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Rallakis, D., Michels, R., Cathelineau, M., Parize, O., & Brouand, M. (2021). Conditions for uranium biomineralization during the formation of the Zoovch Ovoo roll-front-type uranium deposit in East Gobi Basin, Mongolia. Ore Geology Reviews, 138, 104351.
Abstract: The Zoovch Ovoo uranium roll-front-type deposit is hosted in the Sainshand Formation, a Late Cretaceous siliciclastic reservoir, which constitutes the upper part of the post-rift infilling of the Mesozoic East Gobi Basin in SE Mongolia. The Sainshand Formation consists of unconsolidated medium-grained sand, silt and clay intervals deposited in fluvial-lacustrine settings. The uranium deposit is confined within a 60–80 m thick siliciclastic sequence inside aquifer-driven systems. The overall system experienced shallow burial and was never subjected to temperatures higher than 40 °C. This study proposes a comprehensive metallogenic model for this uranium deposit. Sedimentological and mineralogical observations from drill core samples to the microscopic scale (optical and Scanning Electron Microscopy) together with in situ geochemistry of late-formed phases (Laser Ablation–Inductively Coupled Plasma Mass Spectrometry, Electron Probe Microanalysis, Fourier Transform–Infrared Spectroscopy) were considered for the reconstruction of the main stages of U trapping. In the mineralized zone, the uranium ore is expressed as Ca–enriched uraninite (UO2) and less commonly as Ca–enriched phospho-coffinite (U, P)SiO4. Trapping mechanisms include i) complexation (i.e. uranyl-carboxyl complexes), ii) adsorption on organic or clay particles) and iii) reduction by pyrite and by bacterial activity to amorphous uraninite. In all cases, the organic matter plays either the role of trap for uranium or nutrient for bacteria that can trap uranium through their metabolism. The shallow burial diagenesis conditions do not allow direct reduction of U(VI) by organic carbon. The δ34S values of the iron disulfide are very diverse, fluctuating in extreme cases between −50 to + 50‰, with an average δ34S value for framboidal pyrite at 2‰, and −20‰ for euhedral pyrite. The positive and negative values reflect close versus open fractionation systems, while bacterial sulphate reduction (BSR) is active during the whole diagenetic history of the deposit as an essential source of reduced sulfur. Therefore, using detrital organic matter as a carbon source, microorganisms play a significant role in uranium trapping, either as a direct reducing agent for uranium or pyrite formation, which will trap uranium through redox driven epigenetic processes.
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Zeng, S., Shen, Y., Sun, B., Zhang, N., Zhang, S., & Feng, S. (2021). Pore structure evolution characteristics of sandstone uranium ore during acid leaching. Nuclear Engineering and Technology, 53(12), 4033–4041.
Abstract: To better understand the permeability of uranium sandstone, improve the leaching rate of uranium, and explore the change law of pore structure characteristics and blocking mechanism during leaching, we systematically analyzed the microstructure of acid-leaching uranium sandstone. We investigated the variable rules of pore structure characteristics based on nuclear magnetic resonance (NMR). The results showed the following: (1) The uranium concentration change followed the exponential law during uranium deposits acid leaching. After 24 h, the uranium leaching rate reached 50%. The uranium leaching slowed gradually over the next 4 days. (2) Combined with the regularity of porosity variation, Stages I and II included chemical plugging controlled by surface reaction. Stage I was the major completion phase of uranium displacement with saturation precipitation of calcium sulfate. Stage II mainly precipitated iron (III) oxide-hydroxide and aluminum hydroxide. Stage III involved physical clogging controlled by diffusion. (3) In the three stages of leaching, the permeability of the leaching solution changed with the pore structure, which first decreased, then increased, and then decreased.
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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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Heine, F., & Einsiedl, F. (2021). Groundwater dating with dissolved organic radiocarbon: A promising approach in carbonate aquifers. Applied Geochemistry, 125, 104827.
Abstract: 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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Jing, M., Kumar, R., Attinger, S., Li, Q., Lu, C., & Heße, F. (2021). Assessing the contribution of groundwater to catchment travel time distributions through integrating conceptual flux tracking with explicit Lagrangian particle tracking. Advances in Water Resources, 149, 103849.
Abstract: Travel time distributions (TTDs) provide an effective way to describe the transport and mixing processes of water parcels in a subsurface hydrological system. A major challenge in characterizing catchment TTD is quantifying the travel times in deep groundwater and its contribution to the streamflow TTD. Here, we develop and test a novel modeling framework for an integrated assessment of catchment scale TTDs through explicit representation of 3D-groundwater dynamics. The proposed framework is based on the linkage between a flux tracking scheme with the surface hydrologic model (mHM) for the soil-water compartment and a particle tracking scheme with the 3D-groundwater model OpenGeoSys (OGS) for the groundwater compartment. This linkage provides us with the ability to simulate the spatial and temporal dynamics of TTDs in these different hydrological compartments from grid scale to regional scale. We apply this framework in the Nägelstedt catchment in central Germany. Simulation results reveal that both shape and scale of grid-scale groundwater TTDs are spatially heterogeneous, which are strongly dependent on the topography and aquifer structure. The component-wise analysis of catchment TTD shows a time-dependent sensitivity of transport processes in soil zone and groundwater to driving meteorological forcing. Catchment TTD exhibits a power-law shape and fractal behavior. The predictive uncertainty in catchment mean travel time is dominated by the uncertainty in the deep groundwater rather than that in the soil zone. Catchment mean travel time is severely biased by a marginal error in groundwater characterization. Accordingly, we recommend to use multiple summary statistics to minimize the predictive uncertainty introduced by the tailing behavior of catchment TTD.
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