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Lartigue, J.E.; Charrasse, B.; Reile, B.; Descostes, M. |
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Title |
Aqueous inorganic uranium speciation in European stream waters from the FOREGS dataset using geochemical modelling and determination of a U bioavailability baseline |
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Journal Article |
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Year |
2020 |
Publication |
Chemosphere |
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251 |
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126302 |
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Bioavailable fraction, Geochemical mapping / baseline, Modelling, Speciation, Stream water, Uranium |
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Abstract |
The concentration of the bioavailable uranium fraction (Ubio) at the European scale was deduced by geochemical modelling considering several definitions found in the literature and the FOREGS European stream waters geochemical atlas dataset to produce a Ubio baseline. A sensitivity analysis was performed using three thermodynamic databases. We also investigated the link between total dissolved uranium (Uaq) concentrations, speciation and global stream water chemistry on the one hand, and the lithology and ages of the surrounding rocks on the other. The more U-enriched the stream sediments or rock type contexts are, which tends to be the case with rocks containing silicates (4.1 mg/kg), the less U-concentrated the stream waters are (0.15 μg/L). Sedimentary rocks lead to slightly higher Uaq concentrations (0.34 μg/L) even if the concentration in sediment (Used) is relatively low (1.6 mg/kg). This trend is reversed for Ubio, with higher concentrations in a crystalline context. The mean estimated Ubio value ranges from 1.5.10−3 to 65.3 ng/L and can fluctuate by 3 orders of magnitude depending on the considered definition as opposed to by 2 orders of magnitude accountable to differences between thermodynamic databases. The classification of the water in relation to the two surrounding rock lithologies makes it possible to reduce the mean variability for the Ubio concentrations. Irrespective of the definition of Ubio considered, in 59% of cases the Ubio fraction represents less than 1% of Uaq. Several threshold values relating to Ubio were proposed, assuming knowledge only of the aqueous concentrations of the major elements and Uaq. |
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0045-6535 |
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THL @ christoph.kuells @ lartigue_aqueous_2020 |
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141 |
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Holmes, M.; Campbell, E.E.; Wit, M. de; Taylor, J.C. |
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Title |
Can diatoms be used as a biomonitoring tool for surface and groundwater?: Towards a baseline for Karoo water |
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Journal Article |
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Year |
2023 |
Publication |
South African Journal of Botany |
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161 |
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211-221 |
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Keywords |
Bioindicator, Diatom, Hydraulic fracturing, Karoo, Water quality |
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Abstract |
The environmental risks from shale gas extraction through the unconventional method of ‘fracking’ are considerable and impact on water supplies below and above ground. Since 2010 the recovery of natural shale gas through fracking has been proposed in parts of the fragile semi-arid ecosystems that make up the Karoo biome in South Africa. These unique ecosystems are heavily reliant on underground water, intermittent and ephemeral springs, which are at great risk of contamination by fracking processes. Diatoms are present in all water bodies and reflect aspects of the environment in which they are located. As the possibility of fracking has not been removed, the aim of the project was to determine if diatoms could be used for rapid biomonitoring of underground and surface waters in the Karoo. Over a period of 24 months, water samples and diatom species were collected simultaneously from 65 sites. A total of 388 diatom taxa were identified from 290 samples with seasonal and substrate variation affecting species composition but not the environmental information. Species diversity information, on the other hand, often varied significantly between substrates within a single sample. Analysis using CCA established that the diatom composition was affected by lithium, oxidized nitrogen, electrical conductivity, and sulphate levels in the sampled water. We conclude that changes in diatom community composition in the Karoo do reflect the water chemistry and could be useful as bioindicators. |
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0254-6299 |
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THL @ christoph.kuells @ holmes_can_2023 |
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163 |
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Min, M.; Xu, H.; Chen, J.; Fayek, M. |
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Title |
Evidence of uranium biomineralization in sandstone-hosted roll-front uranium deposits, northwestern China |
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Journal Article |
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Year |
2005 |
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Ore Geology Reviews |
Abbreviated Journal |
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26 |
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3 |
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198-206 |
