JP2002367623A - Fuel cell separator and fuel cell using the same - Google Patents

Fuel cell separator and fuel cell using the same

Info

Publication number
JP2002367623A
JP2002367623A JP2001169849A JP2001169849A JP2002367623A JP 2002367623 A JP2002367623 A JP 2002367623A JP 2001169849 A JP2001169849 A JP 2001169849A JP 2001169849 A JP2001169849 A JP 2001169849A JP 2002367623 A JP2002367623 A JP 2002367623A
Authority
JP
Japan
Prior art keywords
fuel cell
expanded graphite
resin
solid resin
separator
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
JP2001169849A
Other languages
Japanese (ja)
Inventor
Tomonori Seki
智憲 関
Atsushi Fujita
藤田  淳
Akitsugu Tashiro
了嗣 田代
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.)
Showa Denko Materials Co Ltd
Original Assignee
Hitachi Chemical 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 Hitachi Chemical Co Ltd filed Critical Hitachi Chemical Co Ltd
Priority to JP2001169849A priority Critical patent/JP2002367623A/en
Publication of JP2002367623A publication Critical patent/JP2002367623A/en
Pending legal-status Critical Current

Links

Classifications

    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30Hydrogen technology
    • Y02E60/50Fuel cells

Landscapes

  • Fuel Cell (AREA)

Abstract

PROBLEM TO BE SOLVED: To provide a fuel cell separator with good molding property, without any problem regarding gas impermeability, electric property, liquid swelling property, mechanical strength or the like, and to provide a fuel cell with high efficiency having the above separator. SOLUTION: For the fuel cell separator having a rib part 1 and a flat part 3, the flat part 3 is formed by a layer containing the mixture of swelling graphite powder and a solid resin a, and a layer having a material with insulation property containing solid resin b, here, the melting point of the solid resin a mixed with the swelling graphite powder and the solid resin b contained in the material with insulating property are approximately same with each other.

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、燃料電池の燃料ガ
スと酸化剤ガス(空気又は酸素)を分離するリブ付で、
かつガスと水を供給するための穴部(貫通口)が設けら
れた燃料電池用セパレータ及び燃料電池用セパレータを
用いた燃料電池に関する。
The present invention relates to a fuel cell having a rib for separating fuel gas and oxidizing gas (air or oxygen),
The present invention relates to a fuel cell separator provided with a hole (through hole) for supplying gas and water, and a fuel cell using the fuel cell separator.

【0002】[0002]

【従来の技術】燃料電池は近年、化石燃料消費拡大によ
る地球温暖化防止策、省エネルギー対策等の観点から非
常に注目され、国、大学の研究機関、大手企業等でも研
究開発が盛んに行われ一部商品化されている。
2. Description of the Related Art In recent years, fuel cells have attracted a great deal of attention from the perspective of measures to prevent global warming and energy savings due to the expansion of fossil fuel consumption, and research and development have been actively conducted at national and university research institutions and major companies. Some have been commercialized.

【0003】燃料電池(固体高分子型)は大きく分け
て、イオン交換膜、白金触媒、セパレータから構成され
る。このうちセパレータの働きは、エネルギーを発生さ
せる水素及び酸素の定量的な供給と発生する水の速やか
な排出にあり、電池特性を左右する重要な部材である。
A fuel cell (solid polymer type) is roughly composed of an ion exchange membrane, a platinum catalyst, and a separator. Among them, the function of the separator is to quantitatively supply hydrogen and oxygen for generating energy and to quickly discharge the generated water, which is an important member that affects battery characteristics.

【0004】また、セパレータは、一つの電池(自動車
用)に数百枚使用されるためコンパクト化が急務であ
り、現在セパレータ製造各社ともリブ部デザインの改
良、薄板化及び寸法バランスの改良、重量及び体積低減
対策、コスト低減等セパレータの最適化に凌ぎを削って
いる。
Since several hundred separators are used for one battery (for automobiles), it is urgent to reduce the size of the separators. At present, all separator manufacturers have improved the design of ribs, reduced the thickness and dimensional balance, and improved the weight. In addition, the company has been struggling to optimize separators, such as measures for volume reduction and cost reduction.

【0005】従来型のセパレータは、特開昭60−65
781号公報、特開昭60−12672号公報等に示さ
れるように、黒鉛板を用いリブ部の形状などをプログラ
ムした高精度の切削機で時間をかけ慎重に加工して作製
する方法、りん片状の天然黒鉛を酸処理し加熱処理して
得られる膨張黒鉛を圧縮成形してシート状にし、このシ
ートに液状樹脂を含浸して作製する方法等で製造してい
た。
A conventional separator is disclosed in Japanese Patent Application Laid-Open No. 60-65.
No. 781, Japanese Patent Application Laid-Open No. 60-12672, etc., a method in which a graphite plate is used to carefully and slowly process with a high-precision cutting machine in which the shape of a rib portion and the like are programmed. It has been produced by a method in which flaky natural graphite is subjected to an acid treatment and a heat treatment, and then expanded graphite obtained by compression molding is formed into a sheet, and this sheet is impregnated with a liquid resin.

【0006】しかしながら、上記の方法で得られるセパ
レータは、前者の場合、リブ切削工程及びガスの不浸透
化に時間を要するため、セパレータ一枚当たりの価格が
非常に高くなり、また後者の場合、リブ寸法に限界があ
り、成形時に膨れが発生し易いという問題を有してい
た。
[0006] However, the separator obtained by the above method requires a long time in the rib cutting step and gas impermeability in the former case, so that the price per separator becomes very high. There is a problem in that the rib dimensions are limited and swelling is likely to occur during molding.

【0007】上記の問題に対して、本発明者らは、安価
で正確なリブを形成でき、かつ燃料電池の特性を損なわ
ないセパレータとして、膨張黒鉛シート粉砕粉と特殊樹
脂を併用した新しい成形材料を提案した。しかし、上記
材料で成形したセパレータはリブ部と平坦部との密度が
異なり、平坦部の密度が低くなる傾向があり、ガス不浸
透性と機械強度に問題点がある。
[0007] In order to solve the above-mentioned problems, the present inventors have developed a new molding material using a combination of pulverized powder of expanded graphite sheet and a special resin as a separator capable of forming accurate ribs at low cost and not impairing the characteristics of the fuel cell. Suggested. However, the separator molded from the above-described material has different densities between the rib portion and the flat portion, and the flat portion tends to have a low density, and has problems in gas impermeability and mechanical strength.

【0008】さらに、上記の問題の改善策として、成形
時において平坦部に樹脂含有ガラス繊維を複合化させた
成形体を提案したが、成形材料(混合物)中の粉末状樹
脂の融点及び流れ性とガラス繊維中に含まれる粉末状樹
脂の融点及び流れ性が異なるため、成形時にガラス繊維
樹脂がリブ形成部に流れ込み、そのまま硬化するなどの
不具合を生じさせた。
Further, as a measure for solving the above-mentioned problem, a molded article in which a resin-containing glass fiber is compounded in a flat portion at the time of molding has been proposed. However, the melting point and flowability of a powdery resin in a molding material (mixture) have been proposed. Since the melting point and the flowability of the powdery resin contained in the glass fiber and the glass fiber are different, the glass fiber resin flows into the rib-forming portion during molding and causes problems such as curing as it is.

【0009】[0009]

【発明が解決しようとする課題】請求項1〜7記載の発
明は、燃料電池用セパレータにおいて、ガス不浸透性、
電気特性、液膨潤性、機械強度等に問題がなく、かつ成
形性の良好な、燃料電池用セパレータを提供するもので
ある。また、請求項8及び9記載の発明は、ガス不浸透
性、電気特性、液膨潤性、機械強度等に問題がなく、か
つ成形性の良好な、燃料電池用セパレータを有する、高
性能な燃料電池を提供するものである。
The invention according to claims 1 to 7 is directed to a fuel cell separator which is gas-impermeable,
An object of the present invention is to provide a fuel cell separator which has no problem in electric characteristics, liquid swelling property, mechanical strength and the like and has good moldability. The invention according to claims 8 and 9 provides a high-performance fuel having a fuel cell separator, which has no problem in gas impermeability, electric characteristics, liquid swellability, mechanical strength, etc., and has good moldability. A battery is provided.

