JP2010129247A - Method for manufacturing electrode stack of fuel cell - Google Patents

Method for manufacturing electrode stack of fuel cell Download PDF

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JP2010129247A
JP2010129247A JP2008300354A JP2008300354A JP2010129247A JP 2010129247 A JP2010129247 A JP 2010129247A JP 2008300354 A JP2008300354 A JP 2008300354A JP 2008300354 A JP2008300354 A JP 2008300354A JP 2010129247 A JP2010129247 A JP 2010129247A
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electrolyte membrane
masking film
film
sealing material
fuel cell
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JP5343529B2 (en
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Noriyuki Matsukaze
紀之 松風
Yasuta Nakai
康太 中井
Mitsuhiro Negami
光弘 根上
Masaaki Iwatani
政昭 岩谷
Yuji Sakagami
祐治 阪上
Kiyoshi Ichinose
浄 一瀬
Hidenobu Matsuyama
秀信 松山
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Nissan Motor Co Ltd
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Nissan Motor Co Ltd
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    • Y—GENERAL 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Abstract

<P>PROBLEM TO BE SOLVED: To suppress degradation in electrode quality when an electrode is formed on the surface of an electrolyte membrane and simplify a manufacturing process by eliminating a process for providing a sealing material on an electrolyte membrane in an after-process. <P>SOLUTION: A masking film 13 having double-layer structure comprising a masking film body 9 and an anode gasket 3 is joined to one surface of the electrolyte membrane 1 so that the anode gasket 3 is positioned on the electrolyte membrane 1 side, and a back sheet 17 for reinforcing is joined to the other surface of the electrolyte membrane 1. In this state, an anode layer 19 is formed on the electrolyte membrane 1 by applying catalyst paste from the masking film body 9 side. After that, the masking film body 9 is peeled off from the anode gasket 3, and the back sheet 17 is peeled off from the electrolyte membrane. On the cathode side, a projecting back sheet is joined to the anode side in place of the back sheet 17, and in this state, the same process as that on the anode side is conducted. <P>COPYRIGHT: (C)2010,JPO&INPIT

Description

本発明は、電解質膜の表面に電極触媒層を形成する燃料電池電極積層体の製造方法に関する。   The present invention relates to a method for producing a fuel cell electrode laminate in which an electrode catalyst layer is formed on the surface of an electrolyte membrane.

従来、燃料電池における電解質膜の表面に電極触媒層を形成する際、所定の電極形状に切り抜いたマスキングフィルムを電解質膜上に設け、このマスキングフィルムの上から触媒ペーストを塗布し、塗布後にマスキングフィルムを剥がすようにしている。
特開２００６−１２０４３３号公報 Conventionally, when an electrode catalyst layer is formed on the surface of an electrolyte membrane in a fuel cell, a masking film cut into a predetermined electrode shape is provided on the electrolyte membrane, and a catalyst paste is applied on the masking film. To peel off.
JP 2006-120433 A

ところで、上記した従来のものは、触媒ペーストを塗布する際に、電解質膜の電極形状部分の周縁のマスキングフィルム上にもその一部が塗布され、この一部の触媒ペーストが電解質膜上のペースト電極と連続したものとなりやすい。このため、触媒ペーストを塗布した後にマスキングフィルムを剥がす際には、上記マスキングフィルム上の触媒ペーストとともに電解質膜上の触媒ペーストも一緒に剥がれる恐れがあるので、電池電極の品質低下を招く恐れがある。   By the way, in the above-mentioned conventional one, when applying the catalyst paste, a part thereof is also applied on the masking film at the periphery of the electrode-shaped portion of the electrolyte membrane, and this part of the catalyst paste is paste on the electrolyte membrane. It tends to be continuous with the electrode. For this reason, when the masking film is peeled off after the catalyst paste is applied, the catalyst paste on the electrolyte membrane may be peeled off together with the catalyst paste on the masking film, which may cause deterioration of the quality of the battery electrode. .

そこで、本発明は、電解質膜の表面に電極を形成する際の電極品質の低下を抑えることを目的としている。   Therefore, an object of the present invention is to suppress deterioration of electrode quality when an electrode is formed on the surface of an electrolyte membrane.

本発明は、電解質膜の表面に、マスキングフィルム本体とシール材用フィルムとからなる二層構造のマスキングフィルムを設け、この二層構造のマスキングフィルムの上から電解質膜上に電極触媒層となる触媒ペーストを塗布した後、マスキングフィルム本体をシール材用フィルムから剥がすことを特徴とする。   The present invention provides a two-layered masking film comprising a masking film body and a sealing material film on the surface of an electrolyte membrane, and a catalyst that becomes an electrode catalyst layer on the electrolyte membrane from the two-layered masking film. After the paste is applied, the masking film main body is peeled off from the sealing material film.

本発明によれば、触媒ペーストを塗布する際に、二層構造のマスキングフィルムを電解質膜の表面に設けているので、このマスキングフィルムの表面と電解質膜の表面との間の段差が大きくなる。このため、二層構造のマスキングフィルムの上から触媒ペーストを塗布しても、電解質膜の電極形状部分の周縁のマスキングクフィルム本体上に塗布される一部の触媒ペーストと、電解質膜上の触媒ペーストとが連続したものとなりにくく、したがって、二層構造としたマスキングフィルムのうちマスキングフィルム本体のみを剥がすことで、必要とする電極部分の触媒ペーストの剥がれを抑制でき、電解質膜の表面に電極を形成する際の電極品質の低下を抑えることができる。また、マスキングフィルム本体のみを剥がすことで、シール材用フィルムが電解質膜の周縁表面上に残り、これがシール材となるので、後工程でのシール材を設ける工程を省略でき、製造工程が簡略化する。   According to the present invention, when the catalyst paste is applied, the masking film having a two-layer structure is provided on the surface of the electrolyte membrane, so that the level difference between the surface of the masking film and the surface of the electrolyte membrane is increased. For this reason, even if a catalyst paste is applied on the masking film having a two-layer structure, a part of the catalyst paste applied on the masking film body at the periphery of the electrode-shaped portion of the electrolyte membrane and the catalyst on the electrolyte membrane It is difficult for the paste to become continuous, and therefore, by peeling only the masking film main body out of the two-layered masking film, it is possible to prevent the catalyst paste from peeling off at the required electrode part, and to place the electrode on the surface of the electrolyte membrane. It is possible to suppress the deterioration of the electrode quality when forming. Also, by removing only the masking film body, the film for sealing material remains on the peripheral surface of the electrolyte membrane, which becomes the sealing material, so the process of providing the sealing material in the subsequent process can be omitted, and the manufacturing process is simplified To do.

