Simulation study on 3H behavior in the Fukushima coastal region: Comparison of influences of discharges from the Fukushima Daiichi and rivers.

The release of tritium (3H) to the ocean is planned on the coastal environment in the Fukushima coastal region from Spring or Summer of 2023. Before its release, we evaluate the effect of 3H discharges from the port of Fukushima Daiichi and rivers in the Fukushima coastal region using a three-dimensional hydrodynamic model (3D-Sea-SPEC). The simulation results showed that discharges from the port of Fukushima Daiichi dominantly affected the 3H concentrations in monitoring points within approximately 1 km. Moreover, the results indicate that the effect of riverine 3H discharge was limited around the river mouth under base flow conditions. However, its impact on the Fukushima coastal regions under storm flow conditions was found, and the 3H concentrations in seawater in the Fukushima coastal region were formed around 0.1 Bq/L (mean 3H concentrations in seawater in the Fukushima coastal region) in the near shore.

Temporal variability of 137Cs concentrations in coastal sediments off Fukushima.

Large amounts of radiocesium were released into marine environments following the Fukushima Daiichi Nuclear Power Plant accident in March 2011. Released radiocesium influenced not only marine environment but also marine biota in Fukushima. Since marine biota as fisheries products is important for Japanese market, it is important to assess the distribution of radiocesium in coastal environment off Fukushima for safety concerns of radioactive contamination. Radiocesium concentrations in sediments are important for understanding fishing ground conditions and for proving the safety of fisheries products in Fukushima. In this study, monthly monitoring data collected from May 2011 to March 2020 were analyzed to describe the temporal variability of 137Cs concentrations in coastal sediments off Fukushima (total of 3647 samples from eight lines at depths of 7-125 m off Fukushima, and three sites in Matsukawa-ura Lagoon). The 137Cs concentration in sediment showed a decreasing trend, but our nonlinear model fitting suggested that this rate of decrease had slowed down. Additionally, 137Cs concentrations were up to 4.08 times greater in shallow sampling sites (7, 10, 20 m depth) following heavy rainfall events (before five months vs. after five months), such as typhoons. These observations were consistent with increasing input from particulate 137Cs fluxes from rivers and increasing dissolved 137Cs concentrations in seawater. Finally, our numerical modeling suggested that riverine 137Cs input could maintain 137Cs concentrations in coastal sediment. These results indicate that riverine 137Cs input following heavy rainfall events is the main factor for maintaining 137Cs concentrations in coastal sediments near the Fukushima Daiichi Nuclear Power Plant.

A modeling approach to estimate 3H discharge from rivers: Comparison of discharge from the Fukushima Dai-ichi and inventory in seawater in the Fukushima coastal region.

Estimation of 3H discharge from river catchments is important to evaluate the effect of Fukushima Dai-ichi discharge and future planned 3H release to the ocean on the coastal environment. Using a previously developed model based on the tank model and observed 3H concentration in river water, the 3H discharge from the Abukuma River and 13 other rivers in the Fukushima coastal region were estimated from June 2013 to March 2020. The 3H discharge from catchments of the Abukuma River and 13 other rivers in the Fukushima coastal region during 2014-2019 were estimated to be 1.2-4.0 TBq/y. These values were approximately 2-22 times larger than the annual 3H discharge from the Fukushima Dai-ichi after 2016, indicating the significance of 3H discharge from the catchments through the rivers. This estimation is expected to be useful to evaluate and predict 3H concentrations and inventories in the Fukushima coastal region for consideration of planned 3H release to the ocean.

Remobilisation of radiocaesium from bottom sediments to water column in reservoirs in Fukushima, Japan.

