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 · Tue Dec 05 00:00:00 EST 2017 · Applied Geochemistry

DOI:https://doi.org/10.1016/J.APGEOCHEM.2017.12.001· OSTI ID:1413491

Perdrial, Nicolas ^[1]; Vázquez-Ortega, Angélica ^[2]; Wang, Guohui ^[3]; Kanematsu, Masakazu ^[4]; Mueller, Karl T. ^[3]; Um, Wooyong ^[5]; Steefel, Carl I. ^[6]; O'Day, Peggy A. ^[7]; Chorover, Jon ^[8]

Univ. of Vermont, Burlington, VT (United States). Dept. of Geology
Univ. of Arizona, Tucson, AZ (United States). Dept. of Soil Water and Environmental Science; Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Sciences
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Anchor QEA, LLC, Portland, OR (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Merced, CA (United States). School of Natural Sciences
Univ. of Arizona, Tucson, AZ (United States). Dept. of Soil Water and Environmental Science

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. Here, 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 PO₄-reactant free systems, uranium speciation was controlled initially by precipitation of compreignacite [K₂(UO₂)₆O₄(OH)₆·8H₂O]- and becquerelite [Ca(UO₂)₆O₄(OH)₆·8H₂O]-like species. Subsequent further removal of uranium coincided with that of Si and accumulation of boltwoodite, [(K, Na)(UO₂)₂O₄(HSiO₄)₂•0.5(H₂O)]-like species of uranium at 180 and 365 days. When present, PO₄ exerted a direct and strong control over U speciation. Furthermore, the detection of meta-ankoleite, [K₂(UO₂)₂O₄(PO₄)₂·6H₂O] 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-05CH11231; AC05-76RL01830

OSTI ID:: 1413491

Alternate ID(s):: OSTI ID: 1548954
OSTI ID: 1439679
OSTI ID: 1476618

Report Number(s):: PNNL-SA-133858; PII: S0883292717303657

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

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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

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