▌Evoking dynamic Fe-Nx active sites through the immobilization of molecular Fe catalysts on N-doped graphene quantum dots for the efficient electroreduction of nitrate to ammonia
分子鐵催化劑固定於氮摻雜石墨烯量子點上誘發動態Fe-Nx活性位點實現高效硝酸鹽電還原製氨
Major Contributions
1. Successfully developed a novel catalyst by immobilizing molecular Fe on N-doped graphene quantum dots (NGQDs), achieving remarkable performance with 93% Faradaic efficiency and a high NH3 yield rate of 15.41 mmol h-1 cm-2 at -0.8V vs RHE in alkaline conditions.
2. Demonstrated that the formation of molecular Fe-Nx coordination sites is crucial for activating the nitrate reduction reaction, despite NGQDs being initially inactive, providing new insights into the role of metal-nitrogen coordination in electrocatalysis.
3. Revealed a preferential sequential electron transfer mechanism (2e- followed by 6e-) over the direct 8e- pathway in nitrate reduction reaction, offering new mechanistic understanding for future catalyst design.
主要貢獻
1. 成功開發了一種將分子鐵固定在氮摻雜石墨烯量子點上的新型催化劑,在鹼性條件下於-0.8V vs RHE電位下實現93%的法拉第效率和15.41 mmol h-1 cm-2的高氨產率。
證實了分子Fe-Nx配位位點的形成對啟動硝酸鹽還原反應至關重要,儘管NGQDs最初並不活躍,為金屬-氮配位在電催化中的作用提供了新見解。
揭示了硝酸鹽還原反應中優先採用序貫式電子轉移機制(先2e-後6e-)而非直接8e-途徑,為未來催化劑設計提供了新的機理理解。