【0010】[0010]

【課題を解決するための手段】本発明は、リブ部及び平
坦部を有する燃料電池用セパレータにおいて、平坦部が
膨張黒鉛粉と固形樹脂aの混合物を含む層及び固形樹脂
bを含有した絶縁性を有する材料を含む層からなり、か
つ膨張黒鉛粉と混合する固形樹脂aの融点と絶縁性を有
する材料に含有する固形樹脂bの融点がほぼ同等である
燃料電池用セパレータに関する。また、本発明は、リブ
部が、膨張黒鉛粉と固形樹脂aの混合物を含む層からな
る燃料電池用セパレータに関する。また、本発明は、膨
張黒鉛粉が、膨張黒鉛シート粉砕粉である燃料電池用セ
パレータに関する。また、本発明は、膨張黒鉛粉と混合
する固形樹脂aに比較し、絶縁性を有する材料に含有す
る固形樹脂bのゲル化時間が短い燃料電池用セパレータ
に関する。
According to the present invention, there is provided a fuel cell separator having a rib portion and a flat portion, wherein the flat portion has a layer containing a mixture of expanded graphite powder and a solid resin a and an insulating material containing a solid resin b. The present invention relates to a separator for a fuel cell, comprising a layer containing a material having the following characteristics, wherein the melting point of the solid resin a mixed with the expanded graphite powder is substantially equal to the melting point of the solid resin b contained in the insulating material. Further, the present invention relates to a fuel cell separator in which a rib portion is formed of a layer containing a mixture of expanded graphite powder and solid resin a. Further, the present invention relates to a fuel cell separator in which the expanded graphite powder is a pulverized powder of an expanded graphite sheet. The present invention also relates to a fuel cell separator in which the solid resin b contained in the insulating material has a shorter gelation time than the solid resin a mixed with the expanded graphite powder.

【0011】また、本発明は、セパレータが、リブ部及
び平坦部以外に穴部を有する燃料電池用セパレータに関
する。また、本発明は、絶縁性を有する材料に含有する
固形樹脂bが、架橋点であるエポキシ基を1つ以上有す
るエポキシ樹脂である燃料電池用セパレータに関する。
また、本発明は、絶縁性を有する材料がプリプレグであ
る燃料電池用セパレータに関する。また、本発明は、前
記のセパレータを有してなる燃料電池に関する。さら
に、本発明は、固体高分子型である前記の燃料電池に関
する。
Further, the present invention relates to a fuel cell separator having a hole in addition to a rib and a flat portion. The present invention also relates to a fuel cell separator in which the solid resin b contained in the insulating material is an epoxy resin having one or more epoxy groups that are crosslinking points.
Further, the present invention relates to a fuel cell separator in which the insulating material is a prepreg. The present invention also relates to a fuel cell having the above-mentioned separator. Furthermore, the present invention relates to the above fuel cell, which is a solid polymer type.

【0012】[0012]

【発明の実施の形態】本発明における燃料電池用セパレ
ータにおいて、リブ部は、導電性又は通電性を有し、セ
パレータを電解質膜、燃料極及び空気極を介して重ねた
ときにガスの流路を形成するものである。また、平坦部
は、セパレータの把持部を形成し、上記の流路をガスが
通過するときにガス漏れしないように構成される。さら
に、リブ部は、セパレータを重ねたときに形成された流
路をガスが通過するときにガス漏れしないように構成さ
れる。なお、平坦部は、セパレータを重ねたときに全体
を固定するための把持部となることが好ましい。
BEST MODE FOR CARRYING OUT THE INVENTION In a fuel cell separator according to the present invention, a rib portion has conductivity or electrical conductivity, and a gas flow path is formed when the separator is stacked via an electrolyte membrane, a fuel electrode and an air electrode. Is formed. Further, the flat portion forms a grip portion of the separator, and is configured so that gas does not leak when the gas passes through the flow path. Further, the rib portion is configured such that gas does not leak when gas passes through a flow path formed when the separators are stacked. In addition, it is preferable that the flat part be a grip part for fixing the whole when the separator is stacked.

【0013】また、本発明における燃料電池用セパレー
タは、リブ部及び平坦部以外に穴部を有していてもよ
く、特に平坦部内に穴部を有していることが好ましい。
穴部は、セパレータを多数重ねたときに、重ね方向に長
い穴を形成するように構成され、水素ガス、酸素ガス及
び冷却水を通すための穴が形成されるように構成され
る。それぞれの穴は、セパレータのリブ部によって形成
される水素ガス流路、酸素ガス流路及び冷却水流路と連
結されるように構成される。なお、平坦部には、セパレ
ータを重ねたときに固定用のボルトを通るための穴を有
していてもよい。
Further, the fuel cell separator of the present invention may have a hole in addition to the rib and the flat portion, and particularly preferably has a hole in the flat portion.
The hole is configured to form a long hole in the stacking direction when many separators are stacked, and to form a hole for passing hydrogen gas, oxygen gas, and cooling water. Each hole is configured to be connected to a hydrogen gas flow path, an oxygen gas flow path, and a cooling water flow path formed by the rib portion of the separator. Note that the flat portion may have a hole for passing a fixing bolt when the separator is stacked.

【0014】リブ部と平坦部が、それぞれ膨張黒鉛粉と
固形樹脂aの混合物を含む層を有し、これらの層が連続
している層であることが好ましい。これにより、セパレ
ータを得るための成形時の成形性が良好であり、セパレ
ータに軽量性を付与し、また、セパレータに高靭性、低
弾性という好ましい特性を付与する。
It is preferable that each of the rib portion and the flat portion has a layer containing a mixture of the expanded graphite powder and the solid resin a, and these layers are continuous layers. Thereby, the moldability at the time of molding for obtaining the separator is good, the separator is given light weight, and the separator is given favorable characteristics such as high toughness and low elasticity.

【0015】また、本発明においては平坦部に、固形樹
脂bを含有した絶縁性を含む層として補強層が積層され
るが、この補強層は、平坦部の膨張黒鉛粉と固形樹脂a
の混合物を含む層の密度を高める役目又は平坦部の強度
を改善する役目を担うものである。
In the present invention, a reinforcing layer is laminated on the flat portion as an insulating layer containing the solid resin b, and the reinforcing layer is formed of the expanded graphite powder of the flat portion and the solid resin a.
And a role of increasing the density of the layer containing the mixture of the above or improving the strength of the flat portion.

【0016】本発明におけるセパレータの素材は、膨張
黒鉛粉及び固形樹脂aを原料とし、これを熱圧成形して
得られる。このうち膨張黒鉛粉は、膨張黒鉛を造粒加工
して得られる膨張黒鉛造粒粉が好ましい。膨張黒鉛造粒
粉としては、膨張黒鉛シートの粉砕粉が特に好ましい。
The raw material of the separator in the present invention is obtained by subjecting expanded graphite powder and solid resin a to raw materials and subjecting them to hot pressing. Among these, the expanded graphite powder is preferably an expanded graphite granulated powder obtained by granulating expanded graphite. As the expanded graphite granulated powder, a pulverized powder of an expanded graphite sheet is particularly preferable.

