Direct self-focusing synthesis of monodisperse [Au8(PPh3)7]2+ nanoclusters,Dalton Transactions

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Direct self-focusing synthesis of monodisperse [Au8(PPh3)7]2+ nanoclusters
Dalton Transactions ( IF 3.5 ) Pub Date : 2017-08-21 00:00:00 , DOI: 10.1039/c7dt02657a
Ting Huang _{1,

2,

3,

4} , Li Huang _{1,

2,

3,

4} , Yong Jiang _{1,

2,

3,

4} , Fengchun Hu _{1,

2,

3,

4} , Zhihu Sun _{1,

2,

3,

4} , Guoqiang Pan _{1,

2,

3,

4} , Shiqiang Wei _{1,

2,

3,

4}

Affiliation

Direct and scalable synthesis of monodisperse gold nanoclusters is highly desired but remains a great challenge due to the complexity of chemical reactions. In this regard, a suitable precursor is important as it can simplify the synthesis processes and offer controllability in tuning the product. In this study, we found that Au(PPh₃)₂Cl could be used as an effective precursor for the direct synthesis of atomically monodisperse [Au₈(PPh₃)₇]²⁺ nanoclusters without the need of tedious post-synthetic purification steps. The Au(PPh₃)₂Cl precursor could be directly reduced by NaBH₄ (0.25 molar equivalent) in a dichloromethane solution; this produced Au₈ clusters with a 35% reaction yield. Time-dependent mass spectrometry and in situ UV-vis absorption spectroscopy reveal that the synthesis process is initiated by the rapid formation of the Au₆–Au₈ mixture, followed by a slow spontaneous self-focusing process that converges the mixture into atomically monodisperse Au₈. The success of this direct synthesis has been hypothesized to arise from the relatively stronger Au(I)⋯Au(I) aurophilic attraction between Au(I)-PPh₃ complexes that facilitates the aggregation of Au(I)-PPh₃ on Au(0) cores.

中文翻译：

单分散[Au ₈（PPh ₃）₇ ] ²⁺纳米团簇的直接自聚焦合成

迫切需要直接和可扩展的单分散金纳米簇的合成方法，但由于化学反应的复杂性，仍然是一个巨大的挑战。在这方面，合适的前体很重要，因为它可以简化合成过程并在调节产品时提供可控性。在这项研究中，我们发现Au（PPh ₃）₂ Cl可以用作直接合成原子单分散[Au ₈（PPh ₃）₇ ] ²⁺纳米团簇的有效前体，而无需繁琐的合成后纯化步骤。NaBH ₄可以直接还原Au（PPh ₃）₂ Cl前体（0.25摩尔当量）在二氯甲烷溶液中；这产生了Au ₈簇，反应产率为35％。随时间变化的质谱和原位紫外可见吸收光谱表明，合成过程是由Au ₆ -Au ₈混合物的快速形成引发的，然后是缓慢的自发自聚焦过程，该过程将混合物聚合成原子单分散的Au ₈。这种直接合成的成功已假设从相对较强的Au（对出现我）⋯的Au（我）aurophilic的Au（之间的吸引力我）-PPh _3个配合物便于Au构成的聚合（我）-PPh ₃在Au（0）磁芯上。

更新日期：2017-09-20

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