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Insight into the Structural Ambiguity of Actinide(IV) Oxalate Sheet Structures: A Case for Alternate Coordination Geometries.
Sockwell, A Kirstin; Sweet, Teagan F M; Barth, Brodie; Isbill, Sara B; DiBlasi, Nicole A; Szymanowski, Jennifer E S; Sigmon, Ginger E; Oliver, Allen G; Miskowiec, Andrew J; Burns, Peter C; Hixon, Amy E.
Afiliación
  • Sockwell AK; Civil & Environmental Engineering & Earth Sciences, University of Notre Dame, Notre Dame, Indiana, 46556, USA.
  • Sweet TFM; Department of Chemistry & Biochemistry, University of Notre Dame, Notre Dame, IN 46556, USA.
  • Barth B; Civil & Environmental Engineering & Earth Sciences, University of Notre Dame, Notre Dame, Indiana, 46556, USA.
  • Isbill SB; Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
  • DiBlasi NA; Civil & Environmental Engineering & Earth Sciences, University of Notre Dame, Notre Dame, Indiana, 46556, USA.
  • Szymanowski JES; Current address: Actinide Analytical Chemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
  • Sigmon GE; Civil & Environmental Engineering & Earth Sciences, University of Notre Dame, Notre Dame, Indiana, 46556, USA.
  • Oliver AG; Civil & Environmental Engineering & Earth Sciences, University of Notre Dame, Notre Dame, Indiana, 46556, USA.
  • Miskowiec AJ; Department of Chemistry & Biochemistry, University of Notre Dame, Notre Dame, IN 46556, USA.
  • Burns PC; Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
  • Hixon AE; Civil & Environmental Engineering & Earth Sciences, University of Notre Dame, Notre Dame, Indiana, 46556, USA.
Chemistry ; 29(47): e202301164, 2023 Aug 21.
Article en En | MEDLINE | ID: mdl-37227412
Plutonium(IV) oxalate hexahydrate (Pu(C2 O4 )2 ⋅ 6 H2 O; PuOx) is an important intermediate in the recovery of plutonium from used nuclear fuel. Its formation by precipitation is well studied, yet its crystal structure remains unknown. Instead, the crystal structure of PuOx is assumed to be isostructural with neptunium(IV) oxalate hexahydrate (Np(C2 O4 )2 ⋅ 6 H2 O; NpOx) and uranium(IV) oxalate hexahydrate (U(C2 O4 )2 ⋅ 6 H2 O; UOx) despite the high degree of unresolved disorder that exists when determining water positions in the crystal structures of the latter two compounds. Such assumptions regarding the isostructural behavior of the actinide elements have been used to predict the structure of PuOx for use in a wide range of studies. Herein, we report the first crystal structures for PuOx and Th(C2 O4 )2 ⋅ 6 H2 O (ThOx). These data, along with new characterization of UOx and NpOx, have resulted in the full determination of the structures and resolution of the disorder around the water molecules. Specifically, we have identified the coordination of two water molecules with each metal center, which necessitates a change in oxalate coordination mode from axial to equatorial that has not been reported in the literature. The results of this work exemplify the need to revisit previous assumptions regarding fundamental actinide chemistry, which are heavily relied upon within the current nuclear field.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Chemistry Asunto de la revista: QUIMICA Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Alemania
Texto completo
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Imprimir
XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Chemistry Asunto de la revista: QUIMICA Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Alemania