以下、本発明の実施の形態を図面に基づき説明する。   Hereinafter, embodiments of the present invention will be described with reference to the drawings.

図１，図２は、本発明の一実施形態に係わる燃料電池電極の製造方法を示す模式図であり、図１はアノード側、図２はカソード側のそれぞれの電極について示している。本実施形態では、図３（ａ）に示すように、電解質膜としての固体高分子電解質膜（以下、単に電解質膜と呼ぶ）１の一方の面にアノードガスケット３を、他方の面にカソードガスケット５をそれぞれ接合して設けた積層体７を製造するものである。これら、アノードガスケット３及びカソードガスケット５はシール材用フィルムを構成している。   1 and 2 are schematic views showing a method of manufacturing a fuel cell electrode according to one embodiment of the present invention. FIG. 1 shows the electrode on the anode side, and FIG. 2 shows the electrode on the cathode side. In this embodiment, as shown in FIG. 3A, an anode gasket 3 is provided on one surface of a solid polymer electrolyte membrane (hereinafter simply referred to as an electrolyte membrane) 1 as an electrolyte membrane, and a cathode gasket is provided on the other surface. The laminated body 7 which joined and provided 5 is manufactured. These anode gasket 3 and cathode gasket 5 constitute a film for a sealing material.

これら各ガスケット３，５は、図４（ａ）に示す形状にトリム成形する。すなわち、各ガスケット３，５は、外形が例えば長方形であり、枠形状の外周部３ａ，５ａを残して中央部分が切り抜かれ長方形状の電極形成領域３ｂ，５ｂを形成するとともに、電極形成領域３ｂ，５ｂの両側部分に貫通孔３ｃ，５ｃを複数形成する。これら複数の貫通孔３ｃ，５ｃは、水素ガス，酸化剤ガス及び冷却水のそれぞれのマニホールドを構成するものであり、水素ガス，酸化剤ガス及び冷却水の３つの流体の入口部と出口部に相当し、したがって全部で６個形成してある。   Each of these gaskets 3 and 5 is trim-molded into the shape shown in FIG. That is, each of the gaskets 3 and 5 has an outer shape of, for example, a rectangular shape, and the central portions are cut out so as to leave the frame-shaped outer peripheral portions 3a and 5a, thereby forming rectangular electrode forming regions 3b and 5b. , 5b, a plurality of through holes 3c, 5c are formed. The plurality of through holes 3c and 5c constitute manifolds for hydrogen gas, oxidant gas, and cooling water, and are provided at the inlet and outlet of three fluids of hydrogen gas, oxidant gas, and cooling water. Therefore, a total of six are formed.

ここで、本実施形態では、図４（ｂ）に拡大して示すように、各ガスケット３，５における外周部３ａ，５ａの内周縁３ｄ，５ｄを、内周縁３ｄ，５ｄに沿って波形の凹凸形状としている。なお、各ガスケット３，５は、厚さが２０μｍのＰＥＮ（ポリエチレンナフタレート）製で、電解質膜１に接合する側の面にあらかじめ厚さ１０μｍの粘着剤を塗布してある。   Here, in the present embodiment, as shown in an enlarged view in FIG. 4B, the inner peripheral edges 3d and 5d of the outer peripheral portions 3a and 5a of the gaskets 3 and 5 are corrugated along the inner peripheral edges 3d and 5d. It has an uneven shape. Each of the gaskets 3 and 5 is made of PEN (polyethylene naphthalate) having a thickness of 20 μm, and a pressure-sensitive adhesive having a thickness of 10 μm is previously applied to the surface to be joined to the electrolyte membrane 1.

図１（ａ）及び図２（ａ）に示すように、アノード側，カソード側の各ガスケット３，５の上記粘着剤を塗布した側と反対側の面には、厚さ７５μｍのマスキングフィルム本体９，１１を、厚さ１μｍの接着層のタック性接着剤でそれぞれ接着している。なお、この接着状態は、後述するようにマスキングフィルム本体９，１１を各ガスケット３，５から引き剥がす必要があるので、容易に引き剥がすことができるようにしてある。また、これらマスキングフィルム本体９，１１は、各ガスケット３，５の前記図４（ａ）に示した電極形成領域３ｂ，５ｂの外形とほぼ整合する長方形状の開口部９ａ，１１ａを備えている。   As shown in FIG. 1 (a) and FIG. 2 (a), the masking film main body having a thickness of 75 μm is formed on the surface of each of the gaskets 3 and 5 on the anode side and the cathode side opposite to the side where the adhesive is applied. 9 and 11 are bonded to each other with a tacky adhesive of an adhesive layer having a thickness of 1 μm. In addition, since it is necessary to peel off the masking film main bodies 9 and 11 from the gaskets 3 and 5 as will be described later, this adhesion state can be easily peeled off. The masking film bodies 9 and 11 are provided with rectangular openings 9a and 11a that substantially match the outer shapes of the electrode forming regions 3b and 5b shown in FIG. 4A of the gaskets 3 and 5, respectively. .

上記図１（ａ）のアノードガスケット３とマスキングフィルム本体９とでアノード側の二層のマスキングフィルム１３を構成し、上記図２（ａ）のカソードガスケット５とマスキングフィルム本体１１とでカソード側の二層のマスキングフィルム１５を構成している。   The anode gasket 3 and the masking film body 9 in FIG. 1A constitute a two-layer masking film 13 on the anode side, and the cathode gasket 5 and the masking film body 11 in FIG. A two-layer masking film 15 is formed.

