JP5266777B2 - Nipping body using auxiliary membrane, method for producing electrolyte membrane-catalyst layer assembly with sandwiching body, method for producing electrolyte membrane-electrode assembly with sandwiching body, and method for producing polymer electrolyte fuel cell - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide an auxiliary membrane for a polymer electrolyte fuel cell capable of preventing breakage of an electrolyte membrane. <P>SOLUTION: The auxiliary membrane 4 is bonded to an electrolyte membrane-catalyst layer assembly 10 in which a catalyst layer 3 is formed on both surfaces of the electrolyte membrane 2, or an electrolyte membrane-electrode assembly 20 in which an electrode E comprising the catalyst layer 3 and a gas diffusion layer 5 is formed on both surfaces of the electrolyte membrane 2. The auxiliary membrane 4 has a substrate 41 and an adhesive layer 42 formed on the substrate 41 and containing ionizing radiation-curing resin for bonding with the electrolyte membrane-catalyst layer assembly 10 or the electrolyte membrane-electrode assembly 20 by irradiating light or ionizing radiation, and an easily removable region 44 easily removable for forming an opening part 45 is formed in the center. <P>COPYRIGHT: (C)2009,JPO&amp;INPIT

Description

  The present invention relates to an auxiliary membrane, a sandwich body using the same, an electrolyte membrane-catalyst layer assembly with a sandwich body, an electrolyte membrane-electrode assembly with a sandwich body, a polymer electrolyte fuel cell, and a production method thereof. is there.

  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 to be put to practical use.

  This polymer electrolyte fuel cell uses a solid polymer electrolyte membrane having proton conductivity, and a catalyst layer and a gas diffusion layer are sequentially laminated on both surfaces of the electrolyte membrane. And it has the structure which has arrange | positioned the gasket so that the circumference | surroundings of the electrode which consists of this catalyst layer and a gas diffusion layer may be enclosed, and also this was pinched | interposed with the separator. Further, since the gasket is installed so as to surround the outer side of the electrode from the viewpoint of positional accuracy, a gap is formed between the gasket and the electrode, and the electrolyte membrane corresponding to this gap portion is an electrode. It is in a state where it is not pressed by either of the gaskets. In this state, when power generation / non-power generation is repeated in the polymer electrolyte fuel cell, the electrolyte membrane repeats a wet state and a dry state, but the electrolyte membrane corresponding to the gap is pressed by an electrode or a gasket. Since it is not performed, expansion and contraction are repeated. As a result, there is a problem that stress is generated in the electrolyte membrane and fatigues, and the electrolyte membrane is damaged.

In order to solve this problem, for example, in the polymer electrolyte fuel cell disclosed in Patent Document 1, a reinforcing film is further provided in the gap between the electrode and the gasket, so that the gap between the gasket and the electrode is formed. It restrains and suppresses the expansion / contraction of the electrolyte membrane.
JP 2007-109576 A

  However, since the reinforcing membrane of the polymer electrolyte fuel cell is welded to the electrolyte membrane by hot pressing, it is locally applied to the portion where the reinforcing membrane of the electrolyte membrane is installed by heat and pressure during hot pressing. May cause damage to the electrolyte membrane.

Accordingly, the present invention is capable of preventing damage of the electrolyte membrane, sandwiched body using an auxiliary membrane, holding member with the electrolyte membrane - a method of manufacturing a catalyst layer assembly, holding member with the electrolyte membrane - the production of the electrode assembly method, and an object of the present invention to provide a method for producing a polymer electrolyte fuel cells.

The 1st clamping body which concerns on this invention was made | formed in order to solve the said subject, The electrolyte membrane-catalyst layer assembly by which the catalyst layer was each formed on both surfaces of the electrolyte membrane, or both surfaces of electrolyte membrane An auxiliary film to be bonded to an electrolyte membrane-electrode assembly in which an electrode composed of a catalyst layer and a gas diffusion layer is formed, and is formed on the base material and the base material, and is irradiated with light or ionizing radiation. electrolyte membrane by - catalyst layer assembly or an electrolyte membrane - has an adhesive layer containing an ionizing radiation curable resin for bonding the electrode assembly, formed Disconnect possible easy removal region preparative for forming an opening in the center The auxiliary membranes are arranged so that the adhesive layers face each other, and an electrolyte membrane-catalyst layer assembly or an electrolyte membrane-electrode assembly can be inserted between the auxiliary membranes. The easy removal areas are aligned with each other. To maintain the state, at least a portion of the outer peripheral edge portion are bonded to each other.

In addition, a second sandwiching body according to the present invention is made to solve the above-described problem, and is an electrolyte membrane-catalyst layer assembly in which catalyst layers are formed on both surfaces of the electrolyte membrane, or an electrolyte membrane, respectively. An auxiliary film that is bonded to an electrolyte membrane-electrode assembly in which electrodes comprising a catalyst layer and a gas diffusion layer are formed on both surfaces, and is formed on the substrate and irradiated with light or ionizing radiation. The auxiliary membrane formed in the shape of a frame having an adhesive layer containing an ionizing radiation curable resin that adheres to the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly, and having an opening in the center. The auxiliary membranes are arranged so that the adhesive layers face each other, and an electrolyte membrane-catalyst layer assembly or an electrolyte membrane-electrode assembly can be inserted between the auxiliary membranes, and the openings are mutually connected. Outer rim to maintain alignment At least a portion of the are bonded to each other. Further, the third sandwiching body according to the present invention is made to solve the above problems, and is an electrolyte membrane-catalyst layer assembly in which catalyst layers are respectively formed on both surfaces of the electrolyte membrane, or an electrolyte membrane. An auxiliary film that is bonded to an electrolyte membrane-electrode assembly in which electrodes comprising a catalyst layer and a gas diffusion layer are formed on both surfaces, and is formed on the substrate and irradiated with light or ionizing radiation. By having an adhesive layer containing an ionizing radiation curable resin that adheres to the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly, a removable easily removable region for forming an opening is formed in the center. The auxiliary membrane and the electrolyte membrane in which the catalyst layers are formed on both sides of the electrolyte membrane-the catalyst layer assembly, or the electrolyte membrane in which the electrodes made of the catalyst layer and the gas diffusion layer are formed on both sides of the electrolyte membrane- For electrode assembly An auxiliary film to be applied, which is formed on the base material and cured with ionizing radiation that adheres to the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly by irradiation with light or ionizing radiation. And an auxiliary film formed in a frame shape having an opening in the center, and each auxiliary film is disposed so that the mutual adhesive layers face each other, and between the auxiliary films An electrolyte membrane-catalyst layer assembly or an electrolyte membrane-electrode assembly can be inserted into the at least part of the outer peripheral edge so that the easily removable region and the opening are maintained aligned with each other. ing.

