JPH05144463A - Fuel cell with solid electrolyte - Google Patents

Fuel cell with solid electrolyte

Info

Publication number
JPH05144463A
JPH05144463A JP3301738A JP30173891A JPH05144463A JP H05144463 A JPH05144463 A JP H05144463A JP 3301738 A JP3301738 A JP 3301738A JP 30173891 A JP30173891 A JP 30173891A JP H05144463 A JPH05144463 A JP H05144463A
Authority
JP
Japan
Prior art keywords
fuel cell
solid electrolyte
interconnector
electrode
sintering
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
JP3301738A
Other languages
Japanese (ja)
Inventor
Hiroaki Taira
浩明 平
Hiroshi Takagi
洋 鷹木
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Murata Manufacturing Co Ltd
Original Assignee
Murata Manufacturing Co Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Murata Manufacturing Co Ltd filed Critical Murata Manufacturing Co Ltd
Priority to JP3301738A priority Critical patent/JPH05144463A/en
Publication of JPH05144463A publication Critical patent/JPH05144463A/en
Pending legal-status Critical Current

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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
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0223—Composites
    • H01M8/0228—Composites in the form of layered or coated products
    • 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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • 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
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0215—Glass; Ceramic materials
    • H01M8/0217—Complex oxides, optionally doped, of the type AMO3, A being an alkaline earth metal or rare earth metal and M being a metal, e.g. perovskites
    • 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
    • Y02E60/10—Energy storage using batteries
    • 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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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Materials Engineering (AREA)
  • Ceramic Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Composite Materials (AREA)
  • Fuel Cell (AREA)

Abstract

PURPOSE:To prevent the generation of warp and/or tear at the joint of an interconnector with a spacer in the process of co-sintering. CONSTITUTION:A solid electrolyte 1 is provided consisting of stabilized zirconia (YSZ), and an air electrode 2 and fuel electrode 3 are furnished at the oversurface and undersurface of this solid electrolyte 1. These electrodes 2, 3 are furnished over the surfaces with a distributor 5 made of (La0.8Sr0.2)MnO3 and a distributor 6 made from a hybrid material of NiO and YSZ, respectively. On both sides of these distributors 5, 6, spacers 7, 8 are arranged consisting of CaTiO3. Over and below thereof interconnectors 10, 11 are provided consisting of (La0.7-Ca0.3)CrO3. If these components are subjected to co-sintering, no Ca diffusion takes place from the interconnectors 10, 11 to the spacers 5, 6.

Description

【発明の詳細な説明】Detailed Description of the Invention

【０００１】[0001]

【産業上の利用分野】本発明は、固体電解質型燃料電池
に関する。FIELD OF THE INVENTION The present invention relates to a solid oxide fuel cell.

【０００２】[0002]

【従来の技術と課題】従来より、固体電解質型燃料電池
の固体電解質及びスペーサの材料には安定化ジルコニア
（以下、ＹＳＺという）が用いられている。ＹＳＺは高
いイオン導電率を有し、化学的安定性にも優れているか
らである。また、燃料電池の空気極、燃料極の材料には
それぞれＬａＭｎＯ3、Ｎｉ／ＹＳＺサーメットが用い
られている。さらに燃料電池のインターコネクタの材料
にはＣａを添加したランタンクロマイト、あるいは、Ｃ
ａを添加したランタンクロマイトと合金系材料との複合
材料が用いられる。ここに、Ｃａはランタンクロマイト
の焼結性を良好にするために添加されている。2. Description of the Related Art Conventionally, stabilized zirconia (hereinafter referred to as YSZ) has been used as a material for a solid electrolyte and a spacer of a solid oxide fuel cell. This is because YSZ has high ionic conductivity and excellent chemical stability. Further, LaMnO 3 and Ni / YSZ cermet are used for the materials of the air electrode and the fuel electrode of the fuel cell, respectively. Further, as a material of the interconnector of the fuel cell, lanthanum chromite containing Ca or C is added.
A composite material of lanthanum chromite containing a and an alloy material is used. Here, Ca is added to improve the sinterability of the lanthanum chromite.

