Non-planar Nest-like [Fe2 S2 ] Cluster Sites for Efficient Oxygen Reduction Catalysis.
Angew Chem Int Ed Engl
; 62(22): e202300826, 2023 May 22.
Article
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| MEDLINE
| ID: mdl-36988088
ABSTRACT
Metal-nitrogen-carbon catalysts, as promising alternative to platinum-based catalysts for oxygen reduction reaction (ORR), are still highly expected to achieve better performance by modulating the composition and spatial structure of active site. Herein, we constructed the non-planar nest-like [Fe2 S2 ] cluster sites in N-doped carbon plane. Adjacent double Fe atoms effectively weaken the O-O bond by forming a peroxide bridge-like adsorption configuration, and the introduction of S atoms breaks the planar coordination of Fe resulting in greater structural deformation tension, lower spin state, and downward shifted Fe d-band center, which together facilitate the release of OH* intermediate. Hence, the non-planar [Fe2 S2 ] cluster catalyst, with a half-wave potential of 0.92â
V, displays superior ORR activity than that of planar [FeN4 ] or [Fe2 N6 ]. This work provides insights into the co-regulation of atomic composition and spatial configuration for efficient oxygen reduction catalysis.
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MEDLINE
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En
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Angew Chem Int Ed Engl
Año:
2023
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Article