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Single platinum atoms immobilized on an MXene as an efficient catalyst for the hydrogen evolution reaction

Nature Catalysisvolume 1pages985992 (2018) | Download Citation

Abstract

Single-atom catalysts offer a pathway to cost-efficient catalysis using the minimal amount of precious metals. However, preparing and keeping them stable during operation remains a challenge. Here we report the synthesis of double transition metal MXene nanosheets—Mo2TiC2Tx, with abundant exposed basal planes and Mo vacancies in the outer layers—by electrochemical exfoliation, enabled by the interaction between protons and the surface functional groups of Mo2TiC2Tx. The as-formed Mo vacancies are used to immobilize single Pt atoms, enhancing the MXene’s catalytic activity for the hydrogen evolution reaction. The developed catalyst exhibits a high catalytic ability with low overpotentials of 30 and 77 mV to achieve 10 and 100 mA cm−2 and a mass activity about 40 times greater than the commercial platinum-on-carbon catalyst. The strong covalent interactions between positively charged Pt single atoms and the MXene contribute to the exceptional catalytic performance and stability.

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Acknowledgements

The authors thank P. Li from Nanjing University of Aeronautics and Astronautics, Nanjing for performing DFT calculations. Y. Zheng from the University of Adelaide and Y.-C. Huang from the National Synchrotron Radiation Research Centre are acknowledged for their valuable discussions. The authors acknowledge use of the JEOL 2010 and JEOL JEM-ARM200F STEM within the University of Wollongong (UoW) Electron Microscopy Centre. This project was financially supported by the Australian Research Council (ARC) through ARC Discovery projects (DP160104340 and DP170100436) and a Rail Manufacturing CRC (RMCRC) project.

Author information

Author notes

  1. These authors contributed equally: Jinqiang Zhang and Yufei Zhao.

Affiliations

  1. Center for Clean Energy Technology, School of Mathematical and Physical Sciences, Faculty of Science, University of Technology Sydney, Sydney, New South Wales, Australia

    • Jinqiang Zhang
    • , Yufei Zhao
    • , Xin Guo
    •  & Guoxiu Wang
  2. Department of Chemistry, Tsinghua University, Beijing, China

    • Chen Chen
    •  & Yadong Li
  3. Department of Physics, Tamkang University, Tamsui, Taiwan

    • Chung-Li Dong
  4. Department of Chemistry, National Taiwan University, Taipei, Taiwan

    • Ru-Shi Liu
    •  & Chih-Pin Han
  5. A.J. Drexel Nanomaterials Institute and Department of Materials Science and Engineering, Drexel University, Philadelphia, PA, USA

    • Yury Gogotsi

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Contributions

G.W., J.Z. and Y.Z. conceived the idea. J.Z. and Y.Z. performed the electrochemical experiments. X.G. synthesized the Mo2TiC2Tx MXene. Y.G. provided the MAX materials for this work. J.Z., Y.Z. and X.G. carried out characterizations. C.-L.D., R.-S.L. and C.-P.H. performed and analysed EXAFS and XANES analysis. J.Z., Y.Z., C.C., Y.L., Y.G. and G.W. proposed the mechanism research and discussions. All authors contributed to writing of the manuscript.

Competing interests

The authors declare no competing interests.

Corresponding authors

Correspondence to Yadong Li or Yury Gogotsi or Guoxiu Wang.

Supplementary information

  1. Supplementary Information

    Supplementary Figs 1–31, Supplementary Tables 1–4, Supplementary Notes 1–5 and Supplementary References

  2. Supplementary Data 1

    Atomic coordinates of the optimized (3x3) Mo2TiC2O2–PtSA model

  3. Supplementary Data 2

    Atomic coordinates of the optimized (3x3) Mo2TiC2O2 model

  4. Supplementary Data 3

    Atomic coordinates of the optimized (4x4) Mo2TiC2O2–PtSA model

  5. Supplementary Data 4

    Atomic coordinates of the optimized (4x4) Mo2TiC2O2 model

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DOI

https://doi.org/10.1038/s41929-018-0195-1