Abstract
Tailoring of specific sites on the nanocluster surface can tailor the properties of nanoclusters at the atomic level, for the in-depth understanding of structure and property relationship. In this work, we explore the regulation of surface structure of [Au9Ag12(SAdm)4(Dppm)6Cl6](SbF6)3 nanocluster via alloying. We successfully obtained the well-determined tri-metal [Au9Ag8@Cu4(SAdm)4(Dppm)6Cl6](SbF6)3 by the reaction of [Au9Ag12(SAdm)4(Dppm)6Cl6](SbF6)3 with the CuI(SAdm) complex precursor. X-ray crystallography identifies that the Cu dopants prioritily replace the position of the silver capped by Dppm ligand in the motif. The Cu doping has affected the optical properties of Au9Ag12 alloy nanocluster. DPV spectra, CD spectra and stability tests suggest that the regulation of surface structure via Cu alloying changes the electronic structure, thereby affecting the electrochemical properties, which provides insight into the regulation of surface structure of [Au9Ag12(SAdm)4(Dppm)6Cl6](SbF6)3 via alloying.
Highlights
Precise core-shell nanoclusters have become a promising material in catalysis, biomedicine, and chemical sensing due to the unique quantum confinement effect resulting in optical properties (Jin et al, 2016; Yao et al, 2018; Xu et al, 2019; Jin R. et al, 2021; Sun et al, 2021; Zheng et al, 2021)
The studies on correlation between the properties and structures of cluster compounds based on the determined crystal structures show that the core and shell structures have different effects on the performance of the cluster compounds, and modifications on the core and shell structures may induce variations on clusters properties (AbdulHalim et al, 2014; Chakraborty and Pradeep, 2017; Khatun et al, 2018; Yan et al, 2018; Jin Y. et al, 2021)
X-ray crystallography identifies that the Cu dopants prioritily replace the position of the silver of peripheral structures DppmAg2Cl2(SR)2
Summary
Precise core-shell nanoclusters have become a promising material in catalysis, biomedicine, and chemical sensing due to the unique quantum confinement effect resulting in optical properties (Jin et al, 2016; Yao et al, 2018; Xu et al, 2019; Jin R. et al, 2021; Sun et al, 2021; Zheng et al, 2021). 2019b; Kang et al, 2020) When the third metal is doped into the bimetallic alloy clusters, what site will it occupy and what effect will it have on the overall performance?Recently, for the active metal Cu doping, several surface Cu-doped nanoclusters such as Au13Cux (x 2, 4, 8) (Yang et al, 2013), CuxAu25-x (Yang et al, 2017), Cu3Au34 (Yang et al, 2017), Ag28Cu12 (Yan et al, 2016), Ag30Cu14 (Li at al., 2020) and Cu-internal-doped nanoclusters like Ag61Cu30 have been observed and well-determined by x-ray crystallography (Zou et al, 2020). We use position-determined alloy clusters [Au9Ag12(SAdm)4(Dppm)6Cl6](SbF6) as templates for the doping of the third metal copper (Jin et al, 2018b). This provides a good observation method for understanding the doping position
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