【０００３】ところで、固体電解質型燃料電池の発電効
率を向上させるためには電池の内部インピーダンスを下
げればよい。電池の内部インピーダンスを下げるには、
電池を構成するそれぞれの部分をグリーンシート状にし
て組み立てた後、共焼結（同時に焼成すること）して固
体電解質やインターコネクタを薄膜化すればよいことが
知られている。このとき、それぞれのグリーンシートの
焼結時の収縮率が一致するように、粉体特性やバインダ
ー量等が正確に管理される。しかし、共焼結の際に、ラ
ンタンクロマイトからなるインターコネクタからＹＳＺ
からなるスペーサへＣａが拡散するため、インターコネ
クタの焼結性が変化し、インターコネクタとスペーサの
接合部分にそりや剥がれが生じるという問題があった。By the way, in order to improve the power generation efficiency of the solid oxide fuel cell, the internal impedance of the cell may be lowered. To lower the internal impedance of the battery,
It is known that after assembling each part constituting a battery into a green sheet shape and co-sintering (sintering at the same time), the solid electrolyte and the interconnector may be thinned. At this time, the powder characteristics, the amount of binder, and the like are accurately controlled so that the respective green sheets have the same shrinkage rate during sintering. However, when co-sintering, the lanthanum chromite interconnector
Since Ca diffuses into the spacer made of, the sinterability of the interconnector changes, and there is a problem that warpage or peeling occurs at the joint between the interconnector and the spacer.

【０００４】そこで、本発明の課題は、共焼結の際にイ
ンターコネクタとスペーサの接合部分にそりや剥がれが
生じない固体電解質型燃料電池を提供することにある。Therefore, an object of the present invention is to provide a solid oxide fuel cell in which warping or peeling does not occur at the joint between the interconnector and the spacer during co-sintering.

【０００５】[0005]

【課題を解決するための手段】以上の課題を解決するた
め、本発明に係る固体電解質型燃料電池は、（ａ）酸化
ジルコニウムを主成分とする固体電解質と、（ｂ）空気
極及び燃料極と、（ｃ）少なくともカルシウムを含むラ
ンタンクロマイトを主成分とするインターコネクタと、
（ｄ）少なくともチタン酸カルシウムを含むスペーサ
と、を備えたことを特徴とする。具体的には、固体電解
質としてはイットリウム安定化ジルコニア等が用いられ
る。インターコネクタの材料としては、ランタンクロマ
イトや、ランタンクロマイトの一部のランタン元素がイ
ットリウム、ストロンチウム等のアルカリ土類や希土類
の元素に置換されたり、ランタンクロマイトの一部のク
ロム元素がマンガン、コバルト等の元素に置換されたも
のにＣａを添加した材料等が用いられる。スペーサの材
料としては、チタン酸カルシウム、あるいは少なくとも
チタン酸カルシウムを含み、その他、チタン酸マグネシ
ウム、チタン酸ストロンチウム及びチタン酸バリウムの
うち１種あるいは２種以上を含む材料等が用いられる。In order to solve the above problems, a solid oxide fuel cell according to the present invention comprises (a) a solid electrolyte containing zirconium oxide as a main component, and (b) an air electrode and a fuel electrode. And (c) an interconnector whose main component is lanthanum chromite containing at least calcium,
(D) A spacer containing at least calcium titanate. Specifically, yttrium-stabilized zirconia or the like is used as the solid electrolyte. As materials for interconnectors, lanthanum chromite and some lanthanum elements of lanthanum chromite are replaced with alkaline earth and rare earth elements such as yttrium and strontium, and some chromium elements of lanthanum chromite are manganese, cobalt, etc. For example, a material in which Ca is added to the element replaced with the element is used. As the material of the spacer, calcium titanate, or a material containing at least calcium titanate and one or more of magnesium titanate, strontium titanate and barium titanate, and the like are used.

