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Heptavalent Actinide Tetroxides NpO4- and PuO4-: Oxidation of Pu(V) to Pu(VII) by Adding an Electron to PuO4.
J Phys Chem A ; 121(47): 9156-9162, 2017 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-29136367
The highest known actinide oxidation states are Np(VII) and Pu(VII), both of which have been identified in solution and solid compounds. Recently a molecular Np(VII) complex, NpO3(NO3)2-, was prepared and characterized in the gas phase. In accord with the lower stability of heptavalent Pu, no Pu(VII) molecular species has been identified. Reported here are the gas-phase syntheses and characterizations of NpO4- and PuO4-. Reactivity studies and density functional theory computations indicate the heptavalent metal oxidation state in both. This is the first instance of Pu(VII) in the absence of stabilizing effects due to condensed phase solvation or crystal fields. The results indicate that addition of an electron to neutral PuO4, which has a computed electron affinity of 2.56 eV, counterintuitively results in oxidation of Pu(V) to Pu(VII), concomitant with superoxide reduction.





Texto completo: Disponível Coleções: Bases de dados internacionais Base de dados: MEDLINE Idioma: Inglês Revista: J Phys Chem A Assunto da revista: Química Ano de publicação: 2017 Tipo de documento: Artigo País de afiliação: Estados Unidos