JP2006339062A - Manufacturing method for electrode structure for fuel cell - Google Patents

Manufacturing method for electrode structure for fuel cell Download PDF

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JP2006339062A
JP2006339062A JP2005163808A JP2005163808A JP2006339062A JP 2006339062 A JP2006339062 A JP 2006339062A JP 2005163808 A JP2005163808 A JP 2005163808A JP 2005163808 A JP2005163808 A JP 2005163808A JP 2006339062 A JP2006339062 A JP 2006339062A
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catalyst layer
electrode catalyst
polymer electrolyte
electrolyte membrane
solid polymer
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Fumiyoshi Kurosu
文美 黒須
Hiroshi Shinkai
洋 新海
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Honda 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 form an electrode structure for a fuel cell by applying an electrode catalyst layer without generating wrinkles in a polymer electrolyte film. <P>SOLUTION: This manufacturing method for the electrode structure for the fuel cell wherein a cathode electrode catalyst layer and an anode electrode catalyst layer are formed in a solid polymer electrolytic film respectively comprises a first fixing process that providing a solid polymer electrolytic film on a pressure sensitive adhesive sheet, a first application process applying either cathode electrode catalyst layer paste or anode electrode catalyst layer paste on the fixed solid polymer electrolytic film, and a first removal process removing the pressure sensitive adhesive sheet from the solid polymer electrolytic film. <P>COPYRIGHT: (C)2007,JPO&INPIT

Description

本発明は、燃料電池用電極構造体の製造方法に係り、特に、電解質膜に触媒を形成する際に発生する皺を抑制する技術に関する。   The present invention relates to a method of manufacturing a fuel cell electrode structure, and more particularly to a technique for suppressing soot generated when a catalyst is formed on an electrolyte membrane.

現在、石油資源の枯渇が重大な問題となっており、さらに、化石燃料の消費による大気汚染や地球温暖化等の環境問題が深刻化している。このような状況にあって、二酸化炭素の発生を伴わないクリーンな電動機用電力源として燃料電池が注目されて広範に開発されるとともに、一部では実用化され始めている。   Currently, depletion of petroleum resources is a serious problem, and environmental problems such as air pollution and global warming due to consumption of fossil fuels are becoming more serious. Under such circumstances, fuel cells have attracted attention as a clean electric power source for electric motors that does not generate carbon dioxide and have been extensively developed, and some have begun to be put into practical use.

燃料電池を自動車等に搭載する場合には、高電圧と大電流とが得やすいことから、高分子電解質膜を用いる固体高分子型燃料電池が好適に用いられる。固体高分子型燃料電池に用いる電極構造体として、イオン導伝可能な高分子電解質膜を一対の電極触媒層の間に挟持し、各電極触媒層の上に、拡散層を積層したものが知られている。電極触媒層は、白金等の触媒がカーボンブラック等の触媒担体に担持され、イオン導伝性高分子バインダーにより一体化されることにより形成されている。この電極構造体は、さらに各電極触媒層の上に、ガス通路を兼ねたセパレータを積層することにより、固体高分子型燃料電池を構成する。   When a fuel cell is mounted on an automobile or the like, a solid polymer fuel cell using a polymer electrolyte membrane is preferably used because a high voltage and a large current can be easily obtained. As an electrode structure used for a polymer electrolyte fuel cell, an ion conductive polymer electrolyte membrane is sandwiched between a pair of electrode catalyst layers, and a diffusion layer is laminated on each electrode catalyst layer. It has been. The electrode catalyst layer is formed by supporting a catalyst such as platinum on a catalyst carrier such as carbon black and integrating them with an ion conductive polymer binder. This electrode structure further forms a polymer electrolyte fuel cell by laminating a separator that also serves as a gas passage on each electrode catalyst layer.