次に、図１のアノード側について説明する。図１（ｂ）に示すように、電解質膜１の一方の面に、二層のマスキングフィルム１３を、アノードガスケット３が電解質膜１側となるようにして接合する。また、電解質膜１の他方の面には補強用シートとしてのバックシート１７を接合する。このバックシート１７は、低熱収縮ＰＥＴフィルム（厚さ１００μｍ〜３００μｍ）と、再剥離耐熱粘着層（厚さ５μｍ）と、低熱収縮極薄ＰＥＴフィルム（厚さ１２μｍ）とからなる（例えば、商品名：パナプロテクトＥＴ、パナック株式会社製が適用材料）。   Next, the anode side in FIG. 1 will be described. As shown in FIG. 1B, a two-layer masking film 13 is joined to one surface of the electrolyte membrane 1 so that the anode gasket 3 is on the electrolyte membrane 1 side. A back sheet 17 as a reinforcing sheet is joined to the other surface of the electrolyte membrane 1. The back sheet 17 is composed of a low heat shrink PET film (thickness 100 μm to 300 μm), a re-peeling heat-resistant adhesive layer (thickness 5 μm), and a low heat shrink ultrathin PET film (thickness 12 μm) (for example, trade name) : Panaprotect ET, manufactured by Panac Co., Ltd.)

そして、上記図１（ｂ）のように電解質膜１を中心としてその両側に二層のマスキングフィルム１３とアノードガスケット３とをそれぞれ接合した状態で、加熱プレスかあるいはホットローラにて両側から加熱・加圧してこれらを接合する。   Then, as shown in FIG. 1 (b), with the electrolyte membrane 1 as the center, the two-layer masking film 13 and the anode gasket 3 are joined to both sides, respectively, and heated and heated from both sides with a hot press or hot roller. These are joined by applying pressure.

その後、図１（ｃ）に示すように、マスキングフィルム１３（マスキングフィルム本体９）上から触媒ペーストを塗布する。このとき、アノードガスケット３の電極形成領域３ｂに対応する位置の電解質膜１上に、触媒ペーストを塗布して電極触媒層であるアノード触媒層１９を形成するが、マスキングフィルム本体９の開口部９ａの周縁の上面にも触媒ペーストの一部が塗布されて余剰ペースト２１が形成される。
この余剰ペースト２１と電解質膜１上の触媒ペースト（アノード触媒層１９）との間は、二層構造のマスキングフィルム１３（マスキングフィルム本体９及びアノードガスケット３）によって比較的大きな段差が形成されるので、これら両者は連続せずに互いに離間した状態となりやすい。 Then, as shown in FIG.1 (c), a catalyst paste is apply | coated from on the masking film 13 (masking film main body 9). At this time, a catalyst paste is applied on the electrolyte membrane 1 at a position corresponding to the electrode formation region 3b of the anode gasket 3 to form an anode catalyst layer 19 as an electrode catalyst layer. A part of the catalyst paste is also applied to the upper surface of the peripheral edge of the substrate to form an excess paste 21.
A relatively large step is formed between the surplus paste 21 and the catalyst paste (anode catalyst layer 19) on the electrolyte membrane 1 by the masking film 13 (masking film body 9 and anode gasket 3) having a two-layer structure. Both of these tend to be separated from each other without being continuous.

次に、図１（ｄ）のように、マスキングフィルム本体９をアノードガスケット３から引き剥がす。これにより、電解質膜１の一方の面にアノード触媒層１９を形成するとともに、その周囲の電解質膜１上にアノードガスケット３を設けたことになり、アノード側の電極触媒層の形成作業が終了する。   Next, as shown in FIG. 1 (d), the masking film body 9 is peeled off from the anode gasket 3. Thus, the anode catalyst layer 19 is formed on one surface of the electrolyte membrane 1, and the anode gasket 3 is provided on the surrounding electrolyte membrane 1, so that the operation of forming the electrode catalyst layer on the anode side is completed. .

次に、図２のカソード側について説明する。まず、図２（ｂ）に示すように、前記図１（ｄ）のマスキングフィルム本体９を引き剥がした状態から、この引き剥がした側に補強用凸状シートとしての凸状バックシート２３を接合する。この凸状バックシート２３は、アノードガスケット３の電極形成領域３ｂに入り込む凸部２３ａを有しており、アノードガスケット３の前記図１に示したバックシート１７と同一材質かつ同一厚さ（凸部２３ａを含まない厚さ）でよい。   Next, the cathode side in FIG. 2 will be described. First, as shown in FIG. 2B, from the state in which the masking film main body 9 in FIG. 1D is peeled off, a convex back sheet 23 as a reinforcing convex sheet is joined to the peeled side. To do. This convex backsheet 23 has a convex portion 23a that enters the electrode forming region 3b of the anode gasket 3, and is the same material and the same thickness (convex portion) as the backsheet 17 shown in FIG. The thickness does not include 23a.

その後、図２（ｃ）に示すように、バックシート１７を電解質膜１から引き剥がし、この引き剥がした側の電解質膜１の表面に、図２（ａ）に示してある二層のマスキングフィルム１５を、図２（ｄ）のようにカソードガスケット５が電解質膜１側となるように接合する。このとき、加熱プレスかあるいはホットローラにて両側から加熱・加圧してこれらを接合する。   Thereafter, as shown in FIG. 2 (c), the back sheet 17 is peeled off from the electrolyte membrane 1, and the two-layer masking film shown in FIG. 2 (a) is formed on the surface of the electrolyte membrane 1 on the peeled side. 15 is joined so that the cathode gasket 5 is on the electrolyte membrane 1 side as shown in FIG. At this time, they are heated and pressed from both sides with a hot press or a hot roller to join them.

続いて、図２（ｅ）に示すように、マスキングフィルム１５（マスキングフィルム本体１１）上から触媒ペーストを塗布する。このとき、カソードガスケット５の電極形成領域５ｂに対応する位置の電解質膜１上に、触媒ペーストを塗布して電極触媒層であるカソード触媒層２５を形成するが、マスキングフィルム本体１１の開口部１１ａの周縁の上面にも触媒ペーストが塗布されて余剰ペースト２７が形成される。   Then, as shown in FIG.2 (e), a catalyst paste is apply | coated from on the masking film 15 (masking film main body 11). At this time, a catalyst paste is applied on the electrolyte membrane 1 at a position corresponding to the electrode formation region 5b of the cathode gasket 5 to form the cathode catalyst layer 25 as an electrode catalyst layer. A surplus paste 27 is formed by applying the catalyst paste to the upper surface of the periphery of the substrate.

