[Show abstract][Hide abstract] ABSTRACT: Measurements of radionuclides (RNs) in air made worldwide following the Fukushima accident are quantitatively compared with air and soil measurements made in Japan. Isotopic ratios RN:(137)Cs of (131)I, (132)Te, (134,136)Cs, are correlated with distance from release. It is shown, for the first time, that both within Japan and globally, ratios RN:(137)Cs in air were relatively constant for primarily particle associated radionuclides ((134,136)Cs; (132)Te) but that (131)I shows much lower local (<80 km) isotope ratios in soils relative to (137)Cs. Derived isotope ratios are used to reconstruct external dose rate during the early phase post-accident. Model "blind" tests show more than 95% of predictions within a factor of two of measurements from 15 sites to the north, northwest and west of the power station. It is demonstrated that generic isotope ratios provide a sound basis for reconstruction of early-phase external dose rates in these most contaminated areas.
[Show abstract][Hide abstract] ABSTRACT: It is shown which information can be extracted from the monitoring of radionuclides emitted from the Fukushima Dai-ichi nuclear power plant and transported to Europe. In this part the focus will be on the analysis of the concentration ratios. While (131)I, (134)Cs and (137)Cs were reported by most stations, other detected radionuclides, reported by some, are (95)Nb, (129m)Te, (132)Te, (132)I, (136)Cs and (140)La. From their activity ratios a mean burn-up of 26.7 GWd/t of the fuel from which they originated is estimated. Based on these data, inventories of radionuclides present at the time of the accident are calculated. The caesium activity ratios indicate emissions from the core of unit 4 which had been unloaded into the fuel storage pool prior to the accident.
Journal of Environmental Radioactivity 01/2012; 114:35-40. · 3.67 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Radionuclides emitted from the Fukushima I nuclear power plant have been detected in air all over Europe. Concentrations remained far below levels which could have caused radiological concern: probably the committed thyroid dose due to inhalation remained below about 1 μSv (for 10 y children), within the investigated region. They provided, however, a spatio-temporal signal which could be used to develop and test tools to provide additional information on the large-scale situation (Europe-wide, in this case) during a nuclear emergency. In this part we discuss the spatial distribution of the contaminated air masses over Europe. Using (131)I as an example, we present a method to construct maps of the time-cumulated (131)I concentration in air and of the peak concentrations. Procedures to deal with the statistical limitations of a data set stemming from different monitoring schemes are discussed. As over all results, the mean (over the investigated region) cumulated concentration of particular (131)I is estimated about 9 mBq d/m(3), with observed maximum of about 23 mBq d/m(3). The probability that much higher concentrations occurred at unsampled locations, than have been observed anywhere, is assessed low, e.g. about 2.5% for the cumulated (131)I(part.) concentration to exceed 30 mBq d/m(3). Our method can be used in nuclear emergencies for providing spatial analyses if radionuclide concentrations of health concern are detected by atmospheric monitoring stations. We suggest considering such methods of data harmonization if synoptic assessment based on heterogeneous datasets is attempted.
Journal of Environmental Radioactivity 01/2012; 114:22-34. · 3.67 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Facies analysis, magnetic susceptibility, and analysis of grain size, TOC content and isotopes (137Cs, 210Pb, 226Ra, 228Ra, and 238U concentrations) were used to determine the history of the modern deposits of the Brno reservoir. The sedimentary succession
can be subdivided into two main units. The lower unit is formed predominantly by medium- to coarse-grained silty sands and
is interpreted as a fluvial succession deposited before the Svratka River was dammed. The upper unit consists of brownish
planar laminated silts and rarely of clayey or sandy silts and is interpreted as a product of the reservoir deposition. The
concentrations of 238U reflect the history of uranium mining in the upper part of the Svratka River catchment. As a consequence, 210Pb radionuclide concentrations cannot be used for establishing a sediment chronology. Concentrations of 137Cs show two marked peaks, the upper of which is attributed to the Chernobyl reactor accident in 1986, and the lower one is
attributed to the maximum rate of atomic weapons testing in 1963. From these peaks, mean depositional rates of 3.2cmyear−1 for the time period of 1986–2007 and of 3.4cmyear−1 between 1963 and 1986 are calculated. Based on the known age of the reservoir, which was constructed in 1939, we can also
calculate mean depositional rate for the time period of 1939–1963, which is 3.1cmyear−1.
