JP2774227B2 - Method for joining solid oxide fuel cell stack - Google Patents
Method for joining solid oxide fuel cell stackInfo
- Publication number
- JP2774227B2 JP2774227B2 JP5012623A JP1262393A JP2774227B2 JP 2774227 B2 JP2774227 B2 JP 2774227B2 JP 5012623 A JP5012623 A JP 5012623A JP 1262393 A JP1262393 A JP 1262393A JP 2774227 B2 JP2774227 B2 JP 2774227B2
- Authority
- JP
- Japan
- Prior art keywords
- interconnector
- joining
- electrode film
- solid oxide
- oxide fuel
- 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
-
- 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
- Fuel Cell (AREA)
- Laminated Bodies (AREA)
Description
【０００１】[0001]
【産業上の利用分野】本発明は、固体電解質型燃料電池
スタックの接合方法に係り、特に接合面の電気的接触抵
抗を小さくすることができる、固体電解質型燃料電池ス
タックの接合方法に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for joining a solid oxide fuel cell stack, and more particularly to a method for joining a solid oxide fuel cell stack capable of reducing the electrical contact resistance at the joint surface.
【０００２】[0002]
【従来の技術】固体電解質型燃料電池を構成する各単セ
ルは、インターコネクタを介して電気的に接続されてお
り、インターコネクタは、一般にランタンクロマイト系
のセラミックス、耐熱合金等によって構成されている。
従って、単セルの電極膜とインターコネクタとの接続
は、セラミックス同志またはセラミックスと金属との接
続となる。2. Description of the Related Art Single cells constituting a solid oxide fuel cell are electrically connected via an interconnector, and the interconnector is generally made of lanthanum chromite-based ceramics, heat-resistant alloy, or the like. .
Therefore, the connection between the electrode film of the single cell and the interconnector is between ceramics or between ceramics and metal.
【０００３】しかしながら、単セルの電極材およびイン
ターコネクタ材は変形能が低く、このような変形能の低
い構成材料同志の接合は、たとえ接合面に多少の圧力を
加えたとしても十分な接触面積が得られず、接合面の電
気的接触抵抗が大きくなってしまうという問題がある。[0003] However, the electrode material and the interconnector material of a single cell have low deformability, and the joining of such constituent materials having low deformability requires a sufficient contact area even if some pressure is applied to the joint surface. Therefore, there is a problem that the electrical contact resistance of the joint surface increases.
【０００４】[0004]
【発明が解決しようとする課題】本発明の目的は、上記
従来技術の問題点を解決し、電気が流れるのに十分な接
触面積を確保して接合面の電気的接触抵抗を小さくする
ことができる、固体電解質型燃料電池スタックの接合方
法を提供することにある。SUMMARY OF THE INVENTION It is an object of the present invention to solve the above-mentioned problems of the prior art, to secure a sufficient contact area for electricity to flow, and to reduce the electrical contact resistance at the joint surface. It is an object of the present invention to provide a method for joining a solid oxide fuel cell stack.
【０００５】[0005]
【課題を解決するための手段】上記目的を達成するため
本発明は、単セルをインターコネクタを介して電気的に
接続する固体電解質型燃料電池スタックの接合方法にお
いて、前記単セルの電極膜の、インターコネクタとの接
合面に、該電極膜を構成する電極材のスラリを塗布する
とともに、前記インターコネクタの、前記単セルの電極
膜との接合面に、該インターコネクタを構成するインタ
ーコネクタ材のスラリを塗布し、前記両接合面間に、接
合条件下で前記電極およびインターコネクタの構成材料
よりも変形し易い、電気伝導性の多孔質セラミックスを
介在して接合することを特徴とする。In order to achieve the above object, the present invention provides a method for joining a solid oxide fuel cell stack, wherein a single cell is electrically connected via an interconnector. A slurry of an electrode material forming the electrode film is applied to a bonding surface with the interconnector, and an interconnector material forming the interconnector is formed on a bonding surface of the interconnector with the electrode film of the single cell. And applying an electrically conductive porous ceramic, which is more easily deformed than the constituent materials of the electrode and the interconnector under the joining conditions, between the two joining surfaces.
