Temporal variation of tritium concentration in monthly precipitation collected at a Difficult-to-Return Zone in Namie Town, Fukushima Prefecture, Japan.

This article discusses tritium concentrations in monthly precipitation in part of the Difficult-to-Return Zone in Namie Town during 2012-2021. The tritium concentrations, which were measured with a low background liquid scintillation counter after carrying out an enrichment procedure, fluctuated seasonally from 0.10 ± 0.02 to 0.85 ± 0.02 Bq L-1. This range of concentrations is concluded to not be unusual based on comparisons with the concentrations at other sites and estimates of the past range of the concentrations. Moreover, no significant variations in observed tritium concentrations were observed due to decommissioning work at the Fukushima Dai-ichi Nuclear Power Plant. These results contribute to understanding the background level of tritium concentration in precipitation before the oceanic discharge of treated water from the Fukushima plant. In addition, this article evaluates the amount of tritium supplied to the ocean by terrestrial rainwater pouring into the Pacific Ocean via Ukedo River, which flows through Namie Town; this information will contribute to the discussion on the impact of the oceanic discharge of treated water.

140 years-long sedimentary records of PAHs and CN stable isotopes from Ninomiya River, Japan.

Anthropogenic activities' impacts over 140 years were studied at West Nanao Bay using a variety of geochemical techniques on sedimentary records. The bay is influenced by the Ninomiya River which is fed by a small watershed at which Tatzuruhama Town is located. Sedimentation rate was calculated using 210Pb-excess and 137Cs activities. C/N decreased after 1975, indicating a decrease in lignin-rich organic matter. From δ13C, δ15N and biogenic silica it was indicated that the population increased sewage-discharges until the construction of waste-water treatment plant in 1986. Several recorded changes in the landuse matched with the variation of the particle size. Total PAHs concentration was 1.17-62.78 µg g-1, being highest during Japan's fastest economic growth period (1946-1975). Using diagnostic ratios and PCA analysis, PAHs' sources were identified as pyrogenic for all depths, varying from coal combustion (90.7 %) before 1946 to a mixture of biomass and vehicle combustion after 1961.

DISTRIBUTIONS OF 210PB, 137CS AND PHYSICAL PROPERTIES IN BOTTOM SEDIMENTS OF WEST NANAO BAY, JAPAN.

This study revealed sedimentation processes based on 137Cs and 210Pb distribution, grain size and magnetic susceptibility of bottom sediments in West Nanao Bay, Japan. Surface sediment concentrations and inventories of these radionuclides were relatively low in the middle and eastern areas of the bay and high in the western area, which has several major river mouths, suggesting that the contribution of riverine input affected only the western area. In the middle and eastern areas, the level of 137Cs inventory was much lower than that of the soils, and the excess 210Pb inventory was at the same level or lower. These results indicate that removal effects are stronger than accumulation effects (riverine input) in these areas. The patterns of radionuclides were consistent with the results, that grain size was relatively large in the middle and eastern areas, implying strong current conditions, and that fine sediment accumulated less in these areas.

TEMPORAL VARIATION IN RADIOCESIUM CONCENTRATIONS IN WATERS OF THE NATSUI AND SAME RIVERS, SOUTH FUKUSHIMA PREFECTURE, JAPAN FROM 2011 TO 2020.

In order to determine the long-term impacts of radiocesium contamination on ecosystems in watersheds and coastal areas following the Fukushima Daiichi Nuclear Power Plant accident in March 2011, it was important to monitor the transport behavior of radiocesium from an early stage. In this study, conducted from July 2011 to October 2020, we carried out field research along the Natsui and Same rivers running through watersheds in the south of Fukushima Prefecture, Japan, in which there had been a relatively low accumulation of radiocesium. We found that under normal flow conditions, the total (dissolved + particulate phase) activity of 137Cs decreased with increasing time following the accident. However, the water samples collected after rain events showed higher activity of up to 895 mBq l-1 with a higher percentage (>92% of total) of the particulate phase. These findings indicate that radiocesium deposited on the ground surface is predominantly transported in the particulate phase from watersheds to rivers via precipitation. The decontamination process, which was performed in the farmland during December 2014 to March 2015 and in forest during February 2013 to April 2014, was small effects of the transport of 137Cs. Under normal flow conditions, total 137Cs activity was largely determined by the suspended solids (SS) concentration and/or 137Cs concentration in the SS.

