JPH0676836A - Manufacture of cylindrical solid electrolyte electrolytic cell - Google Patents
Manufacture of cylindrical solid electrolyte electrolytic cellInfo
- Publication number
- JPH0676836A JPH0676836A JP4225434A JP22543492A JPH0676836A JP H0676836 A JPH0676836 A JP H0676836A JP 4225434 A JP4225434 A JP 4225434A JP 22543492 A JP22543492 A JP 22543492A JP H0676836 A JPH0676836 A JP H0676836A
- Authority
- JP
- Japan
- Prior art keywords
- solid electrolyte
- films
- support tube
- film
- air
- 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
Links
- 239000007784 solid electrolyte Substances 0.000 title claims abstract description 18
- 238000004519 manufacturing process Methods 0.000 title claims description 9
- 239000000446 fuel Substances 0.000 claims abstract description 12
- 230000001590 oxidative effect Effects 0.000 claims abstract description 10
- 238000000034 method Methods 0.000 claims description 9
- 239000003792 electrolyte Substances 0.000 claims description 4
- 230000002093 peripheral effect Effects 0.000 claims description 3
- 238000010438 heat treatment Methods 0.000 abstract description 12
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 abstract description 5
- 229910002084 calcia-stabilized zirconia Inorganic materials 0.000 abstract description 3
- 230000035699 permeability Effects 0.000 abstract description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 9
- 238000010248 power generation Methods 0.000 description 5
- 229910052759 nickel Inorganic materials 0.000 description 4
- 238000007613 slurry method Methods 0.000 description 4
- 239000012528 membrane Substances 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 description 3
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 2
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000000151 deposition Methods 0.000 description 2
- 230000006866 deterioration Effects 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000007751 thermal spraying Methods 0.000 description 2
- RUDFQVOCFDJEEF-UHFFFAOYSA-N yttrium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Y+3].[Y+3] RUDFQVOCFDJEEF-UHFFFAOYSA-N 0.000 description 2
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- ODINCKMPIJJUCX-UHFFFAOYSA-N Calcium oxide Chemical compound [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 1
- 241001178829 Konia Species 0.000 description 1
- 229910002254 LaCoO3 Inorganic materials 0.000 description 1
- 229910000943 NiAl Inorganic materials 0.000 description 1
- NPXOKRUENSOPAO-UHFFFAOYSA-N Raney nickel Chemical compound [Al].[Ni] NPXOKRUENSOPAO-UHFFFAOYSA-N 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 1
- 239000000292 calcium oxide Substances 0.000 description 1
- 235000012255 calcium oxide Nutrition 0.000 description 1
- 239000011195 cermet Substances 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 230000008602 contraction Effects 0.000 description 1
- 229910052593 corundum Inorganic materials 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 238000007429 general method Methods 0.000 description 1
- 229910002085 magnesia-stabilized zirconia Inorganic materials 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 229910000480 nickel oxide Inorganic materials 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 229910001845 yogo sapphire Inorganic materials 0.000 description 1
- 229910052845 zircon Inorganic materials 0.000 description 1
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 1
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
-
- 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
Landscapes
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
- Fuel Cell (AREA)
Abstract
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や
高温水蒸気電解装置の電解セルの製造方法に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for producing a solid oxide fuel cell or an electrolytic cell for a high temperature steam electrolyzer.
【０００２】[0002]
【従来の技術】従来の円筒状固体電解質型燃料電池（以
下円筒型ＳＯＦＣと称する）においては、１本の円筒型
支持管に複数のセルを直列に接続する場合、燃料を内
側、空気を外側に流す方式が一般的であった。2. Description of the Related Art In a conventional cylindrical solid oxide fuel cell (hereinafter referred to as a cylindrical SOFC), when a plurality of cells are connected in series to one cylindrical support tube, fuel is inside and air is outside. The general method was to run it on.
【０００３】[0003]
【発明が解決しようとする課題】前述した従来の円筒状
ＳＯＦＣにおいて、固体電解質を緻密化するために熱処
理を施す場合、先ず支持管上に燃料極を成膜し、その後
に電解質を成膜した上で熱処理を行うことになる。この
際、燃料極には一般的にニッケルを使用するため、熱処
理時に溶融し空孔が閉塞するのを避けることから、一旦
酸化ニッケルとし、その後に還元してニッケルに戻す必
要がある。一方、支持管には一般的にカルシア安定化ジ
ルコニア（以下、ＣＳＺと称す）が用いられるが、ＣＳ
Ｚ管は高温で還元雰囲気に曝すと強度が低下する。この
ため、以降の製造工程において破損しやすくなり、製品
の歩留まりが低下する。In the above-mentioned conventional cylindrical SOFC, when heat treatment is performed to densify the solid electrolyte, a fuel electrode is first formed on the support tube, and then the electrolyte is formed. The heat treatment will be performed above. At this time, since nickel is generally used for the fuel electrode, it is necessary to make nickel oxide once and then reduce it back to nickel in order to avoid melting and clogging of the pores during heat treatment. On the other hand, calcia-stabilized zirconia (hereinafter referred to as CSZ) is generally used for the support tube.
