JP2008218275A - Solid oxide fuel cell - Google Patents

Solid oxide fuel cell Download PDF

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JP2008218275A
JP2008218275A JP2007055847A JP2007055847A JP2008218275A JP 2008218275 A JP2008218275 A JP 2008218275A JP 2007055847 A JP2007055847 A JP 2007055847A JP 2007055847 A JP2007055847 A JP 2007055847A JP 2008218275 A JP2008218275 A JP 2008218275A
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electrode layer
power generation
solid electrolyte
solid oxide
electrolyte layer
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Takashi Yamada
喬 山田
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Kansai Electric Power Co Inc
Mitsubishi Materials Corp
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Kansai Electric Power Co Inc
Mitsubishi Materials Corp
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    • 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
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Abstract

<P>PROBLEM TO BE SOLVED: To increase the breaking resistance or the peeling-off resistance of a power generation cell and increase the durability and power generation performance. <P>SOLUTION: In a solid oxide fuel cell 1 having the power generation cell 5 comprising arranged with a fuel electrode layer 4 and an air electrode layer 3 on each side of a solid electrolyte layer 2, a plurality of mutually crossing linear projecting parts 10 are formed on at least one surface of the solid oxide electrolyte layer 2, and the entire surface is partitioned in plural number by these projecting parts 10. <P>COPYRIGHT: (C)2008,JPO&INPIT

Description

本発明は、固体電解質層の両面に燃料極層と空気極層を配して構成した発電セルを備える固体酸化物形燃料電池に関し、特に、発電セルの耐久性向上に関するものである。   The present invention relates to a solid oxide fuel cell including a power generation cell configured by disposing a fuel electrode layer and an air electrode layer on both surfaces of a solid electrolyte layer, and particularly relates to improving the durability of the power generation cell.

固体酸化物形燃料電池は、第３世代の発電用燃料電池として開発が進んでいる。現在、この固体酸化物形燃料電池は、円筒型、モノリス型、および平板積層型の３種類が提案されており、何れも酸化物イオン導電体から成る固体電解質層を空気極層と燃料極層との間に挟んだ積層構造を有し、発電時には、反応用ガスとして空気極層側に酸化剤ガス（酸素) が、また燃料極層側に燃料ガス (Ｈ2、ＣＯ等) が供給される。 Solid oxide fuel cells are being developed as third-generation fuel cells for power generation. At present, three types of solid oxide fuel cells have been proposed: a cylindrical type, a monolith type, and a flat plate type, all of which include a solid electrolyte layer made of an oxide ion conductor as an air electrode layer and a fuel electrode layer. In the power generation, oxidant gas (oxygen) is supplied to the air electrode layer side and fuel gas (H 2 , CO, etc.) is supplied to the fuel electrode layer side during the power generation. The

空気極層側に供給された酸素（例えば空気）は、空気極層内を通って固体電解質層との界面近傍に到達し、この部分で空気極層から電子を受け取って酸化物イオン（Ｏ2-）にイオン化される。この酸化物イオンは、燃料極層に向かって固体電解質層内を拡散移動する。燃料極層との界面近傍に到達した酸化物イオンは、この部分で、燃料ガスと反応して反応生成物（Ｈ2Ｏ、ＣＯ2等）を生じ、燃料極層に電子を放出する。電極反応で生じた電子は、別ルートの外部負荷にて起電力として取り出すことができる。 Oxygen (for example, air) supplied to the air electrode layer side passes through the air electrode layer and reaches the vicinity of the interface with the solid electrolyte layer, and receives electrons from the air electrode layer at this portion to receive oxide ions (O 2 - ) Is ionized. The oxide ions diffuse and move in the solid electrolyte layer toward the fuel electrode layer. Oxide ions that have reached the vicinity of the interface with the fuel electrode layer react with the fuel gas at this portion to generate reaction products (H 2 O, CO 2, etc.), and discharge electrons to the fuel electrode layer. Electrons generated by the electrode reaction can be taken out as an electromotive force at an external load on another route.

