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JP5005214B2 - Fuel cell manufacturing method and fuel cell manufacturing apparatus - Google Patents

Fuel cell manufacturing method and fuel cell manufacturing apparatus Download PDF

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JP5005214B2
JP5005214B2 JP2005364299A JP2005364299A JP5005214B2 JP 5005214 B2 JP5005214 B2 JP 5005214B2 JP 2005364299 A JP2005364299 A JP 2005364299A JP 2005364299 A JP2005364299 A JP 2005364299A JP 5005214 B2 JP5005214 B2 JP 5005214B2
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catalyst layer
electrolyte membrane
film
fuel cell
masking
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JP2007172844A (en
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勇 菊池
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Toshiba Energy Systems and Solutions Corp
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Toshiba Fuel Cell Power Systems Corp
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    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30Hydrogen technology
    • Y02E60/50Fuel cells
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50Manufacturing or production processes characterised by the final manufactured product

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Description

この発明は、燃料電池の製造方法およびその製造装置に関し、特に、電解質膜の両面に電極の触媒層を接合させた電解質膜・触媒層接合体を製造するための方法およびそのための装置に関する。   The present invention relates to a fuel cell manufacturing method and a manufacturing apparatus therefor, and more particularly, to a method for manufacturing an electrolyte membrane / catalyst layer assembly in which an electrode catalyst layer is bonded to both surfaces of an electrolyte membrane and an apparatus therefor.

燃料電池では、電解質層の両面に触媒層を配置し、そこに燃料と酸化剤を供給して電気化学反応により発電する。たとえば、一般的な固体高分子型燃料電池では、イオン交換膜で形成された電解質膜の両面に白金あるいは白金化合物等からなる触媒層と多孔質カーボンペーパー等よりなる電極基材を接合あるいは密着して配置し、さらにその両側にガス供給用の通路を備えた構造をしている。   In a fuel cell, a catalyst layer is disposed on both surfaces of an electrolyte layer, and fuel and an oxidant are supplied to the catalyst layer to generate electricity by an electrochemical reaction. For example, in a general polymer electrolyte fuel cell, a catalyst layer made of platinum or a platinum compound and an electrode base material made of porous carbon paper or the like are bonded or adhered to both surfaces of an electrolyte membrane formed of an ion exchange membrane. Furthermore, it has a structure provided with gas supply passages on both sides thereof.

また、典型的な燃料電池の電解質膜と触媒層の接合体では電解質膜の両面に接合された触媒層の間を電気的に絶縁状態に保つために電解質膜に触媒層を接合した範囲の周辺に触媒層が転写されていない電解質膜の範囲が設けられている。   In addition, in a typical fuel cell electrolyte membrane and catalyst layer assembly, in order to maintain an electrically insulating state between the catalyst layers joined to both surfaces of the electrolyte membrane, the periphery of the range where the catalyst layer is joined to the electrolyte membrane. A range of the electrolyte membrane to which the catalyst layer is not transferred is provided.

ここで、電解質膜と触媒層の接合体を製造する方法として、基材上に触媒層を形成した転写シートから触媒層を電解質膜に転写する方法が知られている(たとえば、特許文献1参照)。また、電解質膜に接合される触媒層の面積を電解質膜の面積より小さくする方法としては、予め基材上に電解質膜より面積の小さい触媒層を形成した後に電解質膜に接合する方法、もしくは予め触媒層を電解質膜より小さく切断した後に電解質膜に接合する方法が知られている(たとえば、特許文献2、3、4参照)。
特開平10−64574号公報 特開2004−165073号公報 特公平3−295171号公報 特開2004−214001号公報
Here, as a method for producing a joined body of an electrolyte membrane and a catalyst layer, a method of transferring the catalyst layer to the electrolyte membrane from a transfer sheet in which the catalyst layer is formed on a base material is known (for example, see Patent Document 1). ). In addition, as a method of making the area of the catalyst layer bonded to the electrolyte membrane smaller than the area of the electrolyte membrane, a method of previously forming a catalyst layer having a smaller area than the electrolyte membrane on the substrate and then bonding to the electrolyte membrane, A method is known in which a catalyst layer is cut smaller than the electrolyte membrane and then joined to the electrolyte membrane (see, for example, Patent Documents 2, 3, and 4).
Japanese Patent Laid-Open No. 10-64574 JP 2004-165073 A Japanese Patent Publication No. 3-295171 Japanese Patent Laid-Open No. 2004-214001

特許文献2による方法では、基材上に触媒層を形成する前に予め触媒の一部を基材上から除去する工程が必要であるという課題があった。また、特許文献2、3、4のいずれの方法でも、触媒層を電解質膜に転写するときに、電解質膜の両面に転写される触媒層の位置ずれを小さくすることが困難であるという課題があった。すなわち、特許文献2による方法では、基材上の触媒層の位置が精度良く形成されていないと接合後の触媒層の位置がずれてしまう。   The method according to Patent Document 2 has a problem that a step of removing a part of the catalyst from the substrate in advance is necessary before forming the catalyst layer on the substrate. Further, in any of the methods of Patent Documents 2, 3, and 4, when transferring the catalyst layer to the electrolyte membrane, there is a problem that it is difficult to reduce the displacement of the catalyst layer transferred to both surfaces of the electrolyte membrane. there were. That is, in the method according to Patent Document 2, if the position of the catalyst layer on the base material is not formed with high accuracy, the position of the catalyst layer after bonding is shifted.

また、特許文献4による方法は、触媒層の外周に沿う形の弾性材の枠を使用して触媒層転写範囲以外の部分を押えつつ、枠内に設置した触媒層を加圧する方法であるが、弾性材の枠と触媒層の外周には僅かな隙間を設ける必要があり、この隙間寸法の範囲内において電解質膜の両面に転写された触媒層の位置がずれる可能性があるとともに、触媒層を含む部材はその厚みが薄いため、容易に弾性材の枠と電解質膜の間に入り込み、位置がずれた状態で接合される場合が生じる。   The method according to Patent Document 4 is a method of pressurizing the catalyst layer installed in the frame while pressing a portion other than the catalyst layer transfer range using a frame of an elastic material along the outer periphery of the catalyst layer. In addition, it is necessary to provide a slight gap between the elastic material frame and the outer periphery of the catalyst layer, and the position of the catalyst layer transferred to both surfaces of the electrolyte membrane may be shifted within the gap dimension, and the catalyst layer Since the member containing is thin, the member easily enters between the frame of the elastic material and the electrolyte membrane, and may be joined in a shifted state.

本発明は、上記のような従来技術の課題を解決するものであって、その目的は、触媒層の位置ずれが少なく、電解質膜よりも面積の小さい触媒層を有する電解質膜・触媒層接合体を容易に製造するための燃料電池製造方法および燃料電池製造装置を提供することにある。   The present invention solves the above-mentioned problems of the prior art, and an object of the present invention is to provide an electrolyte membrane / catalyst layer assembly having a catalyst layer having a smaller area than the electrolyte membrane with little displacement of the catalyst layer. The present invention provides a fuel cell manufacturing method and a fuel cell manufacturing apparatus for easily manufacturing a fuel cell.

上記の目的を達成するため、本発明に係る燃料電池製造方法は、電解質膜の両面に電極の触媒層を接合させた電解質膜・触媒層接合体を有する燃料電池の製造方法において、前記触媒層がフィルム状の基材の片面に形成された触媒層付きフィルムを2枚用意し、前記電解質膜の両面それぞれに、前記触媒層付きフィルムの触媒層よりも小さな寸法の開口部を有するマスキングシートを配置し、これらのマスキングシートをはさみ込むように、前記触媒層付きフィルムを、その触媒層がマスキングシートを向くように配置し、さらに、前記触媒層付きフィルムの外側を、弾性部材を介して互いに押し付けるとともに加熱して、前記マスキングシートの開口部のみで前記触媒層と前記電解質膜とを接合した電解質膜・マスキングシート・触媒層付きフィルム接合体を形成し、前記電解質膜・マスキングシート・触媒層付きフィルム接合体から前記触媒層付きフィルムの基材を剥離し、前記マスキングシートを取り外して前記電解質膜・触媒層接合体を形成する工程を含前記電解質膜の両面に配置された前記マスキングシートの開口部の形状が互いに異なることを特徴とする。 In order to achieve the above object, a method for producing a fuel cell according to the present invention includes a method for producing a fuel cell having an electrolyte membrane / catalyst layer assembly in which electrode catalyst layers are joined to both surfaces of an electrolyte membrane. Prepared two sheets with a catalyst layer formed on one side of a film-like substrate, and a masking sheet having openings smaller in size than the catalyst layer of the film with the catalyst layer on each side of the electrolyte membrane. The film with the catalyst layer is arranged so that the masking sheet is sandwiched between the film with the catalyst layer so that the catalyst layer faces the masking sheet. With an electrolyte membrane, masking sheet, and catalyst layer that is pressed and heated to join the catalyst layer and the electrolyte membrane only at the opening of the masking sheet A film assembly is formed, the base material of the film with the catalyst layer is peeled off from the membrane assembly with the electrolyte membrane / masking sheet / catalyst layer, and the masking sheet is removed to form the electrolyte membrane / catalyst layer assembly. step only contains, the shape of the opening of the masking sheet disposed on both surfaces of the electrolyte membrane is different from each other.