このような固体高分子型燃料電池では、一方の電極触媒層を燃料極として、拡散層を介して水素、メタノール等の還元性ガスを導入するとともに、他方の電極触媒層を酸素極として、拡散層を介して空気、酸素等の酸化性ガスを導入する。燃料極側では、電極触媒層に含まれる触媒の作用により、還元性ガスからプロトン（Ｈ＋）及び電子が生成し、プロトンは高分子電解質膜を介して、酸素極側の電極触媒層に移動する。そして、プロトンは、酸素極側の電極触媒層で、電極触媒層に含まれる触媒の作用により、酸素極に導入される酸化性ガス及び電子と反応して水を生成する。したがって、燃料極と酸素極とを導線により接続することにより、燃料極で生成した電子を酸素極に送る回路が形成され、電流を取り出すことができる。 In such a polymer electrolyte fuel cell, one electrode catalyst layer is used as a fuel electrode, a reducing gas such as hydrogen or methanol is introduced through a diffusion layer, and the other electrode catalyst layer is used as an oxygen electrode for diffusion. An oxidizing gas such as air or oxygen is introduced through the layer. On the fuel electrode side, protons (H + ) and electrons are generated from the reducing gas by the action of the catalyst contained in the electrode catalyst layer, and the protons move to the electrode catalyst layer on the oxygen electrode side through the polymer electrolyte membrane. To do. Then, protons react with the oxidizing gas and electrons introduced into the oxygen electrode by the action of the catalyst contained in the electrode catalyst layer in the electrode catalyst layer on the oxygen electrode side to generate water. Therefore, by connecting the fuel electrode and the oxygen electrode with a conducting wire, a circuit for sending electrons generated at the fuel electrode to the oxygen electrode is formed, and a current can be taken out.

このような電極構造体を作製するには、従来、別途支持体上に電極触媒層を形成し、これと高分子電解質膜を貼り合わせて熱圧着する方法が一般的であった。しかしながら、この方法では、電極触媒層を固化・形成した後に電解質膜上に貼り合わせるので、互いに密着させることが難しく、接触抵抗が高いという問題を有していた。   In order to produce such an electrode structure, conventionally, an electrode catalyst layer is separately formed on a support, and this is bonded to a polymer electrolyte membrane and thermocompression bonded. However, in this method, since the electrode catalyst layer is solidified and formed and then bonded onto the electrolyte membrane, there is a problem that it is difficult to make them adhere to each other and the contact resistance is high.

このような問題に対し、電解質膜上にスクリーン印刷、バーコータ、ドクターブレード等によって電極触媒ペーストを直接印刷し、乾燥させて電極構造体を製造する技術（例えば、特許文献１参照）や、多孔板上に真空引きによって固体高分子電解質膜を吸着保持しながら電極触媒層スラリーを塗布する技術（例えば、特許文献２参照）が提案されている。   With respect to such problems, a technique for producing an electrode structure by directly printing an electrode catalyst paste on the electrolyte membrane by screen printing, a bar coater, a doctor blade or the like and drying it (for example, see Patent Document 1), a perforated plate A technique for applying an electrode catalyst layer slurry while adsorbing and holding a solid polymer electrolyte membrane by evacuation (see, for example, Patent Document 2) has been proposed.

特開２０００−２６８８２９号公報JP 2000-268829 A 特開２００３−１００３１４号公報JP 2003-100314 A

しかしながら、特許文献１に記載の製造方法では、印刷された電極触媒ペーストに含まれる溶媒成分によって高分子電解質膜が膨潤し、また、印刷後の乾燥によって電極触媒層および高分子電解質膜が収縮することによって、高分子電解質膜に皺が発生するという問題があった。さらに、高分子電解質膜上に所望の形状・寸法を確保した電極触媒層を塗布によって形成するのが困難であるという問題を有していた。また、特許文献２に記載の方法では、真空引きを行っている多孔板から固体高分子電解質膜を乾燥工程に移し替える際の取扱いが困難であり、固体高分子電解質膜を破損する虞があった。   However, in the production method described in Patent Document 1, the polymer electrolyte membrane swells due to the solvent component contained in the printed electrode catalyst paste, and the electrode catalyst layer and the polymer electrolyte membrane shrink due to drying after printing. As a result, there is a problem that wrinkles are generated in the polymer electrolyte membrane. Furthermore, there is a problem that it is difficult to form an electrode catalyst layer having a desired shape and size on the polymer electrolyte membrane by coating. In addition, in the method described in Patent Document 2, it is difficult to handle the transfer of the solid polymer electrolyte membrane from the perforated plate being evacuated to the drying step, and the solid polymer electrolyte membrane may be damaged. It was.

