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A universal principle for a rational design of single-atom electrocatalysts

Nature Catalysisvolume 1pages339348 (2018) | Download Citation

  • A Correction to this article was published on 20 July 2018


Developing highly active single-atom catalysts for electrochemical reactions is a key to future renewable energy technology. Here we present a universal design principle to evaluate the activity of graphene-based single-atom catalysts towards the oxygen reduction, oxygen evolution and hydrogen evolution reactions. Our results indicate that the catalytic activity of single-atom catalysts is highly correlated with the local environment of the metal centre, namely its coordination number and electronegativity and the electronegativity of the nearest neighbour atoms, validated by available experimental data. More importantly, we reveal that this design principle can be extended to metal–macrocycle complexes. The principle not only offers a strategy to design highly active nonprecious metal single-atom catalysts with specific active centres, for example, Fe-pyridine/pyrrole-N4 for the oxygen reduction reaction; Co-pyrrole-N4 for the oxygen evolution reaction; and Mn-pyrrole-N4 for the hydrogen evolution reaction to replace precious Pt/Ir/Ru-based catalysts, but also suggests that macrocyclic metal complexes could be used as an alternative to graphene-based single-atom catalysts.

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  • 20 July 2018

    The original Supplementary Information file published with this Article was an older version; it was missing several Tables, and the Methods section was a duplicate of that from the main article. A new Supplementary Information file has been uploaded with these issues corrected.


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This work is supported by the National Natural Science Foundation of China (91634116, 21576008, 21625601).

Author information


  1. Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China

    • Haoxiang Xu
    • , Daojian Cheng
    • , Dapeng Cao
    •  & Xiao Cheng Zeng
  2. State Key Laboratory of Organic-Inorganic Composites, Beijing Key Laboratory of Energy Environmental Catalysis, Beijing University of Chemical Technology, Beijing, China

    • Daojian Cheng
    •  & Dapeng Cao
  3. Department of Chemistry, Department of Chemical & Biomolecular Engineering, and Department of Mechanical & Materials Engineering, University of Nebraska, Lincoln, NE, USA

    • Xiao Cheng Zeng


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D.J.C. and X.C.Z. conceived the original idea and designed the DFT calculations. D.J.C. and H.X. contributed to the density functional theory calculations. D.P.C. analysed the results. All authors wrote the manuscript and have reviewed, discussed and approved the results and conclusions of this article.

Competing interests

The authors declare no competing interests.

Corresponding authors

Correspondence to Daojian Cheng or Dapeng Cao or Xiao Cheng Zeng.

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  1. Supplementary Information

    Supplementary Figures 1–28, Supplementary Tables 1–54, Supplementary References

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