【0017】膨張黒鉛は、原料黒鉛を、酸性物質及び酸
化剤を含む溶液中に浸漬して黒鉛層間化合物を生成させ
る工程及び前記黒鉛層間化合物を加熱して黒鉛結晶のC
軸方向を膨張させて膨張黒鉛とする工程により製造する
ことができる。膨張した黒鉛が虫状形となり方向性のな
い複雑に絡み合った形態となる。
The expanded graphite is prepared by immersing raw graphite in a solution containing an acidic substance and an oxidizing agent to form a graphite intercalation compound, and heating the graphite intercalation compound to form a graphite crystal.
It can be manufactured by a process of expanding in the axial direction to obtain expanded graphite. The expanded graphite becomes a worm-like shape, and has a complicated entangled shape with no directionality.

【0018】膨張黒鉛の倍率は、セパレータの強度とシ
ール性を確保するため高い方が好ましく、特に制限はな
いが150倍以上であることが好ましく、150〜30
0倍であることがさらに好ましい。この膨張黒鉛を粉砕
することにより膨張黒鉛粉とすることができるが、粉砕
の前に、得られた膨張黒鉛に圧力を加えシート状に圧縮
成形して膨張黒鉛シートとすることが好ましい。さら
に、得られた膨張黒鉛粉には、必要に応じて、その粉砕
粉に含まれる酸性根を低減させるための処理(高温処理
など)を施す。
The magnification of the expanded graphite is preferably high in order to ensure the strength and sealing property of the separator, and is not particularly limited, but is preferably 150 times or more, and 150 to 30 times.
More preferably, it is 0 times. The expanded graphite can be made into an expanded graphite powder by pulverizing the expanded graphite. Before the pulverization, it is preferable to apply pressure to the obtained expanded graphite and compression-mold it into a sheet to obtain an expanded graphite sheet. Further, the obtained expanded graphite powder is subjected to a treatment (such as a high-temperature treatment) for reducing acidic roots contained in the pulverized powder, if necessary.

【0019】前記の原料黒鉛としては特に制限はない
が、天然黒鉛、キッシュ黒鉛、熱分解黒鉛等の高度に結
晶が発達した黒鉛が好ましいものとして挙げらる。得ら
れる特性と経済性のバランスを考慮すると天然黒鉛が好
ましい。用いる天然黒鉛としては、特に制限はなく、F
48C(日本黒鉛(株)製、商品名)、H−50(中越黒
鉛(株)製、商品名)等の市販品を用いることができる。
これらは、鱗片状の粉末の形態で使用することが好まし
い。
The raw material graphite is not particularly limited, but is preferably graphite having a high degree of crystal development, such as natural graphite, quiche graphite and pyrolytic graphite. Natural graphite is preferred in consideration of the balance between the obtained characteristics and economy. The natural graphite to be used is not particularly limited.
Commercial products such as 48C (trade name, manufactured by Nippon Graphite Co., Ltd.) and H-50 (trade name, manufactured by Chuetsu Graphite Co., Ltd.) can be used.
These are preferably used in the form of scaly powder.

【0020】原料黒鉛の処理に用いられる酸性物質は、
一般に硫酸などの黒鉛の層間に進入して十分な膨脹能力
を有する酸性根(陰イオン)を発生することができるも
のが使用される。酸性物質の使用量については特に制限
はなく、目的とする膨張倍率で決定され、例えば、黒鉛
100重量部に対して100〜1000重量部使用する
ことが好ましい。
The acidic substances used in the processing of the raw graphite are as follows:
Generally, a material capable of penetrating between layers of graphite such as sulfuric acid to generate an acidic root (anion) having a sufficient expansion ability is used. The amount of the acidic substance to be used is not particularly limited and is determined according to the desired expansion ratio. For example, it is preferable to use 100 to 1000 parts by weight based on 100 parts by weight of graphite.

【0021】また、酸性物質と共に用いられる酸化剤と
しては、過酸化水素、過塩素酸カリウム、過マンガン酸
カリウム、重クロム酸カリウム等の過酸化物や硝酸、塩
酸等の酸化作用のある酸を用いることができ、良好な膨
張黒鉛を得易いという観点から過酸化水素が特に好まし
い。酸化剤として過酸化水素を用いる場合、水溶液とし
て用いることが好ましく、このとき、過酸化水素の濃度
については特に制限はないが、20重量%〜40重量%
が好ましい。その使用量についても特に制限はないが、
黒鉛100重量部に対して過酸化水素水として5重量部
〜60重量部配合することが好ましい。
The oxidizing agent used together with the acidic substance includes peroxides such as hydrogen peroxide, potassium perchlorate, potassium permanganate and potassium dichromate, and acids having an oxidizing action such as nitric acid and hydrochloric acid. Hydrogen peroxide is particularly preferred from the viewpoint that it can be used and good expanded graphite is easily obtained. When hydrogen peroxide is used as the oxidizing agent, it is preferably used as an aqueous solution. At this time, the concentration of hydrogen peroxide is not particularly limited, but is preferably 20% by weight to 40% by weight.
Is preferred. There is no particular limitation on the amount of its use,
It is preferable to mix 5 parts by weight to 60 parts by weight of hydrogen peroxide solution with respect to 100 parts by weight of graphite.

【0022】酸性物質及び酸化剤は、水溶液の形態で使
用することが好ましい。酸性物質としての硫酸は、適宜
の濃度で使用されるが、95重量%以上の濃度のものが
好ましく、濃硫酸を使用することが特に好ましい。
The acidic substance and the oxidizing agent are preferably used in the form of an aqueous solution. Sulfuric acid as an acidic substance is used at an appropriate concentration, but preferably has a concentration of 95% by weight or more, and it is particularly preferable to use concentrated sulfuric acid.

【0023】前記において、膨張黒鉛シートの製法につ
いても特に制限はないが、一般的には上記で得た膨張黒
鉛を、プレス、ロール等で圧力を加えてシート化するこ
とが好ましい。膨張黒鉛をシート化したときのシートの
厚さ及び密度については特に制限はないが、厚さが0.
5mm〜1.5mmの範囲及び密度が200kg/m〜1
200kg/mの範囲のものが好ましい。密度の大き
さは、加圧量、ロールギャップ等の調整により、調整す
ることができる。また、膨張黒鉛シートの粉砕は、粗粉
砕及び微粉砕により行うことが好ましく、この後必要に
応じて分級を行う。
In the above, there is no particular limitation on the method for producing the expanded graphite sheet, but it is generally preferable to apply pressure to the expanded graphite obtained above with a press, roll, or the like to form a sheet. There is no particular limitation on the thickness and density of the sheet when the expanded graphite is formed into a sheet.
A range of 5 mm to 1.5 mm and a density of 200 kg / m 3 to 1
Those having a range of 200 kg / m 3 are preferable. The magnitude of the density can be adjusted by adjusting the amount of pressure, the roll gap, and the like. Further, the pulverization of the expanded graphite sheet is preferably performed by coarse pulverization and fine pulverization, and thereafter, classification is performed as necessary.

【0024】本発明において、原料としての膨張黒鉛粉
の密度については特に制限はないが、100kg/m
〜400kg/mの範囲が好ましい。膨張黒鉛粉の密
度が小さすぎると、樹脂との均一混合性が低下し、得ら
れる成形体(燃料電池用セパレータ)のシール性が低下
する傾向があり、膨張黒鉛粉の密度が大きすぎると目的
とする成形体(燃料電池用セパレータ)の機械的強度及
び導電性の向上効果が低下する傾向がある。
In the present invention, the density of the expanded graphite powder as a raw material is not particularly limited, but is 100 kg / m 3.
It is preferably in the range of 400400 kg / m 3 . If the density of the expanded graphite powder is too low, the uniform mixing property with the resin tends to decrease, and the sealing property of the obtained molded article (fuel cell separator) tends to decrease. There is a tendency that the effect of improving the mechanical strength and conductivity of the molded article (separator for fuel cells) to be used is reduced.