【０００６】[0006]
【作用】単セル電極膜の、インターコネクタとの接合面
に、該電極膜を構成する電極材のスラリを塗布するとと
もに、インターコネクタの、前記単セル電極膜との接合
面に、該インターコネクタを構成するインターコネクタ
材のスラリを塗布することにより、前記電極膜またはイ
ンターコネクタとスラリは、接合時の焼結処理によって
電気的に確実に接続される。また、それぞれ構成材料の
スラリが塗布された単セルの電極膜とインターコネクタ
の接合面との間に、接合条件下で前記電極膜およびイン
ターコネクタの構成材料よりも変形し易い、電気伝導性
の多孔質セラミックスを介在して接合することにより、
前記両スラリが単セル電極面およびインターコネクタを
投錨効果によって前記多孔質セラミックスに確実に接続
するので、広い接触面積を持った、電気的接触抵抗の小
さい接合体が得られる。The slurry of the electrode material constituting the electrode film is applied to the joint surface of the single-cell electrode film with the interconnector, and the interconnector is joined to the joint surface of the interconnector with the single-cell electrode film. Is applied, the electrode film or the interconnector and the slurry are electrically and reliably connected by a sintering process at the time of joining. Further, between the electrode film of the single cell to which the slurry of the constituent material is applied and the bonding surface of the interconnector, the conductive film is more easily deformed than the constituent material of the electrode film and the interconnector under the bonding condition. By joining with porous ceramics,
Since the two slurries reliably connect the single cell electrode surface and the interconnector to the porous ceramics by the anchoring effect, a joined body having a large contact area and a small electric contact resistance can be obtained.
【０００７】本発明において単セルとは、固体電解質膜
の両面に燃料極膜および酸素極膜がそれぞれ積層され
た、固体電解質型燃料電池スタックを構成する電池の最
少単位をいう。またインターコネクタとは、固体電解質
型燃料電池スタックの前記単セル相互間に配置され、該
単セルを電気的に直列または並列に接続する接合部材で
ある。In the present invention, a single cell is the minimum unit of a cell constituting a solid oxide fuel cell stack in which a fuel electrode film and an oxygen electrode film are respectively laminated on both surfaces of a solid electrolyte film. The interconnector is a joining member arranged between the single cells of the solid oxide fuel cell stack and electrically connecting the single cells in series or in parallel.
【０００８】本発明において電気伝導性の多孔質セラミ
ックスとは、単セルの電極材料とほぼ同様の組成を有
し、前記電極材料よりも電気伝導度が大きく、接合条件
下で電極材およびインターコネクタ材よりも変形し易い
セラミックスであり、例えばＮｉ−ＺｒＯ2 −ＳｉＯ2
からなるＮｉサーメットがあげられる。この電気伝導性
の多孔質セラミックスは、単セルの電極面とインターコ
ネクタとに挟持されて集電板としても作用する。In the present invention, the electrically conductive porous ceramic has a composition substantially similar to that of a single-cell electrode material, has a higher electrical conductivity than the electrode material, and has an electrode material and an interconnector under bonding conditions. Ceramics that are more easily deformed than materials, such as Ni—ZrO 2 —SiO 2
Ni cermet consisting of The electrically conductive porous ceramic is sandwiched between the electrode surface of the single cell and the interconnector and also functions as a current collector.
【０００９】電極材スラリおよびインターコネクタ材ス
ラリとは、例えば０．１〜１０μｍに粉砕した電極材ま
たはインターコネクタ材の粉末をそれぞれエタノールお
よびトルエンとの混合液と混合したものであり、混合割
合は使用目的によって任意に選択される。また、このよ
うなスラリにはバインダーを添加することが好ましく、
例えば重量基準で５％のポリビニルブチラール等が使用
される。The electrode material slurry and interconnect material slurry are, for example, powders of the electrode material or interconnect material crushed to 0.1 to 10 μm mixed with a mixture of ethanol and toluene, respectively. It is arbitrarily selected depending on the purpose of use. It is also preferable to add a binder to such a slurry,
For example, 5% by weight of polyvinyl butyral or the like is used.
