JP2003197203A - Fuel cell - Google Patents
Fuel cellInfo
- Publication number
- JP2003197203A JP2003197203A JP2001399889A JP2001399889A JP2003197203A JP 2003197203 A JP2003197203 A JP 2003197203A JP 2001399889 A JP2001399889 A JP 2001399889A JP 2001399889 A JP2001399889 A JP 2001399889A JP 2003197203 A JP2003197203 A JP 2003197203A
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- Prior art keywords
- gas
- electrode
- polymer membrane
- water
- fuel cell
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Classifications
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- 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
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- Inert Electrodes (AREA)
- Fuel Cell (AREA)
Abstract
(57)【要約】
【課題】 加湿されたガス中の加湿水や電気化学反応に
より生成する水を電極層中に均一に分布させることが行
える燃料電池を提供する。
【解決手段】 プロトン伝導性の固体高分子膜（１）
と、この固体高分子膜を狭持する電極（５）と、この電
極と接する面に凹状のガス流路（６）を形成したセパレ
ータ（７）とを備え、前記ガス流路に燃料ガスまたは酸
化剤ガスを流通させて発電を行う燃料電池において、前
記電極は、前記固体高分子膜側に形成された電極触媒層
（３）と、セパレータ側に形成されたガス拡散層（４）
とからなり、これら電極触媒層とガス拡散層の前記ガス
流路と相対する領域は、撥水性を備え、他の領域は親水
性を備える。
(57) [Problem] To provide a fuel cell capable of uniformly distributing humidified water in humidified gas or water generated by an electrochemical reaction in an electrode layer. SOLUTION: Proton-conductive solid polymer membrane (1)
An electrode (5) sandwiching the solid polymer membrane; and a separator (7) having a concave gas flow path (6) formed on a surface in contact with the electrode. In a fuel cell in which power is generated by flowing an oxidizing gas, the electrode includes an electrode catalyst layer (3) formed on the solid polymer membrane side and a gas diffusion layer (4) formed on a separator side.
The region of the electrode catalyst layer and the gas diffusion layer facing the gas flow path has water repellency, and the other regions have hydrophilicity.
Description
【０００１】[0001]
【発明の属する技術分野】本発明は燃料電池に関し、特
に、プロトン伝導性固体高分子膜を狭持した一対の電極
触媒層と、さらにその電極触媒層を外側から挟んだ一対
のガス拡散層とで燃料の流路を形成する流路形成部材を
備えた燃料電池に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a fuel cell, and more particularly to a pair of electrode catalyst layers sandwiching a proton conductive solid polymer membrane, and a pair of gas diffusion layers sandwiching the electrode catalyst layer from the outside. The present invention relates to a fuel cell including a flow path forming member that forms a fuel flow path.
【０００２】[0002]
【従来の技術】プロトン伝導性固体高分子膜を用いた固
体高分子型燃料電池では、プロトン伝導性固体高分子膜
を挟んで一対の電極（酸素極と燃料極）に、水素を含有
する燃料ガスと酸素を有する酸化ガスとをそれぞれ供給
することにより、次式で示される化学反応が生じ、電気
エネルギーが取出される。2. Description of the Related Art In a polymer electrolyte fuel cell using a proton-conducting solid polymer membrane, a fuel containing hydrogen is provided between a pair of electrodes (oxygen electrode and fuel electrode) with a proton-conducting solid polymer membrane interposed therebetween. By supplying the gas and the oxidizing gas containing oxygen, respectively, a chemical reaction represented by the following formula occurs and electric energy is taken out.
【０００３】カソード反応（酸素極）：２Ｈ+＋２ｅ-＋
（１／２）Ｏ2→Ｈ2Ｏ
アノード反応（燃料極）：Ｈ2→２Ｈ+＋２ｅ-
この電気化学反応を行うためには、酸素極側で、反応に
より生成する水を速やかに排出して酸素極側に酸化ガス
を連続的に供給することが必要である。また、プロトン
伝導性固体高分子膜が、高いプロトン伝導性を発現する
ためには、膜が十分に加湿されていることが必要であ
り、そのため、酸化ガス、燃料ガスは十分に加湿されて
供給される。これらの加湿されたガスを燃料極、酸素極
側ともにガス流路側から、プロトン伝導性固体高分子膜
にまで、むらなく拡散させる必要がある。このように、
燃料電池の電極においては、加湿されたガスをプロトン
伝導性固体高分子膜にむらなく均一に供給することと、
生成された水をガス流路側に効率よく、排出させるとい
う異なる特性を両立することが要求される。Cathode reaction (oxygen electrode): 2H + + 2e − +
(1/2) O 2 → H 2 O anode reaction (fuel electrode): H 2 → 2H + + 2e − To carry out this electrochemical reaction, the water generated by the reaction is quickly discharged on the oxygen electrode side. It is necessary to continuously supply the oxidizing gas to the oxygen electrode side. Further, in order for the proton conductive solid polymer membrane to exhibit high proton conductivity, it is necessary that the membrane be sufficiently humidified, and therefore, the oxidizing gas and the fuel gas are sufficiently humidified and supplied. To be done. It is necessary to diffuse these humidified gases evenly from the gas flow path side to the proton conductive solid polymer membrane on both the fuel electrode side and the oxygen electrode side. in this way,
In the fuel cell electrode, the humidified gas is evenly and uniformly supplied to the proton conductive solid polymer membrane,
It is required to satisfy the different characteristics of efficiently discharging the generated water to the gas flow path side.
