Synthesis and Characterization of Non-Isolated-Pentagon-Rule Actinide Endohedral Metallofullerenes U@C1(17418)-C76, U@C1(28324)-C80, and Th@C1(28324)-C80: Low-Symmetry Cage Selection Directed by a Tetravalent Ion
2018
For the first time, actinide endohedral metallofullerenes (EMFs) with non-isolated-pentagon-rule (non-IPR) carbon cages, U@C80, Th@C80, and U@C76, have been successfully synthesized and fully characterized by mass spectrometry, single crystal X-ray diffractometry, UV–vis–NIR and Raman spectroscopy, and cyclic voltammetry. Crystallographic analysis revealed that the U@C80 and Th@C80 share the same non-IPR cage of C1(28324)-C80, and U@C76 was assigned to non-IPR U@C1(17418)-C76. All of these cages are chiral and have never been reported before. Further structural analyses show that enantiomers of C1(17418)-C76 and C1(28324)-C80 share a significant continuous portion of the cage and are topologically connected by only two C2 insertions. DFT calculations show that the stabilization of these unique non-IPR fullerenes originates from a four-electron transfer, a significant degree of covalency, and the resulting strong host–guest interactions between the actinide ions and the fullerene cages. Moreover, because t...
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