Reservoir sediments generally act as a sink for radionuclides derived from nuclear accidents, but under anaerobic conditions, several radionuclides remobilise in bioavailable form from sediments to water columns, which may contribute to the long-term contamination of aquatic products. This study systematically investigated the 137Cs activities of sediment-pore water, providing a direct evidence of the remobilisation of bioavailable 137Cs from sediments in two highly contaminated reservoirs affected by the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. We observed that the dissolved 137Cs activity concentration of pore water (3.0-65.8 Bq L-1) was one to two orders of magnitude higher than that of reservoir water. Moreover, the distribution coefficient (Kd) values for the 137Cs of sediment-pore water (2.6-14 × 103 L kg-1) decreased with depth. The Kd values were significantly and negatively correlated with the concentration of the major 137Cs competing cation NH4+. Our results strongly indicate a competitive ion exchange process between 137Cs and NH4+ via a highly selective interaction with the frayed edge sites of phyllosilicate minerals, which is the major reason for the variability of Kd values of sediment-pore water, even in the Fukushima case. Additionally, the sediment accumulation rates were relatively high, and the annual depositional rate of exchangeable 137Cs prevailed over the annual diffusive flux of 137Cs from the sediment to the overlying water. This finding indicates that even after 10 years since the FDNPP accident, the bioavailable 137Cs is still continuously supplied from the catchment covered by mountainous forests, and reservoir sediments are a long-term important source of bioavailable 137Cs in the riverine system. Our findings provide important parameter values for mid- and long-term assessments of the radiation impact of radionuclide discharges to freshwater environments.

Leaching characteristics of 137Cs for forest floor affected by the Fukushima nuclear accident: A litterbag experiment.

In forest ecosystems, forest litter is considered an active medium for radiocesium (137Cs). To understand discharge mechanisms of highly bioavailable dissolved 137Cs from forests to river systems, we investigated the characteristics of 137Cs leaching from forest litter as observed from litterbag experiments. Leaching experiments with conifer needle and deciduous broadleaf litters were then conducted. After soaking conifer needles and broadleaf litters for 20 min, 140 min, and 1 day, the mean values of the 137Cs leaching ratios were 0.13-2.0% and 0.81-6.6%, respectively, indicating that 137Cs leaching ratios are different between forest litter types. To elucidate the factors affecting 137Cs leaching from forest litter, a multi-regression analysis of 137Cs leaching ratios was conducted against antecedent mean precipitation and temperature before sampling the litterbag and accumulated temperature during the litterbag experiments. The 137Cs leaching ratios showed a negative correlation to the antecedent mean precipitation for both litters and the accumulated temperature for broadleaf litters, whereas it exhibited a positive correlation with the antecedent mean temperature for both litters and the accumulated temperature for conifer needle litters. It was proposed that the fraction of 137Cs in labile sites in forest litter increased/decreased due to litter decomposition by antecedent/accumulated temperature, and that this fraction can be washed off by the antecedent precipitation. The different effects of accumulated temperature on 137Cs leaching from conifer needles and broadleaf litters could be due to their different decomposition rates. Our results contribute further the understanding of the mechanisms associated with dissolved 137Cs discharge from forested catchments.

Calculations for ambient dose equivalent rates in nine forests in eastern Japan from 134Cs and 137Cs radioactivity measurements.

Understanding the relationship between the distribution of radioactive 134Cs and 137Cs in forests and ambient dose equivalent rates (H˙∗(10)) in the air is important for researching forests in eastern Japan affected by the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. This study used a large number of measurements from forest samples, including 134Cs and 137Cs radioactivity concentrations, densities and moisture contents, to perform Monte Carlo radiation transport simulations for H˙∗(10) between 2011 and 2017. Calculated H˙∗(10) at 0.1 and 1 m above the ground had mean residual errors of 19% and 16%, respectively, from measurements taken with handheld NaI(Tl) scintillator survey meters. Setting aside the contributions from natural background radiation, 134Cs and 137Cs in the organic layer and the top 5 cm of forest soil generally made the largest contributions to calculated H˙∗(10). The contributions from 134Cs and 137Cs in the forest canopy were calculated to be largest in the first two years following the accident. Uncertainties were evaluated in the simulation results due to the measurement uncertainties in the model inputs by assuming Gaussian measurement errors. The mean uncertainty (relative standard deviation) of the simulated H˙∗(10) at 1 m height was 11%. The main contributors to the total uncertainty in the simulation results were the accuracies to which the 134Cs and 137Cs radioactivities of the organic layer and top 5 cm of soil, and the vertical distribution of 134Cs and 137Cs within the 5 cm soil layers, were known. Radioactive cesium located in the top 5 cm of soil was the main contributor to H˙∗(10) at 1 m by 2016 or 2017 in the calculation results for all sites. Studies on the 137Cs distribution within forest soil will therefore help explain radiation levels henceforth in forests affected by the FDNPP accident. The merits of this study are that it modelled multiple forests for a long time period, with the important model inputs being informed by field measurements, and it quantified how the measurement uncertainties in these inputs affected the calculation results.

