JP3922063B2 - Porous metal and solid polymer fuel cell using the same - Google Patents
Porous metal and solid polymer fuel cell using the same Download PDFInfo
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- JP3922063B2 JP3922063B2 JP2002082484A JP2002082484A JP3922063B2 JP 3922063 B2 JP3922063 B2 JP 3922063B2 JP 2002082484 A JP2002082484 A JP 2002082484A JP 2002082484 A JP2002082484 A JP 2002082484A JP 3922063 B2 JP3922063 B2 JP 3922063B2
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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
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Description
【0001】
【発明の属する技術分野】
この発明は、電極材料として利用する金属多孔体と、それをガス拡散電極として用いた固体高分子型燃料電池に関する。
【0002】
【従来の技術】
電気化学的な発電装置の一種である固体高分子型燃料電池のガス拡散電極として発泡金属を用いる技術が特許第3211378号公報に示され、また、特開平8−138680号には、選択的(スポット的)に低気孔率部を設けた金属多孔体が開示されている。
【0003】
さらに、金属繊維と有機繊維の混毛織布や混毛不織布をガス拡散電極として用いることが特許第3242736号公報に示されている。
【0004】
【発明が解決しようとする課題】
特許第3211378号公報の発泡金属は、ガス拡散性を良くするために気孔率を高めると接触相手部材との間の接触抵抗が大きくなり、一方、その接触抵抗を下げるために気孔率を下げると、ガスの流路抵抗が上昇し、どちらにしても電池の出力低下を招く。
【0005】
また、気孔率を低下させずに接触抵抗を下げる方法として、接触面を化学的に安定した金や白金で覆う方法があるが、これはコストアップを招く。
【0006】
特開平8−138680号公報の金属多孔体は、端子を溶接する部位の強度を高める目的でその部位を低気孔率にしているが、低気孔率部をスポット的に配置するだけでは、接触抵抗低減に対する寄与度が低い。
【0007】
さらに、特許第3242736号の混毛織布や混毛不織布は、繊維の集合体であり、厚み方向に何本もの繊維が積層して電気通路を構成している。そのため、各繊維間の接触抵抗が合算されて厚み方向の電気抵抗が大きくなる。
【0008】
また、これ等は気孔率が小さい(ガスの流れを遮断する面積が大きい)ため、ガスの流路抵抗が大きく、ガスの拡散性や触媒反応層の各部の均一反応性に問題が生じて燃料電池の総合効率を低下させる。
【0009】
そこで、この発明は、金属多孔体の気孔率低下を極力抑えて接触相手部材との間の接触抵抗を貴金属などを使わずに低下させることを課題としている。
【0010】
【課題を解決するための手段】
上記の課題を解決するため、この発明においては、固体高分子型燃料電池のガス拡散電極用として以下のように構成された金属多孔体、即ち、Fe−Crを主成分とした合金、又はそれに更に、Ni、Mo、Cu、B、Al、Si、Tiの中から選ばれた少なくとも1種の元素を10%未満の割合で添加した合金で形成され、平均孔径が50μm〜1mmの3次元網目構造を有し、一表面又は両表面部に低気孔率層が設けられ、その低気孔率層を除く箇所の気孔率が85%以上、99%以下であり、低気孔率層の気孔率が前記低気孔率層を除く箇所の気孔率よりも少なくとも2%低くなっている金属多孔体を提供する。
【0011】
また、この金属多孔体を、高分子電解質膜の両面部にガス拡散電極として配置した固体高分子型燃料電池を併せて提供する。
【0014】
【作用】
この発明の金属多孔体は、一面又は両面に低気孔率層を有しており、その低気孔率層が相手部材(電極触媒層やセパレータ)と接触するので、相手部材との接触面積が増加し、高価な貴金属等を使わなくても接触抵抗を下げることができる。
【0015】
また、表層部を除く部分は、高気孔率を確保でき、ガス透過性能を高めて触媒反応を促進することができる。
【0016】
従って、この金属多孔体を高分子電解質膜の両面部にガス拡散電極として配置すれば、ガス透過性と電気伝導性に優れる金属多孔体の特性が生かされ、それに表面部の気孔率低下による電極触媒層或いはセパレータとの接触抵抗低減の効果がプラスされて燃料電池の出力向上が可能になる。
【0017】
ここで、金属多孔体の平均孔径を50μm〜1mmの範囲に限定したのは、その平均孔径が50μm未満では流路抵抗が大きくてガスの均一拡散が望み難くなり、一方、その平均孔径が1mmを越えると、相手部材との接触点が減少して接触抵抗が大きくなるからである。
