A critical review and update of modelling of treated water discharging from Fukushima Daiichi NPP.

Since the accident at the Fukushima Daiichi nuclear power plant (FDNPP) in March 2011 seawater is still needed to cool the reactor cores. This water, contaminated with radionuclides, has been collected in tanks and treated on the site of the FDNPP. In 2021, the Japanese government decided to gradually discharge treated water into the ocean, which started on the 24th of August 2023 and will continue for the next 30 years. This paper provides a critical analysis of the models that were used in the different radiological impact studies. Based on the analysis, a hydrodynamic and a compartment models with a harmonized setup were used to estimate the impact of the discharge on humans and biota. Doses obtained with these two models were within one order of magnitude for humans (<0.1 µSv/year) and for biota (<10-6 mGy/d) indicating that harmonization of the model parameters improved the reliability of the simulation results.

Comparison of methods for the radiological impact assessment of aquatic releases to the waters in the low countries.

Accurate assessment of the radiological impact of liquid discharges on the marine environment is challenging despite all developments in recent years. The lack of consensus on this type of assessment manifests itself even stronger when transborder issues are expected, such as in the Low Countries. Belgium and the Netherlands operate nuclear power plants with discharges in the shared estuary of the Western Scheldt, therefore if there are safety concerns, information on both sides of the border must be coherent. This work provides a comparison of two computational methods used for assessment of aquatic releases in the Western Scheldt estuary and the adjacent North Sea.The work demonstrates a fair degree of consistency in modelling the uptake and fate of key anthropogenic radionuclides. Nevertheless, there are also considerable differences found in sediment and sea species with concentrations ranging by over two orders of magnitude in some cases. These explainable differences are methodological in nature, occurring in codes that underwent extensive validation during development. Therefore, the outcomes of this work clearly demonstrate the need to produce explicit guidance that is specifically tailored to the (inter)national water system of concern. This should not be limited to releases from nuclear power plants, but also include other nuclear applications. For all these reasons, more intensive collaboration and model harmonisation across borders is essential, signalling the direction for future investigations.

Planned release of contaminated water from the Fukushima storage tanks into the ocean: Simulation scenarios of radiological impact for aquatic biota and human from seafood consumption.

The radiological impact for human and aquatic biota as a result of a planned release of contaminated water stored in tanks near the Fukushima Dai-ichi Nuclear Power Plant to the Pacific Ocean is assessed. The total activity for 10 dominant radionuclides (3H, 14C, 60Co, 90Sr, 99Tc, 106Ru, 125Sb, 129I, 134Cs, 137Cs) in tanks is estimated. The compartment model POSEIDON-R is applied to compute the concentration of activity for each radionuclide in water, bottom sediments, and biota, and corresponding doses to marine organisms and humans from seafood consumption. Predicted concentrations of activity in marine products in future will not exceed food safety limits in Japan. The computed maximum committed effective dose to humans is less than 1 µSv per year with the highest contribution from 129I and 14C. Maximum absorbed doses to non-human biota are in the order of 0.05 to 20 µGy per year, meaning that no deleterious effects are expected.

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.

Intercomparison on the measurement of the thoron exhalation rate from building materials.

Thoron (220Rn) exhalation from building materials has become increasingly recognized as a potential source for radiation exposure in dwellings. However, contrary to radon (222Rn), limited information on thoron exposure is available. As a result no harmonized test procedures for determining thoron exhalation from building materials are available at present. This study is a first interlaboratory comparison of different test methods to determine the thoron exhalation and a pre-step to a harmonized standard. The purpose of this study is to compare the experimental findings from a set of three building materials that are tested, and to identify future challenges in the development of a harmonized standard.

Development of a reference material for analysing naturally occurring radioactive material from the steel industry.

Accurate measurement of naturally occurring radionuclides in blast furnace slag, a by-product of the steel industry, is required for compliance with building regulations where it is often used as an ingredient in cement. A matrix reference blast furnace slag material has been developed to support traceability in these measurements. Raw material provided by a commercial producer underwent stability and homogeneity testing, as well as characterisation of matrix constituents, to provide a final candidate reference material. The radionuclide content was then determined during a comparison exercise that included 23 laboratories from 14 countries. Participants determined the activity per unit mass for 226Ra, 232Th and 40K using a range of techniques. The consensus values obtained from the power-moderated mean of the reported participant results were used as indicative activity per unit mass values for the three radionuclides: A0(226Ra) = 106.3 (34) Bq·kg-1, A0(232Th) = 130.0 (48) Bq·kg-1 and A0(40K) = 161 (11) Bq·kg-1 (where the number in parentheses is the numerical value of the combined standard uncertainty referred to the corresponding last digits of the quoted result). This exercise helps to address the current shortage of NORM industry reference materials, putting in place infrastructure for production of further reference materials.

Low-dose (S)TEM elemental analysis of water and oxygen uptake in beam sensitive materials.

