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Zhuang, Jiaxin ; Abella, Laura ; Sergentu, Dumitru-Claudiu ; Yao, Yang-Rong ; Jin, Meihe ; Yang, Wei ; Zhang, Xingxing ; Li, Xiaomeng ; Zhang, Duo ; Zhao, Yiming ; et al ( , Journal of the American Chemical Society)
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Cai, Wenting ; Abella, Laura ; Zhuang, Jiaxin ; Zhang, Xingxing ; Feng, Lai ; Wang, Yaofeng ; Morales-Martínez, Roser ; Esper, Ronda ; Boero, Mauro ; Metta-Magaña, Alejandro ; et al ( , Journal of the American Chemical Society)
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Zhang, Xingxing ; Li, Wanlu ; Feng, Lai ; Chen, Xin ; Hansen, Andreas ; Grimme, Stefan ; Fortier, Skye ; Sergentu, Dumitru-Claudiu ; Duignan, Thomas J. ; Autschbach, Jochen ; et al ( , Nature Communications)
Abstract Unsupported non-bridged uranium–carbon double bonds have long been sought after in actinide chemistry as fundamental synthetic targets in the study of actinide-ligand multiple bonding. Here we report that, utilizing
I h(7)-C80fullerenes as nanocontainers, a diuranium carbide cluster, U=C=U, has been encapsulated and stabilized in the form of UCU@I h(7)-C80. This endohedral fullerene was prepared utilizing the Krätschmer–Huffman arc discharge method, and was then co-crystallized with nickel(II) octaethylporphyrin (NiII-OEP) to produce UCU@I h(7)-C80·[NiII-OEP] as single crystals. X-ray diffraction analysis reveals a cage-stabilized, carbide-bridged, bent UCU cluster with unexpectedly short uranium–carbon distances (2.03 Å) indicative of covalent U=C double-bond character. The quantum-chemical results suggest that both U atoms in the UCU unit have formal oxidation state of +5. The structural features of UCU@I h(7)-C80and the covalent nature of the U(f1)=C double bonds were further affirmed through various spectroscopic and theoretical analyses.