KeywordsReservoir deposits-Radiometric dating-Depositional rate-Hydrological changes-Human impact
Journal of Paleolimnology 01/2011; 45(1):41-55. · 2.21 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: For aquatic sediments, the use of (210)Pb originating from the decay of atmospheric (222)Rn is a well-established methodology to estimate sediment ages and sedimentation rates. Traditionally, the measurement of (210)Pb in soils and sediments involved laborious and time-consuming radiochemical separation procedures. Due to the recent development of advanced planar ('n-type') semi-conductors with high efficiencies in the low-energy range which enable the gamma-spectrometric analysis of the 46.5 keV decay line of (210)Pb, sediment dating using this radionuclide has gained renewed interest. In this contribution, potentials and limitations of the (210)Pb methodology and of the models used for estimating sediment ages and sedimentation rates are discussed and illustrated by examples of freshwater and marine sediments. Comparison with the use of (137)Cs shows that the information which may be gained by these two tracers is complementary. As a consequence, both radionuclides should be used in combination for dating of recent sediments. It is shown that for various sedimentation regimes additional information from other sources (e.g. sediment lithology) may be needed to establish a reliable chronology. A strategy for sediment dating using (210)Pb is recommended.
Journal of Environmental Radioactivity 12/2010; 102(5):490-4. · 3.67 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Samples of pasture vegetation, mainly Trifolium pratensis, were collected at the Botanic Garden of the University of Bologna during the period 1998-2000 and measured by gamma-spectrometry for determining thoron progeny. Concentrations of (212)Pb were between 1.5 and 20 Bq m(-2), with individual peaks up to 70 Bq m(-2). Soil samples were collected at the same location and physically characterised. Their chemical composition (particularly Th and U) was determined by X-ray fluorescence spectroscopy. Lead-212 on plants mainly originates from dry and wet deposition of this isotope generated in the lower atmosphere by the decay of its short-lived precursor (220)Rn, which is produced in the upper soil layers as a member of the natural thorium decay chain and exhales into the atmosphere. Concentrations of (220)Rn in the atmosphere depend on (1) the amount of Th present in soil, (2) the radon fraction which escapes from the soil minerals into the soil pore space, (3) its transport into the atmosphere, and (4) its redistribution within the atmosphere. The mobility of radon in soil pore space can vary by orders of magnitude depending on the soil water content, thus being the main factor for varying concentrations of (220)Rn and (212)Pb in the atmosphere. We present a simple model to predict concentrations of thoron in air and its progeny deposited from the atmosphere, which takes into account varying soil moisture contents calculated by the OPUS code. Results of this model show close agreement with our observations.
Journal of Environmental Radioactivity 11/2010; 101(11):992-1001. · 3.67 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Measurements of low-level radioactivity often give results of the order of the detection limit. For many applications, interest is not only in estimating activity concentrations of a single radioactive isotope, but focuses on multi-isotope analyses, which often enable inference on the source of the activity detected (e.g. from activity ratios). Obviously, such conclusions become questionable if the measurement merely gives a detection limit for a specific isotope. This is particularly relevant if the presence of an isotope, which shows a low signal only (e.g. due to a short half-life or a small transition probability), is crucial for gaining the information of interest. This paper discusses a new approach which has the potential to solve these problems. Using Bayesian statistics, a method is presented which allows statistical inference on nuclide ratios taking into account both prior knowledge and all information collected from the measurements. It is shown that our method allows quantitative conclusion to be drawn if counts of single isotopes are low or become even negative after background subtraction. Differences to the traditional statistical approach of specifying decision thresholds or detection limits are highlighted. Application of this new approach is illustrated by a number of examples of environmental low-level radioactivity measurements. The capabilities of our approach for spectrum interpretation and source identification are demonstrated with real spectra from air filters, sewage sludge and soil samples.
Journal of Environmental Radioactivity 05/2009; 100(6):484-8. · 3.67 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Literature data on numerical values obtained for the parameters of the two most popular models for simulating the migration of radionuclides in undisturbed soils have been compiled and evaluated statistically. Due to restrictions on the applicability of compartmental models, the convection-dispersion equation and its parameter values should be preferred. For radiocaesium, recommended values are derived for its effective convection velocity and dispersion coefficient. Data deficiencies still exist for radionuclides other than caesium and for soils of non-temperate environments.
Journal of Environmental Radioactivity 12/2008; 100(9):716-20. · 3.67 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Radioecological assessment models are necessary tools for estimating the radiation exposure of humans and non-human biota. This paper focuses on factors affecting their predictive accuracy, discusses the origin and nature of the different contributions to uncertainty and variability and presents approaches to separate and quantify them. The key role of the conceptual model, notably in relation to its structure and complexity, as well as the influence of the number and type of input parameters, are highlighted. Guidelines are provided to improve the degree of reliability of radioecological models.
