JP2622261B2 - Method for manufacturing solid electrolyte fuel cell - Google Patents
Method for manufacturing solid electrolyte fuel cellInfo
- Publication number
- JP2622261B2 JP2622261B2 JP62249948A JP24994887A JP2622261B2 JP 2622261 B2 JP2622261 B2 JP 2622261B2 JP 62249948 A JP62249948 A JP 62249948A JP 24994887 A JP24994887 A JP 24994887A JP 2622261 B2 JP2622261 B2 JP 2622261B2
- Authority
- JP
- Japan
- Prior art keywords
- fuel cell
- air electrode
- layer
- solid electrolyte
- electrode layer
- 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 - Lifetime
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
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M8/1231—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte with both reactants being gaseous or vaporised
-
- 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
-
- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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、酸素センサなどに使用される固体
電解質燃料電池の製作方法に関する。The present invention relates to a method for manufacturing a solid electrolyte fuel cell used for a fuel cell, an oxygen sensor, and the like.
従来の固体電解質燃料電池の構成を第３図、第４図に
よつて説明する。第３図はその断面図であり、第４図は
第３図のＢ−Ｂ矢視図である。The configuration of a conventional solid oxide fuel cell will be described with reference to FIGS. 3 and 4. FIG. FIG. 3 is a cross-sectional view, and FIG. 4 is a view taken along the line BB of FIG.
第３図、第４図において、１は空気極（一例として
は、LaMnO3のペロプスカイト型酸化物スラリーの焼成膜
で、厚さは数百μｍである気体を通す多孔質膜があげら
れる）、２は電解質（一例としては、イツトリア安定化
ジルコニアYSZの蒸着膜で、電気化学蒸着法、すなわちE
VD法、で作られた50μｍ程度の気密膜）、３は燃料極
（一例としてはNiOとZrO2のサーメツトのスラリー焼成
膜で厚さ数十μｍの多孔質膜）、４はインコネクタ（一
例としてはLaCrO3のEVD法による蒸着膜で厚さ数十μｍ
の気密膜）、５は基体管（一例としてはカルシア安定化
ジルコニアで作られた直径13mm、長さ400mm、厚さ1.6mm
の多孔質セラミツクチユーブ）である。3 and 4, reference numeral 1 denotes an air electrode (as an example, a fired film of a perovskite-type oxide slurry of LaMnO 3 , which is a porous film through which a gas having a thickness of several hundred μm is passed) Reference numeral 2 denotes an electrolyte (for example, a deposited film of yttria-stabilized zirconia YSZ.
3 is a fuel electrode (as an example, a slurry film of cermet slurry of NiO and ZrO 2 with a thickness of several tens of μm) 4 is an in-connector (as an example) Is several tens of μm in thickness by evaporation of LaCrO 3 by the EVD method.
5 is a base tube (13mm in diameter, 400mm in length, 1.6mm in thickness made of calcia stabilized zirconia as an example)
Is a porous ceramic tube).
約1,000℃に保持された上記構成の固体電解質燃料電
池の管内外に、空気とH2,COの燃料を供給すると、燃料
極３でH2,COがNiの触媒作用によりイオン化して電子を
放つ。これにより燃料極３と空気極１との間に電位差が
生じる。今、燃料極３と空気極１をインコネクタ４を介
して外部回路で連ぐと、燃料極３にたまつた電子は外部
回路とインコネクタ４を通つて空気極１へ移動し、基体
管５を通つてきた空気中の酸素をイオン化する。イオン
化した酸素は酸素イオン導電性の電解質２を通つて燃料
極３へ移動し水素イオンと結合して水蒸気となる。When air and H 2 , CO fuel are supplied inside and outside the solid electrolyte fuel cell tube maintained at about 1,000 ° C., H 2 , CO is ionized by the catalytic action of Ni at the fuel electrode 3 to convert electrons. Release. This causes a potential difference between the fuel electrode 3 and the air electrode 1. Now, when the fuel electrode 3 and the air electrode 1 are connected to each other by an external circuit via the in-connector 4, the electrons accumulated at the fuel electrode 3 move to the air electrode 1 through the external circuit and the in-connector 4, and the substrate tube The oxygen in the air passing through 5 is ionized. The ionized oxygen moves to the fuel electrode 3 through the oxygen ion conductive electrolyte 2 and combines with hydrogen ions to form water vapor.
