JPH1171692A - Production of joinded body of ion-exchange membrane and electrode and production device therefor - Google Patents

Production of joinded body of ion-exchange membrane and electrode and production device therefor

Info

Publication number
JPH1171692A
JPH1171692A JP10182570A JP18257098A JPH1171692A JP H1171692 A JPH1171692 A JP H1171692A JP 10182570 A JP10182570 A JP 10182570A JP 18257098 A JP18257098 A JP 18257098A JP H1171692 A JPH1171692 A JP H1171692A
Authority
JP
Japan
Prior art keywords
exchange membrane
ion exchange
electrode
ion
perforated plate
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
JP10182570A
Other languages
Japanese (ja)
Inventor
Miyako Hitomi
美也子 人見
Kazuhiko Nagayama
一彦 永山
Mikimasa Yamaguchi
幹昌 山口
Kayoko Okisawa
加代子 沖沢
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Fuji Electric Co Ltd
Original Assignee
Fuji Electric Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Fuji Electric Co Ltd filed Critical Fuji Electric Co Ltd
Priority to JP10182570A priority Critical patent/JPH1171692A/en
Publication of JPH1171692A publication Critical patent/JPH1171692A/en
Pending legal-status Critical Current

Links

Classifications

    • 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

PROBLEM TO BE SOLVED: To produce a high-quality joined body at a low cost by supplying a catalyst dispersion between the opposed faces of the ion-exchange membrane and perforated plate and discharging the solvent of the dispersion outside the perforated plate to form a catalyst grain layer on the membrane to produce an electrode. SOLUTION: A catalyst dispersion 20 is supplied into the spaces 5a and 5b partitioned by the ion-exchange membrane 4 and perforated plates 2a and 2b, and then a filtrate tank 12 is evacuated by a vacuum pump 14. The negative pressure acts on the openings of the perforated plates 2a and 2b fixed to fixed plates 1a and 1b, and the solvent of the dispersion 20 is discharged finally into the filtrate tank 12 through the openings. Meanwhile, the layer of the catalyst grains of the dispersion 20 is formed between the perforated plates 2a and 2b and the membrane 4. The layer is heated by heating plates 15a and 15b and pressed by a press 19. Consequently, the joined body of the electrode consisting of the catalyst grain layer and membrane 4 is produced with a high adhesion.

Description

【発明の詳細な説明】DETAILED DESCRIPTION OF THE INVENTION

【０００１】[0001]

【発明の属する技術分野】本発明はイオン交換膜と電極
の接合体の製作方法および製作装置に関する。本発明に
よる接合体は、特に、燃料電池、水電解装置、食塩電解
装置、塩酸電解装置、オゾン水製造装置、酸素または水
素の分離装置、各種ガスセンサー等の電気化学装置に用
いることができる。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method and an apparatus for manufacturing a joined body of an ion exchange membrane and an electrode. The joined body according to the present invention can be used particularly for electrochemical devices such as fuel cells, water electrolysis devices, salt electrolysis devices, hydrochloric acid electrolysis devices, ozone water production devices, oxygen or hydrogen separation devices, and various gas sensors.

【０００２】[0002]

【従来の技術】イオン交換膜と電極との接合体は、一般
に膜状に形成された２枚の電極の間にイオン交換膜を挟
んで、加熱、加圧するホットプレス法によって製作され
る。この方法では、高分子板の表面に触媒粒子の分散液
を塗布した後乾燥したり、または濾材の表面に濾過によ
って触媒粒子層を抄造した後乾燥して作製した電極をイ
オン交換膜の表面に加熱、加圧して製作していた。2. Description of the Related Art A bonded body of an ion-exchange membrane and an electrode is generally manufactured by a hot press method in which an ion-exchange membrane is sandwiched between two electrodes formed in a film shape and heated and pressed. In this method, an electrode prepared by applying a dispersion of catalyst particles to the surface of a polymer plate and drying it, or forming a catalyst particle layer by filtration on the surface of a filter medium and then drying, is applied to the surface of the ion exchange membrane. It was made by heating and pressing.

【０００３】しかし、上述した従来の方法で製作される
接合体では、イオン交換膜と電極との接合部の結合強度
が低く、電極が剥離して、電極とイオン交換膜との接合
部界面の電気抵抗が高くなり、長期に安定して高い特性
が得られない欠点があった。However, in the bonded body manufactured by the above-described conventional method, the bonding strength at the junction between the ion-exchange membrane and the electrode is low, and the electrode is peeled off, and the interface at the junction between the electrode and the ion-exchange membrane is reduced. There was a drawback that the electric resistance was increased and high characteristics could not be obtained stably for a long period of time.

【０００４】このような問題を解決する固体高分子膜
（イオン交換膜）と電極との接合体の製造方法として、
特開平３−２０８２６２号公報には２枚の電極で固体高
分子電解質膜を挟持した挟持体をアルコール類、ケトン
類又はエーテル類等の有機溶媒やこれらの有機溶媒と水
の混合溶媒中で加熱・加圧（ホットプレス）することに
より接合体とする方法が開示されている。そしてこのよ
うな方法によると、固体高分子膜が溶媒中で軟化又はそ
の一部が溶解して膨潤した状態となるので、ガス拡散電
極との接合が容易となり、また、固体高分子電解質膜が
ガス拡散電極の反応膜内に入り込み易いので触媒反応面
積が大きくなる等によりイオン導電抵抗が低下すること
が記載されている。[0004] As a method of manufacturing a joined body of a solid polymer membrane (ion exchange membrane) and an electrode to solve such a problem,
JP-A-3-208262 discloses that a sandwich in which a solid polymer electrolyte membrane is sandwiched between two electrodes is heated in an organic solvent such as alcohols, ketones or ethers, or a mixed solvent of these organic solvents and water. A method of forming a joined body by pressing (hot pressing) is disclosed. According to such a method, the solid polymer membrane is softened in a solvent or partially dissolved and becomes a swollen state, so that the bonding with the gas diffusion electrode becomes easy, and the solid polymer electrolyte membrane is It is described that the ion conductive resistance is reduced due to an increase in the catalytic reaction area because the catalyst easily enters the reaction film of the gas diffusion electrode.

【０００５】[0005]

【発明が解決しようとする課題】上記の方法において
は、触媒層は予め別途製作された電極の一面に形成され
ており、この電極の触媒層側の面をイオン交換膜に接し
て配置して溶媒中で接合体に形成するものである。この
ように溶媒中で電極とイオン交換膜とをホットプレスし
て接合体を製造する方法により、有機溶媒又はアルコー
ル中で軟化膨潤したイオン交換膜が触媒層中に入り込む
ことによる触媒反応面積の増大は、発電特性を改善した
が、未ださらなる高特性の要求は大きい。In the above-mentioned method, the catalyst layer is formed on one surface of an electrode manufactured separately in advance, and the surface of the electrode on the catalyst layer side is arranged in contact with the ion exchange membrane. It is formed into a conjugate in a solvent. In this way, the method of hot-pressing the electrode and the ion-exchange membrane in a solvent to produce a joined body increases the catalytic reaction area due to the ion-exchange membrane softened and swollen in an organic solvent or alcohol entering the catalyst layer. Has improved power generation characteristics, but there is still a great demand for higher characteristics.

【０００６】また、上記の方法では、予め触媒層の形成
された電極を用いており、電極への触媒層の形成工程は
別途必要で、製造工程や製造装置数が多くなり、高コス
トとなる欠点があった。本願発明は、上述の要求を満足
すべくさらなる高特性の接合体を提供し、しかも同時
に、上記課題を解決して製造工程の連続化による製造時
間の短縮、低コストを実現し、大量生産可能な接合体の
制作方法を提供するものである。Further, in the above method, an electrode on which a catalyst layer is formed in advance is used, and a step of forming a catalyst layer on the electrode is separately required, which increases the number of manufacturing steps and the number of manufacturing apparatuses, resulting in high cost. There were drawbacks. The invention of the present application provides a joined body having higher characteristics to satisfy the above requirements, and at the same time, solves the above-mentioned problems, realizes a shortened manufacturing time and a low cost by continuation of the manufacturing process, and enables mass production. It is intended to provide a method for producing a complex joint.

【０００７】[0007]

【課題を解決するための手段】本発明によるイオン交換
膜と電極の接合体の製作方法の第１の態様は、イオン交
換膜と多孔板を対面して配置する工程、および前記イオ
ン交換膜と前記多孔板の対向する面の間に触媒分散液を
供給し、かつ該触媒分散液の溶媒を前記多孔板の外側に
排出してイオン交換膜上に触媒粒子層を形成して電極と
する工程を有する。According to a first aspect of the present invention, there is provided a method of manufacturing a bonded body of an ion exchange membrane and an electrode, comprising the steps of arranging the ion exchange membrane and a porous plate facing each other, A step of supplying a catalyst dispersion between opposing surfaces of the perforated plate, and discharging a solvent of the catalyst dispersion to the outside of the perforated plate to form a catalyst particle layer on an ion exchange membrane to form an electrode. Having.

【０００８】本発明によるイオン交換膜と電極の接合体
の製作方法の第２の態様は、イオン交換膜、電極および
多孔板を重ねる工程、前記多孔板の空隙にイオン交換樹
脂液を供給し、前記電極の空隙内および前記イオン交換
膜の表面に前記イオン交換樹脂液を拡散含浸する工程、
および前記イオン交換膜、電極および多孔板を加熱して
拡散含浸したイオン交換樹脂液の溶媒を蒸発除去して前
記電極およびイオン交換膜の表面にイオン交換樹脂の皮
膜を形成する工程を有する。[0008] A second aspect of the method for producing a bonded body of an ion-exchange membrane and an electrode according to the present invention is a step of stacking an ion-exchange membrane, an electrode and a perforated plate, supplying an ion-exchange resin liquid to a void of the perforated plate, A step of diffusing and impregnating the ion-exchange resin liquid in the gaps of the electrode and on the surface of the ion-exchange membrane,
And a step of heating the ion-exchange membrane, the electrode and the perforated plate to evaporate and removing the solvent of the ion-exchange resin liquid which has been diffusely impregnated, thereby forming a film of the ion-exchange resin on the surface of the electrode and the ion-exchange membrane.

【０００９】本発明によるイオン交換膜と電極の接合体
の製作方法の第３の態様は、イオン交換膜、電極および
多孔板を重ねる工程、前記多孔板の空隙に膨潤用液を供
給し、前記電極の空隙を通して前記イオン交換膜の表面
に膨潤用液を含浸させる工程、および前記イオン交換
膜、電極および多孔板を加熱、加圧して前記イオン交換
膜と前記電極とを接合する工程を有する。In a third aspect of the method for producing a bonded body of an ion-exchange membrane and an electrode according to the present invention, a step of stacking an ion-exchange membrane, an electrode and a perforated plate, supplying a swelling liquid to a void of the perforated plate, A step of impregnating the surface of the ion-exchange membrane with a swelling liquid through the gap of the electrode; and a step of heating and pressurizing the ion-exchange membrane, the electrode, and the porous plate to join the ion-exchange membrane and the electrode.