【0018】
また、中心部と表面の低気孔率層の気孔率差が小さ過ぎると、接触抵抗低減の効果が十分に発揮されないので、その差は少なくとも2%とした。
【0019】
なお、金属多孔体の気孔率を下げ過ぎると、ガスの透過性や電気化学反応により電極触媒層で発生する水の排出性が悪化する。この不具合を避けるために、表面の低気孔率層を除く部位の気孔率を85%以上にするのがよい。また、一方で金属多孔体の弾力性を確保するために、低気孔率層を除く部位の気孔率は99%以下にするのがよい。
【0020】
このほか、金属多孔体は、電極用途での耐久性を考えて強度及び耐食性に優れる金属で形成するのが望ましい。
【0021】
Fe−Cr又はNi−Crを主体とした炭素を含む合金や、それに更にNi、Mo、Cu、B、Al、Si、Tiの中から選ばれた少なくとも1種の元素を添加した合金で形成される金属多孔体は、硫酸等の腐食環境において溶出が抑えられ、電池用電極としての適正が高まる。
【0022】
【発明の実施の形態】
図1及び図2に、この発明の金属多孔体の断面を模式化して示す。これ等の金属多孔体1は、平均孔径が50μm以上、1mm以下の3次元網目構造を有しており、シート状の外観をなす。
【0023】
この金属多孔体1は、高気孔率層2と低気孔率層3が積層された構造になっている。低気孔率層3は、図1に示すように一表面部又は図2に示すように両表面部に設けられ、中心部を含めた残りの部位が高気孔率層2になっている。
【0024】
高気孔率層2の気孔率は、既に述べたように85%以上、99%以下が好ましい。低気孔率層3の気孔率は、高気孔率層の気孔率に比べて2%以上低くする。
【0025】
気孔率が厚み方向途中で変化したこの金属多孔体1は、高気孔率層2と低気孔率層3が一体になったものが両層間での接触抵抗を無くせて好ましい。そのような構造の金属多孔体1は、気孔率の異なる金属多孔体を積層して焼結一体化する方法や、金属多孔体の表面に金属と樹脂の混合スラリーを塗布してこれを焼結し、表層部の骨格を太らせる方法などで製造することができる。
【0026】
金属多孔体は、発泡樹脂等を出発材にして特開昭57−174484号公報に示されるメッキ法や、特公昭38−17554号公報に示される塗着スラリーの焼結法などで製造され、従って、気孔率の異なる発泡樹脂等を積層したものを出発材にし、これにメッキした後、出発材を焼却除去し、必要に応じて後工程で金属の拡散処理を行って合金化する方法や、積層出発材に金属粉と樹脂のスラリーを塗布して焼結する方法でもこの発明の金属多孔体を製造し得るが、上述した方法の方が量産品を利用でき、生産性に勝る。
【0027】
金属多孔体1は、本出願人が特願2000−140037号(特開2001−226723号)で提案しているものなどが強度、耐食性、耐熱性に優れていて好ましい。特開2001−226723号の金属多孔体は、主としてFe及びCrを含む合金から成り、組織中にCr炭化物及び/又はFeCr炭化物が均一分散した骨格を有する。また、カーボン含有量は0.1%以上、3.5%以下が好ましいとしており、必要に応じてNi、Cu、Mo、Al、P、B、Si、Tiの中から選ばれた少なくとも1種の元素を更に添加したものもある。
【0028】
カーボンを含むNi−Cr合金(これは上記公報には開示されていない)も強度及び耐食性に優れており、金属多孔体1の材料として使用できる。
【0029】
ここで、カーボンを含むことにより金属多孔体の強度が向上するため、触媒電極層及びセパレータと積層加圧されたときに十分な反力があるため接触抵抗の経時劣化が殆どなく、燃料電池の耐久劣化が小さくなる。また、Cr炭化物相として金属多孔体中に均一分散されるため、不動態膜が形成されても導電性のある炭化物相が接触抵抗の低減にも寄与する。
【0030】
以下に、より詳細な実施例を挙げる。
−実施例1−
表1に示す金属多孔体(一面を低気孔率にし、層2、3を一体化した図1の構造)を製作し、その多孔体の接触抵抗を測定した。結果を表2に示す。
【0031】
接触抵抗は、金属多孔体の両面(低気孔率層の表面と高気孔率層の表面)を表面の清浄なCu電極板に1MPaの圧力で押し付けて測定した。
【0032】
【表1】
【0033】
【表2】
【0034】
−実施例2−
高分子電解質膜としてナフィオン(デュポン社製、膜厚150μm)を用い、その膜の両面に白金触媒を担持したカーボン多孔質体を接合したものを用意してそれを挟むように両側に表1の金属多孔体を配置し、さらに、その金属多孔体の外側にカーボン電極を重ね合わせて固体高分子型燃料電池を作成した。また、比較例として、表1のNo.3の金属多孔体を低気孔率層を設けずに高気孔率層のみとしたものを用いて同様の燃料電池を作製した。なお、この実施例においては、表1の金属多孔体として、低気孔率層を両面に設けたものを適用した。
【0035】
これ等の試作品の性能評価として、電流密度10mA/cm2 時のセル電圧を測定した。結果を表3に示す。
【0036】
【表3】
【0037】
表3から判るように、この発明の金属多孔体を用いると、ガス拡散電極の接触抵抗が低減されて電池の出力が高まる。
【0038】
【発明の効果】
