Some considerations on the dependence to numerical schemes of Lagrangian radionuclide transport models for the aquatic environment.

Lagrangian models present several advantages over Eulerian models to simulate the transport of radionuclides in the aquatic environment in emergency situations. A radionuclide release is simulated as a number of particles whose trajectories are calculated along time and thus these models do not require a spatial discretization (although it is always required in time). In this paper we investigate the dependence of a Lagrangian model output with the grid spacing which is used to calculate concentrations from the final distribution of particles, with the number of particles in the simulation and with the interpolation schemes which are required because of the discrete nature of the water circulation data used to feed the model. Also, a Lagrangian model may describe the exchanges of radionuclides between phases (liquid and solid), which is done in terms of transition probabilities. The dependence of these probabilities with time step is analyzed as well. It was found that the optimum grid size used to calculate concentrations should be carefully checked, and that temporal interpolation is more significant than spatial interpolation to obtain a more accurate solution. A method to estimate the number of particles required to have a certain accuracy level is proposed. Finally, it was found that for low sediment concentrations and small radionuclide kd, exact equations for the transition probabilities should be used; and that phase transitions introduce a stability condition as in Eulerian models.

Development of a dynamic food chain model for assessment of the radiological impact from radioactive releases to the aquatic environment.

The software tool POSEIDON-R was developed for modelling the concentration of radionuclides in water and sediments as well as uptake and fate in the aquatic environment and marine organisms. The software has been actively advanced in the aftermath of the Fukushima Dai-ichi accident. This includes development of an uptake model for the benthic food chain, a kinetic-allometric compartment model for fish and recent advancements for the application of 3H. This work will focus on the food chain model development and its extension to key artificial radionuclides in radioecology such as 3H. Subsequently, the model will be applied to assess the radiological dose for marine biota from 3H, 90Sr, 131I, 134Cs and 137Cs released during and after the Fukushima Dai-ichi accident. The simulation results for 3H, 90Sr, 131I, 134Cs and 137Cs obtained from the coastal box (4-4 km) located at the discharge area of the Fukushima Dai-ichi NPP, and the surrounding regional box (15-30 km) are compared with measurements. The predictions are by and large consistent with experimental findings, although good validation for 3H, 90Sr and 131I is challenging due to lack of data. On the basis of the model predictions a dose assessment for pelagic and benthic fish is carried out. Maximum absorbed dose rates in the coastal box and the regional box are respectively 6000 and 50 µGy d-1 and are found in the pelagic non-piscivorous fish. Dose rates exceeding ICRP's derived consideration levels of 1 mGy d-1 are only found in the direct vicinity of the release and shortly after the accident. During the post-accidental phase absorbed dose rates consistently fall to levels where no deleterious effects to the marine biota are expected. The results also demonstrate the prolonged dose rate from 134Cs and 137Cs, particularly for benthic organisms, due to caesium's affinity with sediment, re-entry of caesium from the sediment into the food chain and external exposure from its high energetic gamma emissions. Uptake of non-organic tritium (HTO) and organically bound tritium (OBT) is modelled and shows some accumulation of OBT in the marine organism. However, dose rates from tritium, even during the accident, are low.

Fukushima 137Cs releases dispersion modelling over the Pacific Ocean. Comparisons of models with water, sediment and biota data.

A number of marine radionuclide dispersion models (both Eulerian and Lagrangian) were applied to simulate 137Cs releases from Fukushima Daiichi nuclear power plant accident in 2011 over the Pacific at oceanic scale. Simulations extended over two years and both direct releases into the ocean and deposition of atmospheric releases on the ocean surface were considered. Dispersion models included an embedded biological uptake model (BUM). Three types of BUMs were used: equilibrium, dynamic and allometric. Model results were compared with 137Cs measurements in water (surface, intermediate and deep layers), sediment and biota (zooplankton, non-piscivorous and piscivorous fish). A reasonable agreement in model/model and model/data comparisons was obtained.

The POSEIDON-R compartment model for the prediction of transport and fate of radionuclides in the marine environment.

