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JP5703186B2 - Electrolyte membrane / electrode structure with resin frame for fuel cell and production method thereof - Google Patents

Electrolyte membrane / electrode structure with resin frame for fuel cell and production method thereof Download PDF

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JP5703186B2
JP5703186B2 JP2011221578A JP2011221578A JP5703186B2 JP 5703186 B2 JP5703186 B2 JP 5703186B2 JP 2011221578 A JP2011221578 A JP 2011221578A JP 2011221578 A JP2011221578 A JP 2011221578A JP 5703186 B2 JP5703186 B2 JP 5703186B2
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electrolyte membrane
resin frame
resin
solid polymer
polymer electrolyte
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JP2013084352A (en
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佐藤 雅彦
雅彦 佐藤
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Honda Motor Co Ltd
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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

本発明は、固体高分子電解質膜の両側に、それぞれ電極触媒層とガス拡散層とを有する電極が設けられるとともに、前記ガス拡散層の外周端部から外方に前記固体高分子電解質膜の外周端部が突出する電解質膜・電極構造体と、前記固体高分子電解質膜の外周を周回して設けられる樹脂製枠部材とを備える燃料電池用樹脂枠付き電解質膜・電極構造体及びその製造方法に関する。   In the present invention, electrodes having an electrode catalyst layer and a gas diffusion layer are provided on both sides of the solid polymer electrolyte membrane, respectively, and the outer periphery of the solid polymer electrolyte membrane is outward from the outer peripheral end of the gas diffusion layer. Electrolyte membrane / electrode structure with resin frame for fuel cell, comprising electrolyte membrane / electrode structure with protruding end, and resin frame member provided around the outer periphery of the solid polymer electrolyte membrane, and method for producing the same About.

一般的に、固体高分子型燃料電池は、高分子イオン交換膜からなる固体高分子電解質膜を採用している。この燃料電池は、固体高分子電解質膜の両側に、それぞれ触媒層(電極触媒層)とガス拡散層(多孔質カーボン)とからなるアノード電極及びカソード電極を配設した電解質膜・電極構造体(MEA)を、セパレータ(バイポーラ板)によって挟持している。この燃料電池は、所定の数だけ積層して燃料電池スタックを構成するとともに、例えば、車載用燃料電池スタックとして燃料電池電気自動車に採用されている。   In general, a polymer electrolyte fuel cell employs a polymer electrolyte membrane made of a polymer ion exchange membrane. This fuel cell comprises an electrolyte membrane / electrode structure in which an anode electrode and a cathode electrode each comprising a catalyst layer (electrode catalyst layer) and a gas diffusion layer (porous carbon) are disposed on both sides of a solid polymer electrolyte membrane ( MEA) is sandwiched between separators (bipolar plates). A predetermined number of the fuel cells are stacked to constitute a fuel cell stack, and for example, the fuel cell is employed in a fuel cell electric vehicle as an in-vehicle fuel cell stack.

通常、燃料電池スタックでは、多数の電解質膜・電極構造体が積層されており、コストを抑制するために、前記電解質膜・電極構造体を安価に構成することが要請されている。従って、特に高価な固体高分子電解質膜の使用量を削減するとともに、構成の簡素化を図るため、種々の提案がなされている。   In general, in a fuel cell stack, a large number of electrolyte membrane / electrode structures are laminated, and in order to reduce costs, it is required to configure the electrolyte membrane / electrode structures at low cost. Therefore, various proposals have been made in order to reduce the amount of use of a particularly expensive solid polymer electrolyte membrane and to simplify the configuration.

例えば、特許文献1に開示されている膜電極組立体が知られている。この膜電極組立体では、図4に示すように、シーリング端部を有する第1のガス拡散支持体1a、第1の電気触媒被覆組成物2a、高分子膜3、第2の電気触媒被覆組成物2b、及び、シーリング端部を有する第2のガス拡散支持体1bを含んで一体化されたMEAを構成している。   For example, a membrane electrode assembly disclosed in Patent Document 1 is known. In this membrane electrode assembly, as shown in FIG. 4, the first gas diffusion support 1a having the sealing end, the first electrocatalyst coating composition 2a, the polymer membrane 3, and the second electrocatalyst coating composition An integrated MEA is configured including the object 2b and the second gas diffusion support 1b having a sealing end.

一体化されたMEAは、熱可塑性ポリマーである流体不浸透性のシール4を含むとともに、第1のガス拡散支持体1a及び第2のガス拡散支持体1bのシーリング端部の中に熱可塑性ポリマーが含浸されている。シール4は、第1のガス拡散支持体1a及び第2のガス拡散支持体1bの両方の周囲領域、並びに高分子膜3を包み込んでいる。   The integrated MEA includes a fluid impermeable seal 4 that is a thermoplastic polymer, and the thermoplastic polymer in the sealing ends of the first gas diffusion support 1a and the second gas diffusion support 1b. Is impregnated. The seal 4 encloses the surrounding region of both the first gas diffusion support 1 a and the second gas diffusion support 1 b and the polymer film 3.

特表2005−516350号公報JP 2005-516350 A

ところで、MEAでは、燃料ガスと酸化剤ガスとの混合を確実に防止するため、ガス拡散層の外形寸法よりも大きな外形寸法の固体高分子電解質膜を有する場合がある。その際、上記の特許文献1を適用して、固体高分子電解質膜の外周縁部に熱可塑性ポリマーを射出成形すると、ガス拡散層の外周端部を超えて延在する固体高分子電解質膜の外周部は、射出成形時の樹脂流れによって移動し、表面に露出するおそれがある。   By the way, the MEA may have a solid polymer electrolyte membrane having an outer dimension larger than the outer dimension of the gas diffusion layer in order to reliably prevent mixing of the fuel gas and the oxidant gas. At that time, when the above-mentioned Patent Document 1 is applied and a thermoplastic polymer is injection-molded on the outer peripheral edge of the solid polymer electrolyte membrane, the solid polymer electrolyte membrane extending beyond the outer peripheral edge of the gas diffusion layer is formed. The outer peripheral portion may move due to the resin flow during injection molding and be exposed on the surface.