【0025】膨張黒鉛粉の粒度については特に制限はな
いが、樹脂との混合性及び成形性を考慮すると、数平均
粒径で50μm〜300μmの範囲であることが好まし
い。ここで数平均粒径が50μm未満であると膨張黒鉛
粉の絡み合いの効果が少なくなり、セパレータの強度低
下が起こり易くなる傾向がある。一方、300μmを超
えると幅の狭いリブへの膨張黒鉛の流れ性が悪化し、平
板が薄くリブの高さが高いセパレータの成形が困難とな
る傾向がある。
The particle size of the expanded graphite powder is not particularly limited, but is preferably in the range of 50 μm to 300 μm in terms of number average particle size in consideration of mixability with resin and moldability. Here, when the number average particle size is less than 50 μm, the effect of entanglement of the expanded graphite powder is reduced, and the strength of the separator tends to easily decrease. On the other hand, when the thickness exceeds 300 μm, the flowability of the expanded graphite to the narrow ribs deteriorates, and it tends to be difficult to form a separator having a thin flat plate and a high rib height.

【0026】また、本発明において、膨張黒鉛粉と混合
する固形樹脂aは、熱硬化性樹脂であれば特に制限はな
いが、コスト及び特性の点でエポキシ樹脂、フェノール
樹脂、メラミン樹脂等が好ましく、特に優れた特性バラ
ンスを示し、経済性、作業性等の点でフェノール樹脂が
好ましい。これらの固形樹脂aの使用形態としては、粉
末状、粒状等が好ましい。また、これらの固形樹脂a
は、必要に応じて、硬化剤、硬化促進剤等と併用して使
用される。硬化剤、硬化促進剤等の使用形態についても
粉末状、粒状等が好ましい。
In the present invention, the solid resin a to be mixed with the expanded graphite powder is not particularly limited as long as it is a thermosetting resin. However, epoxy resin, phenol resin, melamine resin and the like are preferable in terms of cost and characteristics. In particular, phenol resins are preferable because they exhibit an excellent balance of properties and are economical and workable. The form of use of these solid resins a is preferably powdery, granular, or the like. In addition, these solid resins a
Is used, if necessary, in combination with a curing agent, a curing accelerator and the like. The form of use of the curing agent, the curing accelerator, etc. is also preferably in the form of powder, granules, or the like.

【0027】フェノール樹脂としては、粉体特性として
粒径が均一であり、また、ブロッキング(粉の凝集)が
少ないこと、硬化反応時に発生ガスが少なく成形が容易
であること、熱処理が短時間で終了する等の特長を備え
たフェノール樹脂が好ましく、中でも開環重合により重
合するジヒドロベンゾオキサジン環を含むフェノール樹
脂〔一般式(A)及び(B)に示す化学構造単位を有す
る〕を用いることが好ましい。
The phenolic resin has a uniform particle size as a powder property, a small amount of blocking (coagulation of powder), a small amount of gas generated during a curing reaction, easy molding, and a short heat treatment. A phenol resin having characteristics such as termination is preferred, and among them, a phenol resin containing a dihydrobenzoxazine ring polymerized by ring-opening polymerization [having a chemical structural unit represented by general formulas (A) and (B)] is preferably used. preferable.

【0028】[0028]

【化1】 (式中、芳香環に結合する水素はヒドロキシル基のオル
ト位の1つを除き、炭素数1〜3のアルキル基、シクロ
ヘキシル基、フェニル基又は炭素数1〜3のアルキル基
若しくはアルコキシル基で置換されたフェニル基等の炭
化水素基で置換されていてもよい)。
Embedded image (Wherein the hydrogen bonded to the aromatic ring is substituted by an alkyl group having 1 to 3 carbon atoms, a cyclohexyl group, a phenyl group or an alkyl group or an alkoxyl group having 1 to 3 carbon atoms, except for one of the ortho positions of the hydroxyl group. May be substituted by a substituted phenyl group or other hydrocarbon group).

【0029】[0029]

【化2】 (式中、Rは、炭素数1〜3のアルキル基、シクロヘ
キシル基、フェニル基又は炭素数1〜3のアルキル基若
しくはアルコキシル基で置換されたフェニル基等の炭化
水素基であり、芳香環に結合する水素は、同様の炭化水
素基で置換されていてもよい)。
Embedded image (In the formula, R 1 is a hydrocarbon group such as an alkyl group, a cyclohexyl group, a phenyl group substituted with a phenyl group or an alkyl or alkoxyl group having 1 to 3 carbon atoms of 1 to 3 carbon atoms, an aromatic ring May be substituted with a similar hydrocarbon group).

【0030】固形樹脂aとして粉末状樹脂を用いる場
合、その粒度分布に特に制限はないが、膨張黒鉛粉との
乾式での混合性を考慮すると、数平均粒径で1μm〜1
00μmの範囲が好ましく、5μm〜50μmの範囲が
さらに好ましい。数平均粒径が1μm未満の場合、粒子
同士が凝集(ブロッキング)を起こし、作業性が悪いば
かりでなく膨張黒鉛粉との均一混合が望めなくなる傾向
があり、一方、100μmを超える場合、前記と同様に
膨張黒鉛粉との均一混合が難しくなり、得られるセパレ
ータの密度が大きくばらつく傾向がある。
When a powdery resin is used as the solid resin a, its particle size distribution is not particularly limited. However, considering the dry mixability with the expanded graphite powder, the number average particle diameter is 1 μm to 1 μm.
A range of 00 μm is preferable, and a range of 5 μm to 50 μm is more preferable. When the number average particle size is less than 1 μm, the particles aggregate (block), and not only workability is poor, but also there is a tendency that uniform mixing with the expanded graphite powder cannot be expected. Similarly, uniform mixing with the expanded graphite powder becomes difficult, and the density of the obtained separator tends to vary greatly.

【0031】本発明で使用する膨張黒鉛粉と固形樹脂a
との混合割合は、目標とする最終成形体である燃料電池
用セパレータの諸特性の値を考慮して決定されるが、通
常混合比率で膨張黒鉛粉/樹脂=95/5〜30/70
(重量比)の範囲が好ましく、90/10〜50/50
(重量比)の範囲がより好ましく、80/20〜60/
40(重量比)の範囲がさらに好ましい。ここで膨張黒
鉛粉と固形樹脂aとの混合比率が95/5を超える場
合、機械強度が急激に低下する傾向があり、一方、30
/70未満の場合、導電性物質である膨張黒鉛粉の添加
量が少なく、電気特性が悪化する傾向がある。
The expanded graphite powder used in the present invention and the solid resin a
Is determined in consideration of the values of various characteristics of the fuel cell separator, which is the target final molded product, and is usually expanded graphite powder / resin = 95/5 to 30/70 at the mixing ratio.
(Weight ratio) is preferable, and 90/10 to 50/50.
(Weight ratio) is more preferable, and 80/20 to 60 /
A range of 40 (weight ratio) is more preferable. Here, when the mixing ratio of the expanded graphite powder and the solid resin a exceeds 95/5, the mechanical strength tends to sharply decrease, while 30
If it is less than / 70, the amount of the expanded graphite powder that is a conductive substance is small, and the electrical characteristics tend to deteriorate.

【0032】膨張黒鉛粉と固形樹脂aの混合方法に特に
制限はなく、膨張黒鉛粉の微粉化を防止する点で混合時
の膨張黒鉛粉に大きな剪断力が加わらないシエイカー、
Vブレンダー等を使用した乾式混合法によることが好ま
しい。混合時に膨張黒鉛粉が微粉化した場合、得られる
燃料電池用セパレータの機械強度が急激に低下する傾向
がある。
There is no particular limitation on the method of mixing the expanded graphite powder and the solid resin a, and a shaker in which a large shearing force is not applied to the expanded graphite powder at the time of mixing in order to prevent the expansion graphite powder from being finely divided.
It is preferable to use a dry mixing method using a V blender or the like. When the expanded graphite powder is pulverized during mixing, the mechanical strength of the resulting fuel cell separator tends to sharply decrease.

