Impact of the Fukushima Accident on 3H and 14C Environmental Levels: A Review of Ten Years of Investigation.

The investigation of the impact of the Fukushima accident is still going on although more than ten years have passed since the disaster. The main goal of this paper was to summarize the results of tritium and radiocarbon determinations in different environmental samples, possibly connected with the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. A document containing compiled data may serve as a solid basis for further research in the selected fields. To accomplish such effort, we went through dozens of relevant published papers, reporting 3H and 14C activity concentrations in precipitations, groundwater, seawater, river systems, tree rings, and, in some more extraordinary samples, such as herbaceous plants or debris from the damaged reactor buildings. As the referenced results would not be obtainable without adequate analytical techniques, the most common methods for routine measurement of tritium and radiocarbon concentrations are discussed as well. We believe that the correct identification of the affected environmental compartments could help quantify the released 3H and 14C activities and track their following fate, which could be especially important for plans to discharge contaminated water from the FDNPP in the upcoming years.

External Doses Available for Epidemiological Studies Related to the Fukushima Health Management Survey: First 4-month Individual Doses and Municipality-average Doses for the First Year.

BACKGROUND: One of the components of the Fukushima Health Management Survey (FHMS) is the Basic Survey, which estimates individual external doses for the first 4 months after the 2011 nuclear power plant accident. However, external exposure continues long-term. According to estimations by international organizations, the external dose during the first year accounts for a significant part of the long-term dose. Thus, the present study was intended to estimate the first-year doses by extrapolating the Basic Survey results. METHODS: For most municipalities of non-evacuated areas, ambient dose rate had been continuously measured for at least one designated point in each municipality after the accident. In the present study, a municipality-average dose received by residents for a period was assumed to be proportional to the ambient dose measured at the designated point of that municipality during the same period. Based on this assumption, 4-month municipality-average doses calculated from the Basic Survey results were extrapolated to obtain first-year doses. RESULTS: The extrapolated first-year doses for 49 municipalities in the non-evacuated areas had a good correlation with those estimated by UNSCEAR, although the extrapolated doses were generally higher (slope of the regression line: 1.23). The extrapolated municipality-average doses were in reasonable agreement (within 30%) with personal dosimeter measurements, suggesting that the extrapolation was reasonable. CONCLUSION: The present paper reports the first 4-month average doses for all 59 municipalities of Fukushima Prefecture and the extrapolated first-year doses for 49 municipalities. The extrapolated doses will be the basis for future epidemiological studies related to the FHMS.

An assessment on the environmental contamination caused by the Fukushima accident.

The radiological releases from the damaged fuel to the atmosphere and into the cooling water in the Fukushima Daiich Nuclear Power Plant (FDNPP) accident are investigated. Atmospheric releases to the land and ocean mostly occurred during the first week after the accident whereas continuous release from the damaged fuel into the cooling water resulted in an accumulation of contaminated water in the plant during last six years. An evaluation of measurement data and analytical model for the release of radionuclides indicated that atmospheric releases were mainly governed by the volatility of the radionuclides. Using the measurement data on the contaminated water, the mechanism for the release of long-lived radionuclides into the cooling water was analyzed. It was found that the radioactivity concentrations of 90Sr in the contaminated water in the Primary Containment Vessel (PCV) of unit 2 and unit 3 were consistently higher than that of 137Cs and the radioactivity concentration of 90Sr in the turbine building of unit 1 in year 2015 was higher than that in year 2011. It was also observed that the radioactivity concentration of long-lived radionuclides in the contaminated water in the FDNPP is still high even in year 2015. The activity ratio of 238Pu/239+240Pu for the contaminated water was in the range of 1.7-5.4, which was significantly different from the ratios from the soil samples representing the atmospheric releases of FDNPP. It is concluded that the release mechanisms into the atmosphere and cooling water are clearly different and there has been significant amount of long-lived radionuclides released into the contaminated water.

Errata: Internal doses from radionuclides and their health effects following the Fukushima accident (J. Radiol. Prot. 2018 38 1253-68).

This article presents errata on a published article.