また、ガス拡散層の角部に対応する固体高分子電解質膜の部分に負荷が集中し、該部分が破損し易いという問題がある。しかも、MEAの薄型化を図る際に、薄肉化による成形後の樹脂材に反り等が発生するおそれがある。   Further, there is a problem that the load is concentrated on the portion of the solid polymer electrolyte membrane corresponding to the corner portion of the gas diffusion layer, and the portion is easily damaged. And when thinning MEA, there exists a possibility that the resin material after shaping | molding by thinning may generate | occur | produce a curvature.

本発明は、この種の問題を解決するものであり、固体高分子電解質膜の外周端部を周回して薄肉状の樹脂製枠部材を強固且つ容易に接合するとともに、前記樹脂製枠部材の変形を良好に抑制することが可能な燃料電池用樹脂枠付き電解質膜・電極構造体及びその製造方法を提供することを目的とする。   The present invention solves this type of problem. The thin resin frame member is joined firmly and easily around the outer peripheral end of the solid polymer electrolyte membrane, and the resin frame member It is an object of the present invention to provide an electrolyte membrane / electrode structure with a resin frame for a fuel cell and a method for producing the same that can favorably suppress deformation.

本発明は、固体高分子電解質膜の両側に、それぞれ電極触媒層とガス拡散層とを有する電極が設けられるとともに、前記ガス拡散層の外周端部から外方に前記固体高分子電解質膜の外周端部が突出する電解質膜・電極構造体と、前記固体高分子電解質膜の外周を周回して設けられるとともに、前記電極の表面と段差なく且つ同一面上に連続する樹脂製枠部材とを備える燃料電池用樹脂枠付き電解質膜・電極構造体及びその製造方法に関するものである。 In the present invention, electrodes having an electrode catalyst layer and a gas diffusion layer are provided on both sides of the solid polymer electrolyte membrane, respectively, and the outer periphery of the solid polymer electrolyte membrane is outward from the outer peripheral end of the gas diffusion layer. An electrolyte membrane / electrode structure with protruding ends, and a resin frame member provided around the outer periphery of the solid polymer electrolyte membrane and continuous on the same surface with no step from the surface of the electrode The present invention relates to an electrolyte membrane / electrode structure with a resin frame for fuel cells and a method for producing the same.

この燃料電池用樹脂枠付き電解質膜・電極構造体では、樹脂製枠部材は、固体高分子電解質膜の外周端部に直接接合される第1樹脂材と、前記第1樹脂材の外面に接合されるとともに、該第1樹脂材よりも融点が高い第2樹脂材とを備えている。   In this electrolyte membrane / electrode structure with a resin frame for a fuel cell, the resin frame member is joined to the first resin material directly joined to the outer peripheral end of the solid polymer electrolyte membrane and to the outer surface of the first resin material. And a second resin material having a higher melting point than the first resin material.

そして、この燃料電池用樹脂枠付き電解質膜・電極構造体では、固体高分子電解質膜の外周端部は、樹脂製枠部材の外周端部の内側に配置されるとともに、前記固体高分子電解質膜の外周端部と前記樹脂製枠部材の外周端部との間の領域は、第1樹脂材同士が直接接合されている And in this electrolyte membrane / electrode structure with a resin frame for fuel cells, the outer peripheral end of the solid polymer electrolyte membrane is disposed inside the outer peripheral end of the resin frame member, and the solid polymer electrolyte membrane area between the outer peripheral end portion of the outer peripheral edge portion and the resin frame member, the first resin material to each other is directly joined.

さらに、この燃料電池用樹脂枠付き電解質膜・電極構造体の製造方法は、第1樹脂材と前記第1樹脂材よりも融点が高い第2樹脂材とを接合し、一対の樹脂製枠部材を作製する工程と、各樹脂製枠部材の前記第1樹脂材により、固体高分子電解質膜の外周端部を直接挟持した状態で、前記第1樹脂材の融点よりも高温で且つ前記第2樹脂材の融点未満の温度を付与することによって、一対の前記樹脂製枠部材と前記固体高分子電解質膜とを一体に接合する工程とを有している。   Further, in this method of manufacturing an electrolyte membrane / electrode structure with a resin frame for a fuel cell, a first resin material and a second resin material having a melting point higher than that of the first resin material are joined, and a pair of resin frame members And the first resin material of each resin frame member, the outer peripheral end of the solid polymer electrolyte membrane is directly sandwiched between the first resin material and the second resin material at a temperature higher than the melting point of the first resin material. A step of integrally joining the pair of resin frame members and the solid polymer electrolyte membrane by applying a temperature lower than the melting point of the resin material.

そして、固体高分子電解質膜の外周端部は、樹脂製枠部材の外周端部の内側に配置されるとともに、前記固体高分子電解質膜の外周端部と前記樹脂製枠部材の外周端部との間の領域は、第1樹脂材同士が直接接合されている And the outer peripheral end of the solid polymer electrolyte membrane is disposed inside the outer peripheral end of the resin frame member, and the outer peripheral end of the solid polymer electrolyte membrane and the outer peripheral end of the resin frame member region between the first resin material to each other is directly joined.

また、この製造方法では、樹脂製枠部材には、それぞれ燃料ガス、酸化剤ガス及び冷媒体を流通させる複数の連通孔が貫通形成されることが好ましい。   In this manufacturing method, it is preferable that a plurality of communication holes through which the fuel gas, the oxidant gas, and the refrigerant body are circulated are formed through the resin frame member.