【0033】また、上記混合物(混合粉)は、直接成形
材料粉として使用できるが、本発明においては、さらな
る混合性の向上と成形時の作業性を向上させるために、
混合粉を加圧成形しシート状にしたもの(以下、「成形
用シート」という)を使用する。成形用シートの製造法
については特に制限はないが、例えば混合物タンク、材
料を一定厚さにするゲート調整機、一定幅に仕上げるス
リッター、前記加工材料を移送する移送装置、シート化
する圧延ロール等から構成される成形用シートの製造装
置等を使用することができる。平坦部に穴部を有する場
合、成形用シートに穴部が形成されているようにすると
好ましい。
The above mixture (mixed powder) can be used directly as a molding material powder. In the present invention, in order to further improve the mixing property and the workability during molding,
A sheet obtained by press-molding the mixed powder to form a sheet (hereinafter, referred to as a “sheet for molding”) is used. Although there is no particular limitation on the method of manufacturing the forming sheet, for example, a mixture tank, a gate adjuster for making the material to a constant thickness, a slitter for finishing to a constant width, a transfer device for transferring the processing material, a rolling roll for forming a sheet, and the like And an apparatus for manufacturing a sheet for molding composed of the following. When the flat portion has a hole, it is preferable that the hole is formed in the molding sheet.

【0034】成形用シートは、その強度を向上させるた
めに成形用シートに含まれる樹脂の硬化反応を部分的に
進めるか、部分的に(完全にではなく)熱溶融させてか
らセパレータの製造に供することができる。硬化反応又
は熱溶融させる方法に制限はないが、例えば、得られた
成形用シートを加熱する方法、さらに具体的には前記の
圧延ロールを加熱装置が付属されたものとし、この圧延
ロールを通すときに加熱する方法、得られた成形用シー
トを加熱オーブンに通す方法等がある。
In order to improve the strength of the molding sheet, the curing reaction of the resin contained in the molding sheet is partially advanced or partially (not completely) heat-fused before the production of the separator. Can be offered. Although there is no limitation on the method of curing reaction or heat melting, for example, a method of heating the obtained forming sheet, more specifically, the above-mentioned rolling roll is provided with a heating device, and this rolling roll is passed through the rolling roll. Sometimes, there is a method of heating, a method of passing the obtained molding sheet through a heating oven, and the like.

【0035】一方、絶縁性を有する材料に含有する固形
樹脂bは、コスト、作業性、得られるセパレータの特性
等の点で、例えばエポキシ樹脂が好ましい。上記のエポ
キシ樹脂は、成形性、得られるセパレータの外観、形
状、特性等の点で融点が、膨張黒鉛粉と混合する固形樹
脂a、詳しくは成形体を構成する膨張黒鉛粉との混合物
に含有する固形樹脂aとほぼ同等のものを用いることが
必要とされる。なお、上記のほぼ同等とは、膨張黒鉛粉
と混合する固形樹脂aの融点と絶縁性を有する材料に含
有する固形樹脂bの融点の差が、±20℃程度まで、好
ましくは±10℃程度までのものを指す。
On the other hand, the solid resin b contained in the insulating material is preferably, for example, an epoxy resin in terms of cost, workability, characteristics of the obtained separator, and the like. The above epoxy resin has a melting point in terms of moldability, appearance, shape, properties, etc. of the obtained separator, and is contained in a solid resin a mixed with the expanded graphite powder, more specifically, a mixture with the expanded graphite powder constituting the molded body. It is necessary to use a material substantially equivalent to the solid resin a. In addition, the above substantially equivalent means that the difference between the melting point of the solid resin a mixed with the expanded graphite powder and the melting point of the solid resin b contained in the insulating material is up to about ± 20 ° C., preferably about ± 10 ° C. Up to

【0036】また、上記のエポキシ樹脂は、耐熱性、機
械強度等の点で架橋点であるエポキシ基を1つ以上有す
るエポキシ樹脂が好ましい。さらに、上記のエポキシ樹
脂のゲル化時間は、膨張黒鉛粉と混合する固形樹脂に比
較して15秒、好ましくは5秒短いことが望ましい。エ
ポキシ樹脂のゲル化時間が膨張黒鉛粉と混合する固形樹
脂aに比較して長い場合、成形時に混合物が形成すべき
リブなどに流れ込んで硬化し、不良品となる傾向があ
る。
The epoxy resin is preferably an epoxy resin having at least one epoxy group which is a crosslinking point in terms of heat resistance, mechanical strength and the like. Further, the gel time of the epoxy resin is desirably 15 seconds, preferably 5 seconds shorter than the solid resin mixed with the expanded graphite powder. If the gelation time of the epoxy resin is longer than the solid resin a mixed with the expanded graphite powder, the mixture tends to flow into ribs and the like to be formed at the time of molding and harden, resulting in defective products.

【0037】絶縁性を有する材料に含有する固形樹脂b
においても、必要において硬化剤、硬化促進剤等と併用
して使用される。上記のエポキシ樹脂の種類、硬化剤、
硬化促進剤等の種類及びこれらの配合量は、成形体を構
成する混合物に使用される固形樹脂aの分子量、融点、
流れ性、硬化時間等を参考に決定される。上記の性状、
特長及びコスト、保存性等を考慮した場合、エポキシ樹
脂としては、ビスフェノールA/エピクロルヒドリン型
のエポキシ樹脂が好ましく、数平均分子量で900以上
のエポキシ樹脂が特に好ましい。
Solid resin b contained in insulating material b
Is used in combination with a curing agent, a curing accelerator, and the like, if necessary. The type of epoxy resin, curing agent,
The kind of the curing accelerator and the like and the compounding amount thereof are determined by the molecular weight, melting point,
It is determined with reference to flowability, curing time and the like. The above properties,
In consideration of features, cost, storage stability, etc., the epoxy resin is preferably a bisphenol A / epichlorohydrin type epoxy resin, and particularly preferably an epoxy resin having a number average molecular weight of 900 or more.

【0038】上記のエポキシ樹脂と併用して使用される
硬化剤としては、保存性を考慮して潜在性のジシアンジ
アミドが好ましく、硬化促進剤としては、ベンジルジメ
チルアミン(BDMA)が使用される。配合割合は、エ
ポキシ樹脂/ジシアンジアミド/ ベンジルジメチルア
ミン=100/2〜8/1〜0.4(重量比)の範囲が
好ましい。
As a curing agent used in combination with the above epoxy resin, latent dicyandiamide is preferable in consideration of storage stability, and benzyldimethylamine (BDMA) is used as a curing accelerator. The mixing ratio is preferably in the range of epoxy resin / dicyandiamide / benzyldimethylamine = 100/2 to 8/1 to 0.4 (weight ratio).

【0039】また、上記のエポキシ樹脂と併用して使用
される絶縁性を有する材料としては、ガラス布(ガラス
織布又はガラス不織布)が好ましい。このガラス布を平
坦部の補強層として用いる場合は、ガラス布に上記のエ
ポキシ樹脂を含浸し、乾燥させて得られるプリプレグ
(樹脂の硬化度はBステージ状態)を用いることが好ま
しい。
As the insulating material used in combination with the epoxy resin, a glass cloth (glass woven cloth or glass nonwoven cloth) is preferable. When this glass cloth is used as a reinforcing layer for a flat portion, it is preferable to use a prepreg obtained by impregnating the above-mentioned epoxy resin into a glass cloth and drying the resin (the degree of curing of the resin is in a B-stage state).

