JP2003257438A - Roll press device for catalyst layer transfer - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a roll press device for catalyst layer transfer in which a catalyst layer is transferred in a shape of a transfer part to a solid polymer electrolyte membrane by using a heating and pressing roll with the transfer part and damage to the solid polymer electrolyte membrane can be reduced. <P>SOLUTION: This roll press device for catalyst layer transfer has a preventing means 100c for preventing an excess pressing force from acting on the transfer part 100a locally due to the elastic displacement of the transfer part 100a caused by a pressing force acting on the transfer part 100a by the heating and pressing roll 100 with the transfer part. More specifically, since the transfer part 100a is elastically displaced by the pressing force acting thereon, the excess pressing force can be prevented from acting on the transfer part 100a. As a result, the damage to the solid polymer electrolyte membrane by the transfer part 100a can be reduced. <P>COPYRIGHT: (C)2003,JPO

Description

Detailed Description of the Invention

[0001]

TECHNICAL FIELD The present invention relates to a roll press device for transferring a catalyst layer. More specifically, it is a roll press device for transferring a catalyst layer onto a solid polymer electrolyte membrane used in a solid polymer electrolyte membrane fuel cell.

[0002]

2. Description of the Related Art A solid polymer electrolyte membrane used in a solid polymer electrolyte membrane fuel cell is bonded to a catalyst layer to form a catalyst layer.
As a method of forming an electrolyte membrane assembly, Japanese Patent Laid-Open No. 2000-
As described in Japanese Patent No. 90944, "An ink-like or paste-like catalyst mixture is applied onto a catalyst layer-forming substrate by a method such as a precipitation method, a printing method or a spray method to form a uniform catalyst layer. After that, a transfer method has been devised in which the catalyst layer and the electrolyte membrane are integrally joined by heating and press-contacting this with the electrolyte membrane "(Japanese Patent Laid-Open No. 2000-90944, page (2)). In this case hot press (hot press)
Alternatively, the solid polymer electrolyte membrane and the catalyst layer previously formed on the catalyst layer-supporting base material are heated and pressurized using a hot roll (heating and pressure roll) to be integrally bonded.

For example, Japanese Unexamined Patent Publication No. 10-64574 discloses both a method using a hot press (hot press) and a method using a hot roll (heating pressure roll). The method using the hot roll disclosed in this publication is, as shown in FIG. 1, a long solid polymer electrolyte membrane 81 and a long catalyst layer carrying catalyst layers 82 and 83 arranged on both sides thereof. A film 84 as a supporting substrate,
The solid polymer electrolyte membrane 81 and the catalyst layers 82 and 83 are integrally joined by sandwiching 85 and 85 with a pair of heating / pressurizing rolls 86 and heating and pressing, and then the catalyst layer 8
This is a method of peeling the films 84 and 85 carrying 2, 83 from the catalyst layers 82 and 83 using a pair of peeling rolls 87. This publication also discloses a method of transferring the catalyst layer formed on the catalyst layer-supporting substrate to the solid polymer electrolyte membrane using a hot press, but the method of transferring using a hot roll is more solid. Since the transfer of the catalyst layer to the polymer electrolyte membrane can be continuously performed, it is considered to be more productive than the transfer method using hot pressing.

[0004]

However, when transferring the catalyst layer to the solid polymer electrolyte membrane in this way, all the catalyst layer formed on the catalyst layer-supporting substrate is transferred to the solid polymer electrolyte membrane. There is a case where it is desired to transfer a predetermined portion of the catalyst layer formed in the catalyst layer supporting base material to the solid polymer electrolyte membrane, instead of joining.

As shown in FIG. 2, this does not cover the entire surface of the solid polymer electrolyte membrane A with the catalyst layer B, but covers the solid polymer electrolyte membrane A with the catalyst layer B leaving the edge portion. The catalyst layer-electrolyte membrane assembly C, in other words, the solid polymer electrolyte membrane A has a larger area than the catalyst layer B, and the solid polymer electrolyte membrane A protrudes from the catalyst layer B. This is for producing C.

By thus reducing the surface area of the catalyst layer B to be smaller than that of the solid polymer electrolyte membrane A, spacers made of a fluororesin such as polytetrafluoroethylene are formed at the edges not covered with the catalyst layer B. Silicon rubber or the like may be laminated on the spacer as an electrical insulator to seal the catalyst layer so that fuel gas and oxygen gas do not leak. As a result, it is possible to prevent an electrical short circuit from occurring between the anode side separator and the cathode side separator, which are arranged so as to sandwich the catalyst layer-electrolyte membrane assembly from both sides.

The applicant of the present invention discloses a heating and pressurizing roll used for transferring the catalyst layer having a predetermined shape to the solid polymer electrolyte membrane as described above in Japanese Patent Laid-Open No. 2001-196070. As shown in FIG. 3, the heating / pressurizing roll 88 is a roll in which a convex transfer portion 88a having a predetermined shape is engraved on the outer peripheral surface of the heating / pressurizing roll 88. The heating and pressing roll 8 engraved with such a convex transfer portion 88a.
When the film supporting the catalyst layer and the solid polymer electrolyte membrane are heated and pressed using No. 8, heating and pressurization on the catalyst layer and the solid polymer electrolyte membrane act on this convex transfer portion 88a. , Does not act on any portion other than this convex transfer portion 88a. Therefore, the portion of the catalyst layer corresponding to the transfer portion 88a is joined and integrated with the solid polymer electrolyte membrane. Then, the portion of the catalyst layer corresponding to the portion other than the transfer portion is separated together with the film from the portion of the catalyst layer corresponding to the portion of the transfer portion 88a. In this way, the catalyst layer matching the shape of the transfer portion 88a can be transferred to the solid polymer electrolyte membrane.

However, when the convex transfer portion is provided on the outer peripheral surface of the heating and pressing roll in this way, and the portion of the catalyst layer matching the shape of the transfer portion is transferred to the solid polymer electrolyte membrane, the following occurs. It has become clear that various problems will occur.

A solid polymer electrolyte membrane is prepared by using a roll pressing device having a pair of heating and pressing rolls, one heating and pressing roll being a heating and pressing roll with a transfer portion having a convex transfer portion on the outer peripheral surface. In the case of transferring the catalyst layer onto the sheet, as shown in FIG. 4, the heating / pressurizing roll 90 with a transfer portion provided with the convex transfer portion 90a and the normal heating / pressurization without the convex transfer portion are provided. The catalyst layer-supporting base material 93 having the catalyst layer 92 formed on the surface thereof by the roll 91 and the solid polymer electrolyte membrane 94 are sandwiched together and heated and pressed to transfer the catalyst layer 92 to the solid polymer electrolyte membrane 94. In this case, the air cylinder 95 is attached to one of the heating / pressurizing rolls 90 to adjust and control the pressure applied by the two heating / pressurizing rolls 90, 91 and the clearance between the two heating / pressurizing rolls 90, 91. Then, the solid polymer electrolyte membrane 94 and the catalyst layer supporting base material 93 having the catalyst layer 92 formed on the surface thereof are sandwiched. Then, the pair of heating / pressurizing rolls are rotated by using a driving means (not shown) such as a motor to continuously transfer the catalyst layer 92 to the solid polymer electrolyte membrane 94. In the example of the pair of heating / pressurizing rolls 90 and 91 shown in FIG. 4, the air cylinder 95 is attached to the heating / pressurizing roll 90 with the transfer portion to control the transfer pressure.

In this way, the catalyst layer 92 is formed by using the heating / pressurizing roll 90 with the transfer portion and the ordinary heating / pressurizing roll 91.
To transfer to the solid polymer electrolyte membrane 94, the convex transfer portion 90a of the heating / pressurizing roll 90 with the transfer portion has.
The catalyst layer 92, the catalyst layer-supporting base material 93, the solid polymer electrolyte membrane 94, etc., which are pressed by the counterpart normal heating and pressing roll 91, are pushed into the groove portions or concave portions 90b located between them. , The shape will be slightly distorted.

While the pair of heating / pressurizing rolls 90 and 91 are rotating, the catalyst layer-supporting base material 93 carrying the catalyst layer 92 and the solid polymer electrolyte membrane 94 are sequentially sandwiched to continuously press the catalyst layer 92. Since it is transferred to the solid polymer electrolyte membrane 94, as shown in FIG. 5, the catalyst layer 92 is pushed into the groove portion or the concave portion 90b located between the convex transfer materials 90a and slightly distorted. A catalyst layer supporting substrate 93,
The solid polymer electrolyte membrane 94 and the like hit the end portion or the edge of the convex transfer portion 90a, and an excessive pressing force is applied to the sandwiched solid polymer electrolyte membrane 94 and catalyst layer 92. As a result, the problem that the solid polymer electrolyte membrane 94 and the catalyst layer 92 are damaged occurs.

