|In situ studies on controlling an atomically-accurate formation process of gold nanoclusters|
|Yang, LN; Cheng, H; Jiang, Y; Huang, T; Bao, J; Sun, ZH; Jiang, Z; Ma, JY; Sun, FF; Liu, QH; Yao, T; Deng, HJ; Wang, SX; Zhu, MZ; Wei, SQ; Sun, ZH (reprint author), Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China.
|Abstract||Knowledge of the molecular formation mechanism of metal nanoclusters is essential for developing chemistry for accurate control over their synthesis. Herein, the "top-down" synthetic process of monodisperse Au-13 nanoclusters via HCl etching of polydisperse Au-n clusters ( 15 <= n <= 65) is traced by a combination of in situ X-ray/UV-vis absorption spectroscopy and time-dependent mass spectrometry. It is revealed experimentally that the HCl-induced synthesis of Au-13 is achieved by accurately controlling the etching process with two distinctive steps, in sharp contrast to the traditional thiol-etching mechanism through release of the Au(I) complex. The first step involves the direct fragmentation of the initial larger Aun clusters into metastable intermediate Au-8-Au-13 smaller clusters. This is a critical step, which allows for the secondary size-growth step of the intermediates toward the atomically monodisperse Au-13 clusters via incorporating the reactive Au(I)-Cl species in the solution. Such a secondary-growth pathway is further confirmed by the successful growth of Au-13 through reaction of isolated Au-11 clusters with AuClPPh3 in the HCl environment. This work addresses the importance of reaction intermediates in guiding the way towards controllable synthesis of metal nanoclusters.|
|Keyword||Number Au-13 Clusters
|Corresponding Author||Sun, ZH (reprint author), Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China.|
Yang, LN,Cheng, H,Jiang, Y,et al. In situ studies on controlling an atomically-accurate formation process of gold nanoclusters[J]. NANOSCALE,2015,7(34):14452—14459.
Yang, LN.,Cheng, H.,Jiang, Y.,Huang, T.,Bao, J.,...&Sun, ZH .(2015).In situ studies on controlling an atomically-accurate formation process of gold nanoclusters.NANOSCALE,7(34),14452—14459.
Yang, LN,et al."In situ studies on controlling an atomically-accurate formation process of gold nanoclusters".NANOSCALE 7.34(2015):14452—14459.
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