【0040】上記ガラス布のガラス組成については特に
制限はないがCガラスやEガラスを用いることができ
る。ガラスの繊維径については、得られる樹脂含有ガラ
ス繊維(固形樹脂bを含有した絶縁性を有する材料)の
機械強度及び樹脂の含浸性を考慮すると、3μm〜18
μmの範囲が好ましい。ガラス布又はその原料のガラス
繊維は、樹脂との密着性(シール性)を確保するためシ
ラン系の表面処理を行ったものが好ましく、板厚を0.
15mm〜0.33mmとすることが好ましく、このう
ちガラス織布は平織りを主として用いることが好まし
い。
The glass composition of the glass cloth is not particularly limited, but C glass or E glass can be used. The fiber diameter of the glass is 3 μm to 18 μm in consideration of the mechanical strength of the obtained resin-containing glass fiber (insulating material containing the solid resin b) and the resin impregnation.
The range of μm is preferred. The glass cloth or the glass fiber as a raw material thereof is preferably subjected to a silane-based surface treatment in order to secure adhesion (sealability) with the resin, and the thickness of the glass cloth is set to 0.1.
The thickness is preferably from 15 mm to 0.33 mm, and among them, it is preferable to mainly use a plain weave as the glass woven fabric.

【0041】上記のプリプレグにおいて、樹脂の含浸
は、例えば、繊維織布又は繊維不織布に固形樹脂、硬化
剤、硬化促進剤等を有樹溶媒に均一に溶解した樹脂ワニ
スを塗工することにより行うことができる。繊維織布又
は繊維不織布に塗工する樹脂量(固形分)は、ガラス布
に対して30重量部〜60重量部が好ましく、40重量
部〜50重量部がさらに好ましい。樹脂量が30重量部
未満ではガス不透過性のレベルが低下する傾向があり、
60重量部を超えると繊維比率が少なくなり、セパレー
タ平坦部の強度補強効果が低下する傾向がある。
In the above prepreg, the resin impregnation is performed, for example, by applying a resin varnish obtained by uniformly dissolving a solid resin, a curing agent, a curing accelerator and the like in a tree-forming solvent to a woven or nonwoven fabric. be able to. The resin amount (solid content) applied to the fiber woven fabric or the nonwoven fabric is preferably 30 to 60 parts by weight, more preferably 40 to 50 parts by weight, based on the glass cloth. If the resin amount is less than 30 parts by weight, the level of gas impermeability tends to decrease,
If it exceeds 60 parts by weight, the fiber ratio tends to decrease, and the effect of reinforcing the strength of the flat portion of the separator tends to decrease.

【0042】上記のプリプレグの使用形態について、特
に制限はないが、平坦部の補強をしたい部分の形状に加
工したもの、予め成形用シートと同寸法に加工したもの
等を使用すれば、成形加工時間の短縮、得られる成形体
の精度向上に大きく影響し有効である。表面に樹脂を有
しないガラス布を使用する場合、成形時に成形用シート
との接着性を向上させるために、表面を樹脂被覆してお
いてもよい。
There is no particular limitation on the form of use of the prepreg, but if a prepreg processed into the shape of a portion to be reinforced and a pre-processed sheet having the same dimensions as the forming sheet are used, the forming process can be performed. This is effective since it greatly affects the reduction of time and the improvement of the accuracy of the obtained molded body. In the case where a glass cloth having no resin on the surface is used, the surface may be coated with a resin in order to improve the adhesiveness to a molding sheet during molding.

【0043】本発明になる燃料電池用セパレータを得る
ための成形方法については特に制限はないが、圧縮成形
法で成形することが好ましい。また、本発明になる燃料
電池用セパレータの寸法については特に制限はなく、燃
料電池の大きさにより、適宜選定する。
There is no particular limitation on the molding method for obtaining the fuel cell separator according to the present invention, but it is preferable that the molding be performed by a compression molding method. The dimensions of the fuel cell separator according to the present invention are not particularly limited, and are appropriately selected according to the size of the fuel cell.

【0044】本発明の燃料電池用セパレータを用いた燃
料電池の製作は、公知の方法により製作することができ
る。燃料電池は、本発明における燃料電池用セパレータ
により、固体高分子電解質膜などからなる電解質層及び
これを挟む二つのガス拡散層(燃料極と空気極、カーボ
ンペーパー等からなる)を挟むようにして形成されるセ
ルを必要数積層された構造を有する。本発明における燃
料電池用セパレータは、電解質の種類によって分類され
るアルカリ型、固体高分子型、リン酸型、溶融炭酸塩
型、固体酸型等の燃料電池のセパレータとして使用でき
る。
The fuel cell using the fuel cell separator of the present invention can be manufactured by a known method. The fuel cell is formed by the fuel cell separator of the present invention so as to sandwich an electrolyte layer made of a solid polymer electrolyte membrane or the like and two gas diffusion layers (made of a fuel electrode and an air electrode, carbon paper, etc.) sandwiching the electrolyte layer. The required number of cells are stacked. The fuel cell separator according to the present invention can be used as a fuel cell separator of an alkaline type, a solid polymer type, a phosphoric acid type, a molten carbonate type, a solid acid type, or the like classified according to the type of the electrolyte.

【0045】以下、本発明の実施の形態を図面により説
明する。図1は、本発明の実施例になる燃料電池用セパ
レータ(一例)の平面図及び図2は図1のA−A断面図
で、1はガスと冷却水の供給路を確保するためのリブ
(溝)を有するリブ部、2はガスと冷却水を供給するた
めの穴部、3は平坦部及び4はセパレータを補強するた
めのガラスクロスプリプレクグである。
Hereinafter, embodiments of the present invention will be described with reference to the drawings. FIG. 1 is a plan view of a fuel cell separator (one example) according to an embodiment of the present invention, and FIG. 2 is a cross-sectional view taken along line AA of FIG. 1. 1 is a rib for securing a gas and cooling water supply path. A rib portion having (grooves), a hole portion 2 for supplying gas and cooling water, a flat portion 3, and a glass cloth prepreg 4 for reinforcing the separator.

【0046】[0046]

【実施例】以下、実施例により本発明を説明する。 実施例1 (1)成形用混合粉の製造 板厚が1.0mm及び密度が1000kg/mの膨張黒
鉛シート(日立化成工業(株)製、商品名カーボフィッ
トHGP−105)を粗粉砕及び微粉砕機で粉砕し、数
平均粒径が100μmの膨張黒鉛シート粉砕粉0.7k
gを得た。次いでジヒドロベンゾオキサジン環を分子構
造中に有する数平均粒径が30μmの粉末状フェノール
樹脂(日立化成工業(株)製、商品名HR1060)
0.3Kgを加えて小型Vブレンダーで乾式混合し、1.
0kgの混合粉を得た。
The present invention will be described below with reference to examples. Example 1 (1) Production of Molded Powder Mixtures of expanded graphite sheet (Carbofit HGP-105, manufactured by Hitachi Chemical Co., Ltd., trade name: 1.0 mm and density: 1000 kg / m 3 ) Pulverized by a fine pulverizer, pulverized powder of expanded graphite sheet having a number average particle diameter of 100 μm 0.7 k
g was obtained. Next, a powdery phenol resin having a dihydrobenzoxazine ring in the molecular structure and having a number average particle size of 30 μm (trade name: HR1060, manufactured by Hitachi Chemical Co., Ltd.)
Add 0.3 kg and dry mix with a small V blender.
0 kg of a mixed powder was obtained.