Further, in the case where the convex transfer portion is provided on the outer peripheral surface of one of the heating and pressing rolls to transfer the catalyst layer to the solid polymer electrolyte membrane, the heating and pressing roll of the other side is added. It is common to use a rubber-coated heating and pressing roll in which the surface of the pressure surface, that is, the outer peripheral surface is coated with rubber. The rubber coating on the outer peripheral surface of one of the heating / pressurizing rolls in this way absorbs the surface accuracy of the heating / pressurizing roll and the work to make the surface pressure applied to the surface of the transfer portion uniform, thereby preventing transfer defects. This is to prevent it.

As described above, the solid polymer electrolyte membrane and the catalyst layer-supporting base material carrying the catalyst layer are heated and pressurized while rotating the heating and pressure roll with the transfer portion and the rubber-coated heating and pressure roll. When trying to transfer a catalyst layer that matches the shape of the transfer part to the electrolyte membrane, an excessive pressing force is applied even when using the above-mentioned normal heating and pressing roll without rubber coating. It becomes easy to join the end part of.

That is, when the counterpart of the heating / pressurizing roll with the transfer portion is a rubber-coated heating / pressurizing roll, the groove portion, that is, the concave portion located between the convex transfer portions has a rubber-covered heating / pressurizing roll of the counterpart. The rubber coated on the outer peripheral surface is deformed by the pressing force and bites into it. Therefore, due to the rotation of the heating / pressurizing roll, the deformed rubber causes an excessive pressing force to be applied to the end portion of the transfer portion facing the rubber-coated heating / pressurizing roll. as a result,
The portion of the solid polymer electrolyte membrane and the catalyst layer sandwiched between the end of the transfer portion and the deformed rubber is excessively compressed and deformed, and the solid polymer electrolyte membrane and the catalyst layer in this portion are damaged. The problem arises.

Therefore, an object of the present invention is to provide a catalyst layer transfer roll press device for transferring a catalyst layer to a solid polymer electrolyte membrane in the shape of a transfer part by using a heating and pressing roll having a transfer part, It is an object of the present invention to provide a roll press device for transferring a catalyst layer, which can reduce damage to the solid polymer electrolyte membrane.

[0016]

[Means, Actions and Effects for Solving the Problems] (1) As described above, damage to the solid polymer electrolyte membrane is caused by the convex transfer portion and the convex transfer portion of the heating / pressurizing roll with the transfer portion. The catalyst layer-carrying base material having the solid polymer electrolyte membrane or the catalyst layer formed on the surface is pushed by the partner heating and pressing roll toward the concave portion between Rotation causes excessive pressure to act on the edge of the convex transfer part, resulting in excessive pressure on the solid polymer electrolyte membrane or catalyst layer pushed in the direction of the concave part. Occurs in.

(2) First Invention (Claims 1 to 10) In this case, the present inventor sets the transfer section of the heating and pressing roll with the transfer section so as to be elastically displaced. It was thought that it is possible to prevent an excessive pressing force from the other party heating and pressing roll from directly acting on the end portion of the transfer portion.

The present inventor then, as a first invention, presses the solid polymer electrolyte membrane of the fuel cell and the catalyst layer-supporting base material on which the catalyst layer is formed on the surface of the solid polymer electrolyte membrane so as to attach the solid polymer electrolyte membrane to the surface of the solid polymer electrolyte membrane. It has a pair of heating / pressurizing rolls for transferring the catalyst layer, and at least one of the pair of heating / pressurizing rolls has a roll-shaped main body and a convex transfer portion formed on the outer peripheral surface of the main body. In a roll pressing device for a catalyst layer transfer, which is a heating / pressing roll with a transfer part, the heating / pressing roll with a transfer part is locally displaced to the transfer part by elastically displacing the transfer part by the pressing force acting on the transfer part. The present invention has invented a roll-pressing device for transferring a catalyst layer, which has a preventing means for preventing an excessive pressing force from being applied to the roll pressing device.

That is, if the transfer portion is elastically displaced by the pressing force acting on the transfer portion, it is possible to prevent an excessive pressing force from acting on the transfer portion. As a result, the occurrence of damage to the solid polymer electrolyte membrane due to the presence of the transfer portion can be reduced.

In this case, as a preventive means for elastically displacing the transfer portion, the transfer portion itself is elastically deformed without being deformed by the pressing force from the other heating / pressurizing roll. A method of displacing the transfer portion and a method of elastically displacing the surface of the transfer portion by deforming the transfer portion can be considered.

First, the prevention means using a method in which the entire transfer portion is elastically displaced will be described.

The preventing means may be an elastic body interposed between the main body portion and the transfer portion. In this case, it is preferable to use rubber for the elastic body from the viewpoint of high elastic modulus. When an elastic body such as rubber is interposed between the roll-shaped main body of the heating / pressurizing roll and the transfer portion, when the pressing force is applied to the transfer portion from the counterpart heating / pressurizing roll, this elastic body Is elastically deformed, that is, compressed, and the transfer portion itself is elastically displaced toward the center of the heating and pressing roll,
It is possible to prevent an excessive pressing force from acting locally on the transfer portion.

Further, the preventing means may be a spring interposed between the main body portion and the transfer portion. When a spring is interposed between the roll-shaped body of the heating / pressurizing roll and the transfer part, this spring is compressed when the pressing force is applied to the transfer part from the other heating / pressurizing roll, and the transfer is performed. The portion itself is elastically displaced toward the center of the heating and pressing roll, and it is possible to prevent the transfer portion from being locally subjected to an excessive pressing force.

Similarly, the preventing means can be an air cylinder interposed between the main body portion and the transfer portion. Also in this case, when a pressing force is applied to the transfer section from the other heating / pressurizing roll, the air cylinder is compressed and the transferring section itself is elastically displaced in the direction of the center of the heating / pressurizing roller, and is transferred to the transferring section. It is possible to prevent an excessive pressing force from acting locally.

When the preventing means is an elastic body, a spring or an air cylinder interposed between the main body portion and the transfer portion as described above, it is preferable that the end portion of the transfer portion has a tapered surface or an R shape. . By thus forming the end portion of the transfer portion into a tapered surface or an R shape, the pressing force acting on the end portion of the transfer portion does not act on the end portion at once, but gradually acts on the end portion. Can be As a result, it is possible to more effectively prevent an excessive pressing force from acting locally on the transfer portion, and as a result, it is possible to further reduce the occurrence of damage to the solid polymer electrolyte membrane or the catalyst layer. .

Here, "the end portion of the transfer portion is a taper surface" means that a groove portion screen for defining a groove portion, that is, a concave portion between the convex transfer portion and the convex transfer portion is radially formed. On the other hand, it means that the angle between the groove screen of the transfer portion and the transfer surface, that is, the surface of the transfer portion is made larger than a right angle by giving an angle. Further, "the end portion of the transfer portion has an R shape" means that a corner portion formed by the transfer surface of the transfer portion and the groove section screen is rounded to have an R shape.

The heating / pressurizing roll, which is the counterpart of the heating / pressurizing roll with the transfer portion, may be in a form having a roll-shaped main body and a rubber coating portion covering the outer peripheral surface of the main body.

When the preventing means is an elastic body, a spring or an air cylinder interposed between the main body portion and the transfer portion,
It is preferable that the other heating / pressurizing roll of the heating / pressurizing roll with the transfer portion has a roll-shaped main body and a cover made of an elastic body covering the outer peripheral surface of the main body. In this case, it is preferable to use rubber as the elastic body from the viewpoint of high elastic modulus. In this way, by coating the outer peripheral surface of the other heating / pressurizing roll with the transfer part with an elastic body, it is possible to uniformly apply pressure to the transfer part and prevent transfer defects. be able to.

Next, a description will be given of prevention means using a method of deforming the transfer portion and elastically displacing the surface of the transfer portion.

The method of elastically displacing the surface of the transfer portion due to the deformation of the transfer portion is, specifically, to cover the surface of the transfer portion with an elastic body, and the elastic body is pressed by a pressing force. It can be realized by deforming.

That is, the transfer section of the heating and pressing roll with the transfer section has a convex base formed on the outer peripheral surface of the main body and a surface layer made of an elastic material covering the surface of the base,
The prevention means can be an elastic body coated as a surface layer.

