JPH0766814B2 - Method for manufacturing fuel cell electrode - Google Patents

Method for manufacturing fuel cell electrode

Info

Publication number
JPH0766814B2
JPH0766814B2 JP1035403A JP3540389A JPH0766814B2 JP H0766814 B2 JPH0766814 B2 JP H0766814B2 JP 1035403 A JP1035403 A JP 1035403A JP 3540389 A JP3540389 A JP 3540389A JP H0766814 B2 JPH0766814 B2 JP H0766814B2
Authority
JP
Japan
Prior art keywords
electrode
base material
electrode base
catalyst
fuel cell
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.)
Expired - Lifetime
Application number
JP1035403A
Other languages
Japanese (ja)
Other versions
JPH02215049A (en
Inventor
芳昭 阪本
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.)
Mitsubishi Electric Corp
Original Assignee
Mitsubishi Electric Corp
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 Mitsubishi Electric Corp filed Critical Mitsubishi Electric Corp
Priority to JP1035403A priority Critical patent/JPH0766814B2/en
Publication of JPH02215049A publication Critical patent/JPH02215049A/en
Publication of JPH0766814B2 publication Critical patent/JPH0766814B2/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8803—Supports for the deposition of the catalytic active composition
    • H01M4/8814—Temporary supports, e.g. decal
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
    • H01M4/8668—Binders
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8825—Methods for deposition of the catalytic active composition
    • H01M4/8828—Coating with slurry or ink
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
    • H01M4/8882—Heat treatment, e.g. drying, baking
    • H01M4/8885—Sintering or firing
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
    • H01M4/8896—Pressing, rolling, calendering
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8803—Supports for the deposition of the catalytic active composition
    • H01M4/8807—Gas diffusion layers
    • 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

Description

【発明の詳細な説明】 〔産業上の利用分野〕 この発明は燃料電池用電極の製造方法に関するものであ
る。TECHNICAL FIELD The present invention relates to a method for manufacturing an electrode for a fuel cell.

〔従来の技術〕[Conventional technology]

第２図は例えば特開昭60−65465号公報に示す従来の燃
料電池の電極の一般的な模式断面図を示す。図におい
て、（１）は電極基材であり、導電性多孔質のカーボン
繊維から構成されたペーパ状のものである。（２）は触
媒層であり、触媒粉末と撥水性結着剤としてのポリテト
ラフルオロエチレン（以下PTFEと称す）から構成された
ものである。FIG. 2 shows a general schematic sectional view of an electrode of a conventional fuel cell disclosed in, for example, JP-A-60-65465. In the figure, (1) is an electrode base material, which is a paper-like material composed of conductive porous carbon fibers. (2) is a catalyst layer, which is composed of catalyst powder and polytetrafluoroethylene (hereinafter referred to as PTFE) as a water-repellent binder.

従来、燃料電池用電極の製造方法は、触媒粉末と撥水性
結着剤としてのPTFE及び界面活性剤、溶媒等を混合分散
した触媒ペーストをスクリーン印刷法、スプレー法、ド
クターブレード法又はロールコータ法等の方法により電
極基材（１）に直接塗布又は吹付けを行つた後、加熱あ
るいは真空凍結乾燥により溶媒を除去して触媒層（２）
が形成されていた。Conventionally, a method for manufacturing an electrode for a fuel cell is a screen printing method, a spray method, a doctor blade method or a roll coater method in which a catalyst powder, PTFE as a water repellent binder, a surfactant, a catalyst paste in which a solvent and the like are mixed and dispersed. After directly coating or spraying on the electrode base material (1) by a method such as the above, the solvent is removed by heating or vacuum freeze-drying to remove the catalyst layer (2).
Had been formed.

