Dissolved 137Cs Concentrations Research Articles

Applicability of reconstruction of temporal changes in 137Cs concentrations in pond water based on the vertical distribution of bottom sediments: a case in three ponds in the Fukushima evacuation zone.

Long-term changes in particulate and dissolved 137Cs concentrations in rivers and dam reservoirs have been reconstructed using 137Cs depth distributions in bottom sediments near Chornobyl and Fukushima. However, few studies have applied this method to pond water. This study tested the applicability of this reconstruction method in ponds within the Fukushima evacuation zone. Bottom sediments in ponds were collected in November 2019. Our reconstruction of a shallow closed pond disagreed with our observations. Even in ponds where the reconstruction agreed well with observations, underestimations may have occurred because the time constant for the decrease in 137Cs concentration was lower than those previously reported. We conclude that the present reconstruction method may be applied to deeper Fukushima ponds with inflow and outflow, but underestimations of initial 137Cs concentrations in water may lead to uncertainties. For realistic reconstruction, attention should be paid to pond characteristics, catchment conditions, and sediment core selection.

Mechanisms of 137Cs leaching based on long-term observations in forested headwater catchments in Yamakiya, Fukushima Prefecture, Japan

Dissolved radiocesium (mainly 134Cs and 137Cs) is thought to be leached mainly from suspended sediment in downstream rivers, while organic matter, such as leaf litter, contributes to catchments in forested headwater streams. It is also known that dissolved 137Cs in headwater streams exhibit seasonal variation with water temperature. Some mechanisms have been proposed as the causes: ionic competition of potassium ion (K+) and ammonium ion (NH4+), leaching associated with the decomposition of organic matter, and thermodynamic adsorption-desorption processes. We investigated the relationship between K+ and the dissolved organic carbon (DOC) concentrations and seasonal changes in dissolved 137Cs concentration using a large number of samples from a headwater's small catchments. We examined temporal trends in 137Cs concentrations in coarse organic matter, suspended sediments, and dissolved forms at four sites (one decontaminated site and three undecontaminated sites) in the Yamakiya area since 2011. The distribution coefficients (Kdcss and Kdorg) of dissolved 137Cs concentrations relative to suspended sediment and coarse organic matter 137Cs concentrations were calculated, and differences in temporal changes due to decontamination were investigated. In addition, we examined the relationship between water temperature and DOC, K+, NH4+ and 137Cs concentrations in the headwater catchments. The suspended sediment 137Cs concentrations at the decontaminated headwater site (IBO) decreased significantly after decontamination and remained low thereafter. In contrast, dissolved 137Cs concentrations decreased temporarily during the decontamination period, but returned to pre-decontamination levels. Almost no NH4+ has been detected in headwater streams in our catchments. In the SET and ISH watersheds, where the distance from the groundwater spring is short, a correlation was found between DOC concentration and dissolved 137Cs concentration. In contrast, in the IBO watershed, where the distance from the groundwater spring is long, temperature dependence and a good correlation between K+ and 137Cs were observed. Therefore, microbial decomposition of organic matter may have a significant effect on the seasonal variation of dissolved 137Cs in forested headwater streams at short distances from the spring, but the influence of competing ions is expected to increase gradually as the water flows downstream.

Influential factors of long-term and seasonal 137Cs change in agricultural and forested rivers: Temperature, water quality and an intense Typhoon Event

In this study, the effect of temperature, water quality, and the impact of an intense typhoon event on change in 137Cs concentration in the water of agricultural and forested rivers near the Fukushima Daiichi nuclear power plant (Japan) was evaluated using monthly stationary observations obtained under baseflow conditions 2.8–10.6 years after the nuclear accident in 2011. The dissolved 137Cs concentration fluctuated seasonally with water temperature in all rivers, and the increase in dissolved 137Cs concentration for unit increase in temperature was higher in forested rivers than in agricultural rivers. The relationship between water temperature and the apparent distribution coefficient of 137Cs well followed the van ’t Hoff equation in the two agricultural rivers, where the enthalpy of reaction was estimated as −15.6 and −19.6 kJ mol−1. The van ’t Hoff equation was not well followed for a forested river, where the suspended solids mainly comprised organic matter, suggesting that the dominant process determining dissolved 137Cs concentrations in forested rivers is not only water temperature effect on ion exchange, but rather the input of 137Cs and K+ (competing with 137Cs for exchange sites on mineral particles) into the water phase via litter leaching. Suspended solids concentrations in agricultural rivers correlated negatively with 137Cs concentrations in suspended solids, suggesting an increased proportion of coarse particles or the input of soils with low 137Cs concentration from decontaminated agricultural land. At some sites, 137Cs concentrations in dissolved form and in suspended solids were reduced sharply in association with the passage of Typhoon Hagibis in October 2019, suggesting that Typhoon Hagibis caused large-scale surface erosion that removed the source of 137Cs.