本発明によれば、樹脂製枠部材は、低融点の第1樹脂材と高融点の第2樹脂材とが接合されるとともに、一対の前記第1樹脂材が、固体高分子電解質膜の外周端部に直接接合(ホットプレス等)されている。このため、樹脂製枠部材と固体高分子電解質膜とが接合される際に、高融点の第2樹脂材が溶融されることがなく、前記樹脂製枠部材が変形することを確実に阻止することができる。   According to the present invention, in the resin frame member, the first resin material having a low melting point and the second resin material having a high melting point are joined, and the pair of first resin materials are arranged on the outer periphery of the solid polymer electrolyte membrane. It is joined directly to the end (hot press etc.). For this reason, when the resin frame member and the solid polymer electrolyte membrane are joined, the second resin material having a high melting point is not melted, and the resin frame member is reliably prevented from being deformed. be able to.

従って、固体高分子電解質膜の外周端部を周回して薄肉状の樹脂製枠部材を強固且つ容易に接合するとともに、前記樹脂製枠部材の変形を良好に抑制することが可能になる。これにより、樹脂製枠部材を歩留まりよく、しかも組立工数の削減により効率的に製造することができる。   Therefore, the thin resin frame member can be firmly and easily joined around the outer peripheral end of the solid polymer electrolyte membrane, and deformation of the resin frame member can be satisfactorily suppressed. As a result, the resin frame member can be manufactured efficiently with a good yield and by reducing the number of assembly steps.

本発明の実施形態に係る樹脂枠付き電解質膜・電極構造体が組み込まれる固体高分子型燃料電池の要部分解斜視説明図である。It is a principal part disassembled perspective explanatory view of the polymer electrolyte fuel cell in which the electrolyte membrane / electrode structure with a resin frame according to the embodiment of the present invention is incorporated. 前記燃料電池の、図1中、II−II線断面説明図である。FIG. 2 is a sectional view of the fuel cell taken along line II-II in FIG. 1. 前記樹脂枠付き電解質膜・電極構造体の製造方法の説明図である。It is explanatory drawing of the manufacturing method of the said electrolyte membrane and electrode structure with a resin frame. 特許文献1に開示されている膜電極組立体の説明図である。It is explanatory drawing of the membrane electrode assembly currently disclosed by patent document 1. FIG.

図1及び図2に示すように、本発明の実施形態に係る樹脂枠付き電解質膜・電極構造体10は、固体高分子型燃料電池12に組み込まれる。燃料電池12は、樹脂枠付き電解質膜・電極構造体10を第1セパレータ14及び第2セパレータ16により挟持して構成されるとともに、複数積層された燃料電池スタックとして、例えば、燃料電池電気自動車(図示せず)に搭載される。   As shown in FIGS. 1 and 2, an electrolyte membrane / electrode structure 10 with a resin frame according to an embodiment of the present invention is incorporated in a polymer electrolyte fuel cell 12. The fuel cell 12 is configured by sandwiching an electrolyte membrane / electrode structure 10 with a resin frame between a first separator 14 and a second separator 16, and as a stacked fuel cell stack, for example, a fuel cell electric vehicle ( (Not shown).

図1に示すように、燃料電池12の矢印C方向(鉛直方向)の上端縁部には、積層方向である矢印A方向に互いに連通して、酸化剤ガス、例えば、酸素含有ガスを供給するための酸化剤ガス入口連通孔18a、冷却媒体を供給するための冷却媒体入口連通孔20a、及び燃料ガス、例えば、水素含有ガスを供給するための燃料ガス入口連通孔22aが、矢印B方向に配列して設けられる。   As shown in FIG. 1, an oxidant gas, for example, an oxygen-containing gas is supplied to the upper edge of the fuel cell 12 in the arrow C direction (vertical direction) so as to communicate with each other in the arrow A direction that is the stacking direction. An oxidant gas inlet communication hole 18a for supplying a coolant, a cooling medium inlet communication hole 20a for supplying a cooling medium, and a fuel gas inlet communication hole 22a for supplying a fuel gas, for example, a hydrogen-containing gas, are provided in the direction of arrow B. Arranged and provided.

燃料電池12の矢印C方向の下端縁部には、矢印A方向に互いに連通して、燃料ガスを排出するための燃料ガス出口連通孔22b、冷却媒体を排出するための冷却媒体出口連通孔20b、及び酸化剤ガスを排出するための酸化剤ガス出口連通孔18bが、矢印B方向に配列して設けられる。   The lower end edge of the fuel cell 12 in the direction of arrow C communicates with each other in the direction of arrow A, the fuel gas outlet communication hole 22b for discharging the fuel gas, and the cooling medium outlet communication hole 20b for discharging the cooling medium. And oxidant gas outlet communication holes 18b for discharging the oxidant gas are arranged in the direction of arrow B.

第1セパレータ14及び第2セパレータ16は、例えば、鋼板、ステンレス鋼板、アルミニウム板、めっき処理鋼板、あるいはその金属表面に防食用の表面処理を施した縦長形状の金属板により構成される。   The first separator 14 and the second separator 16 are made of, for example, a steel plate, a stainless steel plate, an aluminum plate, a plated steel plate, or a vertically long metal plate obtained by performing a surface treatment for corrosion prevention on the metal surface.

第1セパレータ14及び第2セパレータ16は、平面が矩形状を有するとともに、金属製薄板を波形状にプレス加工することにより、断面凹凸形状に成形される。なお、第1セパレータ14及び第2セパレータ16は、例えば、カーボンセパレータにより構成してもよい。   The first separator 14 and the second separator 16 have a rectangular planar shape, and are formed into a concavo-convex shape by pressing a metal thin plate into a wave shape. In addition, you may comprise the 1st separator 14 and the 2nd separator 16 with a carbon separator, for example.