Applied Radiation and Isotopes 06/2008; 66(11):1750-3. · 1.18 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Ratios of radionuclide activity concentrations are often used to identify sources of small traces of radioactivity in environmental samples. A new approach is presented to consider statistical uncertainties and their impact on decisions based on nuclide ratios particularly for cases where nuclide ratios are calculated from measurements close to or below detection limit. It is pointed out that decision threshold and detection limit are adequate for decisions on the presence of a single nuclide but not necessarily on decisions on nuclide ratios. A statistical analysis based on a Bayesian approach is presented which allows inference on probabilities of nuclide ratio values taking into account jointly the information available for all radionuclides of interest. Examples are discussed to demonstrate the improvements of this approach in spectrum analysis and in source identification. As an important case the detection of Xenon isotopes (135Xe, 133mXe, 133Xe and 131mXe) that are relevant for detecting underground nuclear explosions in the context of the verification of the Comprehensive Nuclear Test-Ban Treaty (CTBT) is discussed. Nuclide ratios are crucial in order to distinguish civil releases from CTBT-relevant sources. A new method is presented for graphical evaluation of the xenon isotope measurements and for assigning potential sources using the statistical approach proposed in this paper.
Nuclear Instruments and Methods in Physics Research Section A Accelerators Spectrometers Detectors and Associated Equipment 01/2008; 594(3):400-406. · 1.14 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: 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.
Journal of Environmental Radioactivity 02/2006; 91(1-2):41-72. · 2.12 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Lichens were collected in France in the surroundings of a military nuclear facility in Burgundy, near the la Hague reprocessing plant and in an area away from any direct source of contamination. Organically bound tritium (OBT) has been analysed on 18 samples and radiocarbon on 11. It appeared that on the most contaminated spots, the OBT activity in lichens was higher than the background by a factor of 1000 and was still a factor 10-100 at a distance of 20 km from the source. Radiocarbon from la Hague could be traced by lichens. The slow metabolism of lichens makes them suitable for the follow-up of (3)H and (14)C, which have been incorporated by photosynthesis.
Science of The Total Environment 06/2004; 323(1-3):253-62. · 3.26 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: For agriculturally used areas, which are contaminated by the debris from a nuclear accident, the use of chemical amendmends (e.g. potassium chloride and lime) is among the most common soil-based countermeasures. These countermeasures are intended to reduce the plant uptake of radionuclides (mainly 137Cs and 90Sr) by competitive inhibition by chemically similar ions. So far, the impacts of countermeasures on soil solution composition - and thus, their effectiveness - have almost exclusively been established experimentally, since they depend on mineral composition and chemical characteristics of the soil affected. In this study, which focuses on caesium contamination, the well-established code PHREEQC was used as a geochemical model to calculate the changes in the ionic compositions of soil solutions, which result from the application of potassium or ammonium in batch equilibrium experiments. The simple ion exchange model used by PHREEQC was improved by taking into account selective sorption of Cs+, NH4+ and K+ by clay minerals. Calculations were performed with three different initial soil solution compositions, corresponding to particular soil types (loam, sand, peat). For loamy and sandy soils, our calculational results agree well with experimental data reported by Nisbet (Effectiveness of soil-based countermeasures six months and one year after contamination of five diverse soil types with caesium-134 and strontium-90. Contract Report NRPB-M546, National Radiation Protection Board, Chilton, 1995.). For peat, discrepancies were found indicating that for organic soils a reliable set of exchange constants of the relevant cations still has to be determined experimentally. For cesium, however, these discrepancies almost disappeared if selective sites were assumed to be inaccessible. Additionally, results of sensitivity analyses are presented by which the influence of the main soil parameters on Cs+ concentrations in solution after soil treatment has been systematically studied. It is shown that calculating the impacts of soil-based chemical countermeasures on soil solution chemistry using geochemical codes such as PHREEQC offers an attractive alternative to establishing these impacts by often time-consuming and site-specific experiments.
