Increased uranium concentrations in ground and surface waters of the Swiss Plateau: A result of uranium accumulation and leaching in the Molasse basin and (ancient) wetlands?

摘要

Increased uranium (U) concentrations are found in certain ground and surface waters of the Swiss Plateau. Analysis of more than 100 public fountains revealed that increased U-238 concentrations frequently occur close to the interface between the Lower Freshwater Molasse and the Upper Marine Molasse, cropping out in the western part of the Swiss Molasse Basin. Out of these locations, Mont Vully, situated ca. 20 km west of Berne, was studied in detail. As this hill consists of the two aforementioned stratigraphic Molasse units, it represents an ideal case study. Two springs at the northern slopes of Mont Vully exhibit the highest U-238 concentrations with more than 300 mBq/L and were thus monitored for almost two years in order to screen possible seasonal variations. Further water samples were collected from spring captures, creeks and drainage pipes. The pipes drain the farmland north of Mont Vully showing U-238 concentrations with more than 600 mBq/L. In order to discover the reason for the duplication in concentration, gamma dose rate measurements were accomplished on the farmland, revealing elevated dose rates of up to 160 nSv/h. These are located above ancient pathways of creeks that originated from Mont Vully. At these locations with elevated dose rates, three shallow sediment drill cores were taken and analyzed for their U content. The sediment cores can essentially be divided into three parts: (i) an upper soil with common U concentrations of about 30 Bq/kg( 238)U, (ii) an U-rich peat horizon with concentrations of up to 500 Bq/kg U-238, and (iii) an impermeable clay unit that acts as an aquitard with again minor U-238 concentrations. Radiocarbon dating of the U-rich peat horizon reveals ages younger than 8.1 kyrs. This study suggests that a wetland was formed on top of the impermeable clay layer after the last glaciation during the Holocene. The stream waters with U-238 concentrations of more than 300 mBq/L originating from Mont Vully contributed significantly to the water supply for the development of the wetland. Due to the reducing conditions that are present in wetlands, the dissolved U in the incoming streams was reduced and adsorbed onto organic matter. Accordingly, an entrapment for U was generated, persisting for at least 6 kyrs - a sufficient time to accumulate up to 500 Bq/kg. In the course of the last century, numerous wetlands in Switzerland were drained by capturing streams and installing drainage pipes to make the land suitable for agriculture. This kind of melioration was also done at the wetlands north of Mont Vully resulting in a subsequent change in redox conditions within the soil. The solubility of U depends on its oxidation state and U can be oxidized by oxygen-rich rainwater. The rainwater leached the U adsorbed on the peat yielding U-238 concentrations of more than 600 mBq/L. Consequently, the duplication of U-238 concentrations in the drainage water as compared to the original concentration that creeks brought into the ancient wetlands has been clarified during this study. Twenty of the analyzed public fountains in the Swiss Plateau exhibited a U-238 concentration of more than 50 mBq/L. All of them could have contributed to the formation of a wetland after the last glaciation, which leads to the assumption that the situation at Mont Vully is not a singularity in the Swiss Plateau.