第1セパレータ14の樹脂枠付き電解質膜・電極構造体10に向かう面14aには、酸化剤ガス入口連通孔18aと酸化剤ガス出口連通孔18bとに連通する酸化剤ガス流路24が、鉛直方向に沿って設けられる。   An oxidant gas flow path 24 communicating with the oxidant gas inlet communication hole 18a and the oxidant gas outlet communication hole 18b is vertically formed on the surface 14a of the first separator 14 facing the electrolyte membrane / electrode structure 10 with a resin frame. It is provided along the direction.

第2セパレータ16の樹脂枠付き電解質膜・電極構造体10に向かう面16aには、燃料ガス入口連通孔22aと燃料ガス出口連通孔22bとに連通する燃料ガス流路26が、鉛直方向に沿って設けられる。   A fuel gas channel 26 communicating with the fuel gas inlet communication hole 22a and the fuel gas outlet communication hole 22b is provided along the vertical direction on the surface 16a of the second separator 16 facing the electrolyte membrane / electrode structure 10 with a resin frame. Provided.

互いに隣接する燃料電池12を構成する第1セパレータ14の面14bと、第2セパレータ16の面16bとの間には、冷却媒体入口連通孔20aと冷却媒体出口連通孔20bとを連通する冷却媒体流路28が、鉛直方向に沿って設けられる。   A cooling medium that connects the cooling medium inlet communication hole 20a and the cooling medium outlet communication hole 20b between the surface 14b of the first separator 14 and the surface 16b of the second separator 16 constituting the fuel cells 12 adjacent to each other. A flow path 28 is provided along the vertical direction.

第1セパレータ14の面14a、14bには、第1シール部材30が、一体的又は個別に設けられるとともに、第2セパレータ16の面16a、16bには、第2シール部材32が、一体的又は個別に設けられる。第1シール部材30及び第2シール部材32は、例えば、EPDM、NBR、フッ素ゴム、シリコーンゴム、フロロシリコンゴム、ブチルゴム、天然ゴム、スチレンゴム、クロロプレーン、又はアクリルゴム等のシール材、クッション材、あるいはパッキン材を使用する。   The first seal member 30 is integrally or individually provided on the surfaces 14a and 14b of the first separator 14, and the second seal member 32 is integrally or individually provided on the surfaces 16a and 16b of the second separator 16. Provided separately. The first seal member 30 and the second seal member 32 are, for example, EPDM, NBR, fluororubber, silicone rubber, fluorosilicone rubber, butyl rubber, natural rubber, styrene rubber, chloroplane, or acrylic rubber, or a cushioning material. Or use packing material.

図2に示すように、樹脂枠付き電解質膜・電極構造体10は、電解質膜・電極構造体34と樹脂製枠部材36とを備える。電解質膜・電極構造体34は、例えば、炭化水素系又はパーフルオロスルホン酸の薄膜に水が含浸された固体高分子電解質膜38と、前記固体高分子電解質膜38を挟持するカソード電極40及びアノード電極42とを備える。   As shown in FIG. 2, the electrolyte membrane / electrode structure 10 with a resin frame includes an electrolyte membrane / electrode structure 34 and a resin frame member 36. The electrolyte membrane / electrode structure 34 includes, for example, a solid polymer electrolyte membrane 38 in which a hydrocarbon-based or perfluorosulfonic acid thin film is impregnated with water, and a cathode electrode 40 and an anode sandwiching the solid polymer electrolyte membrane 38 An electrode 42.

カソード電極40及びアノード電極42は、同一の表面積(外形寸法)を有するとともに、固体高分子電解質膜38は、前記カソード電極40及び前記アノード電極42よりも大きな表面積(外形寸法)を有する。固体高分子電解質膜38の外周端部38endは、カソード電極40の外周端部40end及びアノード電極42の外周端部42endから外方に突出する。 The cathode electrode 40 and the anode electrode 42 have the same surface area (outer dimension), and the solid polymer electrolyte membrane 38 has a larger surface area (outer dimension) than the cathode electrode 40 and the anode electrode 42. An outer peripheral end portion 38 end The solid polymer electrolyte membrane 38 from the outer peripheral end portion 42 end The outer peripheral edge portion 40 end The and the anode electrode 42 of the cathode electrode 40 projects outward.

カソード電極40及びアノード電極42は、固体高分子電解質膜38の両方の面38a、38bに接合される電極触媒層40a、42aと、前記電極触媒層40a、42aに積層されるガス拡散層(多孔質拡散層)40b、42bとを有する。ガス拡散層40b、42bは、電極触媒層40a、42aよりも大きな表面積を有するが、同一の表面積に設定してもよい。   The cathode electrode 40 and the anode electrode 42 are electrode catalyst layers 40a, 42a joined to both surfaces 38a, 38b of the solid polymer electrolyte membrane 38, and a gas diffusion layer (porous) laminated on the electrode catalyst layers 40a, 42a. Quality diffusion layer) 40b, 42b. The gas diffusion layers 40b and 42b have a larger surface area than the electrode catalyst layers 40a and 42a, but may be set to the same surface area.

樹脂製枠部材36は、固体高分子電解質膜38の外周端部38endの両面に直接接合される一対の第1樹脂材44a、44bと、前記第1樹脂材44a、44bの外面に接合されるとともに、該第1樹脂材44a、44bよりも融点が高い一対の第2樹脂材46a、46bとを備える。 The resin frame member 36 is bonded to the outer surfaces of the pair of first resin materials 44a and 44b that are directly bonded to both surfaces of the outer peripheral end portion 38end of the solid polymer electrolyte membrane 38, and the first resin materials 44a and 44b. And a pair of second resin materials 46a and 46b having a higher melting point than the first resin materials 44a and 44b.

