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Author Kharaka, Y.; Harmon, R.; Darling, G.
Title W. Mike Edmunds (1941–2015) Type Journal Article
Year 2015 Publication Applied Geochemistry Abbreviated Journal
Volume 59 Issue Pages 225-226
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Call Number THL @ christoph.kuells @ kharaka_w_2015 Serial 103
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Author Castro, M.C.; Stute, M.; Schlosser, P.
Title Comparison of 4He ages and 14C ages in simple aquifer systems: implications for groundwater flow and chronologies Type Journal Article
Year 2000 Publication Applied Geochemistry Abbreviated Journal
Volume 15 Issue 8 Pages 1137-1167
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Abstract 4He concentrations in excess of the solubility equilibrium with the atmosphere by up to two to three orders of magnitude are observed in the Carrizo Aquifer in Texas, the Ojo Alamo and Nacimiento aquifers in the San Juan Basin, New Mexico, and the Auob Sandstone Aquifer in Namibia. A simple 4He accumulation model is applied to explain these excess 4He concentrations in terms of both in situ production and a crustal flux across the bottom layer of the aquifer. Results from the model simulations suggest variability in the 4He fluxes, ranging from 6×10−6 cm3 STP cm−2 yr−1 for the Auob Sandstone Aquifer to 3.6×10−7 cm3 STP cm−2 yr−1 for the Carrizo aquifer. For the Ojo Alamo and Nacimiento aquifers an intermediate value of 3×10−6 cm3 STP cm−2 yr−1 was estimated. The contribution of in-situ produced 4He to the measured concentrations was also estimated. This contribution is negligible for the Auob Sandstone Aquifer as compared with both the concentrations measured at the top and bottom of the aquifer for most of the pathway. In the Carrizo aquifer, in-situ produced 4He contributes 27.5% and 15.4%, to the total 4He observed at the top and bottom of the aquifer, respectively. For both aquifers of the San Juan Basin in-situ production almost entirely dominates the 4He concentrations at the top of the aquifer for most of the pathway. In contrast, the internal production is negligible as compared with the measured concentrations at the bottom of these aquifers, reaching, at most, 1.1%. The model simulations require an exponential decrease in the horizontal velocity of the water with increasing recharge distance to reproduce the distribution of 4He in these aquifers. For the Auob Sandstone Aquifer the highest range in the velocity values is obtained (25 to 0.4 m yr−1). The simulations for the Carrizo aquifer and both aquifers located in the San Juan Basin require velocities varying from 4 to 0.1 m yr−1, and from 2 to 0.3 m yr−1, respectively. For each aquifer, average permeability values were also estimated. They are generally in agreement with results obtained from pumping tests, hydrodynamic modeling and previous 14C measurements. On the basis of the results obtained by calibrating the model with the measured 4He concentrations, the mean water residence times were estimated. They agree reasonably well with 14C ages. When applied as chronologies for noble gas temperatures in the same aquifers, the calculated 4He ages allow the identification of three different climate periods similar to those previously identified using 14C ages: (1) the Holocene period (0–10 Ka BP), (2) the Last Glacial Maximum (≈18 Ka BP), and (3) the preceeding period (30–150 Ka BP).
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Call Number THL @ christoph.kuells @ castro_comparison_2000 Serial 109
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Author Khoury, H.N.; salameh, E.M.; Clark, I.D.