Ultrastructural Analysis of Large Japanese Field Mouse (Apodemus speciosus) Testes Exposed to Low-Dose-Rate (LDR) Radiation after the Fukushima Nuclear Power Plant Accident.

Since the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, great attention has been paid to the impact of chronic low-dose-rate (LDR) radiation exposure on biological systems. The reproductive system is sensitive to radiation, with implications connected to infertility. We investigated the testis ultrastructure of the wild large Japanese field mouse (Apodemus speciosus) from three areas contaminated after the FDNPP accident, with different levels of LDR radiation (0.29 µSv/h, 5.11 µSv/h, and 11.80 µSv/h). Results showed good preservation of the seminiferous tubules, comparable to the unexposed animals (controls), except for some ultrastructural modifications. Increases in the numerical density of lipid droplet clusters in spermatogenic cells were found at high levels of LDR radiation, indicating an antioxidant activity rising due to radiation recovery. In all groups, wide intercellular spaces were found between spermatogenic cells, and cytoplasmic vacuolization increased at intermediate and high levels and vacuolated mitochondria at the high-level. However, these findings were also related to the physiological dynamics of spermatogenesis. In conclusion, the testes of A. speciosus exposed to LDR radiation associated with the FDNPP accident showed a normal spermatogenesis, with some ultrastructural changes. These outcomes may add information on the reproductive potential of mammals chronically exposed to LDR radiation.

Radioactivity of the atmospheric aerosols detected by CTBTO stations in Africa following the accident at the Fukushima Daiichi nuclear power plant.

Radionuclides from the reactor accident Fukushima Daiichi nuclear power plant were observed in the airborne aerosols at CTBT International Monitoring System (IMS) stations (MRP43, CMP13) in Africa. The maximum activity concentrations in the air measured in Mauritania were 186.44 10-6 Bq.m-3, 264.16 10-6 Bq.m-3 and 1269.94 10-6 Bq.m-3 for 134Cs, 137Cs and 131I respectively, and in Cameroon 16.42 10-6 Bq.m-3, 25.53 10-6 and 37.58 10-6 Bq.m-3 respectively for 134Cs, 137Cs and 131I. The activity ratio of 134Cs/137Cs is almost constant throughout the period of time relevant to this study due to their long half-lives of 30.2 years for 137Cs and 2.06 years for 134Cs. Whereas the 131I/137Cs activity ratio varies in time according to the radioactive decay with a half-live of 8.06 days for 131I and different removal rates of both radionuclides from the atmosphere during transport. The EMAC atmospheric chemistry-general circulation was used to simulate the emission and transport of the isotope 137Cs and map the deposition of the 137Cs deposition over Africa.

Review of the sources and behaviors of plutonium isotopes in the atmosphere and ocean.

Plutonium, as well as fission products such as 137Cs, had been released into the earth environment in 1945 after the first atmospheric nuclear explosion of plutonium bomb in the desert of New Mexico (USA, July 16) and later over Nagasaki (August 9), followed then by many other explosions. Thus, plutonium cycling in the atmosphere and ocean has become a major public concern as a result of the radiological and chemical toxicity of plutonium. However, plutonium isotopes and 137Cs are important transient tracers of biogeochemical and physical processes in the environment, respectively. In this review, we show that both physical and chemical approaches are needed to comprehensively understand the behaviors of plutonium in the atmosphere and ocean. In the atmosphere, plutonium and 137Cs attach with aerosols; thus, plutonium moves according to physical and chemical processes in connection with aerosols; however, since plutonium is a chemically reactive element, its behavior in an aqueous environment is more complicated, because biogeochemical regulatory factors, in addition to geophysical regulatory factors, must be considered. Meanwhile, 137Cs is chemically inert in aqueous environments. Therefore, the biogeochemical characteristics of plutonium can be elucidated through a comparison with those of 137Cs, which show conservative properties and moves according to physical processes. Finally, we suggest that monitoring of both plutonium and 137Cs can help elucidate geophysical and biogeochemical changes from climate changes.

Dataset on Cs-137 in waters surrounding Taiwan.

