期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 132, 期 22, 页码 7696-7701出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja101101d
关键词
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资金
- National Natural Science Foundation of China [10635060, 10725522, 10979047, 10605024, 20701036]
- National Basic Research Program of China [2009CB939901]
Understanding the initial nucleation mechanism of monodisperse nanocrystals (NCs) during synthesis process is an important prerequisite to control the desired sizes and to manipulate the properties of nanoscale materials. The acquisition of information for the small nanocluster nucleation process, however, still remains challenging. Here, using a continuous-flow in situ X-ray absorption fine structure (XAFS) spectroscopy for time-resolved studies, we have clarified the initial kinetic nucleation of Au clusters under the grain size of 1 nm for the classical Au NCs synthesis via the reduction of AuCl4- in aqueous solution. The in situ XAFS results present the experimental revelation of the formation of intermediate Cl3-Au-AuCl3- dimer and the subsequent higher complexes 'AunCln+x' in the initial nucleation stage. We propose a kinetic three-step mechanism involving the initial nucleation, slow growth, and eventual coalescence for the Au NCs formation, which may be helpful for the synthesis of metallic nanomaterials.
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