【００１０】本発明において、単セルの電極膜とインタ
ーコネクタとの接合は、該単セルの電極膜とインターコ
ネクタとの間に電気伝導性の多孔質セラミックスを介し
て積層し、この積層体を、例えば１４００〜１５００℃
で１〜１０時間、１〜５ｋｇ／ｃｍ2 の圧力でプレスす
ることによって行われる。本発明において、単セルの電
極膜とインターコネクタの接合面とにそれぞれ構成材料
スラリを塗布しないで接合しても、前記多孔性セラミッ
クスの変形能が高いので十分な接合面積が得られ、接合
面の電気的接触抵抗は従来技術に較べて非常に小さくな
る。In the present invention, the electrode film of the single cell and the interconnector are joined by interposing an electrically conductive porous ceramic between the electrode film of the single cell and the interconnector. , For example, 1400-1500 ° C
For 1 to 10 hours at a pressure of 1 to 5 kg / cm 2 . In the present invention, even if the electrode film of the single cell and the bonding surface of the interconnector are bonded without applying the constituent material slurry respectively, a sufficient bonding area can be obtained because the deformability of the porous ceramic is high, and the bonding surface can be obtained. Has a very low electrical contact resistance compared to the prior art.
【００１１】[0011]
【実施例】次に、本発明を実施例によりさらに詳細に説
明する。図１は、本発明が適用される平板型高温固体電
解質型燃料電池の説明図である。図において、例えばＹ
ＳＺからなる固体電解質膜３の両面にＮｉ−ＹＳＺ（ニ
ッケル系イットリウム安定化ジルコニア）からなる燃料
側電極膜５およびＬａ（Ｓｒ）ＭｎＯ3 からなる空気側
電極膜４がそれぞれ積層された単セル１は、接合材であ
る電気伝導性の多孔質セラミックス８、およびガスセパ
レータ７のインターコネクタ６を介して接続され、隣接
する単セル相互の空気側電極膜４と燃料側電極膜５との
接続は、ガスセパレータ７に設けられた、例えばＬａ
（Ｃａ）ＣｒＯ3 からなるインターコネクタ６を介して
次のように行われる。すなわち、前記空気側電極膜４の
インターコネクタ６との接合面に、０．１〜１０μｍに
粉砕した、空気極材であるＬａ（Ｓｒ）ＭｎＯ3 の粉末
と、エタノールとトルエンとの混合液を１対１に混合し
たスラリを塗布し、他方、前記インターコネクタ６の前
記空気側電極膜４との接合面に、０．１〜１０μｍに粉
砕したインターコネクタ材であるＬａ（Ｃａ）ＣｒＯ3
粉末と、エタノールとトルエンとの混合液を１対１に混
合したスラリを塗布し、スラリを適度に乾燥させたの
ち、前記両接合面間に、例えばＬａ（Ｓｒ）ＭｎＯ3 か
らなる多孔質セラミックスを介在して積層し、その後、
この積層体を１５００℃で１時間、１ｋｇ／ｃｍ2 〜５
ｋｇ／ｃｍ2の圧力でプレスして接合体を得た。燃料側
電極膜５とインターコネクタ６との接合は、多孔質セラ
ミックス８としてニッケルサーメットを用いて、前記空
気側電極膜４の場合と同様にして接合体を完成させた。Next, the present invention will be described in more detail with reference to examples. FIG. 1 is an explanatory diagram of a flat high-temperature solid oxide fuel cell to which the present invention is applied. In the figure, for example, Y
A single cell 1 in which a fuel-side electrode film 5 made of Ni-YSZ (nickel-based yttrium-stabilized zirconia) and an air-side electrode film 4 made of La (Sr) MnO 3 are respectively stacked on both surfaces of a solid electrolyte film 3 made of SZ. Are connected via an electrically conductive porous ceramics 8 as a bonding material and an interconnector 6 of a gas separator 7. The connection between the air-side electrode film 4 and the fuel-side electrode film 5 between adjacent single cells is established. , Provided on the gas separator 7, for example, La
The operation is performed as follows through the interconnector 6 made of (Ca) CrO 3 . That is, a mixed solution of La (Sr) MnO 3 powder, which is an air electrode material, and a mixture of ethanol and toluene was crushed to a thickness of 0.1 to 10 μm on the surface of the air-side electrode film 4 joined to the interconnector 6. La (Ca) CrO 3, which is an interconnector material pulverized to 0.1 to 10 μm, is coated on the surface of the interconnector 6 with the air-side electrode film 4 by applying a one-to-one mixed slurry.
A slurry obtained by mixing a powder and a mixed solution of ethanol and toluene in a one-to-one ratio is applied, and after the slurry is dried appropriately, a porous ceramic made of, for example, La (Sr) MnO 3 is provided between the two joining surfaces. Interposed and then laminated,
This laminate is heated at 1500 ° C. for 1 hour at 1 kg / cm 2 -5
Pressing was performed at a pressure of kg / cm 2 to obtain a joined body. The joint between the fuel-side electrode film 5 and the interconnector 6 was completed using nickel cermet as the porous ceramics 8 in the same manner as in the case of the air-side electrode film 4.