Title Mineralogy and origin of surficial uranium deposits hosted in travertine and calcrete from central Jordan Type Journal Article
Year 2014 Publication Applied Geochemistry Abbreviated Journal
Volume 43 Issue Pages 49-65
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Abstract Secondary uranium encrustations are hosted in thick travertine and calcrete deposits of Pleistocene–Recent age in central Jordan. The central Jordan varicolored marble and travertine are equivalent to the active metamorphic area in Maqarin, north Jordan. More than 100 samples were collected from the outcrops of the varicolored marble, travertine, calcrete, and the yellow uranium encrustations. The secondary yellow encrustations are mainly composed of uranyl vanadate complexes. Tyuyamunite Ca(UO2)2V25+O8·3(H2O)–strelkinite Na2(UO2)2V2O8·6(H2O) solid solution series are the major components and their composition reflects changes in the Ca/Na ratio in solution. Potentially, new vanadium free calcium uranate phases (restricted to the varicolored marble) were identified with CaO:UO3 ratios different from the known mineral vorlanite (CaU6+)O4. Carbon and oxygen isotope data from calcite in the varicolored marble are characterized by Rayleigh-type enrichment in light isotopes associated with release of 13C and 18O enriched CO2 by high temperature decarbonation during combustion of the bituminous marl. Stable isotope results from uranium hosted travertine and calcrete varieties exhibit a wide range in isotopic values, between decarbonated and normal sedimentary carbonate rocks. The depleted δ13C and δ18O values in the travertine are related to the kinetic reaction of atmospheric CO2 with hyperalkaline Ca(OH)2 water. The gradual enrichment of δ13C and δ18O values in the calcrete towards equilibrium with the surrounding environment is related to continuous evaporation during seasonal dry periods. Uranium mineralization in central Jordan resulted from the interplay of tectonic, climatic, hydrologic, and depositional events. The large distribution of surficial uranium occurrences hosted in travertine and calcrete deposits is related to the artesian ascending groundwater that formed extensive lakes along NNW–SSE trending depressions. Fresh groundwater moved upward through the highly fractured phosphate, bituminous marl and varicolored marble to form unusual highly alkaline water (hydroxide–sulfate type) enriched with sensitive redox elements among which were U and V.
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Call Number THL @ christoph.kuells @ khoury_mineralogy_2014 Serial 121
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Author Mühr-Ebert, E.L.; Wagner, F.; Walther, C.
Title Speciation of uranium: Compilation of a thermodynamic database and its experimental evaluation using different analytical techniques Type Journal Article
Year 2019 Publication Applied Geochemistry Abbreviated Journal
Volume 100 Issue Pages 213-222
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Abstract Environmental hazards are caused by uranium mining legacies and enhanced radioactivity in utilized groundwater and surface water resources. Knowledge of uranium speciation in these waters is essential for predicting radionuclide migration and for installing effective water purification technology. The validity of the thermodynamic data for the environmental media affected by uranium mining legacies is of utmost importance. Therefore, a comprehensive and consistent database was established according to current knowledge. The uranium data included in the database is based on the NEA TDB (Guillaumont et al., 2003) and is modified or supplemented as necessary e.g. for calcium and magnesium uranyl carbonates. The specific ion interaction theory (Brönsted, 1922) is used to estimate activity constants, which is sufficient for the considered low ionic strengths. The success of this approach was evaluated by comparative experimental investigations and model calculations (PHREEQC (Parkhurst and Appelo, 1999)) for several model systems. The waters differ in pH (2.7–9.8), uranium concentration (10−9-10−4 mol/L) and ionic strength (0.002–0.2 mol/L). We used chemical extraction experiments, ESI-Orbitrap-MS and time-resolved laser-induced fluorescence spectroscopy (TRLFS) to measure the uranium speciation. The latter method is nonintrusive and therefore does not change the chemical composition of the investigated waters. This is very important, because any change of the system under study may also change the speciation.
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Call Number THL @ christoph.kuells @ muhr-ebert_speciation_2019 Serial 142
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Author Wilson, G.B.; McNeill, G.W.
Title Noble gas recharge temperatures and the excess air component Type Journal Article
Year 1997 Publication Applied Geochemistry Abbreviated Journal
Volume 12 Issue 6 Pages 747-762
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Abstract The calculation of a groundwater recharge temperature based on the dissolved concentrations of Ne, Ar, Kr and Xe requires a correction for noble gas supersaturation due to excess air entrainment. This entrainment is commonly attributed to the recharge process or to air contamination at the wellhead during sample collection. With the exception of some local studies, most work has concentrated on interpretation of the recharge temperature or quantification of the radiogenic content for palaeoclimatic and dating purposes. The magnitude and source of the excess air is not directly relevant to these studies and so is often ignored. In this work, excess air Ne and other data have been calculated from new and published noble gas data sets for several groundwater systems. For younger groundwaters which have been recharged under one broad climatic regime, the amount of air entrainment increases according to lithology in the order granites, sandstones and limestones respectively. A negative correlation between precipitation and excess air entrainment is identified in at least one aquifer, and some of the mechanisms which may influence the entrainment process are discussed.
