Radionuclides in sediments of the Aare and Rhine river system: Fallouts, discharges, depth-age relations, mass accumulation rates and transport along the river.

The Aare-Rhine river system with its four nuclear power plants on the banks of these rivers and with its intermediate lakes and reservoirs provide the unique chance to analyze the input of radioactivity into the system thereby furnishing information on the sources, to analyze the transport within the sediment and along the rivers, and to refine unsupported 210Pb dating validated by known discharge maxima. At three locations (Lake Biel, Klingnau Reservoir, old branch of the Rhine) in the Aare and Rhine rivers system downstream of the older nuclear power plants (NPPs) Mühleberg and Beznau, the vertical distributions of 137Cs, 210Pb, 214Pb, 214Bi, 40K, 7Be, 239Pu, 240Pu, 241Am, and 237Np in sediment cores were determined. Depth-age relations using the excess 210 Pb were established with the raw and with the piecewise Constant Rate Supply (CRS) models. A comparison of the piecewise CRS method with the imprints of known discharges showed differences of up to two years. Besides typical 137Cs signals (about 100 Bq∙kg-1) from the atmospheric nuclear weapons testing (NWT) and the Chernobyl fallouts, imprints of known 137Cs discharges (10-70 Bq∙kg-1) from the NPPs were found in the sediments. The 237Np distributions (6-10 Bq∙kg-1) essentially follow the 137Cs NWT distributions. In the sediment downstream the NPP Mühleberg (Lake Biel) a239Pu distribution (<3 Bq∙kg-1) was found, which was solely due to the NWT fallout. Downstream the NPP Beznau (Klingnau Reservoir and an old branch of the Rhine), besides the NWT distribution, also imprints of 239Pu discharges (up to 7 Bq∙kg-1) were found within the time interval 1963 to 1986.240Pu/239Pu ratios revealed that the burn-up times of the nuclear fuel in the NPP (235U enrichment of 3.5%), from which the discharges stem, should be about 1 year or less. A comparison between the calculated and the measured 137Cs/239Pu ratio revealed no large discrepancies for the Lake Biel and Rhine positions, but in the Klingnau distribution, the calculated 137Cs/239Pu ratio is one order of magnitude larger than the measured one. The reason could be either a natural uranium research reactor as the source, or strong, short-range 239Pu precipitation after the discharge from the Beznau NPP. The largest 239Pu peak in the Rhine sediment (1968/70) corresponds to no major peak in the Klingnau sediment. For the NPP Mühleberg discharge of 1982 the ratio of the 137Cs deposition in sediments from Lake Biel, Klingnau Reservoir and the Rhine river is about 1 : 0.5 : 2.9. For the 1977/78 239Pu deposition the ratio is 1 : 0.02, for the Klingnau Reservoir and the Rhine sediments, respectively. These numbers indicate a long-range transport of Cs and a rather short-range transport of Pu.

Dating of recent sediments from Lago Maggiore and Lago di Lugano (Switzerland/Italy) using 137Cs and 210Pb.

This paper presents the results of 137Cs and 210Pb dating of sediments from the northern and western basins of Lago Maggiore and the southern basin of Lago di Lugano. Vertical distributions of 137Cs in sediment cores taken in 2017/18 were compared to those of the sediment cores taken almost two decades ago at the same positions. This comparison showed that 137Cs peaks do not alter their shape significantly over time and 137Cs remains a reliable time-marker for many decades. 210Pb dating using for the first time the piecewise "constant rate supply" (CRSPW) model constrained with 137Cs time-markers is performed for sediment cores of Lago Maggiore and Lago di Lugano. "Event-linked" mass accumulation rates (MARs) were derived from the CRSPW model. In combination with the dry bulk density, organic matter content, 40K and 210Pb activity concentrations, these "event-linked" MARs were used for the identification of one or more event layers (turbidites, detrital layers) in 1-cm thick sediment samples. "Continuous" mean MARs which are independent of the event layers were estimated: in Lago Maggiore sediment cores they are 0.066-0.090 g cm-2 yr-1; in Lago di Lugano they vary in the range of 0.032-0.057 g cm-2 yr-1 with higher values in the time interval 1963-1986 as compared to 1986-present.

