TY - JOUR
T1 - Au3(μ3-S)(0e) elementary block
T2 - New insights into ligated gold clusters with μ3-sulfido motifs
AU - Xu, Wen Wu
AU - Zeng, Xiao Cheng
AU - Gao, Yi
N1 - Funding Information:
W. W. X. is supported by the Natural Science Foundation of China (11504396). Y. G. is supported by the National Natural Science Foundation of China (11574340), the "Hundred People Project" from the Chinese Academy of Sciences, and the CAS-Shanghai Science Research Center (CAS-SSRC-YJ-2015-01). X. C. Z. is supported by a grant from the Nebraska Center for Energy Sciences Research and a fund from the Beijing Advanced Innovation Center for Soft Matter Science & Engineering for summer visiting scholars. The computational resources utilized in this research were provided by the Shanghai Supercomputer Center, the National Supercomputing Center in Tianjin and Shenzhen, the special program for applied research on super computation of the NSFC-Guangdong joint fund (second phase), and the Holland Computing Center and NC3 computer facility at the University of Nebraska-Lincoln.
Publisher Copyright:
© 2017 The Royal Society of Chemistry.
PY - 2017/7/14
Y1 - 2017/7/14
N2 - An understanding of the structural stability and formation mechanism of ligated gold nanoclusters with triply coordinated μ3-sulfido (μ3-S) motifs is important not only for gold chemistry but also for the design of more effective catalysts or drug carriers for various applications. In this article, a new elementary block Au3(μ3-S) with zero valence electrons [referred to as Au3(μ3-S)(0e)] has been identified, which describes all crystallized ligated gold clusters with μ3-S motifs, in conjunction with the previously reported Au3(2e) and Au4(2e) elementary blocks, in a grand unified model (GUM). This Au3(μ3-S)(0e) elementary block has a tripod structure with the S atom bonding to three Au atoms in a μ3 bridging mode, and can be considered as a μ3-S atom balancing out the 2e valence electrons of the Au3(2e) block. Using Au3(μ3-S) as a building block, a special group of quasi-fullerene hollow-cage [Au3n(μ3-S)2n]n- gold(i) μ3-S clusters are designed, which exhibit high stabilities. In addition, a series of theoretical structures are predicted to be increasingly stable after introducing μ3-S atoms, based on the crystallized clusters. Overall, the introduction of a Au3(μ3-S)(0e) elementary block can help with the understanding of diverse structures of ligated gold clusters with μ3-S motifs, thereby assisting the rational design of new forms of gold nanoclusters.
AB - An understanding of the structural stability and formation mechanism of ligated gold nanoclusters with triply coordinated μ3-sulfido (μ3-S) motifs is important not only for gold chemistry but also for the design of more effective catalysts or drug carriers for various applications. In this article, a new elementary block Au3(μ3-S) with zero valence electrons [referred to as Au3(μ3-S)(0e)] has been identified, which describes all crystallized ligated gold clusters with μ3-S motifs, in conjunction with the previously reported Au3(2e) and Au4(2e) elementary blocks, in a grand unified model (GUM). This Au3(μ3-S)(0e) elementary block has a tripod structure with the S atom bonding to three Au atoms in a μ3 bridging mode, and can be considered as a μ3-S atom balancing out the 2e valence electrons of the Au3(2e) block. Using Au3(μ3-S) as a building block, a special group of quasi-fullerene hollow-cage [Au3n(μ3-S)2n]n- gold(i) μ3-S clusters are designed, which exhibit high stabilities. In addition, a series of theoretical structures are predicted to be increasingly stable after introducing μ3-S atoms, based on the crystallized clusters. Overall, the introduction of a Au3(μ3-S)(0e) elementary block can help with the understanding of diverse structures of ligated gold clusters with μ3-S motifs, thereby assisting the rational design of new forms of gold nanoclusters.
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U2 - 10.1039/c7nr03508j
DO - 10.1039/c7nr03508j
M3 - Article
C2 - 28644502
AN - SCOPUS:85022334071
SN - 2040-3364
VL - 9
SP - 8990
EP - 8996
JO - Nanoscale
JF - Nanoscale
IS - 26
ER -