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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 |
Publication |
Applied Geochemistry |
Abbreviated Journal |
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Volume |
133 |
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Pages |
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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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 |
Abbreviated Journal |
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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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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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Lawrinenko, M.; Kurwadkar, S.; Wilkin, R.T. |
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Long-term performance evaluation of zero-valent iron amended permeable reactive barriers for groundwater remediation – A mechanistic approach |
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Journal Article |
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Year |
2023 |
Publication |
Geoscience Frontiers |
Abbreviated Journal |
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14 |
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2 |
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101494 |
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Geochemistry, Iron, Permeable reactive barrier, Plating reactions, Reduction potential, Surface passivation |
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Permeable reactive barriers (PRBs) are used for groundwater remediation at contaminated sites worldwide. This technology has been efficient at appropriate sites for treating organic and inorganic contaminants using zero-valent iron (ZVI) as a reductant and as a reactive material. Continued development of the technology over the years suggests that a robust understanding of PRB performance and the mechanisms involved is still lacking. Conflicting information in the scientific literature downplays the critical role of ZVI corrosion in the remediation of various organic and inorganic pollutants. Additionally, there is a lack of information on how different mechanisms act in tandem to affect ZVI-groundwater systems through time. In this review paper, we describe the underlying mechanisms of PRB performance and remove isolated misconceptions. We discuss the primary mechanisms of ZVI transformation and aging in PRBs and the role of iron corrosion products. We review numerous sites to reinforce our understanding of the interactions between groundwater contaminants and ZVI and the authigenic minerals that form within PRBs. Our findings show that ZVI corrosion products and mineral precipitates play critical roles in the long-term performance of PRBs by influencing the reactivity of ZVI. Pore occlusion by mineral precipitates occurs at the influent side of PRBs and is enhanced by dissolved oxygen and groundwater rich in dissolved solids and high alkalinity, which negatively impacts hydraulic conductivity, allowing contaminants to potentially bypass the treatment zone. Further development of site characterization tools and models is needed to support effective PRB designs for groundwater remediation. |
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1674-9871 |
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THL @ christoph.kuells @ lawrinenko_long-term_2023 |
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143 |
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Li, J.; Pang, Z.; Liu, Y.; Hu, S.; Jiang, W.; Tian, L.; Yang, G.; Jiang, Y.; Jiao, X.; Tian, J. |
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Changes in groundwater dynamics and geochemical evolution induced by drainage reorganization: Evidence from 81Kr and 36Cl dating of geothermal water in the Weihe Basin of China |
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Journal Article |
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2023 |
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Earth and Planetary Science Letters |
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623 |
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118425 |
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Kr dating, Cl dating, Geothermal water, Groundwater dynamics, Weihe basin |
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81Kr and 36Cl can both be used to date groundwater beyond the dating range of 14C. 81Kr usually provides reliable groundwater ages because it has uniform initial distribution and negligible subsurface generation, while 36Cl is commonly influenced by subsurface sources or “dead” chloride dissolution. Therefore, the combined use of 81Kr and 36Cl could provide clues on the evolution history of groundwater. In the present study, we performed 36Cl and 81Kr dating of geothermal water in Weihe Basin of China and interpreted the possible cause of disagreement. Two distinct water masses were identified with distinctive isotopic signals: groundwater with significant δ18O shifts (up to −2.0‰), dissolved dead Cl and ages < 1.0 Ma (Cluster A), and older water with little δ18O shifts, negligible dissolved Cl and ages >1.0 Ma (Cluster B). The results confirm the eastward flow path of Cluster B to the Ancient Sanmen Lake with an increasing trend of Cl concentration and age. Modern recharge from the mountains flows to the basin center with intense interaction between water and carbonate under respective reservoir temperatures (100 ∼ 130 °C). These waters flow through the saline stratum emerging from the spillover of the Ancient Sanmen Lake, resulting in higher dead Cl dissolution. A significant linear relationship is observed with the older end-member of ∼1.3Ma under the topographically-driven faster circulation effect. 