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Sp‐Hybridized Nitrogen as New Anchoring Sites of Iron Single Atoms to Boost the Oxygen Reduction Reaction

Von Wiley-VCH zur Verfügung gestellt

Based on the specific structure of graphdiyne (GDY), an atomic Fe catalyst anchored by sp-N was designed and synthesized, which tailored the electronic structure of Fe and thus changed the binding energy between Fe centers and intermediate species in the ORR process. The as-synthesized catalyst (Fe−N−GDY) exhibited excellent oxygen reduction performance and achieved long-term stability in the assembled zinc–air battery.


Abstract

Carbon supported single-atom catalysts with metal-Nx configuration are considered as one of the most efficient catalysts for the oxygen reduction reaction (ORR). However, most of the metal-N x active sites are composed by pyridinic N at the defect locations of graphene-like supports. Here, we employ graphdiyne (GDY) as a new carbon substrate to synthesize an iron (Fe) single atom catalyst (Fe−N−GDY), showing excellent catalytic performance. Benefitting from the abundant acetylenic bonds in GDY, sp-N anchored metal atoms are created without forming defects. The sp-N and OH ligands regulate the electronic structure of Fe atoms and optimize the adsorption energy of ORR intermediates on the active sites by reducing the electron local density of Fe atoms, which accelerates the reaction kinetics and promotes the ORR activity of Fe−N−GDY. Furthermore, the practical application of Fe−N−GDY is corroborated by its high power density and long-term performance via assembling a zinc–air battery.

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