Electrochemical synthesis of ammonia under environmental conditions is a beautiful dream of scientists and entrepreneurs, and has been regarded as an ideal alternative strategy to traditional Haber-Bosch process. In this study of synthetic ammonia, we rationally consider the defects of the current catalysts and propose innovative preparation methods. For the first time, we synthesized independent, highly dispersed zero-valent copper atomic catalysts which were uniformly distributed on 2D graphdiyne (Cu⁰/GDYNA). This catalyst was used for electrochemical NO₃^--to-NH₃ conversion. After dozens of rigorous experiments, an exciting result are presented that the Cu⁰/GDYNA showed the highest NH₃ yield rate (Y_NH3) of 15.45 mmol h⁻¹ cm⁻² and the maximal ammonia Faradaic efficiency (FE) of 81.25% at ambient temperatures and pressures. Furthermore, the Cu⁰/GDYNA could continuously catalyze the ammonia production over a consecutive 36-cycle electrolysis with almost no loss of catalytic performance. The excellent electrocatalytic properties of atomic catalysts show that the incomplete charge transfer behavior between metal atoms and GDY produces continuous high activity, promotes ammonia production rapidly selectively suppresses inhibitory by-products, and achieves ultra-high ammonia yield and FE.

在环境条件下电化学合成氨是科学家和企业家的美好梦想，被视为传统哈伯-博世工艺的理想替代策略。在本次合成氨研究中，我们合理考虑了现有催化剂的缺陷，提出了创新的制备方法。我们首次合成了独立的、高度分散的零价铜原子催化剂，该催化剂均匀分布在二维石墨二炔（Cu ⁰ /GDYNA）上。该催化剂用于电化学NO ₃ ^-至NH ₃转化。经过数十次严格的实验，令人兴奋的结果是Cu ⁰ /GDYNA显示出最高的NH ₃在环境温度和压力下，产率 (Y _NH3 ) 为 15.45 mmol h ^-1 cm ^{-2 ，最大氨法拉第效率 (FE) 为 81.25%。}此外，Cu ⁰ /GDYNA 可以在连续的 36 个循环电解过程中连续催化氨的产生，而催化性能几乎没有损失。原子催化剂优异的电催化性能表明，金属原子与GDY之间不完全的电荷转移行为产生持续的高活性，快速促进氨生成，选择性抑制抑制性副产物，实现超高氨产率和FE。