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[Cu-32(PET)(24)H8Cl2](PPh4)(2): A Copper Hydride Nanocluster with a Bisquare Antiprismatic Core

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Title
[Cu-32(PET)(24)H8Cl2](PPh4)(2): A Copper Hydride Nanocluster with a Bisquare Antiprismatic Core
Author(s)
Sanghwa Lee; Megalamane S. Bootharaju; Guocheng Deng; Sami Malola; Woonhyuk Baek; Hannu Häkkinen; Nanfeng Zheng; Taeghwan Hyeon
Subject
METAL NANOCLUSTERS, ; GOLD NANOCLUSTERS, ; CLUSTERS, ; NANOPARTICLES
Publication Date
2020-08
Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.142, no.32, pp.13974 - 13981
Publisher
AMER CHEMICAL SOC
Abstract
© 2020 American Chemical Society. Atomically precise coinage metal (Au, Ag, and Cu) nanoclusters (NCs) have been the subject of immense interest for their intriguing structural, photophysical, and catalytic properties. However, the synthesis of Cu NCs is highly challenging because of low reduction potential and high reactivity of copper, demonstrating the need for new synthetic methods using appropriate ligand combinations. By designing a diamine-assisted synthetic strategy, here we report the synthesis and total structure characterization of a box-like dianionic Cu NC [Cu-32(PET)(24)H8Cl2](PPh4)(2) coprotected by 2-phenylethanethiolate (PET), hydride, and chloride ligands. Its crystal structure comprises a rare bisquare antiprismatic Cu14H8 core, assembled by two square antiprisms by edge sharing, followed by hydride binding. The rod-shaped Cu14H8 core is clamped by two complex Cu-7(PET)(11)Cl and two simple Cu2PET metal ligand frameworks, constructing the complete structure of Cu-32 NC. The presence, number, and location of hydrides are established by combined experimental and density functional theory results. The electronic structure calculations show the cluster as a zero-free-electron system, reproduce well the measured optical absorption spectrum, and explain the main absorption features. Furthermore, the Cu-32 cluster is found to be a highly active homogeneous catalyst for C-N bond formation in aniline carbonylation reactions at room temperature. We hope that new findings in this work will stimulate and expand the research on Cu and other active metal NCs
URI
https://pr.ibs.re.kr/handle/8788114/7685
DOI
10.1021/jacs.0c06577
ISSN
0002-7863
Appears in Collections:
Center for Nanoparticle Research(나노입자 연구단) > 1. Journal Papers (저널논문)
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