また、本発明に係る燃料電池製造装置は、電解質膜の両面に電極の触媒層を接合させた電解質膜・触媒層接合体を有する燃料電池の製造装置において、開口部を有する2枚のマスキングシートで電解質膜を挟み込み、さらに、前記開口部よりも大きな触媒層がフィルム状の基材の表面に形成された触媒層付きフィルム2枚をその触媒層が内側を向くように配置して前記マスキングシートを前記触媒層付きフィルムで挟み込む重ね合わせ手段と、前記重ね合わせ手段で重ね合わされた2枚の触媒層付きフィルムの外側から弾性部材を介して加圧するとともに加熱して、前記マスキングシートの開口部のみで前記触媒層と前記電解質膜とを接合した電解質膜・マスキングシート・触媒層付きフィルム接合体を形成する加圧加熱手段と、前記電解質膜・マスキングシート・触媒層付きフィルム接合体から前記触媒層付きフィルムの基材を剥離し、前記マスキングシートを取り外して前記電解質膜・触媒層接合体を形成する剥離取り外し手段と、を有し、前記電解質膜の両面に配置された前記マスキングシートの開口部の形状が互いに異なること、を特徴とする。 The fuel cell manufacturing apparatus according to the present invention includes two masking sheets having openings in a fuel cell manufacturing apparatus having an electrolyte membrane / catalyst layer assembly in which an electrode catalyst layer is bonded to both surfaces of an electrolyte membrane. Further, the masking sheet is formed by sandwiching two electrolyte membranes with a catalyst layer larger than the opening formed on the surface of the film-like base material so that the catalyst layer faces inward. Means for sandwiching the film with the film with the catalyst layer, and pressurizing and heating from the outside of the two films with the catalyst layer superimposed by the superposition means through an elastic member, so that only the opening of the masking sheet A pressure heating means for forming an electrolyte membrane, a masking sheet, and a catalyst layer-attached film assembly obtained by joining the catalyst layer and the electrolyte membrane, and the electrolyte - wherein the masking sheet with catalyst layers film assembly was peeled off the base material of the catalyst layer with a film, have a, a peeling removal means for forming the membrane-catalyst layer assembly by removing the masking sheet, the The opening portions of the masking sheets disposed on both surfaces of the electrolyte membrane are different from each other .

本発明によれば、予め触媒の一部を基材上から除去した形状の触媒層付きフィルムを形成したり、接合の際に予め所定の形状に切断された触媒層を電解質膜の中央付近に位置合わせして設置するような手間をかけることなしに、電解質膜の両面に設置したマスキングシートの位置合わせを行なうことによって、触媒層の位置ずれの問題がなく、電解質膜よりも面積の小さい触媒層を有する電解質膜・触媒層接合体を容易に製造することができる。   According to the present invention, a film with a catalyst layer having a shape in which a part of the catalyst is previously removed from the substrate is formed, or the catalyst layer that has been cut into a predetermined shape at the time of bonding is placed near the center of the electrolyte membrane. By aligning the masking sheets installed on both sides of the electrolyte membrane without the trouble of positioning and installing, there is no problem of displacement of the catalyst layer, and the catalyst has a smaller area than the electrolyte membrane. An electrolyte membrane / catalyst layer assembly having a layer can be easily produced.

以下、本発明の実施の形態を、図面を参照して説明する。ここで、相互に同一または類似の構成部分には共通の符号を付し、重複する説明は省略する。   Hereinafter, embodiments of the present invention will be described with reference to the drawings. Here, the same or similar components are denoted by common reference numerals, and redundant description is omitted.

[第1の実施形態]
本発明に係る燃料電池の製造方法および製造装置の第1の実施形態を、図1、図2を用いて説明する。図1は、本発明に係る燃料電池の製造方法の第1の実施形態における電解質膜・触媒層接合体の製造過程を示す模式的展開斜視図である。また図2は、図1の電解質膜・触媒層接合体の完成状態を示す横断面図である。
[First Embodiment]
A fuel cell manufacturing method and manufacturing apparatus according to a first embodiment of the present invention will be described with reference to FIGS. FIG. 1 is a schematic exploded perspective view showing a manufacturing process of an electrolyte membrane / catalyst layer assembly in a first embodiment of a fuel cell manufacturing method according to the present invention. FIG. 2 is a cross-sectional view showing a completed state of the electrolyte membrane / catalyst layer assembly of FIG.

図1に示すように、第1の治具1は、水平に配置された長方形の板状部材1aを有し、この板状部材1aの上面に位置決め治具10が突設されている。位置決め治具10は、たとえば、板状部材1aに固定された円柱状の部材であって、板状部材1aの互いに隣接する2辺の外周近くにそれぞれ2個が配置されている。   As shown in FIG. 1, the 1st jig | tool 1 has the rectangular plate-shaped member 1a arrange | positioned horizontally, and the positioning jig 10 protrudes from the upper surface of this plate-shaped member 1a. For example, the positioning jig 10 is a columnar member fixed to the plate-like member 1a, and two pieces are arranged near the outer periphery of two adjacent sides of the plate-like member 1a.

板状部材1aの上には順に、第1の弾性部材2、第1の触媒付きフィルム3、第1のマスキングシート4、電解質膜5、第2のマスキングシート6、第2の触媒付きフィルム7、第2の弾性部材8、第2の治具9が積層される。この積層に当っては、積層されるそれぞれのものの辺を位置決め治具10に当接させることによって位置合わせをすることができる。   On the plate-like member 1a, the first elastic member 2, the first catalyst-attached film 3, the first masking sheet 4, the electrolyte membrane 5, the second masking sheet 6, and the second catalyst-attached film 7 are sequentially provided. The second elastic member 8 and the second jig 9 are laminated. In this stacking, alignment can be performed by bringing the side of each stacked layer into contact with the positioning jig 10.

第1、第2の触媒付きフィルム3、7は、それぞれ、たとえばポリエチレンテレフタレートからなる基材3a、7aの片面に触媒層3b、7bをあらかじめ形成したものであり、触媒層3b、7bがそれぞれ電解質膜5に面する向きに積層されている。また、第1、第2のマスキングシート4、6には、それぞれ、作成する電解質膜・触媒層接合体における触媒層の形状に相当する形状の開口部4a、6aが設けられている。   Each of the first and second films 3 and 7 with a catalyst is formed by previously forming catalyst layers 3b and 7b on one side of a base material 3a or 7a made of, for example, polyethylene terephthalate, and each of the catalyst layers 3b and 7b is an electrolyte. They are stacked in a direction facing the film 5. The first and second masking sheets 4 and 6 are provided with openings 4a and 6a having shapes corresponding to the shapes of the catalyst layers in the electrolyte membrane / catalyst layer assembly to be created, respectively.

次に、電解質膜・触媒層接合体の製造方法について説明する。触媒層は、図1の積層体を図示されない熱間プレスによって、温度80℃〜200℃、圧力0.5〜20MPaにて加熱および加圧することにより、触媒層3b、7bが電解質膜5に転写される。その後、図1の積層体から、第1、第2の触媒付きフィルム3、7、第1、第2のマスキングシート4、6、および電解質膜5からなる積層部分を取り出し、電解質膜・触媒層接合体から第1、第2の触媒付きフィルム3、7の基材3a、7aを剥離し、さらに第1、第2のマスキングシート4、6を電解質膜5から取り外すことで電解質膜・触媒層接合体が得られる。   Next, a method for producing an electrolyte membrane / catalyst layer assembly will be described. The catalyst layers are transferred to the electrolyte membrane 5 by heating and pressurizing the laminated body of FIG. 1 at a temperature of 80 ° C. to 200 ° C. and a pressure of 0.5 to 20 MPa by hot pressing (not shown). Is done. Then, the laminated part which consists of the 1st, 2nd films 3 and 7, with a catalyst, the 1st and 2nd masking sheets 4 and 6, and the electrolyte membrane 5 is taken out from the laminated body of FIG. The base films 3a and 7a of the first and second catalyst-attached films 3 and 7 are peeled from the joined body, and the first and second masking sheets 4 and 6 are further removed from the electrolyte film 5 to thereby provide an electrolyte membrane / catalyst layer. A joined body is obtained.