Long-term distribution and migration of 137Cs in a small lake ecosystem with organic-rich catchment: A case study of Lake Vorsee (Southern Germany).

In the shallow eutrophic Lake Vorsee with an organic-rich catchment the 137Cs activity concentration in water samples (n = 250) and different fish species (n = 631) was determined for a period of 30 years starting soon after the Chernobyl fallout. To understand the distribution and migration of 137Cs in the ecosystem of Lake Vorsee, also the 137Cs inventory in soils of the catchment area, in sediments, in suspended matter, in water plants, as well as its vertical distribution in soils and sediments were studied. The time dependency of the 137Cs activity concentration in water and fish was modelled with a compartment model (AQUASCOPE) as well as with the sum of two exponential functions. Results for effective half-lives of 137Cs in water are Teff1  = 1.2 a and Teff2  = 7.2 a; for small cyprinidae Teff1  = 0.6 a and Teff2  = 8.9 a; and for pike Teff1  = 1.4 a and Teff2  = 12.1 a. The vertical distribution of 137Cs activity concentration in soils was described by a partial differential equation (diffusion constant D = (1.05 ±â€¯1.16) cm2⋅a-1 and convection speed v = (0.14 ±â€¯0.07) cm⋅a-1) and its distribution in sediments by a system of two coupled partial differential equations (fixation rate f = 2.0 d-1; distribution coefficient Kdex = (543 ±â€¯140) L⋅kg-1; sedimentation rate RS = (0.030 ±â€¯0.010) g⋅(cm2⋅a)-1; bioturbation constant Dbio, decreasing linearly with depth with Dbioabs = (3.3 ±â€¯1.0) cm2⋅a-1 at the surface). According to the extended AQUASCOPE model, the following fractions of the total 137Cs inventory were found in the different compartments of the lake ecosystem in 2016: 9.0⋅10-1 in soils of the catchment area, 1.0⋅10-1 in sediments, 5.5⋅10-5 in water, 1.5⋅10-5 in suspended matter, 1.3⋅10-5 in watermilfoil, and 1.6⋅10-6 in fish.

Dating of sediments from four Swiss prealpine lakes with (210)Pb determined by gamma-spectrometry: progress and problems.

In this paper the most important problems in dating lake sediments with unsupported (210)Pb are summarized and the progress in gamma-spectrometry of the unsupported (210)Pb is discussed. The main topics of these studies concern sediment samples preparation for gamma-spectrometry, measurement techniques and data analysis, as well as understanding of accumulation and sedimentation processes in lakes. The vertical distributions of artificial ((137)Cs, (241)Am, (239)Pu) and natural radionuclides ((40)K, (210,214)Pb, (214)Bi) as well as stable trace elements (Fe, Mn, Pb) in sediment cores from four Swiss lakes were used as examples for the interpretation, inter-comparison and validation of depth-age relations established by three (210)Pb-based models (CF-CSR, CRS and SIT). The identification of turbidite layers and the influence of the turbidity flows on the accuracy of sediment dating is demonstrated. Time-dependent mass sedimentation rates in lakes Brienz, Thun, Biel and Lucerne are discussed and compared with published data.

Influence of fertilizing on the (137)Cs soil-plant transfer in a spruce forest of Southern Germany.

Fertilization with 2.5t/ha limestone: (83% CaCO(3), 8% MgO, 6% K(2)O, 3% P(2)O(5)) reduces the (137)Cs transfer from spruce forest soil into plants like fern (Dryopteris carthusiana) and blackberry (Rubus fruticosus) by a factor of 2-5 during at least 11 years as measured by the aggregated transfer factor T(ag). In 1997 and 2006 these results were confirmed by additional measurements of the (137)Cs transfer factor TF, related to the root zone (O(h) horizon), which were explained by the selective sorption of (137)Cs in the root zone by measurements of the Radiocaesium Interception Potential (RIP) in fertilized (RIP>179meq/kg) and non-fertilized soils (RIP<74meq/kg).

Seasonality of 137Cs in roe deer from Austria and Germany.