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Keywords |
Biomineralization, China, Roll-front uranium deposit, Sandstone |
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We show evidence that the primary uranium minerals, uraninite and coffinite, from high-grade ore samples (U3O8\textgreater0.3%) in the Wuyiyi, Wuyier, and Wuyisan sandstone-hosted roll-front uranium deposits, Xinjiang, northwestern China were biogenically precipitated and psuedomorphically replace fungi and bacteria. Uranium (VI), which was the sole electron acceptor, was likely to have been enzymically reduced. Post-mortem accumulation of uranium may have also occurred through physio-chemical interaction between uranium and negatively-charged cellular sites, and inorganic adsorption or precipitation reactions. These results suggest that microorganisms may have played a key role in formation of the sandstone- or roll-type uranium deposits, which are among the most economically significant uranium deposits in the world. |
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0169-1368 |
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THL @ christoph.kuells @ min_evidence_2005 |
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186 |
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Author |
Rajfur, M.; Kłos, A.; Wacławek, M. |
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Title |
Sorption properties of algae Spirogyra sp. and their use for determination of heavy metal ions concentrations in surface water |
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Journal Article |
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Year |
2010 |
Publication |
Bioelectrochemistry |
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80 |
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1 |
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81-86 |
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Biomonitoring, Heavy metal ions, Algae sp., Sorption kinetics, Langmuir isotherm |
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Kinetics of heavy-metal ions sorption by alga Spirogyra sp. was evaluated experimentally in the laboratory, using both the static and the dynamic approach. The metal ions – Mn2+, Cu2+, Zn2+ and Cd2+ – were sorbed from aqueous solutions of their salts. The static experiments showed that the sorption equilibria were attained in 30min, with 90-95% of metal ions sorbed in first 10min of each process. The sorption equilibria were approximated with the Langmuir isotherm model. The algae sorbed each heavy metal ions proportionally to the amount of this metal ions in solution. The experiments confirmed that after 30min of exposition to contaminated water, the concentration of heavy metal ions in the algae, which initially contained small amounts of these metal ions, increased proportionally to the concentration of metal ions in solution. The presented results can be used for elaboration of a method for classification of surface waters that complies with the legal regulations. |
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1567-5394 |
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A Selection of Papers presented at the 4th International Workshop on Surface Modification for Chemical and Biochemical Sensing (SMCBS 2009) |
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Call Number |
THL @ christoph.kuells @ Rajfur201081 |
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283 |
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Author |
Rallakis, D.; Michels, R.; Cathelineau, M.; Parize, O.; Brouand, M. |
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Title |
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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Year |
2021 |
Publication |
Ore Geology Reviews |
Abbreviated Journal |
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138 |
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Pages |
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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0169-1368 |
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THL @ christoph.kuells @ rallakis_conditions_2021 |
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176 |
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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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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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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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0169-7722 |
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THL @ christoph.kuells @ yabusaki_uranium_2007 |
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156 |
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Heine, F.; Einsiedl, F. |
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Groundwater dating with dissolved organic radiocarbon: A promising approach in carbonate aquifers |
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Journal Article |
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Year |
2021 |
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Applied Geochemistry |
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125 |
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104827 |
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C groundwater dating, deep carbonate aquifer, DOC, SPE-PPL |
