JP3050331B2 - Method for manufacturing solid electrolyte fuel cell - Google Patents
Method for manufacturing solid electrolyte fuel cellInfo
- Publication number
- JP3050331B2 JP3050331B2 JP3029539A JP2953991A JP3050331B2 JP 3050331 B2 JP3050331 B2 JP 3050331B2 JP 3029539 A JP3029539 A JP 3029539A JP 2953991 A JP2953991 A JP 2953991A JP 3050331 B2 JP3050331 B2 JP 3050331B2
- Authority
- JP
- Japan
- Prior art keywords
- solid electrolyte
- air electrode
- fuel cell
- molded article
- composite
- 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
- H01M8/10—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
【０００１】[0001]
【産業上の利用分野】本発明は、固体電解質燃料電池の
製造方法に関するものである。The present invention relates to a method for manufacturing a solid oxide fuel cell.
【０００２】[0002]
【従来の技術】固体電解質燃料電池としては、リン酸型
燃料電池、溶融炭酸塩型燃料電池と類似した構造の平板
型、米国のアルゴンヌ国立研究所によって提案されたモ
ノリシック型、日本の電子技術総合研究所によって開発
中の円筒多素子型、米国のウェスティングハウス社によ
って提案された円筒単素子型が知られているが、現在は
高温におけるガスシールの容易さ、スタック構成の容易
さの点でウェスティングハウス社の円筒単素子型が注目
されている。2. Description of the Related Art Solid electrolyte fuel cells include a phosphoric acid type fuel cell, a flat type having a structure similar to that of a molten carbonate type fuel cell, a monolithic type proposed by the Argonne National Laboratory in the United States, and a Japanese electronic technology. The cylindrical multi-element type under development by the research institute and the cylindrical single-element type proposed by Westinghouse of the United States are known, but the Westin is now easy to use in terms of gas sealing at high temperatures and ease of stacking. Ghaus's cylindrical single-element type is drawing attention.
【０００３】このような固体電解質燃料電池に用いられ
る固体電解質の製造方法としては、プラズマ溶射法、化
学蒸着法（ＣＶＤ）、電気化学蒸着法（ＥＶＤ）、有機
金属ジルコニム塩の熱分解法などが知られているが、緻
密な固体電解質膜が得られる方法としては、プラズマ溶
射法、電気化学蒸着法（ＥＶＤ）があるのみである。As a method for producing a solid electrolyte used in such a solid electrolyte fuel cell, there are a plasma spraying method, a chemical vapor deposition method (CVD), an electrochemical vapor deposition method (EVD), a thermal decomposition method of an organometallic zirconium salt, and the like. As is known, only a plasma spraying method and an electrochemical vapor deposition (EVD) method can be used to obtain a dense solid electrolyte membrane.
【０００４】さらに、上記のような緻密な固体電解質膜
を作成する方法としては、図８のように安定化ジルコニ
ア粉末３をスラリーにし、基材１上に塗布して焼成する
試みもなされている。Further, as a method for producing a dense solid electrolyte membrane as described above, an attempt has been made to make the stabilized zirconia powder 3 into a slurry as shown in FIG. .
【０００５】[0005]
【発明が解決しようとする課題】上記した前者の製造方
法では、高価な製造装置を必要とするうえに、固体電解
質膜を必要とする部分と必要としない部分とを構成する
マスキングに時間がかかるため、電池の量産性に問題が
あった。In the former manufacturing method, an expensive manufacturing apparatus is required, and it takes a long time to form a portion that requires a solid electrolyte membrane and a portion that does not require a solid electrolyte membrane. Therefore, there was a problem in mass productivity of the battery.
【０００６】また、後者の製造方法では、焼成時に安定
化ジルコニア粉末３の粒子が収縮するため、基材１の上
に構成された固体電解質膜８に割れ２を生じたり、固体
電解質膜８が剥離するという問題があった。In the latter manufacturing method, the particles of the stabilized zirconia powder 3 shrink during firing, so that the solid electrolyte membrane 8 formed on the substrate 1 is cracked 2 or the solid electrolyte membrane 8 is There was a problem of peeling.