A detailed description of the advanced version of compartment model POSEIDON-R for the prediction of transport and fate of radionuclides in the marine environment is given. The equations of transfer of radionuclides in the water and bottom sediment compartments along with the dynamical food chain model are presented together with dose module to assess individual and collective doses to the population due to the regular and accidental releases of radionuclides. The method for the numerical solution of model equations is also presented. The modelling results for the northeast Atlantic shelf seas were compared with measurements of 137Cs. •The three-dimensional compartment model POSEIDON-R describes the transfer of radionuclides and their daughter products in marine environment as a results of regular or accidental releases. This includes any transfer through the water column and sediments.•The model is complemented by a dynamic food chain model for transfer of radioactivity in pelagic and benthic food webs.•The dose module in the model calculates internal and external doses for humans and non-human biota.

The marine kd and water/sediment interaction problem.

The behavior of marine distribution coefficients is analyzed with the help of numerical experiments and analytical solutions of equations describing kinetic models for uptake/release of radionuclides. The difficulties in measuring true kd in a marine environment perturbed by an external radionuclide source are highlighted. Differences between suspended matter and bed sediment kd are analyzed. The performances of different kinetic models (1-step/2step; single-layer/multi-layer) are studied in model/model and model/experiment comparisons. Implications for the use of models to assess radioactive contamination after an emergency are given; as well as recommendations when kd data are compiled in order to create a useful database.

Modelling of marine radionuclide dispersion in IAEA MODARIA program: Lessons learnt from the Baltic Sea and Fukushima scenarios.

State-of-the art dispersion models were applied to simulate (137)Cs dispersion from Chernobyl nuclear power plant disaster fallout in the Baltic Sea and from Fukushima Daiichi nuclear plant releases in the Pacific Ocean after the 2011 tsunami. Models were of different nature, from box to full three-dimensional models, and included water/sediment interactions. Agreement between models was very good in the Baltic. In the case of Fukushima, results from models could be considered to be in acceptable agreement only after a model harmonization process consisting of using exactly the same forcing (water circulation and parameters) in all models. It was found that the dynamics of the considered system (magnitude and variability of currents) was essential in obtaining a good agreement between models. The difficulties in developing operative models for decision-making support in these dynamic environments were highlighted. Three stages which should be considered after an emergency, each of them requiring specific modelling approaches, have been defined. They are the emergency, the post-emergency and the long-term phases.

Inter-comparison of dynamic models for radionuclide transfer to marine biota in a Fukushima accident scenario.

We report an inter-comparison of eight models designed to predict the radiological exposure of radionuclides in marine biota. The models were required to simulate dynamically the uptake and turnover of radionuclides by marine organisms. Model predictions of radionuclide uptake and turnover using kinetic calculations based on biological half-life (TB1/2) and/or more complex metabolic modelling approaches were used to predict activity concentrations and, consequently, dose rates of (90)Sr, (131)I and (137)Cs to fish, crustaceans, macroalgae and molluscs under circumstances where the water concentrations are changing with time. For comparison, the ERICA Tool, a model commonly used in environmental assessment, and which uses equilibrium concentration ratios, was also used. As input to the models we used hydrodynamic forecasts of water and sediment activity concentrations using a simulated scenario reflecting the Fukushima accident releases. Although model variability is important, the intercomparison gives logical results, in that the dynamic models predict consistently a pattern of delayed rise of activity concentration in biota and slow decline instead of the instantaneous equilibrium with the activity concentration in seawater predicted by the ERICA Tool. The differences between ERICA and the dynamic models increase the shorter the TB1/2 becomes; however, there is significant variability between models, underpinned by parameter and methodological differences between them. The need to validate the dynamic models used in this intercomparison has been highlighted, particularly in regards to optimisation of the model biokinetic parameters.

Dispersion and fate of 9°Sr in the Northwestern Pacific and adjacent seas: global fallout and the Fukushima Dai-ichi accident.

