Pre- and post-accident environmental transfer of radionuclides in Japan: lessons learned in the IAEA MODARIA II programme.

An international review of radioecological data derived after the accident at the Fukushima Daiichi nuclear power plant was an important component of activities in working group 4 of the IAEA Models and data for radiological impact assessment, phase II (MODARIA II) programme. Japanese and international scientists reviewed radioecological data in the terrestrial and aquatic environments in Japan reported both before and after the accident. The environmental transfer processes considered included: (a) interception and retention radionuclides by plants, (b) loss of radionuclides from plant and systemic transport of radionuclides in plants (translocation), (c) behaviour of radiocaesium in soil, (d) uptake of radionuclides from soil by agricultural crops and wild plants, (e) transfer of radionuclides from feedstuffs to domestic and wild animals, (f) behaviour of radiocaesium in forest trees and forest systems, (g) behaviour of radiocaesium in freshwater systems, coastal areas and in the ocean, (h) transport of radiocaesium from catchments through rivers, streams and lakes to the ocean, (i) uptake of radiocaesium by aquatic organisms, and (j) modification of radionuclide concentrations in food products during food processing and culinary preparation. These data were compared with relevant global data within IAEA TECDOC-1927 'Environmental transfer of radionuclides in Japan following the accident at the Fukushima Daiichi Nuclear Power Plant'. This paper summarises the outcomes of the data collation and analysis within MODARIA II work group 4 and compares the Japan-specific data with existing radioecological knowledge acquired from past and contemporary radioecological studies. The key radioecological lessons learned are outlined and discussed.

Collation of Strontium Concentration Ratios from Water to Aquatic Biota Species in Freshwater and Marine Environments and Factors Affecting the Ratios.

The fate of strontium-90 (90Sr) from water to aquatic biota is of concern since the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident because of continuous small 90Sr releases to the seawater from the FDNPP site. The Japanese diet includes many edible marine and freshwater species, and the environmental parameter, that is, the concentration ratio (CR) from water to biota, is useful to estimate the potential 90Sr intake, especially from frequently consumed seafoods. However, widely used CR data for radiation dose assessment only have provided values for biota types such as fish, crustaceans, macroalgae, and so forth, and thus, it is difficult to identify specific data for each species. In this study, therefore, we collated CR data of Sr for aquatic biota by surveying available open data sources from the 1950s to 2019, not only for edible parts but also for whole and inedible parts. In total, we obtained 3800 CR data: 3013 data for marine biota, 28 data for brackish water biota, and 759 data for freshwater biota. The results showed that species-specific CRs may decrease the uncertainties compared to those published in IAEA documents; however, different diets and living areas by species may lead to different uncertainties for different species.

Changes in the Soil to Brown Rice Concentration Ratio of Radiocaesium before and after the Fukushima Daiichi Nuclear Power Plant Accident in 2011.

Radiocaesium (RCs) mobility in soil is initially relatively high when the nuclide first comes into contact with soil, after which the mobile fraction decreases with time due to RCs fixation to soil particles (aging effect). Consequently, the RCs activity concentration in plants grown in soil was expected to decrease with time after the Fukushima Daiichi nuclear power plant accident in 2011. In this study, we collated data on concentration ratios (CR) of RCs between brown rice grain and paddy soil and compared CR values reported for periods before and after the accident. For this purpose, soil and rice data were collected after the accident specifically from paddy fields that did not have additional potassium fertilizer added (for remediation purposes). The geometric mean rice/soil CR of RCs for all types of soil was 1.2 × 10-2 in 2011 ( n = 62) and by 2013 the value had declined to 3.5 × 10-3 ( n = 32), which was similar to that for 1995-2007 of 3.4 × 10-3 ( n = 120). The comparison suggests that the mean soil-to-rice grain concentration ratio had returned to that prevailing before the accident after less than three years. It was also confirmed that CR values for rice sampled from paddy fields were lower than those obtained from pot experiments.

High-Performance Method for Determination of Pu Isotopes in Soil and Sediment Samples by Sector Field-Inductively Coupled Plasma Mass Spectrometry.

