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Qiu, W.; Yang, Y.; Song, J.; Que, W.; Liu, Z.; Weng, H.; Wu, J.; Wu, J. |
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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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Year |
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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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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THL @ christoph.kuells @ qiu_what_2023 |
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207 |
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Robin, V.; Beaufort, D.; Tertre, E.; Reinholdt, M.; Fromaget, M.; Forestier, S.; Boissezon, H. de; Descostes, M. |
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Title |
Fate of dioctahedral smectites in uranium roll front deposits exploited by acidic In Situ Recovery (ISR) solutions |
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Journal Article |
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Year |
2020 |
Publication |
Applied Clay Science |
Abbreviated Journal |
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Volume |
187 |
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Pages |
105484 |
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Dissolution, In situ recovery, Ion exchange, Post mining, Remediation, Smectite |
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In Situ Recovery (ISR) is the most important process of uranium production in the world (50%). It consists of an injection of a leaching solution into a permeable mineralized aquifer (sandstone), pumping of the solution after dissolution of the ore minerals and recovery of the uranium from the pregnant solution in a surface plant. In this context, the fate of swelling clay minerals such as smectites is of main importance due to their role in the mobility of cationic elements by diverse geochemical processes such as ion-exchange reactions or dissolution. The present study details analysis of dioctahedral smectites before and after in-situ leaching by acidic (H2SO4) ISR solutions. Samples were collected from two sedimentary basins hosting some of the main uranium roll front deposits exploited by acidic ISR (Tortkuduk deposit, Shu-Saryssu basin, Kazakhstan, and Dulaan Uul and Zoovch Ovoo deposits, Sainshand basin, Mongolia). Scanning Electron Microscope and X-Ray Diffraction analysis revealed that dioctahedral smectite is a ubiquitous mineral in all analyzed samples, before and after acidification, and revealed a difference of crystal chemistry of the smectites between deposits of Kazakhstan (beidellite type) and Mongolia (montmorillonite type). Chemical analysis and semi-quantification of the smectites before and after acidification also revealed a difference in chemical reactivity, with a higher dissolution of montmorillonite layers compared to beidellite ones, and the importance of ion-exchange reactions. These findings are consistent with literature data obtained on model systems. The persistence of dioctahedral smectites after several years of acidification is crucial for the understanding of geochemical processes during uranium production or remediation of the aquifers. Finally, based on the analysis of samples from U-deposits hosted in both sedimentary basins, a schematic model of the impact of acid solutions on dioctahedral smectite was proposed. |
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0169-1317 |
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THL @ christoph.kuells @ robin_fate_2020 |
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179 |
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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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Year |
2023 |
Publication |
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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Zhou, Y.; Li, G.; Xu, L.; Liu, J.; Sun, Z.; Shi, W. |
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Title |
Uranium recovery from sandstone-type uranium deposit by acid in-situ leaching – an example from the Kujieertai |
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Journal Article |
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Year |
2020 |
Publication |
Hydrometallurgy |
Abbreviated Journal |
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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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0304-386x |
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THL @ christoph.kuells @ zhou_uranium_2020 |
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205 |
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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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Elevated uranium in drinking water sources in basement aquifers of southern India |
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Journal Article |
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Year |
2021 |
Publication |
Applied Geochemistry |
Abbreviated Journal |
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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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0883-2927 |
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THL @ christoph.kuells @ lapworth_elevated_2021 |
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147 |
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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 |
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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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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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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2020 |
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Applied Geochemistry |
Abbreviated Journal |
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121 |
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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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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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Year |
2022 |
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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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THL @ christoph.kuells @ ren_mineralogical_2022 |
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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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Multi-tracer approach to constrain groundwater flow and geochemical baseline assessments for CO2 sequestration in deep sedimentary basins |
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2023 |
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International Journal of Coal Geology |
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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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THL @ christoph.kuells @ hofmann_multi-tracer_2023 |
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