【００１０】本発明によるイオン交換膜と電極の接合体
の製作方法の第４の態様は、イオン交換膜、電極および
多孔板を重ねる工程、前記多孔板の空隙にイオン交換樹
脂を含有した膨潤用液を供給し、前記電極の空隙を通し
て前記イオン交換膜の表面に膨潤用液を含浸させてイオ
ン交換膜を膨潤させると共に前記電極の空隙内および前
記イオン交換膜の表面に前記イオン交換樹脂液を拡散含
浸する工程、および前記イオン交換膜、電極および多孔
板を加熱、加圧して前記電極およびイオン交換膜の表面
にイオン交換樹脂の皮膜を形成して前記イオン交換膜と
前記電極とを接合する工程を有する。[0010] A fourth aspect of the method for producing a bonded body of an ion exchange membrane and an electrode according to the present invention is a step of laminating an ion exchange membrane, an electrode and a perforated plate, for swelling containing an ion exchange resin in the voids of the perforated plate. The liquid is supplied, and the surface of the ion exchange membrane is impregnated with the swelling liquid through the gap of the electrode to swell the ion exchange membrane, and the ion exchange resin liquid is filled in the gap of the electrode and the surface of the ion exchange membrane. Diffusion impregnating, and heating and pressurizing the ion exchange membrane, the electrode and the perforated plate to form an ion exchange resin film on the surface of the electrode and the ion exchange membrane, and joining the ion exchange membrane and the electrode. Having a process.

【００１１】本発明によるイオン交換膜と電極の接合体
の製作方法の第５の態様は、イオン交換膜と多孔板を対
面して配置する工程、前記イオン交換膜と前記多孔板の
対向する面の間に触媒分散液を供給し、かつ該触媒分散
液の溶媒を前記多孔板の外側に排出してイオン交換膜上
に触媒粒子層を形成して電極とする工程、前記多孔板の
空隙にイオン交換樹脂液を供給し、前記電極の空隙内お
よび前記イオン交換膜の表面に前記イオン交換樹脂液を
拡散含浸する工程、および前記イオン交換膜、電極およ
び多孔板を加熱して拡散含浸したイオン交換樹脂液の溶
媒を蒸発除去して前記電極およびイオン交換膜の表面に
イオン交換樹脂の皮膜を形成する工程、前記多孔板の空
隙に膨潤用液を供給し、前記電極の空隙を通して前記イ
オン交換膜の表面に膨潤用液を含浸させてイオン交換膜
を膨潤させる工程、および前記イオン交換膜、電極およ
び多孔板を加熱、加圧して前記イオン交換膜と前記電極
とを接合する工程を有する。A fifth aspect of the method for producing a bonded body of an ion-exchange membrane and an electrode according to the present invention is a step of arranging the ion-exchange membrane and the porous plate so as to face each other, and the opposing surfaces of the ion-exchange membrane and the porous plate. Supplying a catalyst dispersion during, and discharging the solvent of the catalyst dispersion to the outside of the porous plate to form a catalyst particle layer on the ion exchange membrane to form an electrode; A step of supplying an ion-exchange resin liquid and diffusing and impregnating the ion-exchange resin liquid in the gaps of the electrode and on the surface of the ion-exchange membrane, and heating and diffusing and impregnating the ion-exchange membrane, the electrode and the perforated plate; Evaporating and removing the solvent of the exchange resin liquid to form a film of the ion exchange resin on the surface of the electrode and the ion exchange membrane, supplying a swelling liquid to the gap of the perforated plate, and performing the ion exchange through the gap of the electrode. Membrane surface The swelling liquid impregnated with the step of the bonding process to swell the ion exchange membrane, and the ion-exchange membrane, heating the electrodes and the perforated plate, and said a pressurizing said ion-exchange membrane electrode.

【００１２】本発明によるイオン交換膜と電極の接合体
の製作装置の第１の態様は、互いに対向し、それぞれ表
面に多孔板が取り付けられている２組の固定板と、該２
組の固定板の間に設けられ、２組の固定板と共にイオン
交換膜と電極とを収容する空間を形成する封止材と、前
記空間に触媒分散液を供給する手段と、前記多孔板を通
して前記空間から前記触媒分散液の溶媒を排出する手段
と、前記イオン交換膜と電極を加熱、加圧する手段とを
備えている。A first aspect of the apparatus for manufacturing a bonded body of an ion exchange membrane and an electrode according to the present invention comprises two sets of fixed plates opposed to each other and each having a perforated plate attached to the surface thereof.
A sealing material provided between a pair of fixed plates, forming a space for accommodating the ion exchange membrane and the electrode together with the two sets of fixed plates, a means for supplying a catalyst dispersion to the space, and the space through the perforated plate And a means for heating and pressurizing the ion exchange membrane and the electrode.

【００１３】本発明によるイオン交換膜と電極の接合体
の製作装置の第２の態様は、互いに対向し、それぞれ表
面に多孔板が取り付けられている２組の固定板と、該２
組の固定板の間に設けられイオン交換膜と電極とを固定
する封止材と、前記多孔板を通して前記イオン交換膜と
電極にイオン交換樹脂液を供給する手段と、前記多孔板
を通して前記イオン交換樹脂液の蒸発溶媒を排出する手
段と、前記イオン交換膜と電極を加熱、加圧する手段と
を備えている。A second aspect of the apparatus for manufacturing a bonded body of an ion exchange membrane and an electrode according to the present invention comprises two sets of fixed plates opposed to each other and each having a perforated plate attached to the surface thereof.
A sealing material provided between a set of fixing plates to fix the ion exchange membrane and the electrode, a means for supplying the ion exchange resin liquid to the ion exchange membrane and the electrode through the porous plate, and the ion exchange resin through the porous plate Means for discharging the evaporated solvent of the liquid, and means for heating and pressurizing the ion exchange membrane and the electrode are provided.

【００１４】本発明によるイオン交換膜と電極の接合体
の製作装置の第３の態様は、互いに対向し、それぞれ表
面に多孔板が取り付けられている２組の固定板と、該２
組の固定板の間に設けられイオン交換膜と電極とを固定
する封止材と、前記多孔板を通して前記イオン交換膜と
電極に膨潤用液を供給する手段と、前記多孔板を通して
前記膨潤用液の蒸気を排出する手段と、前記イオン交換
膜と電極を加熱、加圧する手段とを備えている。A third aspect of the apparatus for manufacturing an ion-exchange membrane / electrode assembly according to the present invention comprises two sets of fixed plates opposed to each other and each having a perforated plate attached to the surface thereof.
A sealing material provided between a set of fixed plates to fix the ion exchange membrane and the electrode, a means for supplying a swelling liquid to the ion exchange membrane and the electrode through the porous plate, and a swelling liquid through the porous plate. Means for discharging steam, and means for heating and pressurizing the ion exchange membrane and the electrode are provided.

【００１５】本発明によるイオン交換膜と電極の接合体
の製作装置の第４の態様は、互いに対向し、それぞれ表
面に多孔板が取り付けられている２組の固定板と、該２
組の固定板の間に設けられ、２組の固定板と共にイオン
交換膜と電極とを収容する空間を形成する封止材と、前
記空間に触媒分散液を供給する手段と、前記空間にイオ
ン交換樹脂液を供給する手段と、前記空間に膨潤用液を
供給する手段と、それぞれ前記多孔板を通して前記空間
から、前記触媒分散液の溶媒を排出する手段と前記イオ
ン交換樹脂液の蒸発溶媒および前記膨潤用液の蒸気を排
出する手段と、前記イオン交換膜と電極を加熱、加圧す
る手段とを備えている。A fourth aspect of the apparatus for manufacturing an ion-exchange membrane / electrode assembly according to the present invention comprises two sets of fixed plates opposed to each other and each having a perforated plate attached to the surface thereof.
A sealing member provided between a pair of fixed plates, forming a space for accommodating the ion exchange membrane and the electrode together with the two sets of fixed plates; a means for supplying a catalyst dispersion to the space; and an ion exchange resin in the space. A means for supplying a liquid, a means for supplying a swelling liquid to the space, a means for discharging a solvent of the catalyst dispersion liquid from the space through the perforated plate, and a solvent for evaporating the ion exchange resin liquid and the swelling. Means for discharging the vapor of the liquid for use and means for heating and pressurizing the ion exchange membrane and the electrode are provided.

【００１６】[0016]

【発明の実施の形態】図１、図２および図３は、それぞ
れ本発明による接合体の製作装置の異なる実施例の構成
を示す断面図である。1, 2, and 3 are cross-sectional views each showing a configuration of a different embodiment of an apparatus for manufacturing a joined body according to the present invention.

【００１７】図１の装置において、それぞれ２組の固定
板１ａ，１ｂの表面に取り付けられている多孔板２ａ，
２ｂと固定板１ａ，１ｂの端部に取り付けた封止材（パ
ッキング）３ａ，３ｂとによって密閉空間が形成され
る。封止材３ａ，３ｂは、例えば弾性シリコンゴムある
はアクリル系弾性ゴム等の変形能の大きな材料からな
る。この密閉空間内にイオン交換膜４が配置され、封止
材３ａ，３ｂによって封止されている。従って、イオン
交換膜４とその上下の多孔板２ａ，２ｂの間には空間５
ａ，５ｂが形成される。封止材３ａ，３ｂには空間５
ａ，５ｂに開口する触媒分散液供給通路６ａ，６ｂが設
けられ、この触媒分散液供給通路６ａ，６ｂは配管７
ａ，７ｂおよび仕切り弁８ａ，８ｂを介して触媒分散液
槽９ａ，９ｂに接続している。空間５ａ，５ｂの高さ
（イオン交換膜と多孔板との距離）は、触媒分散液槽９
ａ，９ｂからの触媒分散液が空間内に一様に供給され得
る大きさであり、具体的には、例えば数ｍｍ程度であ
る。一方、固定板１ａ，１ｂには多孔板２ａ，２ｂに接
して開口し空間５ａ，５ｂの外部に連通する濾液排出通
路１０ａ，１０ｂが設けられており、この濾液排出通路
１０ａ，１０ｂには配管１１が接続され、配管１１は濾
液タンク１２に接続している。さらに、濾液タンク１２
には配管１３を介して真空ポンプ１４が接続されてい
る。固定板１ａ，１ｂの多孔板２ａ，２ｂと反対の面に
はヒータ１６ａ，１６ｂが取り付けられた加熱板１５
ａ，１５ｂが配設され、固定板１ａ，１ｂには温度セン
サ１７ａ，１７ｂが挿入されている。加熱板１５ａ，１
５ｂは断熱板１８ａ，１８ｂを介してプレス装置１９の
プレス板１９ａ，１９ｂの間に配置されている。In the apparatus shown in FIG. 1, perforated plates 2a, 2a, 2a, 2b,
An enclosed space is formed by the sealing material (packing) 3a, 3b attached to the end of the fixing plate 1a, 1b. The sealing members 3a and 3b are made of a material having a large deformability, such as elastic silicon rubber or acrylic elastic rubber. The ion exchange membrane 4 is arranged in the closed space, and is sealed by the sealing materials 3a and 3b. Therefore, a space 5 is provided between the ion exchange membrane 4 and the upper and lower perforated plates 2a and 2b.
a, 5b are formed. A space 5 is provided in the sealing materials 3a and 3b.
The catalyst dispersion liquid supply passages 6a and 6b are provided to open into the pipes 7a and 5b.
a, 7b and gate valves 8a, 8b are connected to catalyst dispersion tanks 9a, 9b. The height of the spaces 5a and 5b (the distance between the ion exchange membrane and the perforated plate) depends on the catalyst dispersion tank 9
The size is such that the catalyst dispersion liquid from a and 9b can be uniformly supplied into the space, and specifically, for example, about several mm. On the other hand, the fixed plates 1a, 1b are provided with filtrate discharge passages 10a, 10b which are opened in contact with the porous plates 2a, 2b and communicate with the outside of the spaces 5a, 5b. 11 is connected, and the pipe 11 is connected to the filtrate tank 12. Further, the filtrate tank 12
Is connected to a vacuum pump 14 via a pipe 13. Heating plate 15 on which heaters 16a and 16b are attached is provided on the surface of fixed plates 1a and 1b opposite to perforated plates 2a and 2b.
a, 15b are provided, and temperature sensors 17a, 17b are inserted into the fixed plates 1a, 1b. Heating plate 15a, 1
5b is arranged between the press plates 19a and 19b of the press device 19 via the heat insulating plates 18a and 18b.