By making the surface layer of the transfer portion an elastic body, when a pressing force is applied to the transfer portion from the counterpart heating and pressing roll, this elastic body is elastically deformed and the surface of the transfer portion is displaced. . As a result, it is possible to prevent an excessive pressing force from acting on the surface of the transfer portion, particularly on the end portion of the transfer portion. Therefore, it is possible to reduce a situation in which the solid polymer electrolyte membrane is damaged due to an excessive pressing force.
In this case, it is preferable to use rubber as the elastic body from the viewpoint of high elastic modulus.

In the case where the surface layer is provided on the transfer portion in this way, the heating / pressurizing roll facing the heating / pressurizing roll with the transferring portion may be a normal heating / pressurizing roll having no rubber coating, It is also possible to adopt a form in which is covered with a rubber coating.

In this case, it is preferable that the heating / heating roll facing the heating / pressurizing roll with the transfer portion has no rubber coating. Rather than rubber coating both
The rubber coating on only one side can make the shape of the catalyst layer transferred to the solid polymer electrolyte membrane sharper.

As described above, in the roll pressing device for transferring the catalyst layer of the present invention, the transfer part of the heating / pressurizing roll with the transferring part is elastically displaced by the pressing force from the counterpart heating / pressurizing roll, so that the transferring part is transferred. It is possible to prevent an excessively large pressing force from acting locally, and as a result, it is possible to reduce the occurrence of damage to the solid polymer electrolyte membrane to which the catalyst layer is transferred.

(3) Second invention (claims 10 to 1)
1) Further, the present inventor has found that the excessive pressing force acts on the end portion (edge) of the convex transfer portion even when the groove portion between the transfer portion and the transfer portion, that is, the concave portion is heated by the other party. A pressing force is applied from the pressure roll to the work, that is, the catalyst layer-supporting base material having the solid polymer electrolyte membrane and the catalyst layer formed on the surface, and the pressing force also applied to this concave portion is the rotation of the heating pressure roll. It was thought that this is because it works as it is at the end of the transfer part. Therefore, it is considered that it is sufficient to prevent the pressing force from being applied to the solid polymer electrolyte membrane and the catalyst layer supporting base material from the heating and pressing roll in the concave portion between the transfer portions.

The present inventor then, as a second invention, presses the solid polymer electrolyte membrane of the fuel cell and the catalyst layer-supporting base material on which the catalyst layer is formed on the surface to press the solid polymer electrolyte membrane on the surface of the solid polymer electrolyte membrane. In a roll pressing device for transferring a catalyst layer having a pair of heating / pressurizing rolls for transferring a catalyst layer, the pair of heating / pressurizing rolls are both a roll-shaped main body part and a convex transfer part formed on the outer peripheral surface of the main body part. And the transfer part of one heating and pressing roll and the transferring part of the other heating and pressing roll are plane-symmetrical with the solid polymer electrolyte membrane sandwiched by the pair of heating and pressing rolls as a plane of symmetry. The present invention invented a roll press device for transferring a catalyst layer, which is characterized by

As described above, both of the pair of heating / pressurizing rolls are provided with the transfer portions which are plane-symmetric with respect to the solid polymer electrolyte membrane sandwiched by the heating / pressurizing rolls as planes of symmetry. By rotating a pair of heating / pressurizing rolls in synchronization so that the transfer parts of the rolls correspond to each other, the solid polymer electrolyte membrane and the catalyst layer are formed in the groove part, that is, the concave part located between the transfer parts. It is possible to prevent the catalyst layer-carrying base material formed on the surface thereof from being pinched by the pair of heating and pressing rolls. Therefore, in the concave portion between the transfer portions, no pressing force is applied from the heating / pressurizing roll to the solid polymer electrolyte membrane and the catalyst layer-supporting base material supporting the catalyst layer, and the solid polymer at the end portion of the transfer portion. It is possible to avoid an excessive pressing force acting on the catalyst layer-supporting base material supporting the electrolyte membrane and the catalyst layer. As a result, it is possible to reduce damage to the solid polymer electrolyte membrane and the catalyst layer.

In this case, it is preferable that the end portion of the transfer portion has a tapered surface or an R shape. By thus forming the end portion of the transfer portion into the tapered surface or the R shape, the pressing force does not act at once at the end portion of the transfer portion, but can gradually act on the end portion. . As a result, it is possible to further prevent an excessive pressing force from locally acting on the transfer portion, and as a result, it is possible to further reduce damage to the solid polymer electrolyte membrane and the catalyst layer.

As described above, according to the roll pressing device for transferring the catalyst layer of the present invention, the pressing force is not applied to the solid polymer electrolyte membrane and the catalyst layer in the concave portion located between the transfer portions, so It is possible to prevent an excessive pressing force from being locally applied to the pair of transfer parts opposed to each other by the rotation of the heating and pressing roll, and as a result, the damage to the solid polymer electrolyte membrane to which the catalyst layer is transferred is prevented. Occurrence can be reduced.

[0041]

BEST MODE FOR CARRYING OUT THE INVENTION Embodiments of a roll pressing apparatus for transferring a catalyst layer according to the present invention will be described below.

(1) First, the structure of the roll pressing apparatus for transferring the catalyst layer of the present invention will be described.

The catalyst layer transfer roll pressing apparatus of the present invention comprises a catalyst layer transfer roll pressing apparatus of the first aspect and a second aspect of the present invention.
In any of the roll pressing apparatus for transferring the catalyst layer of the invention, the solid polymer electrolyte membrane of the fuel cell (hereinafter referred to as “electrolyte membrane”)
And a catalyst layer-carrying base material having a catalyst layer formed on the surface thereof are sandwiched to transfer the catalyst layer onto the surface of the electrolyte membrane. is there. In the catalyst layer transfer roll press device of the first invention, at least one of the pair of heating and pressing rolls has a roll-shaped main body and a convex transfer portion formed on the outer peripheral surface of the main body. In the catalyst layer transfer roll pressing device of the second invention, both of the pair of heat and pressure rolls are heat and pressure rolls with a transfer part.

The catalyst layer transfer roll pressing apparatus of the present invention is a catalyst for transferring a catalyst layer onto an electrolyte membrane by using a pair of heating and pressing rolls, except for the feature of the structure of a pair of heating and pressing rolls. It can be realized by using a usual structure of a layer transfer roll press machine. That is, in addition to the pair of heating / pressurizing rolls, a heating device such as a heater for heating the heating / pressurizing rolls, a pressurizing device such as an air cylinder for exerting a pressure between the pair of heating / pressurizing rolls, and the heating / pressurizing rolls. It can be configured by using a driving unit such as a motor for rotating the.

That is, the catalyst layer transfer roll pressing device of the present invention is characterized by a pair of heating and pressing rolls in both the first invention and the second invention, and the other parts are basically the same in structure. It can be realized with the same structure as a normal roll pressing device for transferring a catalyst layer using a pair of heating and pressing rolls.

(2) Next, the form of a pair of heating and pressing rolls that can be used in the catalyst layer transfer roll pressing device of the first invention will be described.

In the pair of heating / pressurizing rolls used in the roll pressing apparatus for transferring the catalyst layer of the first invention, at least one of the pair of heating / pressurizing rolls is formed on the roll-shaped main body and the outer peripheral surface of the main body. A heating / pressurizing roll with a transfer part having a raised transfer part, wherein the heating / pressurizing roll with the transfer part is elastically displaced by the pressing force acting on the transfer part. It has a prevention means for preventing an excessive pressing force from acting locally on the transfer portion.

Regarding this pair of heating and pressing rolls,
One of them may be a heating / pressurizing roll with a transfer portion, and the other may be a normal heating / pressurizing roll having no convex transfer portion. Further, one may be a heating / pressurizing roll having a transfer portion, and the other may be a heating / pressurizing roll having a roll-shaped main body and a rubber coating portion covering the outer peripheral surface of the main body. Further, any of them may be a heating / pressurizing roll with a transfer portion. In this case, the transfer portions of the pair of heating / pressurizing rolls can be configured so as to be plane-symmetrical with the electrolyte membrane sandwiched by the pair of heating / pressurizing rolls as a plane of symmetry.

As a means for preventing the transfer portion from being displaced locally by elastically deforming the surface of the transfer portion and preventing an excessive pressing force from acting locally on the transfer portion, a heating / pressurizing roll with a transfer portion is used. The elastic body covered as the surface layer in the case where the convex transfer portion has a convex base formed on the outer peripheral surface of the main body and a surface layer made of an elastic body covering the surface of the base, Can be mentioned.

In this case, as the elastic body, rubber, highly elastic synthetic resin, thermoplastic elastomer or the like can be used.

