JPH02112161A - Manufacture of carbon component for fuel cell - Google Patents
Manufacture of carbon component for fuel cellInfo
- Publication number
- JPH02112161A JPH02112161A JP63265722A JP26572288A JPH02112161A JP H02112161 A JPH02112161 A JP H02112161A JP 63265722 A JP63265722 A JP 63265722A JP 26572288 A JP26572288 A JP 26572288A JP H02112161 A JPH02112161 A JP H02112161A
- Authority
- JP
- Japan
- Prior art keywords
- separator
- carbon
- less
- firing
- bonding
- 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.)
- Granted
Links
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 27
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 23
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 13
- 239000000446 fuel Substances 0.000 title claims description 13
- 239000000463 material Substances 0.000 claims abstract description 44
- 239000011347 resin Substances 0.000 claims abstract description 9
- 229920005989 resin Polymers 0.000 claims abstract description 9
- 229920001187 thermosetting polymer Polymers 0.000 claims abstract description 8
- 239000000853 adhesive Substances 0.000 claims abstract description 7
- 230000001070 adhesive effect Effects 0.000 claims abstract description 7
- 230000007797 corrosion Effects 0.000 claims abstract description 3
- 238000005260 corrosion Methods 0.000 claims abstract description 3
- 238000000034 method Methods 0.000 claims description 22
- 239000002131 composite material Substances 0.000 claims description 15
- 239000007772 electrode material Substances 0.000 claims description 14
- 238000010304 firing Methods 0.000 claims description 12
- 239000002243 precursor Substances 0.000 claims description 12
- 238000010000 carbonizing Methods 0.000 claims description 4
- 238000005452 bending Methods 0.000 claims description 3
- 230000003746 surface roughness Effects 0.000 claims description 3
- 238000000926 separation method Methods 0.000 abstract 2
- 230000003247 decreasing effect Effects 0.000 abstract 1
- 230000035699 permeability Effects 0.000 abstract 1
- 239000007789 gas Substances 0.000 description 6
- 239000005011 phenolic resin Substances 0.000 description 5
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 4
- 239000012298 atmosphere Substances 0.000 description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 3
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 238000000465 moulding Methods 0.000 description 3
- 230000001590 oxidative effect Effects 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 229920000049 Carbon (fiber) Polymers 0.000 description 2
- YLQBMQCUIZJEEH-UHFFFAOYSA-N Furan Chemical compound C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 2
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 2
- 239000004917 carbon fiber Substances 0.000 description 2
- 238000003763 carbonization Methods 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 238000005304 joining Methods 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000012299 nitrogen atmosphere Substances 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 239000000758 substrate Substances 0.000 description 2
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 description 1
- JZUFKLXOESDKRF-UHFFFAOYSA-N Chlorothiazide Chemical compound C1=C(Cl)C(S(=O)(=O)N)=CC2=C1NCNS2(=O)=O JZUFKLXOESDKRF-UHFFFAOYSA-N 0.000 description 1
- 229920003261 Durez Polymers 0.000 description 1
- 230000005856 abnormality Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 239000001913 cellulose Substances 0.000 description 1
- 229920002678 cellulose Polymers 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 238000007730 finishing process Methods 0.000 description 1
- 239000007849 furan resin Substances 0.000 description 1
- 230000005484 gravity Effects 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 238000002955 isolation Methods 0.000 description 1
- 238000004898 kneading Methods 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229920001568 phenolic resin Polymers 0.000 description 1
- 238000005498 polishing Methods 0.000 description 1
- 229920002239 polyacrylonitrile Polymers 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 230000002265 prevention Effects 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- JOXIMZWYDAKGHI-UHFFFAOYSA-N toluene-4-sulfonic acid Chemical compound CC1=CC=C(S(O)(=O)=O)C=C1 JOXIMZWYDAKGHI-UHFFFAOYSA-N 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
-
- 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
- H01M4/96—Carbon-based electrodes
-
- 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
Description
【発明の詳細な説明】
［産業上の利用分野］
本発明は、電極、セパレークおよびザイドシールを複合
一体的に形成してなるりん酸型燃料電池用カーボン部材
の製造方法に関する。DETAILED DESCRIPTION OF THE INVENTION [Industrial Application Field] The present invention relates to a method for manufacturing a carbon member for a phosphoric acid fuel cell, in which an electrode, a separator, and a zide seal are integrally formed.
