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Isolation of the Au145(SR)60X compound (R = n-butyl, n-pentyl; X = Br, Cl): novel gold nanoclusters that exhibit properties subtly distinct from the ubiquitous icosahedral Au144(SR)60 compound
Nanoscale ( IF 5.8 ) Pub Date : 2021-09-01 , DOI: 10.1039/d1nr04745k
Tiziano Dainese 1 , Sabrina Antonello 1 , Sara Bonacchi 1 , Daniel Morales-Martinez 1 , Alfonso Venzo 2 , David M Black 3 , M Mozammel Hoque 4 , Robert L Whetten 4 , Flavio Maran 1, 5
Affiliation  

We report the identification and quantitative isolation of Au145(SR)60X (R = n-butyl, n-pentyl; X = halide) along with elucidation of key properties as compared to the corresponding ubiquitous chiral-icosahedral Au144(SR)60 cluster known to have a central vacancy. The stoichiometries were assessed by electrospray mass spectrometry (ESI-MS) at isotopic resolution, and induced dissociation patterns indicate the ‘extra’ (Au,Br) atoms are strongly bound components of these structures. Voltammetric and spectroscopic characterization reveals Au145(SR)60X behaviors that are qualitatively similar to yet fascinatingly distinct from those of Au144(SR)60. (1H,13C)-NMR spectra clearly show how both Au145(SR)60X and Au144(SR)60 are capped by 12 distinct ligand types of 5-fold equivalence, as was recently established for Au144(SR)60 capped by shorter ligands, demonstrating that this novel cluster shares the same chiral-icosahedral motif. Intriguingly, Au145(SR)60X is strongly near-IR luminescent, whereas under comparable conditions Au144(SR)60 barely emits. The photoluminescence pattern of Au145(SR)60X is very similar to that observed for Au25(SR)18, which contains the Au13 core. The combined results are interpreted as consistent with neutral Au145(SR)60X as a diamagnetic species, electronically and structurally similar to the corresponding Au144(SR)60 compounds.

中文翻译:

Au145(SR)60X 化合物(R = 正丁基,正戊基;X = Br,Cl)的分离:新型金纳米团簇,其性质与无处不在的二十面体 Au144(SR)60 化合物略有不同

我们报告了 Au 145 (SR) 60 X(R =丁基,戊基;X = 卤化物)的鉴定和定量分离,并阐明了与相应无处不在的手性二十面体 Au 144 (SR)相比的关键特性60集群已知有一个中央空缺。在同位素分辨率下通过电喷雾质谱 (ESI-MS) 评估化学计量,诱导解离模式表明“额外”(Au,Br) 原子是这些结构的强结合成分。伏安和光谱表征显示 Au 145 (SR) 60X 行为在性质上与 Au 144 (SR) 60 的行为相似但又截然不同。( 1 H, 13 C)-NMR 光谱清楚地显示了 Au 145 (SR) 60 X 和 Au 144 (SR) 60如何被 12 种不同的 5 倍等效配体类型覆盖,正如最近为 Au 144 (SR)建立的那样) 60被较短的配体覆盖,表明这个新的簇共享相同的手性二十面体基序。有趣的是,Au 145 (SR) 60 X 具有很强的近红外发光,而在类似条件下 Au 144 (SR) 60几乎不发出。Au 145 (SR) 60 X的光致发光模式与观察到的 Au 25 (SR) 18非常相似,其中包含 Au 13核。综合结果被解释为与作为抗磁性物质的中性 Au 145 (SR) 60 X一致,在电子和结构上与相应的 Au 144 (SR) 60化合物相似。
更新日期:2021-09-09
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