TEMPORAL VARIATION OF POST-ACCIDENT 129I IN ATMOSPHERIC PARTICULATE MATTER COLLECTED FROM AN EVACUATED AREA OF FUKUSHIMA PREFECTURE, JAPAN.

To understand the behavior of atmospheric 129I that originated from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, activity concentrations of 129I in samples of atmospheric particulate matter (PM), comprising coarse (>1.1 µm) and fine (<1.1 µm) fractions (separated using a single stage impactor), were measured on a nearly monthly basis from October 2012 to October 2014 at a site in an area evacuated after the FDNPP accident. Total atmospheric 129I activity concentrations in PM at the site ranged between 0.15 and 2.17 nBq m-3. Specific activity concentration of 129I in total atmospheric PM ranged between 40.8 and 336 mBq kg-1, with a mean and standard deviation of 142 and 77.6 mBq kg-1, respectively. The specific activity in PM tended to be higher than not only the background values reported from soil collected before the FDNPP accident but also than those reported from the contaminated soil after the accident (range: 1.6-57 mBq kg-1; mean and standard deviation: 10.6 and 12.3 mBq kg-1, respectively). Total 129I/127I atomic ratios in PM ranged from 2.0 × 10-8 to 59.8 × 10-8, with a mean and standard deviation of 15.0 × 10-8 and 14.4 × 10-8, respectively. These ratios were generally lower than those of the contaminated soil collected after the FDNPP accident (range: 4.9 × 10-8-443 × 10-8; mean and standard deviation: 74.2 × 10-8 and 85.4 × 10-8, respectively). The 129I concentration and 129I/127I atomic ratio in atmospheric PM showed different characteristics from that of contaminated soils, suggesting that the presence of other atmospheric PMs plays a more important role as the host for 129I.

Environmental processes and fate of PAHs at a shallow and enclosed bay: West Nanao Bay, Noto Peninsula, Japan.

From August 2019 to August 2020, particulate and dissolved polycyclic aromatic hydrocarbons concentrations (PAHs) were analyzed in the water body of West Nanao Bay, Japan, to determinate their levels, environmental pathways, and ecological risks at this remote but shallow and semi-enclosed bay. The 14 targeted PAHs were analyzed by high performance liquid chromatography-fluorescence detector. Even when water column stratifies, the summatory of 14 targeted dissolved PAHs did not follow significantly change with depth. Results agreed with our previous findings in the surface distribution at the bay and can be attributed to long retention time of the water mass of the semi-enclosed bay. Suspended solids start precipitating according to their size; with biggest particles rapidly settling in the proximities of river mouths. Partition coefficients (Kp) varied from 103 to 107, according to molecular weights. In general, highest Kp were found in the nepheloid layer. The risk quotients, RQ∑14 PAHs (NCs) (1.04-174.08), indicated that PAHs represented a very low to low environmental risks.

Geochemical Control of PAHs by Inflowing River Water to West Nanao Bay, Japan, and Its Influences on Ecological Risk: Small-Scale Changes Observed under Near-Background Conditions at an Enclosed Bay.

Polycyclic aromatic hydrocarbons (PAHs), even at low concentrations, have been shown to trigger changes in life cycles and provoke abnormal behaviors in numerous marine organisms. From May 2019 to September 2020, particulate and dissolved PAH concentrations were analyzed on the surface water of West Nanao Bay, Japan, to determinate their levels, emission sources, environmental pathways, and ecological risks at this remote but semi-enclosed bay. The 14 targeted PAHs were analyzed by HPLC-fluorescence detector. Mean total PAH concentrations were lower than 20.0 ng L-1 for most samples. Based on fluoranthene (Flu) to pyrene (Pyr) ([Flu]/[Flu + Pyr]) and benzo[a]anthracene (BaA) to chrysene (Chr) ([BaA]/[BaA + Chr]) isomeric ratios and a varimax rotated PCA, it was established that biomass combustion was the principal source in the particulate phase and that liquid fossil fuel combustion was the principal source in the dissolved phase. From salinity and turbidity distribution, riverine discharges were determined to be the major and continuous transportation pathway of particulate PAHs. It was observed that rain events had a role in the transport of dissolved PAHs. The risk quotients (RQ∑14 PAHs (NCs): 0-84.53) indicated that PAHs represented a very low to low acute environmental risk. The results of this study will contribute to filling the paradigm gap of ecotoxicological studies in remote areas, working as a booster for future in-lab studies of non-lethal implications of endocrine disruptors such as PAHs.

