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Ruiz, O.; Thomson, B.; Cerrato, J.M.; Rodriguez-Freire, L. |
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Title |
Groundwater restoration following in-situ recovery (ISR) mining of uranium |
Type |
Journal Article |
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Year |
2019 |
Publication |
Applied Geochemistry |
Abbreviated Journal |
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Volume |
109 |
Issue |
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104418 |
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Aquifer stabilization, Ground water restoration, In-situ leach mining, In-situ recovery, Uranium |
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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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THL @ christoph.kuells @ ruiz_groundwater_2019 |
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153 |
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Hofmann, H.; Pearce, J.K.; Hayes, P.; Golding, S.D.; Hall, N.; Baublys, K.A.; Raiber, M.; Suckow, A. |
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Title |
Multi-tracer approach to constrain groundwater flow and geochemical baseline assessments for CO2 sequestration in deep sedimentary basins |
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Journal Article |
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Year |
2023 |
Publication |
International Journal of Coal Geology |
Abbreviated Journal |
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104438 |
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CO geological storage, Great Artesian Basin, Groundwater chemistry, Isotopic tracer, Surat Basin |
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Geological storage of gases will be necessary in the push to net zero and the energy transition to reduce carbon emissions to atmosphere. These include CO2 geological storage in suitable sandstone reservoirs. Understanding groundwater flow, connectivity and hydrogeochemical processes in aquifer and storage systems is vital to prevent risk and protect important water resources, such as the Great Artesian Basin. Here, we provide a ‘tool-box’ of geochemical assessment methods to provide information on flow patterns through the basin’s aquifers (changes in chemistry along flow path), stagnant versus flowing conditions (cosmogenic isotopes and noble gases), inter-aquifer connectivity and seal properties (major ions, Sr and stable isotopes), water quality (major ions and metals) and general assessments on residence times of groundwater (cosmogenic isotopes and noble gases). This information can be used with reservoir and groundwater models to inform on possible changes in the above-mentioned processes and serve as input parameters for CO2 injection impact modelling. We demonstrate the use and interpretation on an example of a potential CO2 storage geological sequestration site in the Surat Basin, part of the Great Artesian Basin, and the aquifers that overly the reservoir. The stable water isotopes are depleted compared to average rainfall and most likely indicate greater contributions from monsoonal rain events from the northern monsoonal troughs, where amount and rainout effects lead to the depletion rather than colder recharge climates. This is supported by the modern recharge temperatures from noble gases. Inter-aquifer mixing between the Precipice Sandstone reservoir and the Hutton Sandstone aquifer seems unlikely as the Sr isotope ratios are distinctly different suggesting that the Evergreen Formation is a seal in the locations sampled. Mixing, however, occurs on the edges of the basin, especially in the south-east and east where the Surat Basin transitions into the Clarence-Moreton Basin. Groundwater flow appears to be to the south in the Precipice Sandstone, with a component of flow east to the Clarence-Morton Basin. The cosmogenic isotopes and noble gases strongly indicate very long residence times of groundwater in the central south Precipice Sandstone around a proposed storage site. 14C values below analytical uncertainty, R36Cl ratios at secular equilibrium as well as high He concentrations and high 40Ar/36Ar ratios support the argument that groundwater flow in this area is extremely slow or groundwater is stagnant. The results of this study reflect the geological and hydrogeological complexities of sedimentary basins and that baseline studies, such as this one, are paramount for management strategies. |
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0166-5162 |
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THL @ christoph.kuells @ hofmann_multi-tracer_2023 |
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165 |
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Christofi, C.; Bruggeman, A.; Külls, C.; Constantinou, C. |
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Title |
Hydrochemical evolution of groundwater in gabbro of the Troodos Fractured Aquifer. A comprehensive approach |
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Journal Article |
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Year |
2020 |
Publication |
Applied Geochemistry |
Abbreviated Journal |
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114 |
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104524 |
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geochemistry |
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Pergamon |
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English |
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THL @ christoph.kuells @ Christofi2020hydrochemical |
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13 |
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Ren, Y.; Yang, X.; Hu, X.; Wei, J.; Tang, C. |
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Title |
Mineralogical and geochemical evidence for biogenic uranium mineralization in northern Songliao Basin, NE China |
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Journal Article |
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Year |
2022 |
Publication |
Ore Geology Reviews |
Abbreviated Journal |
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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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0169-1368 |
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THL @ christoph.kuells @ ren_mineralogical_2022 |
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144 |
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Gardiner, J.; Thomas, R.B.; Phan, T.T.; Stuckman, M.; Wang, J.; Small, M.; Lopano, C.; Hakala, J.A. |
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Utilization of produced water baseline as a groundwater monitoring tool at a CO2-EOR site in the Permian Basin, Texas, USA |
