JP2003242989A - Fuel cell - Google Patents
Fuel cellInfo
- Publication number
- JP2003242989A JP2003242989A JP2002035601A JP2002035601A JP2003242989A JP 2003242989 A JP2003242989 A JP 2003242989A JP 2002035601 A JP2002035601 A JP 2002035601A JP 2002035601 A JP2002035601 A JP 2002035601A JP 2003242989 A JP2003242989 A JP 2003242989A
- Authority
- JP
- Japan
- Prior art keywords
- negative electrode
- fuel cell
- positive electrode
- electrode side
- diffusion layer
- 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
Links
Classifications
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、負極に液体燃料を
用いた燃料電池に関するものである。TECHNICAL FIELD The present invention relates to a fuel cell using a liquid fuel for a negative electrode.
【０００２】[0002]
【従来の技術】この種の燃料電池は、正極に酸素を電気
化学的に還元することが可能な触媒を、負極に液体燃
料、とくにメタノールを電気化学的に酸化することの可
能な触媒を、それぞれ用い、電解質にプロトン（Ｈ+ ）
伝導性の電解質膜を用いており、燃料の供給方式の違い
により、気体供給型と液体供給型とがある。2. Description of the Related Art In this type of fuel cell, a positive electrode is provided with a catalyst capable of electrochemically reducing oxygen, and a negative electrode is provided with a catalyst capable of electrochemically oxidizing liquid fuel, particularly methanol. Proton (H + ) is used as electrolyte for each
A conductive electrolyte membrane is used, and there are a gas supply type and a liquid supply type depending on the difference in fuel supply system.
【０００３】このうち、液体供給型は、燃料の供給方式
に毛管力などを利用するもので、外部の燃料供給装置が
不要であり、小型化が可能な電池として、注目されてい
る。この液体供給型の燃料電池は、触媒層をカーボンペ
ーパーなどからなる拡散層に担持させて負極を構成し、
燃料タンクから供給される燃料を上記拡散層を介して触
媒層に導いて酸化し、生成したプロトンを電解質膜を介
して正極側に移動させて酸素と反応させることにより、
発電を行うものである。Among them, the liquid supply type uses a capillary force or the like as a fuel supply system, does not require an external fuel supply device, and is attracting attention as a battery which can be miniaturized. In this liquid supply type fuel cell, a catalyst layer is supported on a diffusion layer made of carbon paper or the like to form a negative electrode,
By guiding the fuel supplied from the fuel tank to the catalyst layer through the diffusion layer and oxidizing it, the generated protons are moved to the positive electrode side through the electrolyte membrane to react with oxygen,
It generates electricity.
【０００４】[0004]
【発明が解決しようとする課題】しかし、このように構
成される従来の燃料電池は、拡散層を介した液体燃料の
供給がスムーズにいかず、出力が不安定になりやすく、
小型化可能な電池として各種用途に利用する場合に、安
定した出力を発揮させにくかった。However, in the conventional fuel cell configured as described above, the liquid fuel cannot be smoothly supplied through the diffusion layer, and the output tends to be unstable,
When used as a miniaturizable battery in various applications, it was difficult to produce a stable output.
【０００５】本発明は、このような事情に照らし、液体
供給型の燃料電池において、負極への液体燃料の供給を
スムーズに行えて、安定した出力を発揮させることがで
きる燃料電池を提供することを目的としている。In view of such circumstances, the present invention provides a liquid supply type fuel cell which can smoothly supply the liquid fuel to the negative electrode and exhibit a stable output. It is an object.
【０００６】[0006]
【課題を解決するための手段】本発明者らは、上記の目
的に対し、鋭意検討した結果、負極触媒層を担持する負
極側拡散層として、界面活性剤などによる親水化処理を
施したカーボンペーパーなどを用いたときに、負極触媒
層への液体燃料の供給がスムーズとなり、安定した出力
を発揮させうることを知り、本発明を完成した。Means for Solving the Problems The inventors of the present invention have made extensive studies as to the above object, and as a result, as a negative electrode side diffusion layer carrying a negative electrode catalyst layer, carbon which has been subjected to a hydrophilic treatment with a surfactant or the like. The present invention has been completed, knowing that the supply of liquid fuel to the negative electrode catalyst layer becomes smooth and stable output can be achieved when paper or the like is used.
