JPH0864222A - Air electrode and air electrode side current collecting plate for solid electrolyte fuel cell - Google Patents
Air electrode and air electrode side current collecting plate for solid electrolyte fuel cellInfo
- Publication number
- JPH0864222A JPH0864222A JP6201935A JP20193594A JPH0864222A JP H0864222 A JPH0864222 A JP H0864222A JP 6201935 A JP6201935 A JP 6201935A JP 20193594 A JP20193594 A JP 20193594A JP H0864222 A JPH0864222 A JP H0864222A
- Authority
- JP
- Japan
- Prior art keywords
- air electrode
- thermal expansion
- linear thermal
- side current
- expansion coefficient
- 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.)
- Granted
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
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
（ＳＯＦＣ）用空気極及び空気極側集電板に係り、特
に、電解質との熱膨張係数の差が小さく、しかも電気伝
導性、電極活性に優れたＳＯＦＣ用空気極及び空気極側
集電板に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a solid oxide fuel cell (SOFC) air electrode and an air electrode side current collecting plate, and in particular, it has a small difference in coefficient of thermal expansion from an electrolyte, and has electrical conductivity and The present invention relates to an SOFC air electrode and an air electrode side current collector having excellent activity.
【０００２】[0002]
【従来の技術】ＳＯＦＣは、イットリア安定化ジルコニ
ア（ＹＳＺ）よりなる電解質膜に燃料極（アノード）及
び空気極（カソード）の電極膜を積層した構成とされて
いる。従来、空気極電極材料及び空気極側集電板材料と
しては、ＳｒをドープしたＬａＭｎＯ3 、即ち、Ｌａ
1-y Ｓｒy ＭｎＯ3 （ｙ＝０．１〜０．４）が広く用い
られている。即ち、ＬａＭｎＯ3 にＳｒをドープするこ
とにより、作動条件下での電気伝導性、電極活性が向上
し、良好な空気極及び空気極側集電板が提供される。こ
の電気伝導性、電極活性の向上効果は、ＬａＭｎＯ3 へ
のＳｒのドープ量に比例し、Ｓｒのドープ量が多い程、
電気伝導性、電極活性に優れた空気極及び空気極側集電
板が提供される。2. Description of the Related Art An SOFC has a structure in which an electrolyte membrane made of yttria-stabilized zirconia (YSZ) is laminated with electrode membranes of a fuel electrode (anode) and an air electrode (cathode). Conventionally, as the air electrode electrode material and the air electrode side current collecting plate material, Sr-doped LaMnO 3 , that is, La
1-y Sr y MnO 3 (y = 0.1 to 0.4) is widely used. That is, by doping LaMnO 3 with Sr, the electrical conductivity under the operating conditions and the electrode activity are improved, and a good air electrode and an air electrode side current collector plate are provided. The effect of improving electrical conductivity and electrode activity is proportional to the amount of Sr doped in LaMnO 3, and the larger the amount of Sr doped,
Provided are an air electrode and an air electrode side current collector excellent in electrical conductivity and electrode activity.
【０００３】[0003]
【発明が解決しようとする課題】しかし、ＬａＭｎＯ3
にＳｒをドープすることにより、この材料の線熱膨張係
数は大きくなり、電解質を構成するジルコニア質材料
（具体的にはイットリア安定化ジルコニア（ＹＳＺ））
の線熱膨張係数（１０×１０-6／Ｋ程度）との整合性は
大きく崩れる。この電解質の線熱膨張係数との整合性
は、ＬａＭｎＯ3 へのＳｒのドープ量が多い程悪化す
る。このような空気極及び空気極側集電板の線熱膨張係
数と電解質の線熱膨張係数との不整合は、電池内部に熱
応力を発生させ、著しい場合には電池を破壊に至らせ
る。[Problems to be Solved by the Invention] However, LaMnO 3
By doping Sr with Sr, the coefficient of linear thermal expansion of this material increases, and a zirconia-based material that constitutes the electrolyte (specifically, yttria-stabilized zirconia (YSZ))
Consistency with the coefficient of linear thermal expansion (about 10 × 10 −6 / K) is greatly lost. The consistency with the coefficient of linear thermal expansion of this electrolyte deteriorates as the amount of Sr doped in LaMnO 3 increases. Such a mismatch between the linear thermal expansion coefficient of the air electrode and the air electrode side current collecting plate and the linear thermal expansion coefficient of the electrolyte causes thermal stress inside the battery, and in a remarkable case, the battery is destroyed.