Science of The Total Environment 05/2002; 289(1-3):83-95. · 3.26 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Soil-to-plant transfer factors are commonly used to estimate the food chain transfer of radionuclides. Their definition assumes that the concentration of a radionuclide in a plant relates linearly solely to its average concentration in the rooting zone of the soil. However, the large range of transfer factors reported in the literature shows that the concentration of a radionuclide in a soil is not the only factor influencing its uptake by a plant. With emphasis on radiocesium and -strontium, this paper reviews the effects of competition with major ions present in the soil-plant system, the effects of rhizosphere processes and soil micro-organisms on bioavailability, the factors influencing transport to and uptake by roots and the processes affecting long-term uptake rates. Attention is given to summarizing the results of recent novel electrophysiological and genetic techniques which provide a physiologically based understanding of the processes involved in the uptake and translocation of radiocesium and -strontium by plants.
Journal of Environmental Radioactivity 02/2002; 58(2-3):97-112. · 2.12 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Lichens were used as biomonitors of Chernobyl fallout 137Cs, of cosmogenic 7Be and of radioactive members of the natural uranium and thorium decay chains. Samples were taken from two locations in France, including lichens sampled at different distances of a coal fired power plant and close to a uranium ore processing waste disposal site. All samples were analyzed gamma-spectrometrically after equilibrium concentrations of short-lived isotopes had been attained. Activity concentrations of the members of the uranium and thorium decay chains in Parmelia sulcata sampled 1994 decrease with distance from the plant, whereas in lichens taken at the waste disposal site a decrease with time was observed. Comparison of 7Be activity concentrations measured in lichens with atmospheric deposition rates confirms that P. sulcata can be used as a quantitative biomonitor of radioactive trace substances. Retention half-lives calculated with a simple one-compartment model are 2.6 +/- 1.2 years for cesium, which was detected in all samples even more than a decade after the Chernobyl accident, and of 0.7 (+/- 0.1) to 3.3 (+/- 0.7) years for lead. Consequences of our results for model identifiability and parameter estimation of a two-compartment model are discussed.
[Show abstract][Hide abstract] ABSTRACT: Fungi sampled in three areas in France were analyzed by gamma-spectrometry for their concentrations of 134Cs, 137Cs, 210Pb and 226Ra. In most of the samples radioactive cesium was detected with a maximum of 2860 Bq kg-1 (dry wt.). Activity concentrations of 210Pb were in the range < 1.76-36.5 Bq kg-1 (dry wt.). Activity concentrations of 226Ra were consistently lower, often by one order of magnitude. Models are developed to estimate the contributions of atmospheric 210Pb deposited onto the fruit bodies to the measured 210Pb concentrations and of the uptake of 222Rn soluted in soil pore water which subsequently decays into 210Pb. It is shown that both pathways are of only minor importance. Comparison with the soil-mushroom concentration ratios of stable lead, which were determined for some of the samples, confirmed that 210Pb in mushrooms mainly originates from direct uptake of 210Pb present in the soil. Despite of the high concentrations of 137Cs detected in most of the mushrooms, radiation doses to individuals due to mushroom consumption are dominated by 210Pb for the majority of the edible mushrooms sampled.
Science of The Total Environment 11/1998; 222(1-2):63-70. · 3.26 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: An important source of uncertainty in predictions of numerical simulation codes of environmental transport processes arises from the assumptions made by the user when interpreting the model and the scenario to be assessed. This type of uncertainty was examined systematically in this study and was compared with uncertainty due to varying parameter values in a code. Three terrestrial food chain codes that are driven by deposition of radionuclides from the atmosphere were used by up to ten participants to predict total deposition of 137Cs and concentrations on pasture and in milk for two release scenarios. Collective uncertainty among the predictions of the ten users for concentrations in milk calculated for one scenario by one code was a factor of 2000, while the largest individual uncertainty was 20 times lower. Choice of parameter values contributed most to user-induced uncertainty, followed by scenario interpretation. Due to the significant disparity in predictions, it is recommended that assessments should not be carried out alone by a single code user.
Journal of Environmental Radioactivity 01/1998; 42(2):177-190. · 2.12 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: The applicability of multi-compartmental models to describe the transport of radioactive trace substances in soil is reconsidered. It is shown that the widely used serial compartmental model implicitly assumes convection-dominated flow and has to be replaced by a model with backflow for diffusion-controlled transport. A compartmental approach provides a valid model of the transport processes only if the number of compartments is set to a specific value which is determined by the physical flow conditions in the soil studied. It is demonstrated that describing diffusional transport by the commonly used serial compartmental model results in apparently time-dependent residence times. Modifications of compartment models made in order to account for complex sorption behavior of the radionuclides are discussed. Consequences for the design and interpretation of field studies are outlined.
Journal of Environmental Radioactivity 01/1998; 38(3):339-352. · 2.12 Impact Factor