JP2506879B2 - Fuel cell - Google Patents
Fuel cellInfo
- Publication number
- JP2506879B2 JP2506879B2 JP63000394A JP39488A JP2506879B2 JP 2506879 B2 JP2506879 B2 JP 2506879B2 JP 63000394 A JP63000394 A JP 63000394A JP 39488 A JP39488 A JP 39488A JP 2506879 B2 JP2506879 B2 JP 2506879B2
- Authority
- JP
- Japan
- Prior art keywords
- electrode
- layer
- separator
- gas
- pore diameter
- 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.)
- Expired - Fee Related
Links
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/023—Porous and characterised by the material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Inert Electrodes (AREA)
- Fuel Cell (AREA)
Description
【発明の詳細な説明】 〔産業上の利用分野〕 本発明は燃料電池に関するものである。TECHNICAL FIELD The present invention relates to a fuel cell.
従来の燃料電池に使用されている２層多孔質電極は特
開昭59−215665号広報に記載されているように、その２
層の界面が平板状になっていた。A two-layer porous electrode used in a conventional fuel cell is disclosed in Japanese Patent Application Laid-Open No. 59-215665, No. 2 thereof.
The interface of the layers was flat.
上記従来技術はセパレータリブと電極とが接する部分
の電極内ガス拡散抵抗の点について配慮がされておら
ず、ガス流路、セパレータリブの幅に比較して２層多孔
質電極（２つの層は細孔径が異なる）構造の細孔径の大
きな層の厚さが小さいため、セパレータリブに接触する
電極部では燃料および酸化剤ガスが電解質に達するまで
の距離が、ガス流路部に接する電極部の電解質までの距
離に比較してかなり長くなり、ガス拡散抵抗が大きく、
性能低下をもたらす問題があった。The above-mentioned prior art does not take into consideration the gas diffusion resistance in the electrode at the portion where the separator rib and the electrode are in contact with each other, and the two-layer porous electrode (two layers are Since the thickness of the layer with a large pore size of the structure) is small, the distance until the fuel and oxidant gas reach the electrolyte at the electrode part contacting the separator rib is the same as that of the electrode part contacting the gas flow path part. Compared to the distance to the electrolyte, it becomes considerably longer, and the gas diffusion resistance is large,
There was a problem that reduced performance.
本発明は以上の点に鑑みなされたものであり、セパレ
ータリブに接する電極のガス拡散抵抗を小さくし、電解
質とガスとの接触面積を増大して性能向上を可能とした
燃料電池を提供することを目的とするものである。The present invention has been made in view of the above points, and provides a fuel cell capable of improving the performance by reducing the gas diffusion resistance of the electrode in contact with the separator rib and increasing the contact area between the electrolyte and the gas. The purpose is.
すなわち本発明は、平均細孔径の大きな層を前記セパ
レータ側に配置し、また平均細孔径の小さな層を電解質
板側に配置するとともに、この２層の界面に凹凸部を設
け、かつ前記平均細孔径の小さな層のセパレータ側へ凸
となる部分が、セパレータリブの下部にくるように形成
し初期の目的を達成するようにしたものである。That is, according to the present invention, a layer having a large average pore diameter is arranged on the separator side, and a layer having a small average pore diameter is arranged on the electrolyte plate side, and a concavo-convex portion is provided at the interface between the two layers, and The portion of the layer having a small pore size, which is convex toward the separator, is formed so as to be located below the separator rib so as to achieve the initial purpose.
すなわちこのように形成された燃料電池であると、平
均細孔径の小さな層、すなわち電解質板側の層のセパレ
ータ側へ凸となっている部分がセパレータリブの下部に
くるようにしたので、セパレータリブと電解質液面との
距離が小さくなってセパレータリブと接する電極のガス
拡散抵抗が小さくなる。また、電解質の液面形状は２層
の界面の凹凸形状と同じ凹凸になって、ガス流路から電
極中の電解質表面（凹凸部）までの拡散距離が電極内で
ほぼ一様となる。更に電解質とガスとの接触する部分も
凹凸部で接触するので従来の電極より大きくなり、セパ
レータリブに接する電極のガス拡散抵抗を小さくし、電
解質とガスとの接触面積を大きくすることができ、燃料
電池の性能を向上することができる。That is, in the fuel cell formed in this way, the layer having a small average pore diameter, that is, the portion of the layer on the electrolyte plate side that is convex toward the separator is located below the separator rib. And the liquid surface of the electrolyte are reduced, and the gas diffusion resistance of the electrode in contact with the separator rib is reduced. Further, the liquid surface shape of the electrolyte has the same unevenness as the uneven shape of the interface between the two layers, and the diffusion distance from the gas flow path to the electrolyte surface (uneven portion) in the electrode is substantially uniform in the electrode. Further, the contact portion between the electrolyte and the gas also comes in contact with the uneven portion, so that it becomes larger than the conventional electrode, the gas diffusion resistance of the electrode in contact with the separator rib can be reduced, and the contact area between the electrolyte and the gas can be increased. The performance of the fuel cell can be improved.