Plutonium is extensively studied in radioecology (e.g., soil to plant transfer and radiological assessment) and geochemistry (e.g., sediment dating). Here, we reported a new chemical separation method for rapid determination of Pu in soil and sediment samples, based on the following investigations: extraction behaviors of interfering elements (IEs, for inductively coupled plasma mass spectrometry (ICPMS) measurement) on TEVA resin; decontamination of U using TEVA, UTEVA, and DGA resins; and the impact of coprecipitation on Pu determination. The developed method consists of four steps: HNO3 leaching for Pu release; CaF2/LaF3 coprecipitation for the removal of major metals and U; the proposed TEVA + UTEVA + DGA procedure for the removal of U, Pb, Bi, Tl, Hg, Hf, Pt, and Dy; and ICPMS measurement. The accuracy of this method in determining 239+240Pu activity and 240Pu/239Pu and 241Pu/239Pu isotopic ratios was validated by analyzing five standard reference materials (soil, fresh water sediment, and ocean sediment). This method is characterized by its stable and high Pu recovery (90-97% for soil; 92-98% for sediment) and high decontamination factor of U (1.6 × 107), which is the highest reported for soil and sediment samples. In addition, the short analytical time of 12 h and the method detection limits, which are the lowest yet reported in literature, of 0.56 µBq g-1 (0.24 fg g-1) for 239Pu, 1.2 µBq g-1 (0.14 fg g-1) for 240Pu, and 0.34 mBq g-1 (0.09 fg g-1) for 241Pu (calculated on the basis of a 1 g soil sample) allow the rapid determination of ultratrace level Pu in soil and sediment samples.

Effects of indoor and outdoor cultivation conditions on 137 Cs concentrations in cultivated mushrooms produced after the Fukushima Daiichi Nuclear Power Plant accident.

BACKGROUND: Radiocesium (134 Cs and 137 Cs) in mushrooms has been a matter of public concern after the accident at Fukushima Daiichi Nuclear Power Plant. To minimize the internal dose by ingestion of cultivated mushrooms, the Japanese government set a guideline level with respect to the radiocesium concentration in bed-logs and mushroom beds; however, the effects of indoor and outdoor cultivation methods on radiocesium concentrations in cultivated mushrooms were not clear. RESULTS: The effects of indoor and outdoor cultivation on the radiocesium concentrations in mushroom were examined using published food monitoring data. 137 Cs concentration data in Lentinula edodes from the Aizu area in Fukushima Prefecture and seven prefectures outside Fukushima were used for the analysis. No statistically significant 137 Cs concentration differences were found between these two cultivation methods. Using detected 137 Cs data in shiitake, the geometric means from each prefecture were less than one-quarter of the standard limit (100 Bq kg-1 ) for total radiocesium under both cultivation conditions. CONCLUSION: It was suspected that re-suspended radiocesium might have been taken up by mushrooms or that radiocesium might have been absorbed into the mushrooms from the soil in the outdoor cultures. However, neither effect was significant for cultivated mushrooms in the areas examined. © 2016 Society of Chemical Industry.

Method for Ultratrace Level (241)Am Determination in Large Soil Samples by Sector Field-Inductively Coupled Plasma Mass Spectrometry: With Emphasis on the Removal of Spectral Interferences and Matrix Effect.

A new method using sector field-inductively coupled plasma mass spectrometry (SF-ICPMS) was developed for the determination of (241)Am in large soil samples to provide realistic soil-plant transfer parameter data for dose assessment of nuclear waste disposal plans. We investigated four subjects: extraction behaviors of interfering elements (Bi, Tl, Hg, Pb, Hf, and Pt) on DGA resin (normal type, abbreviated as DGA-N); soil matrix element removal (Mg, Fe, Al, K, Na) using Fe(OH)3, CaF2, and CaC2O4 coprecipitations; Am and rare earth elements (REEs) separation on DGA-N and TEVA resins; and optimization of SF-ICPMS (equipped with a high efficiency nebulizer (HEN)) for Am determination. Our method utilized concentrated HNO3 to leach Am from 2 to 20 g soil samples. The CaC2O4 coprecipitation was used to remove major metals in soil and followed by Am/interfering elements separation using the proposed UTEVA + DGA-N procedure. After a further separation of REEs on TEVA resin, (241)Am was determined by HEN-SF-ICPMS. This method eliminated the matrix effect in ICPMS (241)Am measurement for large soil samples. The high decontamination factors (DFs) of interfering elements enable their thorough removal, and in particular, the DF of Pu (7 × 10(5)) was the highest ever reported in (241)Am studies; thus, this method is capable of analyzing (241)Pu-contaminated Fukushima Daiichi Nuclear Power Plant (FDNPP) sourced soil samples. A low detection limit of 0.012 mBq g(-1) for (241)Am was achieved. The chemical recovery of Am (76-82%) was stable for soil samples. This method can be employed for the low level (241)Am determination in large size soil samples that are contaminated with (241)Pu.