Thus, the first to third Kyojitai according to the present invention, since the adhesive layer contains an ionizing radiation-curable resin, electrolyte membrane adhesive layer by emitting light or ionizing radiation - catalyst layer assembly It adheres to the body and electrolyte membrane-electrode assembly. Therefore, the auxiliary membrane can be adhered to the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly without using a hot press, so that the electrolyte membrane can be prevented from being damaged. The “easy removal region” is, for example, an outer peripheral edge formed by perforations or cutouts, and can be easily removed by cutting along the perforations. As a result, the catalyst layer or It refers to a region for forming an opening that can expose an electrode except the outer peripheral edge. Furthermore, according to this configuration, as described above, the auxiliary membrane can be adhered to the electrolyte membrane-catalyst layer assembly by irradiation with light or ionizing radiation, and damage to the electrolyte membrane can be prevented. Further, the auxiliary films are not independent from each other, and at least a part of the outer peripheral edge portion is bonded so that the easy-removal regions are aligned with each other, so that the auxiliary films may be displaced from each other. Absent. Therefore, even when the polymer electrolyte fuel cell using this sandwiching body is stacked, stable stacking is possible.

Although the said clamping body can take various structures, it is preferable that the said base material has the gas barrier property which prevents permeation | transmission of fuel gas and oxidizing agent gas, for example. Thereby, gas leak can be prevented more reliably. In this case, the base material may have a gas barrier property as a single substance, or a material having a gas barrier property may be laminated on the base material. As a material having gas barrier properties, for example, inorganic silica can be laminated on the substrate by a vapor deposition method. When the substrate alone has gas barrier properties, the substrate is preferably a biaxially stretched polyethylene naphthalate film.

  In addition, a sandwiching body according to the present invention is made to solve the above-described problem, and includes two of the auxiliary films described above, and the auxiliary films are arranged so that the adhesive layers face each other. In addition, an electrolyte membrane-catalyst layer assembly or an electrolyte membrane-electrode assembly can be inserted between the auxiliary membranes, and at least a part of the outer peripheral edge so as to maintain the respective easy-to-removable regions or openings aligned with each other. Are glued together.

  According to this configuration, as described above, the auxiliary membrane can be adhered to the electrolyte membrane-catalyst layer assembly by irradiation with light or ionizing radiation, and damage to the electrolyte membrane can be prevented. Further, the auxiliary films are not independent from each other, and at least a part of the outer peripheral edge portion is bonded so that the easy-removal regions are aligned with each other, so that the auxiliary films may be displaced from each other. Absent. Therefore, even when the polymer electrolyte fuel cell using this sandwiching body is stacked, stable stacking is possible.

  Moreover, the electrolyte membrane-catalyst layer assembly with a sandwiching body according to the present invention is made to solve the above problems, and the sandwiching body, the electrolyte membrane, and the catalyst layer formed on both surfaces of the electrolyte membrane An electrolyte membrane-catalyst layer assembly comprising: the electrolyte membrane-catalyst layer assembly, wherein each of the auxiliary membranes of the sandwiching body is exposed so that each catalyst layer is exposed from the opening except for an outer peripheral edge. The auxiliary membranes are sandwiched between them, and adhere to the outer peripheral edge of the electrolyte membrane-catalyst layer assembly.

  In the electrolyte membrane-catalyst layer assembly with a sandwiching body configured as described above, the auxiliary membrane constituting the sandwiching body is adhered to the electrolyte membrane-catalyst layer assembly by irradiation with light or ionizing radiation, and hot pressing is performed. Since it is not necessary, damage to the electrolyte membrane can be prevented.

  Moreover, the 1st electrolyte membrane-electrode assembly with a clamping body which concerns on this invention was made | formed in order to solve the said subject, The said electrolyte membrane-catalyst layer assembly with a clamping body, and the said auxiliary membrane And a gas diffusion layer formed on each of the catalyst layers so as to be thicker than the auxiliary film.

  Moreover, the 2nd electrolyte membrane-electrode assembly with a clamp body which concerns on this invention was made | formed in order to solve the said subject, and was formed in both surfaces of the said clamp body, electrolyte membrane, and said electrolyte membrane. An electrolyte membrane-electrode assembly comprising a catalyst layer and a gas diffusion layer formed on each of the catalyst layers, and the electrolyte membrane-electrode assembly includes the gas diffusion layer except for an outer peripheral edge. The auxiliary films are sandwiched between the auxiliary films so as to be exposed from the opening, and the auxiliary films are bonded to the outer peripheral edge of the electrolyte membrane-electrode assembly.

  Thus, in the first and second sandwiched electrolyte membrane-electrode assemblies according to the present invention, the auxiliary membrane is formed with the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly by irradiation with light or ionizing radiation. Since it is bonded and there is no need to perform hot pressing, damage to the electrolyte membrane can be prevented.

  In addition, a polymer electrolyte fuel cell according to the present invention has been made to solve the above problems, and includes any one of the electrolyte membrane-electrode assembly with a sandwiching body, the catalyst layer, and the gas diffusion layer. A gasket installed on each auxiliary membrane so as to surround each electrode, and a separator installed on each electrode and gasket.

  As described above, the auxiliary membrane of the polymer electrolyte fuel cell configured as described above does not need to be hot pressed to adhere to the electrolyte membrane-catalyst layer assembly by irradiation with light or ionizing radiation. It is possible to prevent damage to the electrolyte membrane.

Moreover, the manufacturing method of the 1st electrolyte membrane-catalyst layer assembly | attachment body with a clamp body based on this invention was made | formed in order to solve the said subject, The electrolyte membrane in which the catalyst layer was formed on both surfaces of the electrolyte membrane -Preparing a catalyst layer assembly, and preparing two auxiliary membranes having an adhesive layer containing an ionizing radiation curable resin that adheres to the electrolyte membrane-catalyst layer assembly by irradiation with light or ionizing radiation. And attaching the electrolyte membrane-catalyst layer assembly and adhering at least a part of the outer peripheral edge of each auxiliary membrane so that the two auxiliary membranes are not displaced from each other. a process of forming the holding member, the center of each sub-film of the fabricated holding member, to form an opening for exposing except the outer peripheral edge of the catalyst layer, remove it possible easy Forming a removal region and the easy removal A step of inserting the electrolyte membrane-catalyst layer assembly to a position where the catalyst layer excluding an outer peripheral edge faces the easy removal region between the auxiliary membranes in which the regions are formed; And forming the opening, and after forming the opening, irradiating light or ionizing radiation to adhere each auxiliary membrane to the outer peripheral edge of the electrolyte membrane-catalyst layer assembly. I have.