【０００７】[0007]
【課題を解決するための手段】上記課題を解決するた
め、本発明は安定化剤を添加したジルコニアを含有する
スラリーを、吸水性を有する型に流し込んで電解質成形
体とする工程と、金属酸化物を含有するスラリーを、前
記電解質成形体上に流し込んで空気極成形体とし、電解
質成形体と空気極成形体とを一体化した複合成形体を得
る工程と、この複合成形体から前記型を除去した後焼成
して固体電解質−空気極複合体とする工程と、この固体
電解質−空気極複合体の固体電解質側に燃料極を形成す
る工程とからなることを特徴とするものである。SUMMARY OF THE INVENTION In order to solve the above-mentioned problems, the present invention provides a step of pouring a slurry containing zirconia to which a stabilizer is added into a mold having a water absorbing property to form an electrolyte molded article; A slurry containing the product is poured onto the electrolyte molded body to form an air electrode molded body, and a step of obtaining a composite molded body obtained by integrating the electrolyte molded body and the air electrode molded body; and forming the mold from the composite molded body. It is characterized by comprising a step of removing and firing to form a solid electrolyte-air electrode composite, and a step of forming a fuel electrode on the solid electrolyte side of the solid electrolyte- air electrode composite.
【０００８】[0008]
【作用】上記のように、本発明は吸水性を有する型にス
ラリーを流し込んで電解質成形体と空気極成形体とを構
成してこれらを同時に焼成しているので、緻密な固体電
解質膜と多孔性の空気極とを容易に形成することがで
き、その厚みもスラリーを流す時間によって任意にコン
トロールすることができる。As described above, according to the present invention, the slurry is poured into a water-absorbing mold to form the electrolyte molded body and the air electrode molded body, which are simultaneously fired. The air electrode can be easily formed, and its thickness can be arbitrarily controlled by the time for flowing the slurry.
【０００９】また、前記スラリーから構成される空気極
成形体は、焼成することによって空気極の強度が高まり
基材としての作用もする。Further, the air electrode molded body composed of the slurry is fired to increase the strength of the air electrode, and also acts as a base material.
【００１０】[0010]
【実施例】図１は、本発明の固体電解質燃料電池の製造
方法に使用する型４の断面図で、石膏のような吸水性を
有する材料からなる。FIG. 1 is a cross-sectional view of a mold 4 used in the method of manufacturing a solid oxide fuel cell according to the present invention, which is made of a material having water absorbency such as gypsum.
【００１１】図２は、前記型４に安定化剤としてのイッ
トリアを添加したジルコニア粉末、水、分散剤、バイン
ダー、消泡剤からなるスラリーを流し込んで一定時間放
置して電解質成形体５とした後、余剰のスラリーを除去
した状態の断面図である。なお、上記スラリーには粒径
の小さいジルコニア粉末を含有させ、分散剤を添加する
ことにより、後述する焼成によって緻密な固体電解質膜
を形成することができ、ジルコニア粉末中の立方晶ジル
コニアを増加させることにより、固体電解質膜の電気抵
抗を小さくすることができ、正方晶ジルコニアを増加さ
せることにより、固体電解質膜の強度を高くすることが
できる。FIG. 2 shows that a slurry composed of zirconia powder containing yttria as a stabilizer, water, a dispersant, a binder, and an antifoaming agent is poured into the mold 4 and left for a predetermined time to form an electrolyte molded body 5. FIG. 7 is a cross-sectional view of a state where excess slurry has been removed. Note that the slurry contains zirconia powder having a small particle diameter, and by adding a dispersant, a dense solid electrolyte membrane can be formed by sintering described below, and cubic zirconia in the zirconia powder is increased. Thus, the electric resistance of the solid electrolyte membrane can be reduced, and the strength of the solid electrolyte membrane can be increased by increasing tetragonal zirconia.
