JP2018085329A - 膜電極接合体および固体酸化物形燃料電池 - Google Patents
膜電極接合体および固体酸化物形燃料電池 Download PDFInfo
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Abstract
Description
本発明者らは、特許文献1に開示された従来の固体電解質層積層体(膜電極接合体)に関して鋭意検討を行った。その結果、以下の知見を得た。すなわち、本発明者らは、膜電極接合体を電気化学デバイスに用いるに際して、特許文献1に開示された膜電極接合体よりも、高い発電効率を得ることができる膜電極接合体を見出した。
本発明の実施の形態1に係る膜電極接合体10について、図1を参照して説明する。図1は、本発明の実施の形態1に係る膜電極接合体10の構成を模式的に示す図である。膜電極接合体10は、電気化学デバイスを構成するために用いられる部材であり、図1に示すように、電極11と、第1の固体電解質膜12とを備え、電極11と第1の固体電解質膜12とが接した構造となっている。換言すると、膜電極接合体10は、第1の固体電解質膜12の一方の側面側で電極11と接しており、両者を積層させた構造となっている。
本発明の実施の形態2に係る膜電極接合体20について、図2を参照して説明する。図2は、本発明の実施の形態2に係る膜電極接合体20の構成を模式的に示す図である。膜電極接合体20は、電極11と、第1の固体電解質膜12と、第2の固体電解質膜13とを備え、電極11、第1の固体電解質膜12、第2の固体電解質膜13の順に積層された構造となっている。換言すると、第1の固体電解質膜12は、その一方側の面で電極11と接し、該一方側の面とは反対側となる他方側の面において第2の固体電解質膜13と接する構成となっている。つまり、実施の形態2に係る膜電極接合体20は、実施の形態1に係る膜電極接合体10の構成と比較して、さらに第2の固体電解質膜13を備えた構成である。
本発明の実施の形態3に係る膜電極接合体30について、図3を用いて説明する。図3は、本発明の実施の形態3に係る膜電極接合体30の構成の一例を模式的に示す図である。さらに本発明の実施の形態3の変形例に係る膜電極接合体40について、図4を用いて説明する。図4は、本発明の実施の形態3の変形例に係る膜電極接合体40の構成の一例を模式的に示す図である。
次に、実施の形態1、2、3、および実施の形態3の変形例に係る膜電極接合体10、20、30、および40の構成において示すように、LSC、LSCF、およびLSF、からなる群より選ばれる少なくとも1種類の化合物(酸化物イオン・電子混合伝導体材料)を用いて構成された電極と、組成式がBaZr1−xLuxO3−δ(0<x<1)で表される第1の固体電解質膜12とを組合せた構成を有することで、発電効率が高くなるという知見に至った評価方法について、以下に実施例として説明する。なお、本発明は以下の実施例により制限されるものではない。
[実施例2]電極11がLa0.6Sr0.4Co0.2Fe0.8O3−δ、第1の固体電解質膜12がBaZr0.8Lu0.2O2.90である評価用膜電極接合体100
[実施例3]電極11がLa0.6Sr0.4FeO3−δ、第1の固体電解質膜12がBaZr0.8Lu0.2O2.90である評価用膜電極接合体100
[比較例2]電極11がLa2NiO4+δ、第1の固体電解質膜12がBaZr0.8Lu0.2O2.90である評価用膜電極接合体100
[比較例3]電極11がLa0.6Sr0.4CoO3−δ、第1の固体電解質膜12がBaZr0.8Y0.2O2.90である評価用膜電極接合体100
[比較例4]電極11がLa0.6Sr0.4Co0.2Fe0.8O3−δ、第1の固体電解質膜12がBaZr0.8Y0.2O2.90である評価用膜電極接合体100
[比較例5]電極11がLa0.6Sr0.4FeO3−δ、第1の固体電解質膜12がBaZr0.8Y0.2O2.90である評価用膜電極接合体100
[比較例6]電極11がLaNi0.6Fe0.4O3−δ、第1の固体電解質膜12がBaZr0.8Y0.2O2.90である評価用膜電極接合体100