Ten-year radiocesium fluvial discharge patterns from watersheds contaminated by the Fukushima nuclear power plant accident.

After the Fukushima Dai-ichi nuclear power plant accident in March 2011, the fluvial discharge of 137Cs from watersheds to rivers was analyzed between 2011 and 2021. The concentrations of dissolved and particulate 137Cs were measured in river water samples collected from two rivers (the Hiso and Wariki rivers, mainly draining farmlands and forests, respectively) draining approximately 4-7 km2 watersheds in a montane area (the areal deposition of 134+137Cs; 1-3 MBq·m-2 in March 2011) of Iitate Village, Fukushima. Over the 10 yr analysis, the particulate 137Cs concentrations in the Hiso and Wariki rivers decreased by 70 and 50 times, respectively, and that of the dissolved form decreased by 150 and 130 times, respectively. Moreover, the apparent Kd (distribution coefficient) of 137Cs for water samples from both rivers have increased gradually over these periods. In 2011, the 137Cs discharge rates through the Hiso and Wariki rivers were 0.63% and 0.46% per year of the total amount of 137Cs deposited in their catchments, respectively; however, by 2021, these rates had decreased to 0.09% and 0.03% per year. The cumulative 137Cs discharge rates over 10 yr in the farmland- and forest-dominated rivers were 1.95% and 1.33%, respectively. These rates of the farmland-dominated river were ∼1.4-fold greater than those of the forest-dominated river. Moreover, ∼90% of the of the discharge occurred in particulate form while the remaining ∼10% was in the dissolved form. Thus, 137Cs deposited within these watersheds due to the accident was gradually discharged by the rivers over the 10-yr period; however, the majority remains stored in soils and litters etc. of the catchment area. These results indicate that 137Cs outflow from land-to-ocean will be limited in the future, as the river export of 137Cs is expected to continue decreasing.

Desorption Behavior of Fukushima-derived Radiocesium in Sand Collected from Yotsukura Beach in Fukushima Prefecture.

Beach sand samples were collected along a coastal area 32 km south of the Fukushima Daiichi Nuclear Power Plant (FDNPP) in Fukushima Prefecture, Japan, 5 years after the FDNPP accident. Desorption experiments were performed on the sand samples using seawater in a batch experimental system to understand the forms of existence of radiocesium in sand and their desorption behavior in a coastal environment. The percentage of radiocesium desorption decreased exponentially with an increase in the number of desorption experiments for the four sand samples, with 137Cs radioactivity from 16 to 1077 Bq kg-1 at surface and deeper layers from three sites. Total desorption percentage ranged from 19 to 58% in 12 desorption experiments. The results indicate that the weak adsorption varies with the sampling sites and their depth layer. To understand the desorption behavior of radiocesium in the sand samples, the desorption experiments were performed for a sand sample by using natural and artificial seawater, and NaCl solution in the presence and absence of KCl. The 137Cs desorption from the sand collected at a depth of 100 - 105 cm from the ground surface (137Cs radioactivity 1052 ± 25 Bq kg-1) was 0.1% by ultrapure water, 3.7% by 1/4 seawater and 7.1% by 1/2 seawater, 2.2% by 470 mM NaCl solution (corresponding to a similar concentration of seawater) and 10 - 12% by seawater, artificial seawater and 470 mM NaCl + 8 mM KCl solution. These results indicate that about 10% of radiocesium adsorbed on the sand is mainly desorbed by ion exchange of potassium ion in seawater, though the concentration of major cation, or sodium ion, in seawater makes a small contribution on 137Cs desorption from the sand samples.

Temporal variation of post-accident atmospheric 137Cs in an evacuated area of Fukushima Prefecture: Size-dependent behaviors of 137Cs-bearing particles.