従来の技術では基体管を用いているので、製作可能な
基体管径に限界があり、あまり小さい径の燃料電池や酸
素センサーは製作できない。このため例えば容積当りの
固体電解質燃料電池の発電量は140KW/m3程度であり、大
容量化した場合のスペースが大きくなりすぎ、また基体
管が空気の拡散抵抗となるため電池出力が低下するとい
う問題点がある。In the prior art, since the base tube is used, there is a limit in the base tube diameter that can be manufactured, and a fuel cell or an oxygen sensor having a too small diameter cannot be manufactured. For this reason, for example, the power generation amount of the solid electrolyte fuel cell per volume is about 140 KW / m 3 , the space becomes too large when the capacity is increased, and the cell output decreases because the base tube becomes a diffusion resistance of air. There is a problem.
本発明は上記技術水準に鑑み、従来技術の有する問題
点を解消した固体電解質燃料電池の製作方法を提供しよ
うとするものである。The present invention has been made in view of the above-mentioned state of the art, and an object of the present invention is to provide a method of manufacturing a solid oxide fuel cell which has solved the problems of the prior art.
本発明は電解質層を挟んで燃料極層と空気極層とが重
ね合わされた筒状の固体電解質燃料電池を製作する方法
であつて、上記空気極層か燃料極層かのいずれか一方の
層を構成する材料の粉末スラリーを成形して筒状物と
し、上記電解質層および他の極層を構成するそれぞれの
材料の粉末スラリーを未焼成の状態の上記筒状物表面に
順次塗布乾燥させた後、焼成することを特徴とする固体
電解質燃料電池の製作方法である。The present invention relates to a method for manufacturing a cylindrical solid electrolyte fuel cell in which a fuel electrode layer and an air electrode layer are overlapped with an electrolyte layer interposed therebetween, and wherein either one of the air electrode layer and the fuel electrode layer is provided. The powder slurry of the material constituting the material was formed into a tubular material, and the powder slurry of each material constituting the electrolyte layer and the other electrode layer was sequentially applied to the surface of the unbaked tubular material and dried. Thereafter, firing is performed, followed by firing.
本発明における空気極層として使用される材料として
は、LaCaMnO3,LaCoO3,LaCrO3及びLaMnO3などのペロブス
カイト型酸化物が、電解質層となる材料としてはイツト
リア安定化ジルコニア（YSZ）,CeCaなどが、燃料極層と
して使用される材料としてはNiO/カルシア安定化ジルコ
ニア（CSZ）,NiO/イツトリア安定化ジルコニア（YSZ）
などがあげられる。またインコネクターが使用される
が、この材料としてはNiAl/Al2O3＋NiCr/Al2O3,FeNiCo,
LaCrO3などがあげられる。Materials used as the air electrode layer in the present invention include perovskite oxides such as LaCaMnO 3 , LaCoO 3 , LaCrO 3 and LaMnO 3, and materials used as the electrolyte layer include yttria-stabilized zirconia (YSZ) and CeCa However, the materials used for the fuel electrode layer are NiO / calcia stabilized zirconia (CSZ) and NiO / yttria stabilized zirconia (YSZ)
And so on. An in-connector is used, and the material is NiAl / Al 2 O 3 + NiCr / Al 2 O 3 , FeNiCo,
LaCrO 3 and the like.
空気極層、燃料極層は多孔質なものとする必要がある
ので、その材料の粒径は比較的大きい（例えば１〜100
μ程度）材料をスラリー化して用いられ、インコネクタ
ー、電解質層は緻密質とする必要があるので、その材料
の粒径は比較的小さい（例えば0.1〜１μ程度）材料を
スラリー化して用いられる。Since the air electrode layer and the fuel electrode layer need to be porous, the particle size of the material is relatively large (for example, 1 to 100).
The material is used in the form of a slurry, and the interconnector and the electrolyte layer need to be dense. Therefore, the material having a relatively small particle size (for example, about 0.1 to 1 μ) is used in the form of a slurry.
一例として、空気極を筒状に成形し最内層にする場合
の、それぞれの層の一般的な材料の粒径、スラリー粘
度、スラリー濃度を下記に示す。As an example, the particle diameter, slurry viscosity, and slurry concentration of general materials of each layer in the case where the air electrode is formed into a cylindrical shape to be the innermost layer are shown below.
