Markedly enhanced oxygen reduction activity of single-atom fe catalysts via integration with fe nanoclusters

Xiang Ao, Wei Zhang, Zhishan Li, Jian Gang Li, Luke Soule, Xing Huang, Wei Hung Chiang, Hao Ming Chen, Chundong Wang, Meilin Liu, Xiao Cheng Zeng

Research output: Contribution to journalArticle

27 Scopus citations

Abstract

Single-atom catalysts (SACs) have emerged as one of the most promising alternatives to noble metalbased catalysts for highly efficient oxygen reduction reaction (ORR). While SACs can offer notable benefits in terms of lowering overall catalyst cost, there is still room for improvement regarding catalyst activity. To this end, we designed and successfully fabricated an ORR electrocatalyst in which atomic clusters are embedded in an atomically dispersed Fe-N-C matrix (FeAC@FeSA-N-C), as shown by comprehensive measurements using aberration- corrected scanning transmission electron microscopy (AC-STEM) and X-ray absorption spectroscopy (XAS). The half-wave potential of FeAC@FeSA-N-C is 0.912 V (versus reversible hydrogen 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-platinum-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 measurements and theoretical calculations.

Original languageEnglish (US)
Pages (from-to)11853-11862
Number of pages10
JournalACS Nano
Volume13
Issue number10
DOIs
StatePublished - Oct 22 2019

Keywords

  • DFT computation
  • Electrocatalysts
  • Fe nanoclusters
  • Oxygen reduction
  • Single-atom catalyst

ASJC Scopus subject areas

  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)

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  • Cite this

    Ao, X., Zhang, W., Li, Z., Li, J. G., Soule, L., Huang, X., Chiang, W. H., Chen, H. M., Wang, C., Liu, M., & Zeng, X. C. (2019). Markedly enhanced oxygen reduction activity of single-atom fe catalysts via integration with fe nanoclusters. ACS Nano, 13(10), 11853-11862. https://doi.org/10.1021/acsnano.9b05913