【０００４】従来、この特性を両立する方法として、特
開平９−２４５８００号公報、特開２０００−２５１９
０４号公報に示されているように、電極層の部分がプロ
トン伝導性固体高分子膜側とガス流路側に撥水部を設
け、その間を親水部とすることにより、燃料電池での電
気化学反応により生じた生成水の一部を撥水部により弾
いてプロトン伝導性固体高分子膜に押し戻すことによ
り、プロトン伝導性固体高分子膜が乾燥することを防止
したり、流路形成部材の流路形成部分にかかわる部分と
それ以外の部分とで電極層を形成するガス拡散層のガス
透過率を変更させることにより、電極層を形成し燃料電
池反応を生ぜしめる触媒層への反応ガスの拡散性を均一
化させて高い発電効率を得るようにしている。Conventionally, as a method for satisfying both of these characteristics, Japanese Patent Laid-Open Nos. 9-245800 and 2000-2519.
As disclosed in Japanese Patent Publication No. 04-04, the electrode layer portion is provided with a water repellent portion on the proton conductive solid polymer membrane side and the gas flow channel side, and a hydrophilic portion is provided between them, thereby making electrochemical in a fuel cell. The water-repellent part repels a part of the generated water generated by the reaction and pushes it back to the proton-conducting solid polymer membrane to prevent the proton-conducting solid polymer membrane from drying or to prevent the flow of the flow path forming member from flowing. Diffusion of the reaction gas into the catalyst layer that forms the electrode layer and causes the fuel cell reaction by changing the gas permeability of the gas diffusion layer that forms the electrode layer between the portion related to the passage forming portion and the other portion To achieve high power generation efficiency.
【０００５】[0005]
【発明が解決しようとする課題】しかしながら、特開平
９−２４５８００号公報は、電極層の部分がプロトン伝
導性固体高分子膜側とガス流路側に撥水部を設け、その
間を親水部とし燃料電池反応により生じた生成水の一部
を撥水部から弾いてプロトン伝導性固体高分子膜に押し
戻すことにより、プロトン伝導性固体高分子膜が乾燥す
ることを防止する方法であり、加湿されたガスが流れる
流路部分とそれ以外の部分について同様な処理を行って
いる。このため、ガスに含まれる加湿の水分や燃料電池
反応により生成された生成水は電極部分の平面方向で均
一にならずに、ガス流路部分にのみ多くなってしまい、
プロトン伝導性固体高分子膜に水分が均一に供されな
い。However, Japanese Patent Laid-Open No. 9-245800 discloses that the electrode layer is provided with a water repellent portion on the side of the proton conductive solid polymer membrane and the side of the gas flow path, and a hydrophilic portion is provided between them. This is a method of preventing the proton-conducting solid polymer membrane from drying by repelling part of the water produced by the battery reaction from the water repellent part and pushing it back to the proton-conducting solid polymer membrane. The same process is performed on the flow path part through which the gas flows and other parts. For this reason, the humidified water contained in the gas and the generated water generated by the fuel cell reaction are not uniform in the plane direction of the electrode portion, and are increased only in the gas flow passage portion,
Water is not uniformly supplied to the proton conductive solid polymer membrane.
【０００６】また、特開２０００−２５１９０４号公報
においては、流路形成部材の流路形成部分にかかわる部
分とそれ以外の部分とで電極層を形成するガス拡散層の
ガス透過率を変更させることにより、電極層を形成し燃
料電池反応を生じせしめる触媒層への反応ガスの拡散性
を均一化をはかっている。しかしながら、ガス透過率は
変更させているが親水処理ないしは撥水処理については
特に差を設けていない。このため、加湿されているガス
がガス拡散層部分を通過する途中においてガス拡散層の
表面に水分が付着してしまい十分にプロトン伝導性固体
高分子膜に水分が供給されないという問題点があった。Further, in Japanese Patent Laid-Open No. 2000-251904, the gas permeability of the gas diffusion layer forming the electrode layer is changed between the portion related to the flow passage forming portion of the flow passage forming member and the other portion. Thus, the diffusivity of the reaction gas to the catalyst layer that forms the electrode layer and causes the fuel cell reaction is made uniform. However, although the gas permeability is changed, there is no particular difference in hydrophilic treatment or water repellent treatment. For this reason, there is a problem in that the humidified gas adheres to the surface of the gas diffusion layer while passing through the gas diffusion layer portion, and the moisture is not sufficiently supplied to the proton conductive solid polymer membrane. .
【０００７】本発明は、このような課題に鑑み、加湿さ
れたガス中の加湿水や電気化学反応により生成する水を
電極層中に均一に分布させることが行える燃料電池を提
案する。In view of the above problems, the present invention proposes a fuel cell capable of uniformly distributing humidifying water in a humidified gas or water produced by an electrochemical reaction in an electrode layer.
【０００８】[0008]
【課題を解決するための手段】第１の発明は、プロトン
伝導性の固体高分子膜と、この固体高分子膜を狭持する
電極と、この電極と接する面に凹状のガス流路を形成し
たセパレータとを備え、前記ガス流路に燃料ガスまたは
酸化剤ガスを流通させて発電を行う燃料電池において、
前記電極は、前記固体高分子膜側に形成された電極触媒
層と、セパレータ側に形成されたガス拡散層とからな
り、これら電極触媒層とガス拡散層の前記ガス流路と相
対する領域は、撥水性を備え、他の領域は親水性を備え
る。A first aspect of the present invention is to form a proton-conducting solid polymer membrane, an electrode sandwiching the solid polymer membrane, and a concave gas flow path on a surface in contact with the electrode. In a fuel cell that includes a separator and that generates electric power by circulating a fuel gas or an oxidant gas in the gas flow path,
The electrode is composed of an electrode catalyst layer formed on the solid polymer membrane side and a gas diffusion layer formed on the separator side, and a region of the electrode catalyst layer and the gas diffusion layer facing the gas flow path is , Has water repellency, and has hydrophilicity in other regions.