〔発明が解決しようとする課題〕[Problems to be Solved by the Invention]

従来の燃料電池用電極の製造方法は以上のようにカーボ
ン繊維で構成された多孔質のペーパ状の電極基材（１）
に、直接、塗布又は吹付けるため全面又は部分的に、触
媒ペーストが電極基材（１）の多孔部に浸み込んだり、
あるいは電極基材（１）裏面に浸み出したりするため、
電極基材（１）と触媒層（２）の接合部境界の厚さを均
一に制御することが困難であつた。そのため電極基材
（１）への浸み込みあるいは電極基材（１）裏面への浸
み出し等、触媒ペーストによる電極基材（１）の多孔部
への目詰り、あるいは電極基材（１）裏面に電解質とし
てのリン酸の液路又は液膜が形成され、電極面内におけ
るガス拡散孔の閉塞、減少、及び分布のバラツキ等の問
題点があつた。さらには加熱乾燥の場合触媒層に粒子の
凝集等のためマツドクラツクが発生することも問題の一
つであつた。The conventional method for producing an electrode for a fuel cell is the porous paper-like electrode substrate (1) composed of carbon fibers as described above.
In order to apply or spray directly, the catalyst paste permeates the porous part of the electrode substrate (1) entirely or partially,
Or because it oozes out on the back surface of the electrode substrate (1),
It was difficult to uniformly control the thickness of the boundary between the electrode base material (1) and the catalyst layer (2). Therefore, the electrode base material (1) is soaked in the electrode base material (1) or the back surface of the electrode base material (1) is clogged with the catalyst paste, or the electrode base material (1) is clogged in the porous portion. ) A liquid channel or liquid film of phosphoric acid as an electrolyte is formed on the back surface, which causes problems such as clogging, reduction of gas diffusion holes in the electrode surface, and variation in distribution. Furthermore, in the case of heating and drying, one of the problems is that matte cracks are generated due to agglomeration of particles in the catalyst layer.

この発明は上記のような課題を解決するためなされたも
ので、電極基材と触媒層の接合部境界の厚さを均一化し
高いガス拡散性能を得るとともに触媒層のマツドクラツ
クの発生をなくし、電極の特性及び品質の向上を目的と
する。The present invention has been made to solve the above problems, uniform thickness of the junction boundary between the electrode base material and the catalyst layer to obtain high gas diffusion performance and eliminate the occurrence of the mat crack of the catalyst layer, The purpose is to improve the characteristics and quality of.

〔課題を解決するための手段〕[Means for Solving the Problems]

この発明に係る燃料電池用電極の製造方法は、触媒粉末
と撥水性結着剤及び界面活性剤、溶媒とを混合分散して
得た触媒ペーストをポリマーフイルム上に塗布した後、
電極基材を前記塗布した触媒ペースト上に重ね、触媒ペ
ーストが電極基材の多孔部に侵入しないように、両者を
スペーサを介するなどして電極基材全面をパイプローラ
で軽く押圧して接合する。次に真空凍結乾燥、プレス加
工の工程を経て電極基材上に触媒層を転写形成し一体化
したものである。The method for producing an electrode for a fuel cell according to the present invention is a method in which a catalyst powder, a water-repellent binder and a surfactant, and a catalyst paste obtained by mixing and dispersing a solvent are applied onto a polymer film,
The electrode base material is overlaid on the coated catalyst paste, and the entire surface of the electrode base material is lightly pressed and joined by a pipe roller through a spacer so that the catalyst paste does not enter the porous portion of the electrode base material. . Next, the catalyst layer is transferred and integrated on the electrode base material through the steps of vacuum freeze-drying and pressing.

〔作用〕[Action]

この発明による電極は、電極基材に触媒ペーストを直接
塗布しないで間接的に接合して触媒層を形成するため、
電極基材と触媒層の接合部境界の厚さはバラツキのない
均一化した状態で密着したものである。The electrode according to the present invention forms a catalyst layer by indirectly bonding without directly applying the catalyst paste to the electrode base material,
The thickness of the boundary between the electrode base material and the catalyst layer is uniform and adheres without variation.

〔発明の実施例〕Example of Invention

以下、この発明の実施例について説明する。 Examples of the present invention will be described below.