For example, as rubber, nitrile rubber (NB
R), acrylic rubber (ACM), fluorosilicone rubber (FVMQ), fluororubber (FKM) and the like can be used. Further, as the highly elastic synthetic resin, polyamide resin, polyacrylic resin, polyester resin, phenol resin, cellulose resin, polyimide resin, polyvinyl alcohol resin, polyvinyl chloride resin, polypropylene resin, polybenzimidazole resin, polyurethane resin, polybutadiene resin It is possible to use a material having high elasticity such as. Further, various thermoplastic elastomers can be used. In this case, it is preferable to use rubber from the viewpoint of preventing a rapid pressure increase.

In this case, the thickness of the surface layer made of an elastic body can be set to an appropriate thickness depending on the type of the elastic body used, but it can be set to about 0.1 to 10 mm, preferably. It can be 0.5 to 5 mm.

Here, the convex base 100 of the transfer part 100a is used as the surface layer 100aa of the transfer part 100a of which one side is convex.
A heating / pressurizing roll 90 with a transfer portion having an elastic body coated on the surface of ab, and the other is a normal heating / pressurizing roll 1
A pair of heating and pressing rolls of No. 01 is shown in FIG. In addition, about the code | symbol in FIG. 6, FIG. 7, FIG. 8, FIG. 9 and FIG. 10 below, the same code | symbol was used about the member of the same kind.

The transfer portion 100a of the heating / pressurizing roll 100 with the transfer portion is provided with a convex base 100ab and the base 100a.
Surface layer 100aa made of an elastic material that covers the surface of ab
In the configuration configured by and, the roll-shaped main body 100
b and a convex base 100ab formed on the surface thereof are formed, and the surface of the base 100ab is coated with an elastic body to form a surface layer 100aa, thereby producing the heating / pressurizing roll 100 with a transfer portion. You can

In this case, the roll-shaped main body and the convex base can be integrally formed by engraving a normal heating and pressing roll. When the roll-shaped main body and the convex base are integrally formed in this way, for example, a carbon steel of JIS standard G4051 S45C (hereinafter abbreviated as "S45C") plated with HCr is used as a material. Can be used.

Further, a plate serving as a convex base is prepared in advance, the surface of the plate is covered with an elastic body to form a surface layer, and then the plate on which the surface layer is formed is rolled into a roll-shaped main body portion. It can also be glued to. In this case, the body is made of S45C carbon steel plated with HCr, and the convex base plate is also made of S45C carbon steel plated with HCr. The surface facing the roll-shaped main body can be formed in a shape corresponding to the shape of the main body.

By elastically displacing the transfer portion itself, as a preventive means for preventing an excessively large pressing force from being locally applied to the transfer portion, the transfer portion between the roll-shaped main body portion and the convex-shaped transfer portion is used. An elastic body, a spring, an air cylinder, and the like interposed in the above can be cited.

Here, the roll-shaped main body portion 100b, the convex-shaped transfer portion 100a, and the elastic body 100 interposed therebetween are provided.
FIG. 7 shows a heating / pressurizing roll 100 with a transfer portion having c. The heating / pressurizing roll 100 shown in FIG.
Elastic body 10 interposed between 00b and transfer section 100a
0c covers the entire outer peripheral surface of the main body 100b, and a convex transfer portion 100a is formed on the surface of the elastic body 100c which covers the entire outer peripheral surface of the main body 100b. ing. In this case, the transfer part 100a
Since the elastic body 100c is interposed between the main body portion 100b and the main body portion 100b, the transfer portion 100a has a roll-shaped main body portion 100b.
It can be constituted by a convex plate having a shape adapted to the outer peripheral surface of the. In this case, a convex transfer plate 100a can be formed by bonding a convex plate to the surface of the elastic body 100c that covers the outer peripheral surface of the roll-shaped main body 100b.

As the elastic body used here, rubber, highly elastic synthetic resin, thermoplastic elastomer and the like can be used, as in the elastic body used as the surface layer of the transfer portion described above.

That is, for example, as the rubber, nitrile rubber (N
BR), acrylic rubber (ACM), fluorosilicone rubber (FVMQ), fluororubber (FKM) and the like can be used. Further, as the highly elastic synthetic resin, polyamide resin, polyacrylic resin, polyester resin, phenol resin, cellulose resin, polyimide resin, polyvinyl alcohol resin, polyvinyl chloride resin, polypropylene resin, polybenzimidazole resin, polyurethane resin, polybutadiene resin It is possible to use a material having high elasticity such as. Further, various thermoplastic elastomers can be used. It is preferable to use rubber from the viewpoint of a rapid pressure increase.

In this case, the thickness of the elastic body covering the outer peripheral surface of the roll-shaped main body can be appropriately set according to the type of elastic body used, but is generally 0.5 to
It can be set to 20 mm, preferably 2 to 5 mm.

The heating / pressurizing roll with a transfer portion for interposing the elastic body between the main body portion and the transfer portion has an elastic body only between the transfer portion and the main body portion in addition to the configuration shown in FIG. It can also be in the form of allowing. That is, even if the elastic body is not covered over the entire outer peripheral surface of the main body, the outer peripheral surface of the main body corresponding to the transfer portion can be covered with the elastic body.

FIG. 8 shows a heating / pressurizing roll having a roll-shaped main body portion 100b, a convex-shaped transfer portion 100a, and a spring 100d interposed therebetween. In the heating / pressurizing roll shown in FIG. 8, a gap is provided between the main body 100b and the transfer portion 100a.
The transfer portion 100a itself is elastically displaceable in the radial direction by a spring 100d interposed between b and the transfer portion 100a. That is, the main body 10
When the intervening spring 100d between 0b and the transfer portion 100a is compressed, the transfer portion 100a is also set to be displaced by the compression of the spring 100d toward the radial direction of the heating / pressurizing roll 100 with the transfer portion. There is.

As the spring, a spring such as a coil spring, a leaf spring or a disc spring can be used. In this case, it is preferable to use a coil spring. The coil spring is easy to assemble,
The stroke is excellent and the load can be easily controlled.

In this case, the transfer portion can be constructed by using a convex plate having a shape adapted to the outer peripheral surface of the roll-shaped main body portion with a spring interposed between the transfer portion and the main body portion. Therefore, in this case, the transfer section and the main body section are coupled with each other with the spring interposed between the transfer section and the main body section. When the spring is used as described above, it is preferable that the spring characteristics do not change under heating.

In the heating / pressurizing roll with a transfer portion shown in FIG. 8, the spring portion may be an air cylinder. Even in the case of an air cylinder, a gap is provided between the main body and the transfer unit, and the transfer unit itself is arranged in the radial direction of the heating / pressurizing roll with the transfer unit by the air cylinder interposed between the main unit and the transfer unit. It is configured so that it can be elastically displaced. That is, when the air cylinder interposed between the main body portion and the transfer portion is compressed, the transfer portion is also set to be displaced by the compression around the radial direction of the heating and pressing roll with the transfer portion.

In this case as well, the transfer portion can be constructed by using a convex plate having a shape adapted to the outer peripheral surface of the roll-shaped main body portion with the air cylinder interposed between the transfer portion and the main body portion. . In this case, the transfer portion and the main body portion are coupled with each other through the air cylinder.

In this case, the main body of the heating / pressurizing roll with the transfer portion can be made of a material that can be used for forming a normal heating / pressurizing roll. For example, carbon steel of S45C plated with HCr can be used. Further, as the convex plate used for the convex transfer portion, it is possible to use the carbon steel of S45C plated with HCr.

In these cases, the transfer section using the convex plate and the main body section can be combined as follows. FIG. 9 shows a convex transfer portion 100a and a roll-shaped main body portion 1.
00b shows a partial cross-sectional view of the heating / pressurizing roll 100 with a transfer part, in which a spring 100d is interposed between the same and 00b, when cut in the axial direction. Insertion pins 100f extending in the axial direction of the transfer-applied heating and pressing roll 100 are attached to the end faces on both sides of the transfer unit 100a of the transfer-applied heating and pressing roll 100. Disc-shaped plate bodies 100g are fixed to the end surfaces on both sides of the main body portion 100b by bolts 100i. The disc-shaped plate body 100g is provided with an insertion hole 100h so that the insertion pin 100f can be inserted therein. The insertion hole 100h has a fixed length in the radial direction of the heating / pressurizing roll 100 with the transfer portion, and the insertion pin 100f has the transfer portion within the range of the radial length of the insertion hole 100h. Heat and pressure roll 1
It is possible to move in the radial direction of 00. The insertion pin 100f is fixed in the circumferential direction of the heating / pressurizing roll with a transfer portion.

