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Jana, A.; Unni, A.; Ravuru, S.S.; Das, A.; Das, D.; Biswas, S.; Sheshadri, H.; De, S. |
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Title |
In-situ polymerization into the basal spacing of LDH for selective and enhanced uranium adsorption: A case study with real life uranium alkaline leach liquor |
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Journal Article |
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Year |
2022 |
Publication |
Chemical Engineering Journal |
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Volume |
428 |
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131180 |
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In-situ polymerization, Layered double hydroxide, Leach liquor, Uranium adsorption, Uranium recovery |
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Uranium is used as a fuel for nuclear power plant and can be extracted from different ores, mainly acidic (silicious ore) and alkaline (carbonate ore). Recovery of uranium through acid leaching from silicious ore is well established, whereas, alkaline leaching from carbonate ore is challenging due to the excessive salinity of leach liquor and high concentration of carbonate, bicarbonate and sulphate. Herein, two monomers, acrylic acid (AA) and N, N-methylene bisacrylamide (BAM), selective towards uranyl were intercalated in-situ into the interlayer, followed by their polymerization and cross-linking to form novel polymer intercalated hybrid layered double hydroxide (LDH). The LDH acts as a backbone to overcome coiling and swelling of polymer and anchors them as free-standing. Various parameters, like, the type of metal ions, monomer ratio (AA: BAM) and metal ion ratio (M2+:M3+), were studied to determine the optimum conditions for effective intercalation and polymerization of monomers. Magnesium aluminum (MgAl) LDH with a cross-linked polymer having a monomer ratio of 3:2 (AA: BAM) as intercalating species showed maximum efficiency of uranyl adsorption (1456 mg/g at 30 °C) with highest capacity so far. The distribution coefficient (Kd, l/mg) in the order of 105 suggested that the adsorbent was highly selective for uranyl in the presence of different cations, anions and humic acid. The adsorbent extracts uranium effectively and selectively from a real-life alkaline leach liquor with an efficiency of 96% at 5 g/l dose. Uranium can be recovered from the adsorbent in the form of sodium di-uranate using 2(M) NaOH and was reused for eight cycles. |
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1385-8947 |
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THL @ christoph.kuells @ jana_-situ_2022 |
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209 |
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Wang, B.; Luo, Y.; Qian, J.-zhong; Liu, J.-hui; Li, X.; Zhang, Y.-hong; Chen, Q.-qian; Li, L.-yao; Liang, D.-ye; Huang, J. |
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Title |
Machine learning–based optimal design of the in-situ leaching process parameter (ISLPP) for the acid in-situ leaching of uranium |
Type |
Journal Article |
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Year |
2023 |
Publication |
Journal of Hydrology |
Abbreviated Journal |
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Volume |
626 |
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Pages |
130234 |
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Keywords |
In-situ leaching, Injection rate design, Lixiviant concentration design, Machine learning, Simulation-optimisation, Uncertainty |
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The migration process of leached uranium in the in-situ leaching of uranium is considered a typical reactive transport problem. During this process, the lixiviant concentration and injection rate are important in-situ leaching process parameters (ISLPP) to efficiently recover uranium. However, several uncertain factors affect the outcomes of the ISLPP design. In addition, the repeated use of the reactive transport model (RTM) for investigating the acid in-situ leaching of uranium with the application of the Monte Carlo method leads to a substantial computational load. For this reason, a machine learning (ML)–based surrogate model was developed with the backpropagation neural network (BPNN) method to replace the RTM under the condition of uncertain parameters. Moreover, the simulated annealing optimisation model for ISLPP was created based on the proposed surrogate model. The optimal ISLPP was achieved that generated maximum profits from uranium recovery under different lixiviant prices, uranium prices and exploitation times. The optimal design framework of ISLPP based on the proposed ML algorithm was then applied in the Bayan-Uul sandstone-type uranium deposit in Inner Mongolia, China. From our analysis, it was demonstrated that the ML-based surrogate model exhibited great fitness with the RTM. The optimal results of the ISLPP indicated that the lixiviant concentration and injection rate could be adjusted based on the fluctuations in lixiviant price, uranium price and exploitation time. If the prices of sulphuric acid were high, a specific concentration of hydrogen peroxide could be injected into the injection well to promote the oxidation and dissolution of the uranium ore to increase the income from the uranium recovery. The optimisation model can also use the ISLPP scheme to boost the revenues from different lixiviant prices, uranium prices and exploitation times under the uncertainty of porosity, illustrating the applicability of the ML-based optimal design method of ISLPP in ISL mining. A general framework for developing surrogate models, as well as for conducting uncertainty analyses for a wide range of groundwater models was proposed here yielding valuable insights. |