【０００９】第２の発明は、第１の発明において、前記
ガス拡散層は、積層構造を有し、セパレータ側の層は、
撥水性を備えた前記ガス流路と相対する領域と親水性を
備えた他の領域とからなり、固体高分子膜側の層は、す
べての領域が親水性を備えた領域からなる。In a second aspect based on the first aspect, the gas diffusion layer has a laminated structure, and the layer on the separator side comprises:
It is composed of a region facing the gas channel having water repellency and another region having hydrophilicity, and the solid polymer film side layer has all regions having hydrophilicity.
【００１０】第３の発明は、第１の発明において、前記
電極触媒層とガス拡散層の少なくとも一方は、積層構造
を有し、セパレータ側の層は、撥水性を備えた前記ガス
流路と相対する領域と親水性を備えた他の領域とからな
り、固体高分子膜側の層は、すべての領域が親水性を備
えた領域からなる。In a third aspect based on the first aspect, at least one of the electrode catalyst layer and the gas diffusion layer has a laminated structure, and the layer on the separator side is the gas flow path having water repellency. The layer on the side of the solid polymer film is composed of a region having hydrophilicity and the other region having hydrophilicity.
【００１１】第４の発明は、第２の発明において、前記
電極触媒層の全ての領域が、撥水性を備える。In a fourth aspect based on the second aspect, all regions of the electrode catalyst layer have water repellency.
【００１２】第５の発明は、プロトン伝導性の固体高分
子膜と、この固体高分子膜を狭持する電極と、この電極
と接する面に凹状のガス流路を形成したセパレータとを
備え、前記ガス流路に燃料ガスまたは酸化剤ガスを流通
させて発電を行う燃料電池において、前記電極は、前記
固体高分子膜側に形成された電極触媒層と、セパレータ
側に形成されたガス拡散層とからなり、これら電極触媒
層とガス拡散層の前記ガス流路と相対する領域は、前記
ガス流路の入口側ほど撥水性が強く、出口側ほど親水性
が強くなるように前記電極を形成する。A fifth aspect of the present invention comprises a proton conductive solid polymer membrane, an electrode sandwiching the solid polymer membrane, and a separator having a concave gas flow path formed on a surface in contact with the electrode. In a fuel cell in which a fuel gas or an oxidant gas is circulated in the gas flow channel to generate power, the electrodes are an electrode catalyst layer formed on the solid polymer membrane side and a gas diffusion layer formed on the separator side. In the region of the electrode catalyst layer and the gas diffusion layer facing the gas channel, the electrode is formed such that the inlet side of the gas channel has stronger water repellency and the outlet side has stronger hydrophilicity. To do.
【００１３】[0013]
【発明の効果】第１の発明は、燃料電池の電極は、固体
高分子膜側に形成された電極触媒層と、セパレータ側に
形成されたガス拡散層とからなり、これら電極触媒層と
ガス拡散層の前記ガス流路と相対する領域は、撥水性を
備え、他の領域は親水性を備えるよう形成した。According to the first aspect of the present invention, an electrode of a fuel cell comprises an electrode catalyst layer formed on the solid polymer membrane side and a gas diffusion layer formed on the separator side. The region of the diffusion layer facing the gas flow channel was formed to have water repellency, and the other region was formed to have hydrophilicity.
【００１４】このような構成を有する燃料電池において
は、プロトン伝導性高分子膜と電極触媒層との界面で電
気化学反応により生成した水あるいはガス流路を流れる
ガスに含まれる加湿水は、電極部分へ移動する。移動し
た生成水あるいは加湿水は撥水部分でははじかれ、親水
部分に選択的に移動していく。本発明においては、ガス
流路に相対する電極の領域を撥水性を有するように処理
し、それ以外の部分は親水性を有する処理を行ってい
る。このため、ガス流路から流入した加湿水あるいは電
気化学反応で生じた生成水は撥水処理を行った部分で弾
かれ、ガス流路に相対する部分以外の親水領域に移動し
ていく。このため、電極においては平面状での水分の分
布が均一となり固体高分子膜への水分供給および、ガス
流路への水の排出も均一化され、発電性能の向上あるい
は信頼性を向上させることができる。In the fuel cell having such a structure, the water generated by the electrochemical reaction at the interface between the proton conductive polymer membrane and the electrode catalyst layer or the humidification water contained in the gas flowing through the gas flow path is Move to the part. The generated water or humidified water that has moved is repelled at the water repellent portion and selectively moves to the hydrophilic portion. In the present invention, the region of the electrode facing the gas flow path is treated to have water repellency, and the other portions are treated to be hydrophilic. Therefore, the humidifying water flowing in from the gas flow path or the water generated by the electrochemical reaction is repelled at the portion subjected to the water repellent treatment, and moves to the hydrophilic region other than the portion facing the gas flow path. Therefore, in the electrode, the distribution of water in a plane is uniform, and the water supply to the solid polymer membrane and the water discharge to the gas flow path are also made uniform, improving power generation performance or reliability. You can
【００１５】第２の発明においては、電極触媒層とガス
拡散層の少なくとも一方は、積層構造を有し、セパレー
タ側の層は、撥水性を備えた前記ガス流路と相対する領
域と親水性を備えた他の領域とからなり、固体高分子膜
側の層は、すべての領域が親水性を備えた領域からなる
ため、ガスの流路から流入する加湿水は、電極部分の全
体が親水性となっている部分により拡散し、速やかに電
極部分での水分分布の均一化をはかることができる。In the second invention, at least one of the electrode catalyst layer and the gas diffusion layer has a laminated structure, and the layer on the separator side is hydrophilic with a region facing the gas channel having water repellency. Since the entire area of the solid polymer membrane side layer is made of a hydrophilic area, the humidifying water flowing from the gas flow path is made hydrophilic in the entire electrode area. The water is diffused by the active portion, and the moisture distribution in the electrode portion can be promptly made uniform.
