题 目：Over 56.55% Faradaic efficiency of ambient ammonia synthesis enabled by positively shifting the reaction potential
作 者：Mengfan Wang1, Sisi Liu1, Tao Qian1, Jie Liu1, Jinqiu Zhou1, Haoqing Ji1, Jie Xiong2, Jun Zhong3, Chenglin Yan1
1.College of Energy, Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, 215006, Suzhou, China.
2. University of Electronic Science and Technology of China, 610054, Chengdu Sichuan, China.
3. Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, 215123 Suzhou, China.
摘 要：Ambient electrochemical N2 reduction is emerging as a highly promising alternative to the Haber–Bosch process but is typically hampered by a high reaction barrier and competing hydrogen evolution, leading to an extremely low Faradaic efficiency. Here, we demonstrate that under ambient conditions, a single-atom catalyst, iron on nitrogen-doped carbon, could positively shift the ammonia synthesis process to an onset potential of 0.193?V, enabling a dramatically enhanced Faradaic efficiency of 56.55%. The only doublet coupling representing NH4+ in an isotopic labeling experiment confirms reliable NH3 production data. Molecular dynamics simulations suggest efficient N2 access to the single-atom iron with only a small energy barrier, which benefits preferential N2 adsorption instead of H adsorption via a strong exothermic process, as further confirmed by first-principle calculations. The released energy helps promote the following process and the reaction bottleneck, which is widely considered to be the first hydrogenation step, is successfully overcome.