【０００７】すなわち、本発明は、液体供給型の燃料電
池として、正極に酸素を電気化学的に還元することが可
能な触媒を、負極に液体燃料を電気化学的に酸化するこ
とが可能な触媒を、それぞれ用いた燃料電池において、
負極触媒層を担持する負極側拡散層が親水化処理を施し
た多孔質の炭素材料で構成されていることを特徴とする
燃料電池、とくに上記多孔質の炭素材料がカーボンペー
パーまたはカーボンクロスである上記構成の燃料電池に
係るものである。That is, the present invention is a liquid supply type fuel cell in which a positive electrode is a catalyst capable of electrochemically reducing oxygen and a negative electrode is a catalyst capable of electrochemically oxidizing a liquid fuel. In the fuel cell using
A fuel cell characterized in that the negative electrode side diffusion layer supporting the negative electrode catalyst layer is composed of a porous carbon material subjected to a hydrophilization treatment, and particularly the porous carbon material is carbon paper or carbon cloth. The present invention relates to a fuel cell having the above structure.
【０００８】[0008]
【発明の実施の形態】以下に、本発明の実施の形態につ
いて、説明する。図１は、本発明の燃料電池の基本構成
（モデルセル）を示す概略図である。図１において、１
は正極側集電体、２は正極側拡散層、３は電解質膜、４
は負極側拡散層、５は負極側集電体、６は燃料タンク、
７は正極側集電体１に設けられた空気孔、８は正極触媒
層、９は負極触媒層である。BEST MODE FOR CARRYING OUT THE INVENTION Embodiments of the present invention will be described below. FIG. 1 is a schematic diagram showing the basic configuration (model cell) of the fuel cell of the present invention. In FIG. 1, 1
Is a positive electrode side current collector, 2 is a positive electrode side diffusion layer, 3 is an electrolyte membrane, 4
Is a diffusion layer on the negative electrode side, 5 is a current collector on the negative electrode side, 6 is a fuel tank,
Reference numeral 7 is an air hole provided in the positive electrode side current collector 1, 8 is a positive electrode catalyst layer, and 9 is a negative electrode catalyst layer.
【０００９】正極側集電体１は、空気孔７を介して外気
（酸素）を取り込む通気構造体としての機能を有すると
ともに、集電機能をも有している。正極側拡散層２は、
カーボンペーパーまたはカーボンクロスなどの多孔質の
炭素材料からなり、これに正極触媒層８を担持させて、
正極を構成している。正極側拡散層２は、必要により後
述する負極側拡散層４の場合と同様に、親水化処理を施
したカーボンペーパーまたはカーボンクロスなどで構成
してもよい。正極触媒層８は、酸素を電気化学的に還元
することが可能な触媒、たとえば、白金、金、銀などの
単体、混合物または合金などを用いて、これ単独の粉末
またはカーボン表面に付着させた複合粉末として、塗工
法および加圧成形法により、形成される。The positive electrode side current collector 1 has a function as a ventilation structure for taking in outside air (oxygen) through the air holes 7, and also has a current collecting function. The positive electrode side diffusion layer 2 is
It is made of a porous carbon material such as carbon paper or carbon cloth, and carries the positive electrode catalyst layer 8 thereon,
It constitutes the positive electrode. If necessary, the positive electrode side diffusion layer 2 may be made of carbon paper or carbon cloth that has been subjected to a hydrophilic treatment, as in the case of the negative electrode side diffusion layer 4 described later. The positive electrode catalyst layer 8 was formed by using a catalyst capable of electrochemically reducing oxygen, for example, a simple substance, a mixture, or an alloy of platinum, gold, silver, etc., and adhering it to the powder or carbon surface alone. It is formed as a composite powder by a coating method and a pressure molding method.