The 3D compartment model POSEIDON-R was applied to the Northwestern Pacific and adjacent seas to simulate the transport and fate of (90)Sr in the period 1945-2010 and to perform a radiological assessment on the releases of (90)Sr due to the Fukushima Dai-ichi nuclear accident for the period 2011-2040. The contamination due to runoff of (90)Sr from terrestrial surfaces was taken into account using a generic predictive model. A dynamical food-chain model describes the transfer of (90)Sr to phytoplankton, zooplankton, molluscs, crustaceans, piscivorous and non-piscivorous fishes. Results of the simulations were compared with observation data on (90)Sr for the period 1955-2010 and the budget of (90)Sr activity was estimated. It was found that in the East China Sea and Yellow Sea the riverine influx was 1.5% of the ocean influx and it was important only locally. Calculated concentrations of (90)Sr in water, bottom sediment and marine organisms before and after the Fukushima Dai-ichi accident are in good agreement with available experimental measurements. The concentration of (90)Sr in seawater would return to the background levels within one year after leakages were stopped. The model predicts that the concentration of (90)Sr in fish after the Fukushima Dai-ichi accident shall return to the background concentrations only 2 years later due to the delay of the transfer throughout the food web and specific accumulation of (90)Sr. The contribution of (90)Sr to the maximal dose rate due to the FDNPP accident was three orders of magnitude less than that due to (137)Cs, and thus well below the maximum effective dose limits for the public.

Regional long-term model of radioactivity dispersion and fate in the Northwestern Pacific and adjacent seas: application to the Fukushima Dai-ichi accident.

The compartment model POSEIDON-R was modified and applied to the Northwestern Pacific and adjacent seas to simulate the transport and fate of radioactivity in the period 1945-2010, and to perform a radiological assessment on the releases of radioactivity due to the Fukushima Dai-ichi accident for the period 2011-2040. The model predicts the dispersion of radioactivity in the water column and in sediments, the transfer of radionuclides throughout the marine food web, and subsequent doses to humans due to the consumption of marine products. A generic predictive dynamic food-chain model is used instead of the biological concentration factor (BCF) approach. The radionuclide uptake model for fish has as a central feature the accumulation of radionuclides in the target tissue. The three layer structure of the water column makes it possible to describe the vertical structure of radioactivity in deep waters. In total 175 compartments cover the Northwestern Pacific, the East China and Yellow Seas and the East/Japan Sea. The model was validated from (137)Cs data for the period 1945-2010. Calculated concentrations of (137)Cs in water, bottom sediments and marine organisms in the coastal compartment, before and after the accident, are in close agreement with measurements from the Japanese agencies. The agreement for water is achieved when an additional continuous flux of 3.6 TBq y(-1) is used for underground leakage of contaminated water from the Fukushima Dai-ichi NPP, during the three years following the accident. The dynamic food web model predicts that due to the delay of the transfer throughout the food web, the concentration of (137)Cs for piscivorous fishes returns to background level only in 2016. For the year 2011, the calculated individual dose rate for Fukushima Prefecture due to consumption of fishery products is 3.6 µSv y(-1). Following the Fukushima Dai-ichi accident the collective dose due to ingestion of marine products for Japan increased in 2011 by a factor of 6 in comparison with 2010.

Dependence of milling time on electrochemical properties of nano Si electrodes prepared by ball-milling.

Morphology, crystallinity and electrochemical properties of Si powders fabricated by a mechanical milling process with milling time of 6-40 h were investigated by means of FESEM, XRD, Raman, TEM and cell test. Average size of Si powders was reduced to sub-micrometer scale after 10 h-milling and 40 nm-Si powders could be obtained at 48 h-milling. With increasing milling time, Si powders mostly changes from crystalline Si to amorphous one and the content of amorphous Si was increased. TEM result showed that a negligiable amount of crystalline Si remained even after 48 h-milling. Si electrode with 48 h-milled Si powders exhibited the best electrochemical properties in terms of capacity, efficiency and cycle performance: initial capacity of 3025 mAh g(-1), coulrombic efficiency of 79.4% and the capacity retention of 1000 mAh g(-1) (at 130 cycles). The good electrochemical properties of nano- and amorphous-Si are due to the high resistance against volume change and good reversibility of Li ion.