ところで、上記構造の燃料電池では、長時間運転時の熱サイクルで、発電セル（詳しくは、固体電解質層）にヒビ割れ（クラック）が生じたり、電極層（特に、燃料極層側）に剥離が生じたりするという耐久性に係わる問題があった。   By the way, in the fuel cell having the above structure, the power generation cell (specifically, the solid electrolyte layer) is cracked or peeled off from the electrode layer (especially the fuel electrode layer side) in the thermal cycle during long-time operation. There was a problem related to durability, such as

固体電解質層の割れについては、発電時（昇温時）のセル内の温度分布で生じる熱応力に因るところが大きく、固体電解質層として厚さが数百〜数十μｍの薄いセラミックス材を使用することに起因していると考えられる。薄型の固体電解質を用いるのは、固定電解質層を薄くするこで内部抵抗を低減し、発電性能を向上するためである。
他方、電極層の剥離については、固体電解質層と電極層の各材料の熱膨張係数の差により生じる応力によるもので、例えば、燃料極層に含まれるＮｉ等の金属材料が酸化物の状態で固体電解質層に焼き付けられ、発電時の還元で燃料極層が収縮するためであると考えられている。 The cracks in the solid electrolyte layer are largely due to the thermal stress generated by the temperature distribution in the cell during power generation (temperature rise), and a thin ceramic material with a thickness of several hundreds to several tens of μm is used as the solid electrolyte layer. It is thought that it is caused by doing. The thin solid electrolyte is used in order to reduce the internal resistance and improve the power generation performance by thinning the fixed electrolyte layer.
On the other hand, the electrode layer is peeled off due to the stress generated by the difference in thermal expansion coefficient between the solid electrolyte layer and the electrode layer material. For example, a metal material such as Ni contained in the fuel electrode layer is in an oxide state. It is believed that this is because the fuel electrode layer contracts due to reduction during power generation after being baked on the solid electrolyte layer.

尚、このような三層構造の発電セルの割れや剥離を防止する技術として、例えば、特許文献１が開示されている。
特開２００３−２６３９９６号公報 For example, Patent Document 1 discloses a technique for preventing such a three-layered power generation cell from cracking or peeling.
JP 2003-263996 A

本発明は、上記問題に鑑みなされたもので、発電セルの耐割れ性や耐剥離性を向上した耐久性の高い固体酸化物形燃料電池を提供することを目的としている。   The present invention has been made in view of the above problems, and an object thereof is to provide a solid oxide fuel cell having high durability with improved cracking resistance and peeling resistance of a power generation cell.

すなわち、請求項１に記載の発明は、固体電解質層の両面に燃料極層および空気極層の各電極層を配した発電セルを備える固体酸化物形燃料電池において、前記固体電解質層の少なくとも一方の面に、相互に交差する線状の凸部が複数形成されており、これら凸部により全面が複数に区画されていることを特徴としている。   That is, the invention described in claim 1 is a solid oxide fuel cell comprising a power generation cell in which the electrode layers of the fuel electrode layer and the air electrode layer are arranged on both surfaces of the solid electrolyte layer, and at least one of the solid electrolyte layers. A plurality of linear protrusions intersecting each other are formed on this surface, and the entire surface is partitioned into a plurality by these protrusions.

また、請求項２に記載の発明は、請求項１に記載の固体酸化物形燃料電池において、前記凸部による区画の形状は、格子状または六角形状であることを特徴としている。   The invention described in claim 2 is characterized in that, in the solid oxide fuel cell according to claim 1, the shape of the section by the convex portion is a lattice shape or a hexagonal shape.

また、請求項３に記載の発明は、請求項１または請求項２の何れかに記載の固体酸化物形燃料電池において、前記電極層が、前記凸部によって複数に区画されていることを特徴としている。   The invention according to claim 3 is the solid oxide fuel cell according to claim 1 or 2, wherein the electrode layer is divided into a plurality of portions by the convex portion. It is said.

請求項１〜３に記載の発明によれば、固体電解質層の全面に線状の凸部を形成して複数に区画することにより、固体電解質層の機械的強度が向上し、発電セルの耐割れ性が向上すると共に、この凸部により電極層の熱収縮に伴う応力が緩和されることになり、電極層の耐剥離性が向上する。   According to the first to third aspects of the invention, the linear strength is formed on the entire surface of the solid electrolyte layer so as to be divided into a plurality of sections, thereby improving the mechanical strength of the solid electrolyte layer and improving the resistance of the power generation cell. While the cracking property is improved, the stress accompanying the thermal contraction of the electrode layer is relieved by this convex portion, and the peeling resistance of the electrode layer is improved.

