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Unraveling the highest oxidation states of actinides in solid-state compounds with a particular focus on plutonium.
Physical Chemistry Chemical Physics : PCCP 2018 November 15
The nature and extent of the highest oxidation state (HOS) in solid-state actinide compounds are still unexplored compared with those of small molecules, and there is burgeoning interest in studying the actinide-ligand bonding nature in the condensed state. A comprehensive understanding of the electronic structure and unraveling the possibility of a HOS are of paramount importance in solid-state actinide chemistry. Here, we report the physical OS of the early to middle actinides (Th → Cm) in solid-state compounds via a more rigorous quantum mechanical definition of OS under the DFT+U theoretical frameworks for the first time. This work implies that the highest physical OS of the Pu solid ion is PuV in PuO2F and PuOF4, which can be achieved via tuning the ligand, thus improving our knowledge of oxidation states and chemical bonding in high OS solid-state compounds. We highlight the importance of ligand design in terms of the actinide HOS, employing a highly electronegative ligand and showing the capacity to form multiple bonds.
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