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A complete hydrogeological understanding of the deep Upper Jurassic carbonate aquifer in the South German Molasse Basin is essential for the future development of this important drinking water resource and geothermally used system. Water chemistry data, δ13CDIC, 14C of the dissolved inorganic carbon (14CDIC) and stable water isotope (δ18O and δD) measurements have been used to evaluate a promising groundwater dating approach with 14C of dissolved organic carbon (14CDOC). The pre-concentration of dissolved organic matter (DOM) was performed by the easy applicable solid phase extraction (SPE) with a styrene-divinylbenzene copolymer sorbent (PPL). Based on the sampling campaign of seven groundwater wells conducted between 2017 and 2019, it was shown that the groundwater is mainly of Ca–HCO3 type with some evidence of ion exchange between Ca2+ and Na+ at two of the investigated wells. The δD values ranged from −89.4‰ to −70.9‰ while δ18O values varied between −12.5‰ and −9.8‰. The obtained stable water isotope signatures indicated that the groundwater is of meteoric origin and was recharged during warm climate (Holocene), intermediate climate and cold climate (Pleistocene) infiltration conditions. The measured 14CDOC activities varied from 5.7 pmC to 51.1 pmC and the calculated piston-flow water ages (ORAs) ranged from 4200 years to 25,248 years using an initial 14C0DOC of 85 pmC. The calculated ORAs showed a very good correlation to the infiltration temperature-sensitive δ18O values which were affirmed with noble gas infiltration temperatures for two wells after Weise et al. (1991) and were also in good accordance with the atmospheric temperature record of the northern hemisphere from Dokken et al. (2015). The results reflect a consistent hydrogeological picture of the carbonate aquifer, which also supports the applicability of the SPE-PPL method for 14CDOC dating in groundwater with a low DOC content (<1 mg/l). In contrast, 14CDIC activities of 1.4 pmC to 21.3 pmC led to geochemically corrected piston-flow ages between 8057 years and >30,000 years and generally to an overestimation of the apparent water ages. This study gives insights into the promising approach of 14CDOC groundwater dating in carbonate aquifers with low DOC contents and allows future sustainable groundwater resource management of the investigated aquifer system. |
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0883-2927 |
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THL @ christoph.kuells @ Heine2021104827 |
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216 |
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Hall, S.M.; Gosen, B.S.V.; Paces, J.B.; Zielinski, R.A.; Breit, G.N. |
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Title |
Calcrete uranium deposits in the Southern High Plains, USA |
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Journal Article |
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Year |
2019 |
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Ore Geology Reviews |
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109 |
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50-78 |
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Calcrete, Carnotite, Finchite, Geochemistry, Uranium, Vanadium |
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The Southern High Plains (SHP) is a new and emerging U.S. uranium province. Here, uranyl vanadates form deposits in Pliocene to Pleistocene sandstone, dolomite, and limestone. Fifteen calcrete uranium occurrences are identified; two of these, the Buzzard Draw and Sulfur Springs Draw deposits, have combined in-place resources estimated at about 4 million pounds of U3O8. Ore minerals carnotite and finchite are hosted in dolomite at the Sulfur Springs Draw deposit, with accessory fluorite, celestine, smectite/illite, autunite, and strontium carbonate. Host carbonate at the Sulfur Springs Draw deposit is ∼190 ka and mineralization mobilized as recently as 3.8 ka. Ash collected near the deposit is 631 ka and erupted from the Yellowstone caldera complex. The Triassic Dockum Group that contains sandstone-hosted uranium deposits throughout the region and underlies the SHP is a potential source for uranium and vanadium. Regional uplift and dissection reintroduced oxygenated groundwater into the Dockum Group, mobilizing uranium. Additional uranium may have been contributed to groundwater by weathering of volcanic ash in Pliocene and Pleistocene host rocks. The locations of the uranium occurrences are mostly in modern drainage systems in the southeast portion of the SHP. Modelling of modern groundwater in the SHP carried out in a parallel study shows that a single fluid could form carnotite through evaporation, and that fluids of the requisite composition are more prevalent in the southern portion of the SHP. The southeastern portion of the SHP hosts more uranium occurrences due to a variety of factors including (1) upward transport of groundwater and connectivity between source and host rock, (2) higher uranium and vanadium content of groundwater, (3) higher rates of groundwater recharge in this region to drive the mineralizing system, and (4) shallower groundwater facilitating surface evaporation. Ongoing erosion of host rocks challenges preservation of deposits and may limit their size. |
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0169-1368 |
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THL @ christoph.kuells @ hall_calcrete_2019 |
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124 |
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Rosen, M.R.; Burow, K.R.; Fram, M.S. |
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Anthropogenic and geologic causes of anomalously high uranium concentrations in groundwater used for drinking water supply in the southeastern San Joaquin Valley, CA |
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Journal Article |
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2019 |
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Journal of Hydrology |
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577 |
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124009 |