When the Z tube is exposed to a reducing atmosphere at a high temperature, its strength is reduced. For this reason, it is easily damaged in the subsequent manufacturing steps, and the yield of products is reduced.
【０００４】本発明は上記技術水準に鑑み、上述したよ
うな不具合のない円筒状固体電解質型電解セルの製造方
法を提供しようとするものである。In view of the above-mentioned state of the art, the present invention aims to provide a method for producing a cylindrical solid electrolyte type electrolytic cell which does not have the above-mentioned problems.
【０００５】[0005]
【課題を解決するための手段】本発明は円筒状支持管の
外周部に、順次、高温酸化雰囲気で導電率の比較的高い
ペロブスカイト系酸化物の空気極、固体電解質を成膜し
た後、酸化雰囲気で熱処理して上記支持管、空気極及び
固体電解質を緻密化し、その後、最外層に燃料極を成膜
することを特徴とする円筒状電解質型電解セルの製造方
法である。According to the present invention, an air electrode of a perovskite oxide having a relatively high conductivity and a solid electrolyte are sequentially formed on the outer peripheral portion of a cylindrical support tube in a high temperature oxidizing atmosphere, and then oxidized. A method for producing a cylindrical electrolyte type electrolytic cell, which comprises heat-treating in an atmosphere to densify the support tube, the air electrode and the solid electrolyte, and then forming a fuel electrode on the outermost layer.
【０００６】本発明はセル構成上、カルシア安定化ジル
コニア、マグネシア安定化ジルコニア、イットリア安定
化ジルコニア、Ａｌ2 Ｏ3 などの円筒状支持管上に空気
極を成膜し、その後に固体電解質膜を成膜することによ
り、酸化雰囲気での熱処理を可能とするものである。す
なわち、前記円筒状支持管上に空気極（一般的には高温
酸化雰囲気で導電率の比較的高いペロブスカイト系酸化
物、例えばＬａＭｎＯ 3 、ＬａＣｏＯ3 、ＬａＳｒＭｎ
Ｏ3 、ＬａＣａＭｎＯ3 等が用いられる）を溶射法、ス
ラリ法等により成膜する。次に固体電解質｛例えばＹＳ
Ｚ（イットリア安定化ジルコニア）、ＣｅＯ2 、ＣａＣ
ｅＯ2 （カルシア安定化セリア）、ＹＳＢ（イットリア
安定化ビスマス）等｝を同じく溶射法、スラリ法により
成膜する。その後に、酸化雰囲気で熱処理（例えば１２
８０℃×２時間）を行うが、支持管、空気極、固体電解
質は何れも酸化物であり、安定した状態での熱処理が可
能である。その後、燃料極（例えば、ニッケル、ルテニ
ウム等）を成膜することにてＳＯＦＣのセルを構成す
る。The present invention has a cell structure in which calcia-stabilized zircon is used.
Konia, magnesia stabilized zirconia, yttria stable
Zirconia oxide, Al2O3Air on a cylindrical support tube such as
By depositing the electrode and then depositing the solid electrolyte membrane,
Therefore, heat treatment in an oxidizing atmosphere is possible. You
That is, an air electrode (generally at a high temperature
Perovskite-based oxidation with relatively high conductivity in oxidizing atmosphere
Object such as LaMnO 3, LaCoO3, LaSrMn
O3, LaCaMnO3Etc. are used)
A film is formed by a lari method or the like. Next, solid electrolyte {eg YS
Z (yttria-stabilized zirconia), CeO2, CaC
eO2(Calcia stabilized ceria), YSB (yttria
Stabilized bismuth) etc.} by the thermal spray method and slurry method
Form a film. After that, heat treatment (for example, 12
80 ℃ x 2 hours), but support tube, air electrode, solid electrolysis
All of them are oxides and can be heat-treated in a stable state.
