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通过噻吩衍生物稳定金原子簇:实现金属再分散的可能途径。

Stabilizing gold adatoms by thiophenyl derivatives: a possible route toward metal redispersion.

机构信息

Fritz-Haber-Institut der MPG, Faradayweg 4-6, D-14195 Berlin, Germany.

出版信息

J Am Chem Soc. 2012 Jul 11;134(27):11161-7. doi: 10.1021/ja300304s. Epub 2012 Mar 30.

Abstract

Tris(phenylthio)benzene molecules have been synthesized in order to explore their ability to trap single Au adatoms on an Au(111) surface. The resulting metal-organic complexes have been characterized with low-temperature scanning tunneling microscopy and infrared reflection absorption spectroscopy; possible structure models have been derived from density functional calculations. Upon room temperature deposition, the thiophenyl derivatives form dimer structures, comprising two molecules and six Au adatoms. Below 100 K, isolated molecules are found as well that have trapped up to six Au atoms. On the basis of the experimental results and calculated formation energies of the complexes, we discuss potential applications of the thioethers for the redispersion of metals on a catalyst surface. First experiments performed on Au particle ensembles prepared on alumina thin films suggest that the molecular ligands are indeed able to change the distribution of gold on the oxide surface.

摘要

为了研究它们在金(111)表面捕获单个金原子的能力,合成了三(苯硫基)苯分子。使用低温扫描隧道显微镜和红外反射吸收光谱对所得金属有机配合物进行了表征;从密度泛函计算中推导出可能的结构模型。在室温沉积时,噻吩基衍生物形成二聚体结构,包含两个分子和六个金原子。在 100 K 以下,也发现了孤立的分子,它们捕获了多达六个金原子。基于实验结果和计算出的配合物形成能,我们讨论了硫醚在催化剂表面上重新分散金属的潜在应用。在氧化铝薄膜上制备的金颗粒聚集体上进行的初步实验表明,分子配体确实能够改变金在氧化物表面上的分布。

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