第1樹脂材44aと第2樹脂材46aとにより第1樹脂枠シート36aが構成される一方、第1樹脂材44bと第2樹脂材46bとにより第2樹脂枠シート36bが構成される。固体高分子電解質膜38の外周端部38endと樹脂製枠部材36の外周端部36endとの間の領域は、第1樹脂材44a、44b同士が直接接合される。 The first resin material 44a and the second resin material 46a constitute a first resin frame sheet 36a, while the first resin material 44b and the second resin material 46b constitute a second resin frame sheet 36b. In the region between the outer peripheral end portion 38 end of the solid polymer electrolyte membrane 38 and the outer peripheral end portion 36 end of the resin frame member 36, the first resin materials 44a and 44b are directly joined to each other.

第1樹脂材44a、44bは、熱可塑性樹脂のシート材であり、例えば、融点が135℃程度であることが好ましい。第1樹脂材44a、44bは、具体的には、PP(ポリプロピレン)やABS(アクリルニトリルブタジエンスチレン)等が採用される。第2樹脂材46a、46bは、熱可塑性樹脂のシート材であり、例えば、融点が145℃程度であることが好ましい。第2樹脂材46a、46bは、具体的には、上記のPPやABSのグレード違いによる融点を変えた材料等が採用される。第1樹脂材44a、44b及び第2樹脂材46a、46bは、融点の大小関係が異なればよく、上記の材料に限定されない。   The first resin materials 44a and 44b are thermoplastic resin sheet materials, and preferably have a melting point of about 135 ° C., for example. Specifically, PP (polypropylene), ABS (acrylonitrile butadiene styrene), or the like is employed for the first resin materials 44a and 44b. The second resin materials 46a and 46b are thermoplastic resin sheet materials, and preferably have a melting point of about 145 ° C., for example. Specifically, the second resin materials 46a and 46b are made of a material whose melting point is changed due to the grade difference of PP or ABS described above. The first resin materials 44a and 44b and the second resin materials 46a and 46b are not limited to the above materials as long as they have different melting points.

樹脂製枠部材36の一方の面は、カソード電極40の表面と段差なく同一面上に連続するとともに、前記樹脂製枠部材36の他方の面は、アノード電極42の表面と段差なく同一面上に連続する。第1樹脂材44a、44bの厚さは、第2樹脂材46a、46bの厚さよりも小さく設定されることが好ましい。   One surface of the resin frame member 36 is continuous with the surface of the cathode electrode 40 without a step, and the other surface of the resin frame member 36 is flush with the surface of the anode electrode 42 without being stepped. It is continuous. The thickness of the first resin materials 44a and 44b is preferably set smaller than the thickness of the second resin materials 46a and 46b.

このように構成される燃料電池12において、樹脂枠付き電解質膜・電極構造体10を製造する方法について、以下に説明する。   In the fuel cell 12 configured as described above, a method of manufacturing the resin membrane-attached electrolyte membrane / electrode structure 10 will be described below.

先ず、図3中、(a)に示すように、それぞれ矩形状に形成された第1樹脂材44a、44bと第2樹脂材46a、46bとが用意される。次いで、図3中、(b)に示すように、第1樹脂材44aと第2樹脂材46aとは、前記第1樹脂材44aの融点以上の温度で、ホットプレスにより前記第1樹脂材44aが溶融されて一体化されて第1接合シート50aが得られる。同様に、第1樹脂材44bと第2樹脂材46bとは、ホットプレスにより前記第1樹脂材44bが溶融されて一体化されて第2接合シート50bが得られる。   First, as shown to (a) in FIG. 3, the 1st resin materials 44a and 44b and the 2nd resin materials 46a and 46b each formed in the rectangular shape are prepared. Next, as shown in FIG. 3B, the first resin material 44a and the second resin material 46a are hot-pressed at a temperature equal to or higher than the melting point of the first resin material 44a. Are melted and integrated to obtain the first joining sheet 50a. Similarly, the first resin material 44b and the second resin material 46b are fused and integrated by hot pressing to obtain the second bonding sheet 50b.

一方、図3中、(c)及び図2に示すように、固体高分子電解質膜38の両方の面38a、38bには、電極触媒層40a、42aが設けられる。具体的には、電極触媒層40a、42aは、カーボンブラックに白金粒子を担持した触媒粒子を形成し、イオン導伝性バインダーとして高分子電解質を含む溶液を使用し、この高分子電解質の溶液中に前記触媒粒子を均一に混合して作製された触媒ペーストを有する。   On the other hand, as shown in FIG. 3C and FIG. 2, electrode catalyst layers 40 a and 42 a are provided on both surfaces 38 a and 38 b of the solid polymer electrolyte membrane 38. Specifically, the electrode catalyst layers 40a and 42a form catalyst particles in which platinum particles are supported on carbon black, and use a solution containing a polymer electrolyte as an ion conductive binder. And a catalyst paste prepared by uniformly mixing the catalyst particles.

そして、電極触媒層40a、42aには、多孔質のカーボンからなるガス拡散層40b、42bがホットプレスにより一体化される。このため、電解質膜・電極構造体34が得られる。   Gas diffusion layers 40b and 42b made of porous carbon are integrated with the electrode catalyst layers 40a and 42a by hot pressing. For this reason, the electrolyte membrane / electrode structure 34 is obtained.