【００１６】第４の発明では、電極触媒層の全ての領域
が、撥水性を備えたことにより、プロトン伝導性高分子
膜において生成した生成水も撥水性の部分から、親水性
の部分に移動し、より電極部分での水分分布の均一化を
はかることが可能となる。In the fourth aspect of the invention, since the entire area of the electrode catalyst layer is water repellent, the water produced in the proton conductive polymer membrane also moves from the water repellent portion to the hydrophilic portion. However, it becomes possible to make the water distribution in the electrode portion more uniform.
【００１７】第５の発明では、電極触媒層とガス拡散層
のガス流路と相対する領域は、前記ガス流路の入口側ほ
ど撥水性が強く、出口側ほど親水性が強くなるように前
記電極を形成する。これにより、加湿されたガスはガス
流路の入口部分では、より撥水性の高い電極部分と接触
し、より親水性の高いガス出口方向へと加湿水が移動す
る。このため、ガス流路の入口と出口部分での電極部分
の水分分布が均一化され、プロトン伝導性高分子膜への
水分供給も均一に行われ電性能の向上あるいは信頼性を
向上させることができる。In a fifth aspect of the present invention, the regions of the electrode catalyst layer and the gas diffusion layer that face the gas flow path are made more water repellent on the inlet side of the gas flow path and more hydrophilic on the outlet side. Form electrodes. As a result, the humidified gas comes into contact with the electrode portion having higher water repellency at the inlet portion of the gas flow path, and the humidified water moves toward the gas outlet portion having higher hydrophilicity. Therefore, the water distribution in the electrode part at the inlet and the outlet of the gas flow path is made uniform, and the water is uniformly supplied to the proton conductive polymer membrane, so that the electric performance or reliability can be improved. it can.
【００１８】[0018]
【発明の実施の形態】以下、本発明の燃料電池につい
て、図面を参照しながら説明する。図１は、本発明の一
実施形態を示す燃料電池の発電部の構成を示す断面図で
ある。プロトン伝導性固体高分子電解質膜（以下、高分
子膜という）１を挟んで、その両側に電極触媒層３が、
配置されている。さらにこの電極触媒層３の両外側にガ
ス拡散層４を配置する。電極触媒層３とガス拡散層４と
が燃料電池の電極５を形成する。さらにその外側に燃料
ガスまたは酸化ガスが流通するガス流路６を形成したセ
パレータ板７を配置している。図２は、同様な燃料電池
用電極５の平面を高分子膜側より見た構成を示す図であ
る。ガス流路形成部材であるセパレータ板７には、溝８
が構成され、燃料ガス及び酸化ガスを形成された溝８に
沿って流通可能としている。そのガス流路６を覆う形で
電極５が配置されている。BEST MODE FOR CARRYING OUT THE INVENTION Hereinafter, a fuel cell of the present invention will be described with reference to the drawings. FIG. 1 is a cross-sectional view showing a configuration of a power generation section of a fuel cell showing an embodiment of the present invention. A proton conductive solid polymer electrolyte membrane (hereinafter referred to as polymer membrane) 1 is sandwiched, and electrode catalyst layers 3 are provided on both sides thereof.
It is arranged. Further, gas diffusion layers 4 are arranged on both outer sides of the electrode catalyst layer 3. The electrode catalyst layer 3 and the gas diffusion layer 4 form the electrode 5 of the fuel cell. Further, a separator plate 7 having a gas flow path 6 through which a fuel gas or an oxidizing gas flows is arranged outside thereof. FIG. 2 is a diagram showing a configuration of the same plane of the fuel cell electrode 5 as seen from the polymer membrane side. The groove 8 is formed in the separator plate 7 which is a gas flow path forming member.
Is configured to allow the fuel gas and the oxidizing gas to flow along the formed groove 8. The electrode 5 is arranged so as to cover the gas flow path 6.
【００１９】次に、高分子膜１の両側に配した電極触媒
層３の調製方法について、説明する。粒径が数ミクロン
以下のカーボンブラック粒子に塩化白金酸溶液を用い
て、白金を含浸担持させる。この時に、白金を還元した
状態とするため、還元処理を行う。この時の白金の担持
量は、例えば調整後に５０重量％となるように調製し
た。調製した白金担持カーボンブラック粉末を用いて、
高分子電解質、アルコール溶液、水とを用いて親水性の
カーボンブラックスラリーと、フッ素樹脂粉末の水性デ
ィスバージョン、高分子分解膜、アルコール溶液、水と
を用いて撥水性のカーボンブラックスラリーを調製し
た。この調製した親水性カーボンブラックと撥水性カー
ボンブラックを用いて、高分子膜１の表面に飛沫状にし
て、塗布を行い、電極触媒層３を形成する。この時に、
セパレータ板７の燃料ガス等のガスが流通するガス流路
６と対面する撥水部分（以下、撥水領域３ａという。図
１において斜線部で示す。以下、他の図面においても斜
線部は撥水領域を示す。）には撥水性カーボンブラック
スラリーを塗布し、それ以外の領域（親水領域）３ｂに
ついては親水性カーボンブラックスラリーを塗布するよ
うにする。Next, a method for preparing the electrode catalyst layers 3 arranged on both sides of the polymer membrane 1 will be described. Platinum is impregnated and supported on carbon black particles having a particle size of several microns or less using a chloroplatinic acid solution. At this time, a reduction process is performed to bring the platinum into a reduced state. The amount of platinum supported at this time was adjusted so as to be 50% by weight after adjustment. Using the prepared platinum-supporting carbon black powder,
A hydrophilic carbon black slurry was prepared using a polymer electrolyte, an alcohol solution, and water, and a water-repellent carbon black slurry was prepared using an aqueous dispersion of fluororesin powder, a polymer decomposition film, an alcohol solution, and water. . The prepared hydrophilic carbon black and water-repellent carbon black are applied to the surface of the polymer film 1 in the form of droplets to form the electrode catalyst layer 3. At this time,
A water-repellent portion of the separator plate 7 that faces the gas flow path 6 in which a gas such as a fuel gas flows (hereinafter, referred to as a water-repellent region 3a. The hatched portion is shown in FIG. A water-repellent carbon black slurry is applied to the water region), and a hydrophilic carbon black slurry is applied to the other region (hydrophilic region) 3b.