81Kr ages seem to support the hypothesis that the birth of the modern Yellow River was at about 1.0–1.3 Ma. We inferred the drainage reorganization from the Ancient Sanmen Lake to the modern Yellow River since the Mid-Pleistocene Transition induced the change in groundwater dynamics as well as its chemical evolution. The excavation of the Ancient Sanmen Lake and the accentuated incision of the Weihe River induced groundwater gradient, and therefore the recharge from precipitation from both slopes of the Qinling Mountains in the south and the Beishan Mountains in the north. Our results highlight the effects of dead Cl on 36Cl dating and demonstrate the significant impact of catchment reorganization on groundwater dynamics and its chemistry. |
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0012-821x |
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THL @ christoph.kuells @ Li2023118425 |
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212 |
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Liesch, T.; Hinrichsen, S.; Goldscheider, N. |
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Uranium in groundwater — Fertilizers versus geogenic sources |
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Journal Article |
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2015 |
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Science of The Total Environment |
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536 |
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981-995 |
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Drinking water, Fertilizer, Geogenic background, Groundwater, Uranium |
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Due to its radiological and toxicological properties even at low concentration levels, uranium is increasingly recognized as relevant contaminant in drinking water from aquifers. Uranium originates from different sources, including natural or geogenic, mining and industrial activities, and fertilizers in agriculture. The goal of this study was to obtain insights into the origin of uranium in groundwater while differentiating between geogenic sources and fertilizers. A literature review concerning the sources and geochemical processes affecting the occurrence and distribution of uranium in the lithosphere, pedosphere and hydrosphere provided the background for the evaluation of data on uranium in groundwater at regional scale. The state of Baden-Württemberg, Germany, was selected for this study, because of its hydrogeological and land-use diversity, and for reasons of data availability. Uranium and other parameters from N=1935 groundwater monitoring sites were analyzed statistically and geospatially. Results show that (i) 1.6% of all water samples exceed the German legal limit for drinking water (10μg/L); (ii) The range and spatial distribution of uranium and occasional peak values seem to be related to geogenic sources; (iii) There is a clear relation between agricultural land-use and low-level uranium concentrations, indicating that fertilizers generate a measurable but low background of uranium in groundwater. |
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0048-9697 |
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THL @ christoph.kuells @ liesch_uranium_2015 |
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145 |
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Lightfoot, D.R. |
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Moroccan khettara: Traditional irrigation and progressive desiccation |
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1996 |
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Geoforum |
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27 |
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2 |
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261-273 |
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A 300 km network of khettara (qanat) subsurface irrigation channels was excavated in the Tafilalt basin beginning in the late 14th century. More than 75 of these chains provided perennial water following the breakup of the ancient city of Sijilmassa. Khettara continued to function for much of the northern oasis until the early 1970s, when new technologies and government policies forced changes. Data on origins, maintenance, and current use were collected from archival sources, aerial photographs, Landsat imagery, and from interviews. Insufficient water resources and unsustainable practices have dramatically lowered the water table, drying up khettara. This has resulted in a loss of local control over water resources, abandonment of a sustainable irrigation system, and progressive desiccation. |
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0016-7185 |
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THL @ christoph.kuells @ Lightfoot1996261 |
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257 |
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Lima, G.F.C.; Filho, C.A. de C.; Ferreira, V.G.; Lima, J. da S.D.; Marques, E.D.; Minardi, P.S.P.; Dalmázio, I.; Moreira, R.M. |
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Establishing a water baseline for the unconventional gas industry: A multiple environmental isotopes assessment (18O, 2H, 3H, 13C, and 14C) of surface and groundwater in the São Francisco Basin, Brazil |
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Journal Article |
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2023 |