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Call Number THL @ christoph.kuells @ Wilson1997747 Serial 281
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Author Priestley, S.C.; Payne, T.E.; Harrison, J.J.; Post, V.E.A.; Shand, P.; Love, A.J.; Wohling, D.L.
Title Use of U-isotopes in exploring groundwater flow and inter-aquifer leakage in the south-western margin of the Great Artesian Basin and Arckaringa Basin, central Australia Type Journal Article
Year 2018 Publication Applied Geochemistry Abbreviated Journal
Volume 98 Issue Pages 331-344
Keywords (up) Activity ratios, Central Australia, Great Artesian Basin, Hydrogeology, Sequential extraction, Uranium isotopes
Abstract The distribution of uranium isotopes (238U and 234U) in groundwaters of the south-western margin of the Great Artesian Basin (GAB), Australia, and underlying Arckaringa Basin were examined using groundwater samples and a sequential extraction of aquifer sediments. Rock weathering, the geochemical environment and α-recoil of daughter products control the 238U and 234U isotope distributions giving rise to large spatial variations. Generally, the shallowest aquifer (J aquifer) contains groundwater with higher 238U activity concentrations and 234U/238U activity ratios close to secular equilibrium. However, the source input of uranium is spatially variable as intermittent recharge from ephemeral rivers passes through rocks that have already undergone extensive weathering and contain low 238U activity concentrations. Other locations in the J aquifer that receive little or no recharge contain higher 238U activity concentrations because uranium from localised uranium-rich rocks have been leached into solution and the geochemical environment allows the uranium to be kept in solution. The geochemical conditions of the deeper aquifers generally result in lower 238U activity concentrations in the groundwater accompanied by higher 234U/238U activity ratios. The sequential extraction of aquifer sediments showed that α-recoil of 234U from the solid mineral phases into the groundwater, rather than dissolution of, or exchange with the groundwater accessible minerals in the aquifer, caused enrichment of groundwater 234U/238U activity ratios in the Boorthanna Formation. Decay of 238U in uranium-rich coatings on J aquifer sediments caused resistant phase 234U/238U activity ratio enrichment. The groundwater 234U/238U activity ratio is dependent on groundwater residence time or flow rate, depending on the flow path trajectory. Thus, uranium isotope variations confirmed earlier groundwater flow interpretations based on other tracers; however, spatial heterogeneity, and the lack of clear regional correlations, made it difficult to identify recharge and inter-aquifer leakage.
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Call Number THL @ christoph.kuells @ priestley_use_2018 Serial 115
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Author Lapworth, D.J.; Brauns, B.; Chattopadhyay, S.; Gooddy, D.C.; Loveless, S.E.; MacDonald, A.M.; McKenzie, A.A.; Muddu, S.; Nara, S.N.V.
Title Elevated uranium in drinking water sources in basement aquifers of southern India Type Journal Article
Year 2021 Publication Applied Geochemistry Abbreviated Journal
Volume 133 Issue Pages 105092
Keywords (up) Anthropogenic, Drinking waters, Geogenic, India, Speciation, Uranium
Abstract Groundwater resources in the crystalline basement complex of India are crucial for supplying drinking water in both rural and urban settings. Groundwater depletion is recognised as a challenge across parts of India due to over-abstraction, but groundwater quality constraints are perhaps even more widespread and often overlooked at the local scale. Uranium contamination in basement aquifers has been reported in many parts of India, locally exceeding WHO drinking water guideline values of 30 μg/L and posing a potential health risk. In this study 130 water samples were collected across three crystalline basement catchments to assess hydrochemical, geological and anthropogenic controls on uranium mobility and occurrence in drinking water sources. Groundwaters with uranium concentrations exceeding 30 μg/L were found in all three study catchments (30% of samples overall), with concentrations up to 589 μg/L detected. There appears to be a geological control on the occurrence of uranium in groundwater with the granitic gneiss of the Halli and Bengaluru study areas having higher mean uranium concentrations (51 and 68 μg/L respectively) compared to the sheared gneiss of the Berambadi catchment (6.4 μg/L). Uranium – nitrate relationships indicate that fertiliser sources are not a major control on uranium occurrence in these case studies which include two catchments with a long legacy of intense agricultural land use. Geochemical modelling confirmed uranium speciation was dominated by uranyl carbonate species, particularly ternary complexes with calcium, consistent with uranium mobility being affected by redox controls and the presence of carbonates. Urban leakage in Bengaluru led to low pH and low bicarbonate groundwater hydrochemistry, reducing uranium mobility and altering uranium speciation. Since the majority of inhabitants in Karnataka depend on groundwater abstraction from basement aquifers for drinking water and domestic use, exposure to elevated uranium is a public health concern. Improved monitoring, understanding and treatment of high uranium drinking water sources in this region is essential to safeguard public health.