さらに、第1接合シート50a及び第2接合シート50bは、カソード電極40及びアノード電極42の外形形状に対応して額縁状にトリミングされる。従って、第1樹脂枠シート36a及び第2樹脂枠シート36bが形成される。第1樹脂枠シート36a及び第2樹脂枠シート36bは、電解質膜・電極構造体34の両面に配置される。   Further, the first bonding sheet 50 a and the second bonding sheet 50 b are trimmed into a frame shape corresponding to the outer shape of the cathode electrode 40 and the anode electrode 42. Accordingly, the first resin frame sheet 36a and the second resin frame sheet 36b are formed. The first resin frame sheet 36 a and the second resin frame sheet 36 b are disposed on both surfaces of the electrolyte membrane / electrode structure 34.

ここで、第1樹脂枠シート36aは、第1樹脂材44aが電解質膜・電極構造体34のカソード電極40に対向する一方、第2樹脂枠シート36bは、第1樹脂材44bが前記電解質膜・電極構造体34のアノード電極42に対向する。   Here, in the first resin frame sheet 36a, the first resin material 44a faces the cathode electrode 40 of the electrolyte membrane / electrode structure 34, while in the second resin frame sheet 36b, the first resin material 44b is formed of the electrolyte membrane. -It faces the anode electrode 42 of the electrode structure 34.

次に、図3中、(d)では、第1樹脂枠シート36a及び第2樹脂枠シート36bが、電解質膜・電極構造体34を構成する固体高分子電解質膜38の外周端部38endの両面を直接挟持した状態で、例えば、ホットプレス等により一体化される。 Next, in FIG. 3D, the first resin frame sheet 36a and the second resin frame sheet 36b are formed on the outer peripheral end 38end of the solid polymer electrolyte membrane 38 constituting the electrolyte membrane / electrode structure 34. In a state in which both surfaces are directly sandwiched, for example, they are integrated by a hot press or the like.

その際、第1樹脂材44a、44bの融点よりも高温で且つ第2樹脂材46a、46bの融点未満の温度を付与することによって、前記第1樹脂材44a、44bが溶融し、第1樹脂枠シート36a及び第2樹脂枠シート36bと固体高分子電解質膜38とが一体に接合される。これにより、樹脂製枠部材36が得られる。   At that time, by applying a temperature higher than the melting point of the first resin material 44a, 44b and lower than the melting point of the second resin material 46a, 46b, the first resin material 44a, 44b is melted and the first resin material 44a, 44b is melted. The frame sheet 36a and the second resin frame sheet 36b and the solid polymer electrolyte membrane 38 are joined together. Thereby, the resin frame member 36 is obtained.

そして、図3中、(e)に示すように、樹脂製枠部材36には、酸化剤ガス入口連通孔18a、冷却媒体入口連通孔20a、燃料ガス入口連通孔22a、酸化剤ガス出口連通孔18b、冷却媒体出口連通孔20b及び燃料ガス出口連通孔22bがトリミングにより貫通形成される。従って、樹脂枠付き電解質膜・電極構造体10が製造される。   3, the resin frame member 36 has an oxidant gas inlet communication hole 18a, a cooling medium inlet communication hole 20a, a fuel gas inlet communication hole 22a, and an oxidant gas outlet communication hole. 18b, the coolant outlet communication hole 20b and the fuel gas outlet communication hole 22b are formed by trimming. Therefore, the electrolyte membrane / electrode structure 10 with a resin frame is manufactured.

この場合、本実施形態では、樹脂製枠部材36は、低融点の第1樹脂材44a、44bと高融点の第2樹脂材46a、46bとが接合されるとともに、一対の前記第1樹脂材44a、44bが、固体高分子電解質膜38の外周端部38endの両面に直接接合(ホットプレス等)されている。このため、樹脂製枠部材36と固体高分子電解質膜38とが接合される際に、高融点の第2樹脂材46a、46bが溶融されることがなく、前記樹脂製枠部材36が変形することを確実に阻止することができる。 In this case, in the present embodiment, the resin frame member 36 is formed by joining the low-melting-point first resin materials 44a and 44b and the high-melting-point second resin materials 46a and 46b and a pair of the first resin materials. 44a, 44b are joined directly (hot press or the like) on both sides of the outer peripheral end portion 38 end the solid polymer electrolyte membrane 38. Therefore, when the resin frame member 36 and the solid polymer electrolyte membrane 38 are joined, the high melting point second resin materials 46a and 46b are not melted, and the resin frame member 36 is deformed. This can be reliably prevented.

従って、固体高分子電解質膜38の外周端部38endを周回して薄肉状の樹脂製枠部材36を強固且つ容易に接合するとともに、前記樹脂製枠部材36の変形を良好に抑制することが可能になる。これにより、樹脂製枠部材36を歩留まりよく、しかも組立工数の削減により効率的に製造することができるという効果が得られる。 Therefore, it is possible to firmly and easily join the thin resin frame member 36 by circling the outer peripheral end portion 38 end of the solid polymer electrolyte membrane 38 and to satisfactorily suppress deformation of the resin frame member 36. It becomes possible. Thereby, the effect that the resin-made frame members 36 can be efficiently manufactured with a high yield and a reduction in the number of assembly steps is obtained.

さらにまた、固体高分子電解質膜38の外周端部38endと樹脂製枠部材36の外周端部36endとの間の領域は、第1樹脂材44a、44b同士が直接接合されている。このため、第1樹脂枠シート36aと第2樹脂枠シート36bとは、強固且つ確実に接合され、樹脂製枠部材36と電解質膜・電極構造体34との接合硬度が良好に向上するという利点がある。 Furthermore, in the region between the outer peripheral end portion 38 end of the solid polymer electrolyte membrane 38 and the outer peripheral end portion 36 end of the resin frame member 36, the first resin materials 44a and 44b are directly bonded to each other. Therefore, the first resin frame sheet 36a and the second resin frame sheet 36b are bonded firmly and securely, and the bonding hardness between the resin frame member 36 and the electrolyte membrane / electrode structure 34 is improved favorably. There is.