【００１２】図３は、前記スラリーにストロンチウムを
ドープしたＬａＭｎＯ3 を添加したスラリーを、前記電
解質成形体５が乾燥するまでに、その上に流し込んで一
定時間放置して空気極成形体６とした後、余剰のスラリ
ーを除去した状態の断面図である。なお、この空気極成
形体６を形成するためのスラリーと電解質成形体５を形
成するためのスラリーとは同一のものでなくてもよいこ
とは言うまでもないが、ジルコニア粉末やＬａＭｎＯ3
粉末の粒径を大きくすることにより、後述する焼成によ
って多孔性の空気極を形成することができる。FIG. 3 shows that the slurry obtained by adding LaMnO 3 doped with strontium to the slurry is poured onto the electrolyte molded body 5 and dried for a certain period of time until the electrolyte molded body 5 is dried to form an air electrode molded body 6. FIG. 7 is a cross-sectional view of a state where excess slurry has been removed. It is needless to say that the slurry for forming the air electrode molded body 6 and the slurry for forming the electrolyte molded body 5 need not be the same, but zirconia powder or LaMnO 3
By increasing the particle size of the powder, a porous air electrode can be formed by firing described below.
【００１３】図４は、図３の状態のものを乾燥させて型
４を除去した後焼成して得た固体電解質−空気極複合体
の断面図で、内側に多孔性の空気極７が形成され、外側
に緻密な固体電解質膜８が形成される。FIG. 4 is a cross-sectional view of the solid electrolyte-air electrode composite obtained by drying the state shown in FIG. 3, removing the mold 4, and then sintering. As a result, a dense solid electrolyte membrane 8 is formed on the outside.
【００１４】図５は、前記固体電解質−空気極複合体の
固体電解質膜８側に燃料極９として、Ｎｉ−ＺｒＯ2 サ
ーメットをディッピング法によって形成した状態の断面
図、すなわち本発明の製造方法によって得られた固体電
解質燃料電池の断面図である。なお、燃料極９の形成方
法としては、ディッピング法以外にスラリー塗布法、溶
射法等がある。FIG. 5 shows the solid electrolyte-air electrode composite.
FIG. 3 is a cross-sectional view of a state in which a Ni—ZrO 2 cermet is formed as a fuel electrode 9 on a solid electrolyte membrane 8 side by a dipping method, that is, a cross-sectional view of a solid electrolyte fuel cell obtained by a manufacturing method of the present invention. In addition, as a method of forming the fuel electrode 9, there are a slurry coating method, a thermal spraying method and the like other than the dipping method.
【００１５】こうして得られた図５のような固体電解質
燃料電池を作動温度である７００℃から１０００℃に昇
温し、空気極７側に空気を、燃料極９側に燃料を供給す
ると、燃料によって燃料極９中の酸化ニッケルが還元さ
れる。The solid electrolyte fuel cell thus obtained as shown in FIG. 5 is heated from an operating temperature of 700 ° C. to 1000 ° C., and air is supplied to the air electrode 7 side and fuel is supplied to the fuel electrode 9 side. As a result, nickel oxide in the fuel electrode 9 is reduced.
【００１６】従って、図５の燃料極９と空気極７とを外
部回路に接続すると、空気極７から取り入れられた酸素
は外部回路から供給される電子を取り込んで酸素イオン
となり、この酸素イオンは固体電解質膜８を通って固体
電解質膜８と燃料極９との界面に到達する。Therefore, when the fuel electrode 9 and the air electrode 7 shown in FIG. 5 are connected to an external circuit, oxygen taken in from the air electrode 7 takes in electrons supplied from the external circuit to become oxygen ions, and this oxygen ion is It reaches the interface between the solid electrolyte membrane 8 and the fuel electrode 9 through the solid electrolyte membrane 8.
【００１７】一方、この界面には燃料極９中を拡散して
きた水素もしくは一酸化炭素が存在し、この水素もしく
は一酸化炭素と前記酸素イオンとが反応して水蒸気およ
び二酸化炭素を生成するとともに、外部回路に電子を放
出するので、外部回路には空気極７を正極、燃料極９を
負極とした起電力が生じ、電池としての作用がなされる
ことになる。On the other hand, hydrogen or carbon monoxide diffused in the fuel electrode 9 is present at this interface, and the hydrogen or carbon monoxide reacts with the oxygen ions to generate water vapor and carbon dioxide. Since the electrons are emitted to the external circuit, an electromotive force is generated in the external circuit with the air electrode 7 as a positive electrode and the fuel electrode 9 as a negative electrode, thereby acting as a battery.