この余剰ペースト２７と電解質膜１上の触媒ペースト（カソード触媒層２５）との間は、二層構造のマスキングフィルム１５（マスキングフィルム本体１１及びカソードガスケット５）によって比較的大きな段差が形成されるので、これら両者は連続せずに互いに離間した状態となりやすい。   A relatively large step is formed between the surplus paste 27 and the catalyst paste (cathode catalyst layer 25) on the electrolyte membrane 1 by the masking film 15 (masking film body 11 and cathode gasket 5) having a two-layer structure. Both of these tend to be separated from each other without being continuous.

次に、図２（ｅ）の状態から、バックシート２３をアノードガスケット３及び電解質膜１から引き剥がすとともに、マスキングフィルム本体１１をカソードガスケット５から引き剥がし、さらに規定の製品長さにカットすることで、前記図３(ａ)に示した積層体７が完成する。   Next, from the state of FIG. 2 (e), the back sheet 23 is peeled off from the anode gasket 3 and the electrolyte membrane 1, and the masking film body 11 is peeled off from the cathode gasket 5 and further cut to a specified product length. Thus, the laminate 7 shown in FIG. 3A is completed.

この積層体７は、図３（ｂ）に示すように、アノードガスケット３及びカソードガスケット５の外側にキャリアシールと呼ばれる支持部材２９，３１を配置し、さらにアノード触媒層１９及びカソード触媒層２５上にガス拡散層となるＧＤＬ３３，３５を配置する。これにより、燃料電池用ＭＥＡ（膜電極接合体）３６が完成する。   As shown in FIG. 3 (b), the laminate 7 has support members 29 and 31 called carrier seals arranged outside the anode gasket 3 and the cathode gasket 5, and further on the anode catalyst layer 19 and the cathode catalyst layer 25. GDLs 33 and 35 to be gas diffusion layers are disposed in Thereby, the fuel cell MEA (membrane electrode assembly) 36 is completed.

上記したように本実施形態では、図１（ｃ）の状態からマスキングフィルム本体９を引き剥がす際に、マスキングフィルム本体９上の余剰ペースト２１は、アノード触媒層１９との間に、マスキングフィルム本体９及びアノードガスケット３による段差が形成されている。このため、余剰ペースト２１とアノード触媒層１９とは、連続せずに互いに離間した状態となりやすい。したがって、この離間状態でマスキングフィルム本体９をアノードガスケット３から引き剥がしても、アノード触媒層１９が一緒に剥がれることを抑制でき、電解質膜１の一方の面に電極（アノード）を形成する際の電極品質の低下を抑えることができる。   As described above, in this embodiment, when the masking film main body 9 is peeled off from the state of FIG. 1C, the surplus paste 21 on the masking film main body 9 is between the anode catalyst layer 19 and the masking film main body 19. 9 and a step due to the anode gasket 3 are formed. For this reason, the excess paste 21 and the anode catalyst layer 19 are likely to be separated from each other without being continuous. Therefore, even if the masking film main body 9 is peeled off from the anode gasket 3 in this separated state, the anode catalyst layer 19 can be prevented from being peeled off together, and an electrode (anode) can be formed on one surface of the electrolyte membrane 1. A decrease in electrode quality can be suppressed.

同様にして、図２（ｅ）の状態からマスキングフィルム本体１１を引き剥がす際に、マスキングフィルム本体１１上の余剰ペースト２７は、カソード触媒層２５との間に、マスキングフィルム本体１１及びカソードガスケット５による段差が形成されているので、これら両者は連続せずに互いに離間した状態となりやすい。したがって、この離間状態でマスキングフィルム本体１１をアノードガスケット５から引き剥がしても、カソード触媒層２５が一緒に剥がれることを抑制でき、電解質膜１の他方の表面に電極（カソード）を形成する際の電極品質の低下を抑えることができる。   Similarly, when the masking film body 11 is peeled off from the state of FIG. 2 (e), the surplus paste 27 on the masking film body 11 is between the cathode catalyst layer 25 and the masking film body 11 and the cathode gasket 5. Therefore, the two are not continuous and are likely to be separated from each other. Therefore, even if the masking film body 11 is peeled off from the anode gasket 5 in this separated state, it is possible to prevent the cathode catalyst layer 25 from being peeled off together, and when forming the electrode (cathode) on the other surface of the electrolyte membrane 1. A decrease in electrode quality can be suppressed.

また、本実施形態で製造した積層体７は、二層構造としたマスキングフィルム１３（１５）のうちシール材用フィルム３（５）が電解質膜１の周縁に残り、これがシール材となるので、後工程でのシール材を設ける工程を省略でき、製造工程を簡略化することができる。
また、図１（ｂ）の状態でアノード側の触媒ペーストを塗布するときには、補強用のバックシート１７を塗布側と反対側に設けてあるので、電解質膜１の皺発生を抑制でき、塗布作業の効率化及び積層体７の高品質化を達成することができる。 Moreover, since the laminated body 7 manufactured in the present embodiment has a two-layered masking film 13 (15), the sealing material film 3 (5) remains on the periphery of the electrolyte membrane 1, and this serves as a sealing material. A process of providing a sealing material in a post process can be omitted, and the manufacturing process can be simplified.
Further, when the anode side catalyst paste is applied in the state of FIG. 1B, the reinforcing back sheet 17 is provided on the side opposite to the application side, so that generation of wrinkles in the electrolyte membrane 1 can be suppressed, and the application work It is possible to achieve higher efficiency and higher quality of the laminate 7.

