JP2019008914A - 電気化学セルおよび電気化学スタック - Google Patents
電気化学セルおよび電気化学スタック Download PDFInfo
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Abstract
【解決手段】電気化学セルは、第1の希土類元素を含有するZrO2を含む固体電解質層と、固体電解質層の一方側に配置された空気極と、固体電解質層の他方側に配置された燃料極とを備える。燃料極は、第2の希土類元素を含有するCeO2と、NiまたはNi含有合金とを含む。電気化学セルは、さらに、固体電解質層と燃料極との間に配置された中間層を備える。中間層は、ZrとCeと第1の希土類元素と第2の希土類元素とを含有する固溶体を含む。
【選択図】図4
Description
A−1.構成:
(燃料電池スタック100の構成)
図1は、本実施形態における燃料電池スタック100の外観構成を示す斜視図であり、図2は、図1のII−IIの位置における燃料電池スタック100のYZ断面構成(一部省略)を示す説明図であり、図3は、図1のIII−IIIの位置における燃料電池スタック100のXZ断面構成(一部省略)を示す説明図である。各図には、方向を特定するための互いに直交するXYZ軸が示されている。本明細書では、便宜的に、Z軸正方向を上方向といい、Z軸負方向を下方向といい、Z軸に直交する方向を水平方向というが、燃料電池スタック100は実際にはそのような向きとは異なる向きで設置されてもよい。
各セル110は、筒状(チューブ状)の部材である。燃料電池スタック100に含まれる24個のセル110は、各セル110の軸方向が略平行(Y軸方向)になるように、互いに間隔を空けて配置されている。具体的には、24個のセル110は、水平方向(X軸方向)に3個ずつ並べて配置され、鉛直方向(Z軸方向)に8個ずつ並べて配置されている。
各集電部材104は、ガス透過性を有する導電性材料により形成されている。図3に示すように、各集電部材104は、各セル110を囲むように形成された3つの円筒部分142と、円筒部分142同士を連結する連結部分144とを含む。水平方向に並ぶ3つのセル110が各集電部材104の3つの円筒部分142内に配置されることにより、それらのセル110が互いに電気的に接続される。また、8つの集電部材104は、絶縁多孔体106を間に挟みつつ、上下方向に並べて配置されている。
図1および図2に示すように、燃料電池スタック100に水素を含む燃料ガスFGが供給されると、燃料ガスFGは、各セル110の燃料極層116に形成された燃料ガス導通孔117内に進入する。また、図1および図3に示すように、燃料電池スタック100に酸素を含む酸化剤ガスOG(例えば空気)が供給されると、酸化剤ガスOGは、絶縁多孔体106および集電部材104を透過して、各セル110の空気極層114に至る。各セル110の燃料極層116に燃料ガスFGが供給され、空気極層114に酸化剤ガスOGが供給されると、各セル110において酸化剤ガスOGおよび燃料ガスFGの電気化学反応による発電が行われる。各セル110は、集電部材104および上述した導電パスEPにより互いに電気的に接続されており、また、燃料電池スタック100の上側および下側には、図示しない端子部材が設けられている。各セル110における発電により生じた電力は、負極側および正極側の端子部材に接続された導線等を通して外部に取り出される。なお、複数の燃料電池スタック100を所定方向に配列して燃料電池モジュールを構成してもよい。
次に、上述した構成のセル110の製造方法について説明する。図5は、本実施形態におけるセル110の製造方法の一例を示すフローチャートである。
以上説明したように、本実施形態のセル110は、希土類元素(第1の希土類元素)を含有するZrO2を含む固体電解質層112と、固体電解質層112の一方側に配置された空気極層114と、固体電解質層112の他方側に配置され、希土類元素(第2の希土類元素)を含有するCeO2と、NiまたはNi含有合金と、を含む燃料極活性層220とを備える。本実施形態のセル110は、さらに、固体電解質層112と燃料極活性層220との間に配置され、ZrとCeと上記第1の希土類元素と上記第2の希土類元素とを含有する固溶体を含む中間層190を備える。
上述した実施形態のセル110のサンプルを複数作製し、作製された複数のセル110のサンプルを用いて性能評価を行った。図6は、性能評価結果を示す説明図である。
図6に示すように、各サンプル(S1〜S12)は、固体電解質層112、燃料極活性層220および中間層190の構成が互いに異なっている。具体的には、固体電解質層112に関し、サンプルS1〜S8、S10〜S12では、固体電解質層112がYSZを含むように構成されており、サンプルS9では、固体電解質層112がSc(スカンジウム)を含有するZrO2(以下、「ScSZ」という)を含むように構成されている。なお、以下の説明では、固体電解質層112に含まれる希土類元素を「第1の希土類元素E1」という。サンプルS1〜S8、S10〜S12では、第1の希土類元素E1はYであり、サンプルS9では、第1の希土類元素E1はScである。
各サンプルのセル110を、上述した実施形態において説明した製造方法に従って作製した。各サンプルのセル110の詳細な作製方法は、以下の通りである。