以下、図示した実施例に基づいて本発明を説明する。
第１図から第４図には本発明の一実施例が示されてい
る。第１図に示されているように燃料電池は電解質板１
を挟んで設けられた燃料極２および酸化剤ガス極3,すな
わち電解質板１の上側に燃料極2,下側に酸化剤ガス極３
が設置されている。またこれら燃料極２および酸化剤ガ
ス極３にはセパレータリブ4aを介してセパレータ４が積
層されている。そしてこれら燃料極，酸化剤ガス極（電
極）2,3とセパレータ４との間で、かつ隣接しているセ
パレータリブ4a間には燃料，酸化剤ガスが夫々流通する
ガス流路５が設けられている。Hereinafter, the present invention will be described based on the illustrated embodiments.
1 to 4 show an embodiment of the present invention. As shown in FIG. 1, the fuel cell has an electrolyte plate 1
A fuel electrode 2 and an oxidant gas electrode 3, which are provided so as to sandwich them, that is, a fuel electrode 2 above the electrolyte plate 1 and an oxidant gas electrode 3 below the electrolyte plate 1.
Is installed. Further, a separator 4 is laminated on the fuel electrode 2 and the oxidant gas electrode 3 via a separator rib 4a. A gas flow path 5 is provided between the fuel electrode and the oxidant gas electrodes (electrodes) 2 and 3 and the separator 4 and between the adjacent separator ribs 4a to pass the fuel and the oxidant gas, respectively. ing.
これら電極は、夫々多孔質の２つの層から形成されて
いる。すなわち燃料極２を例にとれば、平均細孔径の大
きな層6aと小さな層6bから形成されているのである。換
言すれば、その一方の層は他方の層より平均細孔径の大
きな層に形成され、他方の層が一方の層より平均細孔径
の小さな層に形成されていると云うことである。Each of these electrodes is formed of two porous layers. That is, taking the fuel electrode 2 as an example, it is formed of a layer 6a having a large average pore diameter and a layer 6b having a small average pore diameter. In other words, the one layer is formed in a layer having a larger average pore diameter than the other layer, and the other layer is formed in a layer having a smaller average pore diameter than the one layer.
そして本実施例では、この平均細孔径の大きな層6aは
セパレータ４側に配置され、平均細孔径の小さな層6bは
電解質板１側に配置され、さらにこの２つの層6a,6bの
界面７には凹凸部が設けられ、かつ平均細孔径の小さな
層6bのセパレータ側へ凸となる部分が、セパレータリブ
4aの下部にくるように形成されている。すなわち、電極
２がセパレータリブ4aに接する部分で細孔径の小さな層
6bが細孔径の大きな層6aに突きだすように形成されてい
るのである。酸化剤ガス極３についてはガスの流れが燃
料極２側に直交して流れるため第１図には電極３内の層
の界面の形状は図示されていないが、燃料極２と同じで
ある。In this example, the layer 6a having a large average pore diameter is arranged on the separator 4 side, the layer 6b having a small average pore diameter is arranged on the electrolyte plate 1 side, and further at the interface 7 between the two layers 6a, 6b. Is a separator rib where the uneven portion is provided, and the portion of the layer 6b having a small average pore diameter that is convex toward the separator is a separator rib.
It is formed to come to the bottom of 4a. That is, a layer having a small pore diameter at the portion where the electrode 2 is in contact with the separator rib 4a
6b is formed so as to protrude into the layer 6a having a large pore diameter. The oxidant gas electrode 3 has the same shape as the fuel electrode 2 though the shape of the interface between layers in the electrode 3 is not shown in FIG. 1 because the gas flow is orthogonal to the fuel electrode 2 side.