図2は、本実施形態によって得られた電解質膜・触媒層接合体の立断面図である。ここで、第1、第2のマスキングシート4、6を介して電解質膜5に面していた触媒層の範囲では、触媒層が電解質膜5に転写されていないため、接合された触媒層3c、7cは電解質膜5よりも面積が小さく、周辺に触媒層を有しない電解質膜の範囲5aが得られる。また、第1、2のマスキングシート4、6をフッ素樹脂もしくは表面にフッ素樹脂層を有する材料とすることにより、電解質膜5とマスキングシート4、6の剥離が容易に行なえるとともに、マスキングシート4、6の表面に電解質層が転写されることがなくなり、マスキングシート4、6を繰り返して製造に使用することが可能となる。フッ素樹脂としては、たとえばテフロン(商標)が適している。   FIG. 2 is an elevational sectional view of the electrolyte membrane / catalyst layer assembly obtained by the present embodiment. Here, in the range of the catalyst layer facing the electrolyte membrane 5 through the first and second masking sheets 4 and 6, the catalyst layer is not transferred to the electrolyte membrane 5, and therefore the joined catalyst layer 3c. 7c has an area smaller than that of the electrolyte membrane 5, and an electrolyte membrane range 5a having no catalyst layer in the periphery is obtained. Further, by using the first and second masking sheets 4 and 6 as a fluororesin or a material having a fluororesin layer on the surface, the electrolyte membrane 5 and the masking sheets 4 and 6 can be easily separated, and the masking sheet 4 The electrolyte layer is not transferred to the surface of 6 and 6, and the masking sheets 4 and 6 can be repeatedly used for production. For example, Teflon (trademark) is suitable as the fluororesin.

第1、第2の弾性部材2、8は、図1に示すように部材を積層したときに第1、2のマスキングシート4、6の開口部4a、6aに相対する部分の厚さを、第1、2のマスキングシート4、6の開口部以外の部分4b、6bに相対する部分の厚さより厚くすることによって、第1、2のマスキングシート4、6の有無による積層方向の厚さの段差が吸収され、全面に均一な面圧を負荷することができる。しかし、厚さ方向に段差のない形状とすれば、マスキングシート4、6に対して精細な位置合わせが不要となるので、下記のとおり、マスキングシート4、6の厚さに対して弾性部材が十分な厚さを持ち、厚さ方向に段差を有しない形状とすること望ましい。   As shown in FIG. 1, the first and second elastic members 2 and 8 have thicknesses of portions corresponding to the openings 4a and 6a of the first and second masking sheets 4 and 6 when the members are laminated, as shown in FIG. By making it thicker than the thickness of the portions facing the portions 4b, 6b other than the openings of the first and second masking sheets 4, 6, the thickness in the stacking direction depending on the presence or absence of the first, second masking sheets 4, 6 The step is absorbed, and a uniform surface pressure can be applied to the entire surface. However, if the shape has no step in the thickness direction, fine positioning with respect to the masking sheets 4 and 6 becomes unnecessary. It is desirable to have a shape with sufficient thickness and no step in the thickness direction.

すなわち、片側のマスキングシート4(6)の厚さをt1、そのマスキングシート4(6)に近い片側の弾性部材2(8)の厚さと縦弾性係数をそれぞれt2、E、触媒層3b、7bを電解質膜5に転写させるための面圧をP1とすると、加熱プレス中にマスキングシート4、6に面する電解質膜5の範囲に負荷される面圧P2は、マスキングシート4、6と電解質膜5および触媒層付きフィルム3、7の面圧による厚さ方向の圧縮変形を無視すると、
P2=P1+E*t1/t2 …(1)
と表される。
That is, the thickness of the masking sheet 4 (6) on one side is t1, the thickness and the longitudinal elastic modulus of the elastic member 2 (8) on one side close to the masking sheet 4 (6) are t2, E, and the catalyst layers 3b and 7b, respectively. When the surface pressure for transferring the pressure to the electrolyte membrane 5 is P1, the surface pressure P2 applied to the range of the electrolyte membrane 5 facing the masking sheets 4 and 6 during the heating press is the masking sheets 4 and 6 and the electrolyte membrane. 5 and ignoring compressive deformation in the thickness direction due to the surface pressure of the films 3 and 7 with a catalyst layer,
P2 = P1 + E * t1 / t2 (1)
It is expressed.

ここで、加熱プレス中にマスキングシート4、6に面する電解質膜5の範囲に負荷される面圧P2の最大許容値をPmaxとすると、P2<Pmaxであればよいので、(1)式より、
Pmax>P2=P1+E*t1/t2 …(2)
となり、(2)式より、次の(3)式が得られる。
Here, if the maximum allowable value of the surface pressure P2 applied to the range of the electrolyte membrane 5 facing the masking sheets 4 and 6 during the heating press is Pmax, P2 <Pmax may be satisfied. ,
Pmax> P2 = P1 + E * t1 / t2 (2)
Thus, the following equation (3) is obtained from the equation (2).

t2 > t1*E/(Pmax−P1) …(3)
したがって、(3)式の範囲内で弾性部材2、8の厚さを決定することによって、弾性部材2、8は厚さ方向に段差を有しない形状とすることが可能になる。
t2> t1 * E / (Pmax−P1) (3)
Therefore, by determining the thickness of the elastic members 2 and 8 within the range of the expression (3), the elastic members 2 and 8 can be formed into a shape having no step in the thickness direction.

たとえば、弾性部材2、8として厚さが一定で、比較的熱伝達率が高く縦弾性係数Eが100MPaの膨張黒鉛シートを使用し、マスキングシート4、6としてポリイミドフィルムの両面にフッ素樹脂をコーティングした厚さt1が0.025mmのシートを使用し、触媒層3b、7bを電解質膜5に転写させるための面圧P1を3MPa、加熱プレス中にマスキングシート4、6に面する電解質膜5の範囲に負荷される面圧P2の最大許容値を4MPaとする。このとき、(3)式より、
t2>t1*E/(Pmax−P1)=0.025*100/(4−3)=2.5
となり、上記の条件においては、弾性部材2、8の厚さt2が2.5mm以上であれば、加熱プレス中にマスキングシート4、6に面する電解質膜5の範囲に負荷される面圧P2がその最大許容値Pmaxを超えない範囲となるため、予め弾性部材2、8に段差等を設ける必要がないといえる。
For example, an expanded graphite sheet having a constant thickness, a relatively high heat transfer coefficient and a longitudinal elastic modulus E of 100 MPa is used as the elastic members 2 and 8, and a fluorine resin is coated on both sides of the polyimide film as the masking sheets 4 and 6. The sheet having a thickness t1 of 0.025 mm is used, the surface pressure P1 for transferring the catalyst layers 3b and 7b to the electrolyte membrane 5 is 3 MPa, and the electrolyte membrane 5 facing the masking sheets 4 and 6 during the heating press. The maximum allowable value of the surface pressure P2 applied to the range is 4 MPa. At this time, from equation (3),
t2> t1 * E / (Pmax−P1) = 0.025 * 100 / (4-3) = 2.5
Under the above conditions, if the thickness t2 of the elastic members 2 and 8 is 2.5 mm or more, the surface pressure P2 applied to the range of the electrolyte membrane 5 facing the masking sheets 4 and 6 during the heating press. Therefore, it can be said that there is no need to provide a step or the like in the elastic members 2 and 8 in advance.

以上説明したように、本実施形態では、予め触媒の一部を基材上から除去した形状の触媒層付きフィルムを形成したり、接合の際に予め所定の形状に切断された触媒層を電解質膜の中央付近に位置合わせして設置するような面倒な作業が不要で、触媒層の位置ずれがなく、電解質膜よりも面積の小さい触媒層を有する電解質膜・触媒層接合体を容易に製造することができる。また、電解質膜・触媒層接合体の接合工程において電解質の全面が加圧されているため、加熱による電解質膜の熱変形が制限され、しわの発生や寸法変化がなく安定した形状の電解質膜・触媒層接合体が得られる。   As described above, in the present embodiment, a catalyst layer-attached film having a shape in which a part of the catalyst has been removed from the substrate in advance is formed, or the catalyst layer that has been cut into a predetermined shape at the time of bonding is used as the electrolyte. Easily manufacture an electrolyte membrane / catalyst layer assembly that has a catalyst layer with a smaller area than the electrolyte membrane, without the need for troublesome work such as positioning it near the center of the membrane. can do. In addition, since the entire surface of the electrolyte is pressurized in the joining process of the electrolyte membrane / catalyst layer assembly, thermal deformation of the electrolyte membrane due to heating is limited, and there is no generation of wrinkles or dimensional changes. A catalyst layer assembly is obtained.

[第2の実施形態]
図3、図4を用いて、本発明の第2の実施形態の構成を説明する。この第2の実施形態の燃料電池の製造方法および製造装置は、第1の実施形態の変形であり、第1、第2のマスキングシート4、6の開口部4a、6aを互いに異なる形状にする。その他の構成および、電解質膜・触媒層接合体の製造方法については第1の実施形態と同様である。図4は、本実施形態によって得られた電解質膜・触媒層接合体の断面図である。
[Second Embodiment]
The configuration of the second embodiment of the present invention will be described with reference to FIGS. The fuel cell manufacturing method and manufacturing apparatus according to the second embodiment is a modification of the first embodiment, and the openings 4a and 6a of the first and second masking sheets 4 and 6 have different shapes. . Other configurations and the manufacturing method of the electrolyte membrane / catalyst layer assembly are the same as those in the first embodiment. FIG. 4 is a cross-sectional view of the electrolyte membrane / catalyst layer assembly obtained by the present embodiment.

