Uranium(VI) attenuation in a carbonate-bearing oxic alluvial aquifer

Nolan, PJ; Bone, Sharon E.; Campbell, Kate M.; Pan, Donald; Healy, Olivia M.; Stange, Marty; Bargar, John R.; Weber, Karrie A.

doi:10.1016/j.jhazmat.2021.125089

Uranium(VI) attenuation in a carbonate-bearing oxic alluvial aquifer

Journal Article · Thu Jan 07 23:00:00 EST 2021 · Journal of Hazardous Materials

DOI:https://doi.org/10.1016/j.jhazmat.2021.125089· OSTI ID:1807547

Nolan, PJ ^[1]; Bone, Sharon E. ^[2]; Campbell, Kate M. ^[3]; Pan, Donald ^[4]; Healy, Olivia M. ^[5]; Stange, Marty ^[6]; Bargar, John R. ^[2]; Weber, Karrie A. ^[7]

Univ. of Nebraska, Lincoln, NE (United States); Golder Associates Inc., Redmond, WA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
US Geological Survey, Boulder, CO (United States)
Univ. of Nebraska, Lincoln, NE (United States); Florida Gulf Coast Univ., Fort Myers, FL (United States)
Univ. of Nebraska, Lincoln, NE (United States)
City of Hastings, NE (United States). Hastings Utilities
Univ. of Nebraska, Lincoln, NE (United States); Univ. of Nebraska, Lincoln, NE (United States). Daugherty Water for Food Global Inst.

Uranium minerals are commonly found in soils and sediment across the United States at an average concentration of 2–4 mg/kg. Uranium occurs in the environment primarily in two forms, the oxidized, mostly soluble uranium(VI) form, or the reduced, sparingly soluble reduced uranium(IV) form. Here we describe subsurface geochemical conditions that result in low uranium concentrations in an alluvial aquifer with naturally occurring uranium in soils and sediments in the presence of complexing ligands under oxidizing conditions. Groundwater was saturated with respect to calcite and contained calcium (78–90 mg/L) with elevated levels of carbonate alkalinity (291–416 mg/L as HCO₃-). X-ray adsorption near edge structure (XANES) spectroscopy identified that sediment-associated uranium was oxidized as a uranium(VI) form (85%). Calcite was the predominant mineral by mass in the ultrafine fraction in uranium-bearing sediments (>16 mg/kg). Furthermore, groundwater geochemical modeling indicated calcite and/or a calcium-uranyl-carbonate mineral such as liebigite in equilibrium with groundwater. The δ¹³C (0.57‰ ± 0.15‰) was indicative of abiotic carbonate deposition. Thus, solid-phase uranium(VI) associated with carbonate is likely maintaining uranium(VI) groundwater levels below the maximum contaminant level (MCL; 30 µg/L), presenting a deposition mechanism for uranium attenuation rather than solely a means of mobilization.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

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

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1807547

Journal Information:: Journal of Hazardous Materials, Journal Name: Journal of Hazardous Materials Vol. 412; ISSN 0304-3894

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Uranium(VI) attenuation in a carbonate-bearing oxic alluvial aquifer

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