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Qiu, W.; Yang, Y.; Song, J.; Que, W.; Liu, Z.; Weng, H.; Wu, J.; Wu, J. |
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Title |
What chemical reaction dominates the CO2 and O2 in-situ uranium leaching?: Insights from a three-dimensional multicomponent reactive transport model at the field scale |
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Journal Article |
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Year |
2023 |
Publication |
Applied Geochemistry |
Abbreviated Journal |
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Volume |
148 |
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105522 |
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Keywords |
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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0883-2927 |
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THL @ christoph.kuells @ qiu_what_2023 |
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207 |
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Smedley, P.L.; Bearcock, J.M.; Ward, R.S.; Crewdson, E.; Bowes, M.J.; Darling, W.G.; Smith, A.C. |
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Title |
Monitoring of methane in groundwater from the Vale of Pickering, UK: Temporal variability and source discrimination |
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Journal Article |
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Year |
2023 |
Publication |
Chemical Geology |
Abbreviated Journal |
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636 |
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121640 |
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Keywords |
Aquifer, Biogenic, Ethane, Hydrocarbons, Methane, Shale gas |
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Groundwater abstracted from aquifers in the Vale of Pickering, North Yorkshire, UK and monitored over the period 2015–2022, shows evidence of variable but commonly high concentrations of dissolved CH4. Sampled groundwater from the Jurassic organic-rich Kimmeridge Clay Formation (boreholes up to 180 m depth) has concentrations up to 57 mg/L, and concentrations up to 59 mg/L are found in groundwater from underlying confined Corallian Group limestone (borehole depths 50–227 m). The high concentrations are mainly from boreholes in the central parts of the vale. Small concentrations of ethane (C2H6, up to 800 μg/L) have been found in the Kimmeridge Clay and confined Corallian groundwaters, and of propane (C3H8, up to 160 μg/L) in deeper boreholes (110–180 m) from these formations. The concentrations are typically higher in groundwater from the deeper boreholes and vary with hydrostatic pressure, reflecting the pressure control on CH4 solubility. The occurrences contrast with groundwater from shallow Quaternary superficial deposits which have low CH4 concentrations (up to 0.39 mg/L), and with the unconfined and semi-confined sections of the Corallian aquifer (up to 0.7 mg/L) around the margins of the vale. Groundwater from the Quaternary, Kimmeridge Clay formations and to a small extent the confined Corallian aquifer, supports local private-water supplies, that from the peripheral unconfined sections of Corallian also supports public supply for towns and villages across the region. Dissolved methane/ethane (C1/C2) ratios and stable-isotopic compositions (δ13C-CH4, δ2H-CH4 and δ13C-CO2) suggest that the high-CH4 groundwater from both the Kimmeridge Clay and confined Corallian formations derives overwhelmingly from biogenic reactions, the methanogenesis pathway by CO2 reduction. A small minority of groundwater samples shows a more enriched δ13C-CH4 composition (−50 to −44 ‰) which has been interpreted as due to anaerobic or aerobic methylotrophic oxidation in situ or post-sampling oxidation, rather than derivation by a thermogenic route. Few of the existing groundwater sites are proximal to abandoned or disused conventional hydrocarbon wells that exist in the region, and little evidence has been found for an influence on groundwater dissolved gases from these sites. The Vale of Pickering has also been under recent consideration for development of an unconventional hydrocarbon (shale-gas) resource. In this context, the monitoring of dissolved gases has been an important step in establishing the high-CH4 baseline of groundwaters from Jurassic deposits in the region and in apportioning their sources and mechanisms of genesis. |
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0009-2541 |
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THL @ christoph.kuells @ smedley_monitoring_2023 |
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172 |
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Veerasamy, N.; Kasar, S.; Murugan, R.; Inoue, K.; Natarajan, T.; Ramola, R.C.; Fukushi, M.; Sahoo, S.K. |
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234U/238U disequilibrium and 235U/238U ratios measured using MC-ICP-MS in natural high background radiation area soils to understand the fate of uranium |
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Journal Article |
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2023 |
Publication |
Chemosphere |
Abbreviated Journal |
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323 |
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138217 |
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HBRA, MC-ICP-MS, Monazites, U/U, Uranium |
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The Chhatrapur-Gopalpur coastal area in Odisha, India is a well-known natural high background radiation (HBRA) area due to the abundance of monazite (a thorium bearing radioactive mineral) in beach sands and soils. Recent studies on Chhatrapur-Gopalpur HBRA groundwater have reported high concentrations of uranium and its decay products. Therefore, the soils of the Chhatrapur-Gopalpur HBRA are reasonably suspected as the sources of these high uranium concentrations in groundwater. In this report, first the uranium concentrations in soil samples were measured using inductively coupled plasma mass spectrometry (ICP-MS) and they were found to range from 0.61 ± 0.01 to 38.59 ± 0.16 mg kg−1. Next, the 234U/238U and 235U/238U isotope ratios were measured to establish a baseline for the first time in Chhatrapur-Gopalpur HBRA soil. Multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) was used for measurement of these isotope ratios. The 235U/238U ratio was observed to be the normal terrestrial value. The 234U/238U activity ratio, was calculated to understand the secular equilibrium between 234U and 238U in soil and it varied from 0.959 to 1.070. To understand the dynamics of uranium in HBRA soil, physico-chemical characteristics of soil were correlated with uranium isotope ratios and this correlation of 234U/238U activity ratio indicated the leaching of 234U from Odisha HBRA soil. |
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0045-6535 |
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THL @ christoph.kuells @ veerasamy_234u238u_2023 |
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149 |
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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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Year |
2023 |
Publication |
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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Mekuria, W.; Tegegne, D. |
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Water harvesting |
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Book Chapter |
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2023 |
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Encyclopedia of Soils in the Environment (Second Edition) |
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593-607 |
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Climate change, Ecosystem services, Environmental benefits, Population growth, Resilient community, Resilient environment, Socio-economic benefits, Urbanizations, Water harvesting, Water quality, Water security |
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Water harvesting is the intentional collection and concentration of rainwater and runoff to offset irrigation demands. Secondary benefits include decreased flood and erosion risk. Water harvesting techniques include micro- and macro-catchment systems, floodwater harvesting, and rooftop and groundwater harvesting. The techniques vary with catchment type and size, and the method of water storage. Micro-catchment water harvesting, for example, requires the development of small structures and targets increased water delivery and storage to the root zone whereas macro-catchment systems collect runoff water from large areas. The sustainability of water harvesting techniques at the local level are usually constrained by several factors such as labor, construction costs, loss of productive land, and maintenance, suggesting that multiple solutions are required to sustain the benefits of water harvesting techniques. |
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Academic Press |
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Oxford |
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Goss, M.J.; Oliver, M. |
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978-0-323-95133-3 |
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THL @ christoph.kuells @ Mekuria2023593 |
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225 |
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