以上のような、本実施形態では第1の実施形態と同等の効果が得られるとともに、電解質膜の両側に形状が異なる触媒層を有する電解質膜・触媒層接合体を容易に製造することができる。一般に、カソードに比べてアノードが小さいと電極の腐食が促進される傾向があるので、この実施形態によってカソードに比べてアノードを大きくしておくことにより、腐食を抑制することができる。   As described above, in this embodiment, the same effect as that of the first embodiment can be obtained, and an electrolyte membrane / catalyst layer assembly having catalyst layers having different shapes on both sides of the electrolyte membrane can be easily manufactured. . In general, when the anode is smaller than the cathode, the corrosion of the electrode tends to be accelerated. Therefore, the corrosion can be suppressed by making the anode larger than the cathode according to this embodiment.

[第3の実施形態]
図5〜図7を用いて、本発明の第3の実施形態の構成を説明する。図5は、本実施形態における電解質膜と触媒層を接合するための装置と各部材の位置関係を説明するための図である。図示のように、一対の熱板11a、11bからなる加熱プレス機11には、第1、第2の弾性部材2、8がそれぞれ固定されており、これらの弾性部材と相対する位置に第1、第2のマスキングシート4、6がそれぞれ間隔をおいて加熱プレス11の開閉方向に対して平行に移動可能に支持されている。第1、第2のマスキングシート4、6には第1の実施形態のマスキングシートと同様に、それぞれ、作成する電解質膜・触媒層接合体における触媒層の形状に相当する形状の図示されない開口部が設けられている。
[Third Embodiment]
The configuration of the third embodiment of the present invention will be described with reference to FIGS. FIG. 5 is a view for explaining the positional relationship between an apparatus for joining the electrolyte membrane and the catalyst layer and each member in the present embodiment. As shown in the figure, the first and second elastic members 2 and 8 are fixed to the heating press 11 composed of a pair of hot plates 11a and 11b, respectively. The second masking sheets 4 and 6 are supported so as to be movable in parallel to the opening and closing direction of the heating press 11 at intervals. The first and second masking sheets 4 and 6 have openings corresponding to the shape of the catalyst layer in the electrolyte membrane / catalyst layer assembly to be formed, as in the masking sheet of the first embodiment. Is provided.

本実施形態では、電解質膜5および第1、第2のマスキングシート4、6はそれぞれ、電解質膜5および第1、第2のマスキングシート4、6が順次1個分ずつ断続的に供給されるように、面方向に連なる複数個分がテープ状になっている。また、これによって作成された電解質膜・触媒層接合体は、複数個分が面方向に並んで連なって出て行くようにテープ状に形成される。   In the present embodiment, the electrolyte membrane 5 and the first and second masking sheets 4 and 6 are supplied intermittently one by one in sequence, respectively. In this way, a plurality of portions that are continuous in the surface direction are tape-shaped. In addition, the electrolyte membrane / catalyst layer assembly produced in this way is formed in a tape shape so that a plurality of the electrolyte membrane / catalyst layer assemblies are arranged side by side in the plane direction.

電解質膜5は、電解質膜供給装置12から第1、第2のマスキングシート4、6の間に連続的に供給されるとともに、接合後の電解質膜・触媒層接合体は接合体収納装置13に収納される。第1、第2の触媒付きフィルム3、7は、それぞれ第1、第2の触媒層付きフィルム供給装置14、15から第1の弾性部材2と第1のマスキングシート4の間、および第2の弾性部材8と第2のマスキングシート6の間に連続的に供給される。また、触媒層3b、7bが電解質膜5に転写された後の基材および電解質膜5に転写されずに基材上に残留した触媒層5は、第1、第2の触媒層付きフィルム回収装置16、17に回収される。   The electrolyte membrane 5 is continuously supplied from the electrolyte membrane supply device 12 between the first and second masking sheets 4 and 6, and the joined electrolyte membrane / catalyst layer assembly is supplied to the assembly housing device 13. Stored. The first and second catalyst-attached films 3 and 7 are respectively provided between the first elastic member 2 and the first masking sheet 4 and the second from the first and second catalyst layer-attached film supply devices 14 and 15, respectively. The elastic member 8 and the second masking sheet 6 are continuously supplied. In addition, the base material after the catalyst layers 3b and 7b are transferred to the electrolyte membrane 5 and the catalyst layer 5 that is not transferred to the electrolyte membrane 5 and remains on the base material are recovered as the first and second catalyst layer-attached films. Collected in the devices 16 and 17.

接合体収納装置13に収納された電解質膜・触媒層接合体は、複数個が面方向に連続して並んだ状態であるので、その後、個々の電解質膜・触媒層接合体に切断され、その結果、図2または図4に示すような電解質膜・触媒層接合体ができる。   Since a plurality of electrolyte membrane / catalyst layer assemblies housed in the assembly housing device 13 are continuously arranged in the plane direction, the individual electrolyte membrane / catalyst layer assemblies are then cut into As a result, an electrolyte membrane / catalyst layer assembly as shown in FIG. 2 or 4 can be obtained.

次に、電解質膜・触媒層接合体の製造方法について説明する。図5に示すように、各部材が加熱プレス機11に供給された状態で加熱プレスの熱板11a、11bの両方もしくは一方が互いに近接する方向に移動する。これとともに、図6に示すように、それぞれ間隔を持って支持されている第1、第2のマスキングシート4、6が互いに位置合わせされた状態で近接させられ、さらに、第1、第2の触媒付きフィルム3、7も電解質膜5に対して互いに近接する方向に移動し、その状態で加熱および加圧される。これにより、第1の実施形態と同様の原理にて、マスキングシートの開口部4a、6aの範囲に相対する部分の触媒層3c、7cが電解質膜5に転写される。   Next, a method for producing an electrolyte membrane / catalyst layer assembly will be described. As shown in FIG. 5, both or one of the hot plates 11 a and 11 b of the hot press move in a direction in which they are close to each other with each member being supplied to the hot press machine 11. At the same time, as shown in FIG. 6, the first and second masking sheets 4 and 6 supported with a gap between them are brought close to each other while being aligned with each other. The films 3 and 7 with a catalyst also move in the direction close to the electrolyte membrane 5, and are heated and pressurized in that state. Thereby, the catalyst layers 3c and 7c corresponding to the range of the openings 4a and 6a of the masking sheet are transferred to the electrolyte membrane 5 on the same principle as in the first embodiment.

その後、加熱プレス11の熱板11a、11bが図5に示す状態まで戻るとともに、第1、第2のマキングシート4、6と電解質膜5と第1、第2の触媒付きフィルム3、7が互いに剥離される。また、以上の触媒層の転写工程が終了後、触媒層3c、7cを転写された電解質膜5は電解質膜・触媒層接合体として接合体収納装置13に収納されるとともに、新たな電解質膜の部分が電解質膜供給装置12から加熱プレス11に供給され、同様に、触媒層3c、7cが電解質膜5に転写された後の基材3a、7aおよび電解質膜5に転写されずに基材上に残留した触媒層3c、7cは、第1、第2の触媒層付きフィルム回収装置16、17に回収されるとともに、新たな触媒層付きフィルム3、7の部分が第1、第2の触媒層付きフィルム供給装置14、15から加熱プレス11に供給される。さらに、上記の接合工程および部材供給工程を連続して行なうことで、複数の電解質膜・触媒層接合体が面方向に、テープ状に連続して得られる。   Thereafter, the hot plates 11a and 11b of the hot press 11 return to the state shown in FIG. 5, and the first and second macking sheets 4 and 6, the electrolyte membrane 5, and the first and second films with catalyst 3, 7 Are separated from each other. In addition, after the transfer process of the catalyst layer is completed, the electrolyte membrane 5 to which the catalyst layers 3c and 7c are transferred is stored in the assembly storage device 13 as an electrolyte membrane / catalyst layer assembly, and a new electrolyte membrane is formed. The portion is supplied from the electrolyte membrane supply device 12 to the heating press 11. Similarly, the catalyst layers 3 c, 7 c are transferred to the electrolyte membrane 5, and are not transferred to the electrolyte membrane 5. The catalyst layers 3c and 7c remaining in the catalyst are recovered by the first and second film recovery devices 16 and 17 with a catalyst layer, and the portions of the new films 3 and 7 with a catalyst layer are the first and second catalysts. It is supplied to the heating press 11 from the film supply devices 14 and 15 with layers. Furthermore, a plurality of electrolyte membrane / catalyst layer assemblies are continuously obtained in a tape shape in the surface direction by continuously performing the above-described joining step and member supply step.