本発明は上記状況に鑑みてなされたものであり、高分子電解質膜に皺を発生させることなく高分子電解質膜上に電極触媒層を塗布によって形成することができ、しかも所望の形状の電極触媒層を形成することができる燃料電池用電極構造体の製造方法を提供することを目的としている。   The present invention has been made in view of the above situation, and an electrode catalyst layer can be formed on a polymer electrolyte membrane by coating without causing wrinkles on the polymer electrolyte membrane, and an electrode catalyst having a desired shape can be formed. It aims at providing the manufacturing method of the electrode structure for fuel cells which can form a layer.

本発明は、固体高分子電解質膜にカソード電極触媒層およびアノード電極触媒層をそれぞれ形成した燃料電池用電極構造体の製造方法であって、固体高分子電解質膜を粘着シート上に設置する第１固定工程と、固定された固体高分子電解質膜上にカソード電極触媒層ペーストまたはアノード電極触媒層ペーストの一方を塗布する第１塗布工程と、粘着シートを固体高分子電解質膜から除去する第１除去工程とを有することを特徴としている。   The present invention is a method for producing an electrode structure for a fuel cell in which a cathode electrode catalyst layer and an anode electrode catalyst layer are formed on a solid polymer electrolyte membrane, respectively, wherein the solid polymer electrolyte membrane is placed on an adhesive sheet. A fixing step, a first application step of applying one of a cathode electrode catalyst layer paste or an anode electrode catalyst layer paste onto the fixed solid polymer electrolyte membrane, and a first removal of removing the adhesive sheet from the solid polymer electrolyte membrane And a process.

本発明の燃料電池用電極構造体の製造方法によれば、カソード（またはアノード）電極触媒層ペースト塗布時において、固体高分子電解質膜が粘着シートの固着によって、ペースト塗布面の裏側から固定されているので、ペーストに含まれる溶媒による固体高分子電解質膜の膨潤に起因する高分子電解質膜の皺の発生を抑制することができる。   According to the method for producing an electrode structure for a fuel cell of the present invention, when applying the cathode (or anode) electrode catalyst layer paste, the solid polymer electrolyte membrane is fixed from the back side of the paste application surface by the adhesion of the adhesive sheet. Therefore, generation | occurrence | production of the wrinkle of the polymer electrolyte membrane resulting from the swelling of the solid polymer electrolyte membrane by the solvent contained in a paste can be suppressed.

本発明は、第１塗布工程と第１除去工程との間に、固体高分子電解質膜上に電極触媒層が設けられてなる複合体の第１乾燥工程を有することを好ましい形態としている。   The present invention preferably includes a first drying step of a composite in which an electrode catalyst layer is provided on a solid polymer electrolyte membrane between the first coating step and the first removal step.

電極触媒層ペースト塗布後の複合体の乾燥工程は任意の段階に行うことができるが、特に、このような形態によれば、第１塗布工程と第１除去工程との間においては、固体高分子電解質膜が粘着シートの固着によって固定されているので、乾燥時における固体高分子電解質膜の収縮を抑制するだけでなく、乾燥時に工程の上流から下流にかけて前後に移動させて扱う際の破損を抑制することができる。   The drying process of the composite after the application of the electrode catalyst layer paste can be performed at an arbitrary stage. In particular, according to such an embodiment, the solids high between the first application process and the first removal process. Since the molecular electrolyte membrane is fixed by sticking the adhesive sheet, it not only suppresses the shrinkage of the solid polymer electrolyte membrane during drying, but also breaks when handling it by moving it back and forth from the upstream to the downstream of the process during drying. Can be suppressed.

