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Novel actinide cluster fullerenes, U 2 C 2 @ I   h  (7)-C 80 and U 2 C 2 @ D  3 h  (5)-C 78 , were synthesized and fully characterized by mass spectrometry, single-crystal X-ray crystallography, UV-vis-NIR, nuclear magnetic resonance spectroscopy (NMR), X-ray absorption spectroscopy (XAS), Raman spectroscopy, IR spectroscopy, as well as density functional and multireference wave function calculations. The encapsulated U 2 C 2 is the first example of a uranium carbide cluster featuring two U centers bridged by a C≡C unit. The U-C bond distances in these U 2 C 2 clusters are in the range between 2.130 and 2.421 Å. While the U 2 C 2 cluster in U 2 C 2 @C 80 adopts a butterfly-shaped geometry with a U-C 2 -U dihedral angle of 112.7° and a U-U distance of 3.855 Å, the U-U distance in U 2 C 2 @C 78 is 4.164 Å and the resulting U-C 2 -U dihedral angle is increased to 149.1°. The combined experimental and quantum-chemical results suggest that the formal U oxidation state is +4 in the U 2 C 2 cluster, and each U center transfers three electrons to the C 2 n  cage and one electron to C 2 . Different from the strong U═C covalent bonding reported for U 2 C@C 80 , the U-C bonds in U 2 C 2 are less covalent and predominantly ionic. The C-C triple bond is somewhat weaker than in HCCH, and the C-C π bonds undergo donation bonding with the U centers. This work demonstrates that the combination of the unique encapsulation effect of fullerene cages and the variable oxidation states of actinide elements can lead to the stabilization of novel actinide clusters, which are not accessible by conventional synthetic methods.

Diuranium(IV) Carbide Cluster U2C2 Stabilized Inside Fullerene Cages

Diuranium(IV) Carbide Cluster U₂C₂ Stabilized Inside Fullerene Cages