Evolution of thiolate-stabilized Ag nanoclusters from Ag-thiolate cluster intermediates

Yitao Cao, Jiahao Guo, Run Shi, Geoffrey I. N. Waterhouse, Jinheng Pan, Zhenxia Du, Qiaofeng Yao, Li-Zhu Wu, Chen-Ho Tung, Jianping Xie and Tierui Zhang ()
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Yitao Cao: Chinese Academy of Sciences
Jiahao Guo: Chinese Academy of Sciences
Run Shi: Chinese Academy of Sciences
Geoffrey I. N. Waterhouse: The University of Auckland
Jinheng Pan: Beijing University of Chemical Technology
Zhenxia Du: Beijing University of Chemical Technology
Qiaofeng Yao: National University of Singapore
Li-Zhu Wu: Chinese Academy of Sciences
Chen-Ho Tung: Chinese Academy of Sciences
Jianping Xie: National University of Singapore
Tierui Zhang: Chinese Academy of Sciences

Nature Communications, 2018, vol. 9, issue 1, 1-6

Abstract: Abstract The synthesis of atomically precise thiolate-stabilized silver (Ag) nanoclusters is the subject of intense research interest, yet the formation mechanism of such nanoclusters remains obscure. Here, electrospray ionization mass spectrometry is successfully applied to monitor the reaction intermediates formed during the sodium-borohydride-reduction of silver 4-tert-butylbenzenethiolate (AgSPh-tBu). We demonstrate a unique evolution route to thiolate-stabilized Ag nanoclusters mediated by Ag-thiolate clusters. The Ag-thiolate clusters form in the initial stage of reduction contain tens of Ag atoms and similar number of ligands, and they are transformed into Ag17(SPh-tBu)123− and Ag44(SPh-tBu)304− nanoclusters in the later reduction process. The number of Ag atoms in the Ag-thiolate clusters determines the reaction path to each final nanocluster product. A similar mechanism is found when silver 2,4-dimethylbenzenethiolate (AgSPhMe2) is used as precursor. This mechanism differs markedly from the long-established bottom-up evolution process, providing valuable new insights into the synthesis of metal nanoclusters.

Date: 2018
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DOI: 10.1038/s41467-018-04837-x

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