特に、請求項２に記載のように、区画形状を格子状または六角形状にすることにより、固体電解質層の全面が均等に補強されるため、固体電解質層の機械的強度はさらに向上し、優れた耐割れ性が得られるようになる。   In particular, as described in claim 2, since the entire surface of the solid electrolyte layer is uniformly reinforced by making the partition shape into a lattice shape or a hexagonal shape, the mechanical strength of the solid electrolyte layer is further improved, and is excellent. High crack resistance can be obtained.

また、請求項３に記載のように、凸部によって電極層が複数の小エリアに区画されることにより、電極層の熱収縮に伴う応力が各区画に分散されるため、電極層の耐剥離性は更に向上する。   In addition, as described in claim 3, since the electrode layer is partitioned into a plurality of small areas by the convex portion, stress due to thermal contraction of the electrode layer is dispersed in each partition, so that the electrode layer is resistant to peeling. The property is further improved.

以下、図１〜図４に基づいて本発明の実施形態を説明する。
図１は本実施形態による平板積層型の固体酸化物形燃料電池の構成を示し、図２は本実施形態による発電セルの内部構造を示し、図３は発電セルの要部拡大を示し、図４は固体電解質層の区画形状を示している。 Hereinafter, embodiments of the present invention will be described with reference to FIGS.
1 shows a configuration of a flat plate type solid oxide fuel cell according to the present embodiment, FIG. 2 shows an internal structure of the power generation cell according to the present embodiment, FIG. 3 shows an enlarged main part of the power generation cell, 4 shows the partition shape of the solid electrolyte layer.

先ず、図１に基づいて本発明が適用された固体酸化物形燃料電池１の構成を説明する。
図１に示すように、固体酸化物形燃料電池１は、固体電解質層２の両面に燃料極層４と空気極層３を配した発電セル５と、燃料極層４の外側に配した燃料極集電体７と、空気極層３の外側に配した空気極集電体６と各集電体６、７の外側のセパレータ８を順番に繰り返し積層することにより構成されている。 First, the configuration of a solid oxide fuel cell 1 to which the present invention is applied will be described with reference to FIG.
As shown in FIG. 1, a solid oxide fuel cell 1 includes a power generation cell 5 in which a fuel electrode layer 4 and an air electrode layer 3 are disposed on both surfaces of a solid electrolyte layer 2, and a fuel disposed on the outside of the fuel electrode layer 4. The electrode current collector 7, the air electrode current collector 6 disposed outside the air electrode layer 3, and the separator 8 outside the current collectors 6 and 7 are sequentially stacked in order.

固体電解質層２は、Ｃｏ添加ランタンガレート（ＬＳＧＭＣ）等で構成され、空気極層３は、Ｓｍ0.5Ｓｒ0.5ＣｏＯ3（ＳＳＣ）等で構成され、燃料極層４は、ＮｉとＣｅ0.8Ｓｍ0.2Ｏ2（ＳＤＣ：サマリウム添加セリア）の混合物等で構成され、空気極集電体６は、Ａｇ等のスポンジ状の多孔質焼結金属板で構成され、燃料極集電体７は、Ｎｉ等のスポンジ状の多孔質焼結金属板で構成され、セパレータ８は、ステンレス等で構成されている。
また、セパレータ８は、発電セル５間を電気的に接続すると共に、発電セル５に対して反応用ガスを供給する機能を有し、内部に燃料ガスを燃料極集電体７に誘導する燃料ガス通路（図示せず）と、酸化剤ガスを空気極集電体６に誘導する酸化剤ガス通路（図示せず）を有する。 The solid electrolyte layer 2 is made of Co-added lanthanum gallate (LSGMC) or the like, the air electrode layer 3 is made of Sm 0.5 Sr 0.5 CoO 3 (SSC) or the like, and the fuel electrode layer 4 is made of Ni and Ce 0.8 Sm 0.2. O 2: consists of a mixture of (SDC samarium doped ceria), an air electrode current collector 6 is formed of a sponge-like porous sintered metal plate such as Ag, anode current collector 7, Ni, etc. The separator 8 is made of stainless steel or the like.
Further, the separator 8 has a function of electrically connecting the power generation cells 5 and supplying a reaction gas to the power generation cells 5, and a fuel that guides the fuel gas to the anode current collector 7 inside. It has a gas passage (not shown) and an oxidant gas passage (not shown) for guiding the oxidant gas to the air electrode current collector 6.

