Green production of NH₃, especially the Li‐mediated electrochemical N₂ reduction reaction (NRR) in non‐aqueous solutions, is attracting research interest. Controversies regarding the NRR mechanism greatly impede its optimization and wide applications. To understand the electrocatalytic process, we treated Au coated carbon fibrous paper (Au/CP) as the model catalyst. In situ XRD confirmed the transformation of lithium intermediates during NRR. Au greatly improved electron transfer kinetics to catalyze metallic Li formation, and accordingly highly accelerated spontaneous NRR. The Faradaic efficiency of NRR on Au/CP reached 34.0 %, and NH₃ yield was as high as 50 μg h⁻¹ cm⁻². Our research shows that the key step of Li‐mediated non‐aqueous NRR is electrocatalytic Li reduction and offers a novel electrocatalyst design method for Li reduction.

中文翻译：

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多米诺骨牌效应：金电催化还原锂加速固氮

NH _3的绿色生产，尤其是在非水溶液中的Li介导的电化学N ₂还原反应（NRR），引起了研究兴趣。有关NRR机制的争议极大地阻碍了其优化和广泛应用。为了了解电催化过程，我们将Au涂层碳纤维纸（Au / CP）作为模型催化剂。原位XRD证实了NRR期间锂中间体的转变。金极大地改善了电子转移动力学，以催化金属Li的形成，并因此大大加速了自发NRR。NRR对Au / CP的法拉第效率达到34.0％，NH ₃产率高达50μgh ^-1  cm ^-2。我们的研究表明，Li介导的非水NRR的关键步骤是电催化还原Li，并为Li还原提供了一种新颖的电催化剂设计方法。