第２図には第１図に示す燃料極側の電解質液形状と電
極２内のガスの流れが示されている。平均細孔径が電極
２内の界面７を境にしてセパレータ４側と電解質板側と
で異なるため、電解質（MCFCでは炭酸リチウムと炭酸カ
リウムを共晶塩）液の毛細管力の差により、電極２内の
電解質液のレベルLeの形状は同図下部のように、２層の
界面７の凹凸形状と同じ凹凸となる。ガス流路５内の燃
料ガス（MCFCでは水素ガス）８は平均細孔径の大きな層
6aを同図に示されているように界面７の凹凸に向って拡
散し、電解質液面に到達し、電極２表面で電気化学反応
により電気を発生する。このような燃料ガス８あるいは
酸化剤ガスの電極内移動については従来、電解質中をガ
スが液中拡散する速度が非常に遅いのに比較すれば、電
極内の気相中ガス拡散速度は問題とならないほど速いと
され、その抵抗は考えなくてもよいとされていた。しか
し、電極内のガス拡散係数を実測した結果、第３図に示
すようなデータが得られた。同図は縦軸のCO2拡散係数
をとり横軸に温度をとって、温度と拡散係数との関係が
示されている。同図に示されているように気相（電極な
どのように屈曲した細孔構造などのない空間）中に比較
し、平均細孔径10μｍの電極内の拡散係数Ｄは約1/10か
ら1/20になっている。拡散によるガスの移動距離は拡散
係数Ｄと時間ｔとの積の平方根 に比例、すなわち に比例することになる。従って例えば電解質液中のCO2
拡散係数が10-5cm2/S,電極（平均細孔径10μｍ）中のガ
ス拡散係数は測定により約10-2cm2/Sであるので、電解
質液膜厚さが１μｍ程度としても液中の移動時間（L2/
D）ｌ（但しＬは電解質の液膜の厚さ、Ｄは拡散係数、
ｌは液体を示す添字である）の値は10-3sec、一方、電
極内のガス移動距離は0.2から0.5mmとすれば、その電極
中の移動時間（L2/D）ｇ（但しＬはガス相の厚さ、Ｄは
拡散係数、ｇは気相を示す添字である）は４×10-2〜2.
5×10-1secとなる。このことから電極中のガス拡散は液
中のガス拡散よりも遅く、物質移動過程の律速段階とな
ることが判る。FIG. 2 shows the shape of the electrolyte solution on the fuel electrode side shown in FIG. 1 and the gas flow in the electrode 2. Since the average pore diameter is different between the separator 4 side and the electrolyte plate side with the interface 7 in the electrode 2 as a boundary, the electrode 2 is affected by the difference in the capillary force of the electrolyte (MCFC eutectic salt of lithium carbonate and potassium carbonate) liquid. The shape of the level Le of the electrolyte solution inside has the same unevenness as the uneven shape of the interface 7 between the two layers as shown in the lower part of the figure. The fuel gas (hydrogen gas in MCFC) 8 in the gas flow path 5 is a layer with a large average pore diameter.
6a is diffused toward the unevenness of the interface 7 as shown in the figure, reaches the electrolyte liquid surface, and generates electricity by an electrochemical reaction on the surface of the electrode 2. Regarding the movement of the fuel gas 8 or the oxidant gas in the electrode, the gas diffusion rate in the gas phase in the electrode is a problem as compared with the conventional case where the gas diffusion rate in the electrolyte is very slow. It was said that it was so fast that it would not be necessary, and it was said that the resistance did not have to be considered. However, as a result of actually measuring the gas diffusion coefficient in the electrode, the data as shown in FIG. 3 was obtained. The figure shows the relationship between the temperature and the diffusion coefficient by plotting the CO 2 diffusion coefficient on the ordinate and the temperature on the abscissa. As shown in the figure, the diffusion coefficient D in the electrode having an average pore diameter of 10 μm is about 1/10 to 1 as compared with that in the gas phase (a space without a bent pore structure such as an electrode). It is / 20. The migration distance of gas due to diffusion is the square root of the product of diffusion coefficient D and time t. Proportional to, ie Will be proportional to. Therefore, for example, CO 2 in the electrolyte solution
The diffusion coefficient is 10 -5 cm 2 / S, and the gas diffusion coefficient in the electrode (average pore size 10 μm) is about 10 -2 cm 2 / S, so even if the electrolyte film thickness is about 1 μm Travel time (L 2 /
D) l (where L is the thickness of the electrolyte liquid film, D is the diffusion coefficient,
The value of (l is a subscript indicating a liquid) is 10 -3 sec. On the other hand, if the gas moving distance in the electrode is 0.2 to 0.5 mm, the moving time in the electrode (L 2 / D) g Is the thickness of the gas phase, D is the diffusion coefficient, and g is a subscript indicating the gas phase) is 4 × 10 -2 to 2.
