Toward Understanding the Growth Mechanism: Tracing All Stable Intermediate Species from Reduction of Au(I)鈥揟hiolate Complexes to Evolution of Au25 Nanoclusters

详细信息    查看全文

• 作者：Zhentao Luo ; Vairavan Nachammai ; Bin Zhang ; Ning Yan ; David Tai Leong ; De-en Jiang ; Jianping Xie
• 刊名：Journal of the American Chemical Society
• 出版年：2014
• 出版时间：July 30, 2014
• 年：2014
• 卷：136
• 期：30
• 页码：10577-10580
• 全文大小：317K
• ISSN：1520-5126

文摘

Despite 20 years of progress in synthesizing thiolated gold nanoclusters (Au NCs), the knowledge of their growth mechanism still lags behind. Herein the detailed process from reduction of Au(I)鈥搕hiolate complex precursors to the eventual evolution of and focusing to the atomically precise Au₂₅ NCs was revealed for the first time by monitoring the time evolution of Au(I) precursor and Au NC intermediate species with ESI-MS. A two-stage, bottom-up formation and growth process was proposed: a fast stage of reduction-growth mechanism, followed by a slow stage of intercluster conversion and focusing. Balanced reactions of formation for each identified NC were suggested, backed by theoretical calculations of the thermodynamic driving force. This work advances one step further toward understanding the mechanism of formation and growth of thiolated Au NCs.