Kinetic Control and Thermodynamic Selection in the Synthesis of Atomically Precise Gold Nanoclusters

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• 作者：Zhikun Wu ; Mark A. MacDonald ; Jenny Chen ; Peng Zhang ; Rongchao Jin
• 刊名：Journal of the American Chemical Society
• 出版年：2011
• 出版时间：June 29, 2011
• 年：2011
• 卷：133
• 期：25
• 页码：9670-9673
• 全文大小：778K
• 年卷期：v.133,no.25(June 29, 2011)
• ISSN：1520-5126

文摘

This work presents a combined approach of kinetic control and thermodynamic selection for the synthesis of monodisperse 19 gold atom nanoclusters protected by thiolate groups. The step of kinetic control allows the formation of a proper size distribution of initial size-mixed Au_n(SR)_m nanoclusters following the reduction of a gold precursor. Unlike the synthesis of Au₂₅(SR)₁₈ nanoclusters, which involves rapid reduction of the gold precursor by NaBH₄ followed by size focusing, the synthesis of 19-atom nanoclusters requires slow reduction effected by a weaker reducing agent, borane鈥?i>tert-butylamine complex. The initially formed mixture of nanoclusters then undergoes size convergence into a monodisperse product by means of a prolonged aging process. The nanocluster formula was determined to be Au₁₉(SC₂H₄Ph)₁₃. This work demonstrates the importance of both kinetic control of the initial size distribution of nanoclusters prior to size focusing and subsequent thermodynamic selection of stable nanoclusters as the final product.