Origin of magic stability of thiolated gold clusters:: A case study on Au25(SC6H13)18
Origin of magic stability of thiolated gold clusters:: A case study on Au25(SC6H13)18
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DOI：
10.1021/ja073580
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发表时间：
2007-09-19
影响因子：
15
通讯作者：
Tsukuda, Tatsuya
中科院分区：
文献类型：
--
作者：
Negishi, Yuichi;Chaki, Nirmalya K.;Tsukuda, Tatsuya
本工作旨在通过监测Au：S核的电荷状态来验证Au-25（SC 6 H 13）（18）电子壳层模型的有效性，从而阐明魔稳定性的起源。电喷雾电离质谱显示，Schiffrin方法产生的[Au-25（SC 6 H13）（18）]（x）具有电荷态分布，其随着还原时间向负值移动。[Au-25（SC 6 H13）（18）]（0）经化学氧化和还原可分别合成稳定的离子[Au-25（SC 6 H13）（18）]（1+）和[Au-25（SC 6 H13）（18）]（1-）。这些发现使我们得出结论，电子壳层闭合不是[Au-25（SC 6 H 13）（18）]（x）（X = 1-，0，1+）高稳定性的关键因素。我们归因于魔术稳定性的核心笼结构理论预测。
The present work aims to test the validity of the electronic shell model for Au-25(SC6H13)(18) by monitoring the charge state of the Au: S core and thereby to elucidate the origin of magic stability. Electrospray ionization mass spectrometry revealed that the Schiffrin method yields [Au-25(SC6H13)(18)](x) with a distribution of charge states, which shifts toward negative values with reduction time. The stable ions [Au-25(SC6H13)(18)](1+) and [Au-25(SC6H13)(18)](1-) can be synthesized by chemical oxidation and reduction of [Au-25(SC6H13)(18)](0), respectively. These findings lead us to conclude that electronic shell closing is not a crucial factor for the high stability of [Au-25 (SC6H13)(18)](x) (X = 1-, 0, 1+). We ascribe magic stability to the core-in-cage structure predicted theoretically.