It becomes 5 × 10 -1 sec. From this, it is understood that the gas diffusion in the electrode is slower than the gas diffusion in the liquid and is the rate-determining step of the mass transfer process.
第４図は本実施例による電極内の電解質液面形状がど
のようにガス拡散過程と関連しているかを示したもの
で、本実施例によれば電解質液の厚さはセパレータリブ
4aに接する電極部で厚くなり、そのため燃料あるいは酸
化剤ガス８の流れは従来の２層多孔質電極に比較し、セ
パレータリブ部の電解質液への移動距離が短くなり、電
極全体でのガス拡散距離が一様となり、ガス移動に伴う
抵抗が小さくなり、電池性能が向上する。また電解質液
の気相と接する部分が凹凸部で従来の点線表示のように
平坦部でないので、従来の電極よりも面積的に大きくな
り、それだけ反応有効面積も増大し、性能が向上する。FIG. 4 shows how the shape of the electrolyte liquid surface in the electrode according to the present embodiment is related to the gas diffusion process. According to the present embodiment, the thickness of the electrolyte solution depends on the separator rib.
The electrode portion in contact with 4a becomes thicker, so that the flow of fuel or oxidant gas 8 is shorter than that of the conventional two-layer porous electrode because the moving distance of the separator rib portion to the electrolyte solution is shorter, and gas diffusion in the entire electrode The distance becomes uniform, the resistance due to gas movement is reduced, and the battery performance is improved. Further, since the portion in contact with the gas phase of the electrolyte solution is an uneven portion and is not a flat portion as in the conventional dotted line display, the area is larger than that of the conventional electrode, and the reaction effective area is increased accordingly, and the performance is improved.
このように本実施例によれば平均細孔径の異なる層を
その界面で凹凸部を設けて構成し、平均細孔径の小さな
層が大きな層に突き出す部分がセパレータリブと電極と
が接する部分と一致することにより、電極内での電解質
液までのガス拡散抵抗が電極内で一様となり、物質移動
に伴う抵抗が小さくなるのみならず反応面積が増大する
ので、電池性能の向上が達成できる。As described above, according to this example, layers having different average pore diameters are formed by providing uneven portions at their interfaces, and a portion where a layer having a small average pore diameter protrudes into a large layer coincides with a portion where the separator rib and the electrode are in contact. By doing so, the gas diffusion resistance up to the electrolyte solution in the electrode becomes uniform in the electrode, not only the resistance due to mass transfer decreases but also the reaction area increases, so that improvement in battery performance can be achieved.
第５図には本発明の他の実施例が示されている。本実
施例では凹凸部の凸部をセパレータリブ4aの下部のみな
らず、ガス流路５の下部にも位置するようにした。すな
わち凹凸部を、セパレータリブ4aのピッチに対して整数
分の１とした。このようにすることにより凸部すなわち
突き出し部が増大した分だけ反応面積が増加し、前述の
場合よりも燃料電池の性能が向上する。FIG. 5 shows another embodiment of the present invention. In this embodiment, the convex portion of the concave-convex portion is located not only below the separator rib 4a but also below the gas flow path 5. That is, the uneven portion was set to be an integral fraction of the pitch of the separator rib 4a. By doing so, the reaction area is increased by the amount of the protrusions, that is, the protrusions, and the performance of the fuel cell is improved as compared with the case described above.
上述のように本発明はセパレータリブに接する電極の
ガス拡散抵抗を小さくし、電解質しガスとの接触面積を
増大して性能向上を可能とした燃料電池を得ることがで
きる。As described above, according to the present invention, it is possible to obtain a fuel cell in which the gas diffusion resistance of the electrode in contact with the separator rib is reduced and the contact area with the electrolyte and gas is increased to improve the performance.