【０００４】本発明は上記従来の問題点を解決し、電解
質との線熱膨張係数の整合性に優れ、しかも電気伝導
性、電極活性に優れたＳＯＦＣ用空気極及び空気極側集
電板を提供することを目的とする。The present invention solves the above-mentioned conventional problems, and provides an SOFC air electrode and an air electrode side current collecting plate having excellent linear thermal expansion coefficient matching with an electrolyte and excellent electric conductivity and electrode activity. The purpose is to provide.
【０００５】[0005]
【課題を解決するための手段】本発明のＳＯＦＣ用空気
極及び空気極側集電板は、｛（Ｌａ1-x Ｙx ）1-y Ｓｒ
y ｝ＭｎＯ3 （ただし、０＜ｘ≦０．４，０．１≦ｙ≦
０．４）で表される導電性セラミックス材料で構成され
ることを特徴とする。The SOFC air electrode and the air electrode side current collector of the present invention are {(La 1-x Y x ) 1-y Sr.
y } MnO 3 (where 0 <x ≦ 0.4, 0.1 ≦ y ≦
0.4), which is composed of a conductive ceramic material.
【０００６】即ち、本発明者らは、従来の空気極及び空
気極側集電板材料であるＬａ1-y Ｓｒy ＭｎＯ3 はＳｒ
のドープ量を大きくする程電気伝導度は向上するが、電
解質との線熱膨張係数の整合性は失われるのに対し、Ｙ
ＭｎＯ3 系の材料は線熱膨張係数が小さいことに着目
し、ＬａＭｎＯ3 に電気伝導度を向上させる目的でＳｒ
をドープしつつ、線熱膨張係数の整合性を保つ目的でＹ
をドープすることを見出し、本発明を完成させた。That is, the inventors of the present invention used La 1-y Sr y MnO 3 which is a conventional air electrode and air electrode side current collector material as Sr.
Although the electrical conductivity increases as the doping amount of Y increases, the matching of the coefficient of linear thermal expansion with the electrolyte is lost, while Y
Paying attention to the fact that the MnO 3 type material has a small coefficient of linear thermal expansion, Sr was added to LaMnO 3 for the purpose of improving electric conductivity.
For the purpose of maintaining the consistency of the coefficient of linear thermal expansion while doping
The present invention has been completed by finding out that doping is performed.
【０００７】以下に本発明を詳細に説明する。The present invention will be described in detail below.
【０００８】本発明において、空気極及び空気極側集電
板の構成材料として用いる導電性セラミックスは、
｛（Ｌａ1-x Ｙx ）1-y Ｓｒy ｝ＭｎＯ3 （ただし、０
＜ｘ≦０．４，０．１≦ｙ≦０．４）で表されるもので
ある。In the present invention, the conductive ceramics used as the constituent material of the air electrode and the air electrode side current collecting plate are:
{(La 1-x Y x ) 1-y Sry y MnO 3 (where 0
<X ≦ 0.4, 0.1 ≦ y ≦ 0.4).
【０００９】ここで、Ｓｒドープによるｙが０．１未満
では、電気伝導性及び電極活性の改善効果が十分でな
く、ｙが０．４を超えるとＹの効果を打消すほどに線熱
膨張係数が大きくなる。Here, if y by Sr doping is less than 0.1, the effect of improving electrical conductivity and electrode activity is not sufficient, and if y exceeds 0.4, the linear thermal expansion is such that the effect of Y is canceled out. The coefficient becomes large.