Empirical data on the (137)Cs activity concentration in meat of roe deer (Capreolus capreolus) roaming in 3 spruce forest areas and one peat bog area are presented and compared. They cover time series of nearly 20 years after a spike contamination in 1986 originating from Chernobyl. A model is presented which considers three soil compartments to describe the change of the availability of (137)Cs with time. The time-dependency of the (137)Cs activity concentration in meat of roe deer is a combination of two components: (1) an exponential decay and (2) a peak in the second half of each year during the mushroom season. The exponential decay over the years can be described by a sum of two exponential functions. The additional transfer of (137)Cs into roe deer during the mushroom season depends on precipitation. On the peat bog the (137)Cs activity concentration in roe deer is higher and more persistent than in spruce forest.

Migration and bioavailability of (137)Cs in forest soil of southern Germany.

To give a quantitative description of the radiocaesium soil-plant transfer for fern (Dryopteris carthusiana) and blackberry (Rubus fruticosus), physical and chemical properties of soils in spruce and mixed forest stands were investigated. Of special interest was the selective sorption of radiocaesium, which was determined by measuring the Radiocaesium Interception Potential (RIP). Forest soil and plants were taken at 10 locations of the Altdorfer Wald (5 sites in spruce forest and 5 sites in mixed forest). It was found that the bioavailability of radiocaesium in spruce forest was on average seven times higher than in mixed forest. It was shown that important factors determining the bioavailability of radiocaesium in forest soil were its exchangeability and the radiocaesium interception potential (RIP) of the soil. Low potassium concentration in soil solution of forest soils favors radiocaesium soil-plant transfer. Ammonium in forest soils plays an even more important role than potassium as a mobilizer of radiocaesium. The availability factor - a function of RIP, exchangeability and cationic composition of soil solution - characterized reliably the soil-plant transfer in both spruce and mixed forest. For highly organic soils in coniferous forest, radiocaesium sorption at regular exchange sites should be taken into account when its bioavailability is considered.

Ecological half-lives of 90Sr and 137Cs in terrestrial and aquatic ecosystems.

This paper describes the long-term behaviour of (90)Sr and (137)Cs in foods, feeds and a variety of environmental media. The long-term behaviour is quantified by means of the ecological half-life which integrates all processes that cause a decrease of activity in a given medium such as leaching, fixation and erosion. A large number of long-term time series of concentrations of radiocaesium and radiostrontium in these media have been identified and re-evaluated using a standardised statistical procedure to establish reference data sets of ecological half-lives. By example of undisturbed soils and marine water bodies it is shown that the ecological half-life concept is questionable if the distribution of the radionuclide of interest within the medium studied is non-uniform and if mixing and transport processes within this medium, therefore, are of considerable importance during the time period of observation.

Comparative study of 137Cs partitioning between solid and liquid phases in Lakes Constance, Lugano and Vorsee.

The methodology for estimating radiocaesium distribution between solid and liquid phases in lakes is applied for three prealpine lakes: Lake Constance (Germany), Lake Lugano (Switzerland) and Lake Vorsee (Germany). It is based on use of the exchangeable distribution coefficient and application of the exchangeable radiocaesium interception potential (RIPex). The methodology was tested against experimental data. Good agreement was found between estimated and measured 137Cs concentrations in Lake Constance and Lake Lugano, whereas for Lake Vorsee a discrepancy was found. Bottom sediments in Lake Vorsee are composed mainly of organic material and probably cannot be described in terms of the specific sorption characteristics attributed to illitic clay minerals.

Time-dependence of the radiocaesium contamination of roe deer: measurement and modelling.

In spruce forest and peat bog, the migration of 137Cs from soil to plants, fungi, roe deer and consumers has been surveyed. In spruce forest the 137Cs activity concentration in roe deer decreases slowly with time and has superimposed periodic maxima in autumn which are correlated with the mushroom season. The decrease with time can be described by an effective half-life of 3.5 yr caused by a fraction of the 137Cs in the soil becoming unavailable for green grazing plants with time. The additional transfer of 137Cs into roe deer meat during the mushroom season depends on precipitation in July, August and September which also determines the yield of fungi in autumn. Our model confirms the assumption that fungi also have access to a fraction of the 137Cs in the soil which is unavailable for green plants. On peat bog the 137Cs activity concentration in roe deer is higher than in spruce forest and its effective half-life is about 17 yr, due to reversible binding of 137Cs to organic matter in the peat bog.