Abstract
The use of liquid gallium as a solvent for catalytic reactions has enabled access to well-dispersed metal atoms configurations, leading to unique catalytic phenomena, including activation of neighbouring liquid atoms and mobility-induced activity enhancement. To gain mechanistic insights into liquid metal catalysts, here we introduce a GaSn0.029Ni0.023 liquid alloy for selective propylene synthesis from decane. Owing to their mobility, dispersed atoms in a Ga matrix generate configurations where interfacial Sn and Ni atoms allow for critical alignments of reactants and intermediates. Computational modelling, corroborated by experimental analyses, suggests a particular reaction mechanism by which Sn protrudes from the interface and an adjacent Ni, below the interfacial layer, aligns precisely with a decane molecule, facilitating propylene production. We then apply this reaction pathway to canola oil, attaining a propylene selectivity of ~94.5%. Our results offer a mechanistic interpretation of liquid metal catalysts with an eye to potential practical applications of this technology.
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Data availability
The datasets generated during the current study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.
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Acknowledgements
We thank D. Thomas of the Spectroscopy Laboratory and the Nuclear Magnetic Resonance Facility at the University of New South Wales, Sydney for his technical assistance. We also thank M. B. Ghasemian at the University of New South Wales, Sydney for his technical assistance. This work was supported by the Australian Research Council (ARC) Laureate Fellowship grant (FL180100053).
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Junma Tang initiated the concept and designed the experiments along with K.K.-Z. Junma Tang also conducted the experiments and carried out the characterizations, with the help of M.A.R. and K.K.-Z. The molecular dynamics simulations were performed by A.J.C., N.M. and S.P.R.; M.T. helped with the mass spectrometry experiments and analysis. P.V.K. and J.A.Y. performed the Bader charge analyses. The following individuals contributed to the data analyses, scientific discussions and authorship of the paper: A.J.C., J.S., M.T., N.M., Q.Z., Jianbo Tang, L.D., G.M., S.P.R., R.B.K., M.A.R. and K.K.-Z. All authors revised the manuscript and provided helpful comments.
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Nature Nanotechnology thanks Shinya Furukawa, Yian Zhu and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Supplementary Discussions 1–10, Figs. 1–22 and Tables 1–6.
Supplementary Video 1
The video shows the gaseous bubbles produced from the scaled-up experiment, using GaSn0.029Ni0.023 as the catalyst and canola oil as the feedstock.
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Tang, J., Christofferson, A.J., Sun, J. et al. Dynamic configurations of metallic atoms in the liquid state for selective propylene synthesis. Nat. Nanotechnol. 19, 306–310 (2024). https://doi.org/10.1038/s41565-023-01540-x
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DOI: https://doi.org/10.1038/s41565-023-01540-x