【００１８】図１の装置を用いてイオン交換膜と電極と
の接合体を製作する方法について説明する。図示するよ
うに、イオン交換膜４を固定板１ａ，１ｂに設けられた
封止材３ａ，３ｂの間に配置し、固定板１ａ，１ｂがプ
レス装置１９のプレス板１９ａ，１９ｂに断熱板１８
ａ，１８ｂを介して配置された加熱板１５ａ，１５ｂに
接するように設置する。触媒分散液槽９ａ，９ｂに触媒
分散液２０を満たし、仕切り弁８ａ，８ｂを開いて、封
止材３ａ，３ｂに設けられた触媒分散液供給通路６ａ，
６ｂを通してイオン交換膜４と多孔板２ａ，２ｂで仕切
られた空間５ａ，５ｂ内に触媒分散液２０を供給する。
次いで、濾液タンク１２に接続した真空ポンプ１４を作
動して濾液タンク１２内を負圧にする。その結果、固定
板１ａ，１ｂの表面に取り付けた多孔板２ａ，２ｂの空
隙内に負圧が作用し、空間５ａ，５ｂ内の触媒分散液２
０の溶媒が多孔板２ａ，２ｂの空隙と固定板１ａ，１ｂ
の濾液排出通路１０ａ，１０ｂおよび配管１１を経由し
て濾液タンク１２に排出される。一方、多孔板２ａ，２
ｂとイオン交換膜４との間には触媒分散液２０の触媒粒
子が層状に形成される。そこで、ヒータ１６ａ，１６ｂ
に電流を流して加熱板１５ａ，１５ｂを加熱するととも
に、プレス装置１９によって固定板１ａ，１ｂを加圧す
る。この時、前述したように封止材３ａ，３ｂは弾性変
形能の大きな材料でできているので、プレス装置による
加圧は触媒粒子層からなる電極に及び、触媒粒子層から
なる電極をイオン交換膜４の面上に圧接する。このよう
にして、電極のイオン交換膜と接する面がイオン交換膜
内に食い込んで、高い結合強度を有するイオン交換膜と
電極との接合体が製作される。A method for manufacturing a joined body of an ion exchange membrane and an electrode using the apparatus shown in FIG. 1 will be described. As shown in the figure, the ion exchange membrane 4 is disposed between the sealing members 3a and 3b provided on the fixed plates 1a and 1b, and the fixed plates 1a and 1b are attached to the heat insulating plates 18a and 19b of the press device 19.
The heating plates 15a and 15b are disposed so as to be in contact with the heating plates 15a and 15b arranged via the a and 18b. The catalyst dispersion tanks 9a and 9b are filled with the catalyst dispersion liquid 20, the gate valves 8a and 8b are opened, and the catalyst dispersion liquid supply passages 6a and 6b provided in the sealing members 3a and 3b are opened.
The catalyst dispersion liquid 20 is supplied into the spaces 5a and 5b separated by the ion exchange membrane 4 and the perforated plates 2a and 2b through 6b.
Next, the vacuum pump 14 connected to the filtrate tank 12 is operated to make the inside of the filtrate tank 12 a negative pressure. As a result, a negative pressure acts on the voids of the perforated plates 2a, 2b attached to the surfaces of the fixed plates 1a, 1b, and the catalyst dispersion 2 in the spaces 5a, 5b.
0 solvent and the gap between the perforated plates 2a, 2b and the fixed plates 1a, 1b
Is discharged to the filtrate tank 12 via the filtrate discharge passages 10a and 10b and the pipe 11. On the other hand, the perforated plates 2a, 2a
The catalyst particles of the catalyst dispersion liquid 20 are formed in a layer between b and the ion exchange membrane 4. Therefore, the heaters 16a, 16b
The heating plates 15a and 15b are heated by applying an electric current to the fixing plates 1a and 1b by the pressing device 19. At this time, since the sealing members 3a and 3b are made of a material having a large elastic deformation ability as described above, the pressurization by the press device is applied to the electrodes composed of the catalyst particle layer and the electrodes composed of the catalyst particle layer are ion-exchanged. It is pressed against the surface of the membrane 4. In this way, the surface of the electrode in contact with the ion-exchange membrane digs into the ion-exchange membrane, and a conjugate of the electrode and the ion-exchange membrane having high bonding strength is manufactured.

【００１９】触媒分散液層９ａ，９ｂに同じ触媒分散液
を収容しておけばイオン交換膜の両面に同質の電極を形
成することができ、異なる触媒分散液を収容しておけば
イオン交換膜の両面に異なる電極を形成することができ
る。If the same catalyst dispersion is contained in the catalyst dispersion layers 9a and 9b, electrodes of the same quality can be formed on both surfaces of the ion exchange membrane. Different electrodes can be formed on both surfaces of the substrate.

【００２０】図１に示した実施例では、触媒分散液槽を
２個設けているが、収容される触媒分散液が同じ場合に
は、触媒分散液槽を１個とし、配管系統を２組にしても
良いことは言うまでもない。In the embodiment shown in FIG. 1, two catalyst dispersion liquid tanks are provided. However, when the same catalyst dispersion liquid is contained, one catalyst dispersion liquid tank is used and two sets of piping systems are provided. Needless to say, this is acceptable.

【００２１】図２の装置においては、予め製作された多
孔性の、あるいは多くの空隙を有する２枚の電極３０
ａ，３０ｂに挟まれたイオン交換膜４が多孔板２ａ，２
ｂの間に配置され、封止板３ａ，３ｂによって封止され
ている。電極３０ａ，３０ｂと多孔板２ａ，２ｂは接し
ている。固定板１ａ，１ｂにはそれぞれ液供給通路２２
ａ，２２ｂおよび溶媒蒸気排出通路２３ａ，２３ｂが設
けられており、液供給通路２２ａ，２２ｂは配管２４
ａ，２４ｂおよび仕切り弁２５を介して液タンク２６に
接続され、溶媒蒸気排出通路２３ａ，２３ｂは配管２
７、凝縮用冷却器２８を介して回収容器２９に接続され
ている。その他の構成は図１の構成と同様である。In the apparatus shown in FIG. 2, two electrodes 30 each having a porous or many voids formed in advance are used.
a, 30b is the ion exchange membrane 4 between the porous plates 2a, 2b.
b, and is sealed by the sealing plates 3a, 3b. The electrodes 30a, 30b are in contact with the perforated plates 2a, 2b. The liquid supply passages 22 are respectively provided in the fixed plates 1a and 1b.
a, 22b and solvent vapor discharge passages 23a, 23b, and the liquid supply passages 22a, 22b
a, 24b and a gate valve 25 to a liquid tank 26, and the solvent vapor discharge passages 23a, 23b
7. It is connected to a collection container 29 via a condenser 28 for condensation. Other configurations are the same as those in FIG.

【００２２】図２に示した装置を用いてイオン交換膜と
電極との接合体を製作する方法について説明する。ま
ず、予め準備した２枚の電極３０ａ，３０ｂの間にイオ
ン交換膜を挟み、２枚の多孔板２ａ，２ｂの間に配置す
る。次いで、仕切り弁２５を開き液タンク２６内に満た
されたイオン交換樹脂液３１を配管２４と液供給通路２
２ａ，２２ｂを通して多孔板２ａ，２ｂの空隙内に供給
し、電極３０ａ，３０ｂの空隙内とイオン交換膜４の表
面にイオン交換樹脂液を含浸させる。次に、ヒータ１６
ａ，１６ｂに電流を流して加熱板１５ａ，１５ｂを加熱
して電極３０ａ，３０ｂの空隙内およびイオン交換膜４
に供給されたイオン交換樹脂液の溶媒を蒸発させる。蒸
発した溶媒は多孔板２ａ，２ｂの空隙、溶媒蒸気排出通
路２３ａ，２３ｂおよび配管２７を通って凝縮用冷却器
２８に入って冷却されて凝縮し回収容器２９に回収され
る。一方、電極３０ａ，３０ｂとイオン交換膜４にはイ
オン交換樹脂の皮膜が形成される。ここで、加熱状態の
ままで、プレス装置１９によって固定板１ａ，１ｂを加
圧することによって、電極３０ａ，３０ｂをイオン交換
膜４の面上に圧接する。このようにして、電極のイオン
交換膜と接する面がイオン交換膜内に食い込み、さらに
イオン交換樹脂液の樹脂成分がイオン交換膜の表面に皮
膜を形成して電極とイオン交換膜とを接着する接着剤の
働きをするため、高い結合強度を有するイオン交換膜と
電極との接合体が形成され、かつ、イオン交換樹脂液の
樹脂成分が電極の触媒層内に含浸して、形成された皮膜
が触媒層内に電解質を形成するため、触媒反応面積が電
極とイオン交換膜との接合面のみならず接合面から離れ
た触媒層の３次元方向にも拡大された接合体が形成され
る。A method for manufacturing a joined body of an ion exchange membrane and an electrode using the apparatus shown in FIG. 2 will be described. First, an ion exchange membrane is sandwiched between two electrodes 30a and 30b prepared in advance, and is disposed between the two porous plates 2a and 2b. Next, the gate valve 25 is opened and the ion exchange resin liquid 31 filled in the liquid tank 26 is supplied to the pipe 24 and the liquid supply passage 2.
The liquid is supplied into the gaps between the perforated plates 2a and 2b through 2a and 22b, and the gaps between the electrodes 30a and 30b and the surface of the ion exchange membrane 4 are impregnated with the ion exchange resin liquid. Next, the heater 16
a, 16b is heated to heat the heating plates 15a, 15b, so that the inside of the gap between the electrodes 30a, 30b and the ion exchange membrane 4 are heated.
The solvent of the ion exchange resin liquid supplied to is evaporated. The evaporated solvent passes through the gaps between the perforated plates 2a and 2b, the solvent vapor discharge passages 23a and 23b, and the pipe 27, enters the condensing cooler 28, is cooled, condensed, and collected in the collecting container 29. On the other hand, a film of an ion exchange resin is formed on the electrodes 30a and 30b and the ion exchange membrane 4. Here, the electrodes 30a, 30b are pressed against the surface of the ion exchange membrane 4 by pressing the fixing plates 1a, 1b by the press device 19 in the heated state. In this way, the surface of the electrode in contact with the ion exchange membrane digs into the ion exchange membrane, and the resin component of the ion exchange resin liquid forms a film on the surface of the ion exchange membrane to adhere the electrode to the ion exchange membrane. A film formed by forming a bonded body of an ion exchange membrane and an electrode having a high bonding strength to act as an adhesive, and impregnating a catalyst layer of the electrode with a resin component of an ion exchange resin liquid. Forms an electrolyte in the catalyst layer, so that a bonded body is formed in which the catalytic reaction area is enlarged not only in the bonding surface between the electrode and the ion exchange membrane but also in the three-dimensional direction of the catalyst layer away from the bonding surface.