  Moreover, the manufacturing method of the 2nd electrolyte membrane-catalyst layer assembly | attachment body with a clamp body based on this invention was made | formed in order to solve the said subject, The electrolyte membrane by which the catalyst layer was formed on both surfaces of the electrolyte membrane A step of preparing a catalyst layer assembly, and a frame having an adhesive layer containing an ionizing radiation curable resin that adheres to the electrolyte membrane-catalyst layer assembly by irradiating light or ionizing radiation and having an opening in the center Arranging the auxiliary membranes on both surfaces of the electrolyte membrane-catalyst layer assembly, emitting light or ionizing radiation, and bonding each auxiliary membrane to the electrolyte membrane-catalyst layer assembly; It has.

  Thus, according to the first and second manufacturing methods according to the present invention, the auxiliary membrane is adhered to the electrolyte membrane-catalyst layer assembly by irradiating light or ionizing radiation without using a hot press. Therefore, damage to the electrolyte membrane can be prevented.

  Moreover, the manufacturing method of the 1st electrolyte membrane-electrode assembly with a clamping body which concerns on this invention was made | formed in order to solve the said subject, The electrolyte membrane-catalyst layer assembly with any said clamping body The manufacturing method further includes a step of forming a gas diffusion layer thicker than the auxiliary film on each catalyst layer exposed from the opening.

In addition, the second method for producing an electrolyte membrane-electrode assembly with a sandwiching body according to the present invention is made to solve the above-mentioned problems, and an electrode comprising a catalyst layer and a gas diffusion layer on both surfaces of the electrolyte membrane. A step of preparing an electrolyte membrane-electrode assembly in which an electrode is formed, and two auxiliary layers having an adhesive layer containing an ionizing radiation curable resin that adheres to the electrolyte membrane-electrode assembly by irradiation with light or ionizing radiation Preparing a membrane and stacking each other, and at least part of the outer peripheral edge of each auxiliary membrane so that the electrolyte membrane-electrode assembly can be inserted and the two auxiliary membranes are not displaced from each other a process of forming an adhesive to holding member, the center of each sub-film of the fabricated holding member, to form an opening for exposing except the outer peripheral edge portion of the electrode, preparative possible Disconnect Easy removal area And inserting the electrolyte membrane-electrode assembly between the auxiliary membrane in which the easy-removal region is formed, to a position where the electrode excluding an outer peripheral edge faces the easy-removal region; Removing the easy-removable region to form an opening, and after forming the opening, irradiating light or ionizing radiation to adhere the auxiliary films to the outer peripheral edge of the electrolyte membrane-electrode assembly; Adhering the outer peripheral edges of each auxiliary membrane.

  In addition, a third method for producing an electrolyte membrane-electrode assembly with a sandwiching body according to the present invention has been made to solve the above-mentioned problems, and an electrode comprising a catalyst layer and a gas diffusion layer on both surfaces of the electrolyte membrane. And a step of preparing an electrolyte membrane-electrode assembly formed with an adhesive layer including an ionizing radiation curable resin that adheres to the electrolyte membrane-electrode assembly by irradiating light or ionizing radiation and opening in the center A step of disposing a frame-like auxiliary membrane having a portion on both surfaces of the electrolyte membrane-electrode assembly so that the adhesive layer faces the electrolyte membrane-electrode assembly, and emitting light or ionizing radiation, Adhering each auxiliary membrane to the electrolyte membrane-electrode assembly.

  Thus, the manufacturing method of the 1st-3rd electrolyte membrane with a clamp body-electrode assembly which concerns on this invention does not use a hot press, but irradiates light or ionizing radiation, and an auxiliary membrane is electrolyte membrane- Since the catalyst layer assembly or the electrolyte membrane-electrode assembly is adhered, damage to the electrolyte membrane can be prevented.

  In addition, a method for producing a solid polymer fuel cell according to the present invention has been made to solve the above-mentioned problems, and in any one of the above methods for producing an electrolyte membrane-electrode assembly with a sandwich, A step of installing a gasket on each of the auxiliary membranes so as to surround each electrode comprising a layer and a gas diffusion layer, and a step of installing a separator on each of the electrodes and the gasket.

  According to this method, the auxiliary membrane is adhered to the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly by irradiating light or ionizing radiation without using a hot press, so that the electrolyte membrane is damaged. Can be prevented.

According to the present invention, to more reliably prevent breakage of the electrolyte membrane, sandwiched body using the auxiliary film, holding member with the electrolyte membrane - a method of manufacturing a catalyst layer assembly, holding member with the electrolyte membrane - the production of the electrode assembly method, and method for producing a solid polymer electrolyte fuel cells can provide.

  Embodiments of the present invention will be described below with reference to the drawings. FIG. 1 is a plan view of a sandwiching body according to this embodiment, and FIG. 2 is a cross-sectional view taken along line AA of FIG.

As shown in FIGS. 1 and 2, the sandwiching body 40 includes two auxiliary films 4 having a rectangular shape in plan view. Each auxiliary film 4 is composed of a base material 41 having a gas barrier property made of a polyester-based resin and an adhesive layer 42 made of an ionizing radiation curable resin applied on the base material 41. In addition, on the base material 41, a flow coat method,
The adhesive layer 42 can be applied by a method such as spray coating, die coating, knife coating, gravure coating, or screen coating. The auxiliary films 4 thus formed are arranged so that the adhesive layers 42 face each other, and the upper, right, and lower outer peripheral edge portions 43 are bonded to each other, leaving the left outer peripheral edge portion in FIG. Has been. The left non-adhered outer peripheral edge portion forms an inlet for inserting an electrolyte membrane-catalyst layer assembly 10 or an electrolyte membrane-electrode assembly 20 described later between the auxiliary membranes 4. Each auxiliary film 4 has an easy-removal region 44 formed at the center thereof. The easy removal region 44 refers to a region that can be easily removed, and in this embodiment, it is formed by perforations so that the outer peripheral edge is easily broken. When the easy removal region 44 is removed, an opening 45 is formed in each auxiliary film 4. In addition, it is preferable that the film thickness of the said base material 41 shall be 5-50 micrometers, and it is preferable that the film thickness of the contact bonding layer 42 shall be 1-50 micrometers.

  Next, the polymer electrolyte fuel cell 1 using the above-described sandwiching body 40 will be described with reference to the drawings. FIG. 3 is a front sectional view of the polymer electrolyte fuel cell according to the present embodiment, FIG. 4 is a plan view of an electrolyte membrane-electrode assembly with a sandwich body according to the present embodiment, and FIG. 5 is an electrolyte membrane with a sandwich body. -It is an expanded front sectional view which shows the detail of the outer periphery part of an electrode assembly.