このように構成される燃料電池12の動作について、以下に説明する。   The operation of the fuel cell 12 configured as described above will be described below.

先ず、図1に示すように、酸化剤ガス入口連通孔18aに酸素含有ガス等の酸化剤ガスが供給されるとともに、燃料ガス入口連通孔22aに水素含有ガス等の燃料ガスが供給される。さらに、冷却媒体入口連通孔20aに純水やエチレングリコール、オイル等の冷却媒体が供給される。   First, as shown in FIG. 1, an oxidant gas such as an oxygen-containing gas is supplied to the oxidant gas inlet communication hole 18a, and a fuel gas such as a hydrogen-containing gas is supplied to the fuel gas inlet communication hole 22a. Further, a cooling medium such as pure water, ethylene glycol, or oil is supplied to the cooling medium inlet communication hole 20a.

このため、酸化剤ガスは、酸化剤ガス入口連通孔18aから第1セパレータ14の酸化剤ガス流路24に導入される。酸化剤ガスは、矢印C方向下方に移動しながら、樹脂枠付き電解質膜・電極構造体10を構成するカソード電極40に供給される。   For this reason, the oxidant gas is introduced into the oxidant gas flow path 24 of the first separator 14 from the oxidant gas inlet communication hole 18a. The oxidant gas is supplied to the cathode electrode 40 constituting the electrolyte membrane / electrode structure 10 with a resin frame while moving downward in the direction of arrow C.

一方、燃料ガスは、燃料ガス入口連通孔22aから第2セパレータ16の燃料ガス流路26に導入される。この燃料ガスは、矢印C方向下方に移動しながら、樹脂枠付き電解質膜・電極構造体10を構成するアノード電極42に供給される。   On the other hand, the fuel gas is introduced into the fuel gas flow path 26 of the second separator 16 from the fuel gas inlet communication hole 22a. This fuel gas is supplied to the anode electrode 42 constituting the electrolyte membrane / electrode structure 10 with a resin frame while moving downward in the direction of arrow C.

従って、樹脂枠付き電解質膜・電極構造体10では、カソード電極40に供給される酸化剤ガスと、アノード電極42に供給される燃料ガスとが、電極触媒層40a、42a内で電気化学反応により消費され、発電が行われる。   Therefore, in the electrolyte membrane / electrode structure 10 with the resin frame, the oxidant gas supplied to the cathode electrode 40 and the fuel gas supplied to the anode electrode 42 are electrochemically reacted in the electrode catalyst layers 40a and 42a. It is consumed and power is generated.

次いで、カソード電極40に供給されて消費された酸化剤ガスは、酸化剤ガス出口連通孔18bに沿って矢印A方向に排出される。一方、アノード電極42に供給されて消費された燃料ガスは、燃料ガス出口連通孔22bに沿って矢印A方向に排出される。   Next, the oxidant gas consumed by being supplied to the cathode electrode 40 is discharged in the direction of arrow A along the oxidant gas outlet communication hole 18b. On the other hand, the fuel gas consumed by being supplied to the anode electrode 42 is discharged in the direction of arrow A along the fuel gas outlet communication hole 22b.

また、冷却媒体入口連通孔20aに供給された冷却媒体は、第1及び第2セパレータ14、16間の冷却媒体流路28に導入され、矢印C方向下方に流通する。この冷却媒体は、樹脂枠付き電解質膜・電極構造体10を冷却した後、冷却媒体出口連通孔20bに排出される。   The cooling medium supplied to the cooling medium inlet communication hole 20a is introduced into the cooling medium flow path 28 between the first and second separators 14 and 16, and flows downward in the direction of arrow C. This cooling medium is discharged to the cooling medium outlet communication hole 20b after the electrolyte membrane / electrode structure 10 with a resin frame is cooled.

10…樹脂枠付き電解質膜・電極構造体 12…燃料電池
14、16…セパレータ 18a…酸化剤ガス入口連通孔
18b…酸化剤ガス出口連通孔 20a…冷却媒体入口連通孔
20b…冷却媒体出口連通孔 22a…燃料ガス入口連通孔
22b…燃料ガス出口連通孔 24…酸化剤ガス流路
26…燃料ガス流路 28…冷却媒体流路
34…電解質膜・電極構造体 36…樹脂製枠部材
36a、36b…樹脂枠シート 38…固体高分子電解質膜
40…カソード電極 42…アノード電極
36end、38end、40end、42end…外周端部
40a、42a…電極触媒層 40b、42b…ガス拡散層
44a、44b、46a、46b…樹脂材 50a、50b…接合シート
DESCRIPTION OF SYMBOLS 10 ... Electrolyte membrane electrode assembly with resin frame 12 ... Fuel cell 14, 16 ... Separator 18a ... Oxidant gas inlet communication hole 18b ... Oxidant gas outlet communication hole 20a ... Cooling medium inlet communication hole 20b ... Cooling medium outlet communication hole 22a ... Fuel gas inlet communication hole 22b ... Fuel gas outlet communication hole 24 ... Oxidant gas flow channel 26 ... Fuel gas flow channel 28 ... Cooling medium flow channel 34 ... Electrolyte membrane / electrode structure 36 ... Resin frame members 36a, 36b ... resin frame sheet 38 ... solid polymer electrolyte membrane 40 ... cathode electrode 42 ... anode electrode 36 end , 38 end , 40 end , 42 end ... outer peripheral edge 40a, 42a ... electrode catalyst layer 40b, 42b ... gas diffusion layer 44a, 44b, 46a, 46b ... Resin material 50a, 50b ... Joining sheet

