Turn the Harm into A Benefit: Axial Cl Adsorption on Curved Fe‐N ₄ Single Sites for Boosted Oxygen Reduction Reaction in Seawater

Seawater electrocatalysis is urgently needed for various energy storage and conversion systems. However, the adsorption of chloride ions (Cl^-) to the active sites can degrade the oxygen reduction reaction (ORR) activity and stability, thus reducing the catalytic performance. In this paper, a curved FeN₄ single atomic structure is designed by utilizing curvature engineering, which can turns the harmful Cl adsorption into a benefit on the Fe single site that changes the rate determining step of ORR and reduces the overall energy barrier according to density functional theory (DFT) calculation. Experimental studies reveal the prepared highly-curved single-atom iron catalyst (HC-Fe_SA) exhibits excellent ORR activity in different electrolytes, with half-wave potentials of 0.90 V in 0.1 M KOH, 0.90 V in simulated seawater, and 0.75 V in natural seawater, respectively. This work opens up an avenue for the synthesis of high-performance seawater-based single-atom ORR catalysts through regulating the local atomic curvature.