The performance stability of organic photovoltaics (OPVs) is largely determined by their nanoscale morphology and composition and is highly dependent on the interaction with oxygen and water from air. Low-dose cryo-(S)TEM techniques, in combination with OPV donor-acceptor model systems, can be used to assess oxygen- and water-uptake in the donor, acceptor and their interface. By determining a materials dependent critical electron dose from the decay of the oxygen K-edge intensity in Electron Energy Loss Spectra, we reliably measured oxygen- and water-uptake minimizing and correcting electron beam effects. With measurements below the dose limit the capability of STEM-EDX, EFTEM and STEM-EELS techniques are compared to qualitatively and quantitatively measure oxygen and water uptake in these OPV model systems. Here we demonstrate that oxygen and water is mainly taken up in acceptor-rich regions, and that specific oxygen uptake at the donor-acceptor interphase does not occur. STEM-EELS is shown to be the best suitable technique, enabling quantification of the local oxygen concentration in OPV model systems.

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.

Thoron exposure in Dutch dwellings - An overview.

In the Netherlands considerable attention has been given to the exposure from thoron progeny in dwellings. For this purpose a nationwide survey on the thoron exhalation and thoron progeny concentration has been completed in 2015. Furthermore, extensive laboratory studies have been performed to measure activity concentrations and thoron exhalation rates from regular Dutch building materials. The purpose of this study is to demonstrate if the findings from both field experiments and laboratory results are consistent. For this reason measured properties of building materials and surface barriers, in-situ measurements on air ventilation and thoron(progeny) in dwellings as well as advanced computational modelling on indoor air and aerosol behaviour have been used. The results demonstrate that median and mean thoron progeny concentrations of 0.53 and 0.64 Bq·m-3 found in the survey are comparable with the mean concentration of 0.57 Bq·m-3 obtained from laboratory testing and calculation. Furthermore, upper thoron progeny concentrations from the survey and the calculations are with respectively 13 and 14 Bq·m-3 also in good agreement. Such elevated concentrations lead to an effective doses of around 4 mSv per year. The study also includes worst-case scenarios on the application of surface materials high on 232Th, and the expected reduction in thoron progeny when using mainstream mitigation measures.

Thoron Mitigation from Building Materials with Surface Barriers.

Thoron (Rn) exhalation from building materials has become increasingly recognized as a potential source for radiation exposure in dwellings. However, few studies have focused on mitigation strategies to reduce exposure from thoron and its progeny. Therefore, the purpose of this study is to (1) determine the reduction in thoron exhalation from building materials applied with regularly available surface barriers and (2) investigate the effects from surface roughness of the base material, barrier thickness, and surface cover on the thoron-retaining action of the surface barrier. The findings from this study demonstrate that regular surface barriers provide a potentially significant reduction in thoron exhalation, which can reach more than 90%. Despite this reduction, there are also materials that provide no reduction at all. Based on this work, no commonly available product property could be identified that provides good guidance on the barriers' performance to reduce thoron exhalation.

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.

Mesoscopic simulations of hydrophilic cross-linked polycarbonate polyurethane networks: structure and morphology.

Polyurethane (PU) cross-linked networks are frequently used in biomedical and marine applications, e.g., as hydrophilic polymer coatings with antifouling or low-friction properties and have been reported to exhibit characteristic phase separation between soft and hard segments. Understanding this phase-separation behavior is critical to design novel hydrophilic polymer coatings. However, most of the studies on the structure and morphology of cross-linked coatings are experimental, which only assess the phase separation via indirect methods. Herein we present a mesoscopic simulation study of the network characteristics of model hydrophilic polymer networks, consisting of PU with and without methyl-polyethylene glycol (mPEG) dangling chains. The systems are analyzed using a number of tools, such as the radial distribution function, the cross-link point density distribution and the Voronoi volume distribution (of the cross-linking points). The combined results show that the cross-linked networks without dangling chains are rather homogeneous but contain a small amount of clustering of cross-linker molecules. A clear phase separation is observed when introducing the dangling chains. In spite of that, the amount of cross-linker molecules connected to dangling chains only, i.e., not connected to the main network, is relatively small, leading to about 3 wt% extractables. Thus, these cross-linked polymers consist of a phase-separated, yet highly connected network. This study provides valuable guidelines towards new self-healing hydrophilic coatings based on the molecular design of cross-linked networks in direct contact with water or aqueous fluids, e.g., as anti-fouling self-repairing coatings for marine applications.

Impact from indoor air mixing on the thoron progeny concentration and attachment fraction.

Despite the considerable amount of work in the field of indoor thoron exposure, little studies have focussed on mitigation strategies to reduce exposure to thoron and its progeny. For this reason an advanced computer model has been developed that describes the dispersion and aerosol modelling from first principal using Computational Fluid Dynamics. The purpose of this study is to investigate the mitigation effects from air mixing on the progeny concentration and attachment with aerosols. The findings clearly demonstrate a reduction in thoron progeny concentration due to air mixing. The reduction in thoron progeny is up to 60% when maximum air mixing is applied. In addition there is a reduction in the unattached fraction from 1.2% under regular conditions to 0.3% in case of maximum mixing.

A comparison of marine radionuclide dispersion models for the Baltic Sea in the frame of IAEA MODARIA program.