ところで、上述の固体電解質層２は、図２に示すように、燃料極層４と接する面に線状の凸部１０が複数形成されており、これら線状の凸部１０により固体電解質層２の一方の面の全面が複数に小区画化された状態となっている。
本実施形態では、これら凸部１０による区画形状を、図４（ａ）に示すような格子状、或いは、図４（ｂ）に示すような多数の六角形状としている。 Incidentally, as shown in FIG. 2, the solid electrolyte layer 2 has a plurality of linear protrusions 10 formed on the surface in contact with the fuel electrode layer 4, and the solid electrolyte layer 2 is formed by the linear protrusions 10. The entire surface of one of the surfaces is divided into a plurality of sections.
In this embodiment, the partition shape by these convex parts 10 is made into the grid | lattice form as shown to Fig.4 (a), or many hexagonal shapes as shown to FIG.4 (b).

これらは、何れも、固体電解質層２を形成する際に、ドクターブレード法等により薄板状に成形された厚さ約２００μｍ程のグリーンシートの片面上に、例えば、スクリーン印刷等により電解質材料と同じ材料を塗布することにより簡単に形成することができる。
また、区画形状は、印刷に使用するスクリーンパターンの穴形を変えることで自由に設定することが可能であり、形成される凸部１０の幅は０．１ｍｍ程、高さは２０μｍ程である。 These are the same as the electrolyte material by, for example, screen printing on one side of a green sheet having a thickness of about 200 μm formed into a thin plate by the doctor blade method or the like when forming the solid electrolyte layer 2. It can be easily formed by applying a material.
The partition shape can be freely set by changing the hole shape of the screen pattern used for printing. The width of the formed convex portion 10 is about 0.1 mm, and the height is about 20 μm. .

また、この固体電解質層２の凸部１０形成面に燃料極層４を形成する場合、図３（ａ）に示すように、凸部１０の頂部１０ａにも燃料極層４を形成するようにしても良く、或いは、図３（ｂ）に示すように、凸部１０の頂部１０ａが露出するように燃料極層４を形成しても良い。後者の場合には、凸部１０によって燃料極層４が複数に小区画化されることになる。   Further, when the fuel electrode layer 4 is formed on the surface of the solid electrolyte layer 2 where the convex portion 10 is formed, the fuel electrode layer 4 is also formed on the top portion 10a of the convex portion 10 as shown in FIG. Alternatively, as shown in FIG. 3B, the fuel electrode layer 4 may be formed so that the top portion 10a of the convex portion 10 is exposed. In the latter case, the fuel electrode layer 4 is subdivided into a plurality of sections by the convex portion 10.

以上のように、本実施形態では、固体電解質層２の全面に線状の凸部１０を形成することにより、固体電解質層２の機械的強度が向上し、熱応力に対する発電セル５の耐割れ性が向上する。この場合、凸部１０による区画形状を、図４に示すように、格子状または六角形状にすると、固体電解質層２の全面が均等に補強されるようになるため、固体電解質層２の機械的強度は更に向上し、優れた耐割れ性が得られるようになる。   As described above, in the present embodiment, by forming the linear protrusions 10 on the entire surface of the solid electrolyte layer 2, the mechanical strength of the solid electrolyte layer 2 is improved and the cracking resistance of the power generation cell 5 against thermal stress is increased. Improves. In this case, as shown in FIG. 4, when the partition shape by the convex portion 10 is a lattice shape or a hexagonal shape, the entire surface of the solid electrolyte layer 2 is uniformly reinforced, so that the mechanical properties of the solid electrolyte layer 2 are increased. The strength is further improved, and excellent crack resistance can be obtained.

また、上記に加え、発電時の燃料極層４の熱収縮に伴う応力が凸部１０を形成することにより緩和されるため、燃料極層４の耐剥離性が向上する。
特に、図３（ｂ）のように、凸部１０の形成によって燃料極層４が複数の小エリアに区画されている場合は、燃料極層４に加わる応力は各区画に分散され、各区画に加わる応力は小さいものとなるため、燃料極層４の耐剥離性は更に向上する。 Further, in addition to the above, the stress accompanying thermal contraction of the fuel electrode layer 4 during power generation is alleviated by forming the projections 10, so that the peel resistance of the fuel electrode layer 4 is improved.
In particular, as shown in FIG. 3B, when the fuel electrode layer 4 is partitioned into a plurality of small areas by the formation of the convex portion 10, the stress applied to the fuel electrode layer 4 is distributed to each partition. Since the stress applied to is small, the peel resistance of the fuel electrode layer 4 is further improved.

