Determination of strontium radioisotopes in routine and emergency samples.

We present the radioanalytical strategies used for the determination of strontium radioisotopes in routine and emergency samples. While in routine monitoring, the main goal is to achieve limits of detection as low as possible. In emergency, priority is given to the rapid procurement of data about a contamination. The parameters accuracy, precision and detection limit of the radiochemical methods are shown. We present the results obtained over the past 22 years in proficiency tests and in the analysis of reference materials.

Isotopic signatures of plutonium and uranium at Bikar atoll, northern Marshall Islands.

We present plutonium (Pu) and uranium (U) isotopic fingerprints (or signatures) in environmental samples collected at Bikar Atoll. Bikar is the second -most northern atoll of the Republic of the Marshall Islands, and therefore an important reference point to evaluate the extension of the regional fallout from the Pacific Proving Grounds (PPG) in Bikini and Enewetak Atolls. Previous studies have shown that regional fallout from atmospheric nuclear weapon testing (NWT) in Bikini and Enewetak has resulted in elevated levels of fallout radionuclides in this atoll. In order to optimally interpret the isotopic fingerprints, we compare our results with data obtained in eleven certified reference materials, representing different contamination sources. As well as 238Pu, 239Pu, 240Pu, 241Pu, 238U and 235U, this study also encompasses less commonly reported radionuclides such as 242Pu, 244Pu and 236U. We show the importance of combining numerous fingerprints for improved assessment of the source of a nuclear contamination. In samples from Bikar, Pu and U isotope ratios were found to vary within narrow ranges. Pu and U fingerprints suggest that regional fallout from the Castle Bravo test in March 1954 was the main source of the contamination. This was further confirmed by two different age dating approaches that estimated 1954 as the year of the contamination. We demonstrate that use of an exponential function to approximate the yield of heavy radionuclides in thermonuclear explosions with increasing mass is a valid approach for estimating the age of a contamination. We show that, if sufficient radionuclide activity concentration measurement results with low uncertainties are available, this method is robust.

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.

Persistent Mercury Contamination in Shooting Range Soils: The Legacy from Former Primers.

Mercury (Hg) compounds were used in the past in primers for rifle and handgun ammunition. Despite its toxicity, little is known about the contamination of shooting-range soils with this metal. We present new data about the Hg contamination of surface soils from numerous shooting ranges of Switzerland. Our study demonstrates that Hg is measurable at high levels in surface soils from the shooting ranges. In three of the investigated ranges, concentrations above the maximum Swiss guidance value of Hg in soil of 500 µg kg-1 were measured. Since the use of mercury-containing ammunition was stopped in the 1960s, our results demonstrate the high persistence of Hg in soils and their slow recovery by natural mechanisms.

Long-term behavior of (90)Sr and (137)Cs in the environment: Case studies in Switzerland.

We present long-term records of the (137)Cs and (90)Sr activity concentrations in soil, grass and milk from two lowland and two alpine pastures of Switzerland. The data is used for better understanding the long-term behavior of these radionuclides in the environment. Transfer factors between compartments are used as qualitative indicators of the magnitude of transfer and as a way to compare different elements (e.g. Cs and Sr) in similar conditions. The long-term behavior was quantified by means of the effective half-life which integrates all processes that cause a decrease of activity in a given medium such as leaching, fixation, erosion and radioactive decay. Our study shows that (90)Sr is more likely transferred from alpine soil to grass than (137)Cs. This is explained by a stronger fixation of Cs in the soils. We observed higher transfers of (90)Sr to grass in soils with lower Ca concentrations, and vice versa. In contrast, the transfer of (137)Cs to grass was not affected by the variations of the K content in the soil. We provide evidence that shows that (137)Cs, after intake by dairy cattle, is more likely transferred to milk than (90)Sr. However, as the (90)Sr and Ca transfers to milk are influenced by parameters/processes that were not taken into account in our study, our result cannot be entirely validated. The effective half-lives of (137)Cs and (90)Sr in soil, grass and milk corresponded with previous estimates in alpine soils. We have found that processes other than radioactive decay are responsible for a major decrease of the (90)Sr activity in soil. For (137)Cs, on the other hand, radioactive decay is among the most relevant process. Our data shows to be of interest in studying the trends of behavior of radionuclides in alpine regions.

Historical trends of organochlorine pesticides in a sediment core from the Gulf of Batabanó, Cuba.

Sediments can be natural archives to reconstruct the history of pollutant inputs into coastal areas. This is important to improve management strategies and evaluate the success of pollution control measurements. In this work, the vertical distribution of organochlorine pesticides (DDTs, Lindane, HCB, Heptachlor, Aldrin and Mirex) was determined in a sediment core collected from the Gulf of Batabanó, Cuba, which was dated by using the (210)Pb dating method and validated with the (239,240)Pu fallout peak. Results showed significant changes in sediment accumulation during the last 40 years: recent mass accumulation rates (0.321 g cm(-2) yr(-1)) double those estimated before 1970 (0.15 g cm(-2) yr(-1)). This change matches closely land use change in the region (intense deforestation and regulation of the Colon River in the late 1970s). Among pesticides, only DDTs isomers, Lindane and HCB were detected, and ranged from 0.029 to 0.374 ng g(-1) dw for DDTs, from<0.006 to 0.05 ng g(-1) dw for Lindane and from<0.04 to 0.134 ng g(-1) dw for HCB. Heptachlor, Aldrin and Mirex were below the detection limits (∼0.003 ng g(-1)), indicating that these compounds had a limited application in the Coloma watershed. Pesticide contamination was evident since the 1970s. DDTs and HCB records showed that management strategies, namely the banning the use of organochlorine contaminants, led to a concentration decline. However, Lindane, which was restricted in 1990, can still be found in the watershed. According to NOAA guidelines, pesticides concentrations encountered in these sediments are low and probably not having an adverse effect on sediment dwelling organisms.

Radioactive and chemical contamination of the water resources in the former uranium mining and milling sites of Mailuu Suu (Kyrgyzstan).

An assessment of the radioactive and chemical contamination of the water resources at the former uranium mines and processing sites of Mailuu-Suu, in Kyrgyzstan, was carried out. A large number of water samples were collected from the drinking water distribution system (DWDS), rivers, shallow aquifers and drainage water from the mine tailings. Radionuclides and trace metal contents in water from the DWDS were low in general, but were extremely high for Fe, Al and Mn. These elements were associated with the particle fractions in the water and strongly correlated with high turbidity levels. Overall, these results suggest that water from the DWDS does not represent a serious radiological hazard to the Mailuu Suu population. However, due to the high turbidities and contents of some elements, this water is not good quality drinking water. Water from artesian and dug wells were characterized by elevated levels of U (up to 10 µg/L) and some trace elements (e.g. As, Se, Cr, V and F) and anions (e.g. Cl(-), NO3(-), SO4(2-)). In two artesian wells, the WHO guideline value of 10 µg/L for As in water was exceeded. As the artesian wells are used as a source of drinking water by a large number of households, special care should be taken in order to stay within the WHO recommended guidelines. Drainage water from the mine tailings was as expected highly contaminated with many chemicals (e.g. As) and radioactive contaminants (e.g. U). The concentrations of U were more than 200 times the WHO guideline value of 30 µg/L for U in drinking water. A large variation in (234)U/(238)U isotopic ratios in water was observed, with values near equilibrium at the mine tailings and far from equilibrium outside this area (reaching ratios of 2.3 in the artesian well). This result highlights the potential use of this ratio as an indicator of the origin of U contamination in Mailuu Suu.