Noh. Then the fuel electrode (for example, nickel, ruthenium
A SOFC cell by forming a film
It
【０００７】[0007]
【作用】支持管上に空気極、次に電解質を成膜した状態
で熱処理を行うことにより、下記の作用が奏される。 全て酸化物で構成されており、ニッケル等の反応を
防ぐことができる。 支持管を発電中も酸化雰囲気で使うことにより強度
低下を防ぐことができる。 溶射法等のドライプロセスで成膜した場合は、熱処
理により膜質が安定化され耐久性の向上が図られる。 各セルチューブの集電がセルの外表面で可能とな
り、余分なリード線（集電線）が不要となる。The following effects are achieved by performing heat treatment with the air electrode and then the electrolyte film formed on the support tube. Since it is composed entirely of oxide, it is possible to prevent the reaction of nickel and the like. By using the support tube in an oxidizing atmosphere even during power generation, it is possible to prevent strength deterioration. When the film is formed by a dry process such as a thermal spraying method, the heat treatment stabilizes the film quality and improves the durability. Current collection for each cell tube is possible on the outer surface of the cell, eliminating the need for extra lead wires (current collecting wires).
【０００８】[0008]
【実施例】以下、図１に示す工程図によって本発明の円
筒状固体電解質型電解セルの製造方法の一実施例を説明
する。先ず、ガス透過性を有するカルシア安定化ジルコ
ニア製円筒状支持管１の外周面上に、高温酸化雰囲気で
導電率の比較的高いペロブスカイト系酸化物（ＬａＳｒ
ＭｎＯ3 ）の空気極２を等間隔に複数個スラリ法により
成膜する。次に、セル間からのガスリークを防止するた
めに空気極２の隙間をふさぐように気密膜（例えばＡｌ
2 Ｏ3 ）３を同じくスラリ法により成膜し、さらに空気
極２上にイットリア安定化ジルコニアよりなる固体電解
質４をスラリ法によって成膜する。（以上、第１工程）EXAMPLES An example of a method for manufacturing a cylindrical solid electrolyte type electrolytic cell of the present invention will be described below with reference to the process chart shown in FIG. First, on the outer peripheral surface of a calcia-stabilized zirconia cylindrical support tube 1 having gas permeability, a perovskite oxide (LaSr) having a relatively high conductivity in a high temperature oxidizing atmosphere is used.
A plurality of air electrodes 2 of MnO 3 ) are formed at equal intervals by a slurry method. Next, in order to prevent gas leakage from between the cells, an airtight film (for example, Al
2 O 3 ) 3 is also formed by the slurry method, and further, the solid electrolyte 4 made of yttria-stabilized zirconia is formed on the air electrode 2 by the slurry method. (The above is the first step)
【０００９】次に、固体電解質４までを成膜したセルチ
ューブを約１３００℃の酸化状態で数時間加熱し、固体
電解質膜４及び気密膜３を緻密化する。ここで加熱温度
は高い程、加熱時間は長い程各膜は緻密化するが、膜の
収縮による亀裂の発生、空気極２の分解及び反応が生じ
ないよう注意する必要がある。（以上、第２工程）Next, the cell tube on which the solid electrolyte 4 is deposited is heated in an oxidized state at about 1300 ° C. for several hours to densify the solid electrolyte membrane 4 and the airtight membrane 3. Here, as the heating temperature is higher and the heating time is longer, the respective films are densified, but it is necessary to take care so that cracks due to the contraction of the films, decomposition of the air electrode 2 and reaction do not occur. (The above is the second step)
【００１０】第２工程で熱処理を施したセルは、各セル
を接続するインタコネクタ（ＮｉＡｌ）５、さらに燃料
極（Ｎｉ／ＹＳＺサーメット）６を成膜し完成する。
（以上、第３工程）The cells subjected to the heat treatment in the second step are completed by forming an interconnector (NiAl) 5 for connecting the cells and a fuel electrode (Ni / YSZ cermet) 6 as a film.
(The above is the third step)
【００１１】発電時には円筒状支持管１１の内側に空気
７を、外側に燃料８を流すようにすれば発電は良好に行
なえる。At the time of power generation, if air 7 is flown inside the cylindrical support tube 11 and fuel 8 is flown outside, power generation can be performed well.