Four radionuclide dispersion models have been applied to simulate the transport and distribution of (137)Cs fallout from Chernobyl accident in the Baltic Sea. Models correspond to two categories: box models and hydrodynamic models which solve water circulation and then an advection/diffusion equation. In all cases, interactions of dissolved radionuclides with suspended matter and bed sediments are included. Model results have been compared with extensive field data obtained from HELCOM database. Inventories in the water column and seabed, as well as (137)Cs concentrations along 5 years in water and sediments of several sub-basins of the Baltic, have been used for model comparisons. Values predicted by the models for the target magnitudes are very similar and close to experimental values. Results suggest that some processes are not very relevant for radionuclide transport within the Baltic Sea, for instance the roles of the ice cover and, surprisingly, water stratification. Also, results confirm previous findings concerning multi-model applications.

Single-walled carbon nanotube networks in conductive composite materials.

Electrically conductive composite materials can be used for a wide range of applications because they combine the advantages of a specific polymeric material (e.g., thermal and mechanical properties) with the electrical properties of conductive filler particles. However, the overall electrical behaviour of these composite materials is usually much below the potential of the conductive fillers, mainly because by mixing two different components, new interfaces and interphases are created, changing the properties and behaviours of both. Our goal is to characterize and understand the nature and influence of these interfaces on the electrical properties of composite materials. We have improved a technique based on the use of sodium carboxymethyl cellulose (CMC) to disperse single-walled carbon nanotubes (SWCNTs) in water, followed by coating glass substrates, and drying and removing the CMC with a nitric acid treatment. We used electron microscopy and atomic force microscopy techniques to characterize the SWCNT films, and developed an in situ resistance measurement technique to analyse the influence of both the individual components and the mixture of an epoxy/amine system on the electrical behaviour of the SWCNTs. The results showed that impregnating a SWCNT network with a polymer is not the only factor that affects the film resistance; air exposure, temperature, physical and chemical properties of the individual polymer components, and also the formation of a polymeric network, can all have an influence on the macroscopic electrical properties of the initial SWCNT network. These results emphasize the importance of understanding the effects that each of the components can have on each other before trying to prepare an efficient polymer composite material.

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.

Measurement of thoron exhalation rates from building materials.

Thoron (220Rn) exhalation from building materials has become increasingly recognized as a potential source for radiation exposure in dwellings. However, contrary to radon (220Rn), limited information on thoron exposure is available. The purpose of this study is to develop a test method for the determination of the thoron exhalation rate from building materials. The method is validated, and subsequently the thoron exhalation rates from 10 widely-applied concretes, gypsums, brick, limestone, and mortar are determined. The measured thoron exhalation rates of these materials range from 0.01 Bq m-2 s-1 to 0.43 Bq m-2 s-1, with relative standard uncertainties between 6% to 14%.

The molecular configuration of a DOPA/ST monolayer at the air-water interface: a molecular dynamics study.

In this study, surface pressure-area isotherms for N-stearoyldopamine (DOPA) and 4-stearylcatechol (ST) monolayers are obtained by means of molecular dynamics simulations and compared to experimental isotherms. The difference between DOPA and ST is an amide group, which is present in the alkyl tails of DOPA molecules. We find a large difference between the isotherms for DOPA and ST monolayers. Upon using TIP4P/2005 for water and OPLS force fields for the organic material and a relatively large system size, the simulated results are found to be consistent with experiments. With molecular dynamics simulations, the configurations of molecules in the monolayers can be directly analyzed. When the surface pressure is high, a regular molecular orientation is observed for ST molecules, whereas regular orientations are only observed in local domains for DOPA molecules. The differences between DOPA and ST monolayers are attributed to the amide groups in DOPA molecules, which are useful for both steric effects and the formation of hydrogen bonds in the DOPA monolayers. This study clearly demonstrates that hydrogen bonds, due to the presence of the amide group in DOPA, are the cause of the disorder in its Langmuir monolayers. Thus, the conclusion may be helpful in making ordered organic monolayers in the future.

Self-replenishing ability of cross-linked low surface energy polymer films investigated by a complementary experimental-simulation approach.

Nowadays, many self-healing strategies are available for recovering mechanical damage of bulk polymeric materials. The recovery of surface-dependent functionalities on polymer films is, however, equally important and has been less investigated. In this work we study the ability of low surface energy cross-linked poly(ester urethane) networks containing perfluorinated dangling chains to self-replenish their surface, after being submitted to repeated surface damage. For this purpose we used a combined experimental-simulation approach. Experimentally, the cross-linked films were intentionally damaged by cryo-microtoming to remove top layers and create new surfaces which were characterized by water Contact Angle measurements and X-Ray Photoelectron Spectroscopy. The same systems were simultaneously represented by a Dissipative Particles Dynamics simulation method, where the damage was modeled by removing the top film layers in the simulation box and replacing it by new "air" beads. The influence of different experimental parameters, such as the concentration of the low surface energy component and the molecular mobility span of the dangling chains, on the surface recovery is discussed. The combined approach reveals important details of the self-replenishing ability of damaged polymer films such as the occurrence of multiple-healing events, the self-replenishing efficiency, and the minimum "healing agent" concentration for a maximum recovery.