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Journal Article |
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Year |
2020 |
Publication |
Applied Geochemistry |
Abbreviated Journal |
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121 |
Issue |
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104688 |
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CO storage, Enhanced oil recovery, Geochemical baseline, Groundwater monitoring, Produced water, Solubility trapping |
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Carbon dioxide (CO2) enhanced oil recovery (EOR) provides a pathway for economic reuse and storage of CO2, a greenhouse gas. One challenge with this practice is ensuring CO2 injection does not result in target reservoir fluids migrating into overlying shallow (\textless1000 m) groundwater formations. Effective monitoring for leakage from storage formations could involve measuring sensitive chemical indicators in overlying groundwater units and within the producing formation itself for evidence of deviation from an initial state. In this study, produced waters and overlying groundwaters were monitored over a five-year period to evaluate which geochemical signals may be useful to ensure that oilfield produced waters did not impact overlying groundwaters. During this five-year period, a mature carbonate oil reservoir in the Permian Basin transitioned from a waterflooding operation to a water-alternating-gas injection (WAG), in which the formation was flooded with CO2 and various mixtures of produced water. Significant increases in dissolved inorganic constituents [alkalinity, TDS, Na+, Cl−, SO42−] were observed in produced waters following CO2 injection; however, carbonate reservoir dissolution-precipitation reactions appear to be minimal and injected CO2 appears to be stored via solubility trapping. Although there are statistically significant geochemical variations following CO2 injection, applying isometric log-ratios to certain parameters establishes a narrow range for post-CO2 injection produced waters. This narrow range can be considered a baseline for post-CO2 injection produced waters; this baseline can be utilized to monitor overlying local groundwaters for produced water intrusion. Additionally, certain parameters [Na+, Ca2+, K+, Cl−, alkalinity, and TDS] display large concentration disparities between produced water and overlying groundwaters; these parameters would be sensitive indicators of produced water intrusion into overlying groundwaters. |
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0883-2927 |
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THL @ christoph.kuells @ gardiner_utilization_2020 |
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171 |
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Christofi, C.; Bruggeman, A.; Külls, C.; Constantinou, C. |
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Isotope hydrology and hydrogeochemical modeling of Troodos Fractured Aquifer, Cyprus: The development of hydrogeological descriptions of observed water types |
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Journal Article |
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2020 |
Publication |
Applied Geochemistry |
Abbreviated Journal |
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123 |
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104780 |
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Isotope hydrology, Hydrogeochemical modelling, Hydrochemistry, Kargiotis, Troodos |
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The origin of groundwater recharge and subsequent flow paths are often difficult to establish in fractured, multi-lithological, and highly compartmentalized aquifers such as the Troodos Fractured Aquifer (TFA). As the conjunctive use of stable isotopes and hydrogeochemical data provides additional information, we established a monitoring network for stable isotopes in precipitation in Cyprus. The local meteoric water line, altitude effect and seasonal variation of stable isotopes in precipitation are derived from monitoring data. Stable isotopes and hydrogeochemical data are combined to model water-rock interactions and groundwater evolution along a complete ophiolite sequence. As a result a generic hydrogeologic description for the observed water types is developed. Isotope hydrology was applied in conjunction with hydrogeochemical modelling in Kargiotis Watershed, a major north-south transect of the TFA. PHREEQC was used for hydrogeochemical modelling to establish generic descriptions for observed water types. Mean precipitation-weighted values from 16 monitoring stations were used to calculate the Local Meteoric Water Line (LMWL), which was found to be equal to δ2H = (6.58 ± 0.13)*δ18O + (12.64 ± 0.91). A general decrease of 1.22‰ for δ2H and 0.20‰ for δ18O in precipitation was calculated per 100 m altitude. A generic groundwater evolution path was established: 1. Na/MgClHCO3, 2. MgHCO3, 3. Ca/MgHCO3, 4. Ca/MgNaHCO3, 4a. MgNa/CaHCO3/Cl, 5. NaMg/CaHCO3/Cl, 6. NaHCO3, 7. Na/MgHCO3SO4, 8. NaSO4Cl/HCO3. Hydrogeologic descriptions, consisting of groundwater origin, flow path and possible active water-rock processes, have been realised for the observed water types. The first two water types occur in serpentine and ultramafic-gabbro springs. Type 3 waters represent early stages of recharge and/or short flow paths, in gabbro whereas types 4 and 5 are typical for further percolating waters in gabbro and diabase. Water types 6 and 7 occur both in diabase and in the basal group and represent the regional flow. Water type 8 is the end member of regional, upwelling groundwater in the basal group. The presented descriptions and methods have practical applications in groundwater exploration, characterization, and protection. The methodology can be applied in other complex aquifer systems. |
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english |
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english |
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0883-2927 |
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Cyprus |
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THL @ christoph.kuells @ Christofi2020104780 |
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76 |
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Marteleto, T. de P.; Abreu, A.E.S. de; Barbosa, M.B.; Yoshinaga-Pereira, S.; Bertolo, R.A.; Enzweiler, J. |
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Groundwater apparent ages and isotopic composition in Crystalline, Diabase and Tubarão aquifers contact area in Campinas, Southeastern Brazil |
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Journal Article |
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Year |
2024 |
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Journal of South American Earth Sciences |