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Applied Geochemistry |
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159 |
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105818 |
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Fracking, Groundwater dating, Indaiá river, Isotopes assessment, Shale gas, Unconventional hydrocarbons |
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Unconventional hydrocarbon production has become the target of an intensive environmental debate due to the risks it poses to water resources. Fracking, while enabling the extraction of oil and gas from ultra-low permeability reservoirs, also possesses the risk of polluting water systems through failures from hydraulic fracturing and its associated procedures. The need to foster national industrial development with a transitional energy matrix has led Brazil to discuss the environmental suitability before producing its large unconventional reserves. Many studies have highlighted the need for a robust environmental characterization before the development of the unconventional industry. In this sense, multiple environmental isotopes may work as a proxy for identifying water contamination right from the early stages. Environmental isotopes may also be applied to enhance the understanding of the natural geochemical processes intrinsic to a given area. This study presents an environmental isotopes baseline for the groundwater and riverine water systems within the São Francisco Basin, a proven tight gas reservoir in Brazil, in a pre-operational context. δ18O, δ2H, 3H, δ13C, and Δ14C were evaluated in three different seasons in groundwater and surface water samples, along with other auxiliary parameters such as physical-chemical parameters (in situ), major ions, and d-excess. The δ2H and δ18O in surface water shows an upstream → downstream enrichment trend, with some variations suggesting baseflow interactions in the surface water systems. An evaporation line for the study area was defined as δ2H = 4.6903 δ18O + 10.362. δ13C indicates a mutual dissolution of silicates and carbonates in the groundwater system and suggests a group of samples highly related to the recharge areas. Groundwater dating denotes the Serra da Saudade Formation as a modern fractured aquifer with a strong recharge capacity. These findings support stakeholders in environmental monitoring and management of the unconventional gas industry. |
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0883-2927 |
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THL @ christoph.kuells @ lima_establishing_2023 |
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173 |
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Lim, S.; Chase, B.M.; Chevalier, M.; Reimer, P.J. |
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50,000years of vegetation and climate change in the southern Namib Desert, Pella, South Africa |
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Journal Article |
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2016 |
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Palaeogeography, Palaeoclimatology, Palaeoecology |
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451 |
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197-209 |
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Climate reconstruction, Late Quaternary, Namib Desert, Pollen, Rock hyrax middens, South Africa |
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This paper presents the first continuous pollen record from the southern Namib Desert spanning the last 50,000years. Obtained from rock hyrax middens found near the town of Pella, South Africa, these data are used to reconstruct vegetation change and quantitative estimates of temperature and aridity. Results indicate that the last glacial period was characterised by increased water availability at the site relative to the Holocene. Changes in temperature and potential evapotranspiration appear to have played a significant role in determining the hydrologic balance. The record can be considered in two sections: 1) the last glacial period, when low temperatures favoured the development of more mesic Nama-Karoo vegetation at the site, with periods of increased humidity concurrent with increased coastal upwelling, both responding to lower global/regional temperatures; and 2) the Holocene, during which time high temperatures and potential evapotranspiration resulted in increased aridity and an expansion of the Desert Biome. During this latter period, increases in upwelling intensity created drier conditions at the site. Considered in the context of discussions of forcing mechanisms of regional climate change and environmental dynamics, the results from Pella stand in clear contrast with many inferences of terrestrial environmental change derived from regional marine records. Observations of a strong precessional signal and interpretations of increased humidity during phases of high local summer insolation in the marine records are not consistent with the data from Pella. Similarly, while high percentages of Restionaceae pollen has been observed in marine sediments during the last glacial period, they do not exceed 1% of the assemblage from Pella, indicating that no significant expansion of the Fynbos Biome has occurred during the last 50,000years. These findings pose interesting questions regarding the nature of environmental change in southwestern Africa, and the significance of the diverse records that have been obtained from the region. |
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0031-0182 |
