IWW Rheinisch-Westfälisches Institut für Wasser Beratungs- und Entwicklungsgesellschaft mbH, Moritzstraße 26, 45476 Mülheim an der Ruhr, Germany.
IWW Rheinisch-Westfälisches Institut für Wasser Beratungs- und Entwicklungsgesellschaft mbH, Moritzstraße 26, 45476 Mülheim an der Ruhr, Germany.
Water Res. 2018 Feb 1;129:29-38. doi: 10.1016/j.watres.2017.11.001. Epub 2017 Nov 2.
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 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.
大多数关于地下水铀(U)发生的知识来自于现场原位操作实验、计算模型研究或实验室分析,这些研究分别研究了 U 迁移的个别过程。由于铀的重要氧化还原化学性质,它经常与许多其他元素循环(例如硫、碳、铁和锰)同时相互作用,这使得很难预测自然环境中的 U 浓度。为了本研究,分析了一个大型数据集,以根据基本水化学预测地下水中 U 的存在。该数据集由来自 2000 多个采样点的 8000 多个地下水化学分析(包括铀浓度)组成。观察到 U 浓度与电导率和碱度之间存在很强的关系,表明地球成因源材料的风化和解吸从矿物表面是 U 释放的主要机制。除了具有强烈还原条件的含水层外,在大多数情况下,该过程导致 U 在地下水中缓慢但持续地积累。重要的是,含水层中的流行氧化还原条件会调节 U 的发生。在好氧条件下 U 浓度适中,在锰和硝酸盐还原条件下(异养和自养硝酸盐还原)最高。只有在铁和硫酸盐还原地下水中,U 浓度超过 1μg/L 的可能性几乎为零,因为这些地下水是 U 的汇。矿物风化(尤其是碳酸盐)与锰和硝酸盐还原条件下 U 的迁移相结合,导致检测到 U 的风险最高。相比之下,与地下水的低 pH 值(<7)和低矿化度相关的风险较低,例如在花岗岩集水区的情况。我们的研究结果进一步提供了证据,表明农业实践(如石灰处理、施肥和灌溉)会以多种方式影响地下水的 U 发生。因此,未来对农田下含水层的准确管理将变得越来越重要。总之,我们发现含水层对升高的 U 浓度的脆弱性不能用单一因素来解释。这使得针对饮用水生产中提取的地下水升高的 U 浓度的靶向努力变得更加复杂。