【００１０】また、ｘが０．４を超えるとペロブスカイ
トの単相構造ではなく、他の相が表出し、また、電気伝
導度が低下してくるため、ｘは０．４以下とする。ｘは
０．４以下の範囲で大きい程線熱膨張係数を電解質であ
るＹＳＺの線熱膨張係数に近づけることができ、線熱膨
張係数の整合性の面から好ましい。ｘは少な過ぎるとＹ
ドープによる線熱膨張係数及び電気伝導度の改善効果が
十分に得られないことから、ｘは特に０．２〜０．４で
あることが好ましい。When x exceeds 0.4, the perovskite does not have a single-phase structure, other phases are exposed, and the electrical conductivity decreases, so x is set to 0.4 or less. The larger the x is in the range of 0.4 or less, the closer the linear thermal expansion coefficient to the linear thermal expansion coefficient of YSZ, which is the electrolyte, and it is preferable from the viewpoint of the consistency of the linear thermal expansion coefficient. If x is too small, Y
Since the effect of improving the linear thermal expansion coefficient and the electric conductivity by the doping cannot be sufficiently obtained, x is particularly preferably 0.2 to 0.4.
【００１１】このような導電性セラミックス材料で構成
される本発明のＳＯＦＣ用空気極又は空気極側集電板
は、常法に従って、Ｌａ，Ｙ，Ｓｒ，Ｍｎの各成分の酸
化物や酢酸塩等の出発原料を所定の組成となるように混
合した後、１０００〜１２００℃で固相反応させ、その
後、成形、焼成することにより容易に製造することがで
きる。The SOFC air electrode or air electrode side current collecting plate of the present invention made of such a conductive ceramic material is an oxide or acetate of each of La, Y, Sr and Mn in accordance with a conventional method. It can be easily produced by mixing starting materials such as the above so as to have a predetermined composition, solid-phase reacting at 1000 to 1200 ° C., and then molding and firing.
【００１２】[0012]
【作用】Ｙイオンはペロブスカイト構造の中で、Ｌａイ
オンと同じ３価の状態にある上に、そのサイトもＬａと
同じＡサイトを占有すると考えられる。このようなこと
から、ＹＭｎＯ3 系材料はＬａＭｎＯ3 系材料と全率固
溶する。In the perovskite structure, the Y ion is considered to have the same trivalent state as the La ion, and its site occupies the same A site as La. Because of this, the YMnO 3 based material forms a solid solution with the LaMnO 3 based material.
【００１３】ところで、ＹＭｎＯ3 系材料は電解質材料
であるＹＳＺよりも線熱膨張係数が小さく、一方、Ｌａ
ＭｎＯ3 系材料はＹＳＺよりも線熱膨張係数が大きい。By the way, the YMnO 3 type material has a smaller coefficient of linear thermal expansion than YSZ which is an electrolyte material.
The MnO 3 based material has a larger coefficient of linear thermal expansion than YSZ.
【００１４】そこで、従来の空気極及び空気極側集電板
材料であるＬａ1-y Ｓｒy ＭｎＯ３において、Ｌａサイ
トの一部をＹで置換したところ、線熱膨張係数を小さく
することができ、これにより、Ｓｒドープによる効果で
電気伝導度及び電極活性に優れ、しかも、Ｙドープによ
る効果で電解質との線熱膨張係数の整合性に優れた材料
が得られる。なお、このＹドープによれば、電気伝導度
についても良好な向上効果が得られる。Therefore, in La 1-y Sr y MnO 3 which is a conventional air electrode and air electrode side current collecting plate material, when a part of the La site is replaced with Y, the linear thermal expansion coefficient can be reduced. This makes it possible to obtain a material that is excellent in electrical conductivity and electrode activity due to the effect of Sr doping, and is excellent in matching of the linear thermal expansion coefficient with the electrolyte due to the effect of Y doping. In addition, according to this Y-doping, a good effect of improving the electric conductivity can be obtained.