【００１０】電解質膜３は、負極で発生したプロトンを
正極側に輸送する機能と、さらに正極と負極との短絡を
防止するセパレータとしての機能を備えてなるものであ
る。具体的には、デュボン社製の商品名「ナフイオ
ン」、畑硝子社製の商品名「フレミオン」、ＴＯＫＵＹ
ＡＭＡ社製の商品名「ネオセブタＣＭ−１」などのフツ
素樹脂や炭化水素系樹脂を骨格としたカチオン交換能を
有するカチオン交換膜、固体電解質として公知となって
いるリン酸ドープＳｉＯ2 膜、高分子および酸化物に酸
性溶液を含浸したゲル電解質などが用いられる。The electrolyte membrane 3 has a function of transporting protons generated at the negative electrode to the positive electrode side, and a function as a separator for preventing a short circuit between the positive electrode and the negative electrode. Specifically, the product name "Nafion" manufactured by Dubon, the product name "Flemion" manufactured by Hata Glass, and TOKUY
A cation exchange membrane having a cation exchange capacity with a fluorinated resin or a hydrocarbon resin such as "Neocebuta CM-1" manufactured by AMA Co., Ltd., a phosphoric acid-doped SiO 2 membrane known as a solid electrolyte, A gel electrolyte obtained by impregnating a polymer and an oxide with an acidic solution is used.
【００１１】負極側集電体５は、燃料タンク６に収納さ
れた液体燃料、たとえばメタノール水溶液などをはじめ
とする水素を含む有機系の水溶液を、毛管力などを利用
して電池内に取り込む機能を有するとともに、集電機能
をも有している。負極側拡散層４は、本発明において最
も重要な構成要素であり、親水化処理を施した多孔質の
炭素材料、とくに親水化処理を施したカーボンペーパー
またはカーボンクロスからなり、これに負極触媒層９を
担持させて、負極を構成している。負極触媒層９は、上
記の液体燃料を電気化学的に酸化することが可能な触
媒、たとえば、白金微粒子や、鉄、ニッケル、コバル
ト、錫、ルテニウムまたは金などと白金との合金微粒子
などを用いて、これら単独の粉末またはカーボン表面に
付着させた複合粉末として、塗工法および加圧成形法に
より、形成される。The negative electrode side current collector 5 has a function of taking in a liquid fuel contained in the fuel tank 6, for example, an organic aqueous solution containing hydrogen such as an aqueous methanol solution into the cell by utilizing capillary force or the like. In addition to having a current collecting function. The negative electrode side diffusion layer 4 is the most important component in the present invention, and is made of a hydrophilic carbon material having a hydrophilic property, in particular, a hydrophilic carbon paper or a carbon cloth. 9 is supported to form the negative electrode. The negative electrode catalyst layer 9 uses a catalyst capable of electrochemically oxidizing the above liquid fuel, for example, platinum fine particles or alloy fine particles of platinum with iron, nickel, cobalt, tin, ruthenium or gold. Then, these single powders or composite powders adhered to the carbon surface are formed by a coating method and a pressure molding method.