［従来の技術］
近時、燃料電池を構成するカーボン部材において、機械
的強度の向上、電気的・熱的抵抗の低減およびセル組立
の簡素化を図るために電極とセパレータの両部材を予め
一体形成して複合構造とする試みが盛んに進められてい
る。[Prior Art] In recent years, in carbon components that constitute fuel cells, electrodes and separators have been integrated in advance in order to improve mechanical strength, reduce electrical and thermal resistance, and simplify cell assembly. Attempts to form composite structures are actively underway.
このような複合部材の製造手段としては、例えば特開昭
６０−２０４７１号公報、実開昭６０−１５７５９号公
報などに開示されているような電極材、セパレータ材お
よびサイドシール材を接着剤で結合したのち焼成処理す
る接合焼成法が実用性に優れて（る。この接合焼成法に
は、カーボン材からなる電極、セパレータおよびサイド
シールを接合して焼成する方法と、カーボン化（焼成炭
化）前の成形基材であるグリーン前駆体段階の電極、セ
パレータおよびサイドシールを接合して焼成する方法と
がある。As a means of manufacturing such a composite member, for example, an electrode material, a separator material, and a side seal material as disclosed in Japanese Patent Application Laid-Open No. 60-20471 and Japanese Utility Model Application Publication No. 60-15759 are bonded with an adhesive. The bonding and firing method, in which the electrodes, separators, and side seals made of carbon materials are bonded and fired, is highly practical. There is a method in which the electrodes, separators, and side seals at the green precursor stage, which are the previous molding base materials, are bonded and fired.
一般に、上記の燃料電池用複合部材を製造するにあたっ
て要求されるポイントは、複合構成としての性能確保、
接合部分（とくにサイドシール部）の信顧性確保、そし
て工程の短縮、簡略化にあるが、上述した接合焼成法の
うち後者のグリーン前駆体接合方式はこれらの要求項目
を一応満たすものといえる。In general, the points required in manufacturing the above-mentioned composite members for fuel cells are ensuring performance as a composite structure,
The aim is to ensure the reliability of the joint parts (especially the side seal parts) and to shorten and simplify the process, and among the above-mentioned joint firing methods, the latter green precursor joining method can be said to meet these requirements. .
ところが、グリーン前駆体接合方式の場合にはサイドシ
ール部の設置に困難性があって同時接合ができないため
、電極基材の接合処理後に別途接合しなければならない
工程上の煩雑性があった。However, in the case of the green precursor bonding method, it is difficult to install the side seal portion and simultaneous bonding is not possible, resulting in a complicated process in which bonding must be performed separately after the electrode base material bonding process.
上記の欠点を解消する方策として、特定性状のガス隔離
セパレータ部ならびにガス漏出防止縁部（サイドシール
部）とが炭化焼成により一体化された燃料電池セパレー
タ及びその製造方法（特開昭６１−１９０７１号公報）
、気体不透過性炭素質板の両面に縁端部分を除いて互い
に直交する方向に凹設部を設ｉＪることによりサイドシ
ール部とセパレータ材を−・体に形成し、この凹設部に
樹脂含浸した多孔性シートを介して電極材を接合したの
ち焼成処理する燃料電池用複合電極の製造方法（特開昭
６２−１８８１７３号公報）などが提案されている。As a measure to eliminate the above-mentioned drawbacks, a fuel cell separator in which a gas isolation separator part having a specific property and a gas leakage prevention edge part (side seal part) are integrated by carbonization firing and its manufacturing method (Japanese Patent Laid-Open No. 61-19071 Publication No.)
, by forming recessed portions on both sides of the gas-impermeable carbonaceous plate in directions perpendicular to each other except for the edge portions, the side seal portion and the separator material are formed into a body, and in the recessed portions. A method for manufacturing a composite electrode for a fuel cell (Japanese Patent Application Laid-Open No. 188173/1983) has been proposed, in which electrode materials are bonded via a resin-impregnated porous sheet and then fired.