【００２３】図２に示した装置を用いてイオン交換膜と
電極との接合体を製作する他の方法について説明する。
まず、予め準備した２枚の電極３０ａ，３０ｂの間にイ
オン交換膜を挟み、２枚の多孔板２ａ，２ｂの間に配置
する。次いで、仕切り弁２５を開き液タンク２６内に満
たされた膨潤用液３２を配管２４と液供給通路２２ａ，
２２ｂを通して多孔板２ａ，２ｂの空隙内に供給する。
膨潤用液３２は電極３０、３０の空隙に浸み込んでイオ
ン交換膜４に達し、その表面を濡らす。イオン交換膜４
は膨潤用液３２を含んで膨潤する。次にヒータ１６ａ，
１６ｂに電流を流して加熱板１５ａ，１５ｂを加熱し、
プレス装置１９によって固定板１ａ，１ｂを加圧して、
膨潤したイオン交換膜４と電極３０ａ，３０ｂとを圧接
する。さらに加熱、加圧を続けると、イオン交換膜４と
電極３０ａ，３０ｂに含まれていた膨潤用液３２が蒸発
し、蒸発した膨潤用液は多孔板の空隙と溶媒蒸気排出通
路２３ａ，２３ｂと配管２７を通って凝縮用冷却器２８
に入って冷却され、凝縮する。一方、イオン交換膜４と
電極３０ａ，３０ｂは乾燥され、電極のイオン交換膜と
接する面がイオン交換膜内に食い込んで、高い結合強度
を有するイオン交換膜と電極との接合体が製作される。Another method of manufacturing a joined body of an ion exchange membrane and an electrode using the apparatus shown in FIG. 2 will be described.
First, an ion exchange membrane is sandwiched between two electrodes 30a and 30b prepared in advance, and is disposed between the two porous plates 2a and 2b. Next, the swelling liquid 32 filled in the liquid tank 26 is opened by opening the gate valve 25 and the pipe 24 and the liquid supply passage 22a,
It is supplied into the gaps between the perforated plates 2a and 2b through 22b.
The swelling liquid 32 penetrates into the gaps between the electrodes 30, 30, reaches the ion exchange membrane 4, and wets the surface. Ion exchange membrane 4
Swells with the swelling liquid 32. Next, the heaters 16a,
A current is passed through 16b to heat the heating plates 15a and 15b,
By pressing the fixing plates 1a and 1b by the press device 19,
The swollen ion exchange membrane 4 and the electrodes 30a and 30b are pressed. When heating and pressurization are further continued, the swelling liquid 32 contained in the ion-exchange membrane 4 and the electrodes 30a and 30b evaporates, and the evaporated swelling liquid passes through the pores of the perforated plate and the solvent vapor discharge passages 23a and 23b. Condensing cooler 28 through pipe 27
Enters and cools and condenses. On the other hand, the ion-exchange membrane 4 and the electrodes 30a and 30b are dried, and the surfaces of the electrodes that are in contact with the ion-exchange membrane bite into the ion-exchange membrane, thereby producing a bonded body of the ion-exchange membrane and the electrode having high bonding strength. .

【００２４】ここで、本方法と特開平３−２０８２６２
号に記載された方法との差異は、本方法においては、膨
潤用液３２を多孔板２ａ，２ｂの空隙内を通して供給す
ることにあり、これによって、イオン交換膜４の表面を
均一でむらなく膨潤用液３２に含浸することができ、ま
たさらに、イオン交換膜４が膨潤用液３２により膨潤さ
れる際の厚さの増大としわの発生を防ぎ、イオン交換膜
４を適正な厚み及び形態を保持した状態で電極３０ａ，
３０ｂと接合させることが可能となる。よって、接合体
を燃料電池のセル等に組み込んだ際に、イオン交換膜の
しわによるガス漏れを生じたり、イオン交換膜の厚さが
大きすぎセルに収納できないなどの欠陥のない接合体を
製作することができる。Here, the present method and Japanese Patent Application Laid-Open No. 3-208262 are disclosed.
The difference from the method described in the above is that in the present method, the swelling liquid 32 is supplied through the gaps between the perforated plates 2a and 2b, thereby making the surface of the ion exchange membrane 4 uniform and even. The swelling liquid 32 can be impregnated. Further, when the ion-exchange membrane 4 is swollen by the swelling liquid 32, the thickness of the ion-exchange membrane 4 can be prevented and wrinkling can be prevented. While the electrodes 30a,
30b. Therefore, when the assembly is assembled into a cell of a fuel cell, etc., a joint is manufactured without defects such as gas leakage due to wrinkling of the ion exchange membrane, or the thickness of the ion exchange membrane being too large to be housed in the cell. can do.

【００２５】なお、多孔板２ａ，２ｂは、図１乃至３に
記載のいずれの装置も有しており、いずれも、上述の作
用効果を奏するものである。The perforated plates 2a and 2b have any of the devices shown in FIGS. 1 to 3, and all have the above-described effects.

【００２６】図３の装置においては、図１の装置と同様
に、それぞれ２組の固定板１ａ，１ｂの表面に取り付け
られている多孔板２ａ，２ｂと固定板１ａ，１ｂの端部
に取り付けた封止材（パッキング）３ａ，３ｂとによっ
て密閉空間が形成される。この密閉空間内にイオン交換
膜４が配置され、封止材３ａ，３ｂによって封止され、
イオン交換膜４とその上下の多孔板２ａ，２ｂの間には
空間５ａ，５ｂが形成される。封止材３ａ，３ｂには空
間５ａ，５ｂに開口する触媒分散液供給通路６ａ，６ｂ
が設けられ、この触媒分散液供給通路６ａ，６ｂは配管
７ａ，７ｂおよび仕切り弁８ａ，８ｂを介して触媒分散
液槽９ａ，９ｂに接続している。一方、固定板１ａ，１
ｂには多孔板２ａ，２ｂに接して開口し空間５ａ，５ｂ
の外部に連通する濾液排出通路１０ａ，１０ｂが設けら
れており、この濾液排出通路１０ａ，１０ｂには配管１
１が接続され、配管１１は濾液タンク１２に接続してい
る。さらに、濾液タンク１２には配管１３を介して真空
ポンプ１４が接続されている。さらに、固定板１ａ，１
ｂにはそれぞれ液供給通路２２ａ，２２ｂおよび溶媒蒸
気排出通路２３ａ，２３ｂが設けられており、液供給通
路２２ａ，２２ｂは配管２４に接続し、配管２４は仕切
り弁２５ａ，２５ｂを介して液タンク２６ａ，２６ｂに
接続され、溶媒蒸気排出通路２３ａ，２３ｂは配管２
７、凝縮用冷却器２８を介して回収容器２９に接続され
ている。その他の構成は図１および図２の構成と同様で
ある。In the apparatus shown in FIG. 3, similarly to the apparatus shown in FIG. 1, two sets of fixed plates 1a, 1b are attached to the surfaces of the perforated plates 2a, 2b and attached to the ends of the fixed plates 1a, 1b. A sealed space is formed by the sealing materials (packing) 3a and 3b. An ion exchange membrane 4 is arranged in this closed space, and is sealed by sealing materials 3a and 3b.
Spaces 5a and 5b are formed between the ion exchange membrane 4 and the upper and lower perforated plates 2a and 2b. Catalyst dispersion liquid supply passages 6a, 6b opening to the spaces 5a, 5b are provided in the sealing members 3a, 3b.
These catalyst dispersion liquid supply passages 6a, 6b are connected to catalyst dispersion liquid tanks 9a, 9b via pipes 7a, 7b and gate valves 8a, 8b. On the other hand, the fixed plates 1a, 1
b are open in contact with the perforated plates 2a and 2b and have spaces 5a and 5b
There are provided filtrate discharge passages 10a and 10b communicating with the outside of the pipe.
1 is connected, and the pipe 11 is connected to the filtrate tank 12. Further, a vacuum pump 14 is connected to the filtrate tank 12 via a pipe 13. Further, the fixing plates 1a, 1
b are provided with liquid supply passages 22a and 22b and solvent vapor discharge passages 23a and 23b, respectively. The liquid supply passages 22a and 22b are connected to a pipe 24, and the pipe 24 is connected to liquid tanks via gate valves 25a and 25b. 26a, 26b, and the solvent vapor discharge passages 23a, 23b
7. It is connected to a collection container 29 via a condenser 28 for condensation. Other configurations are the same as those in FIGS. 1 and 2.

【００２７】図３の装置を用いてイオン交換膜と電極と
の接合体を製作する方法について説明する。図示するよ
うに、イオン交換膜４を多孔板を固定板１ａ，１ｂに設
けられた封止材３ａ，３ｂの間に配置する。触媒分散液
槽９ａ，９ｂに触媒分散液２０を満たし、仕切り弁８
ａ，８ｂを開いて、封止材３ａ，３ｂに設けられた触媒
分散液供給通路６ａ，６ｂを通してイオン交換膜４と多
孔板２ａ，２ｂで仕切られた空間５ａ，５ｂ内に触媒分
散液２０を供給する。次いで、濾液タンク１２に接続し
た真空ポンプ１４を作動して濾液タンク内を負圧にす
る。その結果、濾液排出通路１０ａ，１０ｂと固定板１
ａ，１ｂの表面に取り付けた多孔板２ａ，２ｂの空隙内
に負圧が作用し、空間５ａ，５ｂ内の触媒分散液２０が
多孔板２ａ，２ｂによって濾過され、濾液（触媒分散液
の溶媒）が多孔板２ａ，２ｂの空隙と固定板１ａ，１ｂ
の濾液排出通路１０ａ，１０ｂおよび配管１１を経由し
て濾液タンク１２に排出される。一方、多孔板２ａ，２
ｂとイオン交換膜４との間には触媒分散液２０の触媒粒
子が層状に形成され、イオン交換膜４の両面に触媒電極
が形成される。そこで、ヒータ１６ａ，１６ｂに電流を
流して加熱板１５ａ，１５ｂを加熱して形成された触媒
電極を乾燥した後、ヒータ１６ａ，１６ｂの電流を遮断
し、仕切り弁２５ａを開いて、液タンク２６ａ内のイオ
ン交換樹脂液３１を配管２４と液供給通路２２ａ，２２
ｂを通して多孔板２ａ，２ｂの空隙に導き入れ、触媒電
極の空隙とイオン交換膜の表面に浸み込ませる。再びヒ
ータ１６ａ，１６ｂに電流を流して加熱板１５ａ，１５
ｂを加熱して浸み込んだイオン交換樹脂液３１の溶媒を
蒸発させて、触媒電極とイオン交換膜４の表面にイオン
交換樹脂皮膜を形成する。蒸発した溶媒の蒸気は多孔板
２ａ，２ｂの空隙と溶媒蒸気排出通路２３ａ，２３ｂお
よび配管２７を通して凝縮用冷却器に導かれ、凝縮して
回収容器２９内に回収される。次に、ヒータ１６ａ，１
６ｂの電流を遮断し、仕切り弁２５ｂを開いて、液タン
ク２６ｂ内の膨潤用液３２を配管２４と液供給通路２２
ａ，２２ｂを通して多孔板２ａ，２ｂの空隙内に導き入
れ、電極内の空隙とイオン交換膜４の表面に浸み込ませ
てイオン交換膜４を膨潤させる。ヒータ１６ａ，１６ｂ
に電流を流して加熱板１５ａ，１５ｂを加熱するととも
に、プレス装置１９によって固定板１ａ，１ｂを加圧す
ると、触媒電極が膨潤したイオン交換膜４の表面に食い
込み圧接される。さらに加熱、加圧を続けると膨潤用液
は蒸発して多孔板２ａ，２ｂの空隙と溶媒蒸気排出通路
２３ａ，２３ｂおよび配管２７を通して凝縮用冷却器に
導かれ、凝縮して回収容器２９内に回収される。一方、
イオン交換膜４は膨潤した状態から乾燥して収縮し、高
い結合強度を有するイオン交換膜と電極との接合体が製
作される。A method of manufacturing a joined body of an ion exchange membrane and an electrode using the apparatus shown in FIG. 3 will be described. As shown in the drawing, the ion exchange membrane 4 is disposed between the sealing members 3a and 3b provided on the fixed plates 1a and 1b. The catalyst dispersion tanks 9a and 9b are filled with the catalyst dispersion liquid 20, and the gate valve 8
a, 8b are opened, and the catalyst dispersion liquid 20 is passed through the catalyst dispersion liquid supply passages 6a, 6b provided in the sealing materials 3a, 3b and into the spaces 5a, 5b partitioned by the ion exchange membrane 4 and the porous plates 2a, 2b. Supply. Next, the vacuum pump 14 connected to the filtrate tank 12 is operated to make the inside of the filtrate tank a negative pressure. As a result, the filtrate discharge passages 10a and 10b and the fixed plate 1
A negative pressure acts on the gaps between the perforated plates 2a and 2b attached to the surfaces of the a and 1b, the catalyst dispersion 20 in the spaces 5a and 5b is filtered by the perforated plates 2a and 2b, and the filtrate (solvent of the catalyst dispersion) ) Are the gaps between the perforated plates 2a, 2b and the fixing plates 1a, 1b.
Is discharged to the filtrate tank 12 via the filtrate discharge passages 10a and 10b and the pipe 11. On the other hand, the perforated plates 2a, 2a
The catalyst particles of the catalyst dispersion liquid 20 are formed in a layer between the b and the ion exchange membrane 4, and catalyst electrodes are formed on both surfaces of the ion exchange membrane 4. Then, after the heaters 16a and 16b are supplied with current to heat the heating plates 15a and 15b to dry the formed catalyst electrodes, the current of the heaters 16a and 16b is shut off, the gate valve 25a is opened, and the liquid tank 26a is opened. The ion-exchange resin liquid 31 in the inside is connected to the pipe 24 and the liquid supply passages 22a and 22a.
b through the pores of the perforated plates 2a and 2b to permeate the pores of the catalyst electrode and the surface of the ion exchange membrane. An electric current is again applied to the heaters 16a and 16b so that the heating plates 15a and 15b
b is heated to evaporate the solvent of the immersed ion-exchange resin liquid 31 to form an ion-exchange resin film on the surface of the catalyst electrode and the ion-exchange membrane 4. The vapor of the evaporated solvent is guided to the condensing cooler through the gaps in the perforated plates 2a and 2b, the solvent vapor discharge passages 23a and 23b, and the pipe 27, and is condensed and collected in the collection container 29. Next, the heaters 16a, 1
6b, the gate valve 25b is opened, and the swelling liquid 32 in the liquid tank 26b is supplied to the pipe 24 and the liquid supply passage 22.
The ion-exchange membrane 4 is swelled by being introduced into the gaps between the perforated plates 2a and 2b through the holes a and 22b and penetrating into the gaps in the electrodes and the surface of the ion-exchange membrane 4. Heaters 16a, 16b
When the heating plates 15a and 15b are heated by applying an electric current to the fixing plates 1a and 1b by the pressing device 19, the catalyst electrodes bite into the swollen surface of the swollen ion-exchange membrane 4 and are pressed. When the heating and pressurization are further continued, the swelling liquid evaporates and is led to the condenser for cooling through the gaps of the perforated plates 2a and 2b, the solvent vapor discharge passages 23a and 23b and the pipe 27, and is condensed into the collecting vessel 29 Collected. on the other hand,
The ion-exchange membrane 4 dries and shrinks from the swollen state, and a bonded body of the ion-exchange membrane and the electrode having high bonding strength is manufactured.