また、本発明は、第１除去工程の後に、複合体を裏返して粘着シート上に複合体の電極触媒層側を設置する第２固定工程と、固定された複合体の固体高分子電解質膜側にアノード電極触媒層ペーストまたはカソード電極触媒層ペーストの他方を塗布する第２塗布工程と、粘着シートを複合体から除去する第２除去工程とを有することを好ましい形態としている。   In addition, the present invention provides a second fixing step in which the composite is turned over and the electrode catalyst layer side of the composite is placed on the adhesive sheet after the first removal step, and the solid polymer electrolyte membrane side of the fixed composite It is preferable to have a second application step of applying the other of the anode electrode catalyst layer paste or the cathode electrode catalyst layer paste and a second removal step of removing the adhesive sheet from the composite.

このような形態によれば、電極触媒層ペースト塗布時において、すでに形成された電極触媒層が粘着シートの固着によって固定され、この電極触媒層がさらに固体高分子電解質膜を固定しているので、ペーストに含まれる溶媒による固体高分子電解質膜の膨潤に起因する固体高分子電解質膜の皺の発生を抑制することができる。   According to such a form, when the electrode catalyst layer paste is applied, the already formed electrode catalyst layer is fixed by fixing the adhesive sheet, and this electrode catalyst layer further fixes the solid polymer electrolyte membrane. Occurrence of wrinkles of the solid polymer electrolyte membrane due to swelling of the solid polymer electrolyte membrane by the solvent contained in the paste can be suppressed.

本発明は、第２塗布工程と第２除去工程との間に、複合体の第２乾燥工程を有することを好ましい形態としている。   This invention makes it a preferable form to have a 2nd drying process of a composite_body | complex between a 2nd application | coating process and a 2nd removal process.

このような形態によれば、第１塗布工程と第１除去工程との間における乾燥工程と同様に、第２塗布工程と第２除去工程との間においても、すでに塗布された電極触媒層が粘着シートの固着によって固定されているので、固体高分子電解質膜の収縮を抑制することができる。   According to such a form, like the drying process between the first application process and the first removal process, the electrode catalyst layer already applied is also applied between the second application process and the second removal process. Since it is fixed by the adhesion of the pressure-sensitive adhesive sheet, shrinkage of the solid polymer electrolyte membrane can be suppressed.

以下、本発明の好適な実施形態について、適宜図面を参照しながら説明する。
図１は、本発明の実施形態を示す模式図である。図１において符号１は、一連の工程を行うための例えばアルミニウム製やＳＵＳ製の保持基材である。保持基材１上には、粘着性を有する粘着シート２が固定されている。 Hereinafter, preferred embodiments of the present invention will be described with reference to the drawings as appropriate.
FIG. 1 is a schematic diagram showing an embodiment of the present invention. In FIG. 1, the code | symbol 1 is an aluminum-made or SUS-made holding base material for performing a series of processes. An adhesive sheet 2 having adhesiveness is fixed on the holding substrate 1.

まず、固体高分子電解質膜３を粘着シート２上に貼り付ける（第１固定工程）。続いて、バーコータやドクターブレード等の任意の塗布手段５によって、カソード電極触媒層ペースト４を固体高分子電解質膜３上に塗布し（第１塗布工程）、粘着シート２によって固着させたままの状態で固体高分子電解質膜３およびカソード電極触媒層４を乾燥させる。乾燥後、これらを粘着シート２から剥離し（第１除去工程）、裏返し、カソード電極触媒層４側を粘着シート２に貼り付ける（第２固定工程）。塗布手段５によってアノード電極触媒層ペースト６を固体高分子電解質膜３上に塗布し（第２塗布工程）、粘着シート２によって固着させたままの状態で固体高分子電解質膜３およびアノード電極触媒層６を乾燥させる。乾燥後、粘着シート２から剥離し（第２除去工程）、固体高分子電解質膜３の両面にカソード電極触媒層４およびアノード電極触媒層６が形成された膜−電極複合体を得る。   First, the solid polymer electrolyte membrane 3 is affixed on the adhesive sheet 2 (first fixing step). Subsequently, the cathode electrode catalyst layer paste 4 is applied onto the solid polymer electrolyte membrane 3 by an arbitrary application means 5 such as a bar coater or a doctor blade (first application step), and is kept fixed by the adhesive sheet 2. Then, the solid polymer electrolyte membrane 3 and the cathode electrode catalyst layer 4 are dried. After drying, these are peeled from the pressure-sensitive adhesive sheet 2 (first removal step), turned over, and the cathode electrode catalyst layer 4 side is attached to the pressure-sensitive adhesive sheet 2 (second fixing step). The anode electrode catalyst layer paste 6 is applied onto the solid polymer electrolyte membrane 3 by the application means 5 (second application step), and the solid polymer electrolyte membrane 3 and the anode electrode catalyst layer are kept fixed by the adhesive sheet 2. 6 is dried. After drying, the film is peeled from the pressure-sensitive adhesive sheet 2 (second removal step) to obtain a membrane-electrode complex in which the cathode electrode catalyst layer 4 and the anode electrode catalyst layer 6 are formed on both surfaces of the solid polymer electrolyte membrane 3.

