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[Ag21{S2P(OiPr)2}12]+: an eight-electron superatom
Rajendra S Dhayal1, Jian-Hong Liao, Yu-Chiao Liu
1Department of Chemistry, National Dong Hwa University, No. 1, Sec. 2, Da Hsueh Rd. Shoufeng, Hualien 97401 (Taiwan R.O.C.) http://faculty.ndhu.edu.tw/∼cwl/index.htm.
Angewandte Chemie (International Ed. in English)
|January 30, 2015
Summary
Researchers synthesized a novel silver nanocluster, [Ag21{S2P(OiPr)2}12](PF6), featuring a unique icosahedral core. Its stability is explained by an 8-electron superatom configuration, aligning with the Jellium model.
Area of Science:
- Inorganic Chemistry
- Materials Science
- Nanotechnology
Background:
- Discrete metal nanoclusters offer tunable properties based on their size and composition.
- Understanding the structure-property relationships of silver nanoclusters is crucial for developing new materials.
- Dithiophosphate ligands are effective in stabilizing metal nanoclusters.
Purpose of the Study:
- To synthesize and characterize a novel silver nanocluster with a unique structural motif.
- To investigate the electronic structure and stability of the synthesized nanocluster.
- To explore the application of the Jellium model in describing the stability of silver nanoclusters.
Main Methods:
- Single-crystal X-ray diffraction for structural determination.
- Nuclear Magnetic Resonance (NMR) spectroscopy (1H, 31P) for structural and electronic analysis.
- Electrospray Ionization (ESI) mass spectrometry, X-ray Photoelectron Spectroscopy (XPS), Energy-Dispersive X-ray Spectroscopy (EDS), and UV/Vis spectroscopy for characterization.
- Density Functional Theory (DFT) calculations to confirm electronic configuration.
Main Results:
- A novel discrete nanocluster, [Ag21{S2P(OiPr)2}12](PF6), was successfully synthesized.
- The nanocluster exhibits an unprecedented silver-centered icosahedral core capped by eight additional silver atoms.
- The framework is stabilized by twelve dithiophosphate ligands.
- DFT calculations and the spherical Jellium model confirm an 8-electron superatom configuration (1S(2)1P(6)) contributing to the nanocluster's stability.
Conclusions:
- The successful synthesis and characterization of the [Ag21{S2P(OiPr)2}12](PF6) nanocluster represent a significant advancement in discrete metal nanocluster chemistry.
- The unprecedented Ag21 core structure provides new insights into cluster assembly and stability.
- The study validates the applicability of the spherical Jellium model and DFT calculations for predicting the electronic stability of complex silver nanoclusters.
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