the electrolyte membrane 24 interposed therebetween. Transferred to form a joined body.

  The catalyst layer-supported electrolyte membrane 50 used in this case may be manufactured by the bonded body manufacturing apparatus and the bonded body manufacturing method according to the present embodiment, or other than the bonded body manufacturing method according to the present embodiment. The catalyst layers 28 and 30 may be formed on the electrolyte membrane 24 by the spray method, the printing method, the transfer method, or the like.

  The diffusion layer 52 is not particularly limited as long as it is a material having high conductivity and high diffusibility of raw materials such as fuel and air, but is preferably a porous conductor material. Examples of the highly conductive material include a metal plate, a metal film, a conductive polymer, a carbon material, and the like. Carbon materials such as carbon cloth and glassy carbon are preferable, and porous carbon materials such as carbon cloth are preferable. More preferably. The film thickness of the diffusion layer 52 is, for example, in the range of 100 μm to 1000 μm, preferably 200 μm to 600 μm.

  The heating temperature in the heating and pressurizing parts 16A and 16B is represented by the surface temperature of the heat conductive elastic body 36, the kind of the catalyst material of the fuel electrode 28 and the air electrode 30 to be used, the kind of the electrolyte membrane 24 to be used, and the glass. There is no particular limitation as long as it is determined according to the transition temperature, the type of material of the diffusion layer 52, etc., but it is set in the range of, for example, 100 ° C. to 300 ° C., and the electrolyte membrane 24 is a solid polymer electrolyte such as perfluorosulfonic acid. In the case of a film, it is usually set in the range of 80 ° C to 120 ° C.

  The heating temperatures in the heating and pressurizing sections 16A and 16B may be the same or different, and may be determined according to the types of catalyst materials for the fuel electrode 28 and the air electrode 30 to be used.

  The pressure applied between the heat conductive elastic bodies 36 in the heating and pressurizing units 16A and 16B and the cooling and pressurizing units 18A and 18B depends on the type of the catalyst material of the fuel electrode 28 and the air electrode 30 to be used and the type of the electrolyte membrane 24. It may be set according to the type of material of the diffusion layer 52, etc., and is usually adjusted within the range of 0.1 MPa to 10 MPa, but is not limited thereto. The pressurization is applied by a pressurizer (not shown). Moreover, it is good also as a different pressure by the heating pressurization parts 16A and 16B and the cooling pressurization parts 18A and 18B.

  The cooling temperature in the cooling and pressurizing portions 18A and 18B is represented by the surface temperature of the heat conductive elastic body 36, the kind of the catalyst material of the fuel electrode 28 and the air electrode 30 to be used, the kind of the electrolyte membrane 24 to be used, and the glass. There is no particular limitation as long as it is determined according to the transition temperature, the type of material of the diffusion layer 52, and the like, but it is set in the range of, for example, 10 ° C to 30 ° C, and the electrolyte membrane 24 is a solid polymer electrolyte such as perfluorosulfonic acid. In the case of a film, it is usually set in the range of 20 ° C to 25 ° C.

  The cooling temperatures of the cooling and pressurizing sections 18A and 18B may be the same or different, and may be determined according to the type of the catalyst material of the fuel electrode 28 and the air electrode 30 to be used.

  Further, before forming the catalyst layers 28, 30 or the diffusion layer 52 on the electrolyte membrane 24 or the catalyst layer-supported electrolyte membrane 50, the electrolyte membrane 24 or the catalyst layer-supported electrolyte membrane 50 is formed by preheating means (not shown). You may preheat. By preheating, the binding strength between the catalyst layers 28 and 30 and the electrolyte membrane 24 or the binding strength between the catalyst layer-supporting electrolyte membrane 50 and the diffusion layer 52 is increased, so that the catalyst layers 28 and 30 or the diffusion layer 52 Separation from the electrolyte membrane 24 or the catalyst layer-supported electrolyte membrane 50 can be suppressed.

  Further, the conveying speed of the electrolyte membrane 24 and the catalyst layer carrying film 26, or the catalyst layer carrying electrolyte membrane 50 and the diffusion layer carrying film 54; the contact portions (here, the heating and pressing portions 16A and 16B and the cooling and pressing portions 18A and 18B) The contact area of the heat conductive elastic bodies 36, 44); the heating temperature or the cooling temperature in the heating / pressurizing unit 16 and the cooling / pressurizing unit 18; Alternatively, improvement in productivity can be achieved.

