Markedly Enhanced Oxygen Reduction Activity of Single-Atom Fe Catalysts via Integration with Fe Nanoclusters

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Abstract
Single-atom catalysts (SACs) have emerged as one of the most promising alternatives to noble metal-based catalysts for highly efficient oxygen reduction reaction (ORR). While SACs can offer notable benefits in terms of lowering overall cata-lyst cost, there is still room for improvement regarding catalyst activity. To this end, we designed and successfully fabricated a ORR electrocatalyst in which atomic clusters are embedded in atomically dispersed Fe-N-C matrix ([email protected]), as shown by comprehensive measurements using aberration-corrected scanning transmission electron microscope (AC-STEM) and X-ray absorption spectroscopy (XAS). The half-wave potential of [email protected] is 0.912 V (versus reversible hydro-gen electrode (RHE)), exceeding that of commercial Pt/C (0.897 V), FeSA-N-C (0.844 V), as well as the half-wave potentials of most reported non-precious-group metal catalysts. The ORR activity of the designed catalyst stems from single-atom active centers but is markedly enhanced by the presence of Fe nanoclusters, as confirmed by both experimental measure-ments and theoretical calculations.
Funding Information
  • Ministry of Education of the People's Republic of China (2019KFYXMBZ076, 2018KFYYXJJ051)
  • Ministry of Science and Technology of the People's Republic of China (2017YFE0120500)
  • China Scholarship Council
  • National Natural Science Foundation of China (51502099)
  • Hubei ?Chu-Tian Young Scholar? program

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