Neptunium(V) partitioning to uranium(VI) oxide and peroxide solids.
Metaschoepite, [(UO2)8O2(OH)12] x 10H2O, and metastudtite, UO4 x 4H2O, are alteration phases anticipated in a spent nuclear fuel repository following the moist oxidation of UO2 on a geologic time scale. Dissolved concentrations and hence potential mobility of other radionuclides in the fuel, such as the neptunyl cation (NpO2+), will likely be determined by the extent of their partitioning into these U(VI) solids. 237Np is of particular interest due to its potential high mobility and long half-life (2.1 x 10(6) years.) In this study, metaschoepite has been precipitated and subsequently transformed to studtite in the presence of dissolved Np. The metaschoepite and studtite solids that formed initially contained <10 and 6500 ppm Np, respectively. Batch dissolution studies of these solids at pH 6 demonstrate release of Np that exceeds congruent dissolution of U from metastudtite; furthermore, the released Np cation remains in solution. Thus, although the Np partitions into the metastudtite solid initially, it is released to solution over time, indicating that metastudtite is not likely to serve as a host solid for Np incorporation or sorption of the neptunyl cation on long time scales.
Washington State University, Department of Chemistry, Pullman, Washington 99164-4630, USA.
Matthew
M
Douglas
Sue B
SB
Clark
Judah I
JI
Friese
Bruce W
BW
Arey
Edgar C
EC
Buck
Brady D
BD
Hanson
D000327:Adsorption; D002412:Cations; D011232:Chemical Precipitation; D006863:Hydrogen-Ion Concentration; D008855:Microscopy, Electron, Scanning; D009405:Neptunium / Q000032:analysis / Q000737:chemistry*; D010084:Oxidation-Reduction; D010545:Peroxides / Q000032:analysis / Q000737:chemistry*; D012990:Soil Pollutants, Radioactive; D012995:Solubility; D013696:Temperature; D013997:Time Factors; D017974:Uranium Compounds / Q000032:analysis / Q000737:chemistry*; D014875:Water Pollutants, Radioactive
D002412:Cations; D010545:Peroxides; D012990:Soil Pollutants, Radioactive; D017974:Uranium Compounds; D014875:Water Pollutants, Radioactive; D009405:Neptunium; C012597:uranium dioxide