Electrochemical N₂ reduction reaction (ENRR) at ambient temperature is a futuristic method for the artificial synthesis of ammonia, but it is still not efficient enough to be applied on a large scale. Inspired by the molybdenum-containing nitrogen-fixing enzymes of rhizobia in nature, single Mo sites are predicted to serve as an effective catalyst for ENRR. Herein, B/N codoped porous carbon nanotube-supported single Mo site catalysts (Mo/BCN) were rationally designed and synthesized. Mo/BCN exhibits the highest catalytic activity toward N₂ fixation to NH₃ with a yield rate of 37.67 μg h^–1 mg_cat^–1 and a faradaic efficiency of 13.27% in 0.1 M KOH, which is better than those of nonprecious metal electrocatalysts. Density functional theory and extended X-ray absorption fine structure analysis indicated that single-atom Mo sites could be anchored on BCN nanotubes and act as sufficient active sites for nitrogen reduction. The present work may provide a theoretical and experimental strategy for developing efficient single-atom catalysts for ENRR.

中文翻译：

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在 B/N 共掺杂多孔碳纳米管上锚定 Mo 单原子位点用于将 N2 电化学还原为 NH3

环境温度下的电化学 N ₂还原反应 (ENRR) 是一种用于人工合成氨的未来方法，但其效率仍不足以大规模应用。受自然界中根瘤菌的含钼固氮酶的启发，预测单个 Mo 位点可作为 ENRR 的有效催化剂。在此，合理设计和合成了 B/N 共掺杂多孔碳纳米管负载的单 Mo 位点催化剂 (Mo/BCN)。Mo/BCN 对 N ₂固定到 NH ₃的催化活性最高，产率为 37.67 μg h ^–1 mg _cat ^–1在 0.1 M KOH 中的法拉第效率为 13.27%，优于非贵金属电催化剂。密度泛函理论和扩展 X 射线吸收精细结构分析表明，单原子 Mo 位点可以锚定在 BCN 纳米管上，并作为氮还原的足够活性位点。目前的工作可以为开发高效的 ENRR 单原子催化剂提供理论和实验策略。