  As shown in FIGS. 3 and 4, the polymer electrolyte fuel cell 1 includes an electrolyte membrane 2 having a rectangular shape in plan view, and a plan view that is slightly smaller than the electrolyte membrane 2 on the upper and lower surfaces of the electrolyte membrane 2. A rectangular catalyst layer 3 is formed. A structure in which the catalyst layer 3 is formed on both surfaces of the electrolyte membrane 2 is referred to as an electrolyte membrane-catalyst layer assembly 10. Thus, since the catalyst layer 3 is formed slightly smaller than the electrolyte membrane 2, the catalyst layer 3 is not formed on the outer peripheral edge 21 of the electrolyte membrane 2. In addition, it is preferable that the distance C (refer FIG. 5) from the outer periphery of the electrolyte membrane 2 to the outer periphery of the catalyst layer 3 is 0-5 mm. When the distance C is 0 mm, the electrolyte membrane 2 and the catalyst layer 3 have the same shape and the same size, and are formed so that the entire catalyst layer 3 covers both surfaces of the electrolyte membrane 2. The catalyst layer 3 is also formed on the outer peripheral edge 21 (see FIG. 9).

And the clamping body 40 mentioned above is installed so that this electrolyte membrane-catalyst layer assembly 10 may be clamped. At this time, the easy removal region 44 of the sandwiching body 40 is removed to form an opening 45. In a state where the sandwiching body 40 sandwiches the electrolyte membrane-catalyst layer assembly 10, the catalyst layer 3 is exposed from the opening 45 of the auxiliary membrane 4 except for the outer peripheral edge 31, and the outer peripheral edge of the catalyst layer 3. The outer peripheral edge 21 of the portion 31 and the electrolyte membrane 2 is covered with the auxiliary membrane 4. In addition, it is preferable that the distance B (refer FIG. 5) from the outer periphery of the catalyst layer 3 to the inner periphery of the auxiliary | assistant film | membrane 4 shall be 1-10 mm. The auxiliary membrane 4 is formed to be slightly larger than the electrolyte membrane 2, and the outer peripheral edge portions 43 of the auxiliary membranes 4 protruding from the electrolyte membrane 2 are bonded to each other outside the electrolyte membrane 2. The distance D (see FIG. 5) from the outer peripheral edge of the auxiliary membrane 4 to the outer peripheral edge of the electrolyte membrane 2 is preferably 1 to 100 mm. In addition, what clamped the electrolyte membrane-catalyst layer assembly 10 with the sandwiching body 40 corresponds to the sandwiched electrolyte membrane-catalyst layer assembly of the present invention.

  A gas diffusion layer 5 having a rectangular shape in plan view is formed on the catalyst layer 3 exposed from the opening 45 of the auxiliary membrane 4. The distance A (see FIG. 5) from the outer peripheral edge of the gas diffusion layer 5 to the inner peripheral edge of the auxiliary film 4 is preferably 0 to 5 mm. Thus, the gas diffusion layer 5 is formed on the catalyst layer 3 to constitute the electrode E, and the electrode E formed on both surfaces of the electrolyte membrane 2 is called an electrolyte membrane-electrode assembly 20. As in the present embodiment, the electrolyte membrane-catalyst layer assembly 10 is sandwiched by the sandwiching body 40, and the gas diffusion layer 5 is further formed on the catalyst layer 3, so that the electrolyte membrane with sandwiching body of the present invention- It corresponds to an electrode assembly.

  A frame-shaped gasket 6 is installed so as to surround the periphery of the electrode E, and a separator 7 is installed on the electrode E and the gasket 6. In the separator 7, a gas flow path 71 is formed in a region facing the gas diffusion layer 5.

  Next, the material of each component of the polymer electrolyte fuel cell 1 configured as described above will be described.

  The electrolyte membrane 2 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 2 is about 20-250 micrometers normally, Preferably it is about 20-80 micrometers.

  The catalyst layer 3 is a known platinum-containing catalyst layer (cathode catalyst and anode catalyst). Specifically, the catalyst layer 3 contains carbon particles supporting catalyst particles and a hydrogen ion conductive polymer electrolyte. 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 2 mentioned above can be used.

  The auxiliary film 4 is composed of a base material 41 and an adhesive layer 42. The base material 41 is made of polyester, polyamide, polyimide, polymethyl tempene, polyphenylene having barrier properties against water vapor, water, fuel gas and oxidant gas. Oxide, polysulfone, polyether ether ketone, polyphenylene sulfide, and the like can be preferably used. Specific examples of the polyester include polyethylene terephthalate, polyethylene naphthalate, polybutylene terephthalate, and polybutylene naphthalate.

  In addition, an ionizing radiation curable resin is used as the material of the adhesive layer 42. The ionizing radiation curable resin has a polymerized unsaturated bond or a cationic polymerizable functional group in the molecule, and is cured by ionizing radiation. Possible prepolymers (including so-called oligomers) or monomers are used alone or in an appropriate mixture. More specifically, a monomer having two or more radically polymerizable unsaturated groups such as a (meth) acryloyl group and (meth) acryloyloxy group, a cationically polymerizable functional group such as an epoxy group, or a thiol group in the molecule. Alternatively, a prepolymer is used alone or in combination. In addition, the said (meth) acryloyl group is used by the meaning of an acryloyl group or a methacryloyl group.

  Examples of the prepolymer having a radically polymerizable unsaturated group include polyester (meth) acrylate, urethane (meth) acrylate, epoxy (meth) acrylate, melamine (meth) acrylate, triazine (meth) acrylate and the like. The molecular weight is usually about 250 to 100,000.

  Examples of the prepolymer having a cationic polymerizable functional group include epoxy resins such as bisphenol type epoxy resins and novolac type epoxy resins, and vinyl ether resins such as aliphatic vinyl ethers and aromatic vinyl ethers. .

  Examples of the monofunctional monomer having a radically polymerizable unsaturated group include a monofunctional monomer of a (meth) acrylate compound. Specifically, methyl (meth) acrylate, 2-ethylhexyl ( Examples thereof include meth) acrylate and phenoxyethyl (meth) acrylate.

  Examples of polyfunctional monomers having radically polymerizable unsaturated groups include diethylene glycol di (meth) acrylate, propylene glycol di (meth) acrylate, trimethylolpropane tri (meth) acrylate, trimethylolpropane ethylene oxide tri (meth) ) Acrylate, dipentaerythritol penta (meth) acrylate, dipentaerythritol hexa (meth) acrylate, and the like.

  Examples of the monomer having a thiol group include trimethylolpropane trithioglycolate, dipentaerythritol tetrathioglycolate, and the like.

  In the case of irradiating ultraviolet rays as ionizing radiation, a photopolymerization initiator is added as a sensitizer in the ionizing radiation curable resin. As a photopolymerization initiator used for curing a resin system having a radical polymerizable unsaturated group, acetophenones, benzophenones, thioxanthones, benzoin, benzoin methyl ether, etc. can be used alone or in combination. . In addition, as a photopolymerization initiator used for curing a resin system having a cationic polymerizable functional group, an aromatic diazonium salt, an aromatic sulfonium salt, an aromatic iodonium salt, a metatheron compound, a benzoin sulfonic acid ester, etc. Or can be used in combination. In addition, the addition amount of these photoinitiators is about 1 to 10 weight% with respect to 100 weight% of ionizing radiation curable resins.

