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酸素に富んだペロブスキート酸化物を開発するためのカチオン置換戦略は,高効率の窒素電解をアンモニアに可能にします
Kaibin Chu1,2, Wei Zong1, Guohao Xue1
1The Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, International Joint Research Laboratory for Nano Energy Composites, Jiangnan University, Wuxi 214122, China.
Journal of the American Chemical Society
|September 20, 2023
まとめ
研究者らは,アンモニアを合成する電気触媒性窒素還元反応 (eNITRR) のための新しいペロブスキート亜微繊維を開発した. 銅で置き換えられたLaFe0.9Cu0.1O3-δは,酸素の空隙と表面の可能性を最適化することによって,アンモニアの収量と選択性を著しく高めました.
科学分野:
- 材料科学
- 電気化学
- カタリシス
背景:
- 電子触媒性窒素還元反応 (eNITRR) は,アンモニア合成の有望な経路である.
- 現在のeNITRR方法は,複雑なマルチ電子プロセスにより,選択性が低い課題に直面しています.
研究 の 目的:
- 強化されたENITRRのための新しいペロブスキート亜微細繊維の設計と合成.
- 電気触媒性能に対するB位カチオン置換の効果を調査する.
主な方法:
- 酸素濃度の高いLaFe0.9M0.1O3-δ (M = Co,Ni,Cu) のペロブスキート亜微繊維の合成
- アンモニア合成の電気触媒性能試験
- COMSOL マルチフィジックシミュレーションと現地特徴付け
- 反応メカニズムを解明するための密度関数理論 (DFT) の計算.
主要な成果:
- LaFe0.9Cu0.1O3-δは,高いアンモニア出力率 (349 ± 15 μg h-1 mg-1cat) とファラダイク効率 (48 ± 2%) を示した.
- 銅の置換により酸素の空白が増加し,陽性な表面ポテンシャルが生まれ,窒素の吸収が強化され,水素の進化が抑制された.
- DFT計算では,最初の陽子電子結合ステップが,エネルギーバリアが低下した速度決定ステップであると特定されました.
結論:
- ペロブスキットのカチオン置換は,ENITRRの性能を改善するための効果的な戦略です.
- 最適化されたLaFe0.9Cu0.1O3-δ触媒は,効率的な電気触媒アンモニア合成のための有望な経路を提供します.
- 反応メカニズムの理解は,将来の電気触媒の設計のための洞察を提供します.
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