第１図は本発明の燃料電池の一実施例の単位電池の維断
側面図、第２図は第１図の燃料極側での電解質液形状を
示す説明図、第３図は同じく一実施例のCO2拡散係数と
温度との関係を示す特性図、第４図は同じく一実施例に
よる電極内でのガス拡散状況を示す説明図、第５図は本
発明の燃料電池の他の実施例の単位電池要部の縦断側面
図である。 １……電解質板、２……燃料極、３……酸化剤ガス極、
４……セパレータ、4a……セパレータリブ、５……ガス
流路、6a…平均細孔径の大きな層、6b……平均細孔径の
小さな層、７……界面、８……燃料ガス。FIG. 1 is a side view of the unit cell of one embodiment of the fuel cell of the present invention, FIG. 2 is an explanatory view showing the shape of the electrolyte solution on the fuel electrode side of FIG. 1, and FIG. FIG. 4 is a characteristic diagram showing the relationship between the CO 2 diffusion coefficient and temperature in the example, FIG. 4 is an explanatory diagram showing the gas diffusion state in the electrode according to the embodiment, and FIG. 5 is another embodiment of the fuel cell of the present invention. It is a vertical side view of the unit battery main part of an example. 1 ... Electrolyte plate, 2 ... Fuel electrode, 3 ... Oxidizer gas electrode,
4 ... Separator, 4a ... Separator rib, 5 ... Gas flow path, 6a ... Layer with large average pore diameter, 6b ... Layer with small average pore diameter, 7 ... Interface, 8 ... Fuel gas.
Claims (1)
化剤ガス極と、これら燃料極および酸化剤ガス極にセパ
レータリブを介して積層されたセパレータとを備え、前
記電極と前記セパレータとの間には燃料，酸化剤ガスが
夫々流通するガス流路が設けられており、かつ前記電極
は２層に形成されており、その一方の層は他方の層より
平均細孔径の大きな層に形成され、他方の層は一方の層
より平均細孔径の小さな層に形成されている燃料電池に
おいて、 前記平均細孔径の大きな層を前記セパレータ側に配置
し、前記平均細孔径の小さな層を前記電解質板側に配置
するとともに、 この２層の界面に凹凸部を設け、 かつ前記平均細孔径の小さな層のセパレータ側へ凸とな
る部分が、前記セパレータリブの下部にくるように形成
したことを特徴とする燃料電池。1. A fuel electrode and an oxidant gas electrode sandwiching an electrolyte, and a separator laminated on the fuel electrode and the oxidant gas electrode via separator ribs. A gas flow path through which a fuel and an oxidant gas respectively flow is provided between them, and the electrode is formed in two layers, one of which is formed in a layer having a larger average pore diameter than the other. In the fuel cell in which the other layer is formed in a layer having a smaller average pore diameter than the one layer, the layer having a larger average pore diameter is arranged on the separator side, and the layer having a smaller average pore diameter is the electrolyte. In addition to being arranged on the plate side, a concavo-convex portion is provided at the interface between the two layers, and the portion of the layer having the smaller average pore diameter that is convex toward the separator is formed so as to be located below the separator rib. Fuel cell.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63000394A JP2506879B2 (en) | 1988-01-06 | 1988-01-06 | Fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63000394A JP2506879B2 (en) | 1988-01-06 | 1988-01-06 | Fuel cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH01176664A JPH01176664A (en) | 1989-07-13 |
| JP2506879B2 true JP2506879B2 (en) | 1996-06-12 |
Family
ID=11472590
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP63000394A Expired - Fee Related JP2506879B2 (en) | 1988-01-06 | 1988-01-06 | Fuel cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2506879B2 (en) |
Families Citing this family (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2831061B2 (en) * | 1989-11-28 | 1998-12-02 | 三菱重工業株式会社 | Gas diffusion electrode and solid polymer electrolyte fuel cell body using the same |
| DK166747B1 (en) * | 1989-12-05 | 1993-07-05 | Topsoe Haldor As | FUEL CELL AND FUEL CELL STABLE |
| DE19541619A1 (en) * | 1995-11-08 | 1997-05-15 | Bosch Gmbh Robert | Electrochemical sensor and method for producing an electrochemical sensor |
-
1988
- 1988-01-06 JP JP63000394A patent/JP2506879B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPH01176664A (en) | 1989-07-13 |
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