Journal
SCIENCE ADVANCES
Volume 9, Issue 23, Pages -Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.adg0366
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Here, a conceptual strategy for introducing spatial sulfur (S)-bridge ligands to regulate the coordination environment of Fe-Co-N dual-metal centers (Spa-S-Fe,Co/NC) is reported. The Spa-S-Fe,Co/NC catalyst showed significantly enhanced oxygen reduction reaction (ORR) performance and satisfactory long-term durability in acidic electrolyte. Experimental and theoretical studies revealed that the excellent acidic ORR activity with remarkable stability observed for Spa-S-Fe,Co/NC is attributable to the charge-modulation of Fe-Co-N bimetallic centers by the spatial S-bridge ligands, achieving optimal adsorption-desorption of ORR oxygenated intermediates. These findings provide a unique perspective to optimize the electrocatalytic performance of catalysts with dual-metal centers by regulating their local coordination environment.
Here, we report a conceptual strategy for introducing spatial sulfur (S)-bridge ligands to regulate the coordination environment of Fe-Co-N dual-metal centers (Spa-S-Fe,Co/NC). Benefiting from the electronic modulation, Spa-S-Fe,Co/NC catalyst showed remarkably enhanced oxygen reduction reaction (ORR) performance with a half-wave potential (E1/2) of 0.846 V and satisfactory long-term durability in acidic electrolyte. Combined experimental and theoretical studies revealed that the excellent acidic ORR activity with a remarkable stability observed for Spa-S-Fe,Co/NC is attributable to the optimal adsorption-desorption of ORR oxygenated intermediates achieved through charge-modulation of Fe-Co-N bimetallic centers by the spatial S-bridge ligands. These findings provide a unique perspective to regulate the local coordination environment of catalysts with dual-metal-centers to optimize their electrocatalytic performance.
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