[比較例7]電極11がLa2NiO4+δ、第1の固体電解質膜12がBaZr0.8Y0.2O2.90である評価用膜電極接合体100
以下、実施例1〜3および比較例1〜7における評価用膜電極接合体100の製造方法について説明する。
続いて、上記の製造方法により製造した評価用膜電極接合体100において電極11と第1の固体電解質膜12との間に生じる接触抵抗の測定方法について図7を参照して説明する。図7は、本発明の実施例および比較例に係る第1の固体電解質膜12の厚みとIR抵抗との相関関係の一例を示すグラフである。図7では、電極11にAgを用いたときの第1の固体電解質膜12の層厚とIR抵抗との相関関係を実線のグラフで示している。また、本発明の実施例および比較例に係る第1の固体電解質膜12の層厚とIR抵抗との相関関係については破線により示している。なお、評価用膜電極接合体100における電極11と第1の固体電解質膜12との間に生じる接触抵抗を、交流インピーダンス法によって測定した。
11 電極
12 第1の固体電解質膜
13 第2の固体電解質膜
14 アノード電極
20 膜電極接合体
30 膜電極接合体
40 膜電極接合体
100 評価用膜電極接合体
Claims (5)
- ランタンストロンチウムコバルト複合酸化物、ランタンストロンチウムコバルト鉄複合酸化物、およびランタンストロンチウム鉄複合酸化物からなる群より選ばれる少なくとも1種類の化合物、または該化合物および電解質材料の複合体からなる電極と、
組成式がBaZr1−xLuxO3−δ(0<x<1)で表される第1の固体電解質膜と、を備え、
前記電極と前記第1の固体電解質膜とが接している膜電極接合体。 - 組成式がBaZr1−x1M1 x1O3−δ(M1は、La、Pr、Nd、Pm、Sm、Eu、Gd、Tb、Dy、Ho、Er、Tm、Yb、Y、Sc、Mn、Fe、Co、Ni、Al、Ga、およびInからなる群より選ばれる少なくとも1種類の元素、0<x1<1)で表される第2の固体電解質膜をさらに備え、
前記第1の固体電解質膜は、一方側の面で前記電極と接し、該一方側の面とは反対側となる他方側の面において、前記第2の固体電解質膜と接しており、
前記電極、前記第1の固体電解質膜、前記第2の固体電解質膜の順に積層されている請求項1に記載の膜電極接合体。 - 前記電極はカソード電極であり、
BaZr1−x2M2 x2O3−δ、BaCe1−x3M3 x3O3−δ、およびBaZr1−x4−y4Cex4M4 y4O3−δ(M2、M3、M4は、La、Pr、Nd、Pm、Sm、Eu、Gd、Tb、Dy、Ho、Er、Tm、Yb、Y、Sc、Mn、Fe、Co、Ni、Al、Ga、In、およびLuからなる群より選ばれる少なくとも1種類の元素、0<x2<1、0<x3<1、0<x4<1、0<y4<1)のうちのいずれか1つの組成式で表される化合物と、Niとを含むアノード電極をさらに備え、
前記第1の固体電解質膜は、前記カソード電極と一方側の面で接し、該一方側の面とは反対側となる他方側の面において、前記アノード電極と接しており、
前記カソード電極、前記第1の固体電解質膜、前記アノード電極の順に積層されている請求項1に記載の膜電極接合体。 - 前記電極はカソード電極であり、
BaZr1−x2M2 x2O3−δ、BaCe1−x3M3 x3O3−δ、およびBaZr1−x4−y4Cex4M4 y4O3−δ(M2、M3、M4は、La、Pr、Nd、Pm、Sm、Eu、Gd、Tb、Dy、Ho、Er、Tm、Yb、Y、Sc、Mn、Fe、Co、Ni、Al、Ga、In、およびLuからなる群より選ばれる少なくとも1種類の元素、0<x2<1、0<x3<1、0<x4<1、0<y4<1)のうちのいずれか1つの組成式で表される化合物と、Niとを含むアノード電極をさらに備え、
前記第2の固体電解質膜は、一方側の面で前記第1の固体電解質膜と接し、該一方側の面とは反対側となる他方側の面において、前記アノード電極と接しており、
前記カソード電極、前記第1の固体電解質膜、前記第2の固体電解質膜、前記アノード電極の順に積層されている請求項2に記載の膜電極接合体。 - 請求項1〜4のいずれか1項に記載の膜電極接合体を備える固体酸化物形燃料電池。
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