  As the gas diffusion layer 5, various types of gas diffusion layers constituting a fuel electrode and an air electrode can be used. In order to efficiently supply fuel gas and oxidant gas as fuel to the catalyst layer 3, the gas diffusion layer 5 is porous. It is made of a conductive substrate. Examples of the porous conductive substrate include carbon paper and carbon cloth.

  As the gasket 6, it is possible to use a gasket that has a strength sufficient to withstand heat pressing and has a gas barrier property that does not leak fuel and oxidant to the outside. For example, a polyethylene terephthalate sheet or Teflon ( (Registered trademark) sheet, silicon rubber sheet, and the like.

  The separator 7 may be any known conductive plate that is known and stable even in the environment within the fuel cell. In general, a carbon plate in which a gas flow path 71 is formed is used. In addition, the separator 7 is made of a metal such as stainless steel, and the surface of the metal is formed with a coating made of a conductive material such as chromium, a platinum group metal or oxide thereof, or a conductive polymer. It is also possible to use a metal having a metal surface plated with a material such as silver, a platinum group composite oxide, or chromium nitride.

  Next, a method for producing the above-described polymer electrolyte fuel cell 1 will be described with reference to the drawings. FIG. 6 is an explanatory view showing a method for producing the polymer electrolyte fuel cell 1 according to the present embodiment.

As shown in FIG. 6, an electrolyte membrane 2 made of the above-described material is prepared, and a catalyst layer forming transfer sheet 8 is placed on both surfaces of the electrolyte membrane 2 in an overlapping manner. Here, the transfer sheet 8 for forming a catalyst layer is one in which the transferred catalyst layer 3 is formed on a transfer substrate 81. The production method of the catalyst layer forming transfer sheet 8 will be described. First, the above-described carbon particles supporting the catalyst particles and the hydrogen ion conductive polymer electrolyte are mixed and dispersed in an appropriate solvent to prepare a catalyst paste. . Then, the catalyst paste is applied onto the transfer substrate 81 through a release layer as necessary in accordance with a known method so that the formed catalyst layer 3 has a desired film thickness. At this time, the catalyst paste is applied to the transfer substrate 81 so that the catalyst layer 3 has a shape slightly smaller than the electrolyte membrane 2. Examples of the method for applying the catalyst paste include known coating methods such as screen printing, spray coating, die coating, and knife coating. 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. As the transfer substrate 81, for example, polyimide, polyethylene terephthalate, polyparvanic acid aramid, polyamide (nylon), polysulfone, polyethersulfone, polyphenylene sulfide, polyether ether ketone, polyetherimide, polyarylate, polyethylene naphthalate. And the like. 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. Further, the transfer substrate 81 may be 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 transfer substrate 81 is usually about 6 to 100 μm, preferably about 10 to 30 μm, from the viewpoints of handleability and economy. Therefore, the transfer substrate 81 is preferably a polymer film that is inexpensive and easily available, and more preferably polyethylene terephthalate.

  Then, after applying the catalyst paste, the catalyst layer 3 is formed on the transfer substrate 81 by drying at a 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.

Returning to FIG. 6, the description of the method for producing the polymer electrolyte fuel cell will be continued. The transfer sheet 8 for forming a catalyst layer prepared as described above is arranged so that the catalyst layer 3 faces the electrolyte membrane 2 (FIG. 6A), and a heat press is applied from the back side of the transfer sheet 8 to apply the catalyst layer. 3 is transferred to the electrolyte membrane 2, and the transfer substrate 81 of the transfer sheet 8 is peeled off (FIG. 6B). In consideration of workability, it is preferable to simultaneously laminate the catalyst layer 3 on both surfaces of the electrolyte membrane 2, but the catalyst layer 3 can also be formed on each side. The pressure level of the heating press is usually about 0.5 to 20 MPa, preferably about 1 to 10 MPa in order to avoid transfer failure. Further, it is preferable to heat the pressing surface during this pressing operation in order to avoid transfer failure. The heating temperature is usually 200 ° C. or lower, preferably 150 ° C. or lower, in order to avoid damage or deformation of the electrolyte membrane 2. Thus, the electrolyte membrane-catalyst layer assembly 10 is formed by forming the catalyst layers 3 on both surfaces of the electrolyte membrane 2. At this time, since the catalyst layer 3 is slightly smaller than the electrolyte membrane 2, the outer peripheral edge 21 of the electrolyte membrane 2 is exposed.

  Next, the clamping body 40 is attached to the electrolyte membrane-catalyst layer assembly 10 thus formed (FIG. 6C). Details of this step will be described with reference to FIG. FIG. 7 is a plan view showing a method for manufacturing an electrolyte membrane-catalyst layer assembly with a sandwiching body. As shown in FIG. 7, first, the two auxiliary films 4 made of the above-described materials are overlapped so that the adhesive layer 42 faces each other, and masking is performed so that the upper side, right side, and lower side constituting the U-shape are exposed. (FIG. 7A). Then, by irradiating with ionizing radiation, the U-shaped portions of the adhesive layer 42 exposed without being masked are bonded to each other. As a result, the two auxiliary films 4 form a bag body in which an adhesive portion is formed in a U-shape and the left side is open (FIG. 7B). The ionizing radiation means high-energy ionizing radiation such as electron beams (including beta rays), ultraviolet rays, X-rays, and gamma rays. That is, it is necessary to have energy capable of passing through the base material 41 of the auxiliary film 4 and curing the adhesive layer 42 by a crosslinking / polymerization reaction. For example, when an electron beam is used as the ionizing radiation, the higher the acceleration voltage, the deeper the penetration depth into the irradiated object. Therefore, when the thickness of the auxiliary film 4 is 0.1 to 10 mm, the acceleration voltage is 150 keV or more, preferably 1 MeV or more. As the irradiation device, various electron beam accelerators such as a Cockloft Walton type, a bandegraft type, a resonant transformer type, an insulating core transformation type, a linear type, a dynamitron type, and a high frequency type are used. Alternatively, beta rays emitted from radioactive nuclei such as 60Co (cobalt 60) and 170Tm (thulium 170) may be used. The amount of irradiation energy is about 10 to 500 kGy in absorbed dose. When gamma rays are used as ionizing radiation, there is no particular limitation because gamma rays basically have higher energy than electron beams. For example, 60Co (cobalt 60) 1.17 MeV and 1.33 MeV gamma rays or 226 Ra (radium 226) 2.2 MeV gamma rays are used as gamma ray line types. When X-rays are used as ionizing radiation, a betatron, a linear accelerator, or the like can be used as an X-ray irradiation device. When ultraviolet rays are used as the ionizing radiation, low-pressure mercury vapor, high-pressure mercury vapor, excimer lamp, ultraviolet laser, or the like is used as the ultraviolet ray source.

