Identification of Intermediate Au22(SR)4(SR′)14 Cluster on Ligand-Induced Transformation of Au25(SR)18 Nanocluster,The Journal of Physical Chemistry Letters

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Identification of Intermediate Au22(SR)4(SR′)14 Cluster on Ligand-Induced Transformation of Au25(SR)18 Nanocluster
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2019-07-24 00:00:00 , DOI: 10.1021/acs.jpclett.9b01856
Anu George ₁ , Anusree Sundar ₁ , Akhil S. Nair ₂ , Manju P. Maman ₁ , Biswarup Pathak ₂ , Nitya Ramanan ₃ , Sukhendu Mandal ₁

Affiliation

We report the ligand-exchange-induced transformation from an icosahedral Au₂₅(SR)₁₈ cluster (where SR = 2-phenylethanethiol (PET)) to a bitetrahedral Au₂₂(SR)₄(SR′)₁₄ cluster (where SR′ = 4-tert-butylbenzenethiol (TBBT)). This partial exchange of the ligands was achieved by controlling the concentration of the incoming TBBT ligand. Being a bulky and aromatic ligand, TBBT can efficiently distort the atomic structure of the Au₂₅PET₁₈ cluster, resulting in Au₂₂(PET)₄(TBBT)₁₄, which is highly stable and considered to be an intermediate with a bitetrahedral structure. Time-dependent mass spectrometry and optical spectroscopy revealed the dissociation of the parent cluster and gave a deep insight on the ligand-exchange mechanism. Theoretical calculations and extended X-ray absorption fine structure studies confirm the formation of the Au₂₂ structure. Identifying the atomic structure of the intermediate species opens a new avenue to study the transformation of one cluster to another.

中文翻译：

在配体诱导的Au ₂₅（SR）₁₈纳米团簇转化中鉴定中间Au ₂₂（SR）₄（SR'）₁₄团簇

我们报告了配体交换诱导的从二十面体Au ₂₅（SR）₁₈簇（其中SR = 2-苯基乙硫醇（PET））到二面体Au ₂₂（SR）₄（SR'）₁₄簇（其中SR'= 4-叔丁基苯硫醇（TBBT））。配体的这种部分交换是通过控制进入的TBBT配体的浓度来实现的。TBBT是一种庞大且芳香的配体，可有效扭曲Au ₂₅ PET ₁₈团簇的原子结构，从而产生Au ₂₂（PET）₄（TBBT）₁₄，它是高度稳定的，被认为是具有二面体结构的中间体。时变质谱和光学光谱揭示了母体簇的解离，并提供了对配体交换机理的深刻见解。理论计算和扩展的X射线吸收精细结构研究证实了Au ₂₂结构的形成。鉴定中间物种的原子结构为研究一个簇向另一个簇的转化开辟了一条新途径。

更新日期：2019-07-24

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