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California, Central Valley, Geochemistry, Groundwater San Joaquin Valley, Uranium |
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Concentrations of uranium (U) \textgreater30 µg/L in groundwater are relatively uncommon in drinking water in the United States but can be of concern in those areas where complex interactions of aquifer materials and anthropogenic alterations of the natural flow regime mobilize U. High concentrations (\textgreater30 µg/L) of U in the southeastern San Joaquin Valley, California, USA, have been detected in 24 percent of 257 domestic, irrigation, and public-supply wells sampled across an approximately 110,000 km2 area. In this study we evaluated mechanisms for mobilization of U in the San Joaquin Valley proposed in previous studies, confirming mobilization by HCO3 and refuting mobilization by NO3 and we refined our understanding of the geologic sources of U to the scale of individual alluvial fans. The location of high concentrations depends on the interactions of geological U sources from fluvial fans that originate in the Sierra Nevada to the east and seepage of irrigation water that contains high concentrations of HCO3 that leaches U from the sediments. In addition, interactions with PO4 from fertilized irrigated fields may sequester U in the aquifer. Principal component analysis of the data demonstrates that HCO3 and ions associated with high total dissolved solids in the aquifer and the percentage of agriculture near the well sampled are associated with high U concentrations. Nitrate concentrations do not appear to control release of U to the aquifer. Age dating of the groundwater and generally increasing U concentrations of the past 25 years in resampled wells where irrigation is prevalent suggests that high U concentrations are associated with younger water, indicating that irrigation of fields over the past 100 years has significantly contributed to increasing concentrations and mobilizing U. In some places, the groundwater is supersaturated with uranyl-containing minerals, as would be expected in roll front deposits. In general, the interaction of natural geological sources high in U, the anthropogenically driven addition of HCO3 and possibly phosphate fertilizer, control the location and concentration of U in each individual fluvial fan, but the addition of nitrate in fertilizer does not appear control the location of high U. These geochemical interactions are complex but can be used to determine controls on anomalously high U in alluvial aquifers. |
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0022-1694 |
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THL @ christoph.kuells @ rosen_anthropogenic_2019 |
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158 |
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Qiu, W.; Yang, Y.; Song, J.; Que, W.; Liu, Z.; Weng, H.; Wu, J.; Wu, J. |
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Title |
What chemical reaction dominates the CO2 and O2 in-situ uranium leaching?: Insights from a three-dimensional multicomponent reactive transport model at the field scale |
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Journal Article |
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2023 |
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Applied Geochemistry |
Abbreviated Journal |
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148 |
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105522 |
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Carbonate minerals, In-situ leaching (ISL) of uranium, Pyrite oxidation, Reactive transport modeling (RTM) |
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Abstract |
The complex behavior of uranium in recovery is mostly driven by water-rock interactions following lixiviant injection into ore-bearing aquifers. Significant challenges exist in exploring the geochemical processes responsible for uranium release and mobilization. Herein this study provides an illustration of a ten-year field scale CO2 and O2 in-situ leaching (ISL) process at a typical sandstone-hosted uranium deposit in northern China. We also conducte a three-dimensional (3-D) multicomponent reactive transport model to assess the effects of potential chemical reactions on uranium recovery, in particular, to focus on the role of sulfide mineral pyrite (FeS2). Numerical simulations are performed considering three potential ISL reaction pathways to determine the relative contributions to uranium release, and the results indicate that bicarbonate promotes the oxidative dissolution of uranium-bearing minerals and further accelerates the uranium leaching in a neutral geochemical system. Moreover, the presence of FeS2 exerts a strong competitive role in the uranium-bearing mineral dissolution by increasing oxygen consumption, favoring the formation of iron oxyhydroxide, and therefore causing an associated decrease in uranium recovery rates. The simulation model demonstrates that dissolution of carbonate neutralizes acidic water generated from pyrite oxidation and aqueous CO2 dissociation. In addition, the cation concentrations (i.e., Ca and Mg) are increasing in the pregnant solutions, showing that the recycling of lixiviants and kinetic dissolution of carbonate generates a larger number of dissolved Ca and Mg and inevitably triggers the secondary dolomite mineral precipitation. The findings improve our fundamental understanding of the geochemical processes in a long-term uranium ISL system and provide important environmental implications for the optimal design of uranium recovery, remediation, and risk exposure assessment. |
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0883-2927 |
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THL @ christoph.kuells @ qiu_what_2023 |
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207 |
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