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Priestley, S. C., Payne, T. E., Harrison, J. J., Post, V. E. A., Shand, P., Love, A. J., et al. (2018). Use of U-isotopes in exploring groundwater flow and inter-aquifer leakage in the south-western margin of the Great Artesian Basin and Arckaringa Basin, central Australia. Applied Geochemistry, 98, 331–344.
Abstract: The distribution of uranium isotopes (238U and 234U) in groundwaters of the south-western margin of the Great Artesian Basin (GAB), Australia, and underlying Arckaringa Basin were examined using groundwater samples and a sequential extraction of aquifer sediments. Rock weathering, the geochemical environment and α-recoil of daughter products control the 238U and 234U isotope distributions giving rise to large spatial variations. Generally, the shallowest aquifer (J aquifer) contains groundwater with higher 238U activity concentrations and 234U/238U activity ratios close to secular equilibrium. However, the source input of uranium is spatially variable as intermittent recharge from ephemeral rivers passes through rocks that have already undergone extensive weathering and contain low 238U activity concentrations. Other locations in the J aquifer that receive little or no recharge contain higher 238U activity concentrations because uranium from localised uranium-rich rocks have been leached into solution and the geochemical environment allows the uranium to be kept in solution. The geochemical conditions of the deeper aquifers generally result in lower 238U activity concentrations in the groundwater accompanied by higher 234U/238U activity ratios. The sequential extraction of aquifer sediments showed that α-recoil of 234U from the solid mineral phases into the groundwater, rather than dissolution of, or exchange with the groundwater accessible minerals in the aquifer, caused enrichment of groundwater 234U/238U activity ratios in the Boorthanna Formation. Decay of 238U in uranium-rich coatings on J aquifer sediments caused resistant phase 234U/238U activity ratio enrichment. The groundwater 234U/238U activity ratio is dependent on groundwater residence time or flow rate, depending on the flow path trajectory. Thus, uranium isotope variations confirmed earlier groundwater flow interpretations based on other tracers; however, spatial heterogeneity, and the lack of clear regional correlations, made it difficult to identify recharge and inter-aquifer leakage.
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Strandmann, P. A. E. P. von, Reynolds, B. C., Porcelli, D., James, R. H., Calsteren, P. van, Baskaran, M., et al. (2006). Assessing continental weathering rates and actinide transport in the Great Artesian Basin. Geochimica et Cosmochimica Acta, 70(18, Supplement), 497.
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Frumkin, A., & Gvirtzman, H. (2006). Cross-formational rising groundwater at an artesian karstic basin: the Ayalon Saline Anomaly, Israel. Journal of Hydrology, 318(1), 316–333.
Abstract: It is proposed that a geothermal artesian karstic system at the central part of the Yarkon–Taninim aquifer creates the ‘Ayalon Saline Anomaly’ (ASA), whose mechanism has been under debate for several decades. A 4-year-long detailed groundwater monitoring was carried out at 68 new shallow boreholes in the Ayalon region, accompanied by a comprehensive survey of karstic voids. Results indicate the rising of warm-brackish groundwater through highly permeable swarms of karstic shafts, serving as an outflow of the artesian geothermal system. The ASA area contains ‘hot spots’, where groundwater contrasts with ‘normal’ water hundreds of meters away. The ASA temperature reaches 30°C (∼5°C warmer than its surroundings), chloride concentration reaches 528mg/l (50–100mg/l in the surrounding), H2S concentration reaches 5.6mg/l (zero all around) and pH value is 7.0 (compared with 7.8 around). Subsequently, the hydrothermal water flows laterally of at the watertable horizon through horizontal conduits, mixing with ‘normal’ fresh water which had circulated at shallow depth. Following rainy seasons, maximal watertable rise is observed in the ASA compared to its surroundings. Regional hydrogeology considerations suggest that the replenishment area for the ASA water is at the Samaria Mountains, east of the ASA. The water circulates to a great depth while flowing westward, and a cross-formational upward flow is then favored close the upper sub-aquifer’s confinement border.
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Smedley, P. L., & Kinniburgh, D. G. (2023). Uranium in natural waters and the environment: Distribution, speciation and impact. Applied Geochemistry, 148, 105534.