【００２０】次にガス拡散層４の撥水処理について説明
する。厚さ４００ミクロンのカーボン不織布の電極触媒
層３側に、撥水処理を施したいセパレータ板７のガス流
路６に面する部分を切り欠いたパターンをかぶせ、電極
触媒層３側からフッ素樹脂粉末の水性ディスバージョン
を飛沫状にして塗布する。この時に、フッ素樹脂粉末の
水性ディスバージョンを塗布するのと同時に、ガス流路
６側から真空ポンプにより空気を吸い込んでカーボン不
織布の断面方向へのフッ素樹脂粉末の拡散させて、断面
方向について撥水剤が均一に行き渡るようにしてもよ
い。このようにしてフッ素樹脂粉末を付着させた、カー
ボン不織布を乾燥後、４００℃で熱処理してガス拡散層
４を形成する。Next, the water repellent treatment of the gas diffusion layer 4 will be described. On the side of the electrode catalyst layer 3 of the carbon non-woven fabric having a thickness of 400 microns, a part of the separator plate 7 to be subjected to the water repellent treatment facing the gas flow path 6 is covered with a cutout pattern, and the electrode catalyst layer 3 side is covered with fluororesin powder. Apply the water-based dispersant in the form of droplets. At this time, at the same time as the aqueous dispersion of the fluororesin powder is applied, air is sucked in from the gas flow path 6 side by the vacuum pump to diffuse the fluororesin powder in the cross-sectional direction of the carbon non-woven fabric so that the cross-sectional direction becomes water repellent. The agent may be evenly distributed. Thus, the carbon nonwoven fabric to which the fluororesin powder is attached is dried and then heat-treated at 400 ° C. to form the gas diffusion layer 4.
【００２１】このようにして調製した、ガス拡散層４
を、高分子膜１にカーボンブラックを塗布して形成され
た電極触媒層３にのせ、温度１４０℃、圧力１００ｋｇ
ｆ／ｃｍ2で９０秒間ホットプレスして、接合一体化を
はかる。電極触媒層３とガス拡散層４とを接合一体化し
た燃料電池用の電極５を用い、その両側からガス流路６
を有するセパレータ板７で挟み、燃料電池の単電池を得
た。The gas diffusion layer 4 thus prepared
Is placed on the electrode catalyst layer 3 formed by coating the polymer film 1 with carbon black, and the temperature is 140 ° C. and the pressure is 100 kg.
Hot pressing is performed at f / cm 2 for 90 seconds to achieve joint integration. A fuel cell electrode 5 in which an electrode catalyst layer 3 and a gas diffusion layer 4 are joined and integrated is used, and a gas flow path 6 is provided from both sides thereof.
It was sandwiched between the separator plates 7 having a to obtain a unit cell of a fuel cell.
【００２２】このようにして形成された単電池の特性評
価を行った。特性評価は、電流密度を０から１．２Ａ／
ｃｍ2まで流し、その時の電圧変化を測定して、図３に
示す燃料電池単セルのＩ−Ｖ特性を得た。電極触媒層の
カーボンブラックスラリーとして、撥水性のカーボンブ
ラックスラリーのみを用いたもの（図３中の比較例１）
と比較すると、電流密度が高くなるほど本発明の単セル
の出力電圧（実施例１で示す）が比較例１より向上して
いることが明らかである。The characteristics of the unit cell thus formed were evaluated. Characteristic evaluation is that the current density is 0 to 1.2 A /
After flowing up to cm 2 , the voltage change at that time was measured, and the IV characteristic of the fuel cell single cell shown in FIG. 3 was obtained. As the carbon black slurry for the electrode catalyst layer, only the water repellent carbon black slurry was used (Comparative Example 1 in FIG. 3).
It is clear that the output voltage (shown in Example 1) of the single cell of the present invention is higher than that of Comparative Example 1 as the current density is increased.
【００２３】次に作用について説明する。Next, the operation will be described.
【００２４】高分子膜１と電極触媒層３との界面で電気
化学反応により生成した水あるいはガス流路６を流れる
ガス（燃料ガスまたは酸化ガス）に含まれる加湿水は、
電極９内へ移動する。移動した生成水あるいは加湿水は
電極触媒層３あるいはガス拡散層４の撥水領域３ａで弾
かれ、親水領域３ｂに選択的に移動、拡散していく。The water generated by the electrochemical reaction at the interface between the polymer membrane 1 and the electrode catalyst layer 3 or the humidifying water contained in the gas (fuel gas or oxidizing gas) flowing through the gas flow path 6 is
Move into the electrode 9. The produced water or humidified water that has moved is repelled by the water repellent region 3a of the electrode catalyst layer 3 or the gas diffusion layer 4, and selectively moves and diffuses into the hydrophilic region 3b.