  For example, in order to suppress warpage of the joined body, it is preferable to lower the heating temperature in the heating and pressurizing units 16A and 16B and to reduce the conveyance speed. In order to improve productivity, it is preferable to increase the heating temperature in the heating and pressurizing units 16A and 16B to increase the conveyance speed and to further increase the contact area.

  In the joined body manufacturing apparatus 1 according to the present embodiment, the heating and pressurizing units 16A and 16B and the cooling and pressurizing units 18A and 18B can have the following configuration in addition to the above configuration.

  FIG. 6 is a diagram illustrating another example of the configuration of the joined body manufacturing apparatus 1 according to the embodiment of the present invention. The heating and pressing units 16A and 16B include an elastic belt 56, a roller 38, a heating unit 40, and the like as shown in FIG. An endless elastic belt 56 is held by one or more, preferably a plurality of rollers 38. The surface of the roller 38 is heated by the heating unit 40 provided inside the roller 38, and the elastic belt 56 is heated. The endless elastic belt 56 constituting the caterpillar, the electrolyte membrane 24, and the catalyst layer supporting films 26A and 26B are conveyed in a pressable manner, and the heated elastic belt 56 is heated to each of the catalyst layer supporting films 26A and 26B. The electrolyte membrane 24 and the catalyst layers 28 and 30 are joined by surface-contacting the catalyst layers 28 and 30 via the film 32 and heating and pressurizing one surface of each catalyst layer 28 and 30. Thereby, heating and pressurization can be performed uniformly over the entire surfaces of the catalyst layers 28 and 30, and warpage of the joined body can be prevented. Moreover, it can heat and press continuously by using a belt system.

  Similarly, the cooling and pressurizing units 18A and 18B include an elastic belt 58, a roller 46, a cooling unit 48 and the like as shown in FIG. The elastic belt 58 is held by one or more, preferably a plurality of rollers 46. The surface of the roller 46 is cooled by the cooling unit 48 provided inside the roller 46, and the elastic belt 58 is cooled. The endless elastic body belt 58 constituting the caterpillar and the joined body are conveyed so as to be pressed, and the cooled elastic body belt 58 comes into surface contact with the catalyst layers 28 and 30 via the film 32 to each catalyst layer. By cooling and pressurizing one surface of 28 and 30, the joined body is cooled. Thereby, cooling and pressurization can be performed uniformly over the entire surfaces of the catalyst layers 28 and 30, and warpage of the joined body can be prevented. In addition, the cooling and pressurization can be continuously performed by using the belt system.

  As the elastic belt 58, a material similar to that of the heat conductive elastic body 36 can be used. By using the elastic belt 58, compared to the case of using a combination of the metal plates 34, 42, the heat conductive elastic bodies 36, 44, and the rollers 38, 46 as shown in FIGS. There may be excellent rotational stability such as low vibration.

  The distance between the plurality of rollers 38 that hold the elastic belt 56 and the distance between the plurality of rollers 46 that hold the elastic belt 58 are appropriate so that the elastic belts 56 and 58 do not bend. It is preferable to take a long distance.

  FIG. 7 is a diagram illustrating another example of the configuration of the joined body manufacturing apparatus 1 according to the embodiment of the present invention. The heating and pressing units 16A and 16B include a large deformation elastic body roller 60, a heating unit 40 and the like as shown in FIG. The surface of the large deformation elastic body roller 60 is heated by the heating unit 40. The electrolyte membrane 24 and the catalyst layer supporting films 26A and 26B are conveyed so as to be pressable, and the heated large deformation elastic body roller 60 is pressure deformed by a pressurizing means (not shown), and the catalyst layer supporting film 26A. And the electrolyte membrane 24 and the catalyst layers 28 and 30 are joined by surface-contacting each catalyst layer 28 and 30 of 26B and 26B through the film 32, and heating and pressurizing one surface of each catalyst layer 28 and 30. . Thereby, heating and pressurization can be performed uniformly over the entire surfaces of the catalyst layers 28 and 30, and warpage of the joined body can be prevented. Moreover, it can heat-press continuously by using a large deformation elastic body roller system.

  Similarly, the cooling and pressurizing units 18A and 18B include a large deformation elastic body roller 62, a cooling unit 48 and the like as shown in FIG. The surface of the large deformation elastic body roller 62 is cooled by the cooling unit 48. The joined body is conveyed so as to be pressed, and the cooled large deformable elastic body roller 62 is pressurized and deformed by a pressurizing means (not shown), and is brought into surface contact with the catalyst layers 28 and 30 via the film 32. The joined body is cooled by cooling and pressurizing one surface of each of the catalyst layers 28 and 30. Thereby, cooling and pressurization can be performed uniformly over the entire surfaces of the catalyst layers 28 and 30, and warpage of the joined body can be prevented. Further, the cooling and pressurization can be continuously performed by adopting a large deformation elastic body roller system.

