Reconstructing 1D Fe Single‐atom Catalytic Structure on 2D Graphene Film for High‐Efficiency Oxygen Reduction Reaction

Abstract The ordinary intrinsic activity and disordered distribution of metal sites in zero/one‐dimensional (0D/1D) single‐atom catalysts (SACs) lead to inferior catalytic efficiency and short‐term endurance in the oxygen reduction reaction (ORR), which restricts the large‐scale application of hydrogen−oxygen fuel cells and metal−air batteries. To improve the activity of SACs, a mild synthesis method was chosen to conjugate 1D Fe SACs with 2D graphene film (Fe SAC@G) that realized a composite structure with well‐ordered atomic‐Fe coordination configuration. The product exhibits outstanding ORR electrocatalytic efficiency and stability in 0.1 M KOH aqueous solution. DFT‐D computational results manifest the intrinsic ORR activity of Fe SAC@G originated from the newly‐formed FeN 4 −O−FeN 4 bridge structure with moderate adsorption ability towards ORR intermediates. These findings provide new ways for designing SACs with high activity and long‐term stability.