Reservoir sediments as a long-term source of dissolved radiocaesium in water system; a mass balance case study of an artificial reservoir in Fukushima, Japan.

Because of their large mobility and high bioavailability, it is necessary to elucidate the origins and dynamics of dissolved radionuclides in river and reservoir systems to assess the transfer of those radionuclides from water to crops and aquatic organisms. Elution from contaminated reservoir sediments, a potential source of dissolved radionuclides, presents a long-term concern, particularly for long-lived radionuclides. In this study, we systematically investigated caesium-137 (137Cs) concentrations using a time-series suite of input and output water samples collected from 2014 to 2019 from the Ogaki Dam Reservoir, which has a catchment with a high 137Cs inventory due to the Fukushima Dai-ichi Nuclear Power Plant accident. The results of our study showed that dissolved 137Cs concentration was significantly higher in the output water than that in the main input water, and that the effective ecological half-life of dissolved 137Cs in the output water was longer than in the main input water. We quantitatively evaluated the mass balance of dissolved 137Cs in the reservoir to elucidate how much dissolved 137Cs from the rivers and production from reservoir sediments contribute to 137Cs in the reservoir output. The annual output of dissolved 137Cs was significantly higher than the total input of dissolved 137Cs, with approximately 32%-40% of the dissolved 137Cs in the output water presumably being produced from reservoir sediments. Consequently, the estimated dissolved 137Cs fluxes from reservoir sediments to overlying water were 0.57-1.3 × 104 Bq m-2 y-1. This implies that approximately 0.04%-0.09% of 137Cs accumulated in the sediments was released through elution to the overlying water each year. Reservoir sediments containing high 137Cs levels may thus become even more important as sources of bioavailable dissolved 137Cs in the future.

A modeling approach to estimate the 137Cs discharge in rivers from immediately after the Fukushima accident until 2017.

We developed a simple model to evaluate and predict the 137Cs discharge from catchments using a tank model and the L-Q equation. Using this model, the 137Cs discharge and discharge ratio from the Abukuma River and 13 other rivers in the Fukushima coastal region were estimated from immediately after the Fukushima accident up to 2017. The 137Cs discharge (and discharge ratio to the deposition inventory in the catchment) of the Abukuma River and 13 other rivers in the Fukushima coastal region during the initial six months after the accident were estimated to be 18 TBq (3.1%) and 11 TBq (0.79%), respectively. These values of 137Cs discharge ratio were 1-2 orders of magnitude higher than those observed after June 2011 in previous studies (Ueda et al., 2013; Tsuji et al., 2016; Iwagami et al., 2017a), indicating that the initial 137Cs discharge from the catchments through the rivers was significant. The simulated initial 137Cs discharge rates for the initial six months after the Fukushima accident were about 9-30 times larger in each catchment than those after that point until 2017, though initial 137Cs concentration in river water was derived from an extrapolation of data based on a two exponentially decreasing fitting. However, it was found that the impact on the ocean from the initial 137Cs discharge through the rivers can be limited because the 137Cs discharge from the Abukuma River and the 13 other rivers in the Fukushima coastal region (29 TBq) was two orders of magnitude smaller than the direct release from Fukushima Dai-ichi Nuclear Power Plant (FDNPP) into the ocean (3.5 PBq) and from atmospheric deposition into the ocean (7.6 PBq) (Kobayashi et al., 2013). This model is expected to be useful to evaluate and predict 137Cs discharge from catchments in future water management and in the estimation of 137Cs discharge into reservoirs and the ocean.

Numerical study of transport pathways of 137Cs from forests to freshwater fish living in mountain streams in Fukushima, Japan.