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THL @ christoph.kuells @ lim_50000years_2016 |
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107 |
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Liu, Z.; Tan, K.; Li, C.; Li, Y.; Zhang, C.; Song, J.; Liu, L. |
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Geochemical and S isotopic studies of pollutant evolution in groundwater after acid in situ leaching in a uranium mine area in Xinjiang |
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Journal Article |
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2023 |
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Nuclear Engineering and Technology |
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55 |
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4 |
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1476-1484 |
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Acid in situ leaching of uranium, Pollution evolution, Sulfate elimination, Sulfur isotopes analysis |
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Laboratory experiments and point monitoring of reservoir sediments have proven that stable sulfate reduction (SSR) can lower the concentrations of toxic metals and sulfate in acidic groundwater for a long time. Here, we hypothesize that SSR occurred during in situ leaching after uranium mining, which can impact the fate of acid groundwater in an entire region. To test this, we applied a sulfur isotope fractionation method to analyze the mechanism for natural attenuation of contaminated groundwater produced by acid in situ leaching of uranium (Xinjiang, China). The results showed that δ34S increased over time after the cessation of uranium mining, and natural attenuation caused considerable, area-scale immobilization of sulfur corresponding to retention levels of 5.3%–48.3% while simultaneously decreasing the concentration of uranium. Isotopic evidence for SSR in the area, together with evidence for changes of pollutant concentrations, suggest that area-scale SSR is most likely also important at other acid mining sites for uranium, where retention of acid groundwater may be strengthened through natural attenuation. To recapitulate, the sulfur isotope fractionation method constitutes a relatively accurate tool for quantification of spatiotemporal trends for groundwater during migration and transformation resulting from acid in situ leaching of uranium in northern China. |
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1738-5733 |
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THL @ christoph.kuells @ liu_geochemical_2023 |
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192 |
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Liu, Z.; Li, C.; Tan, K.; Li, Y.; Tan, W.; Li, X.; Zhang, C.; Meng, S.; Liu, L. |
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Study of natural attenuation after acid in situ leaching of uranium mines using isotope fractionation and geochemical data |
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Journal Article |
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2023 |
Publication |
Science of The Total Environment |
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865 |
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161033 |
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Acid in situ leaching, Geochemical and isotopic tracing, Groundwater contamination, Natural attenuation, Uranium post-mining |
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Acid in situ leaching (AISL) is a subsurface mining approach suitable for low-grade ores which does not generate tailings, and has been adopted widely in uranium mining. However, this technique causes an extremely high concentration of contaminants at post-mining sites and in the surroundings soon after the mining ceases. As a potential AISL remediation strategy, natural attenuation has not been studied in detail. To address this problem, groundwater collected from 26 wells located within, adjacent, upgradient, and downgradient of a post-mining site were chosen to analyze the fate of U(VI), SO42−, δ34S, and δ238U, to reveal the main mechanisms governing the migration and attenuation of the dominant contaminants and the spatio-temporal evolutions of contaminants in the confined aquifer of the post-mining site. The δ238U values vary from −0.07 ‰ to 0.09 ‰ in the post-mining site and from −1.43 ‰ to 0.03 ‰ around the post-mining site. The δ34S values were found to vary from 3.3 ‰ to 6.2 ‰ in the post-mining site and from 6.0 ‰ to 11.0 ‰ around the post-mining site. Detailed analysis suggests that there are large differences between the range of isotopic composition variation and the range of pollutants concentration distribution, and the estimated Rayleigh isotope fractionation factor is 0.9994–0.9997 for uranium and 1.0032–1.0061 for sulfur. The isotope ratio of uranium and sulfur can be used to deduce the migration history of the contaminants and the irreversibility of the natural attenuation process in the anoxic confined aquifer. Combining the isotopic fractionation data for U and S with the concentrations of uranium and sulfate improved the accuracy of understanding of reducing conditions along the flow path. The study also indicated that as long as the geological conditions are favorable for redox reactions, natural attenuation could be used as a cost-effective remediation scheme. |
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0048-9697 |
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THL @ christoph.kuells @ liu_study_2023 |
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155 |
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