New Insight into Intermediate Precursors of Brust–Schiffrin Gold Nanoparticles Synthesis
New Insight into Intermediate Precursors of Brust–Schiffrin Gold Nanoparticles Synthesis
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DOI：
10.1021/jp402116x
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发表时间：
2013-05
影响因子：
3.7
通讯作者：
Li‐Lan Zhu;Chen Zhang;Chengchen Guo;Xiaoliang Wang;Pingchuan Sun;Dongshan Zhou;Wei Chen;G. Xue-G.-X
中科院分区：
文献类型：
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作者：
Li‐Lan Zhu;Chen Zhang;Chengchen Guo;Xiaoliang Wang;Pingchuan Sun;Dongshan Zhou;Wei Chen;G. Xue-G.-X
关于添加还原剂之前的中间前驱体，关于金纳米粒子的形成机理一直存在着激烈的争论。本文对广泛使用的Brust-Schiffrin两相法制备金纳米粒子提出了新的详细观点。通过核磁共振、紫外-可见光谱、傅里叶变换拉曼光谱等手段对这些反应的前驱体进行了鉴定和定量，证明了四烷基铵金络合物([TOA][AuX2])和可溶性硫代金([TOA][AuSRX]和[TOA][Au(SR)2])是可被核磁共振检测到的前驱体。它们的相对含量取决于反应物的浓度。较高的反应物浓度有利于形成可溶的硫酸盐。在特定条件下，聚合硫代金[Au(I)SR]n最终可从溶液中析出。这里提出的清晰的机理对于定制最终产品的大小和性能具有重要意义。
There is an ongoing intensive debate on the mechanism of gold nanoparticles formation regarding the intermediate precursors prior to the addition of reducing agent. A new detailed view of the widely used Brust–Schiffrin two-phase method to prepare gold nanoparticles is presented here. Precursor species of these reactions have been identified and quantified by NMR, UV–visible, Fourier-transform Raman spectroscopy, etc. We demonstrate that tetraalkylammonium gold complexes ([TOA][AuX2]) and soluble gold thiolate ([TOA][AuSRX] and [TOA][Au(SR)2]) were detectable as the precursors by NMR spectroscopy. Their relative contents depend on the concentration of reactants. Higher concentration of the reactants is favorable for the formation of soluble thiolate. Polymeric gold thiolate [Au(I)SR]n could eventually precipitate from the solution under specific conditions. The clear mechanism presented here is of great significance to tailor the size and properties of the final products.