空気極を筒状に成形し最内層とする場合、空気極とな
る材料の導電率が低い場合には膜厚を厚くしなければな
らぬが、膜厚を厚くすると酸素の拡散が不十分となるの
で両者の兼ね合いでその膜厚を決定すべきである。 When the air electrode is formed into a cylindrical shape and used as the innermost layer, the thickness must be increased if the material of the air electrode is low in conductivity, but if the thickness is increased, diffusion of oxygen is insufficient. Therefore, the film thickness should be determined in consideration of both.
また筒状に成形して最内層とするのが、空気極であつ
ても、また燃料極であつても、その強度の点から、その
膜厚は300μ以上にするのが好ましい。Regardless of whether it is an air electrode or a fuel electrode formed into a cylindrical shape to form the innermost layer, it is preferable that the film thickness be 300 μm or more from the viewpoint of strength.
一般的に空気極は1000℃以上、燃料極は1300℃以上、
電解質及びインコネクターは1300℃以上で焼成される
が、本発明においては構成材料を一度で焼結するため
に、焼成温度は少なくとも1300℃以上にするべきであ
る。Generally, the air electrode is over 1000 ℃, the fuel electrode is over 1300 ℃,
The electrolyte and the interconnector are fired at 1300 ° C. or higher, but in the present invention, the firing temperature should be at least 1300 ° C. in order to sinter the constituent materials at one time.
本発明によれば基体管の使用を排除しているので小型
の固体電解質燃料電池が得られ、そのため例えば5mmの
直径の電池を作ることができ、その場合従来の直径15mm
の電池に比べて容積当りの発電量は９倍になり、また直
径3mmの電池を作れば、直径15mmの従来電池の発電量の2
5倍となる。また基体管がないため空気が空気極へ拡散
しやすく空気極の酸素分圧が増加して電池出力が増加す
る。According to the present invention, the use of a base tube is eliminated, so that a small solid electrolyte fuel cell can be obtained, so that a cell having a diameter of, for example, 5 mm can be produced, in which case a conventional diameter of 15 mm is used.
The amount of power generation per volume is 9 times that of a conventional battery, and if a 3 mm diameter battery is made, the power generation of a 15 mm diameter conventional battery is
5 times. Further, since there is no base tube, air is easily diffused to the air electrode, and the oxygen partial pressure of the air electrode increases, so that the battery output increases.
〔実施例１〕 以下、本発明の一実施例を第１図及び第２図によつて
説明する。第１図はこの実施例によつて製作された固体
電解質燃料電池の断面図であり、第２図は第１図のＡ−
Ａ矢視図である。この実施例においては、１は空気極、
２は電解質、３は燃料極、４はインコネクターである。Embodiment 1 Hereinafter, an embodiment of the present invention will be described with reference to FIG. 1 and FIG. FIG. 1 is a sectional view of a solid oxide fuel cell manufactured according to this embodiment, and FIG.
FIG. In this embodiment, 1 is an air electrode,
2 is an electrolyte, 3 is a fuel electrode, and 4 is an in-connector.
先ず、LaMnO3粒子（１〜10μ）の70％濃度のスラリー
（粘度∞）をプレスまたは押出し成形機で厚さ500μの
円筒形多孔質管に成形し空気極１を形成する。First, a slurry (viscosity の) of 70% concentration of LaMnO 3 particles (1 to 10 μ) is formed into a cylindrical porous tube having a thickness of 500 μ by a press or an extruder to form an air electrode 1.
