期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 144, 期 5, 页码 2156-2163出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c10450
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资金
- JSPS KAKENHI [JP16H06509]
The asymmetric induction of metal clusters through ligation of chiral ligands allows for the twisting and stabilization of the resulting chiral structure, which has significant implications for the design of asymmetric catalysts and chiroptical materials.
Asymmetric induction of metal clusters by ligation of chiral ligands is intriguing in terms of the mechanism of chirality transfer and the stability of the resulting chiral structure. Here we report the asymmetric induction of C-centered hexagold(I) CAu6I clusters into an asymmetrically twisted structure through monodentate, chiral benzimidazolylidene-based N-heterocyclic carbene (NHC) ligands. X-ray diffraction analysis revealed that the NHC-ligated CAu6I cluster was diastereoselectively twisted with directionally selective, bond length expansion, and contraction of the Au center dot center dot center dot Au contacts and that the original cluster with high symmetry was transformed into an optically pure, asymmetric CAu6I cluster with C-1 symmetry. Moreover, the circular dichroism spectroscopy and the time-dependent density functional theory calculation confirmed that the asymmetrically twisted CAu6I structure was maintained even in solution. Such asymmetric induction of configurationally stable metal clusters would greatly expand the molecular design possibilities of asymmetric catalysts and chiroptical materials by utilizing library chiral NHC ligands.
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