Contrasting seasonality of 137Cs concentrations in two stream animals that share a trophic niche

Understanding the seasonality of 137Cs concentrations in aquatic animals is crucial for reviving local inland fisheries. The seasonality of 137Cs concentrations in animals is expected to vary, even if focal species consume similarly contaminated foods because the 137Cs excretion rate is species-specific, and 137Cs uptake by foraging autochthonous food resources also vary among seasons. Here, we conducted a seasonal monitoring survey of dissolved 137Cs concentrations as an indicator of the contamination level of food resources and measured 137Cs concentrations in two carnivorous aquatic animals (Palaemon paucidens and Rhinogobius sp.) that share a trophic niche in a stream connected to a dam reservoir. The dissolved 137Cs concentration had clear seasonality—high in summer and low in winter. The 137Cs concentrations in the animals revealed a different seasonal pattern—it peaked in October in P. paucidens and peaked in February in Rhinogobius. Overall, the 137Cs concentration was relatively higher in P. paucidens than in Rhinogobius, suggesting that P. paucidens has a lower excretion rate than Rhinogobius. Consequently, the seasonality of the 137Cs concentration in P. paucidens showed temporal changes similar to those of the dissolved 137Cs concentration, which were likely affected by 137Cs uptake through foraging, whereas that in Rhinogobius was controlled by 137Cs excretion. This study shows that the seasonality of 137Cs concentration can differ between sympatric animals that share a trophic niche. Accumulating knowledge and comparing the seasonality of 137Cs concentrations in fisheries species based on the balance between uptake and excretion will be valuable to determine the appropriate seasons to obtain less-contaminated products.

Watershed‐Geochemical Model to Simulate Dissolved and Particulate 137Cs Discharge From a Forested Catchment

AbstractMeasurements in forest catchments in Fukushima Prefecture indicate that cesium‐137 (137Cs) leaching from forest litter affects dissolved 137Cs levels in river water. Existing simulations have been unsuccessful in reproducing this phenomenon due to mechanistic limitations in the models connecting the forest ecosystem and the river system. This paper introduces a new coupled watershed‐geochemical model to address this. We connected a forest ecosystem compartment model to the 3D watershed model General‐purpose Terrestrial Fluid‐Flow Simulator to describe 137Cs transfer between forests and the river system. The compartment model included nonleachable and leachable 137Cs sites in the organic layer. The latter sites model how leachable 137Cs stocks increase with ambient temperature owing to decomposing organic matter. The model was tested by simulating dissolved and particulate 137Cs discharges from a forested catchment upstream of the Ohta River, Fukushima Prefecture. The results for dissolved 137Cs concentrations in river water for 1 January 2014, to 31 December 2015, correlated well with catchment measurements. The simulations reproduced dissolved 137Cs concentration peaks that occurred during three typhoon events and the seasonal variations under baseflow conditions. The results support the theory that leaching from the organic layer in forests is a primary factor affecting river water dissolved 137Cs concentrations. The wider contribution of this study is it introduces a coupled watershed‐geochemical model, applicable not only for evaluating the dynamics of 137Cs, but also those of other substances that adsorb onto sediments and soil particles, and leach from forest organic matter.

Effects of forest litter on dissolved 137Cs concentrations in a highly contaminated mountain river in Fukushima

Study regionThe upper, forested reaches of the Ota River, 24.4 km northwest of the Fukushima Daiichi nuclear power plant, was studied. Study focusThere is concern about the effects of dissolved radiocesium (137Cs) released from forest litter on long-term contamination of aquatic ecosystems caused by the Fukushima nuclear accident. Therefore, hydrology and water quality measurements were performed under base flow and storm flow conditions in a high-dose-rate forest watershed in Fukushima Prefecture, to investigate the involvement of litter in 137Cs release. New hydrological insights for the regionUnder base flow conditions, the dissolved 137Cs activity concentration significantly positively correlated with the dissolved organic carbon and potassium ion concentrations (the main components leached from litter) over the entire study period. Differences in the annual variations in the 137Cs activity concentrations and potassium ion concentrations indicated that litter indirectly increased 137Cs concentrations in river water by releasing potassium ions that caused 137Cs to desorb from river sediment and riparian soil. In each large runoff event, the dissolved 137Cs activity concentration was higher at the time of maximum runoff than at the start of the event. The relationships between the dissolved 137Cs, dissolved organic carbon, and potassium ion concentrations strongly suggested that 137Cs leached from litter in runoff was directly responsible for the increase in the 137Cs activity concentration in river water.

