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.

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.

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.

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.

Determination of 241Pu in nuclear waste slurries: a comparative study using LSC and ICP-MS.

(241)Pu was determined in slurry samples from a nuclear reactor decommissioning project at the Paul Scherrer Institute (Switzerland). To validate the results, the (241)Pu activities of five samples were determined by LSC (TriCarb and Quantulus) and ICP-MS, with each instrument at a different laboratory. In lack of certified reference materials for (241)Pu, the methods were further validated using the (241)Pu information values of two reference sediments (IAEA-300 and IAEA-384). Excellent agreement with the results was found between LSC and ICP-MS in the nuclear waste slurries and the reference sediments.

PU and NP analysis of soil and sediment samples with ICP-MS.

A method to analyse Pu and Np was optimised to achieve low detection limits and high sample throughput. Soil and sediment samples were ashed and digested with a borate fusion. After dissolving the melt in nitric acid, Pu and Np were separated on a TEVA extraction chromatopraphy column. It was measured with a sector field ICP-MS. Detection limits in soils and sediments as low as 1x10(-15)g/g for Pu and Np were achieved. The method was applied to reference materials, soil profiles from Switzerland and sediment samples from the river Yenisei (RU), where radioactive nuclides have been discharged.

Determination of U(IV) and U(VI) by ion chromatography-inductively coupled plasma mass spectrometry and its application to kinetic studies.

The ions normally formed by actinides in aqueous solutions by the oxidation states III-VI are M3-, M4+, MO2+ and MO2(+2), respectively. Oxidation state representatives such as Am3+, Th4+, NpO+ and UO+, which resist oxidation state changes, were used to investigate a method to separate the oxidised species (MO2 and MO2(2+)) from the reduced species (M3+ and M4+). With this method the hexavalent state of uranium could be separated from the tetravalent state of uranium in aqueous media in less than 8 min. Uranium concentrations down to 10(-9) M could be analysed without changing the redox composition during the separation. The oxidation kinetics of the tetravalent uranium for different hydrochloric acid concentrations was investigated. The measurements showed good agreement with values found in the literature, although the uranium concentrations were one million times lower.

Clients' characteristics as mediating variables in perception of counselors' social influence.

48 clients in a rehabilitation center viewed two 12-min, videotapes each, one depicting a counselor high in social influence and the other one of low influence. They then rated the counselors on the Counselor Rating Form and the Empathy subscale of the Barrett-Lennard Relationship Inventory. Black subjects and subjects at lower educational levels rated the counselor of low social influence significantly higher than did whites and better educated subjects on all measures. White subjects and subjects at higher educational levels rated the counselor of high social influence significantly higher on Trustworthiness and Empathy than did blacks and less educated subjects. Results are discussed in light of the research on clients' characteristics as mediating variables in the counseling process and outcome.