【００２８】このように、本発明においては、イオン交
換膜上で触媒分散液を濾過してイオン交換膜に電極を形
成し、加熱、加圧してイオン交換膜と電極とを接合する
ので、あるいは電極と接する多孔膜を通じてイオン交換
樹脂液を電極とイオン交換膜の表面に浸み込ませ、加
熱、加圧することによって電極とイオン交換膜にイオン
交換樹脂膜を形成し、加熱、加圧してイオン交換膜と電
極とを接合するので、あるいはイオン交換膜と電極とを
重ね、電極と接する多孔板を通して膨潤用液を電極とイ
オン交換膜に浸み込ませてイオン交換膜を膨潤し、加
熱、加圧することによってイオン交換膜の表面に電極を
圧接、乾燥してイオン交換膜と電極とを接合するので、
接合強度の高いイオン交換膜と電極の接合体を製作する
ことができる。As described above, in the present invention, the catalyst dispersion is filtered on the ion-exchange membrane to form an electrode on the ion-exchange membrane, and heated and pressurized to join the ion-exchange membrane and the electrode. The ion-exchange resin liquid is infiltrated into the surface of the electrode and the ion-exchange membrane through the porous membrane in contact with the electrode, and heated and pressed to form the ion-exchange resin membrane on the electrode and the ion-exchange membrane. Since the exchange membrane and the electrode are joined, or the ion exchange membrane and the electrode are overlapped, the swelling liquid is infiltrated into the electrode and the ion exchange membrane through a porous plate in contact with the electrode, thereby swelling the ion exchange membrane, heating, Pressing the electrode to the surface of the ion exchange membrane by pressing, drying and joining the ion exchange membrane and the electrode,
A joined body of an ion exchange membrane and an electrode having high joining strength can be manufactured.

【００２９】さらに本発明は、イオン交換膜上への触媒
層の形成、イオン交換樹脂液の含浸、及び膨潤用液の含
浸等の接合体の各製作工程が、図３に示す単一の装置で
連続的に行われる。従って本発明は、製造装置の削減お
よび工程の簡素化により製造コストを低減し、かつ製作
工程の連続化により製造時間の短縮も実現するものであ
る。Further, according to the present invention, the steps of manufacturing a joined body such as formation of a catalyst layer on an ion exchange membrane, impregnation of an ion exchange resin solution, and impregnation of a swelling solution are performed by a single apparatus shown in FIG. Is performed continuously. Therefore, the present invention reduces the manufacturing cost by reducing the number of manufacturing apparatuses and simplifying the process, and also realizes the shortening of the manufacturing time by making the manufacturing process continuous.

【００３０】なお、図２の装置を用いてイオン交換膜と
電極との接合体を製作するに際し、供給するイオン交換
樹脂液の溶媒をエチルアルコールなどのアルコールとす
ると、アルコールにはイオン交換膜を膨潤する特性があ
るので、イオン交換樹脂液を電極とイオン交換膜に浸み
込ませ、加熱、加圧することによって、電極とイオン交
換膜にイオン交換樹脂膜を形成するとともに、膨潤した
イオン交換膜に電極が圧接され乾燥された接合体を製作
することができる。In the case where the ion exchange resin solution to be supplied is made of alcohol such as ethyl alcohol when producing a joined body of the ion exchange membrane and the electrode using the apparatus shown in FIG. Since it has the property of swelling, the ion-exchange resin liquid is immersed in the electrode and the ion-exchange membrane, heated and pressurized to form the ion-exchange resin membrane on the electrode and the ion-exchange membrane, and the swollen ion-exchange membrane The electrode can be pressed and dried to produce a dried assembly.

【００３１】また、イオン交換膜と多孔板との間に触媒
分散液を供給し、濾過して電極を形成し、加熱、加圧し
て乾燥し、多孔板を通してイオン交換樹脂液を電極とイ
オン交換膜に浸み込ませて乾燥し、加熱、加圧すること
によって電極とイオン交換膜にイオン交換樹脂膜を形成
し、続けて多孔板を通して電極とイオン交換膜に膨潤用
液を浸み込ませてイオン交換膜を膨潤した後に溶媒を乾
燥除去するので、予め電極を作成する必要がなく、迅速
にしかも接合強度の高い接合体を製作することができ
る。Also, a catalyst dispersion is supplied between the ion exchange membrane and the porous plate, filtered to form an electrode, heated, pressed and dried, and the ion exchange resin liquid is exchanged with the electrode through the porous plate. By infiltrating into the membrane, drying, heating and applying pressure, an ion exchange resin membrane is formed on the electrode and the ion exchange membrane, and then the swelling liquid is impregnated into the electrode and the ion exchange membrane through the porous plate. Since the solvent is dried and removed after swelling the ion-exchange membrane, it is not necessary to prepare an electrode in advance, and a bonded body can be quickly manufactured with high bonding strength.

【００３２】[0032]

【実施例】【Example】

実施例１ 図１の装置を用いてイオン交換膜と電極の接合体を製作
した。多孔板としてポリテトラフルオロエチレン（ＰＴ
ＦＥ）製の高分子フィルタを使用し、２枚の高分子フィ
ルタの間にイオン交換膜としてデュポン社製の厚さ２０
ミル（約５１μｍ）のＮａｆｉｏｎ１１２（商品名）を
設置し、Ｐｔ触媒とポリ四フッ化エチレン粉末を１０：
１の割合で純水に分散した液を、それぞれ上部の多孔板
とＮａｆｉｏｎ１１２の間および下部の多孔板とＮａｆ
ｉｏｎ１１２の間に供給し、上下の多孔板により濾過し
てＮａｆｉｏｎ１１２の表面に電極を形成した。電極の
量は、一例として、３ｍｇ／ｃｍ2であった。次いで、
１４０℃、５０ｋｇ／ｃｍ2の条件で加熱、加圧して接
合体を製作した。Example 1 A bonded body of an ion exchange membrane and an electrode was manufactured using the apparatus of FIG. Polytetrafluoroethylene (PT
FE) polymer filter and a thickness of 20 manufactured by DuPont as an ion exchange membrane between two polymer filters.
A mill (about 51 μm) of Nafion 112 (trade name) was installed, and a Pt catalyst and polytetrafluoroethylene powder were added in 10:
The liquid dispersed in pure water at a ratio of 1 was placed between the upper perforated plate and the Nafion 112, and the lower perforated plate and the Nafion 112, respectively.
The mixture was supplied between the ionic 112 and filtered through the upper and lower perforated plates to form an electrode on the surface of the Nafion 112. The amount of the electrode was, for example, 3 mg / cm 2 . Then
Heating and pressing were performed at 140 ° C. and 50 kg / cm 2 to produce a joined body.

【００３３】この接合体を５０ｃｍ2の燃料電池セルに
組み込み、水素及び空気を供給し、常圧、運転温度８０
℃、及び電流密度０．４Ａ／ｃｍ2の条件で試験を行っ
た結果、セル電圧０．６７Ｖが得られ良好な特性を示し
た。一方、これとは別に、この接合体を温水中に入れて
膨潤した状態としたのち、水電解セルに組み込み、電解
温度を８０℃、電解電流密度を１Ａ／ｃｍ2として大気
圧下で純水の電解を実施したところ、電解電圧は１．５
８Ｖ、エネルギー効率は９２．３％の長期に安定した特
性が得られた。This assembly was assembled in a fuel cell of 50 cm 2 , and hydrogen and air were supplied.
As a result of conducting a test under the conditions of ° C. and a current density of 0.4 A / cm 2 , a cell voltage of 0.67 V was obtained, showing good characteristics. On the other hand, separately from this, the joined body was put into warm water to be in a swollen state, and then assembled into a water electrolysis cell. The electrolysis temperature was set to 80 ° C., and the electrolysis current density was set to 1 A / cm 2. The electrolysis voltage was 1.5
8V, the energy efficiency was 92.3%, and the long-term stable characteristics were obtained.

