4.8 Article

Understanding of Neighboring Fe-N4-C and Co-N4-C Dual Active Centers for Oxygen Reduction Reaction

Journal

ADVANCED FUNCTIONAL MATERIALS
Volume 31, Issue 22, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202011289

Keywords

catalytic mechanism; dual active centers; neighboring M‐ N‐ C centers; oxygen reduction reaction

Funding

  1. National Natural Science Foundation of China [51974114, 51672075, 21908049]
  2. China Postdoctoral Science Foundation [2020M682560]
  3. science and technology innovation Program of Hunan Province [2020RC2024]
  4. Hunan Provincial Natural Science Foundation of China [2020JJ4175]
  5. Fundamental Research Funds for the Central Universities

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The study reports FeCo-N-doped hollow carbon nanocages as efficient catalysts with neighboring Fe-N-4-C and Co-N-4-C dual active centers, showing better catalytic activity than Fe single-metal catalyst for oxygen reduction reaction. This highlights the important role of synergy between dual active centers in reducing the reaction energy barriers for ORR.
Single atomic dispersed M-N-C (M = Fe, Co, Ni, Cu, etc.) composites display excellent performance for catalytic reactions. However, the analysis and understanding of neighboring M-N-C centers at the atomic level are still insufficient. Here, FeCo-N-doped hollow carbon nanocages (FeCo-N-HCN) with neighboring Fe-N-4-C and Co-N-4-C dual active centers as efficient catalysts are reported. Spherical aberration-corrected high angle annular dark-field scanning transmission electron microscopy, small area (1 nm(2)) electron energy loss spectroscopy, and X-ray absorption spectroscopy data analysis and fitting prove the neighboring Fe-N-4-C and Co-N-4-C dual active structure in FeCo-N-HCN. Experimental tests and density functional theory calculation results reveal that the FeCo-N-HCN catalyst displays better catalytic activity than Fe single-metal catalyst for oxygen reduction reaction (ORR), which is attributed to the synergistic effect of Fe-N-4-C and Co-N-4-C dual active centers reducing the reaction energy barriers for ORR. Although the catalytic performance of the FeCo-N-HCN catalyst is not comparable to the-state-of-art catalysts reported due to the low metal contents (Fe: 1.96 wt% and Co: 1.31 wt%), these results can refresh the understanding of neighboring M-N-C centers at the atomic level and provide guidance for the design of catalysts in the future.

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