As described above, the insertion pin 100f attached to the end surface of the transfer portion 100a is inserted into the insertion hole 100h of the disk-shaped plate body 100g attached to the main body portion 100b, whereby the transfer portion 100a is radially moved. It can be movably connected to the main body 100b. When the convex transfer portion 100a is pressed, this insertion pin 100f
The transfer portion 100a can be displaced in the radial direction within a range in which the transfer can be performed in the radial direction.

Here, the case where the spring 100d is interposed has been described as an example, but the connection can be made in this manner even if an air cylinder is interposed instead of the spring. Further, even when an elastic body such as rubber is interposed, the connection can be made in this way.

In the case where one of the pair of heating / pressurizing rolls has the main body portion, the transfer portion, and the elastic body, the spring or the air cylinder interposed between them, as described above, It is preferable that the end portion of the transfer portion has a tapered surface or an R shape. When the end portion of the transfer portion is a tapered surface, the angle between the groove section screen of the transfer section and the transfer surface of the transfer section, that is, the surface is the angle between the transfer surface and the groove section screen is 100 to 15.
It is preferably 0 degree.

When the end portion of the transfer portion has an R shape, the radius of the R shape is preferably approximately 0.2 to 1 mm.

When one of the pair of heating / pressurizing rolls is provided with the transfer part, the heating / pressurizing roll has a main body part, a transfer part, and an elastic body, a spring or an air cylinder interposed therebetween. The other heating / pressurizing roll is, as shown in FIG. 10, a heating member with an elastic body covering portion having a roll-shaped main body portion 102a and a covering portion 102b made of an elastic body and covering the outer peripheral surface of the main body portion. The pressure roll 102 is preferable. In this case, the thickness of the covering portion 102b made of an elastic body can be set to an appropriate thickness depending on the type of the elastic body, but can be about 0.5 to 20 mm, preferably 2 to 5 mm. be able to.

In this way, by making the outer peripheral surface of the other heating / pressurizing roll an elastic body, variations in surface accuracy of the transfer portion of the heating / pressurizing roll are absorbed at the time of transfer, so that the electrolyte membrane and both sides thereof are It is possible to uniformly apply pressure to the catalyst-supporting base material having the catalyst layer supported on the surface on which it is located. As a result, transfer failure can be prevented.

Also in this case, as the elastic body, the same elastic body as the above-mentioned elastic body for covering the surface of the transfer portion can be used. That is, rubber, highly elastic synthetic resin, thermoplastic elastomer or the like can be used. As rubber,
For example, nitrile rubber (NBR), acrylic rubber (AC
M), fluorosilicone rubber (FVMQ), fluororubber (FKM) and the like can be used. Further, as the highly elastic synthetic resin, polyamide resin, polyacrylic resin,
Polyester resin, phenol resin, cellulose resin,
Polyimide resin, polyvinyl alcohol resin, polyvinyl chloride resin, polypropylene resin, polybenzimidazole resin, polyurethane resin, polybutadiene resin or the like having a large elasticity can be used. Further, as the thermoplastic elastomer, various thermoplastic elastomers can be used. It is preferable to use rubber from the viewpoint of preventing a rapid pressure increase.

The diameter of the heating / pressurizing roll is not particularly limited, and a heating device for heating the heating / pressurizing roll, a pressure device such as an air cylinder for exerting a pressure between the pair of heating / pressurizing rolls, heating / pressurizing The size can be set to an appropriate size in consideration of the ability of a driving unit such as a motor for rotating the roll.

The heating / pressurizing roll with a transfer portion is not particularly limited and can be set to an appropriate size.
The diameter of the roll-shaped main body is set to about 200 to 300 mm, and the diameter including the transfer portion is 300 to 500 mm.
It is preferably set to about mm.

(3) The form of a pair of heating and pressing rolls that can be used in the roll pressing device for transferring the catalyst layer of the second invention will be described with reference to the drawings.

The pair of heating / pressurizing rolls used in the roll pressing device for transferring the catalyst layer of the second invention each have a roll-shaped main body and a convex transfer portion formed on the outer peripheral surface of the main body. The transfer part of one heating and pressing roll and the transfer part of the other heating and pressing roll are plane-symmetric with respect to the electrolyte membrane sandwiched between the pair of heating and pressing rolls as a plane of symmetry.

Here, the pair of heating / pressurizing rolls 110,
111 is shown in FIG. This pair of heating and pressing rolls 11
Reference numerals 0 and 111 include roll-shaped main body portions 110b and 111b and convex-shaped transfer portions 110a and 111a formed on the outer peripheral surfaces of the main body portions 110b and 111b. The transfer portion 111a of the other heating / pressurizing roll 111 is a pair of heating / pressurizing rolls 11
Since the electrolyte membrane (not shown) sandwiched between 0 and 111 is plane-symmetrical, the pair of heating and pressing rolls 11
In the concave portions 110e and 111e of 0 and 111,
No pressing force works on the sandwiched electrolyte membrane.

The heating / pressurizing roll used in the roll pressing device for transferring the catalyst layer of the second invention is, for example, a heating / pressurizing roll made of S45C carbon steel plated with HCr. By engraving the outer peripheral surface according to the shape and forming the transfer portion, the roll-shaped main body portion and the convex transfer portion can be integrally formed.

The diameter of the heating / pressurizing roll is not particularly limited, and a heating device for heating the heating / pressurizing roll, a pressure device such as an air cylinder for exerting a pressure between the pair of heating / pressurizing rolls, heating / pressurizing The size can be set to an appropriate size in consideration of the ability of a driving unit such as a motor for rotating the roll. Generally, the diameter of the heating and pressing roll is φ300 to 500
It is preferably set to about mm.

In this case, it is preferable that the end portion of the transfer portion has a tapered surface or an R shape. When the end portion of the transfer portion has a tapered surface, the angle between the groove section screen of the transfer section and the transfer surface of the transfer section, that is, the surface, is preferably 100 to 150 degrees between the transfer surface and the groove section screen. .

When the end portion of the transfer portion has an R shape, the radius of the R shape is preferably about 0.1 to 1 mm.

(4) Example Here, one heating / pressurizing roll is a heating / pressurizing roll having a roll-shaped main body part, a transfer part, and a spring interposed between the main body part and the transfer part, and the other heating / pressurizing roll is heated. A roll pressing device for a catalyst layer transfer using a pair of heating and pressing rolls, which is a heating and pressing roll having a roll-shaped main body and a coating portion made of rubber coated on the outer peripheral surface of the main body. An example in which the catalyst layer is transferred to the electrolyte membrane will be described using.

In the transfer of the catalyst layer to the electrolyte membrane, as in the usual case, the electrolyte membrane was arranged at the center, and a sheet having the anode catalyst layer formed on the both sides and a cathode catalyst layer were formed on the surface. The sheets were stacked, and the two sheets carrying the catalyst layer and the electrolyte membrane between them were put together and sandwiched by a pair of heating and pressing rolls, and heated and pressed.

In this embodiment, the pressure applied between the pair of heating / pressurizing rolls is controlled by using an air cylinder so that the transfer surface pressure becomes 3 MPa. Further, the maximum load of the spring interposed between the transfer portion and the main body portion was set so as not to exceed 4 MPa. The temperature of the pair of heating and pressing rolls is
The temperature was set to 120 ° C using a bar heater.

The feeding speed of the heating / pressurizing roll was set to 1 m / min using a drive motor.

Under these conditions, the contact pressure behavior when transferring the anode and cathode catalyst layers to the electrolyte membrane was measured by a load cell. At this time, the pressure-sensitive paper was used to measure the surface contact.

As a comparative example, an ordinary heating / pressurizing roll with a transfer portion, which is not provided with a preventing means such as a spring, a roll-shaped main body portion, and a rubber covered portion which covers the outer peripheral surface of the main body portion. The catalyst layer was transferred to the electrolyte membrane by using a catalyst layer transfer roll pressing device provided with a pair of heat and pressure rolls. In this comparative example, "the spring load is set so as to be maximum and not exceed 4 MPa."
The conditions were the same except that

In the comparative example, the transfer surface pressure is from 1 MPa to 5 MP.
Therefore, the variation of the transfer surface pressure is approximately ±
It was as large as about 2 MPa, and in particular, the variation was remarkable around the edges of the transfer portion.

On the other hand, in the embodiment, the transfer surface pressure is 3MP.
It was possible to keep the variation between a and 4 MPa, so that the variation of the transfer surface pressure could be suppressed to about ± 0.5 MPa. As a result, transfer failure with the electrolyte membrane, poor adhesion, and damage to the electrolyte membrane due to excessive surface pressure were suppressed, making it possible to manufacture a good catalyst layer-electrolyte membrane assembly.