  When the bag is formed by the auxiliary membrane 4, next, an easily removable region 44 that is slightly smaller than the catalyst layer 3 of the electrolyte membrane-catalyst layer assembly 10 is formed at the center of each auxiliary membrane 4 constituting the bag. (FIG. 7 (c)). Thereby, the clamping body 40 is formed. The electrolyte membrane-catalyst layer assembly 10 is inserted into the sandwiching body 40 from the left side which is not bonded and moved to a predetermined position (FIG. 7D). The predetermined position refers to a position where the catalyst layer 3 of the electrolyte membrane-catalyst layer assembly 10 faces the easy removal region 44 except for the outer peripheral edge 31.

After the electrolyte membrane-catalyst layer assembly 10 is moved to a predetermined position, the perforation at the outer periphery of the easy removal region 44 is cut and the easy removal region 44 is removed from each auxiliary membrane 4, thereby An opening 45 is formed in the center (FIG. 7E). When the easy removal regions 44 are thus removed from the auxiliary membranes 4 to form the openings 45, the catalyst layer 3 of the electrolyte membrane-catalyst layer assembly 10 is removed from the openings 45 except for the outer peripheral edge 31. It will be exposed. Then, by irradiating with ionizing radiation, the auxiliary membrane 4 adheres to the outer peripheral edge portion 31 of the catalyst layer 3 of the electrolyte membrane -catalyst layer assembly 10 and the outer peripheral edge portion 21 of the electrolyte membrane 2, and the auxiliary membrane 4. They are bonded to each other at the outer peripheral edge 43. Through the above steps, the sandwiched electrolyte membrane-catalyst layer assembly is completed (FIGS. 7 (f) and 6 (c)).

  Returning to FIG. 6, the description of the method for producing the polymer electrolyte fuel cell 1 will be continued. On the catalyst layer 3 exposed from the opening 45 of the electrolyte membrane-catalyst layer assembly with the sandwiched body described above, the gas diffusion layer 5 is laminated by thermocompression bonding to complete the electrolyte membrane-electrode assembly with the sandwiched body. (FIG. 6D). A gasket 6 is disposed on the auxiliary membrane 4 so as to surround the periphery of the electrode E composed of the catalyst layer 3 and the gas diffusion layer 5. Further, the separator 7 is disposed on the gas diffusion layer 5 and the gasket 6 so that the gas flow path 71 faces the gas diffusion layer 5 so that the gas diffusion layer 5 and the separator 7 are electrically connected. By sandwiching the electrolyte membrane-electrode assembly with the separator 7, the polymer electrolyte fuel cell 1 is completed (FIG. 6E).

  As described above, in the present embodiment, the auxiliary membrane 4 is bonded to the electrolyte membrane-catalyst layer assembly 10 by irradiating with ionizing radiation without using a hot press as in the conventional method. There is no risk of damaging the electrolyte membrane. Further, the auxiliary films 4 are not independent from each other, and at least a part of the outer peripheral edge portion 43 is bonded so that the easy-removal regions 44 are aligned with each other. There is no gap. Therefore, even when the polymer electrolyte fuel cell 1 in which the sandwiching body 40 is used is stacked, stable stacking is possible.

  As mentioned above, although embodiment of this invention was described, this invention is not limited to these, A various change is possible unless it deviates from the meaning of this invention. For example, in the above-described embodiment, the outer peripheral edge portions 43 on the upper side, the right side, and the lower side of each auxiliary film 4 are bonded, but it is sufficient that the auxiliary films 4 are bonded to such an extent that they do not shift each other. It is only necessary to form an inlet to the extent that the membrane-catalyst layer assembly 10 or the electrolyte membrane-electrode assembly 20 can be inserted. For example, only the upper and right outer peripheral edge portions 43 are bonded, or the right outer peripheral edge portion 43 is bonded. Can also be glued only.

  Moreover, in the said embodiment, after once forming the clamping body 40 with the auxiliary | assistant film | membrane 4, it is made to adhere | attach on the electrolyte membrane-catalyst layer assembly 10, However, It is not necessarily limited to this method. For example, the auxiliary membrane 4 in which the opening 45 is formed in advance is prepared, and the auxiliary membrane 4 is disposed on both surfaces of the electrolyte membrane-catalyst layer assembly 10 so that the adhesive layer 42 faces the electrolyte membrane-catalyst layer assembly 10. Deploy. The auxiliary membrane 4 can be adhered to both surfaces of the electrolyte membrane-catalyst layer assembly 10 by irradiating with ionizing radiation.

  Further, in the above embodiment, the electrolyte membrane, the catalyst layer, the gas diffusion layer, etc. constituting the solid polymer fuel cell are all formed in a rectangular shape in plan view, but the shape is not particularly limited, It can also be formed in a circular shape in plan view. Similarly, the sandwiching body, that is, the auxiliary film is also formed in a rectangular shape in plan view in the above embodiment, but the shape is not particularly limited. When the polymer electrolyte fuel cell is formed in a circular shape in a plan view, the auxiliary membrane and the easy removal region are preferably formed in a circular shape in a plan view.

  In the above embodiment, the perforation is formed along the outer peripheral edge of the easy-removal region 44 so that the outer peripheral edge can be easily broken, and the easy-removable region 44 can be easily removed. It is not limited to, for example, it is possible to make it easy to break by making a cut along the outer peripheral edge, leaving only a part, or by making the part along the outer peripheral edge thinner. it can.

  Further, in the above embodiment, the catalyst layer 3 is formed so as to be exposed except for the outer peripheral edge portion 31 from the opening 45 of each auxiliary membrane 4. However, as shown in FIG. The gas diffusion layer 5 can also be formed so as to be exposed except the outer peripheral edge portion 51 from the portion 45. In this case, first, the electrolyte membrane-electrode assembly 20 is prepared, and the electrolyte membrane-electrode assembly 20 is sandwiched and bonded by the sandwiching body, whereby the electrolyte membrane-electrode assembly with the sandwiching body is manufactured. . And after that, the gasket 6 and the separator 7 are installed similarly to the said embodiment, and a polymer electrolyte fuel cell is produced.

  Moreover, in the said embodiment, although the contact bonding layer 42 was formed in the whole surface of the auxiliary | assistant film | membrane 4, the contact bonding layer 42 can also be formed, for example only in an easily removable area | region.

  The present invention will be described more specifically with reference to the following examples and comparative examples. In addition, this invention is not limited to the following Example.

Example 1
As the electrolyte membrane 2, NRE212CS (manufactured by Dupont) having a film thickness of 53 μm cut to a size of 63 × 63 mm was used.