【００１８】以上の説明は、型４が円筒型複合成形体を
製造するためのものであったが、図６のような型４を使
用すれば平板型の複合成形体を、図７のような型４を使
用すればモノリシック型の複合成形体を製造できること
は言うまでもない。In the above description, the mold 4 is for producing a cylindrical composite molded article. However, if the mold 4 as shown in FIG. 6 is used, a flat composite molded article can be obtained as shown in FIG. It is needless to say that a monolithic composite molded article can be manufactured by using a simple mold 4.
【００１９】[0019]
【発明の効果】上記した如く、本発明は緻密な固体電解
質膜８と多孔性の空気極７とが容易に形成でき、その厚
みもスラリーを流す時間によって任意にコントロールす
ることができ、スラリー中のジルコニア粉末に添加する
安定化剤の種類や量を変化させることによって固体電解
質膜８の抵抗と機械的強度とをコントロールすることが
できるので、容易に高性能な固体電解質燃料電池を得る
ことができる。As described above, according to the present invention, a dense solid electrolyte membrane 8 and a porous air electrode 7 can be easily formed, and the thickness thereof can be arbitrarily controlled by the time of flowing the slurry. Since the resistance and mechanical strength of the solid electrolyte membrane 8 can be controlled by changing the type and amount of the stabilizer added to the zirconia powder, it is possible to easily obtain a high-performance solid electrolyte fuel cell. it can.
【００２０】また、吸水性を有する型４にスラリーを流
し込んで電解質成形体５と空気極成形体６とを構成して
焼成しているので、製造工程の簡素化を図ることができ
る。Also, since the slurry is poured into the water-absorbing mold 4 to form the electrolyte molded body 5 and the air electrode molded body 6 and fired, the manufacturing process can be simplified.
【図１】本発明の固体電解質燃料電池の製造方法に使用
する型４の断面図である。FIG. 1 is a cross-sectional view of a mold 4 used in a method for manufacturing a solid oxide fuel cell according to the present invention.
【図２】図１の型４にスラリーを流し込んで一定時間放
置して電解質成形体５とした後、余剰のスラリーを除去
した状態の断面図である。FIG. 2 is a cross-sectional view of a state in which a slurry is poured into a mold 4 of FIG. 1 and left for a certain period of time to form an electrolyte molded body 5;
【図３】図２の電解質成形体５の上にスラリーを流し込
んで一定時間放置して空気極成形体６とした後、余剰の
スラリーを除去して複合成形体とした状態の断面図であ
る。3 is a cross-sectional view of a state in which a slurry is poured onto an electrolyte molded body 5 of FIG. 2 and left for a certain period of time to form an air electrode molded body 6, and then excess slurry is removed to form a composite molded body. .
【図４】図３の複合成形体から型４を除去した後焼成し
て得た固体電解質−空気極複合体の断面図である。FIG. 4 is a cross-sectional view of a solid electrolyte-air electrode composite obtained by removing the mold 4 from the composite molded body of FIG. 3 and then firing.
【図５】固体電解質−空気極複合体の外側に燃料極９を
形成した状態の断面図である。FIG. 5 is a cross-sectional view showing a state in which a fuel electrode 9 is formed outside a solid electrolyte-air electrode composite.
【図６】本発明の他の実施例に係る複合成形体とした状
態の断面図である。FIG. 6 is a cross-sectional view of a composite molded body according to another embodiment of the present invention.
【図７】本発明の他の実施例に係る複合成形体とした状
態の断面図である。FIG. 7 is a cross-sectional view of a composite molded body according to another embodiment of the present invention.
【図８】従来の固体電解質燃料電池の製造方法により製
造された固体電解質膜８の断面図である。FIG. 8 is a cross-sectional view of a solid electrolyte membrane 8 manufactured by a conventional method of manufacturing a solid electrolyte fuel cell.
