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U2@D3h(5)-C78: Experimental Validation of a Theoretically Predicted Structure and Insights into U-U Bonding in a
Songlin Jiang1, Bowei Lv1, Zhiwen He1
1College of Chemistry, Chemical Engineering and Materials Science, and Jiangsu Key Laboratory of Radiation Injury Prevention and Hazardous Substance Control, Soochow University, Suzhou, Jiangsu215123, P. R. China.
Abstract:
The nature of U-U bonding remains one of the most challenging issues in actinide chemistry. Recent theoretical studies have predicted that the fullerene C78 cage can stabilize a U2 dimer in two distinct bonding configurations, namely, a long-bonding model with a weak bond and a short-bonding model featuring a long-sought triple bond. Herein, we report the synthesis, isolation, and molecular characterization of U2@D3h(5)-C78, providing experimental validation of this theoretically proposed system. Single-crystal X-ray diffraction analysis reveals that the U2 dimer is located on the 3-fold axis of the D3h(5)-C78 cage, with a U-U distance of 4.073 Å. This geometry is in good agreement with the predicted long-bonding configuration, indicating a weak bond between the two U atoms. Further analysis indicates a plausible strategy for achieving shorter U-U distances through modulation of cage size. These findings highlight the tunability of U-U bonding in confined carbon cages and provide valuable guidance for the future exploration of higher-order U-U multiple bonding within fullerene cages.
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