▌Hydroxyl-rich nanocavities on perovskite enable nearly barrierless intramolecular hydrogen transfer for nitrate electroreduction to ammonia
鈣鈦礦表面富羥基奈米空腔實現近乎無能障的分子內氫轉移,用於硝酸根電還原產氨
Mingkai Xu, Ruizhao Wang, Zaixing Wang, Zheng Tang, Wei-Hsiang Huang, Wang Tan, Lingjie Yuan, Huanhuan Tao, Zhongliang Dong, Min-Hsin Yeh, Chih-Wen Pao, Jun Yin, Zhiwei Hu, Jie Dai* and Yinlong Zhu*
https://doi.org/10.1038/s41467-026-74405-1
SEED Member: Min-Hsin Yeh, Wei-Hsiang Huang

Major Contributions
1. Constructed hydroxyl-rich nanocavities on La₀.₄Sr₀.₆FeO₃₋δ perovskite by electrochemical reduction-assisted selective Sr leaching, creating nanocavity walls enriched with hydroxyl groups.
2. Experiments and theory reveal a nearly barrierless hydrogen-transfer pathway along intramolecular hydrogen bonds between hydroxyls, boosting active hydrogen generation and hopping for NO₃⁻ hydrogenation.
3. The catalyst reaches a Faradaic efficiency of 97.81% and an NH₃ yield of 51.37 mg h⁻¹ cm⁻² at −0.8 V vs RHE, and ampere-level conversion at 2.23 V in a renewable-powered electrolyzer; techno-economic analysis supports its viability.
主要貢獻
1. 以電化學還原輔助選擇性溶出鍶離子,在 La₀.₄Sr₀.₆FeO₃₋δ 鈣鈦礦表面建構壁面富含羥基的奈米空腔。
2. 實驗與理論計算顯示,氫可沿羥基間的分子內氫鍵以近乎無能障的路徑轉移,促進活性氫生成與跳躍,加速 NO₃⁻ 氫化。
3. 於 −0.8 V vs RHE 下法拉第效率 97.81%、NH₃ 產率 51.37 mg h⁻¹ cm⁻²;在再生能源供電的電解槽中以 2.23 V 達到安培級電流,技術經濟分析顯示具可行性。




