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

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† Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh, Pennsylvania 15213, United States
‡ Key Laboratory of Materials Physics, Anhui Key Laboratory of Nanomaterials and Nanotechnology, Institute of Solid State Physics, Chinese Academy of Sciences (CAS), Hefei 230031, Anhui, China
§ Department of Chemistry and Institute for Research in Materials, Dalhousie University, Halifax, Nova Scotia, Canada B3H 4J3
[email protected]; [email protected]
Cite this: J. Am. Chem. Soc. 2011, 133, 25, 9670–9673
Publication Date (Web):June 2, 2011
https://doi.org/10.1021/ja2028102
Copyright © 2011 American Chemical Society
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Abstract

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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 Aun(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–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.

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Experimental details of the synthesis and characterization of the material (Supporting Figures S1–S5). This material is available free of charge via the Internet at http://pubs.acs.org.

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