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A single-Pt-atom-on-Ru-nanoparticle electrocatalyst for CO-resilient methanol oxidation

Nature Catalysis volume 5, pages 231–237 (2022)Cite this article

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Abstract

Single Pt atom catalysts are key targets because a high exposure of Pt substantially enhances electrocatalytic activity. In addition, PtRu alloy nanoparticles are the most active catalysts for the methanol oxidation reaction. To combine the exceptional activity of single Pt atom catalysts with an active Ru support we must overcome the synthetic challenge of forming single Pt atoms on noble metal nanoparticles. Here we demonstrate a process that grows and spreads Pt islands on Ru branched nanoparticles to create single-Pt-atom-on-Ru catalysts. By following the spreading process by in situ TEM, we found that the formation of a stable single atom structure is thermodynamically driven by the formation of strong Pt–Ru bonds and the lowering of the surface energy of the Pt islands. The stability of the single-Pt-atom-on-Ru structure and its resilience to CO poisoning result in a high current density and mass activity for the methanol oxidation reaction over time.

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Fig. 1: In situ TEM of the spreading process.
Fig. 2: Characterization of the single Pt atoms on a Ru nanoparticle.
Fig. 3: Electrochemical performance of catalysts in the MOR.
Fig. 4: DFT modelling of the MOR pathways for three PtRu nanoparticle catalysts.

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All data are available from the corresponding authors upon reasonable request.

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Acknowledgements

We acknowledge funding under an Australian Research Council Linkage grant (LP150101014, to L.G., J.J.G. and R.D.T.), the Discovery Project (DP190102659 and DP200100143, to R.D.T., and DP210102698, to J.J.G.) and a LIEF grant (LE200100033). A.R.P. thanks the UNSW Scientia PhD Scholarship Scheme. We also acknowledge support from Microscopy Australia and the Mark Wainwright Analytical Centre and Electron Microscope Unit at the University of New South Wales. W.S. acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany´s Excellence Strategy – EXC 2033 – 390677874 – RESOLV. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science. Los Alamos National Laboratory, an affirmative action equal opportunity employer, is managed by Triad National Security for the US DOE’s NNSA under contract 89233218CNA000001. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, a wholly owned subsidiary of Honeywell International, for the US DOE’s National Nuclear Security Administration under contract DE-NA-0003525. The views expressed in this article do not necessarily represent the views of the US DOE or the United States Government. The use of the K3 IS camera was provided courtesy of Gatan. DFT calculations were performed using the National Computational Infrastructure (NCI Australia) at the Australian National University, allocated through both the National Computational Merit Allocation Scheme (NCMAS) and the ANU Merit Allocation Scheme (ANUMAS), and supported by the Australian Research Council (LE190100021). A.H. was supported by award OISE-1357113 from the US National Science Foundation. XAS measurements were performed at the 10-ID-B beamline of the Advanced Photon Source, a US DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract DE-AC02-06CH11357. The 10-ID-B beamline is further supported by the Materials Research Collaborative Access Team and its member institutions. We thank H. Hashiguchi from JEOL for his assistance with TEM imaging presented in Fig. 2b. We thank J. Wright for his assistance with XAS experiments. This work was supported by the National Key Research and Development Program (grant no. 2018YFA0208600). W.Z. is supported by a USTC Tang Scholarship. The calculations were partially performed on the supercomputing system at USTC-SCC.

Author information

Author notes

  1. These authors contributed equally: Agus R. Poerwoprajitno, Lucy Gloag.

Authors and Affiliations

  1. School of Chemistry, The University of New South Wales, Sydney, New South Wales, Australia

    Agus R. Poerwoprajitno, Lucy Gloag, Aaron Henson, Peter B. O’Mara, Tania M. Benedetti, J. Justin Gooding & Richard D. Tilley

  2. Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, NM, USA

    John Watt

  3. Mark Wainwright Analytical Centre, The University of New South Wales, Sydney, New South Wales, Australia

    Soshan Cheong & Richard D. Tilley

  4. Integrated Materials Design Laboratory, Department of Applied Mathematics, Research School of Physics, The Australian National University, Canberra, Australian Capital Territory, Australia

    Xin Tan, Hassan A. Tahini & Sean C. Smith

  5. Department of Chemical Physics, University of Science and Technology of China, Hefei, China

    Han Lei

  6. Department of Materials Science and Engineering, North Carolina State University, Raleigh, NC, USA

    Aaron Henson

  7. School of Chemical Engineering, University of New South Wales, Sydney, New South Wales, Australia

    Bijil Subhash & Nicholas M. Bedford

  8. Gatan, Pleasanton, CA, USA

    Benjamin K. Miller

  9. Center for Integrated Nanotechnologies, Sandia National Laboratories, Albuquerque, NM, USA

    Dale L. Huber

  10. Hefei National Laboratory for Physical Sciences at the Microscale, Synergetic Innovation Centre of Quantum Information and Quantum Physics, Department of Material Science and Technology, University of Science and Technology of China, Hefei, China

    Wenhua Zhang

  11. Australian Research Council Centre of Excellence in Convergent Bio-Nano Science and Technology, University of New South Wales, Sydney, New South Wales, Australia

    J. Justin Gooding

  12. Analytical Chemistry – Center for Electrochemical Sciences, Faculty of Chemistry and Biochemistry, Ruhr-Universität Bochum, Bochum, Germany

    Wolfgang Schuhmann

Authors
  1. Agus R. Poerwoprajitno
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Contributions

R.D.T., W.S. and J.J.G. conceived and supervised the project. A.R.P and L.G. designed the experiments and prepared the manuscript. S.C. carried out EDX analysis and atomic-resolution HAADF-STEM imaging. X.T., H.A.T., W.Z., H.L. and S.C.S. performed DFT modelling and analysis. A.H. synthesized the nanoparticles. B.S. and N.M.B. carried out EXAFS and XANES analysis. J.W. performed ETEM experiments. B.K.M. helped with the in situ ETEM analysis. P.B.O’M. and T.M.B. were involved in the electrochemistry experiments. D.L.H. advised on the synthesis of the nanoparticles. All authors contributed to and commented on this paper.

Corresponding authors

Correspondence to Sean C. Smith, J. Justin Gooding, Wolfgang Schuhmann or Richard D. Tilley.

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Nature Catalysis thanks Ovidiu Ersen, Jiye Fang, Wenyue Guo, Ulrike Krewer and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–19, Notes 1 and 2, and Tables 1–7.

Supplementary Video 1

In situ TEM recording of a Pt island spreading into single Pt atoms on Ru.

Supplementary Data 1

Atomic coordinates for single Pt atom on Ru and adsorbed intermediates.

Supplementary Data 2

Atomic coordinates for Pt island on Ru and adsorbed intermediates.

Supplementary Data 3

Atomic coordinates for PtRu and adsorbed intermediates.

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Poerwoprajitno, A.R., Gloag, L., Watt, J. et al. A single-Pt-atom-on-Ru-nanoparticle electrocatalyst for CO-resilient methanol oxidation. Nat Catal 5, 231–237 (2022). https://doi.org/10.1038/s41929-022-00756-9

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