【００１２】[0012]
【発明の効果】本発明により以下の効果が得られる。 熱処理を行う際、構成材は全て酸化物であり、安定
した状態で緻密化することができる。 支持管は製作時、発電時を含めて全て酸化状態で使
用することになり、強度低下を防ぐことができる。 固体電解質、空気極を溶射法等のドライプロセスに
より成膜した場合は、発電前にさらに高温の状態を経る
ことにより、膜質の安定化、界面状態の安定化が図ら
れ、耐久性の向上が期待できる。 各セルチューブ間の集電がセルの表面で可能とな
り、余分な集電線等が不要となる。The following effects can be obtained by the present invention. When the heat treatment is performed, the constituent materials are all oxides and can be densified in a stable state. The support tube will be used in an oxidized state during production, including during power generation, and strength deterioration can be prevented. When a solid electrolyte or an air electrode is formed by a dry process such as a thermal spraying method, the film quality is stabilized and the interface state is stabilized by passing through a higher temperature state before power generation, which improves durability. Can be expected. Current collection between each cell tube is possible on the surface of the cell, and no extra current collecting wires are needed.
【図１】本発明の円筒状固体電解質型電解セルの製造方
法の一実施例の工程図。FIG. 1 is a process drawing of an example of a method for manufacturing a cylindrical solid electrolyte type electrolytic cell of the present invention.
Claims (1)
化雰囲気で導電率の比較的高いペロブスカイト系酸化物
の空気極、固体電解質を成膜した後、酸化雰囲気で熱処
理して上記支持管、空気極及び固体電解質を緻密化し、
その後、最外層に燃料極を成膜することを特徴とする円
筒状電解質型電解セルの製造方法。1. An air electrode of a perovskite oxide having a relatively high conductivity and a solid electrolyte are sequentially formed on the outer peripheral portion of a cylindrical support tube in a high temperature oxidizing atmosphere, and then heat treated in an oxidizing atmosphere to support the above. Densify the tube, air electrode and solid electrolyte,
After that, a method for manufacturing a cylindrical electrolyte type electrolytic cell is characterized in that a fuel electrode is formed on the outermost layer.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP4225434A JPH0676836A (en) | 1992-08-25 | 1992-08-25 | Manufacture of cylindrical solid electrolyte electrolytic cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP4225434A JPH0676836A (en) | 1992-08-25 | 1992-08-25 | Manufacture of cylindrical solid electrolyte electrolytic cell |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH0676836A true JPH0676836A (en) | 1994-03-18 |
Family
ID=16829313
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP4225434A Pending JPH0676836A (en) | 1992-08-25 | 1992-08-25 | Manufacture of cylindrical solid electrolyte electrolytic cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0676836A (en) |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5496655A (en) * | 1994-10-12 | 1996-03-05 | Lockheed Idaho Technologies Company | Catalytic bipolar interconnection plate for use in a fuel cell |
| JPH08269760A (en) * | 1995-03-29 | 1996-10-15 | Agency Of Ind Science & Technol | Cylindrical high-temperature steam electrolytic cell |
| WO1998013892A1 (en) * | 1996-09-26 | 1998-04-02 | Wolfgang Winkler | Fuel cell installation with tubular high temperature fuel cells |
| US7045243B2 (en) * | 2001-05-22 | 2006-05-16 | Nissan Motor Co., Ltd. | Cell plate structure for fuel cell, manufacturing method thereof and solid electrolyte type fuel cell |
| JP2012038583A (en) * | 2010-08-06 | 2012-02-23 | Ngk Insulators Ltd | Structure of fuel cell |
| EP2721667A4 (en) * | 2011-06-15 | 2016-01-27 | Lg Fuel Cell Systems Inc | FUEL CELL SYSTEM WITH INTERCONNECTION PLATE |
-
1992
- 1992-08-25 JP JP4225434A patent/JPH0676836A/en active Pending
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5496655A (en) * | 1994-10-12 | 1996-03-05 | Lockheed Idaho Technologies Company | Catalytic bipolar interconnection plate for use in a fuel cell |
| JPH08269760A (en) * | 1995-03-29 | 1996-10-15 | Agency Of Ind Science & Technol | Cylindrical high-temperature steam electrolytic cell |
| WO1998013892A1 (en) * | 1996-09-26 | 1998-04-02 | Wolfgang Winkler | Fuel cell installation with tubular high temperature fuel cells |
| US7045243B2 (en) * | 2001-05-22 | 2006-05-16 | Nissan Motor Co., Ltd. | Cell plate structure for fuel cell, manufacturing method thereof and solid electrolyte type fuel cell |
| JP2012038583A (en) * | 2010-08-06 | 2012-02-23 | Ngk Insulators Ltd | Structure of fuel cell |
| EP2721667A4 (en) * | 2011-06-15 | 2016-01-27 | Lg Fuel Cell Systems Inc | FUEL CELL SYSTEM WITH INTERCONNECTION PLATE |
| US9531013B2 (en) | 2011-06-15 | 2016-12-27 | Lg Fuel Cell Systems Inc. | Fuel cell system with interconnect |
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