以上述べたように、この発明の金属多孔体は、表層部の気孔率を下げてその他の部位の気孔率を高くするので、ガスの透過性、電極触媒層で生じた水の排出性を悪化させずに、また、高価な貴金属等を使わずに接触抵抗を下げることができ、燃料電池の出力を経済的に高めることを可能ならしめる。
【0039】
なお、金属多孔体の材質を特定したものは、腐食環境においても溶出を抑えて耐久性を高めることができる。
【0040】
また、低気孔率部を除く部位の気孔率を85%以上、99%以下にしたものは、十分なガス透過性と十分な弾力性を確保できる。
【0041】
従って、この発明の金属多孔体をガス拡散電極として用いた固体高分子型燃料電池は、コスト増を招かずに出力特性を高めることができる。
【図面の簡単な説明】
【図1】この発明の金属多孔体の一例を示す断面の模式図
【図2】他の例の断面の模式図
【符号の説明】
1 金属多孔体
2 高気孔率層
3 低気孔率層[0001]
BACKGROUND OF THE INVENTION
This invention includes a metal porous body for use as an electrode materials, a solid polymer electrolyte fuel cell using the same as a gas diffusion electrode.
[0002]
[Prior art]
Japanese Patent No. 3211378 discloses a technique of using a foam metal as a gas diffusion electrode of a polymer electrolyte fuel cell which is a kind of electrochemical power generator, and JP-A-8-138680 discloses a selective ( A metal porous body provided with a low porosity portion in a spot-like manner is disclosed.
[0003]
Furthermore, Japanese Patent No. 3242636 discloses that a mixed woven fabric or mixed non-woven fabric of metal fibers and organic fibers is used as a gas diffusion electrode.
[0004]
[Problems to be solved by the invention]
In the metal foam of Japanese Patent No. 3211378, if the porosity is increased in order to improve gas diffusibility, the contact resistance with the contact member increases, while the porosity decreases in order to reduce the contact resistance. The gas flow path resistance increases, and in any case, the output of the battery decreases.
[0005]
Further, as a method for reducing the contact resistance without reducing the porosity, there is a method of covering the contact surface with chemically stable gold or platinum, but this increases the cost.
[0006]
The porous metal body disclosed in Japanese Patent Laid-Open No. 8-138680 has a low porosity for the purpose of increasing the strength of the portion where the terminal is welded. Low contribution to reduction.
[0007]
Furthermore, the mixed hair woven fabric or the mixed hair nonwoven fabric disclosed in Japanese Patent No. 3242636 is an aggregate of fibers, and a number of fibers are laminated in the thickness direction to form an electrical path. For this reason, the contact resistance between the fibers is added together, and the electrical resistance in the thickness direction is increased.