【００１２】図２は、空気側電極膜４とインターコネク
タ６との接合面を模式的に示した拡大図であり、図２ａ
は、本実施例方法により接合した場合、図２ｂは従来方
法により接合した場合を示す図である。図２ａにおい
て、本実施例方法によって接合した接合体は、空気側電
極膜４およびインターコネクタ６の、凹凸を有する接合
面９間に多孔質セラミックス８が満たされており、広い
接合面で良好に接合されていることが分かる。一方、図
２ｂに示した従来の接合方法による接合体は、空気側電
極膜４とインターコネクタ６との接合面間に空間部１０
が残っており、電気的接触抵抗が大きくなることが容易
に推測される。FIG. 2 is an enlarged view schematically showing a joint surface between the air-side electrode film 4 and the interconnector 6, and FIG.
FIG. 2B is a diagram showing a case where bonding is performed by the conventional method, and FIG. In FIG. 2A, the joined body joined by the method of the present embodiment is filled with the porous ceramics 8 between the uneven side joining surfaces 9 of the air electrode film 4 and the interconnector 6, and is excellent in a wide joining surface. It can be seen that they are joined. On the other hand, the joined body according to the conventional joining method shown in FIG. 2B has a space 10 between the joined surfaces of the air-side electrode film 4 and the interconnector 6.
Remain, and it is easily assumed that the electrical contact resistance increases.
【００１３】表１に本実施例と従来例とによって得られ
た接合体の、接合部分の接触抵抗を比較して示す。Table 1 shows a comparison of the contact resistance of the joints of the joined bodies obtained by the present embodiment and the conventional example.
【００１４】[0014]
【表１】 註） ＬＳＭ：Ｌａ（Ｓｒ）ＭｎＯ3 （空気側電極膜） ＬＣＣ：Ｌａ（Ｃａ）ＣｒＯ3 （インターコネクタ） 多孔質：多孔質セラミックス Ni YSZ：燃料側電極膜 （ＡＩＲ、Ｈ2 ）：接触抵抗測定時の雰囲気 本実施例によれば、電極膜４、５およびインターコネク
タ６の接合面にそれぞれ、電極材スラリおよびインター
コネクタ材スラリを塗布し、両接合面間に多孔質セラミ
ックス８を介在して接合したことにより、前記スラリと
電極膜４、５、およびスラリとインターコネクタ６とが
それぞれ焼結によって電気的に確実に接続されるととも
に、前記両スラリが単セル電極膜およびインターコネク
タを多孔質セラミックス８に投錨効果によって電気的に
確実に接続し、しかも前記多孔質セラミックス８が電極
膜４、５およびインターコネクタ６表面の凹凸を吸収す
るように変形して接触面積を広くするので、接合面にお
ける電気的接触抵抗を著しく低減することができる。[Table 1] Note) LSM: La (Sr) MnO 3 (Air side electrode film) LCC: La (Ca) CrO 3 (Interconnector) Porous: Porous ceramic Ni YSZ: Fuel side electrode film (AIR, H 2 ): Contact resistance Atmosphere at the time of measurement According to the present embodiment, the electrode material slurry and the interconnector material slurry are applied to the joint surfaces of the electrode films 4, 5 and the interconnector 6, respectively, and the porous ceramics 8 is interposed between the joint surfaces. And the slurry is electrically connected to each other by sintering the slurry and the electrode films 4 and 5, and the slurry and the interconnector 6, respectively. Electrically connected to the porous ceramics 8 by an anchoring effect, and the porous ceramics 8 is connected to the electrode films 4 and 5 and the interconnector 6. Since a wider deformed by the contact area to absorb the unevenness of the surface, it is possible to significantly reduce the electrical contact resistance at the joint surface.
【００１５】本実施例において、電気伝導性の多孔質セ
ラミックス８は集電板としても作用する。In this embodiment, the electrically conductive porous ceramics 8 also functions as a current collector.
