Abstract

Electrochemical reduction of CO2 to chemical fuel offers a promising strategy for managing the global carbon balance, but presents challenges for chemistry due to the lack of effective electrocatalyst. Here we report atomically dispersed nickel on nitrogenated graphene as an efficient and durable electrocatalyst for CO2 reduction. Based on operando X-ray absorption and photoelectron spectroscopy measurements, the monovalent Ni(i) atomic center with a d9 electronic configuration was identified as the catalytically active site. The single-Ni-atom catalyst exhibits high intrinsic CO2 reduction activity, reaching a specific current of 350 A gcatalyst−1 and turnover frequency of 14,800 h−1 at a mild overpotential of 0.61 V for CO conversion with 97% Faradaic efficiency. The catalyst maintained 98% of its initial activity after 100 h of continuous reaction at CO formation current densities as high as 22 mA cm−2.

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Acknowledgements

We would like to acknowledge funding support from the National Key Projects for Fundamental Research and Development of China (2016YFA0202804), the Strategic Priority Research Programme of the Chinese Academy of Sciences (XDB17020400), Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1: RG10/16 and RG111/15, Singapore A*Star Science and Engineering Research Council—Public Sector Funding (PSF): 1421200075, the National Research Foundation (NRF), Prime Minister’s Office, Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) programme.

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Affiliations

  1. School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore, Singapore

    • Hong Bin Yang
    • , Song Liu
    • , Liping Zhang
    • , Xiang Huang
    • , Hsin-Yi Wang
    • , Weizheng Cai
    • , Rong Chen
    • , Jiajian Gao
    •  & Bin Liu
  2. Institute for Materials Science and Devices, Suzhou University of Science and Technology, Suzhou, China

    • Hong Bin Yang
    •  & Chang Ming Li
  3. Department of Chemistry, National Taiwan University, Taipei, Taiwan

    • Sung-Fu Hung
    •  & Hao Ming Chen
  4. State Key Laboratory of Catalysis, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China

    • Song Liu
    • , Shu Miao
    • , Xiaofeng Yang
    • , Yanqiang Huang
    •  & Tao Zhang
  5. Department of Physics, National University of Singapore, Singapore, Singapore

    • Kaidi Yuan
    •  & Wei Chen

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Contributions

H.B.Y., Y.H., T.Z. and B.L. conceived and designed the project. S.H., H.W. and H.M.C performed the X-ray absorption experiments. H.B.Y., S.L., J.G. and C.L. performed the electrochemical experiments and analyzed the electrochemical data. K.Y. and W.C. conducted the photoelectron spectroscopy measurements. S.M., L.Z. and R.C contributed to the structure characterizations. X.H., W.C. and X.Y. carried out the theoretical calculations. H.B.Y., Y.H., T.Z. and B.L. analyzed the experimental data and prepared the manuscript. All authors reviewed and contributed to the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to Yanqiang Huang or Tao Zhang or Bin Liu.

Supplementary information

  1. Supplementary Information

    Supplementary Figs. 1–9, Supplementary Tables 1–5 and Supplementary References

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DOI

https://doi.org/10.1038/s41560-017-0078-8

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