The Fukushima accident released short-lived Cs-134 and longer-lived Cs-137 to the ocean. The amount, although substantial, is much less than that produced during the atomic bomb tests 60 yrs ago. Cs-134 and Cs-137 are anthropogenic radionuclides and soluble in seawater; hence, the radioactivity can be used as a tracer for special events or currents. Samples of Cs-134 and Cs-137 in seawater were collected around Taiwan, including the Kuroshio, the northern South China Sea, the Taiwan Strait, and the southern East China Sea from 2018 to 2021. The average surface Cs-137 activity was 1.18±0.25 Bq m - 3, and the activities of Cs-134 samples were all under the detection limit. Complete data are archived, including sampling date, location, water depth, temperature, salinity, and Cs-137 activity; the total sample amount is 577.

Strontium-90 levels in seawater southeast of Jeju Island during 2021-2023.

This study introduces an efficient method for determining 90Sr activity levels in seawater, reducing the processing time to <3 h for 50 L of seawater. The key feature of the proposed method is the chemical separation of 90Y when it is in equilibrium with 90Sr, which is achieved by utilizing custom-made sample-loading equipment and an automated radionuclide separation instrument. As a result, the procedure consistently yields a recovery rate > 90 % for 90Y. Investigations of 90Sr levels were conducted in the ocean southeast of Jeju Island from November 2021 to January 2023. Owing to the regional ocean circulation, this region was among the first within the Korean Peninsula to experience the impact of the Fukushima-accident-derived radionuclides. Throughout the investigation period, the observed 90Sr activity concentration ranged from 0.57 to 1.0 Bq m-3. No distinct temporal variation of 90Sr was observed in the selected area during the investigation.

Removal of iodine by dry adsorbents in filtered containment venting system after 10 years of Fukushima accident.

Radioactive iodine is a hazardous fission product and a major concern for public health. Special attention is paid to iodine out of 80 fission products because of its short half-life of 8.02 days, high activity, and potential health hazards like its irreversible accumulation in thyroid gland and ability to cause thyroid cancer locally. Radioactive iodine can get released in the form of aerosols (cesium iodide), elemental iodine, and organic iodide after a nuclear accident and can cause off-site and on-site contamination. Filtered containment venting system (FCVS) is a safety system whose main objective is mitigation of severe accidents via controlled venting and removal of different forms of iodine to ensure safety of people and environment. After nuclear accidents like Fukushima, extensive research has been done on the removal of iodine by using dry scrubbers. This review paper presents research status of iodine removal by dry adsorbents especially after 10 years of Fukushima to assess the progress, research gap, and challenges that require more attention. A good adsorbent should be cost-effective; it should have high selective adsorption towards iodine, high thermal and chemical stability, and good loading capacity; and its adsorption should remain unaffected by aging and the presence of inhibitors like CO, NO2, CH3Cl, H2O, and Cl2 and radiation. Research on different dry adsorbents was discussed, and their capability as a potential filter for FCVS was reviewed on the basis of all the above-mentioned features. Metal fiber filters have been widely used for removal of aerosols especially micro- and nanoscale aerosols. For designing a metal fiber filter, optimal size or combination of sizes of fibers, number of layers, and loading capacity of filter should be decided according to feasibility and requirement. Balance between flow resistance and removal efficiency is also very important. Sand bed filters were successful in retention of aerosols, but they showed low trapping of iodine and no trapping of methyl iodide at all. For iodine and methyl iodide removal, many adsorbents like activated carbon, zeolites, metal organic frameworks (MOFs), porous organic frameworks (POPs), silica, aerogels, titanosilicates, etc. have been used. Impregnated activated carbon showed good results but low auto-ignition temperature and decline in adsorption due to aging and inhibitors like NOx made them less suitable. Silver zeolites have been very successful in methyl iodide and iodine removal, but they are expensive and affected by presence of CO. Titanosilicates, macroreticular resins, and chalcogels were also studied and they showed good adsorption capacities, but their thermal stability was low. Other adsorbents like silica, MOFs, aerogels, and POPs also showed promising results for iodine adsorption and good thermal stability, but very limited or no research is available on their performance in severe accident conditions. This review will be very helpful for researchers to understand the merits and demerits of different types of dry adsorbents, the important operating parameters that need optimization for designing an efficient scrubber, margin of research, and foreseeable challenges in removal of different forms of iodine.

