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Paradis, C.J.; Hoss, K.N.; Meurer, C.E.; Hatami, J.L.; Dangelmayr, M.A.; Tigar, A.D.; Johnson, R.H. |
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Title |
Elucidating mobilization mechanisms of uranium during recharge of river water to contaminated groundwater |
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Journal Article |
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Year |
2022 |
Publication |
Journal of Contaminant Hydrology |
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251 |
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Pages |
104076 |
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Keywords |
Desorption, Dissolution, Groundwater, Surface water, Tracer, Uranium |
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Abstract |
The recharge of stream water below the baseflow water table can mobilize groundwater contaminants, particularly redox-sensitive and sorptive metals such as uranium. However, in-situ tracer experiments that simulate the recharge of stream water to uranium-contaminated groundwater are lacking, thus limiting the understanding of the potential mechanisms that control the mobility of uranium at the field scale. In this study, a field tracer test was conducted by injecting 100 gal (379 l) of oxic river water into a nearby suboxic and uranium-contaminated aquifer. The traced river water was monitored for 18 days in the single injection well and in the twelve surrounding observation wells. Mobilization of uranium from the solid to the aqueous phase was not observed during the tracer test despite its pre-test presence being confirmed on the aquifer sediments from lab-based acid leaching. However, strong evidence of oxidative immobilization of iron and manganese was observed during the tracer test and suggested that immobile uranium was likely in its oxidized state as U(VI) on the aquifer sediments; these observations ruled out oxidation of U(IV) to U(VI) as a potential mobilization mechanism. Therefore, desorption of U(VI) appeared to be the predominant potential mobilization mechanism, yet it was clearly not solely dependent on concentration as evident when considering that uranium-poor river water (\textless0.015 mg/L) was recharged to uranium-rich groundwater (≈1 mg/L). It was possible that uranium desorption was limited by the relatively higher pH and lower alkalinity of the river water as compared to the groundwater; both factors favor immobilization. However, it was likely that the immobile uranium was associated with a mineral phase, as opposed to a sorbed phase, thus desorption may not have been possible. The results of this field tracer study successfully ruled out two common mobilization mechanisms of uranium: (1) oxidative dissolution and (2) concentration-dependent desorption and ruled in the importance of advection, dispersion, and the mineral phase of uranium. |
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0169-7722 |
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THL @ christoph.kuells @ paradis_elucidating_2022 |
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135 |
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Yabusaki, S.B.; Fang, Y.; Long, P.E.; Resch, C.T.; Peacock, A.D.; Komlos, J.; Jaffe, P.R.; Morrison, S.J.; Dayvault, R.D.; White, D.C.; Anderson, R.T. |
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Title |
Uranium removal from groundwater via in situ biostimulation: Field-scale modeling of transport and biological processes |
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Journal Article |
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Year |
2007 |
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Journal of Contaminant Hydrology |
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93 |
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1 |
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216-235 |
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Bioremediation, Biostimulation, Field experiment, Iron, Reactive transport, Sulfate, Uranium |
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During 2002 and 2003, bioremediation experiments in the unconfined aquifer of the Old Rifle UMTRA field site in western Colorado provided evidence for the immobilization of hexavalent uranium in groundwater by iron-reducing Geobacter sp. stimulated by acetate amendment. As the bioavailable Fe(III) terminal electron acceptor was depleted in the zone just downgradient of the acetate injection gallery, sulfate-reducing organisms came to dominate the microbial community. In the present study, we use multicomponent reactive transport modeling to analyze data from the 2002 field experiment to identify the dominant transport and biological processes controlling uranium mobility during biostimulation, and determine field-scale parameters for these modeled processes. The coupled process simulation approach was able to establish a quantitative characterization of the principal flow, transport, and reaction processes based on the 2002 field experiment, that could be applied without modification to describe the 2003 field experiment. Insights gained from this analysis include field-scale estimates of the bioavailable Fe(III) mineral threshold for the onset of sulfate reduction, and rates for the Fe(III), U(VI), and sulfate terminal electron accepting processes. |
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THL @ christoph.kuells @ yabusaki_uranium_2007 |