Abstract: The concentrations of U in natural waters are usually low, being typically less than 4 μg/L in river water, around 3.3 μg/L in open seawater, and usually less than 5 μg/L in groundwater. Higher concentrations can occur in both surface water and groundwater and the range spans some six orders of magnitude, with extremes in the mg/L range. However, such extremes in surface water are rare and linked to localized mineralization or evaporation in alkaline lakes. High concentrations in groundwater, substantially above the WHO provisional guideline value for U in drinking water of 30 μg/L, are associated most strongly with (i) granitic and felsic volcanic aquifers, (ii) continental sandstone aquifers especially in alluvial plains and (iii) areas of U mineralization. High-U groundwater provinces are more common in arid and semi-arid terrains where evaporation is an additional factor involved in concentrating U and other solutes. Examples of granitic and felsic volcanic terrains with documented high U concentrations include several parts of peninsular India, eastern USA, Canada, South Korea, southern Finland, Norway, Switzerland and Burundi. Examples of continental sandstone aquifers include the alluvial plains of the Indo-Gangetic Basin of India and Pakistan, the Central Valley, High Plains, Carson Desert, Española Basin and Edwards-Trinity aquifers of the USA, Datong Basin, China, parts of Iraq and the loess of the Chaco-Pampean Plain, Argentina. Many of these plains host eroded deposits of granitic and felsic volcanic precursors which likely act as primary sources of U. Numerous examples exist of groundwater impacted by U mineralization, often accompanied by mining, including locations in USA, Australia, Brazil, Canada, Portugal, China, Egypt and Germany. These may host high to extreme concentrations of U but are typically of localized extent. The overarching mechanisms of U mobilization in water are now well-established and depend broadly on redox conditions, pH and solute chemistry, which are shaped by the geological conditions outlined above. Uranium is recognized to be mobile in its oxic, U(VI) state, at neutral to alkaline pH (7–9) and is aided by the formation of stable U–CO3(±Ca, Mg) complexes. In such oxic and alkaline conditions, U commonly covaries with other similarly controlled anions and oxyanions such as F, As, V and Mo. Uranium is also mobile at acidic pH (2–4), principally as the uranyl cation UO22+. Mobility in U mineralized areas may therefore occur in neutral to alkaline conditions or in conditions with acid drainage, depending on the local occurrence and capacity for pH buffering by carbonate minerals. In groundwater, mobilization has also been observed in mildly (Mn-) reducing conditions. Uranium is immobile in more strongly (Fe-, SO4-) reducing conditions as it is reduced to U(IV) and is either precipitated as a crystalline or ‘non-crystalline’ form of UO2 or is sorbed to mineral surfaces. A more detailed understanding of U chemistry in the natural environment is challenging because of the large number of complexes formed, the strong binding to oxides and humic substances and their interactions, including ternary oxide-humic-U interactions. Improved quantification of these interactions will require updating of the commonly-used speciation software and databases to include the most recent developments in surface complexation models. Also, given their important role in maintaining low U concentrations in many natural waters, the nature and solubility of the amorphous or non-crystalline forms of UO2 that result from microbial reduction of U(VI) need improved quantification. Even where high-U groundwater exists, percentage exceedances of the WHO guideline value are variable and often small. More rigorous testing programmes to establish usable sources are therefore warranted in such vulnerable aquifers. As drinking-water regulation for U is a relatively recent introduction in many countries (e.g. the European Union), testing is not yet routine or established and data are still relatively limited. Acquisition of more data will establish whether analogous aquifers elsewhere in the world have similar patterns of aqueous U distribution. In the high-U groundwater regions that have been recognized so far, the general absence of evidence for clinical health symptoms is a positive finding and tempers the scale of public health concern, though it also highlights a need for continued investigation.
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Ammar, F. H., Deschamps, P., Chkir, N., Zouari, K., Agoune, A., & Hamelin, B. (2020). Uranium isotopes as tracers of groundwater evolution in the Complexe Terminal aquifer of southern Tunisia. Quaternary International, 547, 33–49.
Abstract: The Complexe Terminal (CT) multi-layer aquifer is formed by Neogene/Paleogene sand deposits, Upper Senonian (Campanian-Maastrichtian limestones) and Turonian carbonates. The chemical composition and isotopes of carbon and uranium were investigated in groundwater sampled from the main hydrogeological units of the (CT) aquifer in southern Tunisia. We paid special attention to the variability of uranium contents and isotopes ratio (234U/238U) to provide a better understanding of the evolution of the groundwater system. Uranium concentrations range from 1.5 to 19.5 ppb, typical of oxic or mildly reducing conditions in groundwaters. The lowest concentrations are found southeast of the study area, where active recharge is supposed to take place. When looking at the isotope composition, it appears that all the samples, including those from carbonate levels, are in radioactive disequilibrium with significant 234U excess. A clear-cut distinction is observed between Turonian and Senonian carbonate aquifers on the one hand, with 234U/238U activity ratios between 1.1 and 1.8, and the sandy aquifer on the other hand, showing higher ratios from 1.8 to 3.2. The distribution of uranium in this complex aquifer system seems to be in agreement with the lithological variability and are ultimately a function of a number of physical and chemical factors including the uranium content of the hosting geological formation, water-rock interaction and mixing between waters having different isotopic signatures. Significant relationships also appear when comparing the uranium distribution with the major ions composition. It is noticeable that uranium is better correlated with sulfate, calcium and magnesium than with other major ions as chloride or bicarbonate. The 14C activities and δ13C values of DIC cover a wide range of values, from 1.1 pmc to 30.2 pmc and from −3.6‰ to −10.7‰, respectively. 14C model ages estimated by the Fontes and Garnier model are all younger than 22 Ka and indicate that the recharge of CT groundwater occurred mainly during the end of the last Glacial and throughout the Holocene.
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