【００２５】本発明においては、セパレータ板７のガス
流路６に対面する領域３ａに撥水性を有するように処理
し、それ以外の領域３ｂは親水性を有する処理を行って
いる。したがって、ガス流路６から流入した加湿水ある
いは電気化学反応により生成した生成水は、撥水処理を
施した領域３ａで弾かれ、ガス流路６に対面する部分以
外の親水領域３ｂに移動していく。このため、電極部分
においては平面状での水分の分布が均一となり高分子膜
１への水分供給および、ガス流路６への水の排出も均一
化され、燃料電池の発電性能の向上あるいは信頼性を向
上させることができる。In the present invention, the region 3a of the separator plate 7 facing the gas flow path 6 is treated to have water repellency, and the other region 3b is treated to be hydrophilic. Therefore, the humidifying water flowing in from the gas flow path 6 or the generated water generated by the electrochemical reaction is repelled in the water-repellent-treated area 3 a and moves to the hydrophilic area 3 b other than the portion facing the gas flow path 6. To go. Therefore, in the electrode portion, the distribution of water in a plane is uniform, and the water supply to the polymer membrane 1 and the water discharge to the gas flow path 6 are made uniform, so that the power generation performance of the fuel cell is improved or the reliability is improved. It is possible to improve the sex.
【００２６】図４は第２の実施形態を示す構成図であ
り、図１に示す第１の実施形態の構成に対して、ガス拡
散層４を２層構造にし、ガス流路６側のガス拡散層４Ａ
は第１の実施形態のガス拡散層４と同様の構成としつ
つ、高分子膜１側のガス拡散層４Ｂは、その全面を親水
性カーボン不織布を用いて親水性とした構成を有するよ
うにしたものである。FIG. 4 is a configuration diagram showing a second embodiment. In the configuration of the first embodiment shown in FIG. 1, the gas diffusion layer 4 has a two-layer structure and the gas on the gas flow path 6 side is formed. Diffusion layer 4A
While having the same structure as the gas diffusion layer 4 of the first embodiment, the gas diffusion layer 4B on the side of the polymer film 1 has a structure in which the entire surface is made hydrophilic by using a hydrophilic carbon nonwoven fabric. It is a thing.
【００２７】したがって、ガス流路６側の電極部分に対
峙して撥水性、それ以外で親水性を有するガス拡散層４
Ａを形成させ、さらにその高分子膜１側に全面を親水性
としたガス拡散層４Ｂを設けているため、ガス流路６か
ら流入する加湿水は、電極部分の全体が親水性となって
いるガス拡散層４Ｂにより拡散し、速やかに電極部分で
の水分分布の均一化をはかることができる。Therefore, the gas diffusion layer 4 is water-repellent when facing the electrode portion on the gas flow path 6 side and has hydrophilicity at other portions.
Since the gas diffusion layer 4B having A formed thereon and having the entire surface made hydrophilic is provided on the side of the polymer film 1, humidifying water flowing from the gas flow path 6 becomes hydrophilic in the entire electrode portion. The gas is diffused by the existing gas diffusion layer 4B, and the moisture distribution in the electrode portion can be promptly made uniform.
【００２８】図５は第３の実施形態の構成を示す図であ
り、本実施形態は、第２の実施形態に対して、電極触媒
層３を２層とした点が異なる。すなわち、２層の電極触
媒層のうち、ガス拡散層４側の電極触媒層３Ａの構成
は、第２の実施形態の電極触媒層３と同様であり、高分
子膜１側の電極触媒層３Ｂは、その全面を親水性カーボ
ンブラックを塗布して親水性として形成されている。FIG. 5 is a diagram showing the structure of the third embodiment. This embodiment differs from the second embodiment in that the electrode catalyst layer 3 is two layers. That is, of the two electrode catalyst layers, the structure of the electrode catalyst layer 3A on the gas diffusion layer 4 side is the same as that of the electrode catalyst layer 3 of the second embodiment, and the electrode catalyst layer 3B on the polymer membrane 1 side is the same. Is coated with hydrophilic carbon black so as to be hydrophilic.
【００２９】したがって、第２の実施形態に比して、よ
り一層速やかに電極部分での水分分布の均一化をはかる
ことができる。Therefore, as compared with the second embodiment, the moisture distribution in the electrode portion can be made more uniform.
【００３０】図６は、第４の実施形態の構成を説明する
図であり、本実施形態は、第２の実施形態に対して、電
極触媒層３の構成を変更したものである。すなわち、電
極触媒層３を撥水性カーボンスラリーによってのみ形成
したものである。FIG. 6 is a diagram for explaining the configuration of the fourth embodiment, and this embodiment is the one in which the configuration of the electrode catalyst layer 3 is changed from that of the second embodiment. That is, the electrode catalyst layer 3 is formed only by the water repellent carbon slurry.
【００３１】前記のガス拡散層の２層構造に加えて、高
分子膜１側に全面が撥水性となる電極触媒層３を設ける
ことにより、高分子膜１において生成した生成水も撥水
性の領域から親水性の領域に移動し、より電極部分での
水分布の均一化をはかることが可能となる。In addition to the two-layer structure of the gas diffusion layer described above, by providing the electrode catalyst layer 3 on the side of the polymer film 1 which is entirely water repellent, the water produced in the polymer film 1 is also water repellent. By moving from the region to the hydrophilic region, it becomes possible to make the water distribution in the electrode portion more uniform.