(5) Next, a process of producing a catalyst layer-electrolyte membrane assembly by using a roll pressing device for catalyst layer transfer in a transfer process of transferring the catalyst layer to the electrolyte membrane will be described.

Outline of Process for Producing Catalyst Layer-Electrolyte Membrane Assembly The outline of the process for producing this catalyst layer-electrolyte membrane assembly is shown in FIG. This step consists of a general step in the case of producing a catalyst layer-electrolyte membrane assembly using a catalyst layer transfer roll pressing device, and the catalyst layer transfer roll pressing device of the present invention is It can be used by incorporating it into a general process.

Therefore, the pair of heating / pressurizing rolls of the catalyst layer transfer roll pressing device that can be used in the steps shown here are the same as the pair of heating / pressurizing rolls used in the catalyst layer transfer roll pressing device of the first invention. It is also possible to use a pair of heating and pressing rolls used in the catalyst layer transfer roll pressing device of the second invention. Note that, in FIG. 12, only a pair of heating / pressurizing rolls included in the catalyst layer transfer roll pressing device are illustrated, and other components and members such as a pressing device, a heating device, and a driving unit are not illustrated.

The step of producing the catalyst layer-electrolyte membrane assembly is performed on the surface of the catalyst layer-carrying substrate as a pre-step of the transfer step of transferring the catalyst layer to the electrolyte membrane by using the catalyst layer transfer roll press machine. The method includes a supporting step of applying a catalyst layer to form a catalyst layer on the surface of the catalyst layer supporting base material and supporting the catalyst layer, and a drying step of drying the catalyst layer formed on the surface of the catalyst layer supporting base material. Further, as a step subsequent to the catalyst layer transfer step, there is a peeling step of peeling the catalyst layer transferred to the electrolyte membrane from the catalyst layer supporting base material.

Carrying Step In the carrying step, the anode sheet AS carrying the anode catalyst layer AN on the surface, the anode sheet unwinding roll 20 for unwinding the anode sheet AS, and the cathode carrying the cathode catalyst layer CT on the surface are used. The sheet CS, the cathode sheet unwinding roll 30 that unwinds the cathode sheet CS, and the anode catalyst layer coating device 25 that coats the anode catalyst layer AN on the surface of the anode sheet AS.
And a cathode catalyst layer CT on the surface of the cathode sheet CS
For coating the cathode catalyst layer coating device 35, and further for feeding the anode sheet AS from the anode sheet unwinding roll 20 to the anode catalyst layer coating device 25. Anode sheet first feeding roll 21 and anode sheet third feeding It can be performed by using the cathode sheet first delivery roll 31 and the cathode sheet third delivery roll 33 that deliver the cathode sheet CS from the roll 23 and the cathode sheet unwind roll 30 to the cathode catalyst layer coating device 35. it can.

The anode sheet AS is a catalyst layer-supporting base material that supports the anode catalyst layer AN, and the cathode sheet CS is a catalyst layer-supporting base material that supports the cathode catalyst layer CT. The anode sheet AS and the cathode sheet CS do not dissolve or react even when they come into contact with the catalyst mixture described later, and are heat-resistant to withstand the temperature in the drying step and the transfer step described later. A sheet made of an elastic material can be used. Fluorine resin film such as polytetrafluoroethylene (tetrafluoride resin), or polyethylene terephthalate (PET)
Etc. can be used.

How the carrying process is performed will be described. The anode sheet AS and the cathode sheet CS are wound around the anode sheet unwinding roll 20 and the cathode sheet unwinding roll 30, respectively. The anode sheet AS and the cathode sheet CS unwound from the anode sheet unwinding roll 20 and the cathode sheet unwinding roll 30 are respectively the anode sheet first feeding roll 21 and the anode third feeding roll 23. Then, the cathode sheet is delivered to the anode catalyst layer coating device 25 and the cathode catalyst layer coating device 35 by the first delivery roll 31 and the third delivery roll 33 for cathode.

Then, the anode catalyst layer coating device 25 coats the anode catalyst layer on the surface of the anode sheet AS, and the cathode catalyst layer coating device 35 coats the cathode catalyst layer on the surface of the cathode sheet CS. In this way, the anode catalyst layer is formed on the surface of the anode sheet AS, and the cathode catalyst layer catalyst layer is formed on the surface of the cathode sheet CS.

The coating of these catalyst layers can be performed continuously by using, for example, a die coater as the catalyst layer coating devices 25 and 35. Further, the catalyst layer can be formed by a spray method.

The catalyst ink or catalyst mixture applied as the catalyst layer can be appropriately selected. This catalyst mixture is in the form of ink, carbon powder in which a catalyst metal such as platinum or other white metal metal or alloys thereof is carried in an alcohol such as ethanol or isopropyl alcohol (IPA), a solvent such as water, and a fluorine-based material. It is possible to use one obtained by adding and stirring an electrolyte solution or the like made of an ion exchange resin. Further, the thickness of the catalyst layer and the content of the catalyst can be appropriately selected.

Drying Step In the drying step, the anode sheet third delivery roll 23 and the cathode catalyst layer CT are applied to the surface so that the anode sheet AS having the anode catalyst layer AN applied to the surface is flatly extended. The cathode sheet third delivery roll 33 installed at a position where the manufactured cathode sheet CS is flatly extended, and the anode sheet AS flatly extended
A warm air dryer (not shown) for drying the anode catalyst layer AN carried on the surface of the cathode and a hot air dryer for drying the cathode catalyst layer CT carried on the surface of the flattened cathode sheet CS ( (Not shown) or the like. The location where the drying process is performed is shown in FIG.
Is indicated by H.

How the drying process is performed will be described. Anode sheet A having the surface coated with the anode catalyst layer AN
The cathode sheet CS coated with S and the cathode catalyst layer CT has an anode sheet third delivery roll 23 and a cathode sheet third delivery roll 3 respectively.
3 is sent from the anode coating device 40 and the cathode coating device 50.

The anode sheet AS and the cathode sheet CS are the anode sheet third delivery roll 2
3 and the cathode sheet third delivery roll 33, the anode catalyst layer AS and the cathode catalyst layer CS can be dried by a warm air dryer.

The dryer used here may be either a warm air heater or a steam heater, and any suitable dryer can be used.

The temperature here can be set at an appropriate temperature depending on the type of solvent used in the catalyst mixture. In this case, since a solvent such as water or alcohol is usually used, the temperature can be set to about 90 to 150 ° C. In this case, it is preferable to raise the temperature stepwise and dry.

The anode catalyst layer AN supported on the surface
Sheet AS for the anode and a sheet CS for the cathode in which the cathode catalyst layer CT carried on the surface is dried
Is the third anode sheet delivery roll 23.
Then, the cathode sheet is sent to the next step by the third sending roller 33.

Transfer Step In the transfer step, the electrolyte membrane unwinding roll 10 around which the electrolyte membrane ME is wound, the electrolyte membrane first unwinding roll 11 through which the electrolyte membrane ME wound around the electrolyte membrane unwinding roll 10 is sent out,
A pair of laminating rolls 40 and a pair of heating / pressurizing rolls 50, 51 for stacking an anode sheet and a cathode sheet, which have dried catalyst layers supported on their respective surfaces in a drying step, on both sides of the fed electrolyte membrane ME. It can be carried out by using a roll pressing device for transferring the catalyst layer having the above. Other members of the roll pressing device for transferring the catalyst layer, such as a heating device, a pressurizing device, and a driving means, are not shown.

How the transfer process is executed will be described. The electrolyte membrane ME is wound around the electrolyte membrane unwinding roll 10. The electrolyte membrane ME wound around the electrolyte membrane unwinding roll 10 is unwound from the electrolyte membrane unwinding roll 10 by the first electrolyte membrane unwinding roll 11. Then, on both sides of the unwound electrolyte membrane ME, the anode sheet AS and the cathode sheet third delivery roll 33 delivered from the anode sheet third delivery roll 23.
The cathode sheet CS sent out from is laminated by the pair of laminating rolls 40.

The electrolyte membrane ME may be a commercially available product or may be manufactured in advance by a known method such as an extrusion method or a casting method. As a commercially available product, a Nafion film under the trade name of DuPont and a Gore Select film under the trade name of Japan Gore-Tech can be used. The electrolyte membrane ME used had a thickness of approximately 30 to 50 μm.