The accident at the Fukushima Dai-ichi Nuclear Power Plant in 2011 released a large quantity of radiocesium into the surrounding environment. Radiocesium concentrations in some freshwater fish caught in rivers in Fukushima Prefecture in October 2018 were still higher than the Japanese limit of 100 Bq kg-1 for general foodstuffs. To assess the uptake of 137Cs by freshwater fish living in mountain streams in Fukushima Prefecture, we developed a compartment model for the migration of 137Cs on the catchment scale from forests to river water. We modelled a generic forest catchment with Fukushima-like parameters to ascertain the importance of three export pathways of 137Cs from forests to river water for the uptake of 137Cs by freshwater fish. The pathways were direct litter fall into rivers, lateral inflow from the forest litter layer, and lateral transfer from the underlying forest soil. Simulation cases modelling only a single export pathway did not reproduce the actual trend of 137Cs concentrations in river water and freshwater fish in Fukushima Prefecture. Simulations allowing a combined effect of the three pathways reproduced the trends well. In the latter simulations, the decreasing trend of 137Cs in river water and freshwater fish was due to a combination of the decreasing trend in the forest leaves/needles and litter compartments, and the increasing trend in soil. The modelled 137Cs concentrations within the forest compartments were predicted to reach an equilibrium state at around ten years after the fallout due to the equilibration of 137Cs cycling in forests. The model suggests that long term 137Cs concentrations in freshwater fish in mountain streams will be controlled by the transfer of 137Cs to river water from forest organic soils.

Trend of 137Cs concentration in river water in the medium term and future following the Fukushima nuclear accident.

It is a critical to examine the migration behavior of radiocesium derived from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident in river systems to predict the future contamination status and propose effective countermeasures to reduce exposure. We conducted a three-year-long observation (April 2015-March 2018) of the 137Cs concentration in two rivers which located surrounding the FDNPP. The result revealed a declining trend for the dissolved and particulate 137Cs concentration in river water from four to seven years after the FDNPP accident. The dissolved and particulate 137Cs concentrations for both rivers had similar temporal patterns and showed declining trends with time. However, the dissolved 137Cs concentration had longer half-life than the particulate 137Cs concentration and large seasonal variations related to water temperature. The environmental half-life for the dissolved 137Cs concentration was longer than previous reported values within three years after the accident, suggesting that the declining trend for the dissolved 137Cs concentration is gradually decreasing with time. The temperature dependency of the dissolved 137Cs concentration became weaker year by year. From the D10 equation we proposed, the dissolved 137Cs concentration will likely remain at the same level for several decades. The results of the present study promote our understanding of both the medium- and long-term impacts of the FDNPP accident on river systems.

Evaluation of particulate 137Cs discharge from a mountainous forested catchment using reservoir sediments and sinking particles.

The time and size dependencies of particulate 137Cs concentrations in a reservoir were investigated to evaluate the dynamics of 137Cs pollution from a mountainous forested catchment. Sediment and sinking particle samples were collected using a vibracorer and a sediment trap at the Ogaki Dam Reservoir in Fukushima, which is located in the heavily contaminated area that formed as a result of the Fukushima Dai-ichi Nuclear Power Plant accident of 2011. The inventory of 137Cs discharged into the reservoir during the post-accident period (965 days) was estimated to be approximately 3.0 × 1012-3.9 × 1012 Bq, which is equivalent to 1.1%-1.4% of the initial estimated catchment inventory. The particulate 137Cs concentration showed a decline with time, but the exponent value between the specific surface area and the 137Cs concentration for the fine-sized (<63 µm) particle fraction remained almost constant from the immediate aftermath of the accident. These quantitative findings obtained by reconstructing the contamination history of particulate 137Cs in reservoir sediments and sinking particles have important implications for the evaluation of 137Cs dynamics in mountainous forested catchments.

Simulation study of the effects of buildings, trees and paved surfaces on ambient dose equivalent rates outdoors at three suburban sites near Fukushima Dai-ichi.