【００１２】上記の負極側拡散層４において、カーボン
ペーパーやカーボンクロスなどの多孔質の炭素材料に親
水化処理を施すには、たとえば、炭素材料に電解酸化
や酸性溶液中での酸化などの処理を施して表面に官能基
を付与する方法、炭素材料にプラズマ処理などを施し
て表面を粗面化する方法、炭素材料の表面に界面活性
剤を付与する方法、炭素材料の表面にＳｉＯ2 やＴｉ
Ｏ2 などの酸化物や電解質膜として用いる材料の液体状
や粉末状のものを付着させる方法などがある。また、親
水化処理を施したカーボンペーパーなどでは、その作製
時にＳｉＯ2 やＴｉＯ2 などの酸化物やその他の親水化
処理物質を混合しておき、これを用いてカーボンペーパ
ーなどを作製するようにしてもよい。In the above negative electrode side diffusion layer 4, in order to apply a hydrophilic treatment to a porous carbon material such as carbon paper or carbon cloth, for example, the carbon material is treated by electrolytic oxidation or oxidation in an acidic solution. To impart a functional group to the surface of the carbon material, a method of roughening the surface of the carbon material by plasma treatment, a method of imparting a surfactant to the surface of the carbon material, SiO 2 or Ti
There is a method of adhering an oxide such as O 2 or a liquid or powder material used as an electrolyte membrane. Further, in the case of carbon paper or the like that has been subjected to a hydrophilization treatment, an oxide such as SiO 2 or TiO 2 or another hydrophilization substance is mixed at the time of its production, and carbon paper or the like is produced using this. May be.
【００１３】このように構成される燃料電池において、
負極側集電体５から供給される液体燃料は負極側拡散層
４を介して負極触媒層９に導かれて酸化され、電子とプ
ロトンに変換され、このプロトンは電解質膜３を介して
正極側に移動する。正極では正極側集電体１から取り込
まれた酸素が還元されて電子を生じ、これと上記のプロ
トンとが反応して水を生成し、この電池反応により、発
電する。なお、正極で生成した上記の水は、正極側拡散
層２および正極側集電体１を介して、外部に放出され
る。また、負極で生成した炭酸ガスなどの反応ガスは、
負極側拡散層４および負極側集電体５を介して、やはり
外部に取り出される。In the fuel cell thus constructed,
The liquid fuel supplied from the negative electrode side current collector 5 is guided to the negative electrode catalyst layer 9 via the negative electrode side diffusion layer 4, is oxidized, and is converted into electrons and protons. This proton is passed through the electrolyte membrane 3 to the positive electrode side. Move to. In the positive electrode, oxygen taken in from the positive electrode side current collector 1 is reduced to generate electrons, and this reacts with the above-mentioned protons to generate water, and this battery reaction causes power generation. The water generated in the positive electrode is discharged to the outside via the positive electrode side diffusion layer 2 and the positive electrode current collector 1. In addition, the reaction gas such as carbon dioxide gas generated at the negative electrode is
It is also taken out through the negative electrode side diffusion layer 4 and the negative electrode side current collector 5.
【００１４】このような電池反応において、既述のとお
り、負極側拡散層４を親水化処理を施した多孔質の炭素
材料で構成したことにより、負極側集電体５から供給さ
れるメタノール水溶液などからなる液体燃料の上記拡散
層４への親和性が良くなり、この拡散層４を介した負極
触媒層９への液体燃料の拡散がスムーズに行われる。そ
の結果、電池反応が安定し、電池の出力が向上する。In such a battery reaction, as described above, since the negative electrode side diffusion layer 4 is made of the porous carbon material subjected to the hydrophilic treatment, the aqueous methanol solution supplied from the negative electrode side current collector 5 is obtained. The affinity of the liquid fuel composed of, for example, with the diffusion layer 4 is improved, and the liquid fuel is smoothly diffused to the negative electrode catalyst layer 9 through the diffusion layer 4. As a result, the battery reaction is stabilized and the battery output is improved.
【００１５】[0015]
【実施例】つぎに、本発明の実施例を記載して、より具
体的に説明する。EXAMPLES Next, examples of the present invention will be described to more specifically describe.
