Citation: 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. doi: 10.6023/A20070317 shu

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

a.
State Key Laboratory of Materials Processing and Die&Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology(HUST), Wuhan 430074, China
b.
Henan Key Laboratory of Functional Salt Materials, Center for Advanced Materials Research, Zhongyuan University of Technology, Zhengzhou 450007, China

Corresponding author: Xie Yunpeng, xieyp@hust.edu.cn Lu Xing, lux@hust.edu.cn
Received Date: 16 July 2020
Available Online: 3 August 2020
Fund Project: the National Natural Science Foundation of China 21771071the National Natural Science Foundation of China 21925104the National Natural Science Foundation of China 51672093Project supported by the National Natural Science Foundation of China (Nos. 21771071, 51672093, 21925104)

Figures(4)

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.
- silver(I)-thiolate clusters,
- Ag₁₄,
- isomerization,
- self-assembly
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沈阳化工大学材料科学与工程学院沈阳 110142

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

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