Designing a Novel C3‐Fe‐N Interface Local Coordination Microenvironment for Efficient Electrocatalytic Water Splitting

Abstract Developing single‐atomic electrocatalysts (SACs) with high activity and stability for electrocatalytic water‐splitting has been challenging. Moreover, the practical utilization of SACs is still far from meeting the the theoretical prediction. Herein a facile and easy scale‐up fabrication method is proposed for designing a novel carbon‐iron‐nitrogen (C‐Fe‐N) electrocatalyst with a single atom electron bridge (C‐Fe‐N SAEBs), which exhibits lower overpotential and impedance than previously reported electrocatalysts. 0.8‐C‐Fe‐N SAEBs exhibits significant activity and excellent stability in the bi‐functional decomposition of water. The excellent performance of the C‐Fe‐N SAEBs electrocatalyst can be attributed to the strong coupling effect at the interface owing to the formation of a single atom C 3 ‐Fe‐N local coordination microenvironment at the interface, which enhance the exposure of active sites and charge transfer, and reduced the adsorption energy barrier of intermediates. Theoretical calculation and synchrotron radiation analysis are performed to understand the mechanistic insights behind the experimental results. The results reveal that the active C 3 ‐Fe‐N local coordination microenvironment at the interface not only improves water‐splitting behavior but also provides a deeper understanding of local‐interface geometry/electronic structure for improving the electrocatalytic activity. Thus, the proposed electrocatalyst, as well as the mechanistic insights into its properties, presents a significant stride toward practical application.