【０００６】[0006]

【作用】以上の構成において、スペーサに少なくともチ
タン酸カルシウムを含む材料を用いたため、共焼結の際
にインターコネクタに含まれているＣａがスペーサへ拡
散しなくなり、インターコネクタの焼結性の変化が小さ
くなる。In the above structure, since the spacer is made of a material containing at least calcium titanate, Ca contained in the interconnector is not diffused into the spacer during co-sintering, and the sinterability of the interconnector changes. Becomes smaller.

【０００７】[0007]

【実施例】以下、本発明に係る固体電解質型燃料電池の
一実施例をその製造方法と共に添付図面を参照して説明
する。図１は固体電解質型燃料電池の分解斜視図であ
る。固体電解質１は矩形状をしており、その材料として
はＹＳＺの粉体とバインダー剤のブチラール系樹脂、溶
剤（トルエン／エタノール）を混合してドクターブレー
ド法でグリーンシート状にしたものを用いる。空気極２
及び燃料極３はそれぞれ固体電解質１の上面、下面に設
けられる。燃料極３の材料としては、ＮｉＯとＹＳＺを
重量比６：４で混合した粉末とブチラール系樹脂、溶剤
（トルエン／エタノール）を混合してグリーンシート状
にしたものを用いる。空気極２の材料としては、（Ｌａ
0.8Ｓｒ0.2）ＭｎＯ3の粉末とブチラール系樹脂、溶剤
（トルエン／エタノール）を混合してグリーンシート状
にしたものを用いる。グリーンシート状にされた固体電
解質１の上下面にそれぞれグリーンシート状にされた空
気極２、燃料極３が熱圧着される。DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS An embodiment of the solid oxide fuel cell according to the present invention will be described below together with its manufacturing method with reference to the accompanying drawings. FIG. 1 is an exploded perspective view of a solid oxide fuel cell. The solid electrolyte 1 has a rectangular shape, and as its material, a YSZ powder, a butyral resin as a binder, and a solvent (toluene / ethanol) are mixed to form a green sheet by a doctor blade method. Air pole 2
The fuel electrode 3 and the fuel electrode 3 are provided on the upper surface and the lower surface of the solid electrolyte 1, respectively. As the material of the fuel electrode 3, a powder obtained by mixing NiO and YSZ at a weight ratio of 6: 4, a butyral resin, and a solvent (toluene / ethanol) are mixed into a green sheet. The material of the air electrode 2 is (La
A powder of 0.8 Sr 0.2 ) MnO 3, a butyral resin, and a solvent (toluene / ethanol) are mixed to form a green sheet. The green sheet-shaped air electrode 2 and the fuel electrode 3 are thermocompression bonded to the upper and lower surfaces of the green sheet-shaped solid electrolyte 1, respectively.

【０００８】ディストリビュータ５，６は空気極２や燃
料極３の表面に設けられ、空気極２や燃料極３に均等に
燃料ガスや空気がゆきわたるように、またそれぞれの電
極２，３と後述のインターコネクタ１０，１１を電気的
に接続するために電極材料と同じ材料にて形成される。
すなわち、ディストリビュータ６は、ＮｉＯとＹＳＺを
重量比６：４で混合した粉末と溶剤等を混合してグリー
ンシート状にしたものを用いる。同様にして、ディスト
リビュータ５は、（Ｌａ0.8Ｓｒ0.2）ＭｎＯ3の粉末と
溶剤等を混合してグリーンシート状にしたものを用い
る。このグリーンシートを複数枚重ねて厚みのある長尺
状のディストリビュータ５，６を成型し、それぞれ空気
極２及び燃料極３の表面に整列させて配設する。The distributors 5 and 6 are provided on the surfaces of the air electrode 2 and the fuel electrode 3 so that the fuel gas and the air are evenly distributed to the air electrode 2 and the fuel electrode 3, respectively, and the respective electrodes 2 and 3 and the below-described electrodes. It is formed of the same material as the electrode material for electrically connecting the interconnectors 10 and 11.
That is, as the distributor 6, a powder obtained by mixing NiO and YSZ at a weight ratio of 6: 4 and a solvent or the like are mixed to form a green sheet. Similarly, for the distributor 5, a powder of (La 0.8 Sr 0.2 ) MnO 3 and a solvent are mixed to form a green sheet. A plurality of thick green sheets are stacked to form long and thick distributors 5 and 6, which are arranged on the surfaces of the air electrode 2 and the fuel electrode 3, respectively.