Claims (3)

固体高分子電解質膜の両側に、それぞれ電極触媒層とガス拡散層とを有する電極が設けられるとともに、前記ガス拡散層の外周端部から外方に前記固体高分子電解質膜の外周端部が突出する電解質膜・電極構造体と、
前記固体高分子電解質膜の外周を周回して設けられるとともに、前記電極の表面と段差なく且つ同一面上に連続する樹脂製枠部材と、
を備える燃料電池用樹脂枠付き電解質膜・電極構造体であって、
前記樹脂製枠部材は、前記固体高分子電解質膜の外周端部に直接接合される第1樹脂材と、
前記第1樹脂材の外面に接合されるとともに、該第1樹脂材よりも融点が高い第2樹脂材と、
を備え
前記固体高分子電解質膜の外周端部は、前記樹脂製枠部材の外周端部の内側に配置されるとともに、
前記固体高分子電解質膜の外周端部と前記樹脂製枠部材の外周端部との間の領域は、前記第1樹脂材同士が直接接合されることを特徴とする燃料電池用樹脂枠付き電解質膜・電極構造体。
Electrodes having an electrode catalyst layer and a gas diffusion layer are provided on both sides of the solid polymer electrolyte membrane, respectively, and the outer peripheral edge of the solid polymer electrolyte membrane protrudes outward from the outer peripheral edge of the gas diffusion layer An electrolyte membrane / electrode structure,
A resin frame member that is provided around the outer periphery of the solid polymer electrolyte membrane and that is continuous with the surface of the electrode without any step ,
An electrolyte membrane / electrode structure with a resin frame for a fuel cell comprising:
The resin frame member is a first resin material joined directly to the outer peripheral end of the solid polymer electrolyte membrane;
A second resin material bonded to the outer surface of the first resin material and having a melting point higher than that of the first resin material;
Equipped with a,
The outer peripheral end of the solid polymer electrolyte membrane is disposed inside the outer peripheral end of the resin frame member,
The solid polymer region between the outer end portion of the outer circumferential edge of the electrolyte membrane and the resin frame component for a fuel cell resin frame with an electrolyte, wherein the first resin material to each other, characterized in Rukoto joined directly Membrane / electrode structure.
固体高分子電解質膜の両側に、それぞれ電極触媒層とガス拡散層とを有する電極が設けられるとともに、前記ガス拡散層の外周端部から外方に前記固体高分子電解質膜の外周端部が突出する電解質膜・電極構造体と、
前記固体高分子電解質膜の外周を周回して設けられるとともに、前記電極の表面と段差なく且つ同一面上に連続する樹脂製枠部材と、
を備える燃料電池用樹脂枠付き電解質膜・電極構造体の製造方法であって、
第1樹脂材と前記第1樹脂材よりも融点が高い第2樹脂材とを接合し、一対の前記樹脂製枠部材を作製する工程と、
各樹脂製枠部材の前記第1樹脂材により、前記固体高分子電解質膜の外周端部を直接挟持した状態で、前記第1樹脂材の融点よりも高温で且つ前記第2樹脂材の融点未満の温度を付与することによって、一対の前記樹脂製枠部材と前記固体高分子電解質膜とを一体に接合する工程と、
を有し、
前記固体高分子電解質膜の外周端部は、前記樹脂製枠部材の外周端部の内側に配置されるとともに、
前記固体高分子電解質膜の外周端部と前記樹脂製枠部材の外周端部との間の領域は、前記第1樹脂材同士が直接接合されることを特徴とする燃料電池用樹脂枠付き電解質膜・電極構造体の製造方法。
Electrodes having an electrode catalyst layer and a gas diffusion layer are provided on both sides of the solid polymer electrolyte membrane, respectively, and the outer peripheral edge of the solid polymer electrolyte membrane protrudes outward from the outer peripheral edge of the gas diffusion layer An electrolyte membrane / electrode structure,
A resin frame member that is provided around the outer periphery of the solid polymer electrolyte membrane and that is continuous with the surface of the electrode without any step ,
A method for producing an electrolyte membrane / electrode structure with a resin frame for a fuel cell, comprising:
Bonding a first resin material and a second resin material having a melting point higher than that of the first resin material to produce a pair of the resin frame members;
With the first resin material of each resin frame member directly sandwiching the outer peripheral end of the solid polymer electrolyte membrane, the temperature is higher than the melting point of the first resin material and less than the melting point of the second resin material. A step of integrally bonding the pair of the resin-made frame members and the solid polymer electrolyte membrane by applying a temperature of
I have a,
The outer peripheral end of the solid polymer electrolyte membrane is disposed inside the outer peripheral end of the resin frame member,
The solid polymer region between the outer end portion of the outer circumferential edge of the electrolyte membrane and the resin frame component for a fuel cell resin frame with an electrolyte, wherein the first resin material to each other, characterized in Rukoto joined directly Manufacturing method of membrane / electrode structure.
請求項記載の製造方法において、前記樹脂製枠部材には、それぞれ燃料ガス、酸化剤ガス及び冷媒体を流通させる複数の連通孔が貫通形成されることを特徴とする燃料電池用樹脂枠付き電解質膜・電極構造体の製造方法。 3. The manufacturing method according to claim 2 , wherein the resin frame member is formed with a plurality of communication holes through which fuel gas, oxidant gas, and a refrigerant body circulate, respectively. Manufacturing method of electrolyte membrane / electrode structure.
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CN111435761B (en) * 2019-01-11 2021-08-10 荣盛盟固利新能源科技有限公司 All-solid-state lithium ion battery and hot-pressing preparation method of multilayer electrolyte membrane thereof

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