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156 |
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Hall, S.M.; Gosen, B.S.V.; Zielinski, R.A. |
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Title |
Sandstone-hosted uranium deposits of the Colorado Plateau, USA |
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Journal Article |
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2023 |
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Ore Geology Reviews |
Abbreviated Journal |
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155 |
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105353 |
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Colorado, Plateau, Uranium, Vanadium |
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More than 4,000 sandstone-hosted uranium occurrences host over 1.2 billion pounds of mined and in situ U3O8 throughout the Colorado Plateau. Most of the resources are in two distinct mineral systems with deposits hosted in the Triassic Chinle and Jurassic Morrison Formations. In the Chinle mineral system, base metal sulfides typically accompany mineralization. The Morrison mineral system is characterized by V/U ratios up to 20. The uranium source was likely volcanic ash preserved as bentonitic mudstones in the Brushy Basin Member of the Morrison Formation, and lithic volcanic clasts, ash shards, and bentonitic clay in the lower part of the Chinle Formation. Vanadium originated from two possible sources: iron–titanium oxides that are extensively altered in bleached rock near deposits or from similar minerals in variably bleached red beds interbedded with and beneath the Morrison. In Chinle-hosted deposits, in addition to volcanic ash, a contributing source of both vanadium and uranium is proposed here for the first time to be underlying red beds in the Moenkopi and Cutler Formations that have undergone a cycle of reddening-bleaching-reoxidation. Transport in both systems was likely in groundwater through the more permeable sandstones and conglomerate units. The association of uranium minerals with carbonate and more rarely apatite, suggests that transport of uranium was as a carbonate or phosphate complex. The first comprehensive examination of paleoclimate, paleotopography, and subsurface structure of aquifers coupled with analysis of the geochronology of deposits suggests that that there were distinct pulses of uranium mineralization/redistribution during the period from about 259 Ma to 12 Ma when oxidized mineralizing fluids were intermittently rejuvenated in the Plateau in response to changes in tectonic regime and climate. Multiple lines of evidence indicate that deposits formed at ambient temperatures of about 25 °C to no greater than about 140 °C. In both systems, deposits formed where groundwater flow slowed and was subject to evaporative concentration. Stagnant conditions allowed for prolonged interaction of U- and V-enriched groundwater with ferrous iron-bearing reductants, such as illite and iron–titanium oxides, and more rarely organic material such as plant debris. Paragenetically late in the sequence, reducing fluids introduced additional organic matter to some deposits. Reducing fluids and introduced organic matter (now amorphous and altered by radiolysis) may originate from regional petroleum systems where peak oil and gas generation was from ∼ 82 to ∼ 5 Ma. Our novel analysis indicates that these reducing fluids bleached rock and protected affected deposits from remobilization during exposure and weathering that followed uplift of the Plateau (∼80 to 40 Ma). |
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0169-1368 |
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THL @ christoph.kuells @ hall_sandstone-hosted_2023 |
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111 |
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Ren, Y.; Yang, X.; Hu, X.; Wei, J.; Tang, C. |
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Mineralogical and geochemical evidence for biogenic uranium mineralization in northern Songliao Basin, NE China |
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Journal Article |
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2022 |
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Ore Geology Reviews |
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141 |
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104556 |
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Bacterial sulfate reduction, In-situ S isotope of pyrite, Northern Songliao basin, Sandstone-type uranium deposit, Sifangtai Formation |
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The sandstone-hosted uranium mineralization areas in the Sanzhao Sag of the northern Songliao Basin have been newly identified. The target stratum is the Upper Cretaceous Sifangtai Formation and the uranium mineralization mainly occurs in the bottom of Sifangtai Formation, corresponding to channel sand bodies in meandering river system, characterized by medium to fine-grained sandstone. This study proposes the uranium metallogenic model through petrographic observation, whole rock geochemistry, mineralogical study of uranium occurrence form (SEM), organic matter rock–eval pyrolysis analysis (REP) and in-situ sulfur isotope determination of different generations of pyrite by LA-MC-ICP-MS. Compared with the sandstones collected in barren reduction and oxidization zones, the mineralized sandstones show obvious increase in the contents