Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments

Perdrial, Nicolas; Vázquez-Ortega, Angélica; Wang, Guohui; Kanematsu, Masakazu; Mueller, Karl T.; Um, Wooyong; Steefel, Carl I.; O'Day, Peggy A.; Chorover, Jon

doi:10.1016/j.apgeochem.2017.12.001

Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments

Journal Article · Thu Feb 01 04:00:00 EST 2018 · Applied Geochemistry

DOI:https://doi.org/10.1016/j.apgeochem.2017.12.001· OSTI ID:1439679

Perdrial, Nicolas; Vázquez-Ortega, Angélica; Wang, Guohui; Kanematsu, Masakazu; Mueller, Karl T.; Um, Wooyong; Steefel, Carl I.; O'Day, Peggy A.; Chorover, Jon

Uranium speciation and lability are strongly coupled to mineral transformations in silicate sediments, particularly for sediments subjected to weathering in acidic, high-level radioactive waste, as occurred at the Department of Energy's Hanford (WA) site. In this study, uncontaminated Hanford sediments were reacted for 365 days with acidic (pH 3), uranium-bearing waste solutions, with and without phosphate in batch experiments, prior to detailed characterizations using electron microscopy, x-ray diffraction and x-ray absorption spectroscopy. In PO(4)(-)reactant free systems, uranium speciation was controlled initially by precipitation of compreignacite [K-2(UO2)(6)O-4(OH)(6)center dot 8H(2)O]-and becquerelite [Ca(UO2)(6)O-4(OH)(6)center dot 8H(2)O]-like species. Subsequent further removal of uranium coincided with that of Si and accumulation of boltwoodite, [(K, Na)(UO2)(2)O-4(HSiO4)(2)center dot 0.5(H2O)]-like species of uranium at 180 and 365 days. When present, PO4 exerted a direct and strong control over U speciation. The detection of meta-ankoleite, [K-2(UO2)(2)O-4(PO4)(2)center dot 6H(2)O] at all reaction times when U was present emphasizes the importance of dissolved phosphate as a control on U speciation. Here, meta-ankoleite appears well crystallized and when it occurs as the principal product of sediment weathering, its low solubility is expected to limit dissolved U(VI) concentrations in groundwater. Although boltwoodite solubility is also low, it is formed more slowly (and only when PO4 is absent), after initial precipitation of more soluble, less crystalline uranyl hydroxides. In the context of Hanford crib waste our results suggest that with PO4 present, nearly all uranium would have precipitated in the upper soil.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (US)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1439679

Report Number(s):: PNNL-SA-133858; KP1702030

Journal Information:: Applied Geochemistry, Journal Name: Applied Geochemistry Journal Issue: C Vol. 89; ISSN 0883-2927

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

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