[0008]
In addition, since the porosity is small (the area for blocking the gas flow is large), the gas flow path resistance is large, causing problems in the gas diffusivity and the uniform reactivity of each part of the catalytic reaction layer. Reduce the overall efficiency of the battery.
[0009]
Accordingly, an object of the present invention is to reduce the contact resistance with the contact partner member without using a noble metal or the like by suppressing the decrease in the porosity of the metal porous body as much as possible.
[0010]
[Means for Solving the Problems]
In order to solve the above problems, in the present invention, a porous metal body configured as follows for a gas diffusion electrode of a polymer electrolyte fuel cell, that is, an alloy mainly composed of Fe-Cr, or a Furthermore, it is formed of an alloy to which at least one element selected from Ni, Mo, Cu, B, Al, Si, and Ti is added at a ratio of less than 10%, and has an average pore diameter of 50 μm to 1 mm. It has an eye structure, a low porosity layer is provided on one surface or both surface portions, and the porosity of the portion excluding the low porosity layer is 85% or more and 99% or less, and the porosity of the low porosity layer There is provided a porous metal body has at least 2% lower Kuna' than the porosity of a portion excluding the low porosity layer.
[0011]
The present invention also provides a solid polymer fuel cell in which this metal porous body is disposed as a gas diffusion electrode on both sides of a polymer electrolyte membrane.
[0014]
[Action]
The metal porous body of the present invention has a low porosity layer on one or both surfaces, and the low porosity layer contacts the mating member (electrode catalyst layer or separator), so the contact area with the mating member increases. In addition, the contact resistance can be reduced without using expensive precious metals.
[0015]
In addition, the portion excluding the surface layer portion can ensure a high porosity, enhance the gas permeation performance, and promote the catalytic reaction.
[0016]
Therefore, if this metal porous body is arranged as a gas diffusion electrode on both sides of the polymer electrolyte membrane, the characteristics of the metal porous body excellent in gas permeability and electrical conductivity are utilized, and the electrode due to a decrease in the porosity of the surface portion. The effect of reducing the contact resistance with the catalyst layer or the separator is added, and the output of the fuel cell can be improved.
[0017]
Here, the average pore diameter of the metal porous body is limited to the range of 50 μm to 1 mm because if the average pore diameter is less than 50 μm, the flow resistance is large and it is difficult to achieve uniform gas diffusion, while the average pore diameter is 1 mm. This is because the contact point with the mating member decreases and the contact resistance increases.
[0018]
In addition, if the porosity difference between the central portion and the low porosity layer on the surface is too small, the effect of reducing contact resistance is not sufficiently exhibited, so the difference was set to at least 2%.
[0019]
In addition, when the porosity of a metal porous body is reduced too much, the permeability | transmittance of the water which generate | occur | produces in an electrode catalyst layer by gas permeability or an electrochemical reaction will deteriorate. In order to avoid this problem, the porosity of the portion excluding the low porosity layer on the surface should be 85% or more. On the other hand, in order to ensure the elasticity of the metal porous body, the porosity of the portion excluding the low porosity layer is preferably 99% or less.
[0020]
In addition, it is desirable that the porous metal body is made of a metal having excellent strength and corrosion resistance in consideration of durability in electrode applications.
[0021]
It is formed of an alloy containing carbon mainly composed of Fe—Cr or Ni—Cr, and an alloy to which at least one element selected from Ni, Mo, Cu, B, Al, Si, and Ti is further added. The metal porous body is suppressed from elution in a corrosive environment such as sulfuric acid, and the suitability as a battery electrode is enhanced.
[0022]
DETAILED DESCRIPTION OF THE INVENTION
1 and 2 schematically show a cross section of the porous metal body of the present invention. These metal
[0023]
This metal
[0024]
As described above, the porosity of the
[0025]
In the metal
[0026]
The metal porous body is manufactured by using a foaming resin or the like as a starting material by a plating method disclosed in JP-A-57-174484, a coating slurry sintering method disclosed in JP-B-38-17554, and the like. Therefore, a laminate of foamed resins having different porosities is used as a starting material, and after plating on this, the starting material is incinerated and removed, and if necessary, a metal diffusion treatment is performed in a subsequent process to form an alloy. The porous metal body of the present invention can also be manufactured by a method of applying a metal powder and resin slurry to a lamination starting material and sintering, but the above-described method can use a mass-produced product and is superior in productivity.