【００１６】実施例１
カーボンペーパーに、１重量％のノニオン系界面活性剤
〔ポリオキシエチレン（１０）オクチルフェニルエーテ
ル〕を吸着させ、親水化処理を施したカーボンペーパー
を得た。また、白金−ルテニウム合金担持カーボンを含
む溶液とイオン交換水を混合し、撹拌したのち、その粘
度を調整して、触媒層用インクとした。これを、上記の
親水化処理を施したカーボンペーパー上に、スクリーン
印刷（スクリーン版は１８０メッシュ）し、乾燥後、ホ
ットプレスした。Example 1 Carbon paper was adsorbed with 1% by weight of a nonionic surfactant [polyoxyethylene (10) octylphenyl ether] to obtain a carbon paper which was subjected to a hydrophilic treatment. Further, a solution containing platinum-ruthenium alloy-supporting carbon and ion-exchanged water were mixed and stirred, and then the viscosity was adjusted to obtain a catalyst layer ink. This was screen-printed (screen mesh was 180 mesh) on the above-mentioned hydrophilic carbon paper, dried, and then hot-pressed.
【００１７】このようにして、親水化処理を施したカー
ボンペーパーからなる負極側拡散層とこれに担持された
白金−ルテニウム合金担持カーボンを含む負極触媒層と
からなる負極を作製した。また、これとは別に、白金担
持カーボンを含む溶液を用いた以外は、上記と同じ方法
にて、親水化処理を施したカーボンペーパーからなる正
極側拡散層とこれに担持された白金担持カーボンを含む
正極触媒層とからなる正極を作製した。これらの負極お
よび正極と、液体燃料として３重量％のメタノール水溶
液を用い、図１に示すようなモデルセルを作製した。In this way, a negative electrode comprising a negative electrode side diffusion layer made of carbon paper subjected to a hydrophilization treatment and a negative electrode catalyst layer containing platinum-ruthenium alloy-supporting carbon supported thereon was produced. Separately from this, except that a solution containing platinum-supporting carbon was used, in the same manner as above, the positive electrode side diffusion layer made of carbon paper subjected to hydrophilic treatment and the platinum-supporting carbon supported thereon were prepared. A positive electrode including the positive electrode catalyst layer containing the positive electrode was prepared. A model cell as shown in FIG. 1 was prepared using these negative and positive electrodes and a 3 wt% aqueous methanol solution as a liquid fuel.
【００１８】比較例１
カーボンペーパーにノニオン系界面活性剤による親水化
処理を施さなかった以外は、実施例１と同様にして、負
極および正極を作製し、これらを用いて、実施例１と同
様にして、図１に示すようなモデルセルを作製した。Comparative Example 1 A negative electrode and a positive electrode were prepared in the same manner as in Example 1 except that the carbon paper was not hydrophilized with a nonionic surfactant, and these were used in the same manner as in Example 1. Then, a model cell as shown in FIG. 1 was produced.
【００１９】上記の実施例１および比較例１のモデルセ
ルについて、２０ｍＡ／cm2 で放電試験を行い、両セル
の出力特性を調べた。結果は、図２に示されるとおりで
あった。この結果から、本発明の実施例１のモデルセル
によると、比較例１のモデルセルに比べて、安定した高
い出力特性が得られることがわかる。The model cells of Example 1 and Comparative Example 1 were subjected to a discharge test at 20 mA / cm 2 and the output characteristics of both cells were examined. The result was as shown in FIG. From this result, it is understood that the model cell of Example 1 of the present invention can obtain stable and high output characteristics as compared with the model cell of Comparative Example 1.
【００２０】[0020]
【発明の効果】以上のように、本発明では、負極触媒層
を担持する負極側拡散層を親水化処理を施したカーボン
ペーパーまたはカーボンクロスなどからなる多孔質の炭
素材料で構成したことにより、液体供給型の燃料電池と
して、負極への液体燃料の供給をスムーズに行え、安定
した出力を発揮できる燃料電池を提供できる。As described above, according to the present invention, the negative electrode side diffusion layer supporting the negative electrode catalyst layer is made of the porous carbon material such as the carbon paper or the carbon cloth which has been subjected to the hydrophilic treatment. As the liquid supply type fuel cell, it is possible to provide a fuel cell that can smoothly supply the liquid fuel to the negative electrode and exhibit a stable output.
【図１】本発明の燃料電池の基本構成（モデルセル）を
示す概略図である。FIG. 1 is a schematic diagram showing a basic configuration (model cell) of a fuel cell of the present invention.
