4.6 Article

One-step preparation of Pt/Ag nanoclusters for CO2 transformation

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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 25, 期 44, 页码 30373-30380

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ROYAL SOC CHEMISTRY
DOI: 10.1039/d3cp02736h

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This study reports the one-step synthesis of Pt/Ag alloy nanoclusters that exhibit high catalytic activity in the cycloaddition reactions of CO2 and epoxides. The molecular structure of the nanoclusters is protected by the shell of phosphine ligands and halides. The research is important for studying structure-performance relationships and the reaction mechanism of heterogeneous metal catalysts.
Structurally precise metal nanoclusters with a facile synthetic process and high catalytic performance have been long pursued. These atomically precise nanocatalysts are regarded as model systems to study structure-performance relationships, surface coordination chemistry, and the reaction mechanism of heterogeneous metal catalysts. Nevertheless, the research on silver-based nanoclusters for driving chemical transformations is sluggish in comparison to gold counterparts. Herein, we report the one-step synthesis of Pt/Ag alloy nanoclusters of [PtAg9(C18H12Br3P)(7)Cl-3](C18H12Br3P), which are highly active in catalysing cycloaddition reactions of CO2 and epoxides. The cluster was obtained in a rather simple way with the reduction of silver and platinum salts in the presence of ligands in one pot. The molecular structure of the titled cluster describes the protection of the Pt-centred Ag-9 crown by the shell of phosphine ligands and halides. Its electronic structure, as revealed by density function theoretical calculations, adopts a superatomic geometry with 1S(2)1P(6) configuration. Interestingly, the cluster displays high activity in the formation of cyclic carbonates from CO2 under mind conditions.

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