The influence of buildings, trees and paved surfaces on outdoor ambient dose equivalent rates (H˙∗(10)) in suburban areas near to the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) was investigated with Monte Carlo simulations. Simulation models of three un-decontaminated sites in Okuma and Tomioka were created with representations of individual buildings, trees and roads created using geographic information system (GIS) data. The 134Cs and 137Cs radioactivity distribution within each model was set using in-situ gamma spectroscopy measurements from December 2014 and literature values for the relative radioactive cesium concentration on paved surfaces, unpaved land, building outer surfaces, forest litter and soil layers, and different tree compartments. Reasonable correlation was obtained between the simulations and measurements for H˙∗(10) across the sites taken in January 2015. The effect of buildings and trees on H˙∗(10) was investigated by performing simulations removing these objects, and their associated 134Cs and 137Cs inventory, from the models. H˙∗(10) were on average 5.0% higher in the simulations without buildings and trees, even though the total 134Cs and 137Cs inventory within each model was slightly lower. The simulations without buildings and trees were then modified to include 134Cs and 137Cs in the ground beneath locations where buildings exist in reality, and the inventory of paved surfaces modelled as if they had high retention of 134Cs and 137Cs fallout like soil areas. H˙∗(10) increased more markedly in these cases than when considering the shielding effect of buildings and trees alone. These results help clarify the magnitude of the effect of buildings, trees and paved surfaces on H˙∗(10) at the un-decontaminated sites within Fukushima Prefecture.

Applicability of Kd for modelling dissolved 137Cs concentrations in Fukushima river water: Case study of the upstream Ota River.

A study is presented on the applicability of the distribution coefficient (Kd) absorption/desorption model to simulate dissolved 137Cs concentrations in Fukushima river water. The upstream Ota River basin was simulated using GEneral-purpose Terrestrial Fluid-flow Simulator (GETFLOWS) for the period 1 January 2014 to 31 December 2015. Good agreement was obtained between the simulations and observations on water and suspended sediment fluxes, and on particulate bound 137Cs concentrations under both base and high flow conditions. By contrast the measured concentrations of dissolved 137Cs in the river water were much harder to reproduce with the simulations. By tuning the Kd values for large particles, it was possible to reproduce the mean dissolved 137Cs concentrations during base flow periods (observation: 0.32 Bq/L, simulation: 0.36 Bq/L). However neither the seasonal variability in the base flow dissolved 137Cs concentrations (0.14-0.53 Bq/L), nor the peaks in concentration that occurred during storms (0.18-0.88 Bq/L, mean: 0.55 Bq/L), could be reproduced with realistic simulation parameters. These discrepancies may be explained by microbial action and leaching from organic matter in forest litter providing an additional input of dissolved 137Cs to rivers, particularly over summer, and limitations of the Kd absorption/desorption model. It is recommended that future studies investigate these issues in order to improve simulations of dissolved 137Cs concentrations in Fukushima rivers.

Evaluation of particulate 137Cs discharge from a mountainous forested catchment using reservoir sediments and sinking particles.

The time and size dependencies of particulate 137Cs concentrations in a reservoir were investigated to evaluate the dynamics of 137Cs pollution from a mountainous forested catchment. Sediment and sinking particle samples were collected using a vibracorer and a sediment trap at the Ogaki Dam Reservoir in Fukushima, which is located in the heavily contaminated area that formed as a result of the Fukushima Dai-ichi Nuclear Power Plant accident of 2011. The inventory of 137Cs discharged into the reservoir during the post-accident period (965 days) was estimated to be approximately 3.0 × 1012-3.9 × 1012 Bq, which is equivalent to 1.1%-1.4% of the initial estimated catchment inventory. The particulate 137Cs concentration showed a decline with time, but the exponent value between the specific surface area and the 137Cs concentration for the fine-sized (<63 µm) particle fraction remained almost constant from the immediate aftermath of the accident. These quantitative findings obtained by reconstructing the contamination history of particulate 137Cs in reservoir sediments and sinking particles have important implications for the evaluation of 137Cs dynamics in mountainous forested catchments.

Applicability of Kd for modelling dissolved 137Cs concentrations in Fukushima river water: Case study of the upstream Ota River.

