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Geochemical and mineralogical investigation of uranium in multi-element contaminated, organic-rich subsurface sediment

Abstract : Subsurface regions of alluvial sediments characterized by an abundance of refractory or lignitic organic carbon compounds and reduced Fe and S bearing minerals, which are referred to as naturally reduced zones (NRZ), are present at the Integrated Field Research Challenge site in Rifle, CO (a former U mill site), and other contaminated subsurface sites. A study was conducted to demonstrate that the NRZ contains a variety of contaminants and unique minerals and potential contaminant hosts, investigate micron-scale spatial association of U with other co-contaminants, and determine solid phase-bounded U valence state and phase identity. The NRZ sediment had significant solid phase concentrations of U and other co-contaminants suggesting competing sorption reactions and complex temporal variations in dissolved contaminant concentrations in response to transient redox conditions, compared to single contaminant systems. The NRZ sediment had a remarkable assortment of potential contaminant hosts, such as Fe oxides, siderite, Fe(II) bearing clays, rare solids such as ZnS framboids and CuSe, and, potentially, chemically complex sulfides. Micron-scale inspections of the solid phase showed that U was spatially associated with other co-contaminants. High concentration, multi-contaminant, micron size (ca. 5–30 μm) areas of mainly U(IV) (53–100%) which occurred as biogenic UO2 (82%), or biomass – bound monomeric U(IV) (18%), were discovered within the sediment matrix confirming that biotically induced reduction and subsequent sequestration of contaminant U(VI) via natural attenuation occurred in this NRZ. A combination of assorted solid phase species and an abundance of redox-sensitive constituents may slow U(IV) oxidation rates, effectively enhancing the stability of U(IV) sequestered via natural attenuation, impeding rapid U flushing, and turning NRZs into sinks and long-term, slow-release sources of U contamination to groundwater.
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https://hal.inrae.fr/hal-02536006
Contributor : Noémie Janot <>
Submitted on : Tuesday, April 7, 2020 - 7:11:46 PM
Last modification on : Friday, February 26, 2021 - 12:44:03 PM

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Nikolla Qafoku, Brandy Gartman, Ravi Kukkadapu, Bruce Arey, Kenneth Williams, et al.. Geochemical and mineralogical investigation of uranium in multi-element contaminated, organic-rich subsurface sediment. Applied Geochemistry, Elsevier, 2014, 42, pp.77-85. ⟨10.1016/j.apgeochem.2013.12.001⟩. ⟨hal-02536006⟩

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