Uranium in groundwater - A synopsis based on a large hydrogeochemical data set

Abstract

Most of the knowledge on the occurrence of Uranium (U) in groundwater comes from in-situ manipulation experiments in the field, computational modelling studies or from laboratory analyses where individual processes of U mobilization were studied in isolation. Because of Uranium's vital redox chemistry it interacts, often simultaneously, with many other element cycles (e.g., sulfur, carbon, iron, and manganese) making it difficult to predict U concentrations in natural environments. For the present study a large data set was analyzed to predict the occurrence of U in groundwater from basic hydrochemistry. The data set consists of more than 8000 chemical groundwater analyses (including Uranium concentrations) from more than 2000 sampling locations. A strong relation between U concentrations and electric conductivity as well as alkalinity was observed, suggesting that weathering of geogenic source material and desorption from mineral surfaces is the principle mechanism of U release. Except for aquifers with strongly reducing conditions this process leads to a slow but continuous accumulation of U in groundwater in most cases. Importantly, the occurrence of U is modulated by the prevailing redox conditions in an aquifer. Uranium concentrations were moderate under oxic conditions and highest under manganese and nitrate-reducing conditions (heterotrophic as wells as autotrophic nitrate reduction). Only in iron- and sulfate-reducing groundwater the probability of U concentrations above 1 μg l^-1 was virtually zero, as these ground waters act as U sinks. The combination of mineral weathering (especially carbonates) with mobilization of U under manganese and nitrate reducing conditions results in the highest risk of detecting U. In contrast, a low risk is associated with low pH (<7) and low mineralization of groundwater, which is the case in granitic catchments, for example. Our results further provide evidence, that agricultural practices such as liming, use of fertilizers and irrigation influence the occurrence of U in groundwater in multiple ways. Accurate management of aquifers underlying farmland will therefore become more and more important in the future. In summary, we find that the vulnerability of an aquifer to elevated U concentrations cannot be explained by a single factor. This complicates efforts to target elevated U concentrations in groundwaters that are abstracted for drinking water production.

Keywords: Drinking water; Geochemistry; Groundwater; Uranium.