A study is presented on the applicability of the distribution coefficient (Kd) absorption/desorption model to simulate dissolved 137Cs concentrations in Fukushima river water. The upstream Ota River basin was simulated using GEneral-purpose Terrestrial Fluid-flow Simulator (GETFLOWS) for the period 1 January 2014 to 31 December 2015. Good agreement was obtained between the simulations and observations on water and suspended sediment fluxes, and on particulate bound 137Cs concentrations under both base and high flow conditions. By contrast the measured concentrations of dissolved 137Cs in the river water were much harder to reproduce with the simulations. By tuning the Kd values for large particles, it was possible to reproduce the mean dissolved 137Cs concentrations during base flow periods (observation: 0.32 Bq/L, simulation: 0.36 Bq/L). However neither the seasonal variability in the base flow dissolved 137Cs concentrations (0.14-0.53 Bq/L), nor the peaks in concentration that occurred during storms (0.18-0.88 Bq/L, mean: 0.55 Bq/L), could be reproduced with realistic simulation parameters. These discrepancies may be explained by microbial action and leaching from organic matter in forest litter providing an additional input of dissolved 137Cs to rivers, particularly over summer, and limitations of the Kd absorption/desorption model. It is recommended that future studies investigate these issues in order to improve simulations of dissolved 137Cs concentrations in Fukushima rivers.

Evaluation of sediment and 137Cs redistribution in the Oginosawa River catchment near the Fukushima Dai-ichi Nuclear Power Plant using integrated watershed modeling.

The Oginosawa River catchment lies 15 km south-west of the Fukushima Dai-ichi nuclear plant and covers 7.7 km2. Parts of the catchment were decontaminated between fall 2012 and March 2014 in preparation for the return of the evacuated population. The General-purpose Terrestrial Fluid-flow Simulator (GETFLOWS) code was used to study sediment and 137Cs redistribution within the catchment, including the effect of decontamination on redistribution. Fine resolution grid cells were used to model local features of the catchment, such as paddy fields adjacent to the Oginosawa River. The simulation was verified using monitoring data for river water discharge rates (r = 0.92), suspended sediment concentrations, and particulate 137Cs concentrations (r = 0.40). Cesium-137 input to watercourses came predominantly from land adjacent to river channels and forest gullies, e.g. the paddy fields in the Ogi and Kainosaka districts, as the ground in these areas saturates during heavy rain and is easily eroded. A discrepancy between the simulation and monitoring results on the sediment discharge rate following decontamination may be explained by fast erosion occurring after decontamination. Forested areas far from the channels only made a minor contribution to 137Cs input to watercourses, total erosion of between 0.001 and 0.1 mm from May 2011 to December 2015, as ground saturation is infrequent in these areas. The 2.3-6.9% y-1 decrease in the amount of 137Cs in forest topsoil over the study period can be explained by radioactive decay (approximately 2.3% y-1), along with a migration downwards into subsoil and a small amount of export. The amount of 137Cs available for release from land adjacent to rivers is expected to be lower in future than compared to this study period, as the simulations indicate a high depletion of inventory from these areas by the end of 2015. However continued monitoring of 137Cs concentrations in river water over future years is advised, as recultivation of paddy fields by returnees may again lead to fast erosion rates and release of the remaining inventory.

Characteristics of radio-cesium transport and discharge between different basins near to the Fukushima Dai-ichi Nuclear Power Plant after heavy rainfall events.

This paper describes watershed modeling of catchments surrounding the Fukushima Dai-ichi Nuclear Power Plant to understand radio-cesium redistribution by water flows and sediment transport. We extended our previously developed three-dimensional hydrogeological model of the catchments to calculate the migration of radio-cesium in both sediment-sorbed and dissolved forms. The simulations cover the entirety of 2013, including nine heavy rainfall events, as well as Typhoon Roke in September 2011. Typhoons Man-yi and Wipha were the strongest typhoons in 2013 and had the largest bearing on radio-cesium redistribution. The simulated 137Cs discharge quantities over the nine events in 2013 are in good agreement with field monitoring observations. Deposition mainly occurs on flood plains and points where the river beds broaden in the lower basins, and within dam reservoirs along the rivers. Differences in 137Cs discharge ratios between the five basins are explained by differences in the initial fallout distribution within the basins, the presence of dam reservoirs, and the input supply to watercourses. It is possible to use these simulation results to evaluate future radioactive material distributions in order to support remediation planning.