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Low-temperature liquid platinum catalyst

Nature Chemistry volume 14, pages 935–941 (2022)Cite this article

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Abstract

Insights into metal–matrix interactions in atomically dispersed catalytic systems are necessary to exploit the true catalytic activity of isolated metal atoms. Distinct from catalytic atoms spatially separated but immobile in a solid matrix, here we demonstrate that a trace amount of platinum naturally dissolved in liquid gallium can drive a range of catalytic reactions with enhanced kinetics at low temperature (318 to 343 K). Molecular simulations provide evidence that the platinum atoms remain in a liquid state in the gallium matrix without atomic segregation and activate the surrounding gallium atoms for catalysis. When used for electrochemical methanol oxidation, the surface platinum atoms in the gallium–platinum system exhibit an activity of \({\sim {2.8} \times {10^7}\,{{{\mathrm{mA}}}}\,{{{{\mathrm{mg}}}}_{{{{\mathrm{Pt}}}}}^{ - 1}}},\) three orders of magnitude higher than existing solid platinum catalysts. Such a liquid catalyst system, with a dynamic interface, sets a foundation for future exploration of high-throughput catalysis.

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Fig. 1: Experimental and computational description of the Ga–Pt catalysts.
Fig. 2: Oxidation of PG over Ga–Pt catalysts.
Fig. 3: Electrochemical oxidation of CH3OH over a Ga–Pt anode.
Fig. 4: Electronic structure analysis and possible pathway for the high catalytic activity of the liquid Ga–Pt system.

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Acknowledgements

We thank the Australian Research Council (ARC) for a Laureate Fellowship grant (FL180100053) and Discovery Early Career Researcher Award (DE210101162) for the financial support of this study. We acknowledge the assistance of supercomputing resources from the National Computational Infrastructure (NCI), supported by the Australian Government, and assistance from Pawsey Supercomputer Centre. We also acknowledge the technical assistance from the Solid State & Elemental Analysis Unit (Mark Wainwright Analytical Centre, UNSW Sydney).

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Authors and Affiliations

  1. School of Chemical Engineering, University of New South Wales (UNSW), Sydney, New South Wales, Australia

    Md. Arifur Rahim, Jianbo Tang, Priyank V. Kumar, Franco Centurion, Zhenbang Cao, Junma Tang, Mahroo Baharfar, Mohannad Mayyas, Francois-Marie Allioux & Kourosh Kalantar-Zadeh

  2. School of Science, STEM College, RMIT University, Melbourne, Victoria, Australia

    Andrew J. Christofferson, Nastaran Meftahi, Christopher F. McConville & Salvy P. Russo

  3. ARC Centre of Excellence in Exciton Science, School of Science, RMIT University, Melbourne, Victoria, Australia

    Andrew J. Christofferson, Nastaran Meftahi & Salvy P. Russo

  4. School of Materials Science and Engineering, University of New South Wales (UNSW), Sydney, New South Wales, Australia

    Pramod Koshy

  5. School of Engineering, RMIT University, Melbourne, Victoria, Australia

    Torben Daeneke

  6. Institute for Frontier Materials, Deakin University (Warren Ponds Campus), Geelong, Victoria, Australia

    Christopher F. McConville

  7. Department of Chemistry and Biochemistry, University of California, Los Angeles (UCLA), Los Angeles, CA, USA

    Richard B. Kaner

  8. Department of Materials Science and Engineering, University of California, Los Angeles (UCLA), Los Angeles, CA, USA

    Richard B. Kaner

Authors
  1. Md. Arifur Rahim
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Contributions

M.A.R. and K.K.-Z. conceived the idea. M.A.R. and Jianbo Tang synthesized the catalysts. M.A.R. designed and performed the experiments with the help of Jianbo Tang, Junma Tang, F.C., Z.C., M.B., M.M., F.-M.A. and T.D. The molecular dynamic simulations were performed by A.J.C., N.M., C.F.M. and S.P.R. The DFT calculations were performed by P.V.K. The phase diagram was prepared by P.K. The draft manuscript was prepared with the help of R.B.K. and K.K.-Z. All the authors discussed the results and contributed to preparing the final draft of the Paper.

Corresponding authors

Correspondence to Md. Arifur Rahim or Kourosh Kalantar-Zadeh.

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Nature Chemistry thanks Wenyue Guo, Frédéric Jaouen and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Methods, Figs. 1–19, Tables 1 and 2, Notes 1 and 2 and references.

Source data

Source Data Fig. 1

Source data for Fig. 1 including solubility data of Pt in liquid Ga, initial and final configurations of the AIMD simulations, and pairwise probability distribution of Pt atoms in Ga matrix in the bulk and interface

Source Data Fig. 2

Source data for Fig. 2 including absorbance at 500 nm for different catalysts over time (PG oxidation), and initial and final configurations of the AIMD simulations

Source Data Fig. 3f

DFT configurations for the methanol oxidation

Source Data Fig. 4a

Density of states calculation

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Rahim, M.A., Tang, J., Christofferson, A.J. et al. Low-temperature liquid platinum catalyst. Nat. Chem. 14, 935–941 (2022). https://doi.org/10.1038/s41557-022-00965-6

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