【０００９】スペーサ７，８は、それぞれ整列されたデ
ィストリビュータ５，６の両側に配置され、空気や燃料
ガスを外気から遮断する。スペーサ７，８の材料として
は、ＣａＴｉＯ3の粉末とブチラール系樹脂、溶剤（ト
ルエン／エタノール）を混合してグリーンシート状にし
たものを用いる。なお、ＣａＴｉＯ3には、さらに焼結
助剤を添加してもよい。このグリーンシートを複数枚重
ねて厚みのある長尺状のスペーサ７，８を成型する。成
型されたスペーサ７，８は、それぞれ空気極２、燃料極
３の表面に接着される。The spacers 7 and 8 are arranged on both sides of the aligned distributors 5 and 6, respectively, and shield air and fuel gas from the outside air. As a material for the spacers 7 and 8, a material in which CaTiO 3 powder, butyral resin, and a solvent (toluene / ethanol) are mixed to form a green sheet is used. A sintering aid may be further added to CaTiO 3 . A plurality of green sheets are stacked to form long spacers 7 and 8 having a large thickness. The molded spacers 7 and 8 are adhered to the surfaces of the air electrode 2 and the fuel electrode 3, respectively.

【００１０】さらに、インターコネクタ１０，１１が上
下に配置される。インターコネクタ１０，１１の材料と
しては、（Ｌａ0.7Ｃａ0.3）ＣｒＯ3の粉末と溶剤等を
混合してグリーンシート状にしたものを用いる。こうし
て組み合わされた固体電解質型燃料電池は、０．１℃／
分の昇温速度で４００℃まで加熱された後、４００℃の
温度で２時間保持され、脱脂される。その後、１３００
℃の温度まで昇温され、この温度で３時間共焼結され
る。このとき、スペーサ７，８の材料として、ＣａＴｉ
Ｏ3を用いたので、インターコネクタ１０，１１に含ま
れているＣａがスペーサ７，８へ拡散しなくなり、イン
ターコネクタ１０，１１とスペーサ７，８の接合部分に
そりや剥がれが生じなくなる。Further, the interconnectors 10 and 11 are arranged vertically. As a material for the interconnectors 10 and 11, a green sheet-like material is used by mixing (La 0.7 Ca 0.3 ) CrO 3 powder and a solvent. The solid oxide fuel cell thus combined has a temperature of 0.1 ° C /
After being heated to 400 ° C. at a heating rate of a minute, the temperature is kept at 400 ° C. for 2 hours for degreasing. Then 1300
The temperature is raised to a temperature of ° C and co-sintered at this temperature for 3 hours. At this time, CaTi is used as a material for the spacers 7 and 8.
Since O 3 is used, Ca contained in the interconnectors 10 and 11 does not diffuse into the spacers 7 and 8, and warpage or peeling does not occur at the joint portion between the interconnectors 10 and 11 and the spacers 7 and 8.

【００１１】以上のようにして作製された固体電解質型
燃料電池は、高温（６００〜１２００℃）に保持された
状態で図１中に示された矢印ａ方向から空気を供給し、
かつ、矢印ｂ方向から燃料ガスを供給することにより、
発電させることができる。なお、本発明に係る固体電解
質型燃料電池は前記実施例に限定するものではなく、そ
の要旨の範囲内で種々に変形することができる。特に、
固体電解質型燃料電池の形状は矩形状に限定されるもの
ではなく、円板状のものであってもよい。The solid oxide fuel cell manufactured as described above supplies air from the direction of arrow a shown in FIG. 1 while being maintained at a high temperature (600 to 1200 ° C.),
And by supplying the fuel gas from the direction of arrow b,
Can generate power. The solid oxide fuel cell according to the present invention is not limited to the above embodiment, but can be variously modified within the scope of the gist. In particular,
The shape of the solid oxide fuel cell is not limited to a rectangular shape, and may be a disk shape.