同様にして、図２（ｄ）の状態でカソード側の触媒ペーストを塗布するときには、補強用の凸状バックシート２３を塗布側と反対側に設けてあるので、電解質膜１の皺発生を抑制でき、塗布作業の効率化及び積層体７の高品質化を達成することができる。このとき、凸状バックシート２３は、アノード触媒層１９に接触するようにアノードガスケット３の電極形成領域３ｂ内に向けて突出する凸部２３ａを備えているので、アノードガスケット３を設けた後であっても、補強用シートとしての機能を発揮でき、電解質膜１の皺発生を抑制できる。   Similarly, when the cathode-side catalyst paste is applied in the state of FIG. 2D, the reinforcing convex back sheet 23 is provided on the side opposite to the application side, so that generation of wrinkles on the electrolyte membrane 1 is suppressed. In addition, the efficiency of the coating operation and the high quality of the laminate 7 can be achieved. At this time, since the convex backsheet 23 includes the convex portion 23a that protrudes into the electrode forming region 3b of the anode gasket 3 so as to be in contact with the anode catalyst layer 19, after the anode gasket 3 is provided, Even if it exists, the function as a sheet | seat for reinforcement can be exhibited and generation | occurrence | production of the flaw of the electrolyte membrane 1 can be suppressed.

このように、本実施形態では、アノード側の電極を形成するときの触媒ペースト塗布時であっても、またアノード側の電極形成後のカソード側の電極を形成するときの触媒ペースト塗布時であっても、厚さが１００μｍ〜３００μｍのバックシート１７もしくは凸状バックシート２３を備えている。このため、電解質膜１や電解質膜１に接合してあるガスケット３，５などを含む接合体の皴やうねり、変形を抑制でき、高品質な積層体７を製造することができる。   Thus, in this embodiment, even when the catalyst paste is applied when forming the anode side electrode, it is also when the catalyst paste is applied when forming the cathode side electrode after forming the anode side electrode. However, the back sheet 17 or the convex back sheet 23 having a thickness of 100 μm to 300 μm is provided. For this reason, it is possible to suppress wrinkling, undulation, and deformation of the joined body including the electrolyte membrane 1 and the gaskets 3 and 5 joined to the electrolyte membrane 1, and the high-quality laminate 7 can be manufactured.

また、本実施形態では、図４（ｂ）に示したように、各ガスケット３，５における電極形成領域３ｂ，５ｂの外側の外周部３ａ，５ａの内周縁３ｄ，５ｄを波形の凹凸形状としているので、内周縁３ｄ，５ｄの周長が、直線状とした場合に比較して長くなる。
例えば、波形状を、半円形状を繰り返す形状とすれば、直線状とした場合に対し１．５７（π／２）倍長くなる。これにより、圧縮された状態の各ガスケット３，５における内周縁３ｄ，５ｄの電解質膜１に作用する荷重が分散され、直線状とした場合に比較して１／１．５７に荷重が減少する。この結果、内周縁３ｄ，５ｄの電解質膜１への食い込み量が低減するので、電解質膜１の部分的な薄肉化を抑制できて、電解質膜１の強度低下を抑制することができ、高品質な燃料電池用ＭＥＡ３６ひいては燃料電池を製造することが可能となる。 In the present embodiment, as shown in FIG. 4B, the inner peripheral edges 3d and 5d of the outer peripheral portions 3a and 5a outside the electrode forming regions 3b and 5b in the gaskets 3 and 5 are formed into corrugated irregular shapes. As a result, the peripheral lengths of the inner peripheral edges 3d and 5d are longer than in the case where they are linear.
For example, if the wave shape is a shape that repeats a semicircular shape, the wave shape is 1.57 (π / 2) times longer than a straight shape. As a result, the load acting on the electrolyte membrane 1 on the inner peripheral edges 3d and 5d in the compressed gaskets 3 and 5 is dispersed, and the load is reduced to 1 / 1.57 as compared with the case where the gaskets are linear. . As a result, the amount of penetration of the inner peripheral edges 3d and 5d into the electrolyte membrane 1 is reduced, so that partial thinning of the electrolyte membrane 1 can be suppressed, and the strength reduction of the electrolyte membrane 1 can be suppressed. Thus, it becomes possible to manufacture a fuel cell MEA 36 and thus a fuel cell.

また、燃料電池の運転時に、アノード，カソード間での差圧によるストレスが加わりやすい反応ガスの入口部，出口部（例えば図４（ａ）のＡ部，Ｂ部）付近や、運転時に温度の上がりやすい反応面中央に対応する部位（例えば図４（ａ）のＣ部，Ｄ部）付近については、他の部位よりも波形状を細かく形成して、周長をより長くしてもよい。これにより、上記ストレスが加わりやすい部位での荷重をより分散でき、各ガスケット３，５における内周縁３ｄ，５ｄの電解質膜１への食い込み量をより低減することができる。   In addition, during operation of the fuel cell, the reaction gas is likely to be stressed due to the pressure difference between the anode and the cathode. In the vicinity of the inlet and outlet of the reaction gas (for example, A and B in FIG. 4A), In the vicinity of the part corresponding to the center of the reaction surface that is likely to rise (for example, part C and part D in FIG. 4A), the peripheral length may be made longer by forming the wave shape finer than other parts. Thereby, the load in the part where the stress is easily applied can be further dispersed, and the amount of biting into the electrolyte membrane 1 of the inner peripheral edges 3d and 5d in the gaskets 3 and 5 can be further reduced.

また、上記図４（ａ）のＡ部，Ｂ部で示す反応ガスの入口部，出口部付近や、図４（ａ）のＣ部，Ｄ部で示す反応面中央に対応する部位付近のみに、凹凸形状を設定してもよい。これにより、特にストレスが加わりやすい部位での荷重を分散でき、各ガスケット３，５における特にストレスが加わりやすい部位での内周縁３ｄ，５ｄの電解質膜１への食い込み量を低減することができる。   Further, only in the vicinity of the reaction gas inlet and outlet portions shown by the A and B portions in FIG. 4A and near the site corresponding to the reaction surface center shown by the C and D portions in FIG. The uneven shape may be set. Thereby, it is possible to disperse the load at a portion where stress is particularly likely to be applied, and to reduce the amount of biting into the electrolyte membrane 1 of the inner peripheral edges 3d and 5d at the portion where stress is particularly likely to be applied.

なお、上記した波形状の凹凸形状に代えて、矩形や鋸歯などの凹凸形状により内周縁３ｄ，５ｄの周長を長くしてもよい。   In addition, instead of the above-described wave-shaped uneven shape, the peripheral lengths of the inner peripheral edges 3d and 5d may be increased by an uneven shape such as a rectangle or a sawtooth.