〔実施例１〕 第１図（ａ）のこの発明の実施例による製造過程の模式
的断面図に示すように、触媒粉末と結着剤としてのPTFE
及び界面活性剤、溶媒とを混合分散して得た触媒ペース
ト（４）をロールコータ法により例えば360×650×0.05
mmのポリマーフイルム（３）、例えばポリイミドフイル
ム（東レ。デユポン製．商品名カプトン）に塗布した
後、PTFE水溶液で撥水処理した例えば360×650×0.1mm
のカーボン繊維からなるペーパ状の電極基材（１）を静
かに重ね、触媒ペースト（４）と電極基材（１）が密着
するようスペーサーを介して軽くパイプローラにより基
材全面を押圧するようにして接合する。次に接合した電
極を予備凍結槽で急速凍結した後、真空凍結乾燥器（図
示せず）内で氷状の溶媒を昇華消失させた後取出し、液
圧プレスにて加圧後、ポリイミドフイルム（３）をはが
し第１図（ｂ）のこの発明による電極の模式的断面図に
示すように、触媒層（21）を電極基材（１）に転写形成
して一体化したものを焼成して電極を作製した。この製
造方法により得た電極は均一な触媒層（21）の膜厚を有
し、従来方法の電極に見られた電極基材（１）への部分
的な浸み込みあるいは浸み出し現象の見られないもので
あり、かつ、触媒層にはマツドクラツクのないものであ
つた。Example 1 As shown in the schematic sectional view of the manufacturing process according to the example of the present invention in FIG. 1 (a), catalyst powder and PTFE as a binder were used.
And a catalyst paste (4) obtained by mixing and dispersing a surfactant and a solvent by a roll coater method, for example, 360 × 650 × 0.05
mm polymer film (3), for example, polyimide film (Toray, made by Dyupon, trade name Kapton), and then water repellent with PTFE aqueous solution, eg 360 × 650 × 0.1mm
Gently stack the paper-like electrode base material (1) made of carbon fiber, and lightly press the entire surface of the base material with a pipe roller through a spacer so that the catalyst paste (4) and the electrode base material (1) are in close contact with each other. And join. Next, the joined electrodes are rapidly frozen in a preliminary freezing tank, and then the ice-like solvent is removed by sublimation in a vacuum freeze dryer (not shown) and then taken out. 3) Peeling off, as shown in the schematic sectional view of the electrode according to the present invention in FIG. An electrode was prepared. The electrode obtained by this manufacturing method has a uniform thickness of the catalyst layer (21), and the electrode substrate (1) seen in the electrode of the conventional method is partially penetrated or exuded. It was not seen, and the catalyst layer had no matte crack.

〔比較例１〕 実施例１と同様の触媒ペースト（４）を、ロールコータ
法により直接例えば360×650×0.1mmの撥水処理した電
極基材（１）に塗布した後、実施例１と同様の製造工程
を経て作製した電極は、塗布時触媒ペースト（４）が基
材に浸み出したため、電極基材（１）裏面に触媒層（2
1）が多量に付着していた。Comparative Example 1 The same catalyst paste (4) as in Example 1 was directly applied to the water-repellent electrode base material (1) of, for example, 360 × 650 × 0.1 mm by the roll coater method, and then In the electrode manufactured through the same manufacturing process, since the catalyst paste (4) leached into the base material during application, the catalyst layer (2) was formed on the back surface of the electrode base material (1).
1) was attached in large amounts.

〔実施例２〕 実施例１と同様の触媒ペースト（４）をロールコータ法
により例えば360×650×0.05mmのポリエチレンテレフタ
レートフイルム（３）（一般商品名マイラー）に塗布し
た後、未揆水の例えば360×650×0.2mmの電極基材
（１）を使用し、実施例１と同様の製造工程を経て電極
を作製した。この製造方法により得た電極は実施例１の
揆水処理をした電極基材（１）を使用して作製した電極
と同様、電極基材（１）への触媒ペースト（４）の浸み
込みあるいは浸み出しは見られず、触媒層（21）のマツ
ドクラツクもないものであつた。[Example 2] The same catalyst paste (4) as in Example 1 was applied to a polyethylene terephthalate film (3) (general trade name: Mylar) having a size of 360 x 650 x 0.05 mm by a roll coater method. For example, the electrode base material (1) having a size of 360 × 650 × 0.2 mm was used, and an electrode was produced through the same manufacturing process as in Example 1. The electrode obtained by this manufacturing method is the same as the electrode produced by using the water-treated electrode base material (1) of Example 1, in which the catalyst paste (4) penetrates into the electrode base material (1). Alternatively, no leaching was observed and there was no matting crack in the catalyst layer (21).