しかしながら、セパレータ材とサイドシール部とを炭化
焼成により一体化する特開昭６１−１９０７１号の方法
では両部材の接合界面における気密性が十分に付与され
ない問題点があり、また特開昭６２１８８１．７３号の
方法は、セパレータ材とサイドシール部間の気密性につ
いては万全に保持されるが、複合構造全体としての性能
に改良の余地があり、例えば実用過程における部材の剥
離、損耗、破損などの現象を払拭することができなかっ
た。However, the method disclosed in JP-A No. 61-19071, in which the separator material and the side seal portion are integrated by carbonization firing, has the problem that sufficient airtightness cannot be provided at the bonding interface between the two members. Although the method of No. 73 completely maintains the airtightness between the separator material and the side seal, there is room for improvement in the performance of the composite structure as a whole, such as peeling, wear, and damage of parts during the practical process. It was not possible to dispel this phenomenon.
本発明は、複合構造としての性能を改善するとともに部
材接合部分の信顧性と製造工程の簡素化を図った製造方
法の捉供を目的とするものである。An object of the present invention is to provide a manufacturing method that improves the performance of a composite structure, improves the reliability of joining parts, and simplifies the manufacturing process.
上記の目的を達成するための本発明による燃料電池用カ
ーボン部材の製造方法は、グリーン前駆体の段階でサイ
ドシール部を形成する縁端部分を残して凹面状に成形し
たセパレータ基材またはこれを焼成炭化したセパレータ
材に、多孔質炭素電極を構成するグリーン前駆体基材ま
たはこれを焼成炭化した電極材を嵌装して一体に接合し
たのち焼成処理して複合構造のカーボン部材を得る方法
において、セパレータ材として熱膨張係数３Ｘ１０−６
゛Ｃ−１以下、曲げ強度９００ｋｇ／ｃ／以上、気体透
過量１０−’ｃｃ／ｃ＋Ｉｔ ・ｍｉｎ以下およびｇ線
電流密度５／７Ａ／ｄ以下のカーボン特性を有する材料
を選択し、かつ接合時、凹面に熱硬化性樹脂系の接着剤
を塗布することを構成上の特徴とする。In order to achieve the above object, the method for producing a carbon member for fuel cells according to the present invention includes a separator base material formed into a concave shape leaving the edge portion forming the side seal portion at the green precursor stage, or In a method of obtaining a carbon member with a composite structure by inserting a green precursor base material constituting a porous carbon electrode or an electrode material obtained by firing and carbonizing this into a fired and carbonized separator material, bonding them together, and then firing them. , thermal expansion coefficient 3X10-6 as separator material
゛C-1 or less, bending strength of 900 kg/c/ or more, gas permeation of 10-'cc/c+It min or less, and g-line current density of 5/7 A/d or less. The structural feature is that a thermosetting resin adhesive is applied to the concave surface.
サイドシール部を備えるセパレータのグリーン前駆体は
、好ましくは黒鉛のようなカーボン質の微粉末とフェノ
ール系あるいはフラン系など高炭化性の熱硬化性樹脂と
の混練物を縁端部分を残して凹面状に成形しえる所定形
態の金型に填めて熱圧することにより形成される。形成
されたグリーン前駆体によるセパレータ基材は、非酸化
雰囲気中で８００°Ｃ以上の温度に加熱処理し樹脂成分
を焼成炭化することによってカーボンセパレータ材とす
ることもできる。The green precursor of the separator with the side seal part is preferably a mixture of carbonaceous fine powder such as graphite and highly carbonizable thermosetting resin such as phenol type or furan type, and is formed into a concave surface with the edges remaining. It is formed by placing it in a mold of a predetermined shape that can be molded into a shape and pressing it under heat. The separator base material made of the formed green precursor can also be made into a carbon separator material by heat-treating it at a temperature of 800° C. or higher in a non-oxidizing atmosphere to sinter and carbonize the resin component.
