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?

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 238U 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 238U 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 238U 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 238U, (ii) an U-rich peat horizon with concentrations of up to 500 Bq/kg 238U, and (iii) an impermeable clay unit that acts as an aquitard with again minor 238U 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 238U 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 238U concentrations of more than 600 mBq/L. Consequently, the duplication of 238U 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 238U 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.

Comparative modeling of an in situ diffusion experiment in granite at the Grimsel Test Site.

An in situ diffusion experiment was performed at the Grimsel Test Site (Switzerland). Several tracers ((3)H as HTO, (22)Na(+), (134)Cs(+), (131)I(-) with stable I(-) as carrier) were continuously circulated through a packed-off borehole and the decrease in tracer concentrations in the liquid phase was monitored for a period of about 2years. Subsequently, the borehole section was overcored and the tracer profiles in the rock analyzed ((3)H, (22)Na(+), (134)Cs(+)). (3)H and (22)Na(+) showed a similar decrease in activity in the circulation system (slightly larger drop for (3)H). The drop in activity for (134)Cs(+) was much more pronounced. Transport distances in the rock were about 20cm for (3)H, 10cm for (22)Na(+), and 1cm for (134)Cs(+). The dataset (except for (131)I(-) because of complete decay at the end of the experiment) was analyzed with different diffusion-sorption models by different teams (IDAEA-CSIC, UJV-Rez, JAEA) using different codes, with the goal of obtaining effective diffusion coefficients (De) and porosity (ϕ) or rock capacity (α) values. From the activity measurements in the rock, it was observed that it was not possible to recover the full tracer activity in the rock (no activity balance when adding the activities in the rock and in the fluid circulation system). A Borehole Disturbed Zone (BDZ) had to be taken into account to fit the experimental observations. The extension of the BDZ (1-2mm) is about the same magnitude than the mean grain size of the quartz and feldspar grains. IDAEA-CSIC and UJV-Rez tried directly to match the results of the in situ experiment, without forcing any laboratory-based parameter values into the models. JAEA conducted a predictive modeling based on laboratory diffusion data and their scaling to in situ conditions. The results from the different codes have been compared, also with results from small-scale laboratory experiments. Outstanding issues to be resolved are the need for a very large capacity factor in the BDZ for (3)H and the difference between apparent diffusion coefficients (Da) from the in situ experiment and out-leaching laboratory tests.

30-y follow-up of a Pu/Am inhalation case.

In 1983, a young man inhaled accidentally a large amount of plutonium and americium. This case was carefully followed until 2013. Since no decorporation measures had been taken, the undisturbed metabolism of Pu and Am can be derived from the data. First objective was to determine the amount of inhaled radionuclides and to estimate committed effective dose. In vivo and excretion measurements started immediately after the inhalation, and for quality assurance, all types of measurements were performed by different labs in Europe and the USA. After dose assessment by various international groups were completed, the measurements were continued to produce scientific data for model validation. The data have been analysed here to estimate lung absorption parameter values for the inhaled plutonium and americium oxide using the proposed new ICRP Human Respiratory Tract Model. As supplement to the biokinetic modelling, biological data from three different cytogenetic markers have been added. The estimated committed effective dose is in the order of 1 Sv. The subject is 30 y after the inhalation, of good health, according to a recent medical check-up.

Green manure addition to soil increases grain zinc concentration in bread wheat.

Zinc (Zn) deficiency is a major problem for many people living on wheat-based diets. Here, we explored whether addition of green manure of red clover and sunflower to a calcareous soil or inoculating a non-indigenous arbuscular mycorrhizal fungal (AMF) strain may increase grain Zn concentration in bread wheat. For this purpose we performed a multifactorial pot experiment, in which the effects of two green manures (red clover, sunflower), ZnSO4 application, soil γ-irradiation (elimination of naturally occurring AMF), and AMF inoculation were tested. Both green manures were labeled with 65Zn radiotracer to record the Zn recoveries in the aboveground plant biomass. Application of ZnSO4 fertilizer increased grain Zn concentration from 20 to 39 mg Zn kg-1 and sole addition of green manure of sunflower to soil raised grain Zn concentration to 31 mg Zn kg-1. Adding the two together to soil increased grain Zn concentration even further to 54 mg Zn kg-1. Mixing green manure of sunflower to soil mobilized additional 48 µg Zn (kg soil)-1 for transfer to the aboveground plant biomass, compared to the total of 132 µg Zn (kg soil)-1 taken up from plain soil when neither green manure nor ZnSO4 were applied. Green manure amendments to soil also raised the DTPA-extractable Zn in soil. Inoculating a non-indigenous AMF did not increase plant Zn uptake. The study thus showed that organic matter amendments to soil can contribute to a better utilization of naturally stocked soil micronutrients, and thereby reduce any need for major external inputs.

Availability of zinc and the ligands citrate and histidine to wheat: does uptake of entire complexes play a role?

Organic ligands in soils affect the availability of trace metals such as Zn to plants. This study investigated the effects of two of these ligands, citrate and histidine, on Zn uptake by wheat under hydroponic conditions. Uptake of (65)Zn in the presence of these ligands was compared to uptake in the presence of EDTA at the same free Zn concentration (Zn(2+) ~ 50 nM). In the presence of citrate Zn root uptake was enhanced ~3.5 times and in the presence of histidine, by a factor of ~9, compared to the EDTA treatments. Citrate uptake was slightly reduced in the treatment containing ligands and Zn compared to the treatment containing the same ligand concentration but no Zn. In addition, a higher uptake of Zn than of citrate was observed. This suggests that the enhanced Zn uptake was primarily due to increased supply of Zn(2+) by diffusion and dissociation of Zn-citrate complexes at the root surface. Histidine uptake was much higher than citrate uptake and not influenced by the presence of Zn. As histidine forms stronger complexes with Zn than citrate, the results suggest that the enhancement of Zn uptake in the presence of histidine was in part due to the uptake of undissociated Zn-histidine complexes.

Pinpointing the source of a lunar meteorite: implications for the evolution of the Moon.

The lunar meteorite Sayh al Uhaymir 169 consists of an impact melt breccia extremely enriched with potassium, rare earth elements, and phosphorus [thorium, 32.7 parts per million (ppm); uranium, 8.6 ppm; potassium oxide, 0.54 weight percent], and adherent regolith. The isotope systematics of the meteorite record four lunar impact events at 3909 +/- 13 million years ago (Ma), approximately 2800 Ma, approximately 200 Ma, and <0.34 Ma, and collision with Earth sometime after 9.7 +/- 1.3 thousand years ago. With these data, we can link the impact-melt breccia to Imbrium and pinpoint the source region of the meteorite to the Lalande impact crater.