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Non-planar Nest-like [Fe2S2] Cluster Sites for Efficient Oxygen Reduction Catalysis |
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| Authors: | Ming Wang Dr. Zhong Zhang Songlin Zhang Dr. Wei Liu Wenzhe Shang Dr. Xiaofang Su Yan Liang Furi Wang Dr. Xujiao Ma Yadong Li Prof. Dr. Yiwei Liu |
| Affiliation: | 1. Zhang Dayu School of Chemistry, Dalian University of Technology, Dalian, 116024 China These authors contributed equally to this work.;2. School of Chemical Engineering, Dalian University of Technology Dalian, 116024 (China) These authors contributed equally to this work.;3. School of Chemical Engineering, Dalian University of Technology Dalian, 116024 (China);4. School of Chemistry and Chemical Engineering, Henan Normal University, Henan, 453007 China;5. Zhang Dayu School of Chemistry, Dalian University of Technology, Dalian, 116024 China;6. Department of Chemistry, Tsinghua University, Beijing, 100084 China |
| 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 [Fe2S2] 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 [Fe2S2] cluster catalyst, with a half-wave potential of 0.92 V, displays superior ORR activity than that of planar [FeN4] or [Fe2N6]. This work provides insights into the co-regulation of atomic composition and spatial configuration for efficient oxygen reduction catalysis. |
| Keywords: | Cluster Nonplanar Oxygen Reduction Reaction Structural Tension Sub-Nanometer |