高分子電解質膜にカソード電極触媒層ペーストおよびアノード電極触媒層ペーストを塗布する手段としては、スクリーン印刷や、バーコーター、ドクターブレードによる印刷等、特に限定されない。   A means for applying the cathode electrode catalyst layer paste and the anode electrode catalyst layer paste to the polymer electrolyte membrane is not particularly limited, such as screen printing, printing with a bar coater, or a doctor blade.

特に、ドクターブレード、バーコータを使用する場合、所望の形状に切り抜かれたラミネーティングフィルムを併用することで、電極触媒層を自由に成形した膜−電極複合体を得ることができる。具体的には、粘着シート上に固体高分子電解質膜を固着させた後、所望の形状に切り抜かれたラミネーティングフィルムを固体高分子電解質膜上に貼り付ける。このラミネーティングフィルムの切り抜かれた範囲内にカソード電極触媒層ペーストを塗布・乾燥し、固体高分子電解質膜を粘着シートから剥離して裏返し、カソード電極触媒層側を粘着シート上に固着させる。続いて所望の形状に切り抜かれた他のラミネーティングフィルムを個体高分子電解質膜上に貼り付け、同様にアノード電極触媒層ペーストを塗布・乾燥する。最後に両面のラミネーティングフィルムを除去することによって、電極触媒層を自由に成形した膜−電極複合体を得ることができる。なお、カソード電極触媒層のラミネーティングフィルムは、カソード電極触媒層の乾燥直後に除去してもよく、また、この実施形態においても、カソード・アノードの塗布順は逆にすることができる。   In particular, when a doctor blade or a bar coater is used, a membrane-electrode composite in which an electrode catalyst layer is freely formed can be obtained by using a laminating film cut into a desired shape. Specifically, after the solid polymer electrolyte membrane is fixed on the pressure-sensitive adhesive sheet, a laminating film cut into a desired shape is attached onto the solid polymer electrolyte membrane. The cathode electrode catalyst layer paste is applied and dried within the cutout range of the laminating film, the solid polymer electrolyte membrane is peeled off from the adhesive sheet and turned over, and the cathode electrode catalyst layer side is fixed on the adhesive sheet. Subsequently, another laminating film cut into a desired shape is attached onto the solid polymer electrolyte membrane, and the anode electrode catalyst layer paste is similarly applied and dried. Finally, by removing the laminating films on both sides, a membrane-electrode assembly in which the electrode catalyst layer is freely formed can be obtained. The laminating film for the cathode electrode catalyst layer may be removed immediately after the cathode electrode catalyst layer is dried. Also in this embodiment, the order of application of the cathode and anode can be reversed.

