A diuranium carbide cluster stabilized inside a C<sub>80</sub> fullerene cage.

Zhang, Xingxing; Li, Wanlu; Feng, Lai; Chen, Xin; Hansen, Andreas; Grimme, Stefan; Fortier, Skye; Sergentu, Dumitru-Claudiu et al. · Nat Commun · 2018

basic_science · Level V

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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<sub>h</sub>(7)-C<sub>80</sub> fullerenes as nanocontainers, a diuranium carbide cluster, U=C=U, has been encapsulated and stabilized in the form of UCU@I<sub>h</sub>(7)-C<sub>80</sub>. This endohedral fullerene was prepared utilizing the Krätschmer-Huffman arc discharge method, and was then co-crystallized with nickel(II) octaethylporphyrin (Ni<sup>II</sup>-OEP) to produce UCU@I<sub>h</sub>(7)-C<sub>80</sub>·[Ni<sup>II</sup>-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<sub>h</sub>(7)-C<sub>80</sub> and the covalent nature of the U(f<sup>1</sup>)=C double bonds were further affirmed through various spectroscopic and theoretical analyses.