The electrolyte membrane ME, the anode sheet AS having the anode catalyst layer AN carried on the surface thereof, and the cathode sheet CS having the cathode catalyst layer CT carried on the surface thereof are laminated by the pair of laminating rolls 40. A pair of heating / pressurizing rolls 50 of the roll pressing device for transferring the catalyst layer,
The anode catalyst layer AN and the cathode catalyst layer CT are transferred to the electrolyte membrane ME by being heated and pressed by 51. In this case, one of the pair of heating / pressurizing rolls is the heating / pressurizing roll 50 with a transfer part having the transferring part 50a, and the other is the heating / pressurizing roll 51 with an elastic body covering part having a covering part 51a whose surface is made of an elastic body. The anode catalyst layer AN and the cathode catalyst layer CT are transferred to the electrolyte membrane ME in a shape corresponding to the shape of the transfer portion 50a.

In this case, the pair of heating and pressing rolls 50, 5
The temperature of 1 can be set to a temperature suitable for the material of the electrolyte membrane ME, the catalyst layer and the like by using a heater (not shown) such as a heater and an oil temperature adjusting device. In this case, the softening temperature usually differs depending on the type of the electrolyte membrane ME, and the electrolyte membrane ME is softened and bonded at a temperature near the glass transition temperature of the electrolyte membrane ME. The temperature may be approximately 80 to 130 ° C. Also, a pair of heating and pressing rolls 50,
The pressure applied between 51 can be set to about 1 to 10 MPa, preferably about 2 to 5 MPa, using a pressure device (not shown) such as an air cylinder.

The feeding speed of the pair of heating / pressurizing rolls 50, 51 can be set to about 0.5 to 10 m / min by using a driving means (not shown) such as a motor, and preferably about 1 to 10 m / min. It can be 5 m / min.

In FIG. 12, there is shown a pair of heating / pressurizing rolls 50 and 51 which can be used in the roll pressing device for transferring the catalyst layer of the first invention, one of which is the heating / pressurizing roll 50 with a transfer portion. The heating / pressurizing roll 51 with an elastic body coating portion, which has a coating portion made of an elastic body on the other side, is illustrated. That is, one heating / pressurizing roll is the heating / pressurizing roll 50 with the transfer portion, and the transfer portion is elastically displaced by the pressing force acting on the transfer portion, so that an excessive pressing force is locally applied to the transfer portion. It is a heating / pressurizing roll having preventive means (not particularly shown) for preventing it from acting.

In this case, the preventive means is, as described above,
Whether it is an elastic body coated as the surface layer of the transfer section, a spring interposed between the main body of the heating / pressurizing roll and the transfer section, an elastic body, or an air cylinder. Good.

In FIG. 12, a pair of heating / pressurizing rolls used in the roll pressing apparatus for transferring the catalyst layer of the first invention is shown, but a pair of heating / pressing rolls in the roller pressing apparatus for transferring the catalyst layer used in this transfer step are shown. The pressure rolls are not limited to the pair of heating and pressure rolls used in the catalyst layer transfer roll pressing device of the first invention. It is also possible to use a pair of heating and pressing rolls used in the catalyst layer transfer roll pressing device of the second invention.

Peeling Step In the peeling step, the anode sheet AS is peeled off from the anode catalyst layer AN transferred to the electrolyte membrane ME to remove the electrolyte membrane ME.
Anode sheet peeling device 26 and a cathode sheet peeling device 36 for peeling the cathode sheet CS from the cathode catalyst layer CT transferred to the anode, and an anode for winding the anode sheet AS from which the transferred anode catalyst layer AN is peeled The sheet take-up roll 24, the cathode sheet take-up roll 34 that winds up the cathode sheet CS from which the transferred cathode catalyst layer CT has been peeled off, the electrolyte membrane ME
A conjugate body winding roll 13 for winding up the catalyst layer-electrolyte membrane assembly MEA formed by transferring the anode catalyst medium layer AN and the cathode catalyst layer CT onto the joint body winding roll 13, and a catalyst layer-electrolyte membrane assembly body on the conjugate body winding roll 13. This can be performed using the bonded body delivery roll 12 or the like that delivers the MEA.
Pressing plates were used as the sheet peeling devices 26 and 36.

The manner in which the peeling process is executed will be described below. In the transfer step, a pair of heating and pressing rolls 50, 5
1 is used to transfer the anode catalyst layer AN and the cathode catalyst layer CT to both sides of the electrolyte membrane ME in the shape of the transfer portion.
Then, the anode sheet CS and the cathode sheet AS, which are laminated on both sides of the electrolyte membrane ME to which the anode catalyst layer AN and the cathode catalyst layer CT have been transferred, are attached to the anode sheet stripping device 26 and the cathode sheet stripping device 36.
By peeling off the catalyst layer-electrolyte membrane assembly M
EA is formed.

In this case, the transfer membrane 50a has the shape of the electrolyte membrane M.
The anode catalyst layer AN and the cathode catalyst layer CT transferred to E are separated from the anode sheet AS and the cathode sheet CS, respectively, and left on the electrolyte membrane ME side,
A catalyst layer-electrolyte membrane assembly MEA is formed. Further, the anode catalyst layer AN and the cathode catalyst layer CT that have not been transferred to the electrolyte membrane ME are left in a state of being carried on the surfaces of the anode sheet AS and the cathode sheet CS.

The catalyst layer-electrolyte membrane assembly MEA comprises
It is sent out by the joined body feeding roll 12 and wound up by the joined body winding roll 13. The anode sheet AS and the cathode sheet CS are wound around the anode sheet winding roll 24 and the cathode sheet winding roll 34.

In this way, the catalyst layer A is formed on the electrolyte membrane ME.
A catalyst layer-electrolyte membrane assembly MEA in which N and CT are transferred can be manufactured.

(6) The step of producing a catalyst layer-electrolyte membrane assembly which can use the catalyst layer transfer roll pressing apparatus of the present invention is not limited to the step described in (5).

For example, the transfer of the anode catalyst layer and the cathode catalyst layer to the electrolyte membrane is performed at the same time in the above example, but can be performed in separate steps. In this case, the transfer process will be performed twice.

Also, the above-mentioned catalyst layer-electrolyte membrane assembly ME
In the step of producing A, the anode catalyst layer AN formed on the surface of the anode sheet AS and the cathode catalyst layer CT formed on the surface of the cathode sheet CS are coated in the drying step before the transfer step. It is common to dry the catalyst layer mixture to remove the solvent in the catalyst layer mixture. Therefore, in the transfer process, the anode catalyst layer AN and the cathode catalyst layer CT are transferred to the electrolyte membrane ME in a dry state. Then, after the anode sheet and the cathode sheet are peeled in the peeling step, the catalyst layer-electrolyte membrane joined body MEA is wound around the joined body winding roll 13 as it is.

However, when the catalyst layer-electrolyte membrane assembly MEA is formed in this manner, the following problems occur. That is, since the anode catalyst layer AN and the cathode catalyst layer CT are transferred to the electrolyte membrane by heating and pressing in a completely dried state, the adhesion between the anode catalyst layer AN and the cathode catalyst layer CT and the electrolyte membrane ME is insufficient. In addition, the anode catalyst layer AN and the cathode catalyst layer CT are plastically deformed and crushed by heating and pressurization, the three-dimensional structure is destroyed, the gas diffusibility is obstructed, and the catalytic reaction activity is lowered.

Therefore, in the drying step, the solvent in the catalyst mixture is not completely removed, but in a so-called pre-dried state, the anode catalyst layer AN and the cathode catalyst layer C are
T can be transferred to the electrolyte membrane.

In this case, the solvent used for the catalyst mixture carried on the anode sheet AS and the cathode sheet CS has a boiling point higher than that of water as a solvent for dispersing the catalyst-supporting powder such as carbon powder carrying the catalytic metal. Moreover, a high boiling point solvent such as propylene glycol, ethylene glycol, or propanol, which has good compatibility with the electrolyte resin such as perfluorosulfonic acid resin, can be used.

The catalyst mixture having such a constitution is applied to an anode sheet and a cathode sheet to form catalyst layers AN and CT.
To form the electrolyte membrane M in a state where the solvent remains.
The catalyst layers AN and CT can be transferred to E.

In the drying step described in this case, in order to partially leave the solvent, the preliminary drying step of the catalyst layers AN and CT is preferably steam drying rather than normal warm air drying. In this case, the temperature is lower than the temperature of the drying step described in (5), and can be approximately 80 to 130 ° C. By doing so, heat generation of the anode and cathode catalyst layers AN and CT and dry-up of the electrolyte membrane ME can be prevented.

In this way, the anode and cathode catalyst layers AN and CT can be transferred to the electrolyte membrane ME in a state in which the high boiling point solvent is partially left. In this case, since the transfer is performed in a state where the high boiling point solvent is partially left, the pressure applied between the pair of heating / pressurizing rolls 50 and 51 can be set to a lower pressure than usual to perform the transfer. For example, the pressure can be set to about 1 to 5 MPa.
Further, the temperature of the pair of heating / pressurizing rolls 50 and 51 can be set to a temperature lower than usual to transfer the image. For example 60
The temperature can be set to about 120 ° C.