【0047】(2)ガラスクロスプリプレグの製造 寸法200mm×200mmに切断したガラスクロス
(日東紡(株)製、商品名WF230 100BS6,
平織)を用意した。一方、粉末状エポキシ樹脂(シエル
化学(株)製、商品名エピコート1004)100g、
ジシアンジアミド(試薬)3g及びベンジルジメチルア
ミン(試薬)0.15gをメチル・オキシトール(有機
溶媒)150gにゆっくり添加し、均一に混合して樹脂
組成物を得た。
(2) Production of glass cloth prepreg Glass cloth cut into dimensions 200 mm × 200 mm (trade name WF230 100BS6, manufactured by Nitto Boseki Co., Ltd.)
Plain weave). On the other hand, 100 g of a powdery epoxy resin (manufactured by Ciel Chemical Co., Ltd., trade name: Epicoat 1004),
3 g of dicyandiamide (reagent) and 0.15 g of benzyldimethylamine (reagent) were slowly added to 150 g of methyl oxytol (organic solvent), and uniformly mixed to obtain a resin composition.

【0048】この後、前記ガラスクロス1枚当たり、樹
脂組成物40重量部及びガラスクロス60重量部の割合
になるように樹脂組成物を含浸塗工したガラスクロスを
2枚作製し、これを160℃で5分間熱処理を行い、厚
さが0.26mmのガラスクロスプリプレグを得た。
Thereafter, two glass cloths impregnated with the resin composition were prepared so as to have a ratio of 40 parts by weight of the resin composition and 60 parts by weight of the glass cloth per one piece of the glass cloth. Heat treatment was performed at 5 ° C. for 5 minutes to obtain a glass cloth prepreg having a thickness of 0.26 mm.

【0049】(3)燃料電池用セパレータの製造 次に、図1及び図2に示す形状の燃料電池用セパレータ
を得るために金型を用意した。下型は成形面(縦、横2
00mm)が平坦な雌型とし、上型は突起部を有する雄
型とした。ただし、上型において、突起部の高さ0.5
mm、突起部ピッチ1.0mm、リブ部1の幅1.0mm
及びリブテーパ10度とした。
(3) Production of Fuel Cell Separator Next, a mold was prepared to obtain a fuel cell separator having the shape shown in FIGS. The lower mold has a molding surface (length, width 2)
00 mm) was a flat female mold, and the upper mold was a male mold having a projection. However, in the upper mold, the height of the protrusion is 0.5.
mm, pitch of protrusions 1.0mm, width of rib 1 1.0mm
And a rib taper of 10 degrees.

【0050】上記の下型を180℃に加熱し、この下型
に(1)で得た混合粉(1m当たり1kg)0.06k
gをロールでシート状に加工した成形用シートを1枚載
置し、さらにその上に、(2)で得たガラスクロスプリプ
レグ4の中央部を切り欠いて平坦部3形状に加工したも
のを1枚載置した後、その上部に上型の突起部を有する
部分を下に向けてセットし、その後190℃面圧19.
6MPa(2×10kg/m)の条件で10分間成
形し、次いで、平坦部3に穴部2を簡易打ち抜き機で打
ち抜いて燃料電池用セパレータを得た。得られた燃料電
池用セパレータのリブ部1及び平坦部3の厚さ(ガラス
クロスプリプレグ4を含む)は1.0mm、リブ部1の
溝の深さは0.5mmであった。
The lower mold was heated to 180 ° C., and the mixed powder (1 kg per m 2 ) of 0.06 k
g was processed into a sheet shape by a roll, and one sheet for forming was placed thereon. Further, the center portion of the glass cloth prepreg 4 obtained in (2) was cut out and processed into a flat portion 3 shape. After placing one sheet, the part having the upper mold protrusion on the upper part is set downward, and then the surface pressure is set at 190 ° C. 19.
Molding was performed for 10 minutes under the conditions of 6 MPa (2 × 10 6 kg / m 2 ), and then the flat portion 3 was punched out of the hole 2 with a simple punching machine to obtain a fuel cell separator. The thickness (including the glass cloth prepreg 4) of the rib portion 1 and the flat portion 3 of the obtained fuel cell separator was 1.0 mm, and the depth of the groove of the rib portion 1 was 0.5 mm.

【0051】比較例1 (1)成形用混合粉の製造 実施例1の(1)と同様の工程を経て成形用混合粉を得
た。 (2)ガラスクロスプリプレグの製造 粉末状エポキシ樹脂として(シエル化学(株)製、商品
名エピコート1001)を使用した以外は、実施例1と
同様の配合量及び同様の工程を経てガラスクロスプリプ
レグを得た。 (3)燃料電池用セパレータの製造 実施例1の(3)と同様の工程を経て燃料電池用セパレー
タを得た。
Comparative Example 1 (1) Production of Mixed Powder for Molding A mixed powder for molding was obtained through the same steps as (1) of Example 1. (2) Production of glass cloth prepreg Except for using (Ciel Chemical Co., Ltd., product name Epicoat 1001) as a powdery epoxy resin, a glass cloth prepreg was produced through the same blending amount and the same process as in Example 1. Obtained. (3) Production of Fuel Cell Separator A fuel cell separator was obtained through the same steps as in Example 1, (3).

【0052】次に、上記実施例1及び比較例1で得られ
た燃料電池用セパレータについて、外観及びガス不浸透
性について評価した。その結果を表1に示す。また、実
施例1及び比較例1で使用した粉末状エポキシ樹脂の融
点及びゲル化時間を合わせて表1に示す。なお、上記実
施例1及び比較例1において、成形用混合粉を得るのに
使用した粉末状フェノール樹脂の融点は、100℃及び
ゲル化時間は、50秒(190℃)であった。
Next, the appearance and gas impermeability of the fuel cell separators obtained in Example 1 and Comparative Example 1 were evaluated. Table 1 shows the results. Table 1 also shows the melting point and the gel time of the powdery epoxy resin used in Example 1 and Comparative Example 1. In Example 1 and Comparative Example 1, the melting point of the powdery phenol resin used to obtain the mixed powder for molding was 100 ° C, and the gelation time was 50 seconds (190 ° C).

【0053】上記に示す融点は、デュランス水銀法によ
り測定した。詳しくは、3±0.005gで秤量した試
料を標準試験管に入れ、電熱器上で加熱して融解させた
後、冷却固化しその上部に50gの水銀を入れ、再度2
℃/分で昇温していき、融解試料が水銀層の上部に見え
たときの温度を融点とした。また、ゲル化時間は、ゲル
化時間測定装置(JIS C2104:熱盤法)を使用
して試料量0.2gについてそれぞれ3回測定し、その
平均値を求めた。
The melting points shown above were measured by the Durance mercury method. Specifically, a sample weighed at 3 ± 0.005 g was placed in a standard test tube, heated and melted on an electric heater, then cooled and solidified, and 50 g of mercury was placed on the upper portion thereof, and the sample was cooled again.
The temperature was raised at a rate of ° C./min, and the temperature at which the molten sample was seen above the mercury layer was defined as the melting point. The gelation time was measured three times for each 0.2 g of sample using a gelation time measuring device (JIS C2104: hot plate method), and the average value was determined.

【0054】また、外観は、成形体のリブ部及びリブ部
と平坦部の界面部を目視観察し、リブ部に少しでもプリ
プレグの樹脂成分が付着した場合及び前記界面部にプリ
プレグの樹脂層が介在した場合を不良とした。ガス不浸
透性(ガス漏れ)は、成形体の平坦部(ガラスクロスプ
リプレグ複合部含む)を切断し、リークデイラクタを用
い0.2MPaの内圧をかけ、水中で発生する水泡の確
認をした。
The appearance of the rib portion of the molded product and the interface between the rib portion and the flat portion were visually observed, and the resin component of the prepreg was slightly adhered to the rib portion. The case where it intervened was regarded as defective. As for gas impermeability (gas leakage), a flat part (including a glass cloth prepreg composite part) of a molded body was cut, and an internal pressure of 0.2 MPa was applied using a leak deactor to confirm water bubbles generated in water.