図7は、本実施形態によって得られた電解質膜・触媒層接合体の斜視図である。ここで、第1、第2のマスキングシート4、6を介して電解質膜5に面していた触媒層の範囲では、触媒層が電解質膜5に転写されていないため、接合された触媒層3c、7cは電解質膜5よりも面積が小さく触媒層の周辺には触媒層を有しない電解質膜の範囲5aが得られる。さらに、触媒層の転写工程において、第1、第2のマキングシート4、6は互いに位置合わせされた状態で近接させられているので、触媒層付きフィルム3、7を加熱プレス11に供給する際に精細な位置合わせを行なうことなしに電解質膜5の両面に転写される触媒層3c、7cの位置ずれがない電解質膜・触媒層接合体が得られる。   FIG. 7 is a perspective view of the electrolyte membrane / catalyst layer assembly obtained by the present embodiment. Here, in the range of the catalyst layer facing the electrolyte membrane 5 through the first and second masking sheets 4 and 6, the catalyst layer is not transferred to the electrolyte membrane 5, and therefore the joined catalyst layer 3c. 7c has an area smaller than that of the electrolyte membrane 5, and an electrolyte membrane range 5a having no catalyst layer is obtained around the catalyst layer. Furthermore, in the transfer process of the catalyst layer, the first and second marking sheets 4 and 6 are brought close to each other while being aligned with each other, so that the films 3 and 7 with the catalyst layer are supplied to the heating press 11. In this case, an electrolyte membrane / catalyst layer assembly can be obtained in which the catalyst layers 3c and 7c transferred to both surfaces of the electrolyte membrane 5 are not displaced without fine alignment.

また、第1、第2のマスキングシート4、6をフッ素樹脂もしくは表面にフッ素樹脂層を有する材料とすることにより、電解質膜5とマスキングシート4、6の剥離が容易に行なえるとともに、マスキングシート4、6の表面に電解質層が転写されることがなくなり、マスキングシート4、6を繰り返して製造に使用することが可能となる。   In addition, by using the first and second masking sheets 4 and 6 as a fluororesin or a material having a fluororesin layer on the surface, the electrolyte membrane 5 and the masking sheets 4 and 6 can be easily peeled off, and the masking sheet. The electrolyte layer is not transferred to the surfaces of 4 and 6, and the masking sheets 4 and 6 can be used repeatedly for production.

また、第1、第2の弾性部材2、8は、第1の実施形態と同様にマスキングシート4、6の厚さに対して十分な厚さを持ち、厚さ方向に段差を有しない形状とすることが望ましい。   The first and second elastic members 2 and 8 have a sufficient thickness with respect to the thickness of the masking sheets 4 and 6 as in the first embodiment, and have no step in the thickness direction. Is desirable.

以上説明したように、本実施形態では、予め触媒の一部を基材上から除去した形状の触媒層付きフィルムを形成したり、接合の際に予め所定の形状に切断された触媒層を電解質膜の中央付近に位置合わせして設置するような面倒な作業が不要で、触媒層の位置ずれがなく、電解質膜よりも面積の小さい触媒層を有する電解質膜・触媒層接合体を容易に連続的に製造することができる。   As described above, in the present embodiment, a catalyst layer-attached film having a shape in which a part of the catalyst has been removed from the substrate in advance is formed, or the catalyst layer that has been cut into a predetermined shape at the time of bonding is used as the electrolyte. There is no need for troublesome work such as positioning it near the center of the membrane, there is no displacement of the catalyst layer, and an electrolyte membrane / catalyst layer assembly that has a catalyst layer with a smaller area than the electrolyte membrane is easily continuous. Can be manufactured automatically.

[第4の実施形態]
図8、図9を用いて、本発明の第4の実施形態について説明する。この第4の実施形態は、第3の実施形態の変形であって、触媒層付きフィルムの使用量を低減させるための燃料電池の製造方法である。
[Fourth Embodiment]
A fourth embodiment of the present invention will be described with reference to FIGS. The fourth embodiment is a modification of the third embodiment, and is a method of manufacturing a fuel cell for reducing the amount of the catalyst layer-attached film used.

上記第3の実施形態の燃料電池の製造方法において、図5の装置にて電解質膜膜・触媒層接合体を製造する場合に、触媒層が電解質膜に転写された後の基材および電解質膜に転写されずに基材上に残留した触媒層は、第1、第2の触媒層付きフィルム回収装置16、17に回収されるとともに、新たな触媒層付きフィルム3、7が第1、第2の触媒層付きフィルム供給装置14、15から加熱プレス11に供給される。このとき、1回の接合工程で第1、第2の弾性部材2、8に挟持され、加熱および加圧された触媒層付きフィルム3、7の範囲を次の接合には使用しないことを目的として、1回の接合工程終了後に第1の触媒層付きフィルム供給装置14から加熱プレス11に供給される触媒層付きフィルム3、7の全長を、第1の弾性部材2の触媒層付きフィルム送り方向の全長とほぼ同じ長さとする。   In the method of manufacturing the fuel cell according to the third embodiment, when the electrolyte membrane / catalyst layer assembly is manufactured with the apparatus of FIG. 5, the base material and the electrolyte membrane after the catalyst layer is transferred to the electrolyte membrane The catalyst layer remaining on the substrate without being transferred to the substrate is recovered by the first and second film recovery devices 16 and 17 with the catalyst layer, and the new films 3 and 7 with the catalyst layer are first and first. 2 are supplied to the heating press 11 from the film supply devices 14 and 15 with a catalyst layer. At this time, the purpose is not to use the range of the films 3 and 7 with the catalyst layer sandwiched between the first and second elastic members 2 and 8 and heated and pressurized in one joining step for the next joining. As a film feed with the catalyst layer of the first elastic member 2, the entire length of the films 3 and 7 with the catalyst layer supplied from the first film supply device 14 with the catalyst layer 14 to the heating press 11 after the end of one joining step The length is almost the same as the total length in the direction.

第3の実施形態の場合、第1の触媒層付きフィルム回収装置16に回収される第1の触媒層付きフィルム3には、図8に示すように、触媒層が転写されない範囲3dが含まれている。しかし、一般に、触媒層には高価な貴金属が含まれているため、燃料電池の製造コスト低減のためには、触媒層付きフィルムの使用量を削減することが好ましい。   In the case of the third embodiment, the first catalyst layer-attached film 3 recovered by the first catalyst layer-attached film recovery device 16 includes a range 3d where the catalyst layer is not transferred, as shown in FIG. ing. However, in general, the catalyst layer contains an expensive noble metal, and therefore it is preferable to reduce the amount of the film with the catalyst layer used in order to reduce the manufacturing cost of the fuel cell.

そこで、この第4の実施形態では、1回の接合工程終了後に第1の触媒層付きフィルム供給装置14から加熱プレス11に供給される触媒層付きフィルム3の全長を、転写される触媒層の触媒層付きフィルム送り方向の全長より僅かに長い寸法とする。この場合の第1の触媒層付きフィルム回収装置16に回収される第1の触媒層付きフィルム3の斜視図を図9に示す。図9に示すように、触媒層付きフィルム3には触媒層が転写されない範囲3eが含まれているが、その面積は、図8における触媒層が転写されない範囲3dよりも小さくなる。したがって、同じ回数の電解質膜・触媒層接合工程に使用される触媒層転写フィルムの全長は図8の場合に比べて短くなる。なお、第2の触媒層付きフィルム7についても同様の方法で使用される触媒層転写フィルムの全長を短くできる。   Therefore, in the fourth embodiment, the entire length of the film 3 with the catalyst layer supplied from the first film supply device 14 with the catalyst layer 14 to the heating press 11 after the end of one joining step is determined by the catalyst layer to be transferred. The size is slightly longer than the total length in the film feeding direction with the catalyst layer. FIG. 9 shows a perspective view of the first catalyst layer-attached film 3 recovered by the first catalyst layer-attached film recovery device 16 in this case. As shown in FIG. 9, the film 3 with a catalyst layer includes a range 3e where the catalyst layer is not transferred, but the area is smaller than the range 3d where the catalyst layer is not transferred in FIG. Therefore, the total length of the catalyst layer transfer film used in the same number of electrolyte membrane / catalyst layer joining steps is shorter than that in the case of FIG. In addition, also about the 2nd film 7 with a catalyst layer, the full length of the catalyst layer transfer film used by the same method can be shortened.

以上説明したように、本実施形態では第3の実施形態と同等の効果が得られるとともに、触媒層付きフィルムの使用量を低減することができる。   As described above, in this embodiment, the same effect as in the third embodiment can be obtained, and the amount of the catalyst layer-attached film can be reduced.

[第5の実施形態]
図10、図11を用いて、本発明の第5の実施形態の構成を説明する。この第5の実施形態の燃料電池の製造方法および製造装置は、第3の実施形態の変形であるが、マスキングシート4,6を連続的に供給する点が第4の実施形態と異なる。すなわち、図5で第1、第2のマスキングシート4、6が加熱プレス11の開閉方向に対して垂直に移動可能に支持されていたのに対し、図10に示すこの第5の実施形態では第1、第2のマスキングシート4、6は、それぞれ、第1、第2のマスキングシート供給装置18、19から加熱プレス11に連続的に供給されるとともに、第1、第2のマスキングシート回収装置20、21にて回収される。
[Fifth Embodiment]
The configuration of the fifth embodiment of the present invention will be described with reference to FIGS. The fuel cell manufacturing method and manufacturing apparatus of the fifth embodiment is a modification of the third embodiment, but differs from the fourth embodiment in that the masking sheets 4 and 6 are continuously supplied. That is, in FIG. 5, the first and second masking sheets 4 and 6 are supported so as to be movable perpendicular to the opening and closing direction of the heating press 11, whereas in the fifth embodiment shown in FIG. The first and second masking sheets 4 and 6 are continuously supplied from the first and second masking sheet supply devices 18 and 19 to the heating press 11, respectively, and the first and second masking sheets are collected. Collected by the devices 20 and 21.