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0022-1694 |
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THL @ christoph.kuells @ wang_machine_2023 |
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210 |
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Zeng, S.; Song, J.; Sun, B.; Wang, F.; Ye, W.; Shen, Y.; Li, H. |
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Title |
Seepage characteristics of the leaching solution during in situ leaching of uranium |
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Journal Article |
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Year |
2023 |
Publication |
Nuclear Engineering and Technology |
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55 |
Issue |
2 |
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566-574 |
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In situ leaching, Leaching solution viscosity, Seepage characteristics, Seepage pressure, Uranium-bearing sandstone |
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Investigating the seepage characteristics of the leaching solution in the ore-bearing layer during the in situ leaching process can be useful for designing the process parameters for the uranium mining well. We prepared leaching solutions of four different viscosities and conducted experiments using a self-developed multifunctional uranium ore seepage test device. The effects of different viscosities of leaching solutions on the seepage characteristics of uranium-bearing sandstones were examined using seepage mechanics, physicochemical seepage theory, and dissolution erosion mechanism. Results indicated that while the seepage characteristics of various viscosities of leaching solutions were the same in rock samples with similar internal pore architectures, there were regular differences between the saturated and the unsaturated stages. In addition, the time required for the specimen to reach saturation varied with the viscosity of the leaching solution. The higher the viscosity of the solution, the slower the seepage flow from the unsaturated stage to the saturated stage. Furthermore, during the saturation stage, the seepage pressure of a leaching solution with a high viscosity was greater than that of a leaching solution with a low viscosity. However, the permeability coefficient of the high viscosity leaching solution was less than that of a low viscosity leaching solution. |
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1738-5733 |
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THL @ christoph.kuells @ zeng_seepage_2023 |
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211 |
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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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Keywords |
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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Gil-Márquez, J.M.; Sültenfuß, J.; Andreo, B.; Mudarra, M. |
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Groundwater dating tools (3H, 3He, 4He, CFC-12, SF6) coupled with hydrochemistry to evaluate the hydrogeological functioning of complex evaporite-karst settings |
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Journal Article |
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2020 |
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Journal of Hydrology |
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580 |
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124263 |
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Groundwater dating, Evaporite karst, Brine spring, Free-shape models |
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The hydrogeological functioning of four different areas in a complex evaporite-karst unit of predominantly aquitard behavior in S Spain was investigated. Environmental dating tracers (3H, 3He, 4He, CFC-12, SF6) and hydrochemical data were determined from spring samples to identify and characterize groundwater flow components of different residence times in the media. Results show a general geochemical evolution pattern, from higher (recharge areas) to lower positions (discharge areas), in which mineralization rises as well as the value of the rCl−/SO42−, evidencing longer water-rock interaction. Ne values show degassing of most of the samples, favored by the high salinity of groundwater and the development of karstification so that the concentration of all the considered gases were corrected according to the difference between the theoretical and the measured Ne. The presence of modern groundwater in every sample was proved by the detection of 3H and CFC-12. At the opposite, the higher amount of radiogenic 4He in most samples also indicates that they have an old component. The 3H/3He dating method does not give reliable ages as a consequence of degassing and the large uncertainty of the 3He/4He ratios of the sources for the radiogenic Helium. The large SF6 concentrations suggest terrigenic production related to halite and dolomite. Binary Mixing and Free Shape Models were created based on 3H and CFC-12 data to interpret the age distribution of the samples. Two parameters (GA50 and >70%) were proposed as an indicator of that distribution, as they provide further information than the mean age. Particularly, GA50 is derived from the median groundwater age and is presented as a new way of interpreting mixed groundwater age data. A greater fraction of old groundwater (3H and CFC-12 free) was identified in discharge areas, while the proportion and estimated infiltration date of the younger fractions in recharge areas were higher and more recent, respectively. The application of different approaches has been useful to corroborate previous theoretical conceptual model proposed for the study area and to test the applicability of the used environmental tracer in dating brine groundwater and karst springs. |