また、固体電解質層２の材料であるＬＳＧＭＣと燃料極層４の材料であるＳＤＣとは、密着性において相性が良いため、これらの組み合わせが電極剥離の防止に対して有利に作用する。   In addition, since LSGMC, which is a material of the solid electrolyte layer 2, and SDC, which is a material of the fuel electrode layer 4, are compatible with each other, their combination has an advantageous effect on prevention of electrode peeling.

このように、本実施形態によれば、長時間運転時の熱サイクルにおいて発電セル５の割れや燃料極層４の剥離を防止し、安定した発電性能を維持できる固体酸化物形燃料電池を実現することができる。   Thus, according to the present embodiment, a solid oxide fuel cell capable of preventing cracking of the power generation cell 5 and peeling of the fuel electrode layer 4 in a thermal cycle during long-time operation and maintaining stable power generation performance is realized. can do.

また、本実施形態では、固体電解質層２の燃料極層４側の面にのみ凸部１０を形成したが、空気極層３側の面、或いは固体電解質層２の両面に設けることも勿論可能である。   Further, in the present embodiment, the convex portion 10 is formed only on the surface of the solid electrolyte layer 2 on the fuel electrode layer 4 side, but it is of course possible to provide it on the surface of the air electrode layer 3 side or both surfaces of the solid electrolyte layer 2. It is.

本発明に係る平板積層型の固体酸化物形燃料電池の構成を示す分解斜視図。1 is an exploded perspective view showing a configuration of a flat plate type solid oxide fuel cell according to the present invention. 本発明に係る発電セルの内部構造を示す断面図。Sectional drawing which shows the internal structure of the electric power generation cell which concerns on this invention. 図２の発電セルの要部拡大を示す断面図。Sectional drawing which shows the principal part expansion of the power generation cell of FIG. 固体電解質層の区画形状を示す平面図。The top view which shows the division shape of a solid electrolyte layer.

符号の説明Explanation of symbols

１ 固体酸化物形燃料電池
２ 固体電解質層
３ 空気極層
４ 燃料極層
５ 発電セル
１０ 凸部 DESCRIPTION OF SYMBOLS 1 Solid oxide fuel cell 2 Solid electrolyte layer 3 Air electrode layer 4 Fuel electrode layer 5 Power generation cell 10 Convex part

Claims (3)

固体電解質層の両面に燃料極層および空気極層の各電極層を配して成る発電セルを備える固体酸化物形燃料電池において、
前記固体電解質層の少なくとも一方の面に、相互に交差する線状の凸部が複数形成されており、これら凸部により全面が複数に区画されていることを特徴とする固体酸化物形燃料電池。 In a solid oxide fuel cell including a power generation cell in which each electrode layer of a fuel electrode layer and an air electrode layer is disposed on both surfaces of a solid electrolyte layer,
A solid oxide fuel cell, wherein a plurality of linear protrusions intersecting each other are formed on at least one surface of the solid electrolyte layer, and the entire surface is partitioned into a plurality by these protrusions. . 前記凸部による区画形状は、格子状または六角形状であることを特徴とする請求項１に記載の固体酸化物形燃料電池。 2. The solid oxide fuel cell according to claim 1, wherein a partition shape by the convex portion is a lattice shape or a hexagonal shape. 前記電極層が、前記凸部によって複数に区画されていることを特徴とする請求項１または請求項２の何れかに記載の固体酸化物形燃料電池。 3. The solid oxide fuel cell according to claim 1, wherein the electrode layer is partitioned into a plurality of portions by the convex portion. 4.
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JP2010146891A (en) * 2008-12-19 2010-07-01 Honda Motor Co Ltd Fuel battery

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JP2001229935A (en) * 1999-12-27 2001-08-24 Corning Inc Solid oxide electrolyte fuel cell module and its production method
JP2004186056A (en) * 2002-12-05 2004-07-02 Nissan Motor Co Ltd Solid electrolyte fuel cell and its manufacturing method

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Publication number Priority date Publication date Assignee Title
JP2001229935A (en) * 1999-12-27 2001-08-24 Corning Inc Solid oxide electrolyte fuel cell module and its production method
JP2004186056A (en) * 2002-12-05 2004-07-02 Nissan Motor Co Ltd Solid electrolyte fuel cell and its manufacturing method

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2010146891A (en) * 2008-12-19 2010-07-01 Honda Motor Co Ltd Fuel battery

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