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135 |
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104783 |
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Fractured aquifer, Groundwater mixing, Isotopes, Water management |
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This study refines the hydrogeological conceptual model of an area with three interconnected aquifers, namely the Crystalline Aquifer System (CAS – igneous and metamorphic rocks), which is in contact with the Tubarão Aquifer System (TAS – sedimentary rocks) and the Diabase Aquifer System (DAS – diabase rocks). The detailed investigation involved geophysical logging and hydraulic and hydrodynamic characterization with straddle packers in a local tubular well, in which groundwater presents high uranium concentrations. Hydrogeochemical and isotope (δ2H, δ18O, 3H, δ13C, 14C) analysis in this well and in other three neighboring wells, with lower U concentrations, showed that ancient and modern waters (3H from <0.8 to 1.12 TU, 14C from 69.43 to 78.72 pMC) mix within the aquifer. During groundwater pumping, vertical fractures in the diabase aquifer possibly induce water mixing and recharge of the deeper levels of the aquifers from shallow layers. The high [U] are related to ancient waters from a confined aquifer hosted in CAS that reaches the wells through hydraulically active fractures located deeper than 159 m depth. Groundwater apparent ages do not increase systematically with depth, revealing a complex circulation model for CAS. The results obtained from the other wells, which are all located on drainage lineaments, reveal that one extracts modern water from DAS and TAS, another one extracts modern and ancient water from DAS and CAS, and the third extracts only ancient water from CAS, confirming the complexity of the local hydrogeology. Regarding regional groundwater management, the study revealed the need to characterize the sources of groundwater in each well, in order to protect modern waters from anthropogenic contamination and to protect ancient groundwater from overexploitation, as CAS hosts groundwaters recharged thousands of years ago or more. |
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0895-9811 |
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THL @ christoph.kuells @ Depaulamarteleto2024104783 |
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221 |
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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 |
Publication |
Applied Geochemistry |
Abbreviated Journal |
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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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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. |
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Title |
Elevated uranium in drinking water sources in basement aquifers of southern India |
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Journal Article |
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Year |
2021 |
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Applied Geochemistry |
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133 |
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105092 |
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Anthropogenic, Drinking waters, Geogenic, India, Speciation, Uranium |
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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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THL @ christoph.kuells @ lapworth_elevated_2021 |
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147 |
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Zhou, Y.; Li, G.; Xu, L.; Liu, J.; Sun, Z.; Shi, W. |
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Uranium recovery from sandstone-type uranium deposit by acid in-situ leaching – an example from the Kujieertai |
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2020 |
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Hydrometallurgy |
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191 |
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105209 |
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Acid in-situ leaching, Sandstone-type uranium deposit, Uranium deportment in the ore, Uranium recovery, Water-rock interaction |
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The factors influencing uranium recovery in water-rock systems during acid in-situ leaching (ISL) were studied at the Kujieertai uranium deposit in Xinjiang. Using an ISL unit, a field leach trial (FLT) had been carried out to test the sequential effects of a leaching solution without oxidant (H2SO4 solution 4–8 g/L) and a leaching solution with oxidant (H2SO4 3–7 g/L, and Fe (III) 2–6 g/L). The observation of the leaching process revealed clearly defined stages of uranium release from the solid mineral to solution. Uranium mobilization from solid mineral into solution can be described in four stages. At the beginning of the acid ISL process, there was no oxidant to be added to the leaching solution and the desorption of hexavalent uranyl ions in the open pores, as well as dissolution of hexavalent uranium minerals, led to a short-term peak in the pregnant solution, which happened while pH decreased from about 5.3 to 2.62. Following the depletion of the adsorbed hexavalent uranium and a decline in uranium dissolution intensity, the addition of Fe(III) facilitated the oxidation of tetravalent uranium, which enabled intensive uranium mobilization again. During this process, the dissolution of uranium had a strong positive correlation with the reduction of Fe(III) and Eh in the leach solution. Beside hydrochemical factors, the deportment of uranium was also an important factor affecting uranium recovery. Uranium located in the open pores can be completely exposed to the solution and the mobilization intensity was significantly affected by hydrogeochemical conditions; but the uranium present in microfissures and in the ore matrix could not be fully exposed to the solution, so, their dissolution intensity was primarily controlled by corrosion and permeability of the ore. In general, the hydrogeochemical conditions and the deportment of uranium were the external and internal factors that significantly affected the dissolution and recovery of uranium in the early and middle stages of the FLT. However, in the latest stages, due to uranium depletion, enhancing the chemical potential of the leaching solution, specifically acidity and/or the amount of oxidant, had little improvement on uranium recovery. |
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THL @ christoph.kuells @ zhou_uranium_2020 |
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205 |
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