JP2023542450A - 燃料電池で金属ナノ粒子を使用してアンモニアを合成する方法 - Google Patents
燃料電池で金属ナノ粒子を使用してアンモニアを合成する方法 Download PDFInfo
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- JP2023542450A JP2023542450A JP2023501251A JP2023501251A JP2023542450A JP 2023542450 A JP2023542450 A JP 2023542450A JP 2023501251 A JP2023501251 A JP 2023501251A JP 2023501251 A JP2023501251 A JP 2023501251A JP 2023542450 A JP2023542450 A JP 2023542450A
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Abstract
Description
本出願は、2020年7月6日に出願された米国仮特許出願第63/048,262号の優先権を主張し、その内容全体が引用により本明細書に組み込まれる。
N2(g)+3H2(g)→2NH3(g)
H2→2H++2e-
N2+6H++6e-→2NH3
電子(e-)は、アノードから電子回路に流れ、カソードに戻り、そこで窒素ガス(N2)を還元するために使用される。電子回路は、電子の流れを使用してデバイスを給電する。
種々の触媒の電気化学的活性を比較するために、プロトン伝導性を有する電解質を使用して、固体酸化物燃料電池を形成した。具体的には、24時間ボールミルによってLGSM粉末と1~3重量%の適切な結合剤系(ポリビニルアルコール)を混合することによって、電解質支持体を作製した。その後、混合物を完全に乾燥するまで(少なくとも1時間)、100℃~200℃の温度で乾燥させ、100μmの篩を用いて分けた。3グラム(3g)の粉末を、10MPaの圧力でディスクペレットにペレット化した。ペレットを4時間1450℃で焼結した。
電極の表面積および対応する生成速度を増加させるために、足場構造の電極を導入した。特に、金属ナノ粒子をLSGM足場に分散させるために2つの方法を使用した。第1の方法では、直接足場上に金属前駆体を浸透させることによって、金属ナノ粒子を合成した。第2の方法では、非常に小さく(約10nm~約30nm)均一なサイズのナノ粒子を、コロイド法によって予め合成し、溶液の形態でLSGM足場上に分散させた。
ナノ粒子の分布は、足場に分散された触媒の量が変化した場合にのみ視覚的に区別され、経験的に決定された初期溶液の濃度および量は、いくつかの金属の均一な分散を達成するのに適していた。特に、分散量を変化させることに関する試験を金属の各々に対して行なったが、本明細書においては、代表例としてニッケルが使用される。
ANSYSソフトウェアを使用した流路の流路流れ設計シミュレーションを使用して、電極の形態学的効果を排除するための研究を行った。特に、流路の設計を評価して、電極の一方の側から他方の側への高い圧力勾配を有する設計を特定したが、この高い圧力勾配は、拡散力を促進すると考えられている。シミュレーションの結果を図5A~5Cに示す。シミュレーションでは、流路の設計をジグザグ型の設計に変更し(図5C)、これにより、アンモニアの生成速度が最大で5.21×10-10mol/cm2*sまで向上した。
非対称燃料電池構成も試験した。特に、アノードおよびカソード各々の材料を変更した。NH3収率を、金アノードと金カソード(サンプルA)、白金アノードと白金カソード(サンプルB)、銀アノードと銀カソード(サンプルC、D、およびE)、および白金アノードと銀浸透LGSMカソード(サンプルF)を有するサンプルについて測定し、結果を図6に示す。サンプルA、B、およびCは1.6Vの電圧を使用し、サンプルD、E、およびFは2Vの電圧を使用した。サンプルEは、流路がジグザグ構成になるように流路の改変を含んだ一方で、サンプルA、B、C、D、およびFは、図5Aの流路構成を使用した。
電気化学インピーダンス分光法(EIS)を、単純な薄膜銀電極(比較)と銀浸透LSGM足場(本発明)を使用して実施した。その後、これらの調製したサンプルをEISにかけた。図7は、X軸上のインピーダンス測定の実部(Z’)およびY軸上のインピーダンス測定の虚部(Z’’)のナイキストプロットを提供する。浸透電極を採用することによって、アンモニア合成を意図した条件下での電気化学的特性が改善される。
Claims (9)
- カソード、アノード、および前記アノードと前記カソードとの間に配された固体酸化物電解質を含む固体酸化物燃料電池であって、
前記固体酸化物電解質が、La0.8Sr0.2Ga0.83Mg0.17O2.815(LSGM)を含み;かつ
前記アノードが多孔性足場を含み、前記多孔性足場が、LSGMと、前記多孔性足場の表面に配された1つまたは複数の金属ナノ粒子とを含み、前記金属ナノ粒子が、白金、ニッケル、金、およびそれらの組み合わせからなる群より選択される、
固体酸化物燃料電池。 - 前記カソードが多孔性足場を含み、前記多孔性足場が、LSGMと、前記多孔性足場の表面に配された1つまたは複数の金属ナノ粒子とを含み、前記金属ナノ粒子が、白金、ニッケル、金、およびそれらの組み合わせからなる群より選択される、請求項1記載の固体酸化物燃料電池。
- 前記カソードが多孔性足場を含み、前記多孔性足場が、前記多孔性足場の1つまたは複数の表面に配された金属系触媒を有する固体酸化物を含む、請求項1記載の固体酸化物燃料電池。
- 前記カソードが、La1-xSrxMnO3(LSM)を浸透させたLa0.6Sr0.4Co0.2Fe0.8O3(LSCF)を含む、請求項1~3のいずれか1項に記載の固体酸化物燃料電池。
- 燃料電池においてアンモニアを生成する方法であって、
水素イオンを生成するために、電子を取り除くことにより燃料電池のアノードで水素ガスをイオン化する工程であり、前記燃料電池が、カソード、前記アノード、および前記アノードと前記カソードとの間のプロトン伝導性電解質を含み、ここで
前記プロトン伝導性電解質が、La0.8Sr0.2Ga0.83Mg0.17O2.815(LSGM)を含み;かつ
前記アノードが多孔性足場を含み、前記多孔性足場が、LSGMと、前記多孔性足場の表面に配された1つまたは複数の金属ナノ粒子とを含み、前記金属ナノ粒子が、白金、ニッケル、金、およびそれらの組み合わせからなる群より選択される工程;
前記水素イオンを、前記プロトン伝導性電解質を介して前記カソードに送る工程;
前記電子を前記アノードから前記カソードに送る工程;および
窒素ガスを前記カソードに送る工程であり、前記水素イオンと前記窒素ガスが反応してアンモニアを生成する工程
を含む方法。 - 前記カソードが多孔性足場を含み、前記多孔性足場が、LSGMと、前記多孔性足場の表面に配された1つまたは複数の金属ナノ粒子とを含み、前記金属ナノ粒子が、白金、ニッケル、金、およびそれらの組み合わせからなる群より選択される、請求項5記載の方法。
- 前記カソードが多孔性足場を含み、前記多孔性足場が、前記多孔性足場の1つまたは複数の表面に配された金属系触媒を有する固体酸化物を含む、請求項5記載の方法。
- 前記カソードが、La1-xSrxMnO3(LSM)を浸透させたLa0.6Sr0.4Co0.2Fe0.8O3(LSCF)を含む、請求項5~7のいずれか1項に記載の方法。
- 前記電子を前記アノードから前記カソードに送る工程が、前記電子を前記アノードから電子回路を通して前記カソードに送ることを含む、請求項5~7のいずれか1項に記載の方法。
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