【００３２】図７は、第１から第４の実施形態の構成を
用いて、燃料電池内のガス流路６に対面する電極触媒層
３とガス拡散層４の撥水性を有する領域と親水性を有す
る領域の比率をガスの入口側ほど、撥水性を有する領域
の割合を高く（例えば、発生性領域７：親水性領域
３）、下流側ほど親水性を有する領域の割合を高くする
ように（図７では中央部で５：５、下流部で３：７）構
成したものを説明する図である（第５の実施形態）。電
極触媒層３での撥水性と親水性の割合の調整は、撥水性
カーボンブラックスラリーと親水性カーボンブラックス
ラリーとの高分子膜１への塗布量を制御することで可能
であり、一方、ガス拡散層４での撥水性と親水性の割合
の調整は、撥水剤であるフッ素樹脂粉末の水性ディスパ
ージョンの塗布量を制御することで可能である。FIG. 7 is a view showing the hydrophilicity of the electrode catalyst layer 3 and the gas diffusion layer 4 which face the gas flow path 6 in the fuel cell and the water-repellent region, which is obtained by using the constitutions of the first to fourth embodiments. As for the ratio of the region having the above, the ratio of the region having water repellency is made higher toward the gas inlet side (for example, the generating region 7: hydrophilic region 3), and the ratio of the region having hydrophilicity is made higher toward the downstream side. (In FIG. 7, 5: 5 in the central part and 3: 7 in the downstream part) FIG. 9 is a diagram for explaining the structure (fifth embodiment). The ratio of water repellency and hydrophilicity in the electrode catalyst layer 3 can be adjusted by controlling the coating amounts of the water repellent carbon black slurry and the hydrophilic carbon black slurry on the polymer film 1, while the gas The ratio of water repellency and hydrophilicity in the diffusion layer 4 can be adjusted by controlling the coating amount of the aqueous dispersion of the fluororesin powder that is the water repellent.
【００３３】したがって、ガス流路６の入口方向から出
口方向に向けて電極部分でガス流路６に対面する部分で
の撥水性／親水性の比率を減少させることにより、加湿
されたガスは、ガス流路６の入口部分では、より撥水性
の高い電極部分と接触し、より親水性の高いガス出口方
向へと加湿水が移動する。このため、ガス流路の入口と
出口部分での電極部分の水分分布が均一化され、高分子
膜１への水分供給も均一に行われ発電性能の向上あるい
は信頼性を向上させることができる。Therefore, by reducing the water repellency / hydrophilicity ratio in the portion of the electrode portion facing the gas flow passage 6 from the inlet direction to the outlet direction of the gas flow passage 6, the humidified gas is At the inlet portion of the gas flow path 6, the humidifying water contacts with the electrode portion having higher water repellency and moves toward the gas outlet portion having higher hydrophilicity. Therefore, the water distribution in the electrode portion at the inlet and the outlet of the gas flow path is made uniform, and the water supply to the polymer film 1 is also made uniform, so that power generation performance or reliability can be improved.
【００３４】なお、これまでの実施形態において、ガス
拡散層４を形成するためにカーボン不織布を用いたが、
これに限られず、例えば、カーボンペーパ（第６の実施
形態）やカーボン繊維（第７の実施形態）を用いて調製
することも可能である。Although the carbon nonwoven fabric is used to form the gas diffusion layer 4 in the above embodiments,
The present invention is not limited to this, and it is also possible to prepare using, for example, carbon paper (sixth embodiment) or carbon fiber (seventh embodiment).
【００３５】カーボン繊維からカーボン不織布を調製す
る場合には、撥水性のカーボン繊維としてのフッ素樹脂
粉末の水性ディスパージョンを付着させたカーボン繊維
と、親水性のカーボン繊維としてフッ素樹脂粉末の水性
ディスパージョンを付着させないカーボン樹脂とを、そ
れぞれ二次平面内で無作為に配向させてカーボン不織布
を形成する。When a carbon non-woven fabric is prepared from carbon fibers, carbon fibers to which an aqueous dispersion of fluororesin powder as water-repellent carbon fibers is attached and aqueous dispersion of fluororesin powder as hydrophilic carbon fibers are used. And a carbon resin that does not adhere to each other are randomly oriented in a quadratic plane to form a carbon nonwoven fabric.
【００３６】二次平面内で無作為に配向させる方法とし
ては、液体の媒体中にカーボン繊維を分散させて製造す
る湿式法や、空気中でカーボン繊維を分散させて降り積
もらせる乾式法を用いることができる。そして、撥水領
域と親水領域との割合は、撥水性のカーボン繊維と親水
性のカーボン繊維との比率を調整することで制御可能で
ある。このようにして、電気化学反応で生成された水や
ガス中の加湿水の燃料電池内での分布を均一にすること
ができ、発電効率を向上することができる。As a method of randomly orienting in a quadratic plane, a wet method in which carbon fibers are dispersed in a liquid medium for production, or a dry method in which carbon fibers are dispersed in air and piled up is used. be able to. The ratio between the water repellent region and the hydrophilic region can be controlled by adjusting the ratio between the water repellent carbon fiber and the hydrophilic carbon fiber. In this way, it is possible to make the distribution of the humidified water in the fuel cell generated by the electrochemical reaction in the fuel cell uniform, and to improve the power generation efficiency.
【００３７】これまで説明してきた実施形態毎の出力特
性を測定した結果を表１に示す。この結果の評価条件
は、電極の面積が２５ｃｍ2である単セルを用いてセル
温度８０℃、水素ガスおよび酸化ガスとして空気を用い
た。加湿条件は、水素ガス、空気ガス側とも１００％と
した。Table 1 shows the results of measuring the output characteristics for each of the embodiments described above. As the evaluation conditions for this result, a single cell having an electrode area of 25 cm 2 was used, a cell temperature was 80 ° C., and air was used as a hydrogen gas and an oxidizing gas. Humidification conditions were 100% for both hydrogen gas and air gas sides.
【００３８】[0038]
【表１】
本発明は、上記した実施形態に限定されるものではな
く、本発明の技術的思想の範囲内でさまざまな変更がな
しうることは明白である。[Table 1] The present invention is not limited to the above-described embodiment, and it is obvious that various modifications can be made within the scope of the technical idea of the present invention.