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0022-1694 |
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THL @ christoph.kuells @ Gilmarquez2020124263 |
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213 |
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Romeo, N.; Mabry, J.; Hillegonds, D.; Kainz, G.; Jaklitsch, M.; Matsumoto, T. |
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Developments of a field gas extraction device and krypton purification system for groundwater radio-krypton dating at the IAEA |
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Journal Article |
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2022 |
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Applied Radiation and Isotopes |
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189 |
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110450 |
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The long-lived radio-krypton isotope 81Kr (t1/2 = 2.29 × 105 yr) is an ideal tracer for old groundwater age dating in the range of 105–106 years which goes beyond the reach of radio-carbon (14C) age dating. Analytical breakthrough made over the last two decades in Atom Trap Trace Analysis (ATTA) has enabled the use of this isotope with extremely low abundance (81Kr/Kr = 6 × 10−13) to be used as a practical dating tool for very old groundwater. The International Atomic Energy Agency aims to provide this new isotope tool for better groundwater resource management of Member States and developed a field sampling device to collect dissolved gas samples from groundwater and a system to separate and purify trace amounts of krypton from the gas samples for the ATTA analysis. The design, setup and performances of our sampling and purification systems are described here. Our system can produce a high purity aliquot of about 5 μL of krypton from 5 L of air sample (recovery yield of >90%). The samples made by our system were confirmed to be acceptable for the ATTA analysis. |
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0969-8043 |
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THL @ christoph.kuells @ Romeo2022110450 |
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214 |
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Musy, S.; Meyzonnat, G.; Barbecot, F.; Hunkeler, D.; Sültenfuss, J.; Solomon, D.K.; Purtschert, R. |
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In-situ sampling for krypton-85 groundwater dating |
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Journal Article |
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2021 |
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Journal of Hydrology X |
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11 |
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100075 |
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Noble gases, Tracers, Groundwater, Dating, Sampling Methodology |
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Krypton-85 and other radioactive noble gases are widely used for groundwater dating purposes. 85Kr analysis require large volumes of water to reach the analytical requirements. Conventionally, this water is pumped to the surface to be degassed with a gas extraction system. The large pumping rate may disturb the natural flow field and requires substantial field logistics. Hence, we propose a new in-situ degassing method, in which membrane contactors are used to degas the groundwater directly in the well and gas is collected at the surface. This way, field work is facilitated, groundwater system disturbance is minimized, and the gas sample is collected at a specific depth. We demonstrate the tightness of the system regarding atmospheric air contamination for a collection times of 24 h, which is sufficient for both low-level counting and laser-based counting methods for 85Kr. The minimal borehole diameter is 7.5 cm for the prototype presented in this research but can easily be reduced to smaller diameters. In a case study, we compare the results obtained with the new passive method with those from a conventional packer setup sampling. Additionally, 3H/3He samples were collected for both sampling regimes and the dating results were compared with those from 85Kr. A good agreement between tracer ages is demonstrated and the age stratigraphy is consistent with the expected age distribution for a porous unconfined aquifer. In addition, our study emphasizes the differences between the age information sampled with various methods. In conclusion, we demonstrate that the new in situ quasi-passive method provides a more representative age stratigraphy with depth in most cases. |
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2589-9155 |
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THL @ christoph.kuells @ Musy2021100075 |
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215 |
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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 |
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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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Musy, S.; Purtschert, R. |
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Reviewing 39Ar and 37Ar underground production in shallow depths with implications for groundwater dating |
