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Single-atom tailoring of platinum nanocatalysts for high-performance multifunctional electrocatalysis

Nature Catalysis volume 2, pages 495–503 (2019)Cite this article

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Abstract

Platinum-based nanocatalysts play a crucial role in various electrocatalytic systems that are important for renewable, clean energy conversion, storage and utilization. However, the scarcity and high cost of Pt seriously limit the practical application of these catalysts. Decorating Pt catalysts with other transition metals offers an effective pathway to tailor their catalytic properties, but often at the sacrifice of the electrochemical active surface area (ECSA). Here we report a single-atom tailoring strategy to boost the activity of Pt nanocatalysts with minimal loss in surface active sites. By starting with PtNi alloy nanowires and using a partial electrochemical dealloying approach, we create single-nickel-atom-modified Pt nanowires with an optimum combination of specific activity and ECSA for the hydrogen evolution, methanol oxidation and ethanol oxidation reactions. The single-atom tailoring approach offers an effective strategy to optimize the activity of surface Pt atoms and enhance the mass activity for diverse reactions, opening a general pathway to the design of highly efficient and durable precious metal-based catalysts.

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Fig. 1: Schematic diagram for SANi-PtNWs.
Fig. 2: Structural characterization of the SANi-PtNWs.
Fig. 3: Electrocatalytic performance of the SANi-PtNWs for HER compared against Pt/C and pure-PtNWs in 1 M KOH electrolyte.
Fig. 4: DFT calculations of the active sites.
Fig. 5: MOR and EOR electrocatalytic activities of the SANi-PtNWs, pure-PtNWs and Pt/C in 1 M KOH electrolyte.

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The data that support the findings of this study are available from the corresponding authors on reasonable request.

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Acknowledgements

Y.H. acknowledges support from the Office of Naval Research (grant no. N000141812155). X.D. acknowledges financial support from the National Science Foundation (grant no. 1800580). T.C. was supported by the Collaborative Innovation Center of Suzhou Nano Science & Technology, the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD) and the 111 Project. W.A.G. was supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under award no. DE‐SC0004993. This work used the Extreme Science and Engineering Discovery Environment (XSEDE) which is supported by National Science Foundation grant no. ACI‐1053575. J.L. acknowledges the National Key R&D Program of China (2017YFA0700104) and National Natural Science Foundation of China (51761165012). STEM experiments were conducted using the facilities in the Irvine Materials Research Institute (IMRI) at the University of California-Irvine. The authors thank S. Fakra for technical support for the EXAFS experiment. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DEAC02-05CH11231. R.Y. acknowledges the National Natural Science Foundation of China (51525102, 51390475). Use of resources of the National Center for Electron Microscopy in Beijing is acknowledged. The calculations were performed on the Hoffman2 cluster at UCLA Institute for Digital Research and Education (IDRE) and the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by the National Science Foundation (grant no. ACI‐1053575).

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Author notes

  1. These authors contributed equally: Mufan Li, Kaining Duanmu, Chengzhang Wan, Tao Cheng.

Authors and Affiliations

  1. Department of Chemistry and Biochemistry, University of California, Los Angeles, CA, USA

    Mufan Li, Chengzhang Wan, Peng Li, Huilong Fei, Zhaoyang Lin, Hongtao Sun, Philippe Sautet & Xiangfeng Duan

  2. Department of Materials Science and Engineering, University of California, Los Angeles, CA, USA

    Mufan Li, Zipeng Zhao, Mengning Ding, Jin Huang & Yu Huang

  3. Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, CA, USA

    Kaining Duanmu & Philippe Sautet

  4. Materials and Process Simulation Center, California Institute of Technology, Pasadena, CA, USA

    Tao Cheng & William A. Goddard III

  5. Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, Jiangsu, China

    Tao Cheng

  6. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Liang Zhang & Jinghua Guo

  7. Department of Materials Science and Engineering, University of California Irvine, Irvine, CA, USA

    Sheng Dai & Xiaoqing Pan

  8. Department of Chemistry, Tsinghua University, Beijing, China

    Wenxin Chen

  9. National Center for Electron Microscopy in Beijing, School of Materials Science and Engineering, Tsinghua University, Beijing, China

    Yuanming Zhu & Rong Yu

  10. Center for Electron Microscopy in Tianjin University of Technology, Tianjin, China

    Jun Luo & Ketao Zang

  11. Irvine Materials Research Institute (IMRI), University of California Irvine, Irvine, CA, USA

    Xiaoqing Pan

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Contributions

X.D., Y.H. and P.S. supervised the project and designed the research. X.D., Y.H. and M.L. conceived the idea. M.L. and C.W. performed the synthesis, electrochemical tests and characterizations. K.D. and P.S. conceived and performed the DFT calculations. T.C. and W.G. performed the model simulations. L.Z. and W.C. performed XAS measurements and analysis. J.G. and W.C. provided expertise for XAS analysis. S.D. and X.P. performed the EELS and HAADF-STEM measurements. Z.Z., Y.Z., R.Y., J.L., K.Z. and Z.L. assisted with material characterizations. Z.Z., P.L., H.F., M.D., J.H. and H.S. assisted with catalytic measurements. M.L., K.D., C.W., P.S., Y.H. and X.D. co-wrote the paper. All authors discussed the results and commented on the manuscript.

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Correspondence to Philippe Sautet, Yu Huang or Xiangfeng Duan.

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Supplementary information

Supplementary Figs. 1–11 and Supplementary Tables 1–4.

Supplementary Data

Atomic coordinates of the optimized computational models.

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Li, M., Duanmu, K., Wan, C. et al. Single-atom tailoring of platinum nanocatalysts for high-performance multifunctional electrocatalysis. Nat Catal 2, 495–503 (2019). https://doi.org/10.1038/s41929-019-0279-6

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