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Stone, A. E. C., & Edmunds, W. M. (2014). Naturally-high nitrate in unsaturated zone sand dunes above the Stampriet Basin, Namibia. Journal of Arid Environments, 105, 41–51.
Abstract: Elevated groundwater nitrate levels are common in drylands, often in excess of WHO guidelines, with concern for human and animal health. In light of recent attempts to identify nitrate sources in the Kalahari this paper presents the first unsaturated zone (USZ) nitrate profiles and recharge rate estimates for the important transboundary Stampriet Basin, alongside the first rainfall chemistry records. Elevated subsurface nitrate reaches 100–250 and 250–525 mg/L NO3–N, with NO3–N/Cl of 4–12, indicating input above evapotranspiration. Chloride mass balance recharge rates range from 4 to 27 mm/y, indicating a vertical movement of these nitrate pulses toward the water table over multi-decadal timescales. These profiles are sampled from dune crests, away from high concentrations of animals and without termite mounds. Given low-density animal grazing is unlikely to contribute consistent spot-scale nitrate over decades, these profiles give an initial estimate of naturally-produced concentrations. This insight is important for the management of the Stampriet Basin and wider Kalahari groundwater. This study expands our knowledge about elevated nitrate in dryland USZs, demonstrating that it can occur as pulses, probably in response to transient vegetation cover and that it is not limited to long-residence time USZs with very limited downward moisture flux (recharge).
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Stone, A. E. C., & Edmunds, W. M. (2014). Naturally-high nitrate in unsaturated zone sand dunes above the Stampriet Basin, Namibia. Journal of Arid Environments, 105, 41–51.
Abstract: Elevated groundwater nitrate levels are common in drylands, often in excess of WHO guidelines, with concern for human and animal health. In light of recent attempts to identify nitrate sources in the Kalahari this paper presents the first unsaturated zone (USZ) nitrate profiles and recharge rate estimates for the important transboundary Stampriet Basin, alongside the first rainfall chemistry records. Elevated subsurface nitrate reaches 100–250 and 250–525 mg/L NO3–N, with NO3–N/Cl of 4–12, indicating input above evapotranspiration. Chloride mass balance recharge rates range from 4 to 27 mm/y, indicating a vertical movement of these nitrate pulses toward the water table over multi-decadal timescales. These profiles are sampled from dune crests, away from high concentrations of animals and without termite mounds. Given low-density animal grazing is unlikely to contribute consistent spot-scale nitrate over decades, these profiles give an initial estimate of naturally-produced concentrations. This insight is important for the management of the Stampriet Basin and wider Kalahari groundwater. This study expands our knowledge about elevated nitrate in dryland USZs, demonstrating that it can occur as pulses, probably in response to transient vegetation cover and that it is not limited to long-residence time USZs with very limited downward moisture flux (recharge).
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Mühr-Ebert, E. L., Wagner, F., & Walther, C. (2019). Speciation of uranium: Compilation of a thermodynamic database and its experimental evaluation using different analytical techniques. Applied Geochemistry, 100, 213–222.
Abstract: Environmental hazards are caused by uranium mining legacies and enhanced radioactivity in utilized groundwater and surface water resources. Knowledge of uranium speciation in these waters is essential for predicting radionuclide migration and for installing effective water purification technology. The validity of the thermodynamic data for the environmental media affected by uranium mining legacies is of utmost importance. Therefore, a comprehensive and consistent database was established according to current knowledge. The uranium data included in the database is based on the NEA TDB (Guillaumont et al., 2003) and is modified or supplemented as necessary e.g. for calcium and magnesium uranyl carbonates. The specific ion interaction theory (Brönsted, 1922) is used to estimate activity constants, which is sufficient for the considered low ionic strengths. The success of this approach was evaluated by comparative experimental investigations and model calculations (PHREEQC (Parkhurst and Appelo, 1999)) for several model systems. The waters differ in pH (2.7–9.8), uranium concentration (10−9-10−4 mol/L) and ionic strength (0.002–0.2 mol/L). We used chemical extraction experiments, ESI-Orbitrap-MS and time-resolved laser-induced fluorescence spectroscopy (TRLFS) to measure the uranium speciation. The latter method is nonintrusive and therefore does not change the chemical composition of the investigated waters. This is very important, because any change of the system under study may also change the speciation.
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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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Silva, M. L. da, & Bonotto, D. M. (2015). Uranium isotopes in groundwater occurring at Amazonas State, Brazil. Applied Radiation and Isotopes, 97, 24–33.
Abstract: This paper reports the behavior of the dissolved U-isotopes 238U and 234U in groundwater providing from 15 cities in Amazonas State, Brazil. The isotope dilution technique accompanied by alpha spectrometry were utilized for acquiring the U content and 234U/238U activity ratio (AR) data, 0.01–1.4µgL−1 and 1.0–3.5, respectively. These results suggest that the water is circulating in a reducing environment and leaching strata containing minerals with low uranium concentration. A tendency to increasing ARs values following the groundwater flow direction is identified in Manaus city. The AR also increases according to the SW–NE directions: Uarini→Tefé; Manacapuru→Manaus; Presidente Figueiredo→São Sebastião do Uatumã; and Boa Vista do Ramos→Parintins. Such trends are possibly related to several factors, among them the increasing acid character of the waters. The waters analyzed are used for human consumption and the highest dissolved U content is much lower than the maximum established by the World Health Organization. Therefore, in view of this radiological parameter they can be used for drinking purposes.
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