【００３４】実施例２ 図２の装置を用いてイオン交換膜と電極の接合体を製作
した。多孔板としてステンレス繊維焼結板を用い、２枚
のステンレス繊維焼結板の間に、抄造法により作成した
厚さ３０μｍのＰｔ電極とデュポン社製の厚さ約５１μ
ｍのＮａｆｉｏｎ１１２と抄造法により作成した厚さ２
０μｍのＰｔ／Ｒｕ合金電極を重ねて配置し、Ｎａｆｉ
ｏｎ液を水で３倍に希釈した液を供給した後、１４０
℃、２０ｋｇ／ｃｍ2の条件で加熱、加圧して接合体を
製作した。Example 2 A bonded body of an ion exchange membrane and an electrode was manufactured using the apparatus shown in FIG. A stainless steel sintered plate is used as a perforated plate, and a Pt electrode having a thickness of 30 μm and a thickness of approximately 51 μm manufactured by DuPont are formed between two stainless steel sintered plates.
m Nafion 112 and thickness 2 prepared by papermaking method
0 μm Pt / Ru alloy electrodes are placed one on top of the other and Nafi
After supplying a liquid obtained by diluting the ON liquid three times with water,
The joined body was manufactured by heating and pressurizing at 20 ° C. and 20 kg / cm 2 .

【００３５】この接合体を５０ｃｍ2の燃料電池セルに
組み込み、ＣＯガスを１０ＰＰＭ含む水素及び空気を供
給し、常圧、運転温度８０℃、及び電流密度０．４Ａ／
ｃｍ 2の条件で試験を行った結果、セル電圧０．６７Ｖ
が得られ良好な特性を示した。[0035] The joined body is 50 cmTwoFuel cell
Supply hydrogen and air containing 10 PPM of CO gas
Supply, normal pressure, operating temperature 80 ° C, and current density 0.4A /
cm TwoAs a result of conducting the test under the conditions described above, the cell voltage was 0.67 V
And obtained good characteristics.

【００３６】実施例３ 図２の装置を用いてイオン交換膜と電極の接合体を製作
した。多孔板としてステンレス繊維焼結板を用い、２枚
のステンレス繊維焼結板の間に、抄造法により作成した
厚さ３０μｍのＩｒＯ2電極とデュポン社製の厚さ約５
１μｍのＮａｆｉｏｎ１１２と抄造法により作成した厚
さ２０μｍのＰｔ黒電極を重ねて配置し、膨潤用液とし
てエチルアルコールを当量の水で希釈した液を供給して
多孔板を通してＩｒＯ2電極とＰｔ電極を通してＮａｆ
ｉｏｎ１１２に浸み込ませ、１２０℃、１０ｋｇ／ｃｍ
2の条件で加熱、加圧して接合体を製作した。Example 3 A joined body of an ion exchange membrane and an electrode was manufactured using the apparatus shown in FIG. A stainless steel sintered plate was used as a perforated plate. An IrO 2 electrode having a thickness of 30 μm formed by a papermaking method and a thickness of about 5 manufactured by DuPont were placed between the two stainless steel sintered plates.
1 μm of Nafion 112 and a 20 μm-thick Pt black electrode prepared by a papermaking method are superposed and arranged, and a liquid obtained by diluting ethyl alcohol with an equivalent amount of water as a swelling liquid is supplied, and the IrO 2 electrode and the Pt electrode are passed through the perforated plate. Naf
ionic 112, 120 ° C, 10kg / cm
Under the conditions of 2 , heating and pressing were performed to produce a joined body.

【００３７】この接合体を温水中に入れて膨潤した状態
としたのち、水電解セルに組み込み、電解温度を８０
℃、電解電流密度を１Ａ／ｃｍ2として大気圧下で純水
の電解を実施したところ、電解電圧は１．５４Ｖ、エネ
ルギー効率は９５．１％の長期に安定した特性が得られ
た。[0037] After this joined body was put into warm water to be in a swollen state, it was assembled in a water electrolysis cell, and the electrolysis temperature was set to 80.
When electrolysis of pure water was carried out under atmospheric pressure at a temperature of 1 ° C. and an electrolysis current density of 1 A / cm 2 , long-term stable characteristics of an electrolysis voltage of 1.54 V and an energy efficiency of 95.1% were obtained.

【００３８】実施例４ 図３の装置を用いてイオン交換膜と電極の接合体を製作
した。多孔板としてステンレス繊維焼結板と高分子フィ
ルターを重ねたものを用い、２枚の多孔板の間にイオン
交換膜として厚さ約５１μｍのＮａｆｉｏｎ１１２を配
置し、一方の多孔板とＮａｆｉｏｎ１１２の間にＰｔ触
媒とポリ四フッ化エチレン粉末を１０：１の割合で純水
に分散して作製した陰極用触媒分散液を供給し、他方の
多孔板とＮａｆｉｏｎ１１２の間にＰｔ／Ｒｕ合金触媒
とポリ四フッ化エチレン粉末を１０：１の割合で純水に
分散して作製した陽極用触媒分散液を供給して、Ｎａｆ
ｉｏｎ１１２の表面に陰極用触媒電極と陽極用触媒電極
を形成した。電極の量はそれぞれ３ｍｇ／ｃｍ2であっ
た。１２０℃、５ｋｇ／ｃｍ2の条件で加熱、加圧し
た。次いで、多孔板を通してイオン交換樹脂液（Ｎａｆ
ｉｏｎ液を水で希釈した液）を供給し、陽極用触媒電極
と陰極用触媒電極の空隙およびイオン交換膜の表面に浸
みこませて、電極とイオン交換膜の表面にイオン交換樹
脂膜を形成し、１２０℃、５ｋｇ／ｃｍ2の条件で加
熱、加圧した。その後、ｔ−ブチルアルコールを水で２
倍に希釈した液を供給してＮａｆｉｏｎ１１２を膨潤
し、１４０℃、２０ｋｇ／ｃｍ2の条件で加熱、加圧し
て接合体を形成した。Example 4 An assembly of an ion exchange membrane and an electrode was manufactured using the apparatus shown in FIG. As a perforated plate, a stainless steel sintered plate and a polymer filter are superimposed, a Nafion 112 having a thickness of about 51 μm is disposed as an ion exchange membrane between two perforated plates, and a Pt catalyst is provided between one perforated plate and the Nafion 112. And a polytetrafluoroethylene powder dispersed in pure water at a ratio of 10: 1 to supply a cathode catalyst dispersion, and a Pt / Ru alloy catalyst and polytetrafluoride between the other porous plate and Nafion 112. A catalyst dispersion for anode prepared by dispersing ethylene powder in pure water at a ratio of 10: 1 is supplied, and Naf
A cathode catalyst electrode and an anode catalyst electrode were formed on the surface of the ion 112. The amount of each electrode was 3 mg / cm 2 . Heating and pressing were performed at 120 ° C. and 5 kg / cm 2 . Next, an ion exchange resin solution (Naf
(ion solution diluted with water), and immersed in the gap between the anode catalyst electrode and the cathode catalyst electrode and the surface of the ion exchange membrane to form an ion exchange resin membrane on the surface of the electrode and the ion exchange membrane. Then, heating and pressurization were performed at 120 ° C. and 5 kg / cm 2 . Then, t-butyl alcohol is added with water for 2 hours.
The liquid diluted twice was supplied to swell the Nafion 112, and heated and pressed at 140 ° C. and 20 kg / cm 2 to form a joined body.

【００３９】この接合体を５０ｃｍ2の燃料電池セルに
組み込み、ＣＯガスを１０ＰＰＭ含む水素及び空気を供
給し、常圧、運転温度８０℃、及び電流密度０．４Ａ／
ｃｍ 2の条件で試験を行った結果、セル電圧０．６７Ｖ
が得られ良好な特性を示した。さらに、本条件で１００
０時間の連続試験を実施したところ、安定した特性が得
られ、その間のセル電圧の低下は、１０ｍＶ以下であっ
た。This joined body is 50 cmTwoFuel cell
Supply hydrogen and air containing 10 PPM of CO gas
Supply, normal pressure, operating temperature 80 ° C, and current density 0.4A /
cm TwoAs a result of conducting the test under the conditions described above, the cell voltage was 0.67 V
And obtained good characteristics. In addition, 100
When a continuous test was performed for 0 hours, stable characteristics were obtained.
During this time, the cell voltage drops by 10 mV or less.
Was.

【００４０】比較例１ 比較のため、従来法により接合体を製作した。抄造法に
より製作した厚さ３０μｍのＰｔ電極、デュポン製のＮ
ａｆｉｏｎ１１２、及び抄造法により製作した厚さ２０
μｍのＰｔ／Ｒｕ電極を１５０℃、５０ｋｇ／ｃｍ2の
条件で加熱、加圧して接合体を製作した。この接合体を
５０ｃｍ2の燃料電池セルに組み込み、ＣＯガスを１０
ＰＰＭ含む水素及び空気を供給し、常圧、運転温度８０
℃、及び電流密度０．４Ａ／ｃｍ2の条件で試験を行っ
た結果、セル電圧０．６３Ｖであった。さらに、本条件
で１０００時間の連続試験を実施した結果、その間のセ
ル電圧の低下は、５０ｍＶ以下であった。 比較例２ 比較のために従来法によって接合体を製作した。抄造法
により作製した厚さ３０μｍのＩｒＯ2電極とデュポン
社製のＮａｆｉｏｎ１１２と抄造法により作成した厚さ
２０μｍのＰｔ黒電極を１５０℃、５０ｋｇ／ｃｍ2の
条件で加熱、加圧して接合体を製作した。この接合体を
温水中に入れて膨潤した状態とし、水電解セルに組み込
み、電解温度を８０℃、電解電流密度を１Ａ／ｃｍ2と
して大気圧下で純水の電解を実施したところ、初期電解
電圧は１．６４Ｖ、エネルギー効率は８８．０％であっ
たが、電解電圧は３００時間経過後では１．７２Ｖに上
昇し、安定した特性が得られなかった。Comparative Example 1 For comparison, a joined body was manufactured by a conventional method. 30 μm thick Pt electrode manufactured by the papermaking method, DuPont N
afion112 and a thickness of 20 manufactured by a papermaking method
A Pt / Ru electrode of μm was heated and pressed at 150 ° C. and 50 kg / cm 2 to produce a joined body. This assembly was assembled in a 50 cm 2 fuel cell, and CO gas was supplied
Supply hydrogen and air including PPM, normal pressure, operating temperature 80
As a result of conducting a test under the conditions of ° C. and a current density of 0.4 A / cm 2 , the cell voltage was 0.63 V. Furthermore, as a result of performing a continuous test under these conditions for 1000 hours, the decrease in the cell voltage during that time was 50 mV or less. Comparative Example 2 A joined body was manufactured by a conventional method for comparison. A 30 μm-thick IrO 2 electrode produced by the papermaking method, Nafion 112 manufactured by DuPont, and a 20 μm-thick Pt black electrode produced by the papermaking method were heated and pressed at 150 ° C. and 50 kg / cm 2 to form a joined body. Made. The joined body was swelled by placing it in warm water, incorporated into a water electrolysis cell, and electrolyzed with pure water under atmospheric pressure at an electrolysis temperature of 80 ° C. and an electrolysis current density of 1 A / cm 2. Although the voltage was 1.64 V and the energy efficiency was 88.0%, the electrolytic voltage rose to 1.72 V after 300 hours, and stable characteristics could not be obtained.

【００４１】[0041]

【発明の効果】以上説明したように、本発明において
は、イオン交換膜と多孔板の間に触媒分散液を供給して
イオン交換膜上での濾過により電極を形成し、あるいは
イオン交換膜と電極と多孔板を重ねて配置し、多孔板を
通して電極の空隙内とイオン交換膜の表面にイオン交換
樹脂液を供給して加熱、加圧して電極とイオン交換膜の
表面にイオン交換樹脂膜を形成し、あるいはイオン交換
膜と電極と多孔板を重ね、多孔板の空隙と電極内部の空
隙をを通してイオン交換膜を膨潤して加熱、加圧して接
合体を製作するので、イオン交換膜と電極との接合強度
が高く、長期に安定して高い特性を示す接合体を製作す
ることができる。As described above, in the present invention, the catalyst dispersion is supplied between the ion exchange membrane and the perforated plate to form an electrode by filtration on the ion exchange membrane. The perforated plates are placed one on top of the other, and the ion exchange resin solution is supplied through the perforated plate to the inside of the electrode gap and the surface of the ion exchange membrane, and heated and pressed to form an ion exchange resin membrane on the electrode and the surface of the ion exchange membrane. Alternatively, the ion-exchange membrane, the electrode and the porous plate are overlapped, and the ion-exchange membrane is swollen through the pores of the porous plate and the pores inside the electrode, heated and pressed to produce a bonded body. A joined body having high joining strength and exhibiting high characteristics stably for a long period of time can be manufactured.

