Formation of Spindle-Like Ag58 Cluster Induced by Isomerization of [Ag14]

doi:10.6023/A20070317

Abstract

The atomically precise silver(I)-thiolate clusters in nanoscale have attracted extensive attention for years due to their attractive aesthetic structures and potential applications. Herein, two novel core-shell structured silver(I)-thiolate clusters of [Ag₅₆S₁₂(^tBuS)₂₀(CF₃CO₂)₁₂]·6CH₃CN·8H₂O (abbreviated as Ag₅₆) and [Ag₅₈S₁₂(^tBuS)₂₀(CF₃CO₂)₁₄(CH₃CN)₆]·6CH₃CN (Ag₅₈) are prepared by employing the self-assembly method in solution. Especially, with the introduction of dimethylformamide (DMF) and bis(diphenylphosphino)methane (DPPM), the ^tBuSAg precursor reacted with CF₃CO₂Ag to produce a novel cluster Ag₅₈ instead of Ag₅₆ that has a similar structure with previous reports. X-ray structural analysis indicates that both clusters have Ag₁₄ core units. But different from the common dodecahedron structure in Ag₅₆, the spindle-shaped Ag₁₄ structure in Ag₅₈ is discovered for the first time and then induces the shell structure of Ag₅₈ to form a rare spindle shape, in which silver atoms are layered in a form of “Ag₄-Ag₈-Ag₁₀-Ag₁₀-Ag₈-Ag₄”. Notably, the spindle-shaped Ag₁₄ is formed by rhombic dodecahedron being symmetrically pulled outward. Thus, there are obvious similarities and differences between the two Ag₁₄ core structures. Compared with the previously reported the face-centered cubic Ag₁₄ prepared by solvothermal methods, the rhombic dodecahedron and the rhombic dodecahedron-like (spindle) Ag₁₄ were obtained at room temperature, which indicates that the formation of the clusters is a thermodynamic control. However, the change of solvent and auxiliary ligands also caused the Ag₁₄ rhombohedral dodecahedron to deform and transform into a spindle-shaped structure, proving that the formation of the clusters is also a process controlled by kinetics. These prove that the synthesis of clusters is a process dominated by both of kinetics and thermodynamics. The UV-Vis absorption and fluorescence spectra show that the structure discrepancies of the two clusters deriving from the isomerization of Ag₁₄ units significantly affect the energy levels and fluorescence properties of the clusters. This study enriches the thiolate-silver cluster family and provides new samples and insights for understanding the formation mechanism and properties of such core-shell architectures.

Key words: silver(I)-thiolate clusters, Ag₁₄, isomerization, self-assembly

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Shen Yanglin, Jin Junling, Duan Guangxiong, Xie Yunpeng, Lu Xing. Formation of Spindle-Like Ag₅₈ Cluster Induced by Isomerization of [Ag₁₄][J]. Acta Chimica Sinica, 2020, 78(11): 1255-1259.

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[Ag₁₄]异构引发的纺锤形Ag₅₈团簇的形成

Formation of Spindle-Like Ag₅₈ Cluster Induced by Isomerization of [Ag₁₄]

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[Ag14]异构引发的纺锤形Ag58团簇的形成