次に、イツトリア安定化ジルコニア（YSZ）粒子（0.1
〜１μ）の50％濃度スラリー（粘度1000cp）を空気極１
上に塗布乾燥して厚さ150μの電解質層２を形成し、更
にその電解質層２の上に、NiO/YSZ（6:4）粒子（１〜10
μ）の60％濃度スラリー（粘度1000cp）を塗布乾燥し厚
さ100μの燃料極層３を形成させる。次いで最後にLaCrO
3粒子（0.1〜１μ）の50％濃度スラリーを、第１図に示
すように露出している空気極１上に塗布乾燥し厚さ100
μのインコネクター４を形成させる。Next, the yttria stabilized zirconia (YSZ) particles (0.1
~ 1μ) 50% concentration slurry (viscosity 1000cp)
On the electrolyte layer 2, a 150 μm thick electrolyte layer 2 is formed by coating and drying, and NiO / YSZ (6: 4) particles (1 to 10
μ) of 60% concentration (viscosity: 1000 cp) is applied and dried to form a fuel electrode layer 3 having a thickness of 100 μ. Then finally LaCrO
A 50% concentration slurry of three particles (0.1 to 1 μm) is applied and dried on the exposed air electrode 1 as shown in FIG.
The μ in connector 4 is formed.
上記したように構成された未焼成の成形体を1300℃以
上で２〜４時間焼成することによつて空気極を最内層と
して有し基体管を省略した固体電解質燃料電池が得られ
る。By firing the unsintered compact having the above-mentioned structure at 1300 ° C. or higher for 2 to 4 hours, a solid electrolyte fuel cell having an air electrode as the innermost layer and omitting the base tube is obtained.
〔実施例２〕 他の実施例を同様に第１図及び第２図によつて説明す
る。この場合、第１図、第２図における１は燃料極、２
は電解質、３は空気極、４はインコネクターである。Embodiment 2 Another embodiment will be described with reference to FIGS. 1 and 2. FIG. In this case, 1 in FIG. 1 and FIG.
Is an electrolyte, 3 is an air electrode, and 4 is an in connector.
先ずNiO/YSZ（6:4）粒子（１〜10μ）の70％濃度スラ
リー（粘度∞）をプレスまたは押出し成形機で厚さ500
μの円筒形多孔質管に成形し燃料極１を成形する。First, a 70% strength slurry (viscosity の) of NiO / YSZ (6: 4) particles (1 to 10μ) is pressed or extruded to a thickness of 500 mm.
The fuel electrode 1 is formed by molding into a cylindrical porous tube of μ.
次に、イツトリア安定化ジルコニア（YSZ）粒子（0.1
〜１μ）の50％濃度スラリー（粘度1000cp）を燃料極１
の上に塗布乾燥し厚さ150μの電解質層２を形成し、更
にその電解質層２の上に、LaMnO3粒子（１〜10μ）の60
％濃度スラリー（粘度1000cp）を塗布乾燥し、厚さ300
μの空気極層３を形成させる。次いで最後にLaCrO3粒子
（0.1〜１μ）の50％濃度スラリーを、第１図に示すよ
うに露出している燃料極１上に塗布乾燥し厚さ100μの
インコネクター４を形成させる。Next, the yttria stabilized zirconia (YSZ) particles (0.1
~ 1μ) 50% concentration slurry (viscosity 1000cp)
Is applied and dried to form an electrolyte layer 2 having a thickness of 150 μm. Further, on the electrolyte layer 2, 60 μm of LaMnO 3 particles (1 to 10 μm) are formed.
% Concentration slurry (viscosity 1000cp)
The air electrode layer 3 of μ is formed. Next, a 50% concentration slurry of LaCrO 3 particles (0.1 to 1 μm) is applied and dried on the exposed fuel electrode 1 as shown in FIG. 1 to form an interconnector 4 having a thickness of 100 μm.
上記したように構成された未焼成の成形体を1300℃以
上で２〜４時間焼成することによつて燃料極を最内層と
して有し基体管を省略した固体電解質燃料電池が得られ
る。By firing the unsintered molded body having the above structure at 1300 ° C. or higher for 2 to 4 hours, a solid electrolyte fuel cell having a fuel electrode as the innermost layer and omitting the base tube is obtained.
基体管がないため電池直径を小さくすることができま
た、空気の拡散抵抗が減つて空気極への空気の拡散が容
易となるため空気極の酸素分圧が増加して電池出力が増
加する。Since there is no base tube, the diameter of the battery can be reduced, and the diffusion resistance of the air decreases, and the diffusion of the air to the air electrode becomes easy. Therefore, the oxygen partial pressure of the air electrode increases, and the battery output increases.