【００４２】さらに、本発明では、多孔板をイオン交換
膜に押圧してイオン交換膜の形態及び形状を保持した状
態で、イオン交換樹脂液、膨潤用液を多孔板内に注入
し、多孔板内の空隙である細孔を経て、液をイオン交換
膜の表面に拡散含浸させるので、イオン交換膜に液を拡
散含浸させる際に厚みの変化、しわの発生を抑制するこ
とができる。イオン交換膜の厚みの増大は、燃料電池等
のセルへ膜を組み込んだ後のカ゛ス洩れの発生、または、
セル内に収納できないというおそれを生じ、また、しわ
の発生はガス洩れの原因となるが、本発明では、これら
の問題を排除できる。Further, in the present invention, an ion exchange resin solution and a swelling liquid are injected into the perforated plate while the perforated plate is pressed against the ion exchange membrane while maintaining the shape and shape of the ion exchange membrane. Since the liquid is diffused and impregnated into the surface of the ion exchange membrane through the pores, which are voids in the inside, it is possible to suppress a change in thickness and generation of wrinkles when the liquid is diffused and impregnated into the ion exchange membrane. The increase in the thickness of the ion-exchange membrane may cause gas leakage after the membrane is incorporated into a cell such as a fuel cell, or
There is a fear that the cell cannot be stored in the cell, and wrinkles cause gas leakage. However, the present invention can eliminate these problems.

【００４３】またさらに、本発明で多孔板を用いること
によって、多孔板の空隙である細孔を経て液がイオン交
換膜に達するため、膜の面内において、均一でむらのな
い含浸が可能となる。また、イオン交換膜と多孔板との
間に触媒分散液を供給し、濾過して電極を形成し、加
熱、加圧して乾燥し、多孔板を通してイオン交換樹脂液
を電極とイオン交換膜に浸み込ませて乾燥し、加熱、加
圧することによって電極とイオン交換膜にイオン交換樹
脂膜を形成し、続けて多孔板を通して電極とイオン交換
膜に膨潤用液を浸み込ませてイオン交換膜を膨潤した後
に溶媒を乾燥除去するので、予め電極を作成する必要が
なく、迅速にしかも接合強度の高い接合体を製作するこ
とができる。Further, by using the perforated plate in the present invention, the liquid reaches the ion exchange membrane through the pores, which are the voids of the perforated plate, so that uniform and even impregnation can be performed within the plane of the membrane. Become. Also, the catalyst dispersion is supplied between the ion exchange membrane and the perforated plate, filtered to form an electrode, heated, pressed and dried, and the ion exchange resin liquid is immersed in the electrode and the ion exchange membrane through the perforated plate. Drying, heating and pressurizing to form an ion-exchange resin membrane on the electrode and the ion-exchange membrane, and then impregnating the electrode and the ion-exchange membrane with the swelling liquid through the perforated plate Since the solvent is dried and removed after swelling, there is no need to prepare an electrode in advance, and a joined body having a high joining strength can be manufactured quickly.

【００４４】すなわち本発明は、イオン交換膜上への触
媒層の形成、イオン交換樹脂液の含浸、及び膨潤用液へ
の含浸等の接合体の各製作工程が、単一の装置で連続的
に行われる。従って本発明は、製造装置の削減および工
程の簡素化により製造コストを低減し、かつ製作工程の
連続化により製造時間の短縮を可能としたものである。That is, according to the present invention, the steps of producing a joined body, such as formation of a catalyst layer on an ion exchange membrane, impregnation of an ion exchange resin liquid, and impregnation of a swelling liquid, are performed continuously by a single apparatus. Done in Therefore, the present invention reduces the manufacturing cost by reducing the number of manufacturing apparatuses and simplifying the steps, and shortens the manufacturing time by making the manufacturing steps continuous.

【図面の簡単な説明】[Brief description of the drawings]

【図１】本発明による接合体の製作装置の一実施例の構
成を示す断面図である。FIG. 1 is a cross-sectional view showing a configuration of an embodiment of an apparatus for manufacturing a joined body according to the present invention.

【図２】本発明による接合体の製作装置の他の実施例の
構成を示す断面図である。FIG. 2 is a sectional view showing the configuration of another embodiment of the apparatus for manufacturing a joined body according to the present invention.

【図３】本発明による接合体の製作装置のさらに他の実
施例の構成を示す断面図である。FIG. 3 is a cross-sectional view showing the configuration of still another embodiment of the apparatus for manufacturing a joined body according to the present invention.

【符号の説明】[Explanation of symbols]

１ａ，１ｂ 固定板 ２ａ，２ｂ 多孔板 ３ａ，３ｂ 封止材 ４ イオン交換膜 ５ａ，５ｂ 空間 ６ａ，６ｂ 触媒分散液供給通路 ７ａ，７ｂ 配管 ８ａ，８ｂ 仕切り弁 ９ａ，９ｂ 触媒分散液槽 １０ａ，１０ｂ 濾液排出通路 １１ 配管 １２ 濾液タンク １３ 配管 １４ 真空ポンプ １５ａ，１５ｂ 加熱板 １６ａ，１６ｂ ヒータ １７ａ，１７ｂ 温度センサ １８ａ，１８ｂ 断熱板 １９ プレス装置 ２０ 触媒分散液 ２１ 濾液 ２２ａ，２２ｂ 液供給通路 ２３ａ，２３ｂ 溶媒蒸気排出通路 ２４ 配管 ２５ 仕切り弁 ２６ 液タンク ２７ 配管 ２８ 凝縮用冷却器 ２９ 回収容器 ３０ａ，３０ｂ 電極 ３１ イオン交換樹脂液 ３２ 膨潤用液 1a, 1b Fixed plate 2a, 2b Perforated plate 3a, 3b Sealing material 4 Ion exchange membrane 5a, 5b Space 6a, 6b Catalyst dispersion liquid supply passage 7a, 7b Piping 8a, 8b Partition valve 9a, 9b Catalyst dispersion liquid tank 10a, 10b Filtrate discharge passage 11 Pipe 12 Filtrate tank 13 Pipe 14 Vacuum pump 15a, 15b Heating plate 16a, 16b Heater 17a, 17b Temperature sensor 18a, 18b Heat insulating plate 19 Press device 20 Catalyst dispersion 21 Filtrate 22a, 22b Liquid supply passage 23a, 23b Solvent vapor discharge passage 24 Pipe 25 Gate valve 26 Liquid tank 27 Pipe 28 Condenser cooler 29 Recovery container 30a, 30b Electrode 31 Ion exchange resin liquid 32 Swelling liquid

───────────────────────────────────────────────────── フロントページの続き (72)発明者 沖沢 加代子 神奈川県横須賀市長坂２丁目２番地１号 株式会社富士電機総合研究所内 ──────────────────────────────────────────────────続 き Continued on the front page (72) Inventor Kayoko Okizawa 2-2-1 Nagasaka, Yokosuka City, Kanagawa Prefecture Inside Fuji Electric Research Laboratory Co., Ltd.

Claims (9)