【図２】実施例１および比較例１のモデルセルの出力特
性を示す特性図である。FIG. 2 is a characteristic diagram showing output characteristics of model cells of Example 1 and Comparative Example 1.
１ 正極側集電体 ２ 正極側拡散層 ３ 電解質膜 ４ 負極側拡散層 ５ 負極側集電体 ６ 燃料タンク ７ 空気孔 ８ 正極触媒層 ９ 負極触媒層 1 Positive electrode side current collector 2 Positive electrode side diffusion layer 3 Electrolyte membrane 4 Negative electrode side diffusion layer 5 Negative electrode side current collector 6 Fuel tank 7 air holes 8 Positive electrode catalyst layer 9 Negative electrode catalyst layer
───────────────────────────────────────────────────── フロントページの続き (72)発明者 石 軍 大阪府茨木市丑寅一丁目１番88号 日立マ クセル株式会社内 (72)発明者 長井 龍 大阪府茨木市丑寅一丁目１番88号 日立マ クセル株式会社内 Ｆターム(参考） 5H018 AA07 AS07 BB00 DD06 EE03 EE05 ─────────────────────────────────────────────────── ─── Continued front page (72) Inventor Stone Army Hitachima, 1-88, Torora, Ibaraki City, Osaka Prefecture Within Kucsel Co., Ltd. (72) Inventor Ryu Nagai Hitachima, 1-88, Torora, Ibaraki City, Osaka Prefecture Within Kucsel Co., Ltd. F term (reference) 5H018 AA07 AS07 BB00 DD06 EE03 EE05
Claims (2)
が可能な触媒を、負極に液体燃料を電気化学的に酸化す
ることが可能な触媒を、それぞれ用いた燃料電池におい
て、負極触媒層を担持する負極側拡散層が親水化処理を
施した多孔質の炭素材料で構成されていることを特徴と
する燃料電池。1. A negative electrode catalyst layer in a fuel cell using a catalyst capable of electrochemically reducing oxygen in a positive electrode and a catalyst capable of electrochemically oxidizing a liquid fuel in a negative electrode, respectively. A fuel cell, wherein the negative electrode side diffusion layer carrying is made of a porous carbon material subjected to a hydrophilic treatment.
親水化処理を施したカーボンペーパーまたはカーボンク
ロスである請求項１に記載の燃料電池。2. The fuel cell according to claim 1, wherein the hydrophilized porous carbon material is hydrophilized carbon paper or carbon cloth.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2002035601A JP2003242989A (en) | 2002-02-13 | 2002-02-13 | Fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2002035601A JP2003242989A (en) | 2002-02-13 | 2002-02-13 | Fuel cell |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JP2003242989A true JP2003242989A (en) | 2003-08-29 |
Family
ID=27777747
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| Application Number | Title | Priority Date | Filing Date |
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| JP2002035601A Pending JP2003242989A (en) | 2002-02-13 | 2002-02-13 | Fuel cell |
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| JP (1) | JP2003242989A (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
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| JP2006147397A (en) * | 2004-11-22 | 2006-06-08 | Toyota Motor Corp | Gas diffusion layer for fuel cell, fuel cell and manufacturing method thereof |
| JP2007257965A (en) * | 2006-03-22 | 2007-10-04 | Toyota Central Res & Dev Lab Inc | Polymer electrolyte fuel cell and fuel cell system |
| JP2009070570A (en) * | 2007-09-10 | 2009-04-02 | Sharp Corp | Fuel cell |
| CN111244476A (en) * | 2018-11-28 | 2020-06-05 | 中国科学院大连化学物理研究所 | Hydrophilic treatment method of carbon paper for fuel cell and application thereof |
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| CN111244476B (en) * | 2018-11-28 | 2021-11-02 | 中国科学院大连化学物理研究所 | Hydrophilic treatment method of carbon paper for fuel cell and application thereof |
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