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Call Number THL @ christoph.kuells @ lapworth_elevated_2021 Serial 147
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Author Ruiz, O.; Thomson, B.; Cerrato, J.M.; Rodriguez-Freire, L.
Title Groundwater restoration following in-situ recovery (ISR) mining of uranium Type Journal Article
Year 2019 Publication Applied Geochemistry Abbreviated Journal
Volume 109 Issue Pages 104418
Keywords (up) Aquifer stabilization, Ground water restoration, In-situ leach mining, In-situ recovery, Uranium
Abstract From 1950 through the early 1980’s New Mexico accounted for roughly half of domestic uranium (U) production for the nuclear power industry and the nation’s weapon programs. Increased interest in nuclear energy has led to proposals for renewed development using both underground mining and uranium in situ recovery (ISR). When feasible, ISR greatly reduces waste generated by the mining and milling processes, however, the ability to restore ground water to acceptable quality after ISR ends is uncertain. This research investigated two methods of stabilizing an aquifer following ISR. Batch and column studies were performed to evaluate chemical and biological methods of stabilization. Columns packed with ore were first leached with an aerated NaHCO3 ground water solution to simulate ISR. Constituents present at elevated concentrations after leaching included molybdenum (Mo), selenium (Se), U, and vanadium (V). Chemical stabilization was studied by passing a phosphate (PO43-) amended solution through the ore to achieve passivation of mineral surfaces by P precipitates. Microbial stabilization was studied by passing a lactate solution through the ore to stimulate growth of anaerobic metal- and sulfate-reducing organisms to reduce U and other elements to less soluble phases. Analyses of the solids from the columns after completion of these experiments by X-ray photo electron spectroscopy (XPS) identified phosphate on samples near the column inlet of the chemically stabilized columns. Microbial populations were characterized by Illumina DNA sequencing and confirmed the presence of metal- and sulfate-reducing organisms. Neither chemical nor microbial stabilization method achieved contaminant immobilization, which is believed due to limited mixing of the stabilization solutions with the contaminated leach solutions. These results emphasize that ground water hydrodynamics, especially mixing, must be considered in aquifer restoration of soluble constituents.
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Call Number THL @ christoph.kuells @ ruiz_groundwater_2019 Serial 153
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Author Heine, F.; Einsiedl, F.
Title Groundwater dating with dissolved organic radiocarbon: A promising approach in carbonate aquifers Type Journal Article
Year 2021 Publication Applied Geochemistry Abbreviated Journal
Volume 125 Issue Pages 104827
Keywords (up) C groundwater dating, deep carbonate aquifer, DOC, SPE-PPL
Abstract 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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Call Number THL @ christoph.kuells @ Heine2021104827 Serial 216
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Author Qiu, W.; Yang, Y.; Song, J.; Que, W.; Liu, Z.; Weng, H.; Wu, J.; Wu, J.
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 Type Journal Article
Year 2023 Publication Applied Geochemistry Abbreviated Journal
Volume 148 Issue Pages 105522
Keywords (up) Carbonate minerals, In-situ leaching (ISL) of uranium, Pyrite oxidation, Reactive transport modeling (RTM)
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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Call Number THL @ christoph.kuells @ qiu_what_2023 Serial 207
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