【００１２】[0012]

【発明の効果】以上の説明で明らかなように、本発明に
よれば、スペーサに少なくともチタン酸カルシウムを含
む材料を用いたので、共焼結の際にインターコネクタと
スペーサの接合部分にそりや剥がれが生じない固体電解
質型燃料電池が得られる。この結果、内部インピーダン
スが低い、従って発電効率が良い固体電解質型燃料電池
を共焼法にて容易に製造することができる。As is apparent from the above description, according to the present invention, since the material containing at least calcium titanate is used for the spacer, the warp or the warp is formed on the joint portion of the interconnector and the spacer during the co-sintering. A solid oxide fuel cell without peeling is obtained. As a result, a solid oxide fuel cell having a low internal impedance and therefore a high power generation efficiency can be easily manufactured by the co-firing method.

【図面の簡単な説明】[Brief description of drawings]

【図１】本発明に係る固体電解質型燃料電池の一実施例
を示す分解斜視図。FIG. 1 is an exploded perspective view showing an embodiment of a solid oxide fuel cell according to the present invention.

【符号の説明】[Explanation of symbols]

１…固体電解質 ２…空気極 ３…燃料極 ７，８…スペーサ １０，１１…インターコネクタ 1 ... Solid electrolyte 2 ... Air electrode 3 ... Fuel electrode 7,8 ... Spacer 10, 11 ... Interconnector

Claims (1)

【特許請求の範囲】[Claims] 【請求項１】 酸化ジルコニウムを主成分とする固体電
解質と、 空気極及び燃料極と、 少なくともカルシウムを含むランタンクロマイトを主成
分とするインターコネクタと、 少なくともチタン酸カルシウムを含むスペーサと、 を備えたことを特徴とする固体電解質型燃料電池。1. A solid electrolyte containing zirconium oxide as a main component, an air electrode and a fuel electrode, an interconnector containing lanthanum chromite as a main component containing at least calcium, and a spacer containing at least calcium titanate. A solid oxide fuel cell characterized by the above.
JP3301738A 1991-11-18 1991-11-18 Fuel cell with solid electrolyte Pending JPH05144463A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP3301738A JPH05144463A (en) 1991-11-18 1991-11-18 Fuel cell with solid electrolyte

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP3301738A JPH05144463A (en) 1991-11-18 1991-11-18 Fuel cell with solid electrolyte

Publications (1)

Publication Number Publication Date
JPH05144463A true JPH05144463A (en) 1993-06-11

Family

ID=17900573

Family Applications (1)

Application Number Title Priority Date Filing Date
JP3301738A Pending JPH05144463A (en) 1991-11-18 1991-11-18 Fuel cell with solid electrolyte

Country Status (1)

Country Link
JP (1) JPH05144463A (en)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0896378A1 (en) * 1997-08-08 1999-02-10 Mitsubishi Heavy Industries, Ltd. Solid electrolyte type fuel battery
JP2007207749A (en) * 2006-01-30 2007-08-16 General Electric Co <Ge> Method for manufacturing solid oxide electrochemical device and solid oxide electrochemical device
US9263749B2 (en) 2011-03-31 2016-02-16 Murata Manufacturing Co., Ltd. Fuel cell

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0896378A1 (en) * 1997-08-08 1999-02-10 Mitsubishi Heavy Industries, Ltd. Solid electrolyte type fuel battery
JP2007207749A (en) * 2006-01-30 2007-08-16 General Electric Co <Ge> Method for manufacturing solid oxide electrochemical device and solid oxide electrochemical device
US9263749B2 (en) 2011-03-31 2016-02-16 Murata Manufacturing Co., Ltd. Fuel cell

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