上記工程において、フェラーとして用いる黒鉛微粉末の
粒度、熱硬化性樹脂バインダーの配合比率、混練の条件
等を調整制御することにより、本発明で特定した熱膨張
係数３ＸｌＯ−’℃−１以下、曲げ強度９００ｋｇ／ｃ
＋ｆ１以上、気体透過量１０−’ｃｃ／ｃ＋ｆｌ ・ｍ
ｉｎ以下および腐蝕電流密度５ハ／ ｃ＋！以下のカー
ボン特性が付与される。In the above process, by adjusting and controlling the particle size of the graphite fine powder used as the feller, the blending ratio of the thermosetting resin binder, the kneading conditions, etc., the thermal expansion coefficient specified in the present invention is 3 Strength 900kg/c
+f1 or more, gas permeation amount 10-'cc/c+fl ・m
in and corrosive current density 5 ha/c+! The following carbon properties are imparted.
なお、これらのカーボン特性のうち、気体透過量は使用
ガス；窒素、圧カニ］ｋｇ／ｃ＋ｆｌ、温度；常温での
測定値、また、ここでいう腐蝕電流密度とは２００°Ｃ
のりん酸中において陽極電位０．８ＶＲＨＥ。Of these carbon properties, the gas permeation amount is the gas used: nitrogen, pressure crab] kg/c+fl, the temperature: the value measured at room temperature, and the corrosion current density here is the value measured at 200°C.
Anode potential 0.8 VRHE in phosphoric acid.
通電開始後５００分後での測定値をさし、更に曲げ強度
はＪＩＳ Ｋ６９１１、熱膨張係数は炭素協会規格ＪＣ
ＡＳ−１８−１９７８を適用して得られた値を用いるも
のとする。但し、熱膨張係数は常温から２００°Ｃまで
のものとする。Refers to the measured value 500 minutes after the start of energization.Furthermore, the bending strength is JIS K6911, and the thermal expansion coefficient is the Carbon Society Standard JC.
The value obtained by applying AS-18-1978 shall be used. However, the coefficient of thermal expansion is from room temperature to 200°C.
上記のカーボン特性は複合構造の性能改善に必要な要件
で、この限界値を外れるとヒートサイクルに伴う部材の
剥離、損耗、破損などの発生が著増する。The above-mentioned carbon properties are necessary for improving the performance of composite structures, and if these limits are exceeded, the occurrence of peeling, wear, damage, etc. of members due to heat cycling increases significantly.
凹面の成形はセパレータ材の片面または両面に形成され
るが、両面に形成する場合には第１図に示すようにサイ
ドシール部１となる縁端部分およびセパレータ材２とな
る凹面の方向が上下面において互いに直交する状態に成
形される。The concave surface can be formed on one or both sides of the separator material, but if it is formed on both sides, the direction of the edge portion that will become the side seal part 1 and the concave surface that will become the separator material 2 is upward, as shown in Figure 1. They are formed so that they are perpendicular to each other on the lower surface.
多孔質炭素電極は、炭素繊維あるいはポリアクリルニト
リル、セルロースなどの有機質繊維を例えばフェノール
樹脂のような熱硬化性樹脂と共にモールド法、抄紙法等
の手段を用いて薄板状に成形し加熱硬化する方法でグリ
ーン前駆体基材が得られ、これを非酸化雰囲気中８００
’Ｃ以上に焼成炭化することによりカーボン化電極材が
形成される。Porous carbon electrodes are produced by molding carbon fibers or organic fibers such as polyacrylonitrile or cellulose together with thermosetting resins such as phenol resin into a thin plate using methods such as molding or papermaking, and then heating and curing the electrodes. A green precursor substrate was obtained, which was heated at 800 °C in a non-oxidizing atmosphere.
A carbonized electrode material is formed by firing and carbonizing the material to a temperature higher than 'C.
サイドシール部を有するセパレータ基材またはセパレー
タ材と電極基板または電極材の接合は、セパレータの凹
面に熱硬化性樹脂系の接着剤を塗布したのち電極部材を
嵌装し５０〜２００°Ｃ程度の温度と１ｋｇ／ｃ＋＋Ｔ
以上の加圧力を適用して熱圧することによっておこなわ
れる。To join the separator base material or separator material having a side seal portion to the electrode substrate or electrode material, apply a thermosetting resin adhesive to the concave surface of the separator, fit the electrode member, and heat at approximately 50 to 200°C. Temperature and 1kg/c++T
This is done by applying the above pressure and applying heat.