次に、電解質膜・触媒層接合体の製造方法について説明する。図10に示すように、電解質膜5を第1、第2のマスキングシート4、6で挟み込み、これを第1、第2の触媒層付きフィルム3、7で挟み込むようにして、加熱プレス機11の熱板11a、11bの間に挟まれる位置に搬送する。このとき熱板11a、11bには、第1、第2の弾性部材2、8があらかじめ取り付けられている。この状態から、熱板11a、11bの両方もしくは一方が互いに近接する方向に移動する。これにより、第1、第2の触媒付きフィルム3、7が電解質膜5に対して近接させられ、その状態で加熱および加圧されることによって、第1の実施形態と同様の原理にて、マスキングシートの開口部4a、6aの範囲に相対する部分の触媒層3c、7cが電解質膜5に転写される。   Next, a method for producing an electrolyte membrane / catalyst layer assembly will be described. As shown in FIG. 10, the electrolyte membrane 5 is sandwiched between the first and second masking sheets 4, 6, and is sandwiched between the first and second films 3, 7 with the catalyst layer. To a position sandwiched between the hot plates 11a and 11b. At this time, the first and second elastic members 2 and 8 are attached in advance to the hot plates 11a and 11b. From this state, both or one of the hot plates 11a and 11b moves in a direction approaching each other. Thereby, the first and second catalyst-attached films 3 and 7 are brought close to the electrolyte membrane 5 and heated and pressurized in this state, whereby the same principle as in the first embodiment is obtained. The portions of the catalyst layers 3c and 7c facing the range of the openings 4a and 6a of the masking sheet are transferred to the electrolyte membrane 5.

その後、加熱プレス11の熱板11a、11bが図10に示す状態まで戻される。そして、第1、第2のマキングシート4、6と電解質膜5と第1、第2の触媒付きフィルム3、7が剥離され、第1、第2のマキングシート4、6は第1、第2のマスキングシート回収装置20、21に回収され、第1、第2の触媒層付きフィルム3、7は第1、第2の触媒層付きフィルム回収装置16、17に回収され、電解質膜・触媒層接合体は接合体収納装置13に収納される。さらに、上記の接合工程および部材供給工程を連続して行なうことで電解質膜・触媒層接合体が連続して得られる。   Thereafter, the hot plates 11a and 11b of the hot press 11 are returned to the state shown in FIG. Then, the first and second Machining sheets 4 and 6, the electrolyte membrane 5, the first and second catalyst-attached films 3 and 7 are peeled off, and the first and second Machining sheets 4 and 6 are the first. The first and second catalyst layer-attached films 3 and 7 are recovered by the first and second catalyst layer-attached film recovery devices 16 and 17, respectively, and the electrolyte film is recovered. The catalyst layer assembly is stored in the assembly storage device 13. Furthermore, an electrolyte membrane / catalyst layer assembly can be continuously obtained by continuously performing the above-described joining step and member supply step.

第1、第2のマスキングシート4、6が加熱プレス11に供給される際には、位置合わせ装置22にてそれぞれの開口部4a、6aを所定の位置に位置合わせされているので触媒層3c、7cの位置ずれがなく電解質膜・触媒層接合体を製造できる。図11はマスキングシート4、6の位置合わせ方法を説明する模擬図である。位置合わせ装置としては、たとえば、図11に示すように、電解質膜5より外側に位置する第1、第2のマスキングシート4、6の両辺に、予め位置決め用貫通孔4c、6cを設置しておき、各位置決め用貫通孔4c、6cを貫通するピン22aを有する位置合わせ装置22を使用することが考えられる。すなわち、ピン22aが位置決め用貫通孔4c、6cを貫通した状態でピン22aを回転駆動することにより、第1、第2のマスキングシート4、6を搬送することができ、また、第1、第2のマスキングシート4、6によって挟まれた電解質膜5を摩擦によって、第1、第2のマスキングシート4、6とともに搬送することができる。   When the first and second masking sheets 4 and 6 are supplied to the heating press 11, the openings 4a and 6a are aligned at predetermined positions by the alignment device 22, so that the catalyst layer 3c. , 7c can be produced, and an electrolyte membrane / catalyst layer assembly can be produced. FIG. 11 is a simulation diagram for explaining a method of aligning the masking sheets 4 and 6. As an alignment apparatus, for example, as shown in FIG. 11, positioning through holes 4c and 6c are previously installed on both sides of the first and second masking sheets 4 and 6 positioned outside the electrolyte membrane 5. In addition, it is conceivable to use an alignment device 22 having a pin 22a penetrating each positioning through hole 4c, 6c. That is, the first and second masking sheets 4 and 6 can be conveyed by rotating the pin 22a while the pin 22a passes through the positioning through holes 4c and 6c. The electrolyte membrane 5 sandwiched between the two masking sheets 4 and 6 can be conveyed together with the first and second masking sheets 4 and 6 by friction.

以上説明したように、本実施形態では、予め触媒の一部を基材上から除去した形状の触媒層付きフィルムを形成したり、接合の際に予め所定の形状に切断された触媒層を電解質膜の中央付近に位置合わせして設置するような面倒な作業が不要で、触媒層の位置ずれがなく、電解質膜よりも面積の小さい触媒層を有する電解質膜・触媒層接合体を容易に連続的に製造することができる。   As described above, in the present embodiment, a catalyst layer-attached film having a shape in which a part of the catalyst has been removed from the substrate in advance is formed, or the catalyst layer that has been cut into a predetermined shape at the time of bonding is used as the electrolyte. There is no need for troublesome work such as positioning it near the center of the membrane, there is no displacement of the catalyst layer, and an electrolyte membrane / catalyst layer assembly that has a catalyst layer with a smaller area than the electrolyte membrane is easily continuous. Can be manufactured automatically.

[第6の実施形態]
図12を用いて、本発明の第6の実施形態の構成を説明する。この第6の実施形態の燃料電池の製造方法および製造装置は、第5の実施形態の変形であって、加熱プレスの代りにホットローラー23を使用する。図12に示すように、ホットローラー23の一対の加熱回転体23a、23bは、その外周部に弾性部材2、8が設置されており、互いに近接する方向に一定の加圧力を有するように保持されている。
[Sixth Embodiment]
The configuration of the sixth embodiment of the present invention will be described with reference to FIG. The fuel cell manufacturing method and manufacturing apparatus of the sixth embodiment is a modification of the fifth embodiment, and uses a hot roller 23 instead of a heating press. As shown in FIG. 12, the pair of heating rotators 23a and 23b of the hot roller 23 is provided with elastic members 2 and 8 on the outer peripheral portion thereof, and is held so as to have a constant pressure in a direction in which they are close to each other. Has been.

加熱回転体23a、23bの間をマスキングシート4、6、触媒層付きフィルム3、7、電解質膜5が一定の速度で通過することによって、第1、第2の触媒付きフィルム3、7が電解質膜5に対して近接させられた状態で加熱および加圧され、マスキングシートの開口部4a、6aの範囲に相対する部分の触媒層3c、7cが電解質膜5に転写される。ここで、第1、第2のマスキングシート4、6がホットローラー23に供給される際には、第5の実施形態と同様の位置合わせ装置22にてそれぞれの開口部4a、6aは所定の位置に位置合わせされているので触媒層5の位置ずれがなく電解質膜・触媒層接合体を製造できる。   The masking sheets 4 and 6, the films 3 and 7 with the catalyst layer 3, and the electrolyte membrane 5 pass between the heating rotators 23a and 23b at a constant speed, so that the first and second films 3 and 7 with the catalyst are electrolytes. Heating and pressing are performed in a state of being close to the membrane 5, and portions of the catalyst layers 3 c and 7 c facing the range of the openings 4 a and 6 a of the masking sheet are transferred to the electrolyte membrane 5. Here, when the first and second masking sheets 4 and 6 are supplied to the hot roller 23, the respective openings 4 a and 6 a are predetermined in the alignment device 22 similar to the fifth embodiment. Since it is aligned with the position, there is no displacement of the catalyst layer 5 and an electrolyte membrane / catalyst layer assembly can be manufactured.

以上説明したように、本実施形態では第5の実施形態と同等の効果が得られる。   As described above, in this embodiment, the same effect as that of the fifth embodiment can be obtained.

[他の実施形態]
以上種々の実施形態について説明したが、これらは単なる例示であって、本発明はこれらに限定されるものではない。
[Other Embodiments]
Although various embodiments have been described above, these are merely examples, and the present invention is not limited thereto.

たとえば、図10では各部材の供給装置はロール成型された部材の送り出し装置を示しており、各部材の回収装置もロール状の巻き取り装置を示しているが、部材が連続的に供給および回収されるのであれば、その方法は本図に限定されず、たとえば、切断済みの部材を1枚ずつ搬送する搬送装置と回収装置の組合せとしてもよい。また、電解質膜・触媒層接合体の収納装置も、図示の形状の巻き取り装置ではなく、切断装置と切断後の電解質膜・触媒層接合体を収納する装置としても良い。   For example, in FIG. 10, the supply device for each member shows a feed device for a roll-formed member, and the recovery device for each member also shows a roll-shaped take-up device, but the members are continuously supplied and recovered. If this is done, the method is not limited to this figure. For example, a combination of a transporting device that transports cut members one by one and a recovery device may be used. The storage device for the electrolyte membrane / catalyst layer assembly may be a device for storing the cutting device and the cut electrolyte membrane / catalyst layer assembly instead of the winding device having the shape shown in the figure.