本発明で使用する粘着シートは、適切な範囲の粘着力を有することが要求される。この粘着力の測定方法は、ＪＩＳ Ｚ０２３７に記載されており、図２に示すように被着体７に粘着シートの試片２（および保持基材１）を張り合わせ、その一端を剥離し、貼り合わせ方向に対して９０度の方向に引き剥がして、引き剥がしに要した力を測定するものである。具体的には、被着体７をステンレス板として測定を行い、粘着力が８４〜１０３ｇｆ／３０ｍｍであると好ましい。粘着力が８４ｇｆ／３０ｍｍ未満であると、固着効果が十分ではなく、電極触媒層ペーストの塗布および乾燥の際の膨潤・収縮を抑えることができず、部分的に剥離して皺が発生してしまう。また、粘着力が１０３ｇｆ／３０ｍｍを越えると、固着効果が強すぎて、保持されている固体高分子電解質膜または電極触媒層を剥離する際に、これらを破損してしまうおそれがある。   The pressure-sensitive adhesive sheet used in the present invention is required to have a suitable range of pressure-sensitive adhesive strength. The method for measuring the adhesive strength is described in JIS Z0237. As shown in FIG. 2, the specimen 2 (and holding substrate 1) of the adhesive sheet is bonded to the adherend 7, and one end thereof is peeled off and attached. It peels in the direction of 90 degrees with respect to the mating direction, and measures the force required for peeling. Specifically, measurement is performed using the adherend 7 as a stainless steel plate, and the adhesive strength is preferably 84 to 103 gf / 30 mm. If the adhesive strength is less than 84 gf / 30 mm, the fixing effect is not sufficient, swelling / shrinkage during application and drying of the electrode catalyst layer paste cannot be suppressed, and wrinkles occur due to partial peeling. End up. On the other hand, if the adhesive strength exceeds 103 gf / 30 mm, the fixing effect is too strong, and there is a risk of damaging these when the held solid polymer electrolyte membrane or electrode catalyst layer is peeled off.

本発明においては、第１固定工程、第１塗布工程、第１乾燥工程および第１除去工程の後に複合体を裏返して第２固定工程、第２塗布工程、第２乾燥工程および第２除去工程を行うことによって膜−電極複合体を形成することを好ましい形態としているが、膜−電極複合体の作製方法としてはこの形態のみに限定されず、第１固定工程〜第１乾燥工程によって片方の電極触媒層を形成した後、他の公知の方法、例えば真空引きや静電吸着等により複合体を固定して第２塗布工程を行い、他方の電極触媒層を形成することもできる。   In the present invention, after the first fixing step, the first coating step, the first drying step, and the first removing step, the composite is turned over and the second fixing step, the second coating step, the second drying step, and the second removing step are performed. However, the method for producing the membrane-electrode complex is not limited to this mode, and one of the processes is performed by the first fixing step to the first drying step. After forming the electrode catalyst layer, the other electrode catalyst layer can be formed by fixing the composite by other known methods such as evacuation or electrostatic adsorption and performing the second coating step.

以下、実施例および比較例を用いて本発明を具体的に説明する。
図２に示す試験方法において、被着体７としてステンレス板を用い、粘着シート２および保持基材１を貼り合わせたものを被着体７に貼り付けた。粘着シート２の一端にテンションゲージを取り付け、図２に示すように、テンションゲージを取り付けた一端から剥離して、貼り合わされた方向に対して９０度の方向に引き剥がし、剥離に要する張力を測定した。この測定を６回行い、平均値を取った。実施例および比較例の測定結果を表１に示す。 Hereinafter, the present invention will be specifically described with reference to Examples and Comparative Examples.
In the test method shown in FIG. 2, a stainless steel plate is used as the adherend 7, and the adhesive sheet 2 and the holding substrate 1 are attached to the adherend 7. A tension gauge is attached to one end of the adhesive sheet 2 and peeled off from one end where the tension gauge is attached as shown in FIG. 2 and then peeled off in a direction of 90 degrees with respect to the bonded direction, and the tension required for peeling is measured. did. This measurement was performed 6 times and an average value was taken. Table 1 shows the measurement results of Examples and Comparative Examples.