of TOC, total sulfur, Y and U. Petrographic observations indicate that organic matters are mainly inherited from land plants. REP data display that the organic matter (OM) disseminated in the sandstone has very low hydrogen index (HI) from around 0 to 21 mg HC/g TOC and varied oxygen index (OI) from 44 to 115 mg CO2/g TOC, corresponding to Type Ⅳ kerogen (degraded kerogen). There are two types of coffinite with different grain size, micro-particles (μm-sized) and large aggregates (generally up to 100 μm) respectively. The coffinite micro spherules exhibit short rod-like or worm-like morphology occurring in clay matrix and cell cavities in degradofusinite or around subidiomorphic-idiomorphic pyrite. The coarse-grained coffinite contains other mineral facies (e.g. pyrite, quartz) and some of large coffinite aggregates display thrombolite-type microbial structures. The irregular pyrite relict particles in coarse-grained colloidal coffinite have light sulfur isotope compositions characterized by δ34S values from –39.96‰ to –49.89‰. The δ34S values of colloidal pyrite in replacement of OM or of the sub-idiomorphic FeS2 cement filling in the cavities of OM range from –52.77‰ to –13.88‰. Some of sub-idiomorphic pyrite cement and idiomorphic crystal have the heavier signature from – 27.06‰ to + 14.23‰. The light sulfur isotope signature suggests that the sulfur originates from bacterial sulfate reduction (BSR). The OM replacement by pyrite and the highest OI values recorded by REP in uranium mineralized samples are lines of evidence of biodegradation. Bacteria use the organic matter as food source and produce isotopically light reduced sulfur species. Oxygenated uranium-bearing waters infiltrated through the denudated windows at Daqing placanticline into the porous reduced sandstones deposited in the Sanzhao Sag. Uranium was indirectly reduced by BSR-derived iron disulfides or directly reduced by sulfate-reducing bacteria. |
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THL @ christoph.kuells @ ren_mineralogical_2022 |
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144 |
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Rallakis, D.; Michels, R.; Cathelineau, M.; Parize, O.; Brouand, M. |
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Conditions for uranium biomineralization during the formation of the Zoovch Ovoo roll-front-type uranium deposit in East Gobi Basin, Mongolia |
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Journal Article |
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2021 |
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Ore Geology Reviews |
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138 |
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104351 |
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Bioreduction, East Gobi Basin, Mongolia, Organic matter, Roll-front, Sulfur isotopes, Uranium |
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The Zoovch Ovoo uranium roll-front-type deposit is hosted in the Sainshand Formation, a Late Cretaceous siliciclastic reservoir, which constitutes the upper part of the post-rift infilling of the Mesozoic East Gobi Basin in SE Mongolia. The Sainshand Formation consists of unconsolidated medium-grained sand, silt and clay intervals deposited in fluvial-lacustrine settings. The uranium deposit is confined within a 60–80 m thick siliciclastic sequence inside aquifer-driven systems. The overall system experienced shallow burial and was never subjected to temperatures higher than 40 °C. This study proposes a comprehensive metallogenic model for this uranium deposit. Sedimentological and mineralogical observations from drill core samples to the microscopic scale (optical and Scanning Electron Microscopy) together with in situ geochemistry of late-formed phases (Laser Ablation–Inductively Coupled Plasma Mass Spectrometry, Electron Probe Microanalysis, Fourier Transform–Infrared Spectroscopy) were considered for the reconstruction of the main stages of U trapping. In the mineralized zone, the uranium ore is expressed as Ca–enriched uraninite (UO2) and less commonly as Ca–enriched phospho-coffinite (U, P)SiO4. Trapping mechanisms include i) complexation (i.e. uranyl-carboxyl complexes), ii) adsorption on organic or clay particles) and iii) reduction by pyrite and by bacterial activity to amorphous uraninite. In all cases, the organic matter plays either the role of trap for uranium or nutrient for bacteria that can trap uranium through their metabolism. The shallow burial diagenesis conditions do not allow direct reduction of U(VI) by organic carbon. The δ34S values of the iron disulfide are very diverse, fluctuating in extreme cases between −50 to + 50‰, with an average δ34S value for framboidal pyrite at 2‰, and −20‰ for euhedral pyrite. The positive and negative values reflect close versus open fractionation systems, while bacterial sulphate reduction (BSR) is active during the whole diagenetic history of the deposit as an essential source of reduced sulfur. Therefore, using detrital organic matter as a carbon source, microorganisms play a significant role in uranium trapping, either as a direct reducing agent for uranium or pyrite formation, which will trap uranium through redox driven epigenetic processes. |
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THL @ christoph.kuells @ rallakis_conditions_2021 |
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176 |
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