Next, a transfer sheet 8 for forming a catalyst layer was produced in the following manner. First, 2 g of platinum catalyst-supported carbon (platinum supported amount: 45.7 wt%, manufactured by Tanaka Kikinzoku Co., Ltd., TEC10E50E), 1 g of 1-butanol, 10 g of 3-butanol, 20 g of a fluororesin (5 wt% Nafion binder, manufactured by DuPont) and 6 g of water was added, and these were stirred and mixed with a disperser to prepare an ink composition for forming a catalyst. Next, the ink was applied to a polyester film (Toray, X44, 25 μm) so that the weight of platinum after drying the catalyst layer was 0.4 mg / cm ² to prepare a transfer sheet 8 for forming a catalyst layer .

The catalyst layer- forming transfer sheet 8 produced as described above was cut into a size of 60 × 60 mm, and placed on both sides of the electrolyte membrane 2 so that the catalyst layer 3 faced the electrolyte membrane 2 side. The catalyst layer 3 was formed on both surfaces of the electrolyte membrane 2 by hot pressing under conditions of 135 ° C., 5.0 MPa, 150 seconds, and the electrolyte membrane-catalyst layer assembly 10 was produced. The catalyst layer 3 has a thickness of 20 μm.

Subsequently, the auxiliary film 4 constituting the sandwiching body 40 was produced. As the base material 41 of the auxiliary film 4, biaxially stretched polyethylene naphthalate (manufactured by Teijin Limited, Teonex, thickness 12 μm) was used. An electron beam curable adhesive (a kind of ionizing radiation curable resin) made of a radical polymerization type polyfunctional urethane acrylate-based prepolymer is formed on the base material 41 by a flow coating method so as to be 14 g / m ² when dried. The adhesive layer 42 was formed. The auxiliary membrane 4 is cut into a size of 80 × 80 mm, and masked so that the upper, right and lower outer peripheral edges 43 are exposed as shown in FIG. By exposing the exposed portions of 43 with an electron beam, the exposed portions were bonded to each other as shown in FIG. In addition, the irradiation conditions of the electron beam at this time are as follows.
・ Ionizing radiation type: Electron beam ・ Irradiation device: Cockcroft-Walton type electron accelerator ・ Acceleration voltage: 2 MeV
・ Irradiation dose: 15 kGy
And the easy removal area | region 44 of a magnitude | size of 50x50 mm was formed in the center of each auxiliary | assistant film | membrane 4, and the clamping body 40 was produced. The electrolyte membrane-catalyst layer assembly 10 described above is inserted from the left side of the sandwiching body 40 that is not bonded, and the catalyst layer 3 is moved to a position facing the easy removal region 44 except for the outer peripheral edge 31. Then, the easy removal region 44 is removed, an opening 45 is formed, and the auxiliary film 4 is adhered to the electrolyte membrane-catalyst layer assembly 10 by irradiating an electron beam under the same irradiation conditions as described above. The outer peripheral edge portions 43 were bonded to each other to produce an electrolyte membrane-catalyst layer assembly with a sandwiching body.

Subsequently, on the catalyst layer 3 exposed from the opening 45 , a 49 × 49 mm carbon paper (manufactured by Toray Industries Inc., carbon paper, TGP-H-090, thickness 280 μm) as a gas diffusion layer 5 is laminated. Then, an electrolyte membrane-electrode assembly with a reinforcing sheet was formed.

(Comparative Example 1)
As the electrolyte membrane, NRE212CS (manufactured by Dupont) having a film thickness of 53 μm cut to a size of 80 × 80 mm was used.

  Next, the catalyst-forming transfer sheet prepared in the same manner as in Example 1 was cut into a size of 50 × 50 mm, and hot-pressed under the same conditions as in Example 1 to obtain a thickness on both surfaces of the electrolyte membrane. A 20 μm catalyst layer was formed to prepare an electrolyte membrane-catalyst layer assembly.

Then, a 25 μm thick polyethylene naphthalate film (manufactured by Teijin Ltd., Teonex, 12 μm thick) is hot-pressed at 160 ° C. and 30 kgf / cm ^{2 on} the outer peripheral edge of the electrolyte membrane where the catalyst layer is not formed, An auxiliary film was formed. And 52 * 52 mm carbon paper (Toray Industries, TGP-H-090, thickness 280 micrometers) which is a gas diffusion layer was laminated | stacked on the catalyst layer, and the electrolyte membrane electrode assembly was produced.

(Evaluation method)
About the electrolyte membrane-electrode assembly with a sandwiching body of Example 1 and the electrolyte membrane-electrode assembly of Comparative Example 1, a polymer electrolyte fuel cell was prepared by installing a gasket 6 and a separator 7, respectively, and a load fluctuation cycle test Carried out. The measurement conditions at this time were a cell temperature of 80 ° C., a fuel utilization rate of 70%, an oxidant utilization rate of 40%, and a humidification temperature of 50 ° C. As a result of the current voltage measurement evaluation, the durability time of the fuel cell of Example 1 was 1000 hours, and no damage to the electrolyte membrane was observed after the evaluation. On the other hand, the durability time of the fuel battery cell of Comparative Example 1 was 500 hours. After evaluation for 500 hours, damage to the electrolyte membrane 2 was visually confirmed. As a result of measuring the leakage current amount after the load fluctuation cycle test, the leakage current amount of the fuel cell of Example 1 was 1 mA / cm ² or less, whereas the leakage current amount of the fuel cell of Comparative Example 1 was 15 mA / cm 2. ^{At 2} or more, gas leakage due to breakage of the electrolyte membrane was observed.

  As described above, in the polymer electrolyte fuel cell of Example 1, since the durability time is increased, it is understood that the problem of the electrolyte membrane breakage was solved by using the polymer electrolyte fuel cell of the present invention. .

It is a top view which shows embodiment of the clamping body which concerns on this invention. It is the sectional view on the AA line of FIG. 1 is a front sectional view showing an embodiment of a polymer electrolyte fuel cell according to the present invention. It is a top view which shows embodiment of the electrolyte membrane-electrode assembly with a clamping body which concerns on this invention. It is an expanded front sectional view showing the details of the outer periphery of the membrane-electrode assembly with a sandwiching body according to the present embodiment. It is explanatory drawing which shows the manufacturing method of the polymer electrolyte fuel cell which concerns on this embodiment. It is explanatory drawing which shows the manufacturing method of the electrolyte membrane-catalyst layer assembly | attachment with a clamp body which concerns on this embodiment. It is front sectional drawing which shows other embodiment of the polymer electrolyte fuel cell which concerns on this invention. It is front sectional drawing which shows other embodiment of the receding polymer fuel cell which concerns on this invention.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Polymer electrolyte fuel cell 2 Electrolyte membrane 21 Outer peripheral edge part 3 of electrolyte membrane Catalyst layer 31 Outer peripheral edge part 40 of catalyst layer 4 Holding body 4 Auxiliary film 41 Base material 42 Adhesive layer 43 Outer peripheral edge part 44 of auxiliary film Easy removal area 45 Opening 5 Gas diffusion layer 51 Outer peripheral edge 6 of gas diffusion layer Gasket 7 Separator