また、上記の実施形態の説明におけるマスキングシート、弾性部材、電解質膜、触媒層付きフィルムについても本発明の目的を果たすことが可能であれば上述の形状および部材に限定されるものではない。   In addition, the masking sheet, the elastic member, the electrolyte membrane, and the film with the catalyst layer in the description of the above embodiment are not limited to the above shapes and members as long as the object of the present invention can be achieved.

本発明に係る燃料電池の製造方法の第1の実施形態における電解質膜・触媒層接合体の製造過程を示す模式的展開斜視図である。1 is a schematic exploded perspective view showing a manufacturing process of an electrolyte membrane / catalyst layer assembly in a first embodiment of a fuel cell manufacturing method according to the present invention. 図1の電解質膜・触媒層接合体の完成状態を示す立断面図である。FIG. 2 is an elevational sectional view showing a completed state of the electrolyte membrane / catalyst layer assembly of FIG. 1. 本発明に係る燃料電池の製造方法の第2の実施形態における電解質膜・触媒層接合体の製造過程を示す模式的展開斜視図である。It is a typical expansion perspective view showing a manufacturing process of an electrolyte membrane / catalyst layer assembly in a 2nd embodiment of a manufacturing method of a fuel cell concerning the present invention. 図3の電解質膜・触媒層接合体の完成状態を示す立断面図である。FIG. 4 is an elevational sectional view showing a completed state of the electrolyte membrane / catalyst layer assembly of FIG. 3. 本発明に係る燃料電池の製造方法の第3の実施形態における電解質膜・触媒層接合体の製造過程を示す模式的立断面図であって、押し付け加熱を行なう前の状態を示す図である。It is a typical elevation sectional view showing a manufacturing process of an electrolyte membrane / catalyst layer assembly in a 3rd embodiment of a manufacturing method of a fuel cell concerning the present invention, and is a figure showing a state before performing pressing heating. 本発明に係る燃料電池の製造方法の第3の実施形態における電解質膜・触媒層接合体の製造過程を示す模式的立断面図であって、押し付け加熱を行なっている状態を示す図である。FIG. 10 is a schematic sectional view showing a manufacturing process of an electrolyte membrane / catalyst layer assembly in a third embodiment of a method for manufacturing a fuel cell according to the present invention, and shows a state where pressing heating is performed. 本発明の第3の実施形態における電解質膜・触媒層接合体を示す斜視図である。It is a perspective view which shows the electrolyte membrane and catalyst layer assembly in the 3rd Embodiment of this invention. 本発明の第3の実施形態において回収された触媒層付きフィルムを示す斜視図である。It is a perspective view which shows the film with a catalyst layer collect | recovered in the 3rd Embodiment of this invention. 本発明の第4の実施形態において回収された触媒層付きフィルムを示す斜視図である。It is a perspective view which shows the film with a catalyst layer collect | recovered in the 4th Embodiment of this invention. 本発明に係る燃料電池の製造方法の第5の実施形態における電解質膜・触媒層接合体の製造過程を示す模式的立断面図であって、押し付け加熱を行なう前の状態を示す図である。It is a typical elevation sectional view showing a manufacturing process of an electrolyte membrane / catalyst layer assembly in a 5th embodiment of a manufacturing method of a fuel cell concerning the present invention, and is a figure showing a state before performing pressing heating. 本発明に係る燃料電池の製造方法の第5の実施形態において、電解質膜を2枚のマスキングシートで挟んで搬送する状況を示す模式的斜視図である。FIG. 10 is a schematic perspective view showing a state in which an electrolyte membrane is sandwiched and transported between two masking sheets in a fifth embodiment of a method for producing a fuel cell according to the present invention. 本発明に係る燃料電池の製造方法の第6の実施形態における電解質膜・触媒層接合体の製造過程を示す模式的立断面図である。It is typical sectional drawing which shows the manufacturing process of the electrolyte membrane and catalyst layer assembly in 6th Embodiment of the manufacturing method of the fuel cell concerning this invention.

符号の説明Explanation of symbols

1…第1の治具、1a…板状部材、2…第1の弾性部材、3…第1の触媒層付きフィルム、3a…第1の触媒層付きフィルムの基材、3b…第1の触媒層付きフィルムの触媒層、3c…第1の触媒層付きフィルムの転写された触媒層、3d…第1の触媒層付きフィルムの転写されなかった触媒層、3e…第1の触媒層付きフィルムの転写されなかった触媒層、4…第1のマスキングシート、4a…第1のマスキングシートの開口部、4b…第1のマスキングシートの開口部以外の部分、4c…第1のマスキングシートの位置合わせ用貫通孔、5…電解質膜、5a…電解質膜の触媒層が転写されていない範囲、6…第2のマスキングシート、6a…第2のマスキングシートの開口部、6b…第2のマスキングシートの開口部以外の部分、6c…第2のマスキングシートの位置合わせ用貫通孔、7…第2の触媒層付きフィルム、7a…第2の触媒層付きフィルムの基材、7b…第2の触媒層付きフィルムの触媒層、7c…第2の触媒層付きフィルムの転写された触媒層、8…第2の弾性部材、9…第2の治具、10…位置決め治具、11…加熱プレス機、11a…加熱プレス機の熱板、11b…加熱プレス機の熱板、12…電解質膜供給装置、13…接合体収納装置、14…第1の触媒層付きフィルム供給装置、15…第2の触媒層付きフィルム供給装置、16…第1の触媒層付きフィルム回収装置、17…第2の触媒層付きフィルム回収装置、18…第1のマスキングシート供給装置、19…第2のマスキングシート供給装置、20…第1のマスキングシート回収装置、21…第2のマスキングシート回収装置、22…位置合わせ装置、22a…ピン、23…ホットローラー、23a…ホットローラーの加熱回転体、23b…ホットローラーの加熱回転体 DESCRIPTION OF SYMBOLS 1 ... 1st jig | tool, 1a ... Plate-shaped member, 2 ... 1st elastic member, 3 ... Film with 1st catalyst layer, 3a ... Base material of film with 1st catalyst layer, 3b ... 1st Catalyst layer of the film with the catalyst layer, 3c ... Transferred catalyst layer of the film with the first catalyst layer, 3d ... Catalyst layer without transfer of the film with the first catalyst layer, 3e ... Film with the first catalyst layer Catalyst layer 4 not transferred, 4 ... first masking sheet, 4a ... first masking sheet opening, 4b ... other than first masking sheet opening, 4c ... first masking sheet position Through hole for alignment, 5 ... electrolyte membrane, 5a ... range where catalyst layer of electrolyte membrane is not transferred, 6 ... second masking sheet, 6a ... opening of second masking sheet, 6b ... second masking sheet 6c, other than the opening of 2 through holes for alignment of the masking sheet, 7... Second film with catalyst layer, 7 a... Base material of film with second catalyst layer, 7 b... Catalyst layer of film with second catalyst layer, 7 c. 2 transferred catalyst layer of the film with the catalyst layer, 8 ... second elastic member, 9 ... second jig, 10 ... positioning jig, 11 ... heating press machine, 11a ... hot plate of heating press machine, DESCRIPTION OF SYMBOLS 11b ... Hot plate of a heating press machine, 12 ... Electrolyte membrane supply apparatus, 13 ... Assembly accommodation apparatus, 14 ... Film supply apparatus with 1st catalyst layer, 15 ... Film supply apparatus with 2nd catalyst layer, 16 ... 1st DESCRIPTION OF SYMBOLS 1 Film recovery apparatus with a catalyst layer, 17 ... 2nd film recovery apparatus with a catalyst layer, 18 ... 1st masking sheet supply apparatus, 19 ... 2nd masking sheet supply apparatus, 20 ... 1st masking sheet collection apparatus , 21 ... second Scan King sheet collecting device, 22 ... positioning device, 22a ... pin, 23 ... hot rollers, 23a ... heating rotator of hot rollers, the heating rotating body 23b ... hot rollers

Claims (12)