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.

Reconstruction of time changes in radiocesium concentrations in the river of the Fukushima Dai-ichi NPP contaminated area based on its depth distribution in dam reservoir's bottom sediments

Radionuclide depth distribution in bottom sediments in deep-water zones of dam reservoirs, where no sediment mixing occurs, can be used to reconstruct time changes in particulate activity concentrations of radionuclides strongly bound to bottom sediments. This approach was used to analyze the 137Cs concentration profile in a bottom sediment core collected from Ogaki dam reservoir on the Ukedo River in the Fukushima Dai-ichi nuclear power plant contaminated zone in October 2019. The derived 137Cs particulate concentrations provided a basis for estimating the dissolved concentration and its temporal trend in the Ukedo River, using the mean value of the apparent 137Cs distribution coefficient. The reconstructed particulate and dissolved 137Cs concentrations and their temporal trends are consistent with monitoring data. The annual mean particulate and dissolved 137Cs wash-off ratios were also calculated for the period of eight years after the accident. Interestingly, the particulate 137Cs wash-off ratios for the Ukedo River at Ogaki dam were found to be similar to those for the Pripyat River at Chernobyl in the same time period after the accident, while the dissolved 137Cs wash-off ratios in the Ukedo River were an order of magnitude lower than the corresponding values in the Pripyat River. Both the particulate and dissolved 137Cs wash-off ratios in the Ukedo River declined faster during the first eight years after the FDNPP accident than predicted by the diffusional model, most likely, due to greater natural attenuation and, to some extent, remediation measures implemented on the catchments in Fukushima.

Radiocesium distribution and mid-term dynamics in the ponds of the Fukushima Dai-ichi nuclear power plant exclusion zone in 2015–2019

This study analyzes the 137Cs behavior in the ponds of Okuma Town from 2015 to 2019 in the Fukushima Dai-ichi nuclear power plant (FDNPP) exclusion zone. A decline in both particulate and dissolved 137Cs activity concentrations was revealed. The decline rate constants for the particulate 137Cs activity concentration were found to be higher than for the dissolved 137Cs activity concentration. In terms of seasonality the dissolved 137Cs concentrations were higher from June to October, depending on the specific pond and year, most likely due to temperature dependence of 137Cs desorption from frayed edge sites of micaceous clay minerals. The apparent Kd(137Cs) in the studied ponds, in absolute value, appeared to be much higher than that for closed and semi-closed lakes of the Chernobyl contaminated area; however, these were comparable to the values characteristic of the rivers and reservoirs of the FDNPP contaminated area. The apparent Kd(137Cs) in the suspended sediment–water system was observed to decrease over time. It was hypothesized that this trend was associated with the decomposition of glassy hot particles. Relying on the theory of selective sorption and fixation, the exchangeable radiocesium interception potential, RIPex(K) was estimated using data on 137Cs speciation in the surface bottom-sediment layer and its distribution in the sediment–water system. For the studied ponds, RIPex(K) was on the average 2050 mEq/kg, which is within the range of values measured in laboratory studies reported in the literature.

Factors controlling dissolved 137Cs concentrations in east Japanese Rivers

To investigate the main factors that control the dissolved radiocesium concentration in river water in the area affected by the Fukushima Daiichi nuclear power plant accident, the correlations between the dissolved 137Cs concentrations at 66 sites normalized to the average 137Cs inventories for the watersheds with the land use, soil components, topography, and water quality factors were assessed. We found that the topographic wetness index is significantly and positively correlated with the normalized dissolved 137Cs concentration. Similar positive correlations have been found for European rivers because wetland areas with boggy organic soils that weakly retain 137Cs are mainly found on plains. However, for small Japanese river watersheds, the building area ratio in the watershed strongly affected the dissolved 137Cs concentration. One reason for this would be because the high concentrations of solutes, such as K+ and dissolved organic carbon, discharged in urban areas would inhibit 137Cs absorption to soil particles. A multiple regression equation was constructed to predict the normalized dissolved 137Cs concentration with the topography, land use, soil component, and water quality data as explanatory variables. The best model had the building land use as the primary predictor. When comparing two multiple regression models in which the explanatory variables were limited to (1) the land use and soil composition and (2) the water quality, the water quality model underestimated the high normalized dissolve 137Cs concentration in urban areas. This poor reproducibility indicates that the dissolved 137Cs concentration value in urban areas cannot be solely explained by the solid-liquid distribution of 137Cs owing to the influence of the water quality, but some specific 137Cs sources in urban areas would control the dissolved 137Cs concentration.

