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Musy, S., Meyzonnat, G., Barbecot, F., Hunkeler, D., Sültenfuss, J., Solomon, D. K., et al. (2021). In-situ sampling for krypton-85 groundwater dating. Journal of Hydrology X, 11, 100075.
Abstract: 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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Romeo, N., Mabry, J., Hillegonds, D., Kainz, G., Jaklitsch, M., & Matsumoto, T. (2022). Developments of a field gas extraction device and krypton purification system for groundwater radio-krypton dating at the IAEA. Applied Radiation and Isotopes, 189, 110450.
Abstract: 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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Gil-Márquez, J. M., Sültenfuß, J., Andreo, B., & Mudarra, M. (2020). Groundwater dating tools (3H, 3He, 4He, CFC-12, SF6) coupled with hydrochemistry to evaluate the hydrogeological functioning of complex evaporite-karst settings. Journal of Hydrology, 580, 124263.
Abstract: 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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Li, J., Pang, Z., Liu, Y., Hu, S., Jiang, W., Tian, L., et al. (2023). 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. Earth and Planetary Science Letters, 623, 118425.
Abstract: 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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Zeng, S., Song, J., Sun, B., Wang, F., Ye, W., Shen, Y., et al. (2023). Seepage characteristics of the leaching solution during in situ leaching of uranium. Nuclear Engineering and Technology, 55(2), 566–574.
Abstract: 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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