18–23 Apr 2010
Casino Conference Centre
UTC timezone

Single crystal X-ray diffraction and Raman characterization of ternary Ce(IV) and Pu(IV) peroxo-carbonate compounds comprised of rare dimeric molecular units

Not scheduled
15m
Casino Conference Centre

Casino Conference Centre

Reitenbergerova 4/95, Marianske Lazne, Czech Republic
Verbal Chemistry of Actinide and Trans-actinide Elements

Speaker

Lucas Sweet (Pacific Northwest National Laboratory)

Description

The environmental fate and transport of transuranium elements and the search for alternative f-element separation methods require a better understanding of the speciation of transuranics under oxidizing alkaline conditions, especially in the presence of ubiquitous ligands such as peroxide and carbonate. From our exploration of the Ce and Pu peroxo-carbonate systems several new structures containing the known [(CO3)3M(O2)2Ce(CO3)3]–8 (M = Ce(IV) or Pu(IV)) dimer were found. A simplified synthetic procedure was used to prepare crystalline products of several novel compounds, namely [NH4]8[(CO3)3Ce(O2)2Ce(CO3)3]•6H2O, [C(NH2)3]8[(CO3)3Ce(O2)2Ce(CO3)3] ]•4H2O, Na8[(CO3)3Ce(O2)2Ce(CO3)3]•12H2O and K8[(CO3)3Pu(O2)2Ce(CO3)3]•12H2O. Structural characterization of the aforementioned compounds was performed using single crystal x-ray diffraction. It was observed that the crystal packing of the [(CO3)3M(O2)2Ce(CO3)3]–8 dimeric unit varied significantly depending on the cation incorporated into the structure (e.g., Na+, K+, NH4+ , and C(NH2)3+). Additional characterization of the f-element compounds was performed on single crystals using a high-resolution microscope-based Raman spectrometer.

Primary author

Lucas Sweet (Pacific Northwest National Laboratory)

Co-authors

Kate Ziegelgruber (Ohio State University) Leah Arrigo (Pacific Northwest National Laboratory) Shane Peper (Pacific Northwest National Laboratory)

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