Non‐planar Nest‐like [Fe <sub>2</sub> S <sub>2</sub> ] Cluster Sites for Efficient Oxygen Reduction Catalysis
Ming Wang, Zhong Zhang, Songlin Zhang, Wei Liu, Wenzhe Shang, Xiaofang Su, Liang Yan, Furi Wang, Xujiao Ma, Yadong Li, Yiwei Liu
Abstract
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 [Fe 2 S 2 ] 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 [Fe 2 S 2 ] cluster catalyst, with a half‐wave potential of 0.92 V, displays superior ORR activity than that of planar [FeN 4 ] or [Fe 2 N 6 ]. This work provides insights into the co‐regulation of atomic composition and spatial configuration for efficient oxygen reduction catalysis.