  As the large deformation elastic body roller 62, the same material as the heat conductive elastic body 36 can be used. By using the large deformation elastic body roller 62, the rotation can be performed as compared with the case of using the combination of the metal plates 34 and 42, the heat conductive elastic bodies 36 and 44, and the rollers 38 and 46 as shown in FIGS. It may be excellent in rotational stability such as little vibration at the time.

  FIG. 8 is a diagram illustrating another example of the configuration of the joined body manufacturing apparatus 1 according to the embodiment of the present invention. The heating and pressing units 16A and 16B include a plurality of small metal rollers 64, the heating unit 40, and the like as shown in FIG. The surfaces of the plurality of small metal rollers 64 are heated by the heating unit 40. The electrolyte membrane 24 and the catalyst layer supporting films 26A and 26B are conveyed so as to be pressed, and a plurality of heated small metal rollers 64 are applied to the film 32 on the catalyst layers 28 and 30 of the catalyst layer supporting films 26A and 26B. The electrolyte membrane 24 and the catalyst layers 28 and 30 are joined by heating and pressurizing one surface of each of the catalyst layers 28 and 30 through contact with a plurality of wires. Thereby, heating and pressurization can be performed uniformly over the entire surfaces of the catalyst layers 28 and 30, and warpage of the joined body can be prevented. Moreover, it can heat and press continuously by using a plurality of small roller systems.

  Similarly, the cooling pressurization units 18A and 18B include a plurality of small metal rollers 66, a cooling unit 48, and the like as shown in FIG. The surfaces of the plurality of small metal rollers 66 are cooled by the cooling unit 48. A plurality of small metal rollers 66 that are conveyed so that the bonded body can be pressed and are cooled are in contact with the catalyst layers 28 and 30 through a plurality of lines through the film 32 to cool and press one surface of each catalyst layer 28 and 30. Thus, the joined body is cooled. Thereby, cooling and pressurization can be performed uniformly over the entire surfaces of the catalyst layers 28 and 30, and warpage of the joined body can be prevented. Further, the cooling and pressurization can be continuously performed by using a plurality of small roller systems.

  As the small metal roller 66, a metal material similar to that of the metal plate 34 and the roller 38 can be used. However, since it is a multi-line contact, the diameter of the small metal roller 66 is reduced in order to approach the surface contact. It is preferable to increase the number of installations. Further, the surface of the contact surface of the small metal roller 66 may be covered with an elastic body made of the same material as the heat conductive elastic body 36.

  In the above description, as shown in FIG. 1 and FIGS. 6 to 8, an example in which the heating and pressurizing method of the heating and pressurizing units 16A and 16B and the cooling method of the cooling and pressurizing units 18A and 18B are the same method. As described above, the heating / pressurizing method of the heating / pressurizing units 16A and 16B may be different from the cooling method of the cooling / pressurizing units 18A and 18B.

  In the embodiment shown in FIGS. 6 to 8, the example in which the catalyst layers (the fuel electrode 28 and the air electrode 30) are provided on both surfaces of the electrolyte membrane 24 to form a joined body has been described. The joined body manufacturing apparatus 1 may be configured to provide at least one of the fuel electrode 28 and the air electrode 30.

  In the embodiment shown in FIGS. 6 to 8, the manufacturing apparatus and the manufacturing method for forming the catalyst layers (the fuel electrode 28 and the air electrode 30) on both surfaces of the electrolyte membrane 24 have been described. Even when the diffusion layer 52 is formed on the catalyst layers 28 and 30 of the catalyst layer-supported electrolyte membrane 50 in which at least one of the air electrodes 30 is formed on one side or both sides of the electrolyte membrane 24, the joined body according to this embodiment is manufactured. Apparatus and assembly manufacturing methods can be used.

  Further, in these embodiments, the contact area of the contact portion when contacting the transfer layer or the joined body so as to be pressable in the heating and pressurizing portions 16A and 16B and the cooling and pressurizing portions 18 and 18 (here, the elastic belt 56, 58 and the contact area when the large deformation elastic body rollers 60 and 62 are pressure-deformed and contacted are equal to or larger than the area of one catalyst layer 28 and 30 or the diffusion layer 52 to be transferred or cooled. I just need it. In the case of a plurality of small roller systems, a plurality of small rollers may be in contact with one or more surfaces of one catalyst layer 28 and 30 or one diffusion layer 52 to be transferred. As a result, it is possible to uniformly apply heat and pressure to the catalyst layers 28 and 30 or the diffusion layer 52 to be transferred or cooled. The contact area is preferably an area where the plurality of catalyst layers 28 and 30 or the diffusion layer 52 can come into contact with each other in order to improve productivity.