使用される熱硬化性樹脂系の接着剤にはフェノール系ま
たはフラン系樹脂の初期縮合物に適宜な硬化剤を配合し
たものが好適であるが、これに黒鉛、コークス等のカー
ボン微粉末を３０〜７０重量％の範囲で均一混合すると
固有抵抗を低下させるために有効である。The thermosetting resin adhesive to be used is preferably a mixture of an initial condensate of phenol or furan resin with an appropriate hardening agent. Uniform mixing in the range of ~70% by weight is effective for lowering the resistivity.
また、接合時、予め凹面を１０μｍＲＺ以上の表面粗さ
に研磨処理することにより、接合強度が著しく向上する
。Moreover, by polishing the concave surface in advance to a surface roughness of 10 μmRZ or more during bonding, the bonding strength is significantly improved.
接合後の複合部材は、常法に従って非酸化性雰囲気下に
１０００〜２０００’Ｃの温度域で焼成炭化し、更に必
要に応して３０００°Ｃの温度で黒鉛化処理をおこなう
。第２図は、焼成処理後の形態を示したもので、１はサ
イドシール部、２はセパレータ材、３はセパレータ材の
上下凹面に一体接合した電極材である。The composite member after bonding is fired and carbonized in a non-oxidizing atmosphere at a temperature range of 1000 to 2000°C according to a conventional method, and further graphitized at a temperature of 3000°C if necessary. FIG. 2 shows the form after the firing process, in which 1 is a side seal part, 2 is a separator material, and 3 is an electrode material integrally joined to the upper and lower concave surfaces of the separator material.
このようにして得られた複合構造のカーボン部材は、第
３図に示すように電極材に所定の溝４を切削するととも
に外形仕上げ加工を施して燃料電池用セルとする。The carbon member having the composite structure thus obtained is made into a fuel cell by cutting a predetermined groove 4 into the electrode material and finishing the outer shape as shown in FIG.
このように、本発明により製造される複合構造の燃料電
池用カーボン部材は、サイドシール部とセパレータ材が
同一材料で一体形成されているためこの部位の気密性お
よび界面剥離が間匙となることはなく、そのうえセパレ
ータ材の材質特性を選択して実用性能の向上を図ってい
るので、ヒートサイクルによる部材の剥離、損耗、破損
等の現象発生は効果的に減少する。As described above, in the carbon member for fuel cells having a composite structure manufactured according to the present invention, since the side seal portion and the separator material are integrally formed of the same material, the airtightness of this portion and interfacial peeling are limited. Moreover, since the material properties of the separator material are selected to improve practical performance, the occurrence of phenomena such as peeling, wear, and damage of members due to heat cycles is effectively reduced.
以下、本発明の実施例を比較例と対比して説明する。 Examples of the present invention will be described below in comparison with comparative examples.
実施例１〜３、比較例１〜２
平均粒径５μｍの黒鉛微粉末と液状フェノール樹脂（住
友デュレズ■製、“ＰＲ９４０” ）をニーグーで均質
に混練したのち、凹形状金型を用い温度１５０°Ｃ１圧
カニ １００ｋｇ ／ ｃｄｌの条件で１５分間熱圧
成形した。成形されたグリーン前駆体は、上下面にサイ
ドシール部を形成する縁端部分を残して厚さＩＩＩＩＩ
ｌｌの凹面が直交状に形成された一辺１５０ｍｍの正方
形薄板であった。ついで、成形品を電気炉に移し、窒素
ガス雰囲気中で１３００″Ｃまでの温度で焼成炭化して
特性の異なる５種類のカーボンセパレータ材（第１図形
状）を得た。Examples 1 to 3, Comparative Examples 1 to 2 Fine graphite powder with an average particle size of 5 μm and liquid phenol resin (manufactured by Sumitomo Durez ■, "PR940") were homogeneously kneaded in a Ni-Goo, and then kneaded at a temperature of 150 using a concave mold. It was hot-pressed for 15 minutes at 100 kg/cdl at 1°C. The molded green precursor has a thickness of Ⅲ, leaving edge portions forming side seals on the top and bottom surfaces.
