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 -O-FeN bridge structure with moderate adsorption ability towards ORR intermediates. These findings provide new ways for designing SACs with high activity and long-term stability.

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http://dx.doi.org/10.1002/cssc.202002359DOI Listing

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