Unveiling the origins and transport processes of radioactive pollutants downstream from a former U-mine site using isotopic tracers and U-238 series disequilibrium.

High U concentrations (reaching up to 14,850 mg â‹… kg-1), were determined in soils and sediments of a wetland downstream of a former U mine in France. This study aims to identify the origin of radioactive contaminants in the wetland by employing Pb isotope fingerprinting, (234U/238U) disequilibrium, SEM, and SIMS observations. Additionally, information about U and 226Ra transport processes was studied using U-238 series disequilibrium. The results of Pb fingerprinting highlighted inherited material inputs of different U-mines with mainly two types of U-ores: i) pitchblende (UO2), and ii) parsonsite (Pb2(UO2)(PO4)2). Moreover, significant disequilibrium of (230Th/238U) and (226Ra/230Th) activity ratios highlighted the mobility of 238U and 226Ra in the wetland, primarily driven by the water table fluctuations. Finally, this work uncovered a limitation of Pb isotope fingerprinting in the case of parsonsite materials, as the high natural Pb content of this mineral may hide the uranogenic Pb signature in the samples.

Do transient hydrological processes explain the variability of strontium-90 activity in groundwater downstream of a radioactive trench near Chernobyl?

The Chernobyl Pilot Site (CPS) was created in 2000 in order to study radionuclide migration processes to the geosphere from radioactive material of the Red forest buried in a trench. In this article, the data collected in the CPS up to 2015 are analyzed to identify the links between hydrological conditions and release of strontium-90 (90Sr) from the trench. Then, a flow-and-transport model is used for simulating distribution of 90Sr both in the unsaturated and saturated zones downstream of the trench. The results show that the 90Sr activity in groundwater is strongly transient in time, due to the high inter-annual variability of both the recharge rate and the groundwater level (some particularly wet winters resulted in saturation of the bottom part of the trench). In addition, the parameters that govern the sorption of 90Sr in trench material appear to vary significantly in space (the retardation factor ranges from 10 to 50 depending on the location). This spatiotemporal variability could hide some critical processes, e.g., related to a long-term trend, and needs to be characterized through an appropriate sampling frequency.

Factorial kriging for estimating and mapping the geochemical background from in situ gamma dose rate measurements downstream of a former uranium mine.

A geostatistical approach is applied for extracting the geochemical background from gamma dose rate data acquired downstream of a former French uranium mining area. The exploratory data analysis shows that the spatial structure of the gamma dose rate consists of two components: a short isotropic component (10 m-range) that corresponds to the geochemical background; and a long anisotropic component (30-60 m-range) that corresponds to the drainage network features previously fed by the mine discharge water. The gamma dose rate on the whole area of interest was estimated and simulated (to deal with uncertainties) through a kriging of the measured values. The spatial component related to the geochemical background was then extracted through factorial kriging. The proportion of the gamma dose rate explained by the geochemical background according to factorial kriging is consistent within uncertainties with geochemical analyses performed on soil and sediment samples. This study thus highlights the potential of such geostatistical approaches for better exploiting radiometric data.

Estimation of fukushima radio-cesium deposits by airborne surveys: Sensitivity to the flight-line spacing.

After Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, airborne gamma-ray detection was used for regional mapping of soil contamination. For such surveys, the flight-line spacing is an important factor controlling the quality of contamination maps. In this study, cesium-137 (137Cs) ground activity is interpolated and mapped using ordinary kriging method; thereafter the error of interpolation is evaluated as a function of flight-line spacing. The analyses were conducted in six 20 km × 20 km test sites with distance of less than 80 km from the FDNPP. In each site, the ordinary kriging estimators were applied to different selections of flight-lines of decreasing density, then punctual and classification errors were calculated. It is demonstrated that these variables are highly correlated (r2 > 0.78): increasing the flight-line spacing for 1 km increases the errors from 3% to 9%, depending on the site location. Therefore, flight-line spacing could be designed as a function of acceptable error, determined in the monitoring objectives.

Combining geostatistics and simulations of flow and transport to characterize contamination within the unsaturated zone.

Characterization of contamination in soils or groundwater resulting from industrial activities is critical for site remediation. In this study, geostatistics and physically-based simulations are combined for estimating levels of contamination within the unsaturated zone. First, a large number of flow and transport simulations are run and their outputs are used to compute empirical non stationary variograms. Then, these empirical variograms, called numerical variograms and which are expected to reproduce the spatial variability of the contaminant plume better than a usual variogram model based on observations only, are used for kriging. The method is illustrated on a two-dimensional synthetic reference test case, with a contamination due to a point source of tritium (e.g. tritiated water). The diversity among the simulated tritium plumes is induced by numerous sets of hydraulic parameter fields conditioned by samples from the reference test case. Kriging with numerical variograms is then compared to ordinary kriging and kriging with an external drift: the results show that kriging with numerical variograms improves the estimates, all the more that few observations are available, underlining the interest of the method. When considering a relatively dense sampling scenario, the mean absolute error with kriging with numerical variograms is reduced by 52% compared to ordinary kriging and by 45% compared to kriging with an external drift. For a scarcer sampling, those errors are respectively reduced of 73% and 34%. However, the performance of the method regarding the classification into contaminated or not contaminated zones depends on the pollution threshold. Yet, the distribution of contamination is better reproduced by kriging with numerical variograms than by ordinary kriging or kriging with an external drift.