The concentrations of 137Cs in the air, which were divided into coarse (>1.1 µm ϕ) and fine (<1.1 µm ϕ) fractions of particulate matter (PM), were measured from October 2012 to December 2014 in an area evacuated after the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. Total atmospheric 137Cs concentrations showed a clear seasonal variation, with high concentrations during summer and autumn related to the dominant easterly wind blowing from the highly radioactivity contaminated area. This seasonal peak was dominated by 137Cs in the coarse PM fraction. The 137Cs specific activity (massic 137Cs concentration) in the coarse PM was also found to increase significantly in summer, whereas that in the fine PM showed no variability during the year. These results show that coarse and fine 137Cs-bearing PM have different origins and behaviors in the resuspension process. The seasonal variation in atmospheric 137Cs concentration was well correlated with the mean 137Cs surface contamination (deposition density) around the observation site weighted by the frequency of wind direction, indicating that the atmospheric 137Cs concentration in the observation site was explained by the distribution of the 137Cs surface contamination and the frequency of different wind directions. We introduced a resuspension factor corrected for wind direction, consisting of the ratio of the atmospheric 137Cs concentration to the weighted mean 137Cs surface contamination, which evaluated the intensity of resuspension better than the conventional resuspension factor. This ratio ranged from 5.7 × 10-11 to 8.6 × 10-10 m-1 and gradually decreased during the study period.

Nuclear accident-derived (3)H in river water of Fukushima Prefecture during 2011-2014.

During 2011-2014, we measured (3)H concentrations in river water samples collected during base flow conditions and during several flood events from two small rivers in a mountainous area in Fukushima Prefecture, which received deposition of (137)Cs from the Fukushima Dai-ichi Nuclear Power Plant accident. (3)H concentrations above background levels were found in water samples collected during both base flow conditions and flood events in 2011. The (3)H concentrations during flood events were generally higher than those during base flow conditions. The (3)H concentrations in both rivers during base flow conditions and flood events decreased with time after the accident and reached almost background levels in 2013. We also measured (3)H concentrations in freshwater samples from 16 other rivers and one dam in eastern Fukushima Prefecture from 2012 to 2014 during base flow conditions. The measured (3)H concentrations were higher than the background level in 2012 and decreased with time. The (137)Cs inventory in the catchment area at each sampling point was estimated from air-borne monitoring results in the literature and compared with the (3)H concentrations. We found surprisingly good correlations between (137)Cs inventories in the catchment areas and (3)H concentrations in the water samples. Further studies will be necessary to clarify the reason for the good correlation.

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

To investigate the behavior of nuclear accident-derived (137)Cs in river water under base-flow conditions, concentrations of dissolved and particulate (137)Cs were measured at 16 sampling points in seven rivers of Fukushima Prefecture, Japan, in 2012 and 2013. The concentration of dissolved (137)Cs was significantly correlated with the mean (137)Cs inventory in the catchment area above each sampling point in both sampling years. These results suggest that the concentration of dissolved (137)Cs under base-flow conditions is primarily determined by the (137)Cs inventory of the catchment area above the sampling point. However, the concentration of particulate (137)Cs did not show a clear relationship with either the mean (137)Cs inventory or the dissolved (137)Cs concentration, thus indicating that particulate and dissolved forms do not effectively interact in rivers. To evaluate the contribution of the (137)Cs inventory within catchment areas, we analyzed relations between the (137)Cs concentration and the mean (137)Cs 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 (137)Cs 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 (137)Cs 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 (137)Cs can originate from a larger area of the catchment even under base-flow conditions; however, particulate (137)Cs did not show such behavior. The results also show that under base-flow conditions, dissolved and particulate (137)Cs behave independently during their transport from river catchments to the ocean.

Deposition records in lake sediments in western Japan of radioactive Cs from the Fukushima Dai-ichi nuclear power plant accident.

Sediment trap observations of lakes in western Japan before and after Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident indicate that changes in the radioactive Cs discharge are influenced by fluctuations in precipitation and geomorphological conditions in each catchment. Contributions of FDNPP-derived (134,137)Cs to the sediment decreased from 19-48% to 10-15% within a few months, implying that the major transport processes of FDNPP-derived (134,137)Cs have changed from direct fallout to transport by soil particles.