第１図、第２図は本発明の固体電解質燃料電池の実施例
を説明するための図で、第１図は固体電解質燃料電池の
断面図、第２図は第１図のＡ−Ａ矢視図である。第３
図、第４図は従来の固体電解質燃料電池の構成を説明す
るための図で、第３図はその断面図、第４図は第３図の
Ｂ−Ｂ矢視図である。1 and 2 are views for explaining an embodiment of a solid electrolyte fuel cell according to the present invention. FIG. 1 is a cross-sectional view of the solid electrolyte fuel cell, and FIG. 2 is an arrow AA in FIG. FIG. Third
FIG. 4 is a view for explaining the configuration of a conventional solid oxide fuel cell, FIG. 3 is a cross-sectional view thereof, and FIG. 4 is a view taken along the line BB of FIG.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 玄後 義 長崎県長崎市飽の浦町１番１号 三菱重 工業株式会社長崎造船所内 (56)参考文献 特開 昭63−261679（ＪＰ，Ａ) 特公 昭45−14730（ＪＰ，Ｂ２) 特公 昭45−33982（ＪＰ，Ｂ２) ──────────────────────────────────────────────────続 き Continuation of the front page (72) Inventor Yoshiyoshi Gengo 1-1, Akunouramachi, Nagasaki City, Nagasaki Prefecture Mitsubishi Heavy Industries, Ltd. Nagasaki Shipyard (56) References JP-A-63-261679 (JP, A) JP 4514730 (JP, B2) JP 45-33982 (JP, B2)
Claims (1)
重ね合わされた筒状の固体電解質燃料電池を製作する方
法であって、上記空気極層か燃料極層かのいずれか一方
の層を構成する材料の粉末スラリーを成形して筒状物と
し、上記電解質層および他の極層を構成するそれぞれの
材料の粉末スラリーを未焼成の状態の上記筒状物表面に
順次塗布乾燥させた後、焼成することを特徴とする固体
電解質燃料電池の製作方法。1. A method for producing a cylindrical solid electrolyte fuel cell in which a fuel electrode layer and an air electrode layer are overlapped with an electrolyte tank interposed therebetween, wherein one of the air electrode layer and the fuel electrode layer is provided. The powder slurry of the material constituting the layer is formed into a cylindrical material, and the powder slurry of each material constituting the electrolyte layer and the other electrode layer is sequentially applied and dried on the surface of the unfired cylindrical material. A method for producing a solid oxide fuel cell, which comprises firing after firing.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62249948A JP2622261B2 (en) | 1987-10-05 | 1987-10-05 | Method for manufacturing solid electrolyte fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62249948A JP2622261B2 (en) | 1987-10-05 | 1987-10-05 | Method for manufacturing solid electrolyte fuel cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH0193065A JPH0193065A (en) | 1989-04-12 |
| JP2622261B2 true JP2622261B2 (en) | 1997-06-18 |
Family
ID=17200563
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP62249948A Expired - Lifetime JP2622261B2 (en) | 1987-10-05 | 1987-10-05 | Method for manufacturing solid electrolyte fuel cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2622261B2 (en) |
Families Citing this family (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH0697613B2 (en) * | 1990-07-12 | 1994-11-30 | 日本碍子株式会社 | Method for producing air electrode material for solid oxide fuel cell |
| JPH04115461A (en) * | 1990-09-03 | 1992-04-16 | Mitsui Eng & Shipbuild Co Ltd | Preparation method of single cell of solid-electrolyte-type fuel battery |
| EP0514552B1 (en) * | 1990-12-10 | 2000-05-17 | Yuasa Corporation | Method for manufacturing solid-state electrolytic fuel cell |
| EP0714104A1 (en) * | 1994-03-18 | 1996-05-29 | Toto Ltd. | Thin solid electrolyte film and method of production thereof |
| WO1999054946A1 (en) | 1998-04-21 | 1999-10-28 | Toto Ltd. | Solid electrolyte fuel cell and method of producing the same |
| NL1014284C2 (en) * | 2000-02-04 | 2001-08-13 | Stichting Energie | A method of manufacturing an assembly comprising an anode-supported electrolyte and a ceramic cell comprising such an assembly. |
| JP4622146B2 (en) * | 2001-04-25 | 2011-02-02 | 株式会社デンソー | Method for manufacturing gas sensor element |
-
1987
- 1987-10-05 JP JP62249948A patent/JP2622261B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0193065A (en) | 1989-04-12 |
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