【００１５】[0015]
【実施例】以下に実施例を挙げて本発明をより具体的に
説明する。EXAMPLES The present invention will be described in more detail with reference to the following examples.
【００１６】実施例１ 下記方法により、（Ｌａ１−ｘ Ｙx ）0.7 Ｓｒ0.3 Ｍ
ｎＯ3 （ただし、ｘ＝０．０，０．２，０．４，０．
６，０．８又は１．０）系導電性セラミックス材料を調
製した。Example 1 (La 1-x Y x ) 0.7 Sr 0.3 M was prepared by the following method.
nO 3 (where x = 0.0, 0.2, 0.4, 0.
6, 0.8 or 1.0) -based conductive ceramic material was prepared.
【００１７】即ち、まず、出発原料として酢酸ランタ
ン、酢酸ストロンチウム、酢酸マンガン、酸化イットリ
ウムを用い、これらを各々所定の組成となるように秤量
した後混合し、４００℃で熱分解した。これを粉砕、混
合した後、一軸プレス成形し、１０００℃で固相反応を
行った。That is, first, lanthanum acetate, strontium acetate, manganese acetate, and yttrium oxide were used as starting materials. These were weighed so as to have respective predetermined compositions, mixed, and pyrolyzed at 400 ° C. This was crushed and mixed, then uniaxially press-molded, and a solid phase reaction was performed at 1000 ° C.
【００１８】この固相反応後の各試料の粉末Ｘ線回折結
果を図１〜６に示す。The results of powder X-ray diffraction of each sample after this solid phase reaction are shown in FIGS.
【００１９】図１〜６より明らかなように、ｘ＝０．
０，０．２，０．４ではペロブスカイト一相であるが、
ｘ＝０．４を超えるＹのドープ量では、ピークがブロー
ドになり、また、ペロブスカイト以外の小さな第２相の
ピークが認められる。As is clear from FIGS. 1 to 6, x = 0.
At 0, 0.2 and 0.4, there is a single phase of perovskite,
When the doping amount of Y exceeds x = 0.4, the peak becomes broad and a small second phase peak other than the perovskite is observed.
【００２０】固相反応後の各試料を各々遊星型ボールミ
ルで粉砕し、一軸プレス成形を行った。これを１５００
℃で５時間、大気中で焼成した。得られた焼結体から、
３ｍｍ×４ｍｍ×１７ｍｍの線熱膨張係数測定用試料
と、２ｍｍ×２ｍｍ×２０ｍｍの電気伝導度測定用試料
を切り出し、各々測定を行った。なお、線熱膨張係数の
測定は、大気中で室温から１４００℃まで行った。ま
た、電気伝導度は１０００℃、大気中で直流４端子法に
より測定した。これらの測定結果を表１に示す。Each sample after the solid phase reaction was crushed by a planetary ball mill and uniaxially press molded. This is 1500
Firing was performed in the air at 5 ° C. for 5 hours. From the obtained sintered body,
A 3 mm x 4 mm x 17 mm sample for linear thermal expansion coefficient measurement and a 2 mm x 2 mm x 20 mm sample for electrical conductivity measurement were cut out and measured respectively. The linear thermal expansion coefficient was measured in the air from room temperature to 1400 ° C. The electric conductivity was measured at 1000 ° C. in the atmosphere by a direct current 4-terminal method. The results of these measurements are shown in Table 1.