【特許請求の範囲】[Claims] 【請求項１】 イオン交換膜と多孔板を対面して配置す
る工程、および前記イオン交換膜と前記多孔板の対向す
る面の間に触媒分散液を供給し、かつ該触媒分散液の溶
媒を前記多孔板の外側に排出してイオン交換膜上に触媒
粒子層を形成して電極とする工程を有することを特徴と
するイオン交換膜と電極の接合体の製作方法。1. A step of arranging an ion exchange membrane and a perforated plate facing each other, supplying a catalyst dispersion between the ion exchange membrane and a facing surface of the perforated plate, and removing a solvent of the catalyst dispersion. A method for producing a bonded body of an ion exchange membrane and an electrode, comprising a step of forming a catalyst particle layer on the ion exchange membrane by discharging the catalyst particle to the outside of the porous plate to form an electrode. 【請求項２】 イオン交換膜、電極および多孔板を重ね
る工程、前記多孔板の空隙にイオン交換樹脂液を供給
し、前記電極の空隙内および前記イオン交換膜の表面に
前記イオン交換樹脂液を拡散含浸する工程、および前記
イオン交換膜、電極および多孔板を加熱して拡散含浸し
たイオン交換樹脂液の溶媒を蒸発除去して前記電極およ
びイオン交換膜の表面にイオン交換樹脂の皮膜を形成す
る工程を有することを特徴とするイオン交換膜と電極の
接合体の製作方法。2. A step of laminating an ion exchange membrane, an electrode and a perforated plate, supplying an ion exchange resin liquid to a void of the porous plate, and applying the ion exchange resin liquid to the inside of the electrode and to the surface of the ion exchange membrane. Diffusion impregnating step, and heating the ion exchange membrane, the electrode and the perforated plate to evaporate and remove the solvent of the diffusion impregnated ion exchange resin liquid to form a film of the ion exchange resin on the surface of the electrode and the ion exchange membrane. A method for producing a joined body of an ion-exchange membrane and an electrode, comprising a step. 【請求項３】 イオン交換膜、電極および多孔板を重ね
る工程、前記多孔板の空隙に膨潤用液を供給し、前記電
極の空隙を通して前記イオン交換膜の表面に膨潤用液を
含浸させる工程、および前記イオン交換膜、電極および
多孔板を加熱、加圧して前記イオン交換膜と前記電極と
を接合する工程を有することを特徴とするイオン交換膜
と電極の接合体の製作方法。3. A step of stacking an ion exchange membrane, an electrode and a perforated plate, a step of supplying a swelling liquid to a gap of the perforated plate, and a step of impregnating the surface of the ion exchange membrane with the swelling liquid through the gap of the electrode. And a step of heating and pressurizing the ion-exchange membrane, the electrode and the porous plate to join the ion-exchange membrane and the electrode. 【請求項４】 イオン交換膜、電極および多孔板を重ね
る工程、前記多孔板の空隙にイオン交換樹脂を含有した
膨潤用液を供給し、前記電極の空隙を通して前記イオン
交換膜の表面に膨潤用液を含浸させてイオン交換膜を膨
潤させると共に前記電極の空隙内および前記イオン交換
膜の表面に前記イオン交換樹脂液を拡散含浸する工程、
および前記イオン交換膜、電極および多孔板を加熱、加
圧して前記電極およびイオン交換膜の表面にイオン交換
樹脂の皮膜を形成して前記イオン交換膜と前記電極とを
接合する工程を有することを特徴とするイオン交換膜と
電極の接合体の製作方法。4. A step of laminating an ion exchange membrane, an electrode and a perforated plate, supplying a swelling liquid containing an ion exchange resin to a space of the perforated plate, and swelling the surface of the ion exchange membrane through a space of the electrode. A step of swelling the ion exchange membrane by impregnating the liquid and diffusing and impregnating the ion exchange resin liquid into the gaps of the electrodes and the surface of the ion exchange membrane;
And heating and pressurizing the ion exchange membrane, the electrode and the porous plate to form a film of an ion exchange resin on the surface of the electrode and the ion exchange membrane, and joining the ion exchange membrane and the electrode. Characteristic method of manufacturing a bonded body of an ion exchange membrane and an electrode. 【請求項５】 イオン交換膜と多孔板を対面して配置す
る工程、前記イオン交換膜と前記多孔板の対向する面の
間に触媒分散液を供給し、かつ該触媒分散液の溶媒を前
記多孔板の外側に排出してイオン交換膜上に触媒粒子層
を形成して電極とする工程、前記多孔板の空隙にイオン
交換樹脂液を供給し、前記電極の空隙内および前記イオ
ン交換膜の表面に前記イオン交換樹脂液を拡散含浸する
工程、および前記イオン交換膜、電極および多孔板を加
熱して拡散含浸したイオン交換樹脂液の溶媒を蒸発除去
して前記電極およびイオン交換膜の表面にイオン交換樹
脂の皮膜を形成する工程、前記多孔板の空隙に膨潤用液
を供給し、前記電極の空隙を通して前記イオン交換膜の
表面に膨潤用液を含浸させてイオン交換膜を膨潤させる
工程、および前記イオン交換膜、電極および多孔板を加
熱、加圧して前記イオン交換膜と前記電極とを接合する
工程を有することを特徴とするイオン交換膜と電極の接
合体の製作方法。5. A step of arranging an ion exchange membrane and a perforated plate facing each other, supplying a catalyst dispersion between the ion exchange membrane and a surface of the perforated plate facing each other, and A step of forming a catalyst particle layer on the ion exchange membrane by discharging to the outside of the perforated plate to form an electrode, supplying an ion exchange resin liquid to the gap of the perforated plate, A step of diffusing and impregnating the surface of the ion-exchange resin liquid with the ion-exchange resin liquid, and evaporating and removing the solvent of the ion-exchange resin liquid diffused and impregnated by heating the ion-exchange membrane, the electrode and the perforated plate, thereby forming a surface of the electrode and the ion-exchange membrane. Forming a film of an ion exchange resin, supplying a swelling liquid to the voids of the perforated plate, and swelling the ion exchange membrane by impregnating the surface of the ion exchange membrane with the swelling liquid through the voids of the electrode; And the A method for producing a bonded body of an ion exchange membrane and an electrode, comprising a step of heating and pressurizing an on-exchange membrane, an electrode, and a porous plate to bond the ion exchange membrane and the electrode. 【請求項６】 互いに対向し、それぞれ表面に多孔板が
取り付けられている２組の固定板と、該２組の固定板の
間に設けられ前記二つの多孔板と共にイオン交換膜を収
容する空間を形成する封止材と、前記多孔板を通して前
記空間に触媒分散液を供給する手段と、前記多孔板を通
して前記空間から前記触媒分散液の溶媒を排出する手段
と、前記イオン交換膜と電極を加熱、加圧する手段とを
備えたことを特徴とするイオン交換膜と電極の接合体の
製作装置。6. Two sets of fixed plates facing each other, each having a perforated plate attached to the surface, and a space provided between the two sets of fixed plates and accommodating the ion exchange membrane together with the two perforated plates. Sealing material, means for supplying a catalyst dispersion to the space through the perforated plate, means for discharging the solvent of the catalyst dispersion from the space through the perforated plate, heating the ion exchange membrane and electrodes, An apparatus for manufacturing a joined body of an ion exchange membrane and an electrode, comprising: means for applying pressure. 【請求項７】 互いに対向し、それぞれ表面に多孔板が
取り付けられている２組の固定板と、該２組の固定板の
間に設けられイオン交換膜と電極とを固定する封止材
と、前記多孔板を通して前記イオン交換膜と電極にイオ
ン交換樹脂液を供給する手段と、前記多孔板を通して前
記イオン交換樹脂液の蒸発溶媒を排出する手段と、前記
イオン交換膜と電極を加熱、加圧する手段とを備えたこ
とを特徴とするイオン交換膜と電極の接合体の製作装
置。7. A pair of fixing plates opposed to each other and each having a perforated plate attached to a surface thereof, a sealing member provided between the two sets of fixing plates to fix the ion exchange membrane and the electrode, Means for supplying the ion exchange resin liquid to the ion exchange membrane and the electrode through the perforated plate; means for discharging the evaporation solvent of the ion exchange resin liquid through the perforated plate; means for heating and pressurizing the ion exchange membrane and the electrode An apparatus for manufacturing a joined body of an ion exchange membrane and an electrode, comprising: 【請求項８】 互いに対向し、それぞれ表面に多孔板が
取り付けられている２組の固定板と、該２組の固定板の
間に設けられイオン交換膜と電極とを固定する封止材
と、前記多孔板を通して前記イオン交換膜と電極に膨潤
用液を供給する手段と、前記多孔板を通して前記膨潤用
液の蒸気を排出する手段と、前記イオン交換膜と電極を
加熱、加圧する手段とを備えたことを特徴とするイオン
交換膜と電極の接合体の製作装置。8. A pair of fixed plates opposed to each other and each having a perforated plate attached to a surface thereof; a sealing member provided between the two sets of fixed plates to fix an ion exchange membrane and an electrode; A means for supplying a swelling liquid to the ion exchange membrane and the electrode through a perforated plate; a means for discharging vapor of the swelling liquid through the perforated plate; and a means for heating and pressurizing the ion exchange membrane and the electrode. An apparatus for manufacturing a joined body of an ion-exchange membrane and an electrode. 【請求項９】 互いに対向し、それぞれ表面に多孔板が
取り付けられている２組の固定板と、該２組の固定板の
間に設けられ、２組の固定板と共にイオン交換膜と電極
とを収容する空間を形成する封止材と、前記空間に触媒
分散液を供給する手段と、前記空間にイオン交換樹脂液
を供給する手段と、前記空間に膨潤用液を供給する手段
と、それぞれ前記多孔板を通して前記空間から、前記触
媒分散液の溶媒を排出する手段と前記イオン交換樹脂液
の蒸発溶媒および前記膨潤用液の蒸気を排出する手段
と、前記イオン交換膜と電極を加熱、加圧する手段とを
備えたことを特徴とするイオン交換膜と電極の接合体の
製作装置。9. Two sets of fixed plates opposed to each other and each having a perforated plate attached to the surface, and provided between the two sets of fixed plates, accommodating the ion exchange membrane and the electrodes together with the two sets of fixed plates. Sealing material forming a space to be formed, means for supplying a catalyst dispersion liquid to the space, means for supplying an ion exchange resin liquid to the space, means for supplying a swelling liquid to the space, Means for discharging the solvent of the catalyst dispersion liquid from the space through the plate, means for discharging the evaporation solvent of the ion exchange resin liquid and the vapor of the swelling liquid, and means for heating and pressurizing the ion exchange membrane and the electrode An apparatus for manufacturing a joined body of an ion exchange membrane and an electrode, comprising:
JP10182570A 1997-07-01 1998-06-29 Production of joinded body of ion-exchange membrane and electrode and production device therefor Pending JPH1171692A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP10182570A JPH1171692A (en) 1997-07-01 1998-06-29 Production of joinded body of ion-exchange membrane and electrode and production device therefor

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
JP9-175752 1997-07-01
JP17575297 1997-07-01
JP10182570A JPH1171692A (en) 1997-07-01 1998-06-29 Production of joinded body of ion-exchange membrane and electrode and production device therefor

Publications (1)

Publication Number Publication Date
JPH1171692A true JPH1171692A (en) 1999-03-16

Family

ID=26496919

Family Applications (1)

Application Number Title Priority Date Filing Date
JP10182570A Pending JPH1171692A (en) 1997-07-01 1998-06-29 Production of joinded body of ion-exchange membrane and electrode and production device therefor

Country Status (1)

Country Link
JP (1) JPH1171692A (en)

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2002005372A1 (en) * 2000-07-06 2002-01-17 Matsushita Electric Industrial Co., Ltd. Method for producing electrolyte film-electrode joint
JP2003524863A (en) * 1999-04-21 2003-08-19 ディーエスエム エヌ．ブイ． Method for preparing a composite membrane
JP2008098152A (en) * 2006-09-11 2008-04-24 Toray Ind Inc Manufacturing method of membrane/electrode assembly
JP2009518817A (en) * 2005-12-12 2009-05-07 ビーワイディー カンパニー リミテッド Method for producing catalyst-coated membrane
JP2019220459A (en) * 2018-06-15 2019-12-26 日本碍子株式会社 Electrochemical cell
US10916789B2 (en) 2016-03-21 2021-02-09 Hydrolite Ltd Alkaline exchange membrane fuel cells system having a bi-polar plate

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2003524863A (en) * 1999-04-21 2003-08-19 ディーエスエム エヌ．ブイ． Method for preparing a composite membrane
JP4807918B2 (en) * 1999-04-21 2011-11-02 ディーエスエム アイピー アセッツ ビー．ブイ． Method for preparing composite membrane
WO2002005372A1 (en) * 2000-07-06 2002-01-17 Matsushita Electric Industrial Co., Ltd. Method for producing electrolyte film-electrode joint
JP2009518817A (en) * 2005-12-12 2009-05-07 ビーワイディー カンパニー リミテッド Method for producing catalyst-coated membrane
JP2008098152A (en) * 2006-09-11 2008-04-24 Toray Ind Inc Manufacturing method of membrane/electrode assembly
US10916789B2 (en) 2016-03-21 2021-02-09 Hydrolite Ltd Alkaline exchange membrane fuel cells system having a bi-polar plate
JP2019220459A (en) * 2018-06-15 2019-12-26 日本碍子株式会社 Electrochemical cell

Similar Documents

Publication Publication Date Title
US4175165A (en) Fuel cell system utilizing ion exchange membranes and bipolar plates
US5631099A (en) Surface replica fuel cell
JP3481010B2 (en) Polymer solid electrolyte membrane / electrode integrated body and method for producing the same
US4505992A (en) Integral gas seal for fuel cell gas distribution assemblies and method of fabrication
JP3555999B2 (en) Method for producing polymer solid electrolyte / electrode assembly for polymer electrolyte fuel cell
US4732637A (en) Method of fabricating an integral gas seal for fuel cell gas distribution assemblies
JP2922132B2 (en) Polymer electrolyte fuel cell
JP3444541B2 (en) Polymer electrolyte fuel cell
US7867668B2 (en) Electrolyte layer for fuel cell, fuel cell, and method of manufacturing electrolyte layer for fuel cell
US5266421A (en) Enhanced membrane-electrode interface
EP1217680A2 (en) An ion exchange and electrode assembly for an electrochemical cell
JP2004139854A (en) Fuel cell
CA2640961A1 (en) Method of making membrane electrode assemblies
US8586265B2 (en) Method of forming membrane electrode assemblies for electrochemical devices
JPH1171692A (en) Production of joinded body of ion-exchange membrane and electrode and production device therefor
JP2008146928A (en) Gas diffusing electrode for fuel cell and its manufacturing method
EP1984967B1 (en) Method of forming membrane electrode assemblies for electrochemical devices
JP2005276847A (en) Polymer solid electrolyte-electrode junction
JP5071646B2 (en) Fuel cell electrode paste, electrode and membrane electrode assembly, and fuel cell system manufacturing method.
JPH0384866A (en) Connecting method and device of electrolyte membrane and electrode
JP4262942B2 (en) Polymer solid electrolyte / electrode assembly for lithium battery and method for producing the same
JP6845436B2 (en) Cell for water electrolysis / fuel cell power generation and cell laminate in which a plurality of these are laminated
JPH08185872A (en) Solid high molecular fuel cell and manufacture thereof
WO2018084175A1 (en) Cell for water electrolysis/fuel cell power generation and cell stack body having a plurality of same cells stacked
JPH10189018A (en) Sealing method for solid macromolecule fuel cell