Journal
INORGANIC CHEMISTRY
Volume 59, Issue 17, Pages 12650-12658Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.0c01756
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Funding
- National Natural Science Foundation of China [21773181, 21573172]
- Nanotechnology Platform Program (Molecule and Material Synthesis) of the Ministry of Education, Culture, Sports, Science, and Technology of Japan
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Four-electron transfer from U to the fullerene cage commonly exists in U@C-2n, (2n < 82) so far, while four- and three-electron transfers, which depend on the cage isomers, simultaneously occur in U@C-82. Herein, detailed quantum-chemicaI methods combined with statistical thermodynamic analysis were applied to deeply probe into U@C-84, which is detected in the mass spectra without any further exploration. With triplet ground states, novel isomers including isolated-pentagon-rule U@C-2(51579)-C-84 and U@D-2(51573) -C-84 as well as nonisolated-pentagon-rule U@C-5(51365)-C-84 were identified as thermodynamically optimal. Surprisingly, there were unexpected three-electron transfers, which directly led to one unpaired electron on the cage, in all of the three isomers. Significant covalent interactions between the cage and U successively weakened for U@D-2(51573)-C-84, U@C-2(51579)-C-84, and U@C-5(51365)-C-84. Besides, the IR absorption spectra were simulated as a reference for further structural identification in the experiment. Last but not least, the potential reaction sites were predicted to facilitate further functionalization and thus achieve promising applications for U@C-84.
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