New Insights into Pb Isotope Fingerprinting of U-Mine Material Dissemination in the Environment: Pb Isotopes as a Memory Dissemination Tracer.

Stable Pb isotope ratios were measured and compared to U distributions in three soil cores located in a wetland highly impacted by water discharge of a former U-mine. Pb isotope ratios showed notable alignments in binary mixing plots, demonstrating the dissemination of radioactive-enriched material from the U-mine. Thanks to these alignments and to the measurement of the 204Pb isotope, a precise characterization of the Pb isotope composition of the U-ore was performed without the use of U-ore samples. The well-defined end-members with the help of a reevaluated isotope mixing model allowed the accurate determination of the radiogenic Pb percentages in the cores that were overall found to be >50%. Noncorrelated distributions of radiogenic 206Pb and U are observed in several of the wetland soil samples. They reveal postdepositional U redistribution explained by major U speciation changes due to redox cycling in the wetland. On the contrary, the radiogenic 206Pb showed no or little postdepositional mobility and thus can be considered to be a memory tracer of the dissemination of U-rich radioactive material: even after an important U loss, the radiogenic 206Pb is able to reveal past contamination by U-rich materials.

Spatial properties of soil analyses and airborne measurements for reconnaissance of soil contamination by 137Cs after Fukushima nuclear accident in 2011.

Following Fukushima nuclear disaster, several data gathering campaigns surveyed the radionuclide propagation in the environment. However, the acquired datasets do not have the same sampling dimension. For example, the airborne measurements are some sort of averaging over a circular field of view, beneath the sensor; while the soil analyses are much more punctual. The objective of this work is to compare the soil samples and an airborne survey to investigate whether these two datasets reflect the same spatial patterns or not. This is prerequisite for combining the multiresolution data to create and update the contamination map in a post-accidental situation. The analyses were performed on square tiles of 20 km side to study large- and small-dimension variations in 137Cs deposition. The former was modelled by fitting a plane (called trend) to the georeferenced data points; and the latter was modelled by computing the difference (called residual) between the trend and the initial data. Dip direction and dip angle of trends as well as minimum spatial correlation distance and anisotropy of residuals were computed for both the soil and airborne datasets and compared. Dip directions are compatible in 73% of the tiles and dip angles are generally close. Anisotropy directions are compatible in 49% of the tiles and minimum spatial correlation distances are significantly more marked for the airborne dataset. The soil samples and airborne measurements are therefore more in agreement in large-dimension (trend) rather than in small-dimension (residual) variations. More generally, both the datasets allow highlighting the main contamination plumes distinguishable because of high concentration values. The airborne dataset yet appears to be more powerful to quantify spatial correlations, which could be linked to the contamination mechanisms.

Occurrence of 1,1'-dimethyl-4,4'-bipyridinium (Paraquat) in irrigated soil of the Lake Chad Basin, Niger.

Increased use of agrochemical products to improve yields for irrigated crops in sub-Saharan Africa has been accompanied by a significant increase in the risk of environmental contamination. Detailed examples of the fate of pesticides after initial spreading on crop fields are scarce in tropical regions, where safe practices and related health risks are poorly understood by smallholder farmers. In the semi-arid environment of the Lake Chad Basin, SE Niger, both intrinsic properties of pesticides and extrinsic factors such as soil and climate helped to characterize processes leading to an accumulation of pesticides in soils. Analysis by HPLC-UV of a 6 m deep soil profile showed the presence of Paraquat at concentrations from 953 ± 102 µg kg(-1) to 3083 ± 175 µg kg(-1) at depths between 0.80 and 2.75 m below the land surface. Soil analysis revealed that up to approximately 15 % of the total soil matrix consists of smectites, a clay mineral capable of retaining cationic pesticides such as Paraquat, and a very low content of organic matter (<0.15 wt.% TOC). Paraquat could be stored and not bioavailable in a clayey barrier at approximately 2-m depth and therefore does not represent an immediate risk for populations or environment in this form. However, if the Paraquat application rate remains constant, the clayey barrier could reach a saturation limit within 150-200 years and 180-220 years if we consider a DT50 in soil of ~1,000 days (FAO). Consequently, it could lead to a deeper infiltration and so a pollution of groundwater. Such a scenario can represent a health risk for drinking water and for the Lake Chad, which is a major resource for this densely populated region of semi-arid Africa. Further analyses should focus on deeper layers and groundwater Paraquat contents to validate or invalidate the hypothesis of storage in this clay-rich layer.