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Journal Article |
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2023 |
Publication |
Science of The Total Environment |
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884 |
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163868 |
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Subsurface production, Argon-39, Argon-37, Muons, Isotope hydrology, Tracers |
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Argon-37 (37Ar) and Argon-39 (39Ar) are used for groundwater dating on timescales from weeks to centuries. For both isotopes, the quantification of underground sources is essential to accurately infer water residence times from sampled dissolved activities. Subsurface production resulting from interactions with neutrons from the natural radioactivity in rocks and with primary cosmogenic neutrons has been known for a long time. More recently, the capture of slow negative muons and reactions with muon-induced neutrons were documented for 39Ar subsurface production in the context of underground particle detectors (e.g. for Dark Matter research). However, the contribution from these particles was never considered for groundwater dating applications. Here, we reevaluate the importance of all potential depth-related production channels at depth ranges relevant for 39Ar groundwater dating [0 − 200 meters below the surface (m.b.s)]. The production of radioargon by muon-induced processes is considered in this depth range for the first time. The uncertainty on the total depth-dependent production rate is estimated with Monte Carlo simulations assuming a uniform distribution of the parameter uncertainties. This work aims to provide a comprehensive framework for interpreting 39Ar activities in terms of groundwater residence times and for exposure age dating of rocks. The production of 37Ar is also addressed since this isotope is relevant as a proxy for 39Ar production, for the timing of river-groundwater exchanges, and in the context of on-site inspections (OSI) within the verification framework of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). In this perspective, we provide an interactive web-based application for the calculation of 37Ar and 39Ar production rates in rocks. |
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0048-9697 |
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THL @ christoph.kuells @ Musy2023163868 |
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217 |
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Aderemi, B.A.; Olwal, T.O.; Ndambuki, J.M.; Rwanga, S.S. |
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Groundwater levels forecasting using machine learning models: A case study of the groundwater region 10 at Karst Belt, South Africa |
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Journal Article |
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Year |
2023 |
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Systems and Soft Computing |
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5 |
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200049 |
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Artificial intelligence, Forecasting model, Groundwater levels, Machine learning, Neural networks, Rainfall, Regression, Temperature, Time series |
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Abstract |
The crucial role which groundwater resource plays in our environment and the overall well-being of all living things can not be underestimated. Nonetheless, mismanagement of resources, over-exploitation, inadequate supply of surface water and pollution have led to severe drought and an overall drop in groundwater resources’ levels over the past decades. To address this, a groundwater flow model and several mathematical data-driven models have been developed for forecasting groundwater levels. However, there is a problem of unavailability and scarcity of the on-site input data needed by the data-driven models to forecast the groundwater level. Furthermore, as a result of the dynamics and stochastic characteristics of groundwater, there is a need for an appropriate, accurate and reliable forecasting model to solve these challenges. Over the years, the broad application of Machine Learning (ML) and Artificial Intelligence (AI) models are gaining attraction as an alternative solution for forecasting groundwater levels. Against this background, this article provides an overview of forecasting methods for predicting groundwater levels. Also, this article uses ML models such as Regressions Models, Deep Auto-Regressive models, and Nonlinear Autoregressive Neural Networks with External Input (NARX) to forecast groundwater levels using the groundwater region 10 at Karst belt in South Africa as a case study. This was done using Python Mx. Version 1.9.1., and MATLAB R2022a machine learning toolboxes. Moreover, the Coefficient of Determination (R2);, Root Mean Square Error (RMSE), Mutual Information gain, Mean Absolute Percentage Error (MAPE), Mean Squared Error (MSE), Mean Absolute Error (MAE), and the Mean Absolute Scaled Error (MASE)) models were the forecasting statistical performance metrics used to assess the predictive performance of these models. The results obtained showed that NARX and Support Vector Machine (SVM) have higher performance metrics and accuracy compared to other models used in this study. |
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2772-9419 |
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THL @ christoph.kuells @ Aderemi2023200049 |
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219 |
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