電解質膜の両面に電極の触媒層を接合させた電解質膜・触媒層接合体を有する燃料電池の製造方法において、
前記触媒層がフィルム状の基材の片面に形成された触媒層付きフィルムを2枚用意し、
前記電解質膜の両面それぞれに、前記触媒層付きフィルムの触媒層よりも小さな寸法の開口部を有するマスキングシートを配置し、これらのマスキングシートをはさみ込むように、前記触媒層付きフィルムを、その触媒層がマスキングシートを向くように配置し、
さらに、前記触媒層付きフィルムの外側を、弾性部材を介して互いに押し付けるとともに加熱して、前記マスキングシートの開口部のみで前記触媒層と前記電解質膜とを接合した電解質膜・マスキングシート・触媒層付きフィルム接合体を形成し、
前記電解質膜・マスキングシート・触媒層付きフィルム接合体から前記触媒層付きフィルムの基材を剥離し、前記マスキングシートを取り外して前記電解質膜・触媒層接合体を形成する工程を含
前記電解質膜の両面に配置された前記マスキングシートの開口部の形状が互いに異なることを特徴とする燃料電池製造方法。
In a method for producing a fuel cell having an electrolyte membrane / catalyst layer assembly in which electrode catalyst layers are joined to both surfaces of an electrolyte membrane,
Prepare two sheets of catalyst layered film in which the catalyst layer is formed on one side of a film-like substrate,
A masking sheet having openings smaller in size than the catalyst layer of the catalyst layer-attached film is disposed on each of both surfaces of the electrolyte membrane, and the catalyst layer-attached film is placed in the catalyst so as to sandwich these masking sheets. Place the layer facing the masking sheet,
Furthermore, the outer side of the film with the catalyst layer is pressed against each other through an elastic member and heated to join the catalyst layer and the electrolyte membrane only with the opening of the masking sheet. With a film assembly,
Wherein the membrane masking sheet with catalyst layers film assembly was peeled off the base material of the catalyst layer with the film, it looks including the step of forming the membrane-catalyst layer assembly by removing the masking sheet,
The method of manufacturing a fuel cell , wherein the shapes of the openings of the masking sheets disposed on both surfaces of the electrolyte membrane are different from each other .
前記弾性部材は、弾性部材が少なくとも前記マスキングシートの開口部の境界に接する位置で段差を有しない部材からなる、ことを特徴とする請求項1に記載の燃料電池製造方法。   2. The fuel cell manufacturing method according to claim 1, wherein the elastic member is a member having no step at a position where the elastic member is at least in contact with the boundary of the opening of the masking sheet. 前記マスキングシートの少なくとも前記電解質膜に接する部分がフッ素樹脂を有する材料からなることを特徴とする請求項1または2に記載の燃料電池製造方法。 3. The fuel cell manufacturing method according to claim 1, wherein at least a portion of the masking sheet in contact with the electrolyte membrane is made of a material having a fluororesin . 前記電解質膜・触媒層接合体の複数個分が面方向に連続して並んで形成されるように、前記電解質膜および前記触媒層付きフィルムのそれぞれの複数個分が面方向に連続して並んだものを順次処理すること、を特徴とする請求項1ないし3のいずれかに記載の燃料電池製造方法。 A plurality of each of the electrolyte membrane and the film with the catalyst layer are continuously arranged in the plane direction so that a plurality of the electrolyte membrane / catalyst layer assemblies are continuously arranged in the plane direction. 4. The fuel cell manufacturing method according to claim 1, wherein the fuel cells are sequentially processed . 電解質膜の両面に電極の触媒層を接合させた電解質膜・触媒層接合体を有する燃料電池の製造装置において、In a fuel cell manufacturing apparatus having an electrolyte membrane / catalyst layer assembly in which an electrode catalyst layer is bonded to both surfaces of an electrolyte membrane,
開口部を有する2枚のマスキングシートで電解質膜を挟み込み、さらに、前記開口部よりも大きな触媒層がフィルム状の基材の表面に形成された触媒層付きフィルム2枚をその触媒層が内側を向くように配置して前記マスキングシートを前記触媒層付きフィルムで挟み込む重ね合わせ手段と、The electrolyte membrane is sandwiched between two masking sheets having openings, and two catalyst-coated films in which a catalyst layer larger than the openings is formed on the surface of the film-like substrate are arranged on the inside. An overlapping means that is arranged so as to face and sandwich the masking sheet with the film with the catalyst layer;
前記重ね合わせ手段で重ね合わされた2枚の触媒層付きフィルムの外側から弾性部材を介して加圧するとともに加熱して、前記マスキングシートの開口部のみで前記触媒層と前記電解質膜とを接合した電解質膜・マスキングシート・触媒層付きフィルム接合体を形成する加圧加熱手段と、An electrolyte in which the catalyst layer and the electrolyte membrane are joined only by an opening of the masking sheet by applying pressure and heat from the outside of the two films with the catalyst layer superimposed by the superimposing means through an elastic member. A pressure heating means for forming a membrane, masking sheet, film assembly with a catalyst layer,
前記電解質膜・マスキングシート・触媒層付きフィルム接合体から前記触媒層付きフィルムの基材を剥離し、前記マスキングシートを取り外して前記電解質膜・触媒層接合体を形成する剥離取り外し手段と、Peeling and removing means for peeling the substrate of the film with the catalyst layer from the membrane assembly with the electrolyte membrane / masking sheet / catalyst layer, removing the masking sheet to form the electrolyte membrane / catalyst layer assembly,
を有し、Have
前記電解質膜の両面に配置された前記マスキングシートの開口部の形状が互いに異なること、を特徴とする燃料電池製造装置。The fuel cell manufacturing apparatus according to claim 1, wherein the shapes of the openings of the masking sheets disposed on both surfaces of the electrolyte membrane are different from each other.
前記電解質膜の複数個分が面方向に連続して並んだものを順次供給する電解質膜供給手段と、
前記触媒層付きフィルムの複数個分が面方向に連続して並んだものを順次供給する第1のフィルム供給手段と、
前記触媒層付きフィルムの複数個分が面方向に連続して並んだものを順次供給する第2のフィルム供給手段と、
をさらに有し、前記重ね合わせ手段および加圧加熱手段は、前記電解質膜・触媒層接合体の複数個分が面方向に連続して並んで形成されるように構成されていること、を特徴とする請求項5に記載の燃料電池製造装置。
An electrolyte membrane supply means for sequentially supplying a plurality of the electrolyte membranes continuously arranged in the plane direction;
A first film supply means for sequentially supplying a plurality of the catalyst layer-equipped films sequentially arranged in the plane direction;
A second film supply means for sequentially supplying a plurality of the catalyst layer-attached films sequentially arranged in the plane direction;
The overlapping means and the pressurizing / heating means are configured such that a plurality of the electrolyte membrane / catalyst layer assemblies are continuously arranged in the plane direction. The fuel cell manufacturing apparatus according to claim 5 .
前記電解質膜供給手段は、前記電解質膜の複数個分が面方向に連続して並んだものを1個分ずつ断続的に順次供給するものであり、
前記第1および第2のフィルム供給手段は、前記触媒層付きフィルムの複数個分が面方向に連続して並んだものをそれぞれ1個分ずつ断続的に順次供給するものであること、を特徴とする請求項6に記載の燃料電池製造装置。
The electrolyte membrane supply means is for intermittently supplying one by one a plurality of electrolyte membranes continuously arranged in the plane direction one by one,
The first and second film supply means are configured to intermittently and sequentially supply a plurality of the catalyst layer-attached films that are continuously arranged in the surface direction one by one. The fuel cell manufacturing apparatus according to claim 6 .
前記第1および第2のフィルム供給手段が供給する触媒層付きフィルムの供給長さが、前記電解質膜供給手段が供給する電解質膜の供給長さよりも短いことを特徴とする請求項7に記載の燃料電池製造装置。 The supply length of the film with a catalyst layer supplied by the first and second film supply means is shorter than the supply length of the electrolyte membrane supplied by the electrolyte membrane supply means. Fuel cell manufacturing equipment. 前記マスキングシートは、前記電解質膜・触媒層接合体の複数個分が面方向に連続して並んだものが形成されており、このマスキングシートを順次供給するマスキングシート供給手段をさらに有すること、を特徴とする請求項6ないし8のいずれかに記載の燃料電池製造装置。 The masking sheet is formed of a plurality of the electrolyte membrane / catalyst layer assemblies continuously arranged in the plane direction, and further includes a masking sheet supply means for sequentially supplying the masking sheets. The fuel cell manufacturing apparatus according to any one of claims 6 to 8, 前記加圧加熱手段はホットローラーを含み、前記加圧加熱手段は、前記マスキングシートの開口部の範囲のみで前記触媒層と前記電解質膜とを接合すること、を特徴とする請求項6に記載の燃料電池製造装置。 The said pressure heating means contains a hot roller, The said pressure heating means joins the said catalyst layer and the said electrolyte membrane only in the range of the opening part of the said masking sheet, It is characterized by the above-mentioned. fuel cell manufacturing device. 前記弾性部材は、弾性部材が少なくとも前記マスキングシートの開口部の境界に接する位置で段差を有しない部材からなる、ことを特徴とする請求項5ないし10のいずれかに記載の燃料電池製造装置。 11. The fuel cell manufacturing apparatus according to claim 5, wherein the elastic member is a member having no step at a position where the elastic member is at least in contact with a boundary of the opening of the masking sheet . 前記マスキングシートの少なくとも前記電解質膜に接する部分がフッ素樹脂を有する材料からなることを特徴とする請求項5ないし11のいずれかに記載の燃料電池製造装置。 12. The fuel cell manufacturing apparatus according to claim 5, wherein at least a portion of the masking sheet that contacts the electrolyte membrane is made of a material having a fluororesin .
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