【0055】[0055]

【表1】 [Table 1]

【0056】表1に示されるように、本発明になる実施
例1の燃料電池用セパレータは、比較例1の燃料電池用
セパレータに比較して外観及びガス不浸透性が優れるこ
とが明らかである。なお、比較例1の燃料電池用セパレ
ータにおいて、水泡の発生箇所は、リブ部と平坦部との
界面部におけるガラスクロスプリプレグの樹脂層の部分
であった。
As shown in Table 1, it is apparent that the fuel cell separator of Example 1 according to the present invention is superior in appearance and gas impermeability to the fuel cell separator of Comparative Example 1. . In the fuel cell separator of Comparative Example 1, the location where the water bubbles occurred was the resin layer portion of the glass cloth prepreg at the interface between the rib portion and the flat portion.

【0057】[0057]

【発明の効果】請求項1〜7記載の燃料電池用セパレー
タは、ガス不浸透性、電気特性、液膨潤性、機械強度等
に問題がなく、かつ成形性の良好な、燃料電池用セパレ
ータである。請求項8及び9記載の燃料電池は、ガス不
浸透性、電気特性、液膨潤性、機械強度等に問題がな
く、かつ成形性の良好な、燃料電池用セパレータを有す
る高性能な燃料電池を提供するものである。
The fuel cell separator according to any one of claims 1 to 7 is a fuel cell separator which has no problem in gas impermeability, electric properties, liquid swelling property, mechanical strength and the like and has good moldability. is there. The fuel cell according to claims 8 and 9 is a high-performance fuel cell having a fuel cell separator which has no problem in gas impermeability, electric characteristics, liquid swelling property, mechanical strength, etc., and has good moldability. To provide.

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

【図1】本発明の実施例になる燃料電池用セパレータの
平面図である。
FIG. 1 is a plan view of a fuel cell separator according to an embodiment of the present invention.

【図2】図1のA−A断面図である。FIG. 2 is a sectional view taken along line AA of FIG.

【符号の説明】[Explanation of symbols]

1 リブ部 2 穴部 3 平坦部 4 ガラスクロスプリプレグ DESCRIPTION OF SYMBOLS 1 Rib part 2 Hole part 3 Flat part 4 Glass cloth prepreg

フロントページの続き (72)発明者 田代 了嗣 茨城県日立市鮎川町三丁目3番1号 日立 化成工業株式会社山崎事業所内 Fターム(参考) 5H026 AA06 CC03 CX05 EE06 EE18Continuation of the front page (72) Inventor Ryoji Tashiro 3-3-1 Ayukawacho, Hitachi City, Ibaraki Prefecture Hitachi Chemical Co., Ltd. Yamazaki Office F-term (reference)

Claims (9)

【特許請求の範囲】[Claims] 【請求項1】リブ部及び平坦部を有する燃料電池用セパ
レータにおいて、平坦部が膨張黒鉛粉と固形樹脂aの混
合物を含む層及び固形樹脂bを含有した絶縁性を有する
材料を含む層からなり、かつ膨張黒鉛粉と混合する固形
樹脂aの融点と絶縁性を有する材料に含有する固形樹脂
bの融点がほぼ同等である燃料電池用セパレータ。
1. A fuel cell separator having a rib portion and a flat portion, wherein the flat portion comprises a layer containing a mixture of expanded graphite powder and a solid resin a and a layer containing an insulating material containing a solid resin b. A fuel cell separator in which the melting point of the solid resin a mixed with the expanded graphite powder is substantially equal to the melting point of the solid resin b contained in the insulating material.
【請求項2】リブ部が、膨張黒鉛粉と固形樹脂aの混合
物を含む層からなる請求項1記載の燃料電池用セパレー
タ。
2. The fuel cell separator according to claim 1, wherein the rib portion comprises a layer containing a mixture of expanded graphite powder and solid resin a.
【請求項3】膨張黒鉛粉が、膨張黒鉛シート粉砕粉であ
る請求項1又は2記載の燃料電池用セパレータ。
3. The fuel cell separator according to claim 1, wherein the expanded graphite powder is a pulverized powder of expanded graphite sheet.
【請求項4】膨張黒鉛粉と混合する固形樹脂aに比較
し、絶縁性を有する材料に含有する固形樹脂bのゲル化
時間が短い請求項1〜3記載の燃料電池用セパレータ。
4. The fuel cell separator according to claim 1, wherein the gelling time of the solid resin b contained in the insulating material is shorter than that of the solid resin a mixed with the expanded graphite powder.
【請求項5】セパレータが、リブ部及び平坦部以外に穴
部を有する請求項1〜4記載の燃料電池用セパレータ。
5. The fuel cell separator according to claim 1, wherein the separator has a hole in addition to the rib portion and the flat portion.
【請求項6】絶縁性を有する材料に含有する固形樹脂b
が、架橋点であるエポキシ基を1つ以上有するエポキシ
樹脂である請求項1〜5記載の燃料電池用セパレータ。
6. A solid resin b contained in an insulating material.
Is an epoxy resin having at least one epoxy group as a cross-linking point.
【請求項7】絶縁性を有する材料が、プリプレグである
請求項1〜6記載の燃料電池用セパレータ。
7. The fuel cell separator according to claim 1, wherein the insulating material is a prepreg.
【請求項8】請求項1〜7のいずれかに記載のセパレー
タを有してなる燃料電池。
8. A fuel cell comprising the separator according to claim 1.
【請求項9】固体高分子型である請求項8記載の燃料電
池。
9. The fuel cell according to claim 8, which is of a solid polymer type.
JP2001169849A 2001-06-05 2001-06-05 Fuel cell separator and fuel cell using the same Pending JP2002367623A (en)

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Country Link
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008159587A (en) * 2006-12-21 2008-07-10 Gm Global Technology Operations Inc Process for molding composite bipolar plate with reinforced outer edge
JP2015002003A (en) * 2013-06-13 2015-01-05 パナソニック株式会社 Separator for fuel cell and method of manufacturing the same

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH11354136A (en) * 1998-04-07 1999-12-24 Hitachi Chem Co Ltd Fuel cell, separator for fuel cell, and manufacture therefor
JP2000164226A (en) * 1998-11-27 2000-06-16 Mitsubishi Plastics Ind Ltd Manufacture of separator for fuel cell
JP2000208154A (en) * 1999-01-12 2000-07-28 Nichias Corp Fuel cell separator and its production
JP2002203574A (en) * 2000-08-25 2002-07-19 Hitachi Chem Co Ltd Separator for fuel cell and fuel cell using separator for fuel cell

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH11354136A (en) * 1998-04-07 1999-12-24 Hitachi Chem Co Ltd Fuel cell, separator for fuel cell, and manufacture therefor
JP2000164226A (en) * 1998-11-27 2000-06-16 Mitsubishi Plastics Ind Ltd Manufacture of separator for fuel cell
JP2000208154A (en) * 1999-01-12 2000-07-28 Nichias Corp Fuel cell separator and its production
JP2002203574A (en) * 2000-08-25 2002-07-19 Hitachi Chem Co Ltd Separator for fuel cell and fuel cell using separator for fuel cell

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008159587A (en) * 2006-12-21 2008-07-10 Gm Global Technology Operations Inc Process for molding composite bipolar plate with reinforced outer edge
US8431283B2 (en) 2006-12-21 2013-04-30 GM Global Technology Operations LLC Process for molding composite bipolar plates with reinforced outer edges
DE102007061127B4 (en) 2006-12-21 2018-05-17 GM Global Technology Operations LLC (n. d. Ges. d. Staates Delaware) A unipolar plate and method of forming a composite unipolar plate for a fuel cell stack
JP2015002003A (en) * 2013-06-13 2015-01-05 パナソニック株式会社 Separator for fuel cell and method of manufacturing the same

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