Reconstruction of long-term dynamics of Chernobyl-derived <sup>137</sup>Cs in the Upa River using bottom sediments in the Scheckino reservoir and semi-empirical modelling

Abstract. Two cores of bottom sediments were collected in 2018 to a depth of ∼200 cm in the deepest part of the Scheckino reservoir on the Upa River (9500 km2), Tula region, Russia. This area was severely contaminated by radiocesium (r-Cs) after the Chernobyl accident in 1986. The fact that 137Cs activity concentrations in a specific horizon of the bottom sediments correspond to 137Cs concentrations associated with suspended matter delivered to the reservoir, provides a basis for constructing the dynamics of particulate 137Cs activity concentrations in the Upa River catchment from 1986 to 2017. Over the time since the Chernobyl accident, the particulate 137Cs concentrations have decreased by more than an order of magnitude, with only minor changes occurring during the last 15 years. Using a typical value for the distribution coefficient Kd for the rivers of the Chernobyl contamination zone, dissolved 137Cs activity concentrations in the Upa River have been estimated and their changes over the past 30 years since the accident have been studied. The resulting estimates of dissolved 137Cs concentrations in the Upa River have been found to be in good agreement with measured data over the period 1987–1991. The proposed and tested method provides a basis for reconstructing the long-term dependence of radionuclide concentrations in rivers and reservoirs based on their vertical distribution in bottom sediments. Reconstructed time dependencies of particulate and dissolved 137Cs activity concentrations in the Upa River were found to be described well by the proposed semi-empirical “diffusion” model based on an assumption that the time dependency of particulate r-Cs in the river corresponds to the time dependency of its concentration in top soil layers across the catchment which can be approximated by a dispersion-convection equation with physically meaningful parameters.

Dissolved 137Cs concentrations in stream water and subsurface water in a forested headwater catchment after the Fukushima Dai-ichi Nuclear Power Plant accident

Numerous studies have been conducted on 137Cs transport in the environment in Fukushima, Japan, since the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. Many studies have monitored river and stream water, and a declining trend in dissolved 137Cs concentrations has been reported. In addition, temporary increases in dissolved 137Cs concentrations have been observed during rainstorm events. However, the source and process of such temporary increases remain poorly understood. To address these gaps in knowledge, intense multi-point sampling and analysis of dissolved 137Cs in stream water, soil water, and groundwater were conducted in a forested headwater catchment in Yamakiya district, located 35 km northwest of the FDNPP, from July 2015 to November 2016. The average dissolved 137Cs concentration in stream water during baseflow conditions was 17 mBq/L, whereas the concentration during rainstorm events was 31 mBq/L (maximum: 170 mBq/L on July 15, 2015). The dissolved 137Cs concentration in groundwater (average: 0.93 mBq/L) was lower than that in stream water. Conversely, high concentrations of dissolved 137Cs in soil water were observed (average: 81 mBq/L), particularly at lower parts of the slope near the spring point and in wet conditions throughout summer. Consequently, the dissolved 137Cs concentrations in stream water were considered to be derived mainly from soil water and diluted by groundwater. The high dissolved 137Cs concentration in soil water may be derived from litter leachate in the shallow soil layer stored on the slope. During rainstorm events, the saturated area expands upward; therefore, the temporary increase in the dissolved 137Cs concentration in stream water observed at the beginning of a rainstorm may be caused by the release of high levels of dissolved 137Cs in soil water stored in the shallow soil layer.