〔比較例２〕 実施例１と同様の触媒ペースト（４）をロールコータ法
により直接未揆水の例えば360×650×0.2mmの電極基材
（１）に塗布し、実施例１と同様の製造工程を経て作製
した電極は触媒ペースト（４）が電極基材（１）裏面に
浸み出すとともに、電極基材（１）裏面に空気留りが生
じ、電極の面内に直径10〜20mm大の斑点状凹凸のある現
象が見られ電極として使用できないものであつた。[Comparative Example 2] The same catalyst paste (4) as in Example 1 was directly applied to the un-watered electrode substrate (1) of, for example, 360 x 650 x 0.2 mm by the roll coater method, and the same as in Example 1. In the electrode manufactured through the manufacturing process, the catalyst paste (4) seeps out to the back surface of the electrode base material (1) and air retention occurs on the back surface of the electrode base material (1), and the diameter of the electrode surface is 10 to 20 mm. The phenomenon with large speckled irregularities was observed, and it could not be used as an electrode.

〔実施例３〕 実施例１と同様の触媒ペースト（４）をスクリーン印刷
法により例えば200×200×0.025mmのポリイミドフイル
ム（３）に塗布した後、例えば150×150×0.4mm,150×1
50×0.1mmのカーボン繊維からなるペーパ状の揆水処理
した基材あるいは未揆水の電極基材（１）をそれぞれ触
媒ペースト（４）と密着するよう軽く、ハケで押圧する
ようにして接合し以後、実施例１と同様の工程で電極を
作製した。これらの実施例による電極においても均一な
触媒層（21）の膜厚が得られ、電極基材（１）への浸み
込みあるいは浸み出しもなく、かつ、マツドクラツクの
ないものが得られた。Example 3 The same catalyst paste (4) as in Example 1 was applied to a polyimide film (3) of, for example, 200 × 200 × 0.025 mm by a screen printing method, and then, for example, 150 × 150 × 0.4 mm, 150 × 1.
Paper-like water-free base material made of 50 x 0.1 mm carbon fibers or un-water-free electrode base material (1) is bonded to the catalyst paste (4) lightly and firmly with a brush. After that, an electrode was produced in the same process as in Example 1. Also in the electrodes according to these examples, a uniform thickness of the catalyst layer (21) was obtained, and the electrode base material (1) was not soaked or exuded, and there was no mat crack. .

以上のようにこの発明に係る電極の製造方法によれば、
電極基材（１）の厚さ、空隙率、及び揆水の有無に関係
なく、電極基材（１）と触媒層（21）の接合部境界の厚
さを均一に制御することが容易になつた。As described above, according to the electrode manufacturing method of the present invention,
Regardless of the thickness of the electrode base material (1), the porosity, and the presence or absence of drainage, it is easy to uniformly control the thickness of the boundary between the electrode base material (1) and the catalyst layer (21). Natsuta.

なお、この発明による電極の製造方法に使用するポリマ
ーフイルム（３）は、実施例ではポリイミド、ポリエチ
レンテレフタレートを使用したがポリエチレン，ポリプ
ロピレンでも可能である。またポリマーフイルム（３）
の厚さは0.025〜0.1mmの範囲が望ましい0.025mm以下で
は、触媒ペースト（４）の塗布時しわが発生し易く、0.
1mm以上の厚さでは、真空凍結乾燥、加圧工程後に、触
媒層（21）からはがす時の剥離が悪くなる傾向にある。The polymer film (3) used in the method of manufacturing the electrode according to the present invention uses polyimide or polyethylene terephthalate in the examples, but polyethylene or polypropylene may be used. Polymer film (3)
The thickness is preferably in the range of 0.025 to 0.1 mm. When the thickness is 0.025 mm or less, wrinkles are apt to occur when the catalyst paste (4) is applied, and
When the thickness is 1 mm or more, peeling off from the catalyst layer (21) tends to be poor after the vacuum freeze-drying and pressurizing steps.