４ 型 ５ 電解質成形体 ６ 空気極成形体 ７ 空気極 ８ 固体電解質膜 ９ 燃料極 4 mold 5 electrolyte formed body 6 air electrode formed body 7 air electrode 8 solid electrolyte membrane 9 fuel electrode
Claims (5)
るスラリーを、吸水性を有する型に流し込んで電解質成
形体とする工程と、金属酸化物を含有するスラリーを、
前記電解質成形体上に流し込んで空気極成形体とし、電
解質成形体と空気極成形体とを一体化した複合成形体を
得る工程と、この複合成形体から前記型を除去した後焼
成して固体電解質−空気極複合体とする工程と、この固
体電解質−空気極複合体の固体電解質側に燃料極を形成
する工程とからなることを特徴とする固体電解質燃料電
池の製造方法。1. A step of pouring a slurry containing zirconia to which a stabilizer has been added into a mold having water absorbability to form an electrolyte molded body, and comprising the steps of:
Casting the electrolyte molded article into an air electrode molded article to obtain a composite molded article obtained by integrating the electrolyte molded article and the air electrode molded article, and firing after removing the mold from the composite molded article. A method for producing a solid electrolyte-air electrode composite, and a step of forming a fuel electrode on the solid electrolyte side of the solid electrolyte- air electrode composite. .
晶ジルコニア、正方晶ジルコニア、部分安定化ジルコニ
アの単独物もしくは複数種の混合物からなることを特徴
とする請求項第１項記載の固体電解質燃料電池の製造方
法。2. The solid electrolyte according to claim 1, wherein the zirconia to which the stabilizer is added comprises one of cubic zirconia, tetragonal zirconia and partially stabilized zirconia, or a mixture of plural kinds thereof. A method for manufacturing a fuel cell.
ム、スカンジウム、イッテルビウム、ネオジウム、ガト
リニウムの酸化物であることを特徴とする請求項第１項
記載の固体電解質燃料電池の製造方法。3. The method according to claim 1, wherein the stabilizer is an oxide of yttrium, calcium, scandium, ytterbium, neodymium, or gatorium.
類金属を添加したＬａＭｎＯ3 、ＬａＣｏＯ3 、ＣａＭ
ｎＯ3 であることを特徴とする請求項第１項記載の固体
電解質燃料電池の製造方法。4. The metal oxide is LaMnO 3 , LaCoO 3 , CaM to which rare earth or alkaline earth metal is added.
Claim method for producing a solid electrolyte fuel cell of claim 1 wherein characterized in that it is a nO 3.
Ｃｏ−ＺｒＯ2 サーメットであることを特徴とする請求
項第１項記載の固体電解質燃料電池の製造方法。5. A fuel electrode comprising: Ni—ZrO 2 cermet;
2. The method for producing a solid electrolyte fuel cell according to claim 1, wherein the method is a Co-ZrO2 cermet.
Priority Applications (5)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3029539A JP3050331B2 (en) | 1991-01-29 | 1991-01-29 | Method for manufacturing solid electrolyte fuel cell |
| EP92900502A EP0514552B1 (en) | 1990-12-10 | 1991-12-09 | Method for manufacturing solid-state electrolytic fuel cell |
| DE69132207T DE69132207T2 (en) | 1990-12-10 | 1991-12-09 | METHOD FOR PRODUCING ELECTROLYTIC SOLID CELL |
| PCT/JP1991/001701 WO1992010862A1 (en) | 1990-12-10 | 1991-12-09 | Method for manufacturing solid-state electrolytic fuel cell |
| US07/915,699 US5290323A (en) | 1990-12-10 | 1991-12-09 | Manufacturing method for solid-electrolyte fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3029539A JP3050331B2 (en) | 1991-01-29 | 1991-01-29 | Method for manufacturing solid electrolyte fuel cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH04289665A JPH04289665A (en) | 1992-10-14 |
| JP3050331B2 true JP3050331B2 (en) | 2000-06-12 |
Family
ID=12278920
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP3029539A Expired - Fee Related JP3050331B2 (en) | 1990-12-10 | 1991-01-29 | Method for manufacturing solid electrolyte fuel cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3050331B2 (en) |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP3458863B2 (en) * | 1993-06-17 | 2003-10-20 | 東邦瓦斯株式会社 | Solid electrolyte sintered body for solid oxide fuel cell |
-
1991
- 1991-01-29 JP JP3029539A patent/JP3050331B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPH04289665A (en) | 1992-10-14 |
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