Interannual changes in radiocesium concentrations in annually laminated tufa following the Fukushima Daiichi Nuclear Power Plant accident

Chemical and radiocesium concentrations in water and riverbed tufa of the Nigori River, flowing out of the southern foot of Mt. Asama volcano in central Japan, were investigated following the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. This tufa is characterized by porous and dense laminae. Its annual lamination (varve) is formed by seasonal changes in dissolved CO2 concentration in water with temperature, and the tufa calcite is mostly precipitated during summer. We analyzed radiocesium concentrations in ∼4-mm-thick tufa samples that included four or five varves collected after the fall in 2011–2014. The activity ratio of 134Cs/137Cs in tufa collected in 2011 and 2014 was 0.96 ± 0.01 and 0.99 ± 0.01, respectively, which implies radiocesium generated as a result of the FDNPP. Sequential extractions indicate that 137Cs in tufa collected in 2011 is occupied in exchangeable and carbonate phases (55.2% and 44.8%, respectively). The 137Cs concentrations equivalent to tufa calcite that were precipitated after 2011 showed variations similar to the amount of summer rainfall during 2011–2014, which may be attributed to increases in dissolved 137Cs concentrations in river water associated with intensified rainfall and microbial action over the summer. In contrast, the 137Cs sorbed to tufa calcite was not retained in the riverbed, and its migration may be attributed to the porous texture of tufa and the high flow rate of the river. Therefore, tufa calcite is easier to dissolve even though it adsorbs compared with other minerals (mica, andosol etc.).

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.

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.

Vertical distribution and temporal dynamics of dissolved 137Cs concentrations in soil water after the Fukushima Dai-ichi Nuclear Power Plant accident

Radiocesium (137Cs) migration from headwater forested areas to downstream rivers has been investigated in many studies since the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, which was triggered by a catastrophic earthquake and tsunami on 11 March 2011. The accident resulted in the release of a huge amount of radioactivity and its subsequent deposition in the environment. A large part of the radiocesium released has been shown to remain in the forest. The dissolved 137Cs concentration and its temporal dynamics in river water, stream water, and groundwater have been reported, but reports of dissolved 137Cs concentration in soil water remain sparse.In this study, soil water was sampled, and the dissolved 137Cs concentrations were measured at five locations with different land-use types (mature/young cedar forest, broadleaf forest, meadow land, and pasture land) in Yamakiya District, located 35 km northwest of FDNPP from July 2011 to October 2012. Soil water samples were collected by suction lysimeters installed at three different depths at each site. Dissolved 137Cs concentrations were analyzed using a germanium gamma ray detector. The dissolved 137Cs concentrations in soil water were high, with a maximum value of 2.5 Bq/L in July 2011, and declined to less than 0.32 Bq/L by 2012. The declining trend of dissolved 137Cs concentrations in soil water was fitted to a two-component exponential model. The rate of decline in dissolved 137Cs concentrations in soil water (k1) showed a good correlation with the radiocesium interception potential (RIP) of topsoil (0–5 cm) at the same site. Accounting for the difference of 137Cs deposition density, we found that normalized dissolved 137Cs concentrations of soil water in forest (mature/young cedar forest and broadleaf forest) were higher than those in grassland (meadow land and pasture land).

Behavior of dissolved radiocesium in river water in a forested watershed in Fukushima Prefecture

AbstractDissolved radiocesium concentrations in river water in a high‐dose‐rate forest watershed in Fukushima Prefecture were investigated under base flow and storm flow conditions. Under base flow conditions, dissolved 137Cs concentrations in water (Bq/L) were relatively high in summer, and these levels were higher than particulate 137Cs concentrations (Bq/L). Under storm flow, particulate 137Cs concentration became dominant as the suspended solid concentration increased. Throughout the monitoring period, dissolved 137Cs concentrations in water (Bq/L) were higher under storm flow than base flow conditions and were positively correlated with runoff intensity. Factors influencing changes in dissolved 137Cs concentrations were investigated by measuring the 137Cs concentration of suspended solid (Bq/kg) and dissolved 137Cs of unsaturated soil water, throughfall, and rainfall, together with other main solute concentrations. The 137Cs concentration per unit weight of suspended solids in river water was not strongly correlated with runoff intensity. Additionally, dissolved 137Cs concentrations of soil water, groundwater, and rainfall were not detected, while higher dissolved 137Cs concentrations were detected in throughfall than river water. K+ concentrations were higher under storm flow than base flow, and dissolved organic carbon increased toward the peak flow rate. These findings suggested that one main factor influencing generation of dissolved 137Cs in the river water was leaching from organic material in flooded areas. However, further investigation is needed to clarify the dominant source of dissolved 137Cs in river water.