Triple-Quadrupole Inductively Coupled Plasma-Mass Spectrometry with a High-Efficiency Sample Introduction System for Ultratrace Determination of (135)Cs and (137)Cs in Environmental Samples at Femtogram Levels.

High yield fission products, (135)Cs and (137)Cs, have entered the environment as a result of anthropogenic nuclear activities. Analytical methods for ultratrace measurement of (135)Cs and (137)Cs are required for environmental geochemical and nuclear forensics studies. Here we report a highly sensitive method combining a desolvation sample introduction system (APEX-Q) with triple-quadrupole inductively coupled plasma mass spectrometry (AEPX-ICPMS/MS) for the determination of (135)Cs and (135)Cs/(137)Cs isotope ratio at femtogram levels. Using this system, we introduced only selected ions into the collision/reaction cell to react with N2O, significantly reducing the isobaric interferences ((135)Ba(+) and (137)Ba(+)) and polyatomic interferences ((95,97)Mo(40)Ar(+), (119)Sn(16)O(+), and (121)Sb(16)O(+)). Compared to the instrument setup of ICPMS/MS, the APEX-ICPMS/MS enables a 10-fold sensitivity increase. In addition, an effective chemical separation scheme consisting of ammonium molybdophosphate (AMP) Cs-selective adsorption and two-stage ion-exchange chromatographic separation was developed to remove major matrix and interfering elements from environmental samples (10-40 g). This separation method showed high decontamination factors (10(4)-10(7)) for major matrix elements (Al, Ca, K, Mg, Na, and Si) and interfering elements (Ba, Mo, Sb, and Sn). The high sensitivity of APEX-ICPMS/MS and the effective removal sample matrix allowed reliable analysis of (135)Cs and (137)Cs with extremely low detection limits (0.002 pg mL(-1), corresponding to 0.006 Bq mL(-1) (137)Cs). The accuracy and applicability of the APEX-ICPMS/MS method was validated by analysis of seven standard reference materials (soils, sediment, and plants). For the first time, ultratrace determination of (135)Cs and (135)Cs/(137)Cs isotope ratio at global fallout source environmental samples was achieved with the ICPMS technique.

Consideration on the Long Ecological Half-Life Component of (137)Cs in Demersal Fish Based on Field Observation Results Obtained after the Fukushima Accident.

Radiocesium concentrations in most marine fish collected off the coast of Fukushima and surrounding prefectures have decreased with time, and four years after the Fukushima Daiichi Nuclear Power Plant accident occurred, radiocesium concentrations have generally fallen below the detectable level (ca. < 10 Bq kg(-1)-raw). Only in some demersal fish species have detectable concentration levels still been found, and even these species have showed slow radiocesium decreases. The food web was considered as the major factor causing this phenomenon; however, slow elimination rates of radiocesium from these fish species also could be the cause. The latter effect was examined by considering that the (137)Cs concentration decreasing trend in fish could be fit with a set of three exponentially decreasing components; that is, having short, intermediate, and long biological half-lives. The long ecological half-life component was calculated using a 400-1500 d period of monitoring results for Japanese rockfish (Sebastes cheni) and compared with previous reported laboratory results for biological half-life. The obtained ecological half-lives ranged from 274-365 d, and these values agreed with the biological half-life of this fish species. This result implied that the long biological half-lives of radiocesium in some demersal fish species made their radiocesium contamination periods longer.