また、図５に示すように、各ガスケット３，５の内周縁３ｄ，５ｄを円弧形状とすることで、内周縁３ｄ，５ｄの電解質膜１への食い込み量を低減させて、電解質膜１の強度低下を抑制することもできる。この際、図５（ａ）に示すレーザ加工ヘッド３７から照射するレーザ光３９や、図５（ｂ）に示す熱板あるいは熱線などの発熱源４１からの放射熱４３によって内周縁３ｄ，５ｄを溶融させることで、溶融表面を表面張力によりＲ形状（円弧形状）とすることができる。   Further, as shown in FIG. 5, the inner peripheral edges 3d and 5d of the gaskets 3 and 5 are formed in an arc shape, so that the amount of biting into the electrolyte film 1 by the inner peripheral edges 3d and 5d can be reduced. Strength reduction can also be suppressed. At this time, the inner peripheral edges 3d and 5d are moved by the laser light 39 irradiated from the laser processing head 37 shown in FIG. 5A and the radiant heat 43 from the heat source 41 such as a hot plate or a heat ray shown in FIG. 5B. By melting, the molten surface can be made into an R shape (arc shape) by surface tension.

なお、上記図５に示した内周縁３ｄ，５ｄの円弧形状は、少なくとも電解質膜１に接触する側のみ形成するようにしてもよい。また、上記円弧形状と、前記図４(ｂ)に示した凹凸形状を組み合わせてもよい。   The arc shape of the inner peripheral edges 3d and 5d shown in FIG. 5 may be formed only at least on the side in contact with the electrolyte membrane 1. Moreover, you may combine the said circular arc shape and the uneven | corrugated shape shown in the said FIG.4 (b).

次に、前記図３（ａ）に示した積層体７の製造工程ついて図６の簡略化した製造装置を用いて説明する。図１（ａ）に示すアノード側の二層のマスキングフィルム１３を構成するマスキングフィルム本体９はフィルム供給部４５から供給されて、その下流のカット手段４７により、中央部分を切り抜くようにカットして開口部９ａを形成すべくトリム成形する。一方、二層のマスキングフィルム１３におけるアノードガスケット３は、ガスケット供給部４９から供給されて、その下流のカット手段５１により、図４（ａ）のように電極形成領域３ｂ及び貫通孔３ｃを形成すべくトリム成形する。   Next, the manufacturing process of the laminate 7 shown in FIG. 3A will be described using the simplified manufacturing apparatus of FIG. The masking film main body 9 constituting the two-layer masking film 13 on the anode side shown in FIG. 1 (a) is supplied from the film supply unit 45 and cut by the cutting means 47 downstream thereof so as to cut out the central portion. Trim forming to form the opening 9a. On the other hand, the anode gasket 3 in the two-layer masking film 13 is supplied from the gasket supply section 49, and the electrode forming region 3b and the through hole 3c are formed by the cutting means 51 downstream thereof as shown in FIG. Trim as much as possible.

なお、カット手段４７，５１としては、本実施形態ではトムソン刃を用いて打ち抜くが、これに限ることはなく、例えばレーザ加工によって切断してもよい。   In this embodiment, the cutting means 47 and 51 are punched using a Thomson blade. However, the cutting means 47 and 51 is not limited to this, and may be cut by laser processing, for example.

上記それぞれトリム成形したマスキングフィルム本体９とアノードガスケット３は、図示しない接着剤塗布手段によって塗布したタック性接着剤により互いに接着し一体化して二層のマスキングフィルム１３とする。そしてこの二層のマスキングフィルム１３と、膜供給部５３から供給する電解質膜１と、バックシート供給部５５から供給するバックシート１７とを、その下流側のホットローラなどの圧着手段５７によって互いに加圧接合する（図１（ｂ））。   The trimmed masking film body 9 and the anode gasket 3 are bonded and integrated with each other by a tacky adhesive applied by an adhesive application means (not shown) to form a two-layer masking film 13. The two-layer masking film 13, the electrolyte membrane 1 supplied from the membrane supply unit 53, and the backsheet 17 supplied from the backsheet supply unit 55 are added to each other by a pressing means 57 such as a hot roller on the downstream side. Pressure bonding is performed (FIG. 1B).

上記圧着手段５７の下流の塗工手段５９では、電解質膜１上に触媒ペーストを塗布してアノード触媒層１９を形成し（図１（ｃ））、その後、ヒータなどの乾燥手段６１によって塗布した触媒ペーストを乾燥させる。乾燥後は、剥離手段６３によってマスキングフィルム本体９をアノードガスケット３から引き剥がし（図１（ｄ））、引き剥がしたマスキングフィルム本体９はローラ６５に巻き取る。   In the coating means 59 downstream of the pressure-bonding means 57, a catalyst paste is applied on the electrolyte membrane 1 to form the anode catalyst layer 19 (FIG. 1 (c)), and then applied by a drying means 61 such as a heater. Dry the catalyst paste. After drying, the masking film main body 9 is peeled off from the anode gasket 3 by the peeling means 63 (FIG. 1 (d)), and the peeled masking film main body 9 is wound around a roller 65.

続いて、その下流側で、バックシート供給手段６７から凸状バックシート２３を供給し、この凸状バックシート２３を上流側から送られてくるアノードガスケット３及びアノード触媒層１９上に接合し（図２（ｂ））、その後、剥離手段６９によってバックシート１７を電解質膜１から引き剥がし（図２（ｃ））、引き剥がした電解質膜１はローラ７１に巻き取る。   Subsequently, on the downstream side, the convex backsheet 23 is supplied from the backsheet supply means 67, and the convex backsheet 23 is joined onto the anode gasket 3 and the anode catalyst layer 19 sent from the upstream side ( After that, the back sheet 17 is peeled off from the electrolyte membrane 1 by the peeling means 69 (FIG. 2C), and the peeled electrolyte membrane 1 is wound around the roller 71.