It was a square thin plate with a side of 150 mm and a concave surface of 150 mm perpendicular to each other. Next, the molded products were transferred to an electric furnace and fired and carbonized at a temperature up to 1300''C in a nitrogen gas atmosphere to obtain five types of carbon separator materials (shaped in FIG. 1) having different characteristics.
炭素繊維チョップ（平均径１５デニール、平均長８ｍｍ
）７０重量部、水溶性フェノール樹脂〔日本ライヒホー
ルド■製、“プライオーフェンＪ３０３ ”“〕１１０
重量および水２０重量部を攪拌混合して均一なスラリー
状分散液を調製した。このスラリーを抄紙法によって薄
板状に成形し、１７０°Ｃで加熱硬化したのち窒素雰囲
気に保持した電気炉中で１０００°Ｃの温度により焼成
炭化して緬１５０ｍ＋ｎ、横１００ｍｍ、厚さｌ ｍｍ
の多孔質炭素電極材を作成した。得られた電極材の特性
は、見掛比重０．５６ｇ／ｃｃ、気孔率６８．１％であ
った。Carbon fiber chop (average diameter 15 denier, average length 8mm)
) 70 parts by weight, water-soluble phenol resin [manufactured by Nippon Reichhold ■, "Pryophen J303"] 110
A uniform slurry-like dispersion was prepared by stirring and mixing 20 parts by weight of water. This slurry was formed into a thin plate shape using a papermaking method, heated and hardened at 170°C, and then fired and carbonized at a temperature of 1000°C in an electric furnace kept in a nitrogen atmosphere to form a sheet with a length of 150m+n, a width of 100mm, and a thickness of 1 mm.
A porous carbon electrode material was created. The characteristics of the obtained electrode material were that the apparent specific gravity was 0.56 g/cc and the porosity was 68.1%.
次に、セパレーク材の上下凹面をサンドペーパ研磨によ
り２０μｍＲＺの表面粗さに仕上げ、この面にフェノー
ル樹脂初期縮合物１００重量部、黒鉛微粉（平均粒径２
０ｆｍ）８０重量部、パラトルエンスルホン酸クロライ
ド５重量部を各配合した接着剤を均質に塗布した。引続
き上下凹面に電極材を嵌装し、８０゛Ｃの温度と５ ｋ
ｇ ／ ｃｉの圧力に１時間保持して接合した。Next, the upper and lower concave surfaces of the separator material were polished with sandpaper to a surface roughness of 20 μm RZ, and this surface was coated with 100 parts by weight of a phenolic resin initial condensate and fine graphite powder (average particle size 2
An adhesive containing 80 parts by weight of 0fm) and 5 parts by weight of para-toluenesulfonic acid chloride was uniformly applied. Subsequently, electrode materials were fitted on the upper and lower concave surfaces, and heated at a temperature of 80°C and 5k.
Bonding was carried out by holding at a pressure of g/ci for 1 hour.
接合部材は、電気炉に移し窒素雰囲気下で１３００°Ｃ
の温度で焼成処理したのち、電極材の溝加工その他の仕
上加工を施して第３図のような複合構造の燃料電池用カ
ーボン部材を製造した。The joining members were transferred to an electric furnace and heated at 1300°C under a nitrogen atmosphere.
After firing at a temperature of , the electrode material was subjected to grooving and other finishing processes to produce a carbon member for a fuel cell having a composite structure as shown in FIG. 3.
上記のようにして製造した各カーボン部材を５セル積層
した試験セルを用いて発電テスト（２００°Ｃ１０，８
ＶＲＨＥ、 １００Ｏｈｒ、 ｌ ｋｇ／ｃ＋ｆｌ）
を実施した。Power generation test (200°C10,8
VRHE, 100Ohr, l kg/c+fl)
was carried out.
その結果をセパレータ材の特性と対比させて下表に示し
た。The results are shown in the table below in comparison with the characteristics of the separator material.
上表に示したように、本発明のセパレータ材′＋ｈ性要
件を満たす実施例はいずれも異常は認められなかった。As shown in the above table, no abnormality was observed in any of the examples satisfying the separator material'+h property requirements of the present invention.