Claims (9)

Adhesive to an electrolyte membrane-catalyst layer assembly in which catalyst layers are formed on both sides of the electrolyte membrane, or to an electrolyte membrane-electrode assembly in which electrodes comprising a catalyst layer and a gas diffusion layer are formed on both sides of the electrolyte membrane, respectively. An auxiliary film comprising a base material and an ionizing radiation curable resin that is formed on the base material and adheres to the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly by irradiation with light or ionizing radiation. have an adhesive layer containing, Disconnect possible easy removal region preparative for forming an opening is formed in the center, with two auxiliary layer,
The auxiliary membranes are arranged so that the adhesive layers face each other, and an electrolyte membrane-catalyst layer assembly or an electrolyte membrane-electrode assembly can be inserted between the auxiliary membranes, and the easy removal regions are aligned with each other. A sandwiching body in which at least a part of the outer peripheral edge portions are bonded to each other so as to maintain the state . Adhesive to an electrolyte membrane-catalyst layer assembly in which catalyst layers are formed on both sides of the electrolyte membrane, or to an electrolyte membrane-electrode assembly in which electrodes comprising a catalyst layer and a gas diffusion layer are formed on both sides of the electrolyte membrane, respectively. An auxiliary film comprising a base material and an ionizing radiation curable resin that is formed on the base material and adheres to the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly by irradiation with light or ionizing radiation. Including two auxiliary films formed in a frame shape having an adhesive layer including and having an opening in the center ;
The auxiliary membranes are arranged so that the adhesive layers face each other, and an electrolyte membrane-catalyst layer assembly or an electrolyte membrane-electrode assembly can be inserted between the auxiliary membranes, and the openings are aligned with each other. A sandwiching body in which at least a part of the outer peripheral edge portions are bonded to each other so as to maintain the same . Adhesive to an electrolyte membrane-catalyst layer assembly in which catalyst layers are formed on both sides of the electrolyte membrane, or to an electrolyte membrane-electrode assembly in which electrodes comprising a catalyst layer and a gas diffusion layer are formed on both sides of the electrolyte membrane, respectively. An auxiliary film comprising a base material and an ionizing radiation curable resin that is formed on the base material and adheres to the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly by irradiation with light or ionizing radiation. An auxiliary film having an adhesive layer including and having a removable easily removable region formed in the center for forming an opening;
Adhesive to an electrolyte membrane-catalyst layer assembly in which catalyst layers are formed on both sides of the electrolyte membrane, or to an electrolyte membrane-electrode assembly in which electrodes comprising a catalyst layer and a gas diffusion layer are formed on both sides of the electrolyte membrane, respectively. An auxiliary film comprising a base material and an ionizing radiation curable resin that is formed on the base material and adheres to the electrolyte membrane-catalyst layer assembly or the electrolyte membrane-electrode assembly by irradiation with light or ionizing radiation. An auxiliary film formed in a frame shape having an adhesive layer including an opening in the center,
Each of the auxiliary membranes is disposed so that the adhesive layers face each other, and an electrolyte membrane-catalyst layer assembly or an electrolyte membrane-electrode assembly can be inserted between the auxiliary membranes, and the easily removable region and the opening A sandwiching body in which at least a part of the outer peripheral edge portions are bonded to each other so as to maintain the state in which they are aligned with each other . The said base material is a clamping body in any one of Claims 1-3 which has gas barrier property which prevents permeation | transmission of fuel gas and oxidizing agent gas. The sandwich body according to claim 4, wherein the base material is a biaxially stretched polyethylene naphthalate film. Preparing an electrolyte membrane-catalyst layer assembly in which a catalyst layer is formed on both sides of the electrolyte membrane;
Preparing two auxiliary films having an adhesive layer containing an ionizing radiation curable resin that adheres to the electrolyte membrane-catalyst layer assembly by irradiating with light or ionizing radiation, and stacking them on each other;
A step of producing a sandwiched body by adhering at least a part of the outer peripheral edge of each auxiliary membrane so that the electrolyte membrane-catalyst layer assembly can be inserted and the two auxiliary membranes are not displaced from each other When,
Forming a center, to form an opening for exposing except the outer peripheral edge of the catalyst layer, remove it possible readily removable region of each sub-film of the fabricated holding member,
Inserting the electrolyte membrane-catalyst layer assembly between the auxiliary membrane in which the easy removal region is formed, until the catalyst layer excluding the outer peripheral edge is opposed to the easy removal region;
Removing each of the easy removal regions and forming an opening;
After forming the opening, irradiating light or ionizing radiation to bond each auxiliary membrane to the outer peripheral edge of the electrolyte membrane-catalyst layer assembly;
A method for producing a sandwiched electrolyte membrane-catalyst layer assembly comprising: In the manufacturing method of the electrolyte membrane-catalyst layer assembly with a clamping body according to claim 6 ,
The manufacturing method of the electrolyte membrane electrode assembly with a clamp body further provided with the process of forming a gas diffusion layer thicker than the thickness of the said auxiliary | assistant film | membrane on each catalyst layer exposed from the said opening part. Preparing an electrolyte membrane-electrode assembly in which electrodes comprising a catalyst layer and a gas diffusion layer are formed on both surfaces of the electrolyte membrane;
Preparing two auxiliary films having an adhesive layer containing an ionizing radiation curable resin that adheres to the electrolyte membrane-electrode assembly by irradiating with light or ionizing radiation and stacking them on each other;
Adhering at least a part of the outer peripheral edge of each auxiliary membrane so that the electrolyte membrane-electrode assembly can be inserted and the two auxiliary membranes are not displaced from each other; ,
Forming a center, to form an opening for exposing except the outer peripheral edge portion of the electrode, you can remove it a readily removable region of each sub-film of the fabricated holding member,
Inserting the electrolyte membrane-electrode assembly between the auxiliary membrane in which the easy removal region is formed, until the electrode excluding an outer peripheral edge faces the easy removal region;
Removing the easy removal region to form an opening;
After forming the opening, irradiating with light or ionizing radiation to bond the auxiliary films to the outer peripheral edge of the electrolyte membrane-electrode assembly and bonding the outer peripheral edges of the auxiliary films to each other;
The manufacturing method of the electrolyte membrane-electrode assembly with a clamp body provided with. The method for producing an electrolyte membrane-electrode assembly with a sandwich according to claim 7 or 8 ,
Installing a gasket on each auxiliary membrane so as to surround each electrode comprising the catalyst layer and the gas diffusion layer; and
Installing a separator on each of the electrode and gasket;
A method for producing a polymer electrolyte fuel cell, further comprising:

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