さらに、その下流側では、カソード側の二層のマスキングフィルム１５を構成するマスキングフィルム本体１１がフィルム供給部７３から供給されて、その下流の前記カット手段４７と同様のカット手段７５により、中央部分を切り抜くようにカットして開口部１１ａを形成すべくトリム成形する。一方、二層のマスキングフィルム１５におけるカソードガスケット５は、ガスケット供給部７７から供給されて、その下流の前記カット手段５１と同様のカット手段７９により、図４（ａ）のように電極形成領域５ｂ及び貫通孔５ｃを形成すべくトリム成形する。   Further, on the downstream side, the masking film body 11 constituting the two-layer masking film 15 on the cathode side is supplied from the film supply unit 73, and the central portion is cut by the cutting means 75 similar to the cutting means 47 on the downstream side. Is trimmed to form an opening 11a. On the other hand, the cathode gasket 5 in the two-layer masking film 15 is supplied from the gasket supply section 77 and is cut by the same cutting means 79 as the cutting means 51 downstream thereof as shown in FIG. And trim forming to form the through holes 5c.

上記それぞれトリム成形したマスキングフィルム本体１１とカソードガスケット５は、図示しない接着剤塗布手段によって塗布したタック性接着剤によって互いに接着して一体化して二層のマスキングフィルム１５とする。そしてこの二層のマスキングフィルム１５を、上記バックシート１７を剥がした電解質膜１上に供給し、これらを前記したアノードガスケット３及び凸状バックシート２３とともにホットローラなどの圧着手段８１によって加圧接合する（図２（ｄ））。   The mask film body 11 and the cathode gasket 5 that have been trim-molded are bonded and integrated with each other by a tacky adhesive applied by an adhesive application means (not shown) to form a two-layer masking film 15. Then, this two-layer masking film 15 is supplied onto the electrolyte membrane 1 from which the back sheet 17 has been peeled off, and these are pressure-bonded together with the above-described anode gasket 3 and convex back sheet 23 by means of pressure bonding means 81 such as a hot roller. (FIG. 2D).

上記圧着手段８１の下流の塗工手段８３では、電解質膜１上に触媒ペーストを塗布してカソード触媒層２５を形成し（図２（ｅ））、その後、ヒータなどの乾燥手段８５によって塗布した触媒ペーストを乾燥させる。乾燥後は、剥離手段８７によってマスキングフィルム本体１１及び凸状バックシート２３を引き剥がし、これら引き剥がしたマスキングフィルム本体１１及び凸状バックシート２３はローラ８９及び９１にそれぞれ巻き取る。   In the coating means 83 downstream of the pressure bonding means 81, a catalyst paste is applied on the electrolyte membrane 1 to form the cathode catalyst layer 25 (FIG. 2 (e)), and then applied by a drying means 85 such as a heater. Dry the catalyst paste. After drying, the masking film main body 11 and the convex back sheet 23 are peeled off by the peeling means 87, and the masking film main body 11 and the convex back sheet 23 thus peeled off are wound around rollers 89 and 91, respectively.

なお、前記した塗工手段５９，８３としては、スプレー，ダイコータ，スクリーン印刷、バーコータなど特に限定するものではない。   The coating means 59 and 83 are not particularly limited, such as spray, die coater, screen printing, and bar coater.

上記マスキングフィルム本体１１及び凸状バックシート２３を引き剥がした後の電解質膜１とその両側のガスケット３，５とからなる三層の連続した帯状積層体は、剥離手段８７の下流側のトリミング手段９３によって規定の大きさ（長さ）にカットして前記図３（ａ）に示した積層体７とする。   A three-layer continuous strip-shaped laminate composed of the electrolyte membrane 1 after peeling off the masking film body 11 and the convex back sheet 23 and the gaskets 3 and 5 on both sides thereof is trimmed on the downstream side of the peeling means 87. The laminated body 7 shown in FIG. 3A is cut into a predetermined size (length) by 93.

なお、上記実施形態では、アノード電極層１９を先に形成しているが、カソード電極層２５を先に形成するようにしてもよい。   In the above embodiment, the anode electrode layer 19 is formed first, but the cathode electrode layer 25 may be formed first.

本発明の一実施形態に係わる燃料電池電極（アノード側）の製造方法を示す模式図である。It is a schematic diagram which shows the manufacturing method of the fuel cell electrode (anode side) concerning one Embodiment of this invention. 本発明の一実施形態に係わる燃料電池電極（カソード側）の製造方法を示す模式図である。It is a schematic diagram which shows the manufacturing method of the fuel cell electrode (cathode side) concerning one Embodiment of this invention. (ａ)は図１，２の製造方法によって製造した積層体の断面図、（ｂ）は（ａ）の積層体を基に製造した燃料電池用ＭＥＡの断面図である。(a) is sectional drawing of the laminated body manufactured by the manufacturing method of FIG.1, 2, (b) is sectional drawing of MEA for fuel cells manufactured based on the laminated body of (a). （ａ）は図３(ａ)におけるガスケットの平面図、（ｂ）は（ａ）のガスケット内周縁の形状を拡大して示す平面図である。(A) is a top view of the gasket in Fig.3 (a), (b) is a top view which expands and shows the shape of the gasket inner periphery of (a). ガスケットの内周縁を円弧形状とする断面図で、（ａ）はレーザ加工によるもの、（ｂ）は発熱源によるものである。It is sectional drawing which makes the inner periphery of a gasket circular arc shape, (a) is based on laser processing, (b) is based on a heat-generation source. 図３（ａ）の積層体を製造するための製造工程図である。It is a manufacturing-process figure for manufacturing the laminated body of Fig.3 (a).