【図１】本発明の一実施形態を示す燃料電池の発電部の
構成を示す断面図である。FIG. 1 is a cross-sectional view showing a configuration of a power generation unit of a fuel cell showing an embodiment of the present invention.
【図２】燃料電池用電極の平面を高分子膜側より見た構
成を示す図である。FIG. 2 is a diagram showing a configuration of a plane of a fuel cell electrode as seen from a polymer membrane side.
【図３】燃料電池単セルのＩ−Ｖ特性図である。FIG. 3 is an IV characteristic diagram of a fuel cell single cell.
【図４】第２の実施形態の図１に対応する部分を示す構
成図である。FIG. 4 is a configuration diagram showing a portion corresponding to FIG. 1 of a second embodiment.
【図５】第３の実施形態の図１に対応する部分を示す構
成図である。FIG. 5 is a configuration diagram showing a portion corresponding to FIG. 1 of a third embodiment.
【図６】第４の実施形態の図１に対応する部分を示す構
成図である。FIG. 6 is a configuration diagram showing a portion corresponding to FIG. 1 of a fourth embodiment.
【図７】第５の実施形態の図２に対応する部分を示す構
成図である。FIG. 7 is a configuration diagram showing a portion corresponding to FIG. 2 of a fifth embodiment.
１ 高分子膜 ３ 電極触媒層 ４ ガス拡散層 ５ 電極 ６ ガス流路 ７ セパレータ板 ８ 溝 1 polymer membrane 3 Electrode catalyst layer 4 Gas diffusion layer 5 electrodes 6 gas flow paths 7 Separator plate 8 grooves
Claims (5)
ータとを備え、 前記ガス流路に燃料ガスまたは酸化剤ガスを流通させて
発電を行う燃料電池において、 前記電極は、前記固体高分子膜側に形成された電極触媒
層と、セパレータ側に形成されたガス拡散層とからな
り、 これら電極触媒層とガス拡散層の前記ガス流路と相対す
る領域は、撥水性を備え、他の領域は親水性を備えたこ
とを特徴とする燃料電池。1. A solid polymer membrane having proton conductivity, an electrode sandwiching the solid polymer membrane, and a separator having a concave gas passage formed on a surface in contact with the electrode, the gas passage In a fuel cell in which a fuel gas or an oxidant gas is circulated to generate electricity, the electrode includes an electrode catalyst layer formed on the solid polymer membrane side and a gas diffusion layer formed on the separator side, The fuel cell is characterized in that the regions of the electrode catalyst layer and the gas diffusion layer facing the gas flow path have water repellency and the other regions have hydrophilicity.
レータ側の層は、撥水性を備えた前記ガス流路と相対す
る領域と親水性を備えた他の領域とからなり、固体高分
子膜側の層は、すべての領域が親水性を備えた領域から
なることを特徴とする請求項１に記載の燃料電池。2. The gas diffusion layer has a laminated structure, and the layer on the separator side is composed of a region facing the gas channel having water repellency and another region having hydrophilicity, and is solid. The fuel cell according to claim 1, wherein the layer on the polymer membrane side is formed of a region having hydrophilicity in all regions.
一方は、積層構造を有し、セパレータ側の層は、撥水性
を備えた前記ガス流路と相対する領域と親水性を備えた
他の領域とからなり、固体高分子膜側の層は、すべての
領域が親水性を備えた領域からなることを特徴とする請
求項１に記載の燃料電池。3. At least one of the electrode catalyst layer and the gas diffusion layer has a laminated structure, and the layer on the separator side has hydrophilicity with a region facing the gas flow channel having water repellency. 2. The fuel cell according to claim 1, wherein the layer on the side of the solid polymer membrane is composed of a region having hydrophilicity.
備えたことを特徴とする請求項２に記載の燃料電池。4. The fuel cell according to claim 2, wherein all regions of the electrode catalyst layer have water repellency.
ータとを備え、 前記ガス流路に燃料ガスまたは酸化剤ガスを流通させて
発電を行う燃料電池において、 前記電極は、前記固体高分子膜側に形成された電極触媒
層と、セパレータ側に形成されたガス拡散層とからな
り、 これら電極触媒層とガス拡散層の前記ガス流路と相対す
る領域は、前記ガス流路の入口側ほど撥水性が強く、出
口側ほど親水性が強くなるように前記電極を形成するこ
とを特徴とする燃料電池。5. A gas flow path comprising a proton conductive solid polymer membrane, an electrode sandwiching the solid polymer membrane, and a separator having a concave gas flow path formed on a surface in contact with the electrode. In a fuel cell in which a fuel gas or an oxidant gas is circulated to generate electricity, the electrode includes an electrode catalyst layer formed on the solid polymer membrane side and a gas diffusion layer formed on the separator side, In the areas of the electrode catalyst layer and the gas diffusion layer facing the gas flow channel, the electrodes are formed such that the inlet side of the gas flow channel has stronger water repellency and the outlet side has stronger hydrophilicity. And a fuel cell.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2001399889A JP3843838B2 (en) | 2001-12-28 | 2001-12-28 | Fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2001399889A JP3843838B2 (en) | 2001-12-28 | 2001-12-28 | Fuel cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JP2003197203A true JP2003197203A (en) | 2003-07-11 |
| JP3843838B2 JP3843838B2 (en) | 2006-11-08 |
Family
ID=27604734
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP2001399889A Expired - Fee Related JP3843838B2 (en) | 2001-12-28 | 2001-12-28 | Fuel cell |
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| Country | Link |
|---|---|
| JP (1) | JP3843838B2 (en) |
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| JP2005174768A (en) * | 2003-12-11 | 2005-06-30 | Equos Research Co Ltd | Membrane electrode assembly, method for producing the same, and method for using the same |
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