【００２１】[0021]
【表１】 [Table 1]
【００２２】表１より、（Ｌａ1-x Ｙx ）0.7 Ｓｒ0.3
ＭｎＯ3 （０＜ｘ≦０．４）であれば、電解質の線熱膨
張係数の整合性に優れ、しかも電気伝導度も高い導電性
セラミックス材料が提供されることが明らかである。From Table 1, (La 1-x Y x ) 0.7 Sr 0.3
It is apparent that MnO 3 (0 <x ≦ 0.4) provides a conductive ceramic material having excellent matching of the linear thermal expansion coefficient of the electrolyte and high electric conductivity.
【００２３】即ち、ｘ＝０．２の割合でＹをドープした
No. ２では、ＹをドープしていないNo. １のものに比べ
て線熱膨張係数は１１．５×１０-6／Ｋと大きく低下
し、電解質材料であるＹＳＺの線熱膨張係数１０×１０
-6／Ｋに近づく。しかも、電気伝導度についてもＹドー
プにより向上効果が認められる。これにより、０＜ｘ≦
０．４のＹドープにより、線熱膨張係数及び電気伝導度
が共に改善されることが明らかである。That is, Y was doped at a ratio of x = 0.2.
In No. 2, the linear thermal expansion coefficient was significantly reduced to 11.5 × 10 −6 / K compared with that of No. 1 in which Y was not doped, and the linear thermal expansion coefficient of YSZ which is an electrolyte material was 10 ×. 10
-6 / K approaching. Moreover, the effect of improving the electric conductivity is also confirmed by the Y doping. As a result, 0 <x ≦
It is clear that a Y doping of 0.4 improves both the coefficient of linear thermal expansion and the electrical conductivity.
【００２４】[0024]
【発明の効果】以上詳述した通り、本発明の固体電解質
型燃料電池によれば、電解質との線熱膨張係数差が小さ
く、従って、電池破壊の問題がなく、しかも、電気伝導
度、電極活性も高いＳＯＦＣ用空気極及び空気極側集電
板が提供される。As described in detail above, according to the solid oxide fuel cell of the present invention, the difference in linear thermal expansion coefficient from the electrolyte is small, and therefore, there is no problem of cell destruction, and the electrical conductivity and electrode An SOFC air electrode and an air electrode side current collector having high activity are provided.
【図１】実施例１で製造した（Ｌａ1-x Ｙx ）0.7 Ｓｒ
0.3 ＭｎＯ3 （ｘ＝０．０）の粉末Ｘ線回折線図であ
る。FIG. 1 is the (La 1-x Y x ) 0.7 Sr produced in Example 1.
0.3 is a powder X-ray diffraction diagram of MnO 3 (x = 0.0).
【図２】実施例１で製造した（Ｌａ1-x Ｙx ）0.7 Ｓｒ
0.3 ＭｎＯ3 （ｘ＝０．２）の粉末Ｘ線回折線図であ
る。FIG. 2 (La 1-x Y x ) 0.7 Sr produced in Example 1
FIG. 3 is a powder X-ray diffraction diagram of 0.3 MnO 3 (x = 0.2).
【図３】実施例１で製造した（Ｌａ1-x Ｙx ）0.7 Ｓｒ
0.3 ＭｎＯ3 （ｘ＝０．４）の粉末Ｘ線回折線図であ
る。FIG. 3 is (La 1-x Y x ) 0.7 Sr produced in Example 1.
0.3 is a powder X-ray diffraction diagram of MnO 3 (x = 0.4).
【図４】実施例１で製造した（Ｌａ1-x Ｙx ）0.7 Ｓｒ
0.3 ＭｎＯ3 （ｘ＝０．６）の粉末Ｘ線回折線図であ
る。FIG. 4 (La 1-x Y x ) 0.7 Sr produced in Example 1
0.3 is a powder X-ray diffraction diagram of MnO 3 (x = 0.6).