（発明の効果）
異常のとおり、本発明に従えばザイトシール部と一体化
したセパレータ材の材質特性を選択することによって複
合構造としての性能、部材接合部の信頼性等を改善した
燃料電池用カーボン部材を簡素なプロセスで製造するこ
とができるから、常に安全な発熱操業が保証される。(Effects of the Invention) As unusual, according to the present invention, carbon for fuel cells has improved performance as a composite structure, reliability of member joints, etc. by selecting the material properties of the separator material integrated with the zyte seal part. Since the parts can be manufactured using a simple process, safe heat-generating operations are always guaranteed.
第１図は本発明のセパレータ材を示した斜視図、第２図
はセパレータ材に電極材を接合して焼成処理した形態を
示す斜視図、第３図は最終形態を示す斜視図である。
１・・・ザイドシール部、 ２・・セパレータ材、３
・・電極材、 ４・・・溝。FIG. 1 is a perspective view showing the separator material of the present invention, FIG. 2 is a perspective view showing a form in which an electrode material is bonded to the separator material and fired, and FIG. 3 is a perspective view showing the final form. 1... Zyde seal part, 2... Separator material, 3
...electrode material, 4...groove.
Claims (1)
縁端部分を残して凹面状に成形したセパレータ基材また
はこれを焼成炭化したセパレータ材に、多孔質炭素電極
を構成するグリーン前駆体基材またはこれを焼成炭化し
た電極材を嵌装して一体に接合したのち焼成処理して複
合構造のカーボン部材を得る方法において、セパレータ
材として熱膨張係数３×１０＾−＾６℃＾−＾１以下、
曲げ強度９００ｋｇ／ｃｍ＾２以上、気体透過量１０＾
−＾５ｃｃ／ｃｍ＾２・ｍｉｎ以下および腐蝕電流密度
５μＡ／ｃｍ＾２以下のカーボン特性を有する材料を選
択し、かつ接合時、凹面に熱硬化性樹脂系の接着剤を塗
布することを特徴とする燃料電池用カーボン部材の製造
方法。 ２、接合時、予め凹面を１０μｍＲＺ以上の表面粗さに
処理する請求項１記載の燃料電池用カーボン部材の製造
方法。[Scope of Claims] 1. A porous carbon electrode is formed on a separator base material formed into a concave shape leaving the edge part forming the side seal part at the green precursor stage, or on a separator material obtained by firing and carbonizing this separator base material. In the method of obtaining a carbon member with a composite structure by inserting a green precursor base material or an electrode material obtained by firing and carbonizing the green precursor base material, bonding them together, and then firing the same, a thermal expansion coefficient of 3 × 10^-^ is used as a separator material. Below 6℃＾-＾1,
Bending strength 900kg/cm^2 or more, gas permeation rate 10^
- A material with carbon properties of less than 5 cc/cm^2 min and a corrosion current density of less than 5 μA/cm^2 is selected, and a thermosetting resin adhesive is applied to the concave surface during bonding. A method for manufacturing a carbon member for a fuel cell. 2. The method for manufacturing a carbon member for a fuel cell according to claim 1, wherein the concave surface is treated in advance to a surface roughness of 10 μm RZ or more during bonding.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63265722A JP2571108B2 (en) | 1988-10-21 | 1988-10-21 | Method for producing carbon member for fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63265722A JP2571108B2 (en) | 1988-10-21 | 1988-10-21 | Method for producing carbon member for fuel cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH02112161A true JPH02112161A (en) | 1990-04-24 |
| JP2571108B2 JP2571108B2 (en) | 1997-01-16 |
Family
ID=17421098
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP63265722A Expired - Lifetime JP2571108B2 (en) | 1988-10-21 | 1988-10-21 | Method for producing carbon member for fuel cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2571108B2 (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2003234110A (en) * | 2002-02-07 | 2003-08-22 | Mitsubishi Pencil Co Ltd | Separator for fuel cell and its manufacturing method |
| US6794078B1 (en) * | 1999-12-06 | 2004-09-21 | Hitachi Chemical Company, Ltd. | Fuel cell, fuel cell separator, and method of manufacture thereof |
| JP2005310804A (en) * | 2005-07-21 | 2005-11-04 | Hitachi Ltd | Separator for solid polymer fuel cell, solid polymer fuel cell using the same, and power generation system |
