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

A diuranium carbide cluster stabilized inside a C80 fullerene cage