  The joined body manufactured in this way is sandwiched between, for example, separators provided with raw material supply passages, and an external terminal connected to an external load from the fuel electrode 28 and the air electrode 30 is provided to constitute a battery. If operation is performed by supplying gas, air, etc., electricity can be taken out from the external terminal.

  Examples of the raw material supplied to the fuel electrode 28 include reducing gas (fuel gas) such as hydrogen and methane, or liquid fuel such as methanol. Examples of the raw material supplied to the air electrode 30 include oxidizing gases such as oxygen and air.

For example, when the raw material supplied to the fuel electrode 28 is hydrogen gas and the raw material supplied to the air electrode 30 is air,
2H ₂ → 4H ⁺ + 4e ⁻
Through the reaction formula shown below, hydrogen ions (H ⁺ ) and electrons (e ⁻ ) are generated from hydrogen gas (H ₂ ). The electrons (e ⁻ ) reach the air electrode 30 from the external terminal through the external circuit. In the air electrode 30, oxygen (O ₂ ) in the supplied air, hydrogen ions (H ⁺ ) that have passed through the electrolyte membrane 24, and electrons (e ⁻ ) that have reached the air electrode 30 through an external circuit,
4H ⁺ + O ₂ + 4e ⁻ → 2H ₂ O
Water is produced through the reaction formula shown below. In this way, a chemical reaction occurs in the fuel electrode 28 and the air electrode 30, and charges are generated to function as a battery. And since the component discharged | emitted in a series of reaction is water, a clean battery is comprised.

  In the conventional hot pressing method, the bonded body may be warped in the process of naturally cooling without being physically constrained after stopping the heating and pressing. In addition, in the transfer by the hot roller, the contact between the catalyst layer-carrying film and the electrolyte membrane and the hot roller is a line contact, and heat is not uniformly applied to the entire catalyst layer-carrying film and the electrolyte membrane. The elastic modulus of the electrolyte membrane and the three layers of the upper and lower catalyst layers, or the three layers of the catalyst layer-supporting electrolyte membrane and the upper and lower diffusion layers thereof are different, resulting in a difference in elongation. Furthermore, in the cooling by the cooling roller after heating and pressing, the contact between the catalyst layer supporting film and the electrolyte membrane and the cooling roller is a line contact, and the entire catalyst layer supporting film and the electrolyte membrane and the like are not cooled uniformly. Also, since the entire catalyst layer is cooled without being physically constrained, the amount of shrinkage when each layer stretched during heating is shrunk due to cooling differs due to the difference in elastic modulus of each layer, which may cause warping of the joined body. It was.

  However, the bonded body manufacturing apparatus 1 and the bonded body manufacturing method according to the present embodiment transfer the catalyst layers 28 and 30 to the electrolyte membrane 24 using the catalyst layer supporting film 26 by heating or pressing, or the diffusion layer supporting film 54. In the transfer or the like of the diffusion layer 52 to the catalyst layer-supported electrolyte membrane 50 using heat, the surface of the catalyst layer or one surface of the diffusion layer is contacted with the surface or a plurality of lines to perform heating and pressure and cooling. Thus, heating and pressure can be uniformly applied to the entire surfaces of the catalyst layers 28 and 30 or the diffusion layer 52, and the entire surfaces of the catalyst layers 28 and 30 or the diffusion layer 52 are physically constrained. Therefore, it is possible to prevent warpage of the obtained bonded body. According to the joined body manufacturing apparatus 1 and the joined body manufacturing method according to the present embodiment, the warped magnitude X of the joined body as shown in FIG. 9 is, for example, 5 mm to 5 mm when manufactured by the conventional hot roller method. Compared to 30 mm, it can be suppressed to 1 mm or less. Thereby, for example, characteristics such as power generation performance in the fuel cell can be further improved, and reliability can be improved.

  In addition, in the conventional hot pressing method, it was possible to prevent warping by cooling in the pressed state, but it was not suitable for continuous production because it was allowed to cool in the pressed state one by one. . According to the joined body manufacturing apparatus and the joined body manufacturing method according to the present embodiment, the production time can be reduced because continuous production is possible as compared with the conventional hot press method, and warpage of the obtained joined body. Can be prevented, and productivity can be improved.

