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

NATURE NANOTECHNOLOGY(2024)

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摘要
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 similar to 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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