Figure 2006339062
Figure 2006339062

図１に示すように、実施例および比較例の各粘着シートをアルミニウム製の保持基材１上に製膜した。その上に固体高分子電解質膜３を設置し、カソード電極触媒層ペースト４を塗布・乾燥し、固体高分子電解質膜３を粘着シート２から剥離して裏返しにしてカソード電極触媒層側を粘着シート２に設置した。続いてアノード電極触媒層ペースト５を塗布・乾燥し、粘着シート２から剥離し、膜−電極複合体を得た。   As shown in FIG. 1, each pressure-sensitive adhesive sheet of Examples and Comparative Examples was formed on an aluminum holding substrate 1. The solid polymer electrolyte membrane 3 is placed thereon, the cathode electrode catalyst layer paste 4 is applied and dried, the solid polymer electrolyte membrane 3 is peeled off from the adhesive sheet 2 and turned over, and the cathode electrode catalyst layer side is attached to the adhesive sheet. 2 was installed. Subsequently, the anode electrode catalyst layer paste 5 was applied and dried, and peeled off from the pressure-sensitive adhesive sheet 2 to obtain a membrane-electrode composite.

実施例１〜３の粘着シートを使用した膜−電極複合体では、粘着シートが適正な範囲の粘着力を有していたため、固体高分子電解質膜および各電極触媒層に皺や破損は観察されなかった。一方、比較例１の粘着シートを使用した膜−電極複合体では、粘着力が不足していたため、乾燥工程において固体高分子電解質膜および電極触媒層の固着力が不足して、皺が発生していた。   In the membrane-electrode composites using the pressure-sensitive adhesive sheets of Examples 1 to 3, since the pressure-sensitive adhesive sheet had a proper range of adhesive strength, wrinkles and damages were observed in the solid polymer electrolyte membrane and each electrode catalyst layer. There wasn't. On the other hand, in the membrane-electrode composite using the pressure-sensitive adhesive sheet of Comparative Example 1, since the adhesive strength was insufficient, the solid polymer electrolyte membrane and the electrode catalyst layer were not sufficiently fixed in the drying step, and wrinkles were generated. It was.

以上、実施例によって本発明の効果を説明したが、本発明は、上記実施例の範囲のみに限定されず、上述したように、第１固定工程〜第１乾燥工程によって片方の電極触媒層を形成した後に他の公知の方法によって他方の電極触媒層を形成する形態をも含む。   As mentioned above, although the effect of this invention was demonstrated by the Example, this invention is not limited only to the range of the said Example, As mentioned above, one electrode catalyst layer is formed by the 1st fixing process-the 1st drying process. It includes a form in which the other electrode catalyst layer is formed by another known method after the formation.

電極触媒層と高分子電解質膜の接触抵抗が改善され、膜−電極複合体の皺・変形が防止され、しかも任意の形状の電極触媒層を有する固体高分子型燃料電池を提供することができる。   The contact resistance between the electrode catalyst layer and the polymer electrolyte membrane is improved, and the membrane-electrode composite is prevented from wrinkling and deformation, and a solid polymer fuel cell having an electrode catalyst layer of any shape can be provided. .

本発明の膜−電極構造体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 membrane-electrode structure of this invention. 本発明における粘着シートの粘着力測定方法の模式図である。It is a schematic diagram of the adhesive force measuring method of the adhesive sheet in this invention.

符号の説明Explanation of symbols

１ 保持基材
２ 粘着シート
３ 固体高分子電解質膜
４ 電極触媒層（ペースト）
５ 塗布手段
６ 電極触媒層（ペースト）
７ 被着体 DESCRIPTION OF SYMBOLS 1 Holding base material 2 Adhesive sheet 3 Solid polymer electrolyte membrane 4 Electrode catalyst layer (paste)
5 Coating means 6 Electrode catalyst layer (paste)
7 adherend

Claims (4)