符号の説明Explanation of symbols

１ 固体高分子電解質膜（電解質膜）
３ アノードガスケット（シール材用フィルム）
３ｄ アノードガスケットの内周縁
５ カソードガスケット（シール材用フィルム）
５ｄ カソードスケットの内周縁
９，１１ マスキングフィルム本体
１３，１５ 二層構造のマスキングフィルム
１７ バックシート（補強用シート）
１９ アノード触媒層（電極触媒層）
２３ 凸状バックシート（補強用凸状シート）
２５ カソード触媒層（電極触媒層） 1 Solid polymer electrolyte membrane (electrolyte membrane)
3 Anode gasket (film for sealing material)
3d Inner peripheral edge of anode gasket 5 Cathode gasket (film for sealing material)
5d Inner peripheral edge of cathode sket 9,11 Masking film body 13,15 Double layer masking film 17 Back sheet (reinforcing sheet)
19 Anode catalyst layer (electrode catalyst layer)
23 Convex Back Sheet (Convex Convex Sheet)
25 Cathode catalyst layer (electrode catalyst layer)

Claims (6)

電解質膜の表面に電極触媒層を形成する燃料電池電極積層体の製造方法において、前記電解質膜の表面に、外周部を残して中央部分が切り抜かれた二層構造のマスキングフィルムを設け、この二層構造のマスキングフィルムは、前記電解質膜の外周部の表面に接合されるシール材用フィルムと、このシール材用フィルムに対し前記電解質膜と反対側に接合されるマスキングフィルム本体とを有し、前記二層構造のマスキングフィルムの上から前記電解質膜上に前記電極触媒層となる触媒ペーストを塗布した後、前記マスキングフィルム本体を前記シール材用フィルムから剥がすことを特徴とする燃料電池電極積層体の製造方法。   In the method of manufacturing a fuel cell electrode laminate in which an electrode catalyst layer is formed on the surface of an electrolyte membrane, a masking film having a two-layer structure in which a central portion is cut out except for an outer peripheral portion is provided on the surface of the electrolyte membrane. The masking film having a layer structure has a sealing material film bonded to the surface of the outer peripheral portion of the electrolyte membrane, and a masking film body bonded to the opposite side of the electrolyte membrane with respect to the sealing material film, A fuel cell electrode laminate comprising: a catalyst paste serving as the electrode catalyst layer is applied on the electrolyte membrane from above the two-layer masking film, and then the masking film body is peeled off from the sealing material film. Manufacturing method. 前記電解質膜を間に挟んで前記二層構造のマスキングフィルムと反対側に補強用シートを設け、この補強用シートを設けた状態で前記触媒ペーストを塗布することを特徴とする請求項１に記載の燃料電池電極積層体の製造方法。   The reinforcing paste is provided on the opposite side to the masking film having the two-layer structure with the electrolyte membrane interposed therebetween, and the catalyst paste is applied in a state where the reinforcing sheet is provided. Manufacturing method of the fuel cell electrode laminate. 前記電解質膜の一方の面に前記二層構造のマスキングフィルムを設けるとともに、前記電解質膜を間に挟んで前記二層構造のマスキングフィルムと反対側に前記補強用シートを設け、前記二層構造のマスキングフィルムの上から前記電解質膜の一方の面に、前記電極触媒層としてアノード触媒層とカソード触媒層とのいずれか一方となる触媒ペーストを塗布した後、前記マスキングフィルム本体を前記シール材用フィルムから剥がし、このシール材用フィルム側に、前記切り抜かれた中央部分に対応する凸部を備える補強用凸状シートを設け、前記補強用シートを前記電解質膜から剥がした後、この剥がした後の前記電解質膜の他方の面に、前記二層構造のマスキングフィルムとは別の二層構造のマスキングフィルムを設け、この二層構造のマスキングフィルムの上から前記電解質膜の他方の面に、前記アノード触媒層とカソード触媒層とのいずれか他方となる触媒ペーストを塗布した後、前記マスキングフィルム本体を前記シール材用フィルムから剥がすとともに、前記補強用凸状シートを前記シール材用フィルム及び、前記アノード触媒層とカソード触媒層とのいずれか一方から剥がすことを特徴とする請求項１または２に記載の燃料電池電極積層体の製造方法。   The two-layered masking film is provided on one surface of the electrolyte membrane, and the reinforcing sheet is provided on the opposite side of the two-layered masking film with the electrolyte membrane interposed therebetween. After applying a catalyst paste serving as either the anode catalyst layer or the cathode catalyst layer as the electrode catalyst layer on one surface of the electrolyte membrane from above the masking film, the masking film body is attached to the sealing material film. The reinforcing sheet is provided with a convex portion corresponding to the cut-out central portion on the sealing material film side, and the reinforcing sheet is peeled off from the electrolyte membrane and then peeled off. A masking film having a two-layer structure different from the masking film having the two-layer structure is provided on the other surface of the electrolyte membrane. After applying a catalyst paste which is either the anode catalyst layer or the cathode catalyst layer to the other surface of the electrolyte membrane from above the king film, the masking film body is peeled off from the sealing material film 3. The fuel cell electrode laminate according to claim 1, wherein the reinforcing convex sheet is peeled off from one of the sealing material film and the anode catalyst layer and the cathode catalyst layer. 4. Method. 前記二層構造のマスキングフィルムのシール材用フィルムは、前記中央部分が切り抜かれた後の内周縁の少なくとも前記電解質膜に接触する側が、該内周縁に沿って凹凸形状とされていることを特徴とする請求項１ないし３のいずれか１項に記載の燃料電池電極積層体の製造方法。   The film for a sealing material of the two-layer masking film is characterized in that at least the side of the inner peripheral edge after the central portion that is cut out contacts with the electrolyte membrane has an uneven shape along the inner peripheral edge. The method for producing a fuel cell electrode laminate according to any one of claims 1 to 3. 前記凹凸形状は、前記シール材用フィルムをシール材として燃料電池に組み込んだときの反応ガスの前記電極触媒層に対する入口部近傍及び出口部近傍に設定してあることを特徴とする請求項４項に記載の燃料電池電極積層体の製造方法。 5. The uneven shape is set in the vicinity of an inlet portion and an outlet portion of a reaction gas with respect to the electrode catalyst layer when the sealing material film is incorporated in a fuel cell as a sealing material. The manufacturing method of the fuel cell electrode laminated body of description. 前記シール材用フィルムの内周縁の少なくとも前記電解質膜に接触する側の縁部が凸の曲面形状とされていることを特徴とする請求項１ないし５のいずれか１項に記載の燃料電池電極積層体の製造方法。   6. The fuel cell electrode according to claim 1, wherein at least an edge of an inner peripheral edge of the sealing material film that contacts the electrolyte membrane has a convex curved shape. A manufacturing method of a layered product.
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