[0027]
As the metal
[0028]
A Ni—Cr alloy containing carbon (which is not disclosed in the above publication) is also excellent in strength and corrosion resistance, and can be used as a material for the
[0029]
Here, since the strength of the metal porous body is improved by including carbon, there is a sufficient reaction force when being laminated and pressurized with the catalyst electrode layer and the separator. Durability deterioration is reduced. Further, since the Cr carbide phase is uniformly dispersed in the metal porous body, even if a passive film is formed, the conductive carbide phase contributes to a reduction in contact resistance.
[0030]
More detailed examples are given below.
Example 1
The porous metal body shown in Table 1 (the structure of FIG. 1 in which one surface has a low porosity and the
[0031]
The contact resistance was measured by pressing both surfaces of the metal porous body (the surface of the low porosity layer and the surface of the high porosity layer) against a clean Cu electrode plate with a pressure of 1 MPa.
[0032]
[Table 1]
[0033]
[Table 2]
[0034]
-Example 2-
As a polymer electrolyte membrane, Nafion (manufactured by DuPont, 150 μm thick) was prepared, and a porous carbon body carrying a platinum catalyst on both sides of the membrane was prepared. A porous metal body was disposed, and a carbon electrode was superimposed on the outside of the porous metal body to produce a polymer electrolyte fuel cell. Further, as a comparative example, a similar fuel cell was manufactured using a porous metal body of No. 3 in Table 1 in which only a high porosity layer was provided without providing a low porosity layer. In this example, the metal porous body shown in Table 1 was provided with low porosity layers on both sides.
[0035]
As a performance evaluation of these prototypes, the cell voltage at a current density of 10 mA / cm 2 was measured. The results are shown in Table 3.
[0036]
[Table 3]
[0037]
As can be seen from Table 3, when the porous metal body of the present invention is used, the contact resistance of the gas diffusion electrode is reduced and the output of the battery is increased.
[0038]
【The invention's effect】
As described above, the porous metal body of the present invention lowers the porosity of the surface layer portion and increases the porosity of other parts, so that the gas permeability and the discharge of water generated in the electrode catalyst layer are deteriorated. In addition, the contact resistance can be lowered without using expensive precious metals or the like, and the output of the fuel cell can be increased economically.
[0039]
In addition, what specified the material of the metal porous body can suppress elution in a corrosive environment, and can improve durability.
[0040]
Moreover, what made the porosity of the site | part except a low-porosity part 85% or more and 99% or less can ensure sufficient gas permeability and sufficient elasticity.
[0041]
Therefore, the polymer electrolyte fuel cell using the porous metal body of the present invention as a gas diffusion electrode can improve the output characteristics without increasing the cost.
[Brief description of the drawings]
FIG. 1 is a schematic cross-sectional view showing an example of a porous metal body of the present invention. FIG. 2 is a schematic cross-sectional view of another example.
1
Claims (2)
平均孔径が50μm〜1mmの3次元網目構造を有し、一表面又は両表面部に低気孔率層が設けられ、その低気孔率層を除く箇所の気孔率が85%以上、99%以下であり、低気孔率層の気孔率が前記低気孔率層を除く箇所の気孔率よりも少なくとも2%低くなっている金属多孔体。 An alloy based on Fe—Cr used as a gas diffusion electrode of a polymer electrolyte fuel cell, or at least one selected from Ni, Mo, Cu, B, Al, Si, and Ti A porous metal body formed of an alloy to which an element of less than 10% is added,
The average pore diameter has a three-dimensional network structure of 50Myuemu~1mm, one surface or both surfaces portions in the low porosity layer is provided, the porosity of the region other than the low porosity layer is 85% or more, 99% or less , and the low porosity layer at least 2% low Kuna' in which the porous metal body than the porosity of the portion porosity excluding the low porosity layer.
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JP6412485B2 (en) * | 2015-11-20 | 2018-10-24 | 株式会社健明 | Fuel cell electrode material and method for producing the same |
JP2020004527A (en) * | 2018-06-26 | 2020-01-09 | 株式会社グラヴィトン | Solid polymer electrolyte fuel cell and electrode manufacturing method |
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