【００１６】[0016]
【発明の効果】本発明によれば、電極膜およびインター
コネクタの接合面にそれぞれ、電極材スラリおよびイン
ターコネクタ材スラリを塗布し、両接合面間に多孔質セ
ラミックスを介在して接合することにより、接合面にお
ける電気的接触抵抗を著しく低減することができる。According to the present invention, the electrode material slurry and the interconnector material slurry are applied to the joint surfaces of the electrode film and the interconnector, respectively, and joined by interposing porous ceramics between the joint surfaces. In addition, the electrical contact resistance at the joint surface can be significantly reduced.
【図１】本発明が適用される平板型高温固体電解質型燃
料電池の説明図。FIG. 1 is an explanatory view of a flat plate type high temperature solid oxide fuel cell to which the present invention is applied.
【図２】空気側電極膜とインターコネクタとの接合部分
を示す拡大模式図。FIG. 2 is an enlarged schematic view showing a joint portion between an air-side electrode film and an interconnector.
１…単セル、３…固体電解質膜、４…空気側電極膜、５
…燃料側電極膜、６…インターコネクタ、７…ガスセパ
レータ、８…多孔質セラミックス（接合材）、９…接合
面、１０…空間部。DESCRIPTION OF SYMBOLS 1 ... Single cell, 3 ... Solid electrolyte membrane, 4 ... Air side electrode membrane, 5
... fuel-side electrode film, 6 ... interconnector, 7 ... gas separator, 8 ... porous ceramics (joining material), 9 ... joining surface, 10 ... space.
Claims (1)
的に接続する固体電解質型燃料電池スタックの接合方法
において、前記単セルの電極膜の、インターコネクタと
の接合面に、該電極膜を構成する電極材のスラリを塗布
するとともに、前記インターコネクタの、前記単セルの
電極膜との接合面に、該インターコネクタを構成するイ
ンターコネクタ材のスラリを塗布し、前記両接合面間
に、接合条件下で前記電極およびインターコネクタの構
成材料よりも変形し易い、電気伝導性の多孔質セラミッ
クスを介在して接合することを特徴とする固体電解質型
燃料電池スタックの接合方法。1. A method for joining a solid oxide fuel cell stack, wherein a single cell is electrically connected via an interconnector, wherein the electrode film is formed on a joint surface of the electrode film of the single cell with the interconnector. The slurry of the electrode material to be applied is applied, and the slurry of the interconnector material constituting the interconnector is applied to the joint surface of the interconnector with the electrode film of the single cell, and the joining is performed between the joining surfaces. A method for joining a solid oxide fuel cell stack, comprising joining an electrically conductive porous ceramic, which is more easily deformed than the constituent materials of the electrode and the interconnector under conditions.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP5012623A JP2774227B2 (en) | 1993-01-28 | 1993-01-28 | Method for joining solid oxide fuel cell stack |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP5012623A JP2774227B2 (en) | 1993-01-28 | 1993-01-28 | Method for joining solid oxide fuel cell stack |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH06223846A JPH06223846A (en) | 1994-08-12 |
| JP2774227B2 true JP2774227B2 (en) | 1998-07-09 |
Family
ID=11810509
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP5012623A Expired - Fee Related JP2774227B2 (en) | 1993-01-28 | 1993-01-28 | Method for joining solid oxide fuel cell stack |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2774227B2 (en) |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| AUPO897897A0 (en) | 1997-09-05 | 1997-09-25 | Ceramic Fuel Cells Limited | An interconnect device for a fuel cell assembly |
| DE10211042A1 (en) * | 2002-03-13 | 2003-10-02 | Andreas Schubert | Bipolar plate for fuel cell stack has porous parts manufactured using powder metallurgical techniques and/or combination of powder metallurgical and conventional manufacturing techniques |
| DE10232075A1 (en) * | 2002-07-15 | 2004-02-05 | Bayerische Motoren Werke Ag | Process for joining single fuel cells to form a fuel cell block or stack comprises placing a foil made from a porous foam structure on the electrode or bipolar plate in a single fuel cell to form a contact layer |
| JP4544874B2 (en) * | 2004-01-28 | 2010-09-15 | 京セラ株式会社 | Fuel cell and fuel cell |
| JP5072305B2 (en) * | 2006-09-28 | 2012-11-14 | 京セラ株式会社 | Heat-resistant alloy member, current collecting member for fuel cell, fuel cell stack, fuel cell |
-
1993
- 1993-01-28 JP JP5012623A patent/JP2774227B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPH06223846A (en) | 1994-08-12 |
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