| JP5924444B1 (en) * | 2015-10-29 | 2016-05-25 | 富士電機株式会社 | Phosphoric acid fuel cell and manufacturing method of phosphoric acid fuel cell |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS62188173A (en) * | 1986-02-13 | 1987-08-17 | Tokai Carbon Co Ltd | Manufacture of complex electrode for fuel cell |
-
1988
- 1988-10-21 JP JP63265722A patent/JP2571108B2/en not_active Expired - Lifetime
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS62188173A (en) * | 1986-02-13 | 1987-08-17 | Tokai Carbon Co Ltd | Manufacture of complex electrode for fuel cell |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6794078B1 (en) * | 1999-12-06 | 2004-09-21 | Hitachi Chemical Company, Ltd. | Fuel cell, fuel cell separator, and method of manufacture thereof |
| JP2003234110A (en) * | 2002-02-07 | 2003-08-22 | Mitsubishi Pencil Co Ltd | Separator for fuel cell and its manufacturing method |
| JP4587632B2 (en) * | 2002-02-07 | 2010-11-24 | 三菱鉛筆株式会社 | Fuel cell separator and method for producing the same |
| JP2005310804A (en) * | 2005-07-21 | 2005-11-04 | Hitachi Ltd | Separator for solid polymer fuel cell, solid polymer fuel cell using the same, and power generation system |
| JP4647421B2 (en) * | 2005-07-21 | 2011-03-09 | 株式会社日立製作所 | Separator for polymer electrolyte fuel cell, seal member thereof, polymer electrolyte fuel cell using the same, and power generation system |
| JP5924444B1 (en) * | 2015-10-29 | 2016-05-25 | 富士電機株式会社 | Phosphoric acid fuel cell and manufacturing method of phosphoric acid fuel cell |
Also Published As
| Publication number | Publication date |
|---|---|
| JP2571108B2 (en) | 1997-01-16 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| JP4361636B2 (en) | Composite carbonaceous heat insulating material and method for producing the same | |
| JPS62123662A (en) | Electrode substrate for fuel cell | |
| KR20100045501A (en) | High thermal conductivity electrode substrate | |
| WO2002092327A1 (en) | Process for complex shape formation using flexible graphite sheets | |
| JPH02112161A (en) | Manufacture of carbon component for fuel cell | |
| JPS6042213A (en) | Manufacture of carbon sheet | |
| JPH03112871A (en) | Silicon carbide zygote and its junction | |
| JP2008268191A (en) | Plasma facing material and method for manufacturing | |
| JPH03248838A (en) | Heat insulation material | |
| JP2004139885A (en) | Fuel cell separator and manufacturing method of the same | |
| JPS6348766A (en) | Composite electrode substrate having different rib height and its manufacture | |
| JP2607409B2 (en) | Oxidation-resistant treatment of carbon fiber reinforced carbon composites. | |
| JPH01255170A (en) | Manufacture of carbon composite member for fuel battery | |
| JP2524820B2 (en) | Method for producing carbonaceous composite base material for fuel cell | |
| JP2603138B2 (en) | Method for manufacturing carbonaceous composite member for fuel cell | |
| JP2002321987A (en) | Bonded graphite material and its manufacturing method | |
| JPH06190962A (en) | Molded heat insulating material | |
| JP3240062B2 (en) | Method for manufacturing fuel cell separator with end seal | |
| JPS59195514A (en) | Molded impermeable carbon body and its manufacture | |
| JPH02103862A (en) | Manufacture of carbon compound member for fuel cell | |
| JPS62126563A (en) | Manufacture of carbon member for fuel cell | |
| JPS63967A (en) | Manufacture of electrode base plate for fuel cell | |
| JPH04169070A (en) | Manufacture of carbonaceous composite electrode substrate for fuel cell | |
| JP2002343374A (en) | Separator for fuel cell, and manufacturing method of the same | |
| JP2004273449A (en) | Separator for fuel cell and manufacturing method of the same |