Dynamic configurations of metallic atoms in the liquid state for selective propylene synthesis

Junma Tang; Andrew J Christofferson; Jing Sun; Qingfeng Zhai; Priyank V Kumar; Jodie A Yuwono; Mohammad Tajik; Nastaran Meftahi; Jianbo Tang; Liming Dai; Guangzhao Mao; Salvy P Russo; Richard B Kaner; Md Arifur Rahim; Kourosh Kalantar-Zadeh

doi:10.1038/s41565-023-01540-x

Dynamic configurations of metallic atoms in the liquid state for selective propylene synthesis

Nat Nanotechnol. 2024 Mar;19(3):306-310. doi: 10.1038/s41565-023-01540-x. Epub 2023 Nov 9.

Authors

Junma Tang^{1

2}, Andrew J Christofferson^{3

4}, Jing Sun⁵, Qingfeng Zhai⁵, Priyank V Kumar⁵, Jodie A Yuwono^{5

6}, Mohammad Tajik⁷, Nastaran Meftahi^{3

4}, Jianbo Tang⁵, Liming Dai⁵, Guangzhao Mao⁵, Salvy P Russo^{3

4}, Richard B Kaner^{8

9}, Md Arifur Rahim^{10

11}, Kourosh Kalantar-Zadeh¹²

Affiliations

¹ School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, New South Wales, Australia. junma.tang@unsw.edu.au.
² School of Chemical Engineering, University of New South Wales (UNSW), Sydney, New South Wales, Australia. junma.tang@unsw.edu.au.
³ School of Science, STEM College, RMIT University, Melbourne, Victoria, Australia.
⁴ ARC Centre of Excellence in Exciton Science, School of Science, RMIT University, Melbourne, Victoria, Australia.
⁵ School of Chemical Engineering, University of New South Wales (UNSW), Sydney, New South Wales, Australia.
⁶ School of Chemical Engineering, The University of Adelaide, Adelaide, South Australia, Australia.
⁷ School of Chemistry, University of New South Wales (UNSW), Sydney, New South Wales, Australia.
⁸ Department of Chemistry and Biochemistry and California NanoSystems Institute, University of California, Los Angeles, CA, USA.
⁹ Department of Materials Science and Engineering, University of California, Los Angeles, CA, USA.
¹⁰ School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, New South Wales, Australia. md.rahim@sydney.edu.au.
¹¹ School of Chemical Engineering, University of New South Wales (UNSW), Sydney, New South Wales, Australia. md.rahim@sydney.edu.au.
¹² School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, New South Wales, Australia. kourosh.kalantarzadeh@sydney.edu.au.

PMID: 37945988
DOI: 10.1038/s41565-023-01540-x

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 GaSn_0.029Ni_0.023 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.

Grants and funding

FL180100053/Centre of Excellence for Electromaterials Science, Australian Research Council (ARC Centre of Excellence for Electromaterials Science)