JP2023529014A - 可逆的固体酸化物電池用プロトン導電性電解質 - Google Patents
可逆的固体酸化物電池用プロトン導電性電解質 Download PDFInfo
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- 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
- H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
- H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
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- H—ELECTRICITY
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- 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
- H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
- H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
- H01M8/126—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides the electrolyte containing cerium oxide
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- H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
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Abstract
Description
本明細書に開示されるのは、固体酸化物燃料電池で使用するためのプロトン導電性電解質を含むバリウムハフニウム酸塩である。開示される電解質はまた、電気分解動作及び二酸化炭素耐性に有用である。
本明細書に記載の材料、化合物、組成物、物品、及び方法は、開示された主題の特定の態様の以下の詳細な説明及びそれに含まれる実施例を参照することによって、より容易に理解することができる。
本明細書及び以下の特許請求の範囲では、以下の意味を有するように定義されるいくつかの用語を参照する。
本明細書における全てのパーセンテージ、比率、及び割合は、別段の指定がない限り、重量比である。全ての温度は、特に明記しない限り、摂氏(℃)である。
BaHfxCe0.8-xY0.1Yb0.1O3-δ
式中、添え字xは、約0.1~約0.5であり、便宜上、開示されるバリウム-ハフネートはBHCYYbとも表される。図2Aに示されるように、BHCYYbは、類似のドーパントレベルでのBZCYYb(ジルコニウム類似体)よりも高い安定性を有し、低ドーパントレベルでの同様の又はより高い導電率を有する。
BaMO3+CO2→BaCO3+MO2(1)
調製
BaHfxCe0.8-xY0.1Yb0.1O3(BHCYYb)及びBaZrxCe0.8-xY0.1Yb0.1O3(BZCYYB)粉末を、固体反応プロセスを使用して合成した(L.Yang et al.,Science(80).2009,326,126参照)。適切なモル比のBaCO3、HfO2又はZrO2、CeO2、Y2O3、及びYb2O3を十分に混合し、大きなパックにプレスし、1100℃で12時間焼成した。得られた粉末を、それぞれ5分の4サイクル、各サイクル間10分の休憩で、850RPMで高エネルギーボールミルした。ボールミルした粉末を再び大きなパックに押し付け、1100℃で10時間焼成し、続いて1450℃で5時間焼成した。最後に、各サイクル間10分の休憩で、粉末を各5分の6サイクルにわたって850RPMで高エネルギーボールミルした。1重量%のNiOを焼結助剤として添加した。粉末を590MPaで13ミリメートルのダイに押し込むことによって緻密ペレットが得られた。次いで、グリーンペレットを1450℃で5時間焼成した。
イオン導電率を求めるために、銀ペースト(燃料電池材料)で試料に銀電極を付着させ、2時間にわたり800℃に焼成した。導電率を、EG&G263Aポテンショスタット及びSolartron SI1255周波数応答分析器を使用して測定した。TGA測定は、1℃/分の冷却速度でCO2雰囲気中のTA Instruments SDT Q600で行った。CuKα1放射線を使用したPanalytical X’Pert Pro Alpha-1及び20~80の2θの範囲のXCelerator検出器で、0.013のo2θのステップサイズ及びステップ当たり68.6秒の有効期間でX線回折測定を行った。絞り込みは、Panalytical HighScore Plusソフトウェアを使用して実施した。走査型電子顕微鏡(SEM,Hitachi SU8010)を使用して、完全電池の断面顕微構造及び形態を調査した。
Ni-BHCYYb/BZCYYb負極支持層、Ni-BHCYYb/BZCYYb負極機能層、及びBHCYYb/BZCYYb電解質層の構成を有する半電池を、共テープ鋳造及び共焼結技術によって作製した。具体的には、BHCYYb/BZCYYb電解質粉末とBHCYYb/BZCYYb及びNiO粉末(NiO:電解質粉末=6:4重量比)との混合物を溶媒中で混合し、それぞれのスラリーを形成した。テープ鋳造用のスラリーはエタノール系であり、粉末に加えて分散剤、結合剤、可塑剤及び他の添加剤が含まれていた。電解質層を最初にマイラフィルム上に鋳造した。乾燥後、負極機能層を電解質層の上に鋳造し、続いて負極支持層を鋳造した。次いで、三層テープを乾燥させ、空気中で、1400℃で5時間共焼成した。有効面積が0.28cm2のPrBa0.5Sr0.5Co1.5Fe0.5O5+δ(PBSCF)陽極を、PBSCF粉末及びテルピネオール(5wt%エチルセルロース)の混合物を電解質層にスクリーン印刷し、950℃で2時間、空気中で焼成することによって調製した。PBSCF粉末を燃焼法により合成した。化学量論量のPr(NO3)3・6H2O、Ba(NO3)2、Sr(NO3)2、Co(NO3)2・6H2O,及びFe(NO3)3・6H2Oを、適切な量のエチレングリコール及び無水クエン酸(1:1比)を有する蒸留水に溶解した。溶液を空気中で350℃まで加熱し、続いて燃焼させて微粉末を形成した。次いで、得られた粉末を粉砕し、900℃で2時間再びか焼した。
Claims (4)
- 以下の式を有するプロトン導電性電解質であって、
BaHfxCe0.8-xY0.1Yb0.1O3-δ
式中、添え字xが、約0.1~約0.5である、プロトン導電性電解質。 - BaHf0.1Ce0.7Y0.1Yb0.1O3、BaHf0.2Ce0.6Y0.1Yb0.1O3、BaHf0.3Ce0.5Y0.1Yb0.1O3、BaHf0.4Ce0.4Y0.1Yb0.1O3、又はBaHf0.5Ce0.3Y0.1Yb0.1O3から選択される、請求項1に記載の電解質。
- 以下の式を有するバリウムハフニウムプロトン導電性電解質を含む固体燃料電池であって、
BaHfxCe0.8-xY0.1Yb0.1O3-δ
式中、添え字xが、約0.1~約0.5である、固体燃料電池。 - BaHf0.1Ce0.7Y0.1Yb0.1O3、BaHf0.2Ce0.6Y0.1Yb0.1O3、BaHf0.3Ce0.5Y0.1Yb0.1O3、BaHf0.4Ce0.4Y0.1Yb0.1O3、又はBaHf0.5Ce0.3Y0.1Yb0.1O3から選択される、請求項3に記載の電解質。
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JP2017076520A (ja) * | 2015-10-14 | 2017-04-20 | 株式会社ノリタケカンパニーリミテド | 固体酸化物形燃料電池用の電極材料とこれを用いた固体酸化物形燃料電池 |
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JP2017076520A (ja) * | 2015-10-14 | 2017-04-20 | 株式会社ノリタケカンパニーリミテド | 固体酸化物形燃料電池用の電極材料とこれを用いた固体酸化物形燃料電池 |
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KR20230018527A (ko) | 2023-02-07 |
US20220123341A1 (en) | 2022-04-21 |
CA3185740C (en) | 2023-06-20 |
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