Effects of Ionizing Radiation on Flora Ten Years after the Fukushima Dai-ichi Disaster.

The aim of this work is to analyze the effects of ionizing radiation and radionuclides (like 137Cs) in several higher plants located around the Fukushima Dai-ichi Nuclear Power Plant (FNPP), evaluating both their adaptive processes and evolution. After the FNPP accident in March 2011 much attention was focused to the biological consequences of ionizing radiation and radionuclides released in the area surrounding the nuclear plant. This unexpected mishap led to the emission of radionuclides in aerosol and gaseous forms from the power plant, which contaminated a large area, including wild forest, cities, farmlands, mountains, and the sea, causing serious problems. Large quantities of 131I, 137Cs, and 134Cs were detected in the fallout. People were evacuated but the flora continued to be affected by the radiation exposure and by the radioactive dusts' fallout. The response of biota to FNPP irradiation was a complex interaction among radiation dose, dose rate, temporal and spatial variation, varying radiation sensitivities of the different plants' species, and indirect effects from other events. The repeated ionizing radiations, acute or chronic, guarantee an adaptation of the plant species, demonstrating a radio-resistance. Consequently, ionizing radiation affects the genetic structure, especially during chronic irradiation, reducing genetic variability. This reduction is associated with the different susceptibility of plant species to chronic stress. This would confirm the adaptive theory associated with this phenomenon. The effects that ionizing radiation has on different life forms are examined in this review using the FNPP disaster as a case study focusing the attention ten years after the accident.

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.

Ten years of investigations of Fukushima radionuclides in the environment: A review on process studies in environmental compartments.

In March 2011, severe nuclear accident happened at the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) after the gigantic earthquake and following huge tsunami wave. A lot of investigations to assess environmental and radiological impacts of released radionuclides have been conducted by domestic and international organizations. Environmental radioactivity research related to the FDNPP accident has spread widely over different scientific fields due to specific features of the accident, and specifically its impact on the marine environment. The present paper summarizes major lessons learned from the environmental investigations of the FDNPP accident. Environmental radioactivity studies have typical interdisciplinary character; especially physics and chemistry are fundamental as a base of process studies in the environment. In this sight, we review chemical aspects regarding FDNPP-derived radiocesium transfer within and between compartments (atmosphere, ocean and land). We also discuss future trends in investigations of behavior of anthropogenic radionuclides in the environment, important not only for a better understanding of impacts of the FDNPP accident on the environment, but also for improving our general knowledge of the total environment in the Anthropocene era and its protection for the future.

An investigation of corium in Fukushima Daiichi Unit-1 accident.

The core melt composition resulting from the Fukushima Daiichi Unit1 Nuclear Power Plant (FD-U1) accident is essential for the corium characterization phase before decommissioning or handling of radioactive waste. Several models were applied by different research groups for the estimation of corium composition. In this paper, the investigation of the isotopic composition, and radioactivity of the radio-nuclides in the corium10 and 50 years post-accident were calculated using Monte Carlo code, MCNPX 2.7. The results showed that the estimated core materials inventory at reactor scram before core melt was about 123.97 ton, and after the formation of the corium melt was about 140.702 ton, which agrees with the predictions calculated using other models. Also, the total corium activity was about 6.046E+17 Bq and 1.89E+17 Bq 10 and 50 years post- accident, respectively. The radionuclide compositions in the corium are necessary for decommissioning plan of F-D-U1. Furthermore, RELAP/SCDAPSIM MOD3.4 code was used for the analysis of thermal performance of the FD-U1 reactor core starting from the time of the accident up to corium formation and slumping to the lower head of the reactor pressure vessel (RPV). Our analysis indicates that the hydrogen generation started on March11th, around 18:39. The results were compared with MELCOR code and OECD/NEA BSAF Phase I results, which were found in good agreement.

The Kuroshio radiocesium stream.