固体高分子電解質膜にカソード電極触媒層およびアノード電極触媒層をそれぞれ形成した燃料電池用電極構造体の製造方法であって、
上記固体高分子電解質膜を粘着シート上に設置する第１固定工程と、
固定された上記固体高分子電解質膜上にカソード電極触媒層ペーストまたはアノード電極触媒層ペーストの一方を塗布する第１塗布工程と、
上記粘着シートを上記固体高分子電解質膜から除去する第１除去工程とを有することを特徴とする燃料電池用電極構造体の製造方法。 A method for producing a fuel cell electrode structure in which a cathode electrode catalyst layer and an anode electrode catalyst layer are formed on a solid polymer electrolyte membrane, respectively,
A first fixing step of installing the solid polymer electrolyte membrane on an adhesive sheet;
A first coating step of coating one of a cathode electrode catalyst layer paste or an anode electrode catalyst layer paste on the solid polymer electrolyte membrane fixed;
And a first removal step of removing the pressure-sensitive adhesive sheet from the solid polymer electrolyte membrane. A method for producing an electrode structure for a fuel cell, comprising: 前記第１塗布工程と前記第１除去工程との間に、前記固体高分子電解質膜上に前記電極触媒層が設けられてなる複合体の第１乾燥工程を有することを特徴とする請求項１に記載の燃料電池用電極構造体の製造方法。   2. A first drying step of a composite comprising the electrode catalyst layer provided on the solid polymer electrolyte membrane between the first coating step and the first removal step. The manufacturing method of the electrode structure for fuel cells of description. 前記第１除去工程の後に、前記複合体を裏返して前記粘着シート上に上記複合体の電極触媒層側を設置する第２固定工程と、
固定された上記複合体の固体高分子電解質膜側にアノード電極触媒層ペーストまたはカソード電極触媒層ペーストの他方を塗布する第２塗布工程と、
上記粘着シートを上記複合体から除去する第２除去工程とを有することを特徴とする請求項１または２に記載の燃料電池用電極構造体の製造方法。 After the first removal step, the second fixing step of turning the composite upside down and placing the electrode catalyst layer side of the composite on the adhesive sheet;
A second application step of applying the other of the anode electrode catalyst layer paste or the cathode electrode catalyst layer paste to the solid polymer electrolyte membrane side of the fixed composite;
The method for producing a fuel cell electrode structure according to claim 1, further comprising a second removing step of removing the pressure-sensitive adhesive sheet from the composite. 前記第２塗布工程と前記第２除去工程との間に、前記複合体の第２乾燥工程を有することを特徴とする請求項３に記載の燃料電池用電極構造体の製造方法。   4. The method of manufacturing a fuel cell electrode structure according to claim 3, further comprising a second drying step of the composite body between the second application step and the second removal step. 5.
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Cited By (4)

* Cited by examiner, † Cited by third party
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WO2011099285A1 (en) * 2010-02-10 2011-08-18 パナソニック株式会社 Catalyst-coated membrane assembly manufacturing method and device
WO2015053304A1 (en) 2013-10-09 2015-04-16 日東電工株式会社 Method for manufacturing fuel-cell membrane electrode assembly
WO2015053303A1 (en) 2013-10-09 2015-04-16 日東電工株式会社 Pressure-sensitive adhesive sheet for conveying electrolyte membrane and method using said pressure-sensitive adhesive sheet to manufacture fuel-cell membrane electrode assembly
US10505200B2 (en) 2013-05-20 2019-12-10 SCREEN Holdings Co., Ltd. Apparatus and method manufacturing composite membrane

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2011099285A1 (en) * 2010-02-10 2011-08-18 パナソニック株式会社 Catalyst-coated membrane assembly manufacturing method and device
JP4879372B2 (en) * 2010-02-10 2012-02-22 パナソニック株式会社 Method and apparatus for manufacturing membrane-catalyst layer assembly
US10505200B2 (en) 2013-05-20 2019-12-10 SCREEN Holdings Co., Ltd. Apparatus and method manufacturing composite membrane
WO2015053304A1 (en) 2013-10-09 2015-04-16 日東電工株式会社 Method for manufacturing fuel-cell membrane electrode assembly
WO2015053303A1 (en) 2013-10-09 2015-04-16 日東電工株式会社 Pressure-sensitive adhesive sheet for conveying electrolyte membrane and method using said pressure-sensitive adhesive sheet to manufacture fuel-cell membrane electrode assembly
KR20160067852A (en) 2013-10-09 2016-06-14 닛토덴코 가부시키가이샤 Method for manufacturing fuel-cell membrane electrode assembly
KR20160067851A (en) 2013-10-09 2016-06-14 닛토덴코 가부시키가이샤 Pressure-sensitive adhesive sheet for conveying electrolyte membrane and method using said pressure-sensitive adhesive sheet to manufacture fuel-cell membrane electrode assembly

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