It is a figure which shows an example of a structure of the conjugate | zygote manufacturing apparatus which concerns on embodiment of this invention. It is a figure which shows an example of a structure of the catalyst support film which concerns on embodiment of this invention. It is a figure which shows an example of a structure of the heating-pressing part which concerns on embodiment of this invention. It is a figure which shows an example of a structure of the cooling pressurization part which concerns on embodiment of this invention. It is a figure which shows another example of the usage method of the conjugate | zygote manufacturing apparatus which concerns on embodiment of this invention. It is a figure which shows another example of a structure of the conjugate | zygote manufacturing apparatus which concerns on embodiment of this invention. It is a figure which shows another example of a structure of the conjugate | zygote manufacturing apparatus which concerns on embodiment of this invention. It is a figure which shows another example of a structure of the conjugate | zygote manufacturing apparatus which concerns on embodiment of this invention. In embodiment of this invention, it is a figure which shows the mode of the curvature of a conjugate | zygote.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 zygote manufacturing apparatus, 10 base material supply roller, 12A, 12B carrying base material supply roller, 14A, 14B guide roller, 16A, 16B heating pressurization part, 18A, 18B cooling pressurization part, 20 joined body winding roller, 22A, 22B film winding roller, 24 electrolyte membrane, 26A, 26B catalyst layer carrying film, 28 fuel electrode (anode catalyst layer), 30 air electrode (cathode catalyst layer), 32, 68 film, 34, 42 metal plate, 36 , 44 Thermal conductive elastic body, 38, 46 roller, 40 heating section, 48 cooling section, 50 catalyst layer carrying electrolyte membrane, 52A, 52B diffusion layer, 54A, 54B diffusion layer carrying film, 56, 58 elastic belt, 60 , 62 Large deformation elastic body roller, 64, 66 Small metal roller.

Claims (9)

A joined body manufacturing apparatus for manufacturing a joined body of a catalyst layer and an electrolyte membrane or a joined body of a diffusion layer and a catalyst layer-supported electrolyte membrane,
A support substrate formed by supporting a plurality of transfer layers, which are either the catalyst layer or the diffusion layer, on one surface, and a substrate formed of a transfer layer, which is either the electrolyte membrane or the catalyst layer-supported electrolyte membrane And heating and pressurizing means for continuously transferring and transferring the transfer layer to the substrate to form a joined body in a state where the transfer layer and the transferred layer are in contact with each other,
Cooling and pressurizing means for continuously cooling and pressurizing the joined body;
Have
The joined body manufacturing apparatus, wherein the heating / pressurizing unit and the cooling / pressurizing unit are in surface contact or multiple line contact with each of the transfer layers. The joined body manufacturing apparatus according to claim 1,
At least one of the heating and pressing unit and the cooling and pressing unit includes a heat conductive elastic body, and the heat conductive elastic body is in surface contact or multiple line contact. The joined body manufacturing apparatus according to claim 1,
At least one of the heating and pressing unit and the cooling and pressing unit includes a metal material, and the metal material is in surface contact or multiple line contact. The joined body manufacturing apparatus according to any one of claims 1 to 3,
At least one of the heating and pressing unit and the cooling and pressing unit is an endless track system. The joined body manufacturing apparatus according to any one of claims 1 to 3,
At least one of the heating and pressing unit and the cooling and pressing unit includes a plurality of rollers, and the plurality of rollers are in contact with each other by a plurality of lines. The joined body manufacturing apparatus according to claim 2,
The joined body manufacturing apparatus, wherein the plate made of the heat conductive elastic body is in surface contact. The joined body manufacturing apparatus according to claim 2,
A joined body manufacturing apparatus in which a belt made of the heat conductive elastic body is in surface contact. The joined body manufacturing apparatus according to claim 2,
An apparatus for manufacturing a joined body, wherein the thermal conductive elastic body is subjected to pressure deformation and brought into surface contact. A joined body production method for producing a joined body of a catalyst layer and an electrolyte membrane or a joined body of a diffusion layer and a catalyst layer-supported electrolyte membrane,
A support substrate formed by supporting a plurality of transfer layers, which are either the catalyst layer or the diffusion layer, on one surface, and a substrate formed of a transfer layer, which is either the electrolyte membrane or the catalyst layer-supported electrolyte membrane Heating and pressing in a state where the transfer layer and the transfer target layer are in contact with each other, and continuously transferring the transfer layer to the substrate to form a joined body,
A cooling and pressurizing step of continuously cooling and pressurizing the joined body;
Including
In the heating and pressing step and the cooling and pressing step, the heating and pressing, and the cooling and pressing are performed by surface contact or multi-line contact with respect to each transfer layer. .

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