【図５】実施例１で製造した（Ｌａ1-x Ｙx ）0.7 Ｓｒ
0.3 ＭｎＯ3 （ｘ＝０．８）の粉末Ｘ線回折線図であ
る。FIG. 5: (La 1-x Y x ) 0.7 Sr produced in Example 1
0.3 is a powder X-ray diffraction diagram of MnO 3 (x = 0.8).
【図６】実施例１で製造した（Ｌａ1-x Ｙx ）0.7 Ｓｒ
0.3 ＭｎＯ3 （ｘ＝１．０）の粉末Ｘ線回折線図であ
る。FIG. 6 is (La 1-x Y x ) 0.7 Sr produced in Example 1.
FIG. 3 is a powder X-ray diffraction diagram of 0.3 MnO 3 (x = 1.0).
Claims (2)
ス材料で構成されることを特徴とする固体電解質型燃料
電池用空気極。 ｛（Ｌａ1-x Ｙx ）1-y Ｓｒy ｝ＭｎＯ3 （ただし、０＜ｘ≦０．４，０．１≦ｙ≦０．４）1. An air electrode for a solid oxide fuel cell, which is composed of a conductive ceramic material represented by the following composition formula. {(La 1-x Y x ) 1-y Sr y} MnO 3 ( however, 0 <x ≦ 0.4,0.1 ≦ y ≦ 0.4)
ス材料で構成されることを特徴とする固体電解質型燃料
電池用空気極側集電板。 ｛（Ｌａ1-x Ｙx ）1-y Ｓｒy ｝ＭｎＯ3 （ただし、０＜ｘ≦０．４，０．１≦ｙ≦０．４）2. An air electrode side current collector plate for a solid oxide fuel cell, comprising a conductive ceramic material represented by the following composition formula. {(La 1-x Y x ) 1-y Sr y} MnO 3 ( however, 0 <x ≦ 0.4,0.1 ≦ y ≦ 0.4)
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP06201935A JP3119084B2 (en) | 1994-08-26 | 1994-08-26 | Air electrode and air electrode side current collector for solid oxide fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP06201935A JP3119084B2 (en) | 1994-08-26 | 1994-08-26 | Air electrode and air electrode side current collector for solid oxide fuel cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH0864222A true JPH0864222A (en) | 1996-03-08 |
| JP3119084B2 JP3119084B2 (en) | 2000-12-18 |
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP06201935A Expired - Fee Related JP3119084B2 (en) | 1994-08-26 | 1994-08-26 | Air electrode and air electrode side current collector for solid oxide fuel cell |
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| Country | Link |
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| JP (1) | JP3119084B2 (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2002013296A1 (en) * | 2000-08-04 | 2002-02-14 | Anan Kasei Co., Ltd. | Composite oxide for air electrode and material of collector of solid electrolyte fuel cell, method for preparation thereof, and solid electrolyte fuel cell |
| JP2010212036A (en) * | 2009-03-10 | 2010-09-24 | Noritake Co Ltd | Solid oxide fuel cell and interconnector for the cell |
| KR101104117B1 (en) * | 2010-05-11 | 2012-01-13 | 한국에너지기술연구원 | Mesh type cathode current collector of tubular solid oxide fuel cell |
-
1994
- 1994-08-26 JP JP06201935A patent/JP3119084B2/en not_active Expired - Fee Related
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2002013296A1 (en) * | 2000-08-04 | 2002-02-14 | Anan Kasei Co., Ltd. | Composite oxide for air electrode and material of collector of solid electrolyte fuel cell, method for preparation thereof, and solid electrolyte fuel cell |
| JP2010212036A (en) * | 2009-03-10 | 2010-09-24 | Noritake Co Ltd | Solid oxide fuel cell and interconnector for the cell |
| KR101104117B1 (en) * | 2010-05-11 | 2012-01-13 | 한국에너지기술연구원 | Mesh type cathode current collector of tubular solid oxide fuel cell |
Also Published As
| Publication number | Publication date |
|---|---|
| JP3119084B2 (en) | 2000-12-18 |
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