The Fukushima accident released short-lived Cs-134 and longer-lived Cs-137 to the ocean. The amount, although substantial, is much less than that produced during the atomic bomb tests 60 years ago. But, the latter has received little attention. Here we found only Cs-137 in waters near the origin of the Kuroshio. The speed of the Kuroshio current generally decreases with water depth, yet, the Cs-137 activity increases with depth to reach a subsurface maximum of 2.4 Bq m-3. As a result, a core of high Cs-137 flux, or a radiocesium stream, exists at approximately 200-400 m in depth. In total, the Kuroshio transports about 1 PBq year-1 Cs-137 northward between 121 and 123°E, 1000 times more than the 0.73-1.0 TBq year-1 discharged to the ocean at Fukushima in 2016-2018.

Late phase radiocesium dynamics in Fukushima forests post deposition.

The long term dynamics of radiocesium in typical forest ecosystems was studied in the radioactive contaminated areas in Fukushima Prefecture. Six observations sites located in Yamakiya Village (Kawamata Town; since 2014), Tsushima Village (Namie Town, since 2015), and Tomioka Town (since 2017) were monitored. The forests consisted of artificial plantations of Japanese cedar (Cryptomeria japonica) at Yamakiya Village, Tsushima Village, and Tomioka Town. Tsushima Village also had a natural mixed forest dominated by Japanese red pine (Pinus densiflora), and Tomioka Town had a young and a mature artificial plantation of Japanese cypress (Chamaecyparis obtuse). Concentrations of 137Cs were monitored in the samples collected from the main aboveground biomass compartments, fresh litterfall, forest litter, and soil. Concentrations of exchangeable forms of 137Cs and stable K were measured in soil samples. During the observation period, the litter radiocesium inventories at all sites decreased significantly to approximately 1% or less of the total ground deposition. Approximately 80% of the total radiocesium inventory is localized in the upper 5-cm layer of soil and there is little downward migration of radiocesium. At the sites with the longest monitoring series (Yamakiya and Tsushima), the radiocesium expectation depths and expectation mass depths were relatively constant at 2-3 cm and 5-6 kg m-2, respectively. Aboveground biomass compartments showed similar decreasing trends in radiocesium aggregated transfer factors, Tag, in the compartments that were exposed to atmospheric fallout in March 2011 (old foliage, small branches, and outer bark). The mean Tag in cedar stand compartments currently are in the range of 10-3-10-2 m2 kg-1 dw. However, the mean Tag and their dynamic trend significantly differed in the wood compartments of the cedar stands, which may indicate root uptake differences of orders of magnitude between observation sites. The difference in radiocesium concentration in wood between the sites becomes less pronounced when normalized by the ratio of exchangeable 137Cs/K in the soils.

Comparison of thyroid doses to the public from radioiodine following the Chernobyl and Fukushima accidents.

Estimates of thyroid doses to the public from radioiodine intake following the accidents at Chernobyl and Fukushima Daiichi nuclear power plants are compared. The basis for thyroid dose estimates after the Chernobyl accident was a large set of measurements of 131I thyroidal content for approximately 400,000 residents in Belarus, Ukraine, and Russia. Due to a lack of direct thyroid measurements after the Fukushima accident (just over 1000 residents were measured), thyroid doses were estimated based on ecological models and are therefore associated with much higher uncertainty than those based on direct thyroid measurements. Thyroid dose estimates for evacuees were up to 50,000 mGy for Chernobyl and up to approximately 100 mGy for Fukushima. This large difference in thyroid dose to the public is mainly due to the different dominant pathways of radioiodine intake: ingestion of fresh, locally produced cows' milk (Chernobyl) and inhalation of contaminated air (Fukushima).

Development of an application tool to support returnees in Fukushima.

To promote radiation protection and health promotion among returning residents (returnees) in coastal areas of Fukushima, eHealth principles were used to develop a new application tool (app) that can record radiation exposure and health status while providing comprehensive support to returnees. Intended users are returnees and health and welfare workers. After assessing their needs, a flowchart and prototype for operational logic were created using commercially available software tools. Professional developers will focus on improving the user interface and ensuring data security. The finished app will be compatible with mobile telephones and tablets. Utility and ease of use are paramount to serve returnees of all ages effectively.

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.