[0133] In this manner, the solvent is partially left under heat and pressure to apply the anode and cathode catalyst layers AN to the electrolyte membrane,
Since CT is transferred, the adhesion between the electrolyte membrane ME and the anode and cathode catalyst layers AN and CT can be improved, and the porosity of the anode and cathode catalyst layers AN and CT can be secured.

Further, when the anode and cathode catalyst layers AN and CT are transferred to the electrolyte membrane ME with a part of the high-boiling point solvent remaining, the solvent in the catalyst layer is completely removed in the stripping step. A drying step can be provided. That is, the anode sheet AS and the cathode sheet C
After the S is separated from the anode catalyst layer AN and the cathode catalyst layer CT transferred to the electrolyte membrane ME to form the catalyst layer-electrolyte membrane assembly MEA, the main drying step is performed to provide the anode and cathode catalyst layers AN, The high boiling point solvent remaining in the CT can be removed by drying. In this case, the temperature of this main drying step is preferably about 100 to 150 ° C.

Since the high boiling point solvent is dried and removed after transferring the anode and cathode catalyst layers to the electrolyte membrane in this manner, the porosity and three-dimensional structure of the anode and cathode catalyst layers can be secured.

As described above, by using the roll pressing device for transferring the catalyst layer of the present invention, the catalyst layer adapted to the shape of the transfer portion can be continuously transferred to the electrolyte membrane without damaging the electrolyte membrane. You can

[Brief description of drawings]

FIG. 1 is a diagram showing how a catalyst layer is transferred onto an electrolyte membrane by using a pair of heating and pressing rolls.

FIG. 2 is a diagram showing a catalyst layer-electrolyte membrane assembly in which the area of a solid polymer electrolyte membrane is wider than the area of a catalyst layer.

FIG. 3 is a view showing a heating / pressurizing roll with a transfer portion.

FIG. 4 is a diagram showing a state in which a catalyst layer is transferred to a solid polymer electrolyte membrane by using a heating / pressurizing roll with a transfer part and a heating / pressurizing roll having no transfer part.

FIG. 5 is a diagram showing how the catalyst layer, the catalyst layer-supporting base material, the solid polymer electrolyte membrane, and the like are distorted in the concave portion of the heating and pressing roll.

FIG. 6 is a pair of heating / pressurizing rolls including a heating / pressurizing roll with a transferring part and an ordinary heating / pressurizing roll having an elastic body coated on the surface of a convex base of the transferring part as a surface layer of the transferring part. It is the figure shown.

FIG. 7 is a view showing a heating / pressurizing roll with a transfer part, which has a roll-shaped main body part, a convex-shaped transfer part, and an elastic body interposed therebetween.

FIG. 8 is a diagram showing a heating / pressurizing roll having a roll-shaped main body portion, a convex-shaped transfer portion, and a spring interposed therebetween.

FIG. 9 is a partial cross-sectional view of a heating / pressurizing roll with a transfer unit in which a transfer unit and a main body unit are joined with a spring interposed.

FIG. 10 is a view showing a roll with an elastic body covering portion having a roll-shaped main body portion and a covering portion made of an elastic body and covering the outer peripheral surface of the main body portion.

FIG. 11 includes a roll-shaped main body portion and a convex-shaped transfer portion formed on the outer peripheral surface of the main body portion, and includes a transfer portion of one heating / pressurizing roll and a transfer portion of the other heating / pressurizing roll. FIG. 4 is a diagram showing a pair of heating and pressing rolls that are plane-symmetric with respect to the electrolyte membrane sandwiched by the pair of heating and pressing rolls as a plane of symmetry.

FIG. 12 is a diagram schematically showing an outline of a step of producing a catalyst layer-electrolyte membrane assembly.

[Explanation of symbols]

100: Heat and pressure roll with transfer part 100a: Convex transfer part 100aa: surface layer 100ab: convex base 100b: Roll-shaped main body 100c: Elastic body 100d: spring 100f: Insertion pin 100 g: disk-shaped plate 100h: insertion hole 100i: bolt 101: Normal heating / pressurizing roll 102: Heating / pressurizing roll with elastic body coating 110: Heat and pressure roll with transfer part 110a: Convex transfer part 110b: Roll-shaped main body 110e: concave portion 111: Heat and pressure roll with transfer part 111a: convex transfer part 111b: Roll-shaped main body 111e: concave portion AN: Anode catalyst layer AS: Anode sheet CT: cathode catalyst layer CS: Cathode sheet ME: Electrolyte membrane MEA: Catalyst layer-electrolyte membrane assembly 10: roll for unwinding electrolyte membrane 11: Electrolyte membrane first delivery roll 12: Bonded body feeding roll 13: Bonded body winding roll 20: Sheet unwinding roll for anode 21: Anode sheet first delivery roll 22: Anode sheet second feed roll 23: Anode sheet third feed roll 24: Sheet winding roll for anode 25: Anode catalyst layer coating device 26: Anode sheet peeling device 30: Sheet unwinding roll for cathode 31: First delivery roll for cathode sheet 32: Second delivery roll for cathode sheet 33: Third delivery roll for cathode sheet 34: Sheet winding roll for cathode 35: Cathode catalyst layer coating device 36: Cathode sheet stripping device 40: a pair of laminating rolls 50: Heating / pressurizing roll with transfer part 50a: Transfer part 51: Heating / pressurizing roll with elastic coating 51a: Cover

Claims (12)

[Claims] 1. A pair of heating for transferring the catalyst layer to the surface of the solid polymer electrolyte membrane by sandwiching the solid polymer electrolyte membrane of the fuel cell and the catalyst layer-supporting substrate having the catalyst layer formed on the surface thereof. At least one of the pair of heating / pressurizing rolls has a pressing roll, and at least one of the pair of heating / pressurizing rolls has a transfer part and has a transfer part having a convex transfer part formed on the outer peripheral surface of the main part. In the roll pressing device for transferring the catalyst layer, the heating / pressurizing roll with the transfer portion is locally excessive in the transfer portion due to elastic displacement of the transfer portion due to the pressing force applied to the transfer portion. A roll pressing device for transferring a catalyst layer, comprising a preventing means for preventing a pressing force from acting. 2. The catalyst layer transfer device according to claim 1, wherein the prevention unit is an elastic body interposed between the main body section and the transfer section. 3. The roll pressing device for transferring a catalyst layer according to claim 2, wherein the elastic body is rubber. 4. The roll pressing device for transferring a catalyst layer according to claim 1, wherein the preventing unit is a spring interposed between the main body and the transfer unit. 5. The roll press apparatus for transferring a catalyst layer according to claim 1, wherein the preventing unit is an air cylinder interposed between the main body and the transfer unit. 6. The roll pressing device for transferring a catalyst layer according to claim 2, wherein an end of the transfer portion has a tapered surface or an R shape. 7. The heating / pressurizing roll, which is the counterpart of the heating / pressurizing roll with a transfer portion, has a roll-shaped main body and a cover made of an elastic body covering the outer peripheral surface of the main body. 6. A roll press device for transferring a catalyst layer according to any one of 6 to 6. 8. The roll pressing apparatus for catalyst transfer according to claim 7, wherein the elastic body is rubber. 9. The transfer section has a convex base formed on the outer peripheral surface of the main body, and a surface layer made of an elastic body that covers the surface of the base, and the preventing means includes the surface layer. The roll pressing apparatus for transferring a catalyst layer according to claim 1, wherein the elastic body is covered with the elastic material. 10. The roll pressing device for transferring a catalyst layer according to claim 9, wherein the elastic body is rubber. 11. A pair of heatings for pressing a solid polymer electrolyte membrane of a fuel cell and a catalyst layer-supporting substrate having a catalyst layer formed on the surface thereof to transfer the catalyst layer to the surface of the solid polymer electrolyte membrane. In a catalyst layer transfer roll press device having a pressure roll, the pair of heating and pressure rolls each have a roll-shaped main body portion and a convex transfer portion formed on an outer peripheral surface of the main body portion. The transfer portion of the heating / pressurizing roll and the transfer portion of the other heating / pressurizing roll are plane-symmetrical with the solid polymer electrolyte membrane sandwiched by the pair of heating / pressurizing rolls as a plane of symmetry. A roll press device for transferring a catalyst layer. 12. The end portion of the transfer portion has a tapered surface or R
The roll press device for transferring a catalyst layer according to claim 11, which is shaped.