Spatial and temporal changes of 137Cs concentrations derived from nuclear power plant accident in river waters in eastern Fukushima, Japan during 2012–2014

Concentrations of 137Cs measured in water collected from seven rivers under base-flow conditions in eastern Fukushima Prefecture in 2014 were combined with previously reported data for the same sampling points from 2012 to 2013. Dissolved 137Cs concentrations at the sampling points were strongly correlated with the 137Cs inventories of the corresponding catchment areas. The ratios of the dissolved 137Cs concentrations to the 137Cs inventories have declined exponentially since the 2011 Fukushima nuclear power plant accident with an effective decreasing coefficient of 0.40 y−1 (effective half-time of 1.7 y), within the range reported in European rivers following the Chernobyl accident.

Temporal changes in dissolved 137Cs concentrations in groundwater and stream water in Fukushima after the Fukushima Dai-ichi Nuclear Power Plant accident

The concentration of dissolved 137Cs in groundwater and stream water in the headwater catchments in Yamakiya district, located ∼35 km north west of Fukushima Dai-ichi Nuclear Power Plant (FDNPP), was monitored from June 2011 to July 2013, after the earthquake and tsunami disaster. Groundwater and stream water were sampled at intervals of approximately 2 months at each site. Intensive sampling was also conducted during rainstorm events. Compared with previous data from the Chernobyl NPP accident, the concentration of dissolved 137Cs in stream water was low. In the Iboishi-yama catchment, a trend was observed for the concentration of dissolved 137Cs in stream water to decline, which could be divided into two phases by October 2011 (a fast flush of activity as a result of rapid washoff and a slow decline as a result of soil fixation and redistribution processes). The highest 137Cs concentration recorded at Iboishi-yama was 1.2 Bq/L on August 6, 2011, which then declined to 0.021–0.049 Bq/L during 2013 (in stream water under normal water-flow conditions). During the rainfall events, the concentration of dissolved 137Cs in stream water increased temporarily. The concentration of dissolved 137Cs in groundwater at a depth of 30 m at Iboishi-yama displayed a decreasing trend from 2011 to 2013, with a range from 0.039 Bq/L to 0.0025 Bq/L. The effective half-lives of stream water in the initial fast flush and secondary phases were 0.10–0.21 and 0.69–1.5 y, respectively in the three catchments. The effective half-life of groundwater was 0.46–0.58 y at Koutaishi-yama and 0.50–3.3 y at Iboishi-yama. The trend for the concentration of dissolved 137Cs to decline in groundwater and stream water was similar throughout 2012–2013, and the concentrations recorded in deeper groundwater were closer to those in stream water. The declining trend of dissolved 137Cs concentrations in stream water was similar to that of the loss of canopy 137Cs by throughfall, as shown in other reports of forest sites in the Yamakiya district.

Effects of radiocesium inventory on 137Cs concentrations in river waters of Fukushima, Japan, under base-flow conditions

To investigate the behavior of nuclear accident-derived 137Cs in river water under base-flow conditions, concentrations of dissolved and particulate 137Cs were measured at 16 sampling points in seven rivers of Fukushima Prefecture, Japan, in 2012 and 2013. The concentration of dissolved 137Cs was significantly correlated with the mean 137Cs inventory in the catchment area above each sampling point in both sampling years. These results suggest that the concentration of dissolved 137Cs under base-flow conditions is primarily determined by the 137Cs inventory of the catchment area above the sampling point. However, the concentration of particulate 137Cs did not show a clear relationship with either the mean 137Cs inventory or the dissolved 137Cs concentration, thus indicating that particulate and dissolved forms do not effectively interact in rivers. To evaluate the contribution of the 137Cs inventory within catchment areas, we analyzed relations between the 137Cs concentration and the mean 137Cs inventory over the area within certain flow path lengths that were traced along the river and slope above the sampling point. Coefficients of determination for dissolved 137Cs concentrations were highest for the longest flow path, i.e., the whole catchment area, and lower for shorter flow paths. Coefficients of determination for particulate 137Cs concentrations were only moderately high for the shortest flow path in 2012, whereas the values were quite low for all flow paths in 2013. These results suggest that dissolved 137Cs can originate from a larger area of the catchment even under base-flow conditions; however, particulate 137Cs did not show such behavior. The results also show that under base-flow conditions, dissolved and particulate 137Cs behave independently during their transport from river catchments to the ocean.