〔発明の効果〕〔The invention's effect〕

以上のようにこの発明によれば、触媒ペーストを直接、
電極基材に塗布せず、ポリマーフイルムに塗布した後、
ポリマーフイルム上に電極基材を重ねて触媒ペーストと
密着するようしたので、電極基材と触媒層の接合部境界
の厚さを均一に制御できるようになつた。そのため、電
極基材の多孔部の触媒層による目詰り、電極基材裏面の
触媒層付着が解消され、従来方法により製造された電極
に比べ、高いガス拡散孔を保有し、マツドクラツクのな
い品質の安定した電極が得られる。As described above, according to the present invention, the catalyst paste is directly
After applying to the polymer film without applying to the electrode substrate,
Since the electrode base material is placed on the polymer film so as to adhere to the catalyst paste, the thickness of the boundary between the electrode base material and the catalyst layer can be controlled uniformly. Therefore, clogging by the catalyst layer of the porous part of the electrode base material, adhesion of the catalyst layer on the back surface of the electrode base material is eliminated, and compared with the electrode manufactured by the conventional method, it has higher gas diffusion holes and has no matte crack quality. A stable electrode can be obtained.

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

第１図（ａ），（ｂ）はこの発明の一実施例による燃料
電池用電極を示す断面図、第２図は従来の燃料電池用電
極を示す断面図である。 図において、（１）は電極基材、（３）はポリマーフイ
ルム、（４）は触媒ペースト、（21）は触媒層である。 なお、各図中、同一符号は同一または相当部分を示す。1 (a) and 1 (b) are sectional views showing a fuel cell electrode according to an embodiment of the present invention, and FIG. 2 is a sectional view showing a conventional fuel cell electrode. In the figure, (1) is an electrode substrate, (3) is a polymer film, (4) is a catalyst paste, and (21) is a catalyst layer. In each drawing, the same reference numerals indicate the same or corresponding parts.

Claims (1)

【特許請求の範囲】[Claims] 【請求項１】触媒粉末と撥水性結着剤及び界面活性剤、
溶媒とを、混合分散して得た触媒ペーストをポリマーフ
イルム上に塗布した後、電極基材を重ねて接合し、真空
凍結乾燥、プレス加工の工程を経て前記電極基材に触媒
層を転写形成し一体化したことを特徴とする燃料電池用
電極の製造方法。1. A catalyst powder, a water-repellent binder and a surfactant,
A catalyst paste obtained by mixing and dispersing a solvent is applied on the polymer film, and then the electrode base materials are laminated and bonded, and the catalyst layer is transferred and formed on the electrode base material through the steps of vacuum freeze-drying and pressing. A method for manufacturing an electrode for a fuel cell, characterized by being integrated with each other.
JP1035403A 1989-02-15 1989-02-15 Method for manufacturing fuel cell electrode Expired - Lifetime JPH0766814B2 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP1035403A JPH0766814B2 (en) 1989-02-15 1989-02-15 Method for manufacturing fuel cell electrode

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP1035403A JPH0766814B2 (en) 1989-02-15 1989-02-15 Method for manufacturing fuel cell electrode

Publications (2)

Publication Number Publication Date
JPH02215049A JPH02215049A (en) 1990-08-28
JPH0766814B2 true JPH0766814B2 (en) 1995-07-19

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Country Status (1)

Country Link
JP (1) JPH0766814B2 (en)

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH09199138A (en) * 1996-01-19 1997-07-31 Toyota Motor Corp Manufacture of electrode for fuel cell or electrode electrolytic film bonding body, and electrode for fuel cell
US20090053583A1 (en) * 2005-01-14 2009-02-26 Umicore Ag & Co Kg Gas diffusion electrode and process for producing it and its use
JP5493756B2 (en) * 2009-11-19 2014-05-14 富士電機株式会社 Manufacturing method of gas diffusion electrode

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