作製された各サンプルのセル110を以下の方法に従い分析した。すなわち、各サンプルのセル110を所定の長さに切断し、エポキシ樹脂に埋め込んで固化した後、各層の積層方向に略平行な断面が観察できるように切断して、鏡面状に研磨した。その後、研磨面(観察面)にカーボン蒸着を行った後、EPMAにより、中間層190についての画像取得、元素ライン分析および元素定量分析を行った。
図7に示すように、作製した各サンプルのセル110について、燃料極層116が露出した部分に第1銀線201および第3銀線203を巻き付け、銀ペーストを塗布することにより、燃料極端子を形成した。また、セル110における空気極層114が形成された部分を白金網205で覆い、白金網205上に第2銀線202および第4銀線204を接続し、白金網205上に集電用の導電性ペーストを塗布して電気炉236で焼き付けることにより、空気極端子を形成した。また、各セル110の両端における固体電解質層112の露出部分を、ガラス材料206によりガスシール固定した。
図6に示すように、いずれのサンプル(S1〜S12)でも、中間層190の固体電解質層112側の界面および燃料極活性層220側の界面において、完全な剥離は発生しなかった。また、いずれのサンプル(S1〜S12)でも、発電性能についての評価結果は、「良(△)」以上であり、「不良(×)」と判定されたものは無かった。そのため、上記実施形態のように、セル110が、第1の希土類元素E1を含有するZrO2を含む固体電解質層112と、固体電解質層112の一方側に配置された空気極層114と、固体電解質層112の他方側に配置され、第2の希土類元素E2を含有するCeO2と、NiまたはNi含有合金と、を含む燃料極活性層220と、固体電解質層112と燃料極活性層220との間に配置され、ZrとCeと第1の希土類元素E1と第2の希土類元素E2とを含有する固溶体を含む中間層190と、を備える構成を採用すれば、燃料極活性層220と固体電解質層112との間の剥離の発生を抑制することができると共に、燃料極活性層220と固体電解質層112との間の相互元素拡散を抑制することができ、セル110の性能が低下することを抑制することができることが確認された。
本明細書で開示される技術は、上述の実施形態に限られるものではなく、その要旨を逸脱しない範囲において種々の形態に変形することができ、例えば次のような変形も可能である。
Claims (9)
- 第1の希土類元素を含有するZrO2を含む固体電解質層と、
前記固体電解質層の一方側に配置された空気極と、
前記固体電解質層の他方側に配置され、第2の希土類元素を含有するCeO2と、NiまたはNi含有合金と、を含む燃料極と、
を備える電気化学セルにおいて、さらに、
前記固体電解質層と前記燃料極との間に配置され、ZrとCeと前記第1の希土類元素と前記第2の希土類元素とを含有する固溶体を含む中間層を備えることを特徴とする、電気化学セル。 - 請求項1に記載の電気化学セルにおいて、
前記中間層におけるZrとCeと前記第1の希土類元素と前記第2の希土類元素との合計量に対する、ZrとCeとの合計量の割合は、30at%以上であることを特徴とする、電気化学セル。 - 請求項1または請求項2に記載の電気化学セルにおいて、
前記中間層におけるZrとCeと前記第1の希土類元素と前記第2の希土類元素との合計量に対する、Ceの量の割合は、10at%以上、70at%以下であることを特徴とする、電気化学セル。 - 請求項1から請求項3までのいずれか一項に記載の電気化学セルにおいて、
前記中間層におけるZrとCeと前記第1の希土類元素と前記第2の希土類元素との合計量に対する、Zrの量の割合は、10at%以上、70at%以下であることを特徴とする、電気化学セル。 - 請求項1から請求項4までのいずれか一項に記載の電気化学セルにおいて、
前記中間層の厚さは、10μm以下であることを特徴とする、電気化学セル。 - 請求項1から請求項5までのいずれか一項に記載の電気化学セルにおいて、
前記中間層におけるZrとCeと前記第1の希土類元素と前記第2の希土類元素との合計量に対する、ZrとCeとの合計量の割合は、90at%以下であることを特徴とする、電気化学セル。 - 請求項1から請求項6までのいずれか一項に記載の電気化学セルにおいて、
前記電気化学セルは、固体酸化物形燃料電池用のセル、または、固体酸化物形電解セル用のセルであることを特徴とする、電気化学セル。 - 複数の電気化学セルを備える電気化学スタックにおいて、
前記複数の電気化学セルの少なくとも1つは、請求項1から請求項7までのいずれか一項に記載の電気化学セルであることを特徴とする、電気化学スタック。 - 請求項8に記載の電気化学スタックにおいて、
前記電気化学スタックは、固体酸化物形燃料電池用のスタック、または、固体酸化物形電解セル用のスタックであることを特徴とする、電気化学スタック。
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WO2023054494A1 (ja) * | 2021-09-30 | 2023-04-06 | 京セラ株式会社 | 電気化学セル、電気化学セル装置、モジュールおよびモジュール収容装置 |
WO2023195246A1 (ja) * | 2022-04-05 | 2023-10-12 | 日本碍子株式会社 | 電気化学セル |
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