The Time-Dependent Transfer Factor of Radiocesium from Soil to Game Animals in Japan after the Fukushima Dai-ichi Nuclear Accident.

Since the Fukushima Dai-ichi accident, monitoring of tissues from hunted game animals ensures compliance with the standard food limits for radionuclides in Japan. We quantified the transfer of (137)Cs from contaminated land to game animals using the Aggregated transfer factor (Tag = activity concentration in meat [Bq kg(-1) fw]/amount in soil [Bq m(-2)]) of (137)Cs for Asian black bear, wild boar, sika deer, green pheasant, copper pheasant and wild duck, collected between 2011 and 2015. Open data sources were used from Fukushima, Miyagi, Ibaraki, Tochigi, and Gunma prefectures. Our initially compiled data showed that the maximum reported (137)Cs activity concentration in wild boar after the Fukushima Dai-ichi accident were lower than those reported after the Chernobyl accident. The geometric mean Tag values (m(2)kg(-1) fw) of (137)Cs in 2015 for Asian black bear, wild boar, sika deer and copper pheasant were similar (1.9-5.1) × 10(-3) while those for green pheasant and wild duck were about 1 order of magnitude lower at (1.0-2.2) × 10(-4). Effective half-lives were 1.2-6.9 y except for sika deer and copper pheasant where no decreases were found. In contrast to the Chernobyl accident, no seasonal change occurred in the meat (137)Cs activity concentrations of the wild animals during the study period.

Effect of ashing temperature on accurate determination of plutonium in soil samples.

An acidic leaching method using HNO3 is widely employed to release the global fallout Pu from soil samples for further chemical separations in radioecology and toxicology studies and in many applications using Pu as a useful tracer. In the method's sample ash treatment step to decompose organic matter in soil, various ashing temperatures (400-900 °C) are used; however, the effect of ashing temperature on the accurate Pu analysis has not been well investigated. In this study, two standard reference soils (IAEA-soil-6 and IAEA-375) were used to determine the ashing temperature effect (from 375 to 600 °C) on the HNO3 leaching method. The Pu analytical results of both standard reference materials showed that lower (239+240)Pu activity was observed when the ashing temperature exceeded 450 °C, and the (239+240)Pu activity continued to decrease as the ashing temperature was raised. Approximately 40% of the Pu content could not be leached out by concentrated HNO3 after ashing for 4 h at 600 °C. The Pu loss was attributed to the formation of refractory materials, which are insoluble in HNO3 solution. This hypothesis was confirmed by the XRD analysis of soil samples, which revealed that plagioclase-like silicate materials were formed after high-temperature ashing. To ensure Pu release efficiency in HNO3 leaching, we recommend 450 °C as the ideal ashing temperature. This recommendation is also useful for analysis of other important artificial radionuclides (e.g., (137)Cs, (90)Sr, (241)Am) for which an ashing process is needed to decompose the organic content in soil samples.

Radiological dose rates to marine fish from the Fukushima Daiichi accident: the first three years across the North Pacific.

A more complete record is emerging of radionuclide measurements in fish tissue, sediment, and seawater samples from near the Fukushima Daiichi Nuclear Power Plant (FDNPP) and across the Pacific Ocean. Our analysis of publicly available data indicates the dose rates to the most impacted fish species near the FDNPP (median 1.1 mGy d(-1), 2012-2014 data) have remained above benchmark levels for potential dose effects at least three years longer than was indicated by previous, data-limited evaluations. Dose rates from (134,137)Cs were highest in demersal species with sediment-associated food chains and feeding behaviors. In addition to (134,137)Cs, the radionuclide (90)Sr was estimated to contribute up to approximately one-half of the total 2013 dose rate to fish near the FDNPP. Mesopelagic fish 100-200 km east of the FDNPP, coastal fish in the Aleutian Islands (3300 km), and trans-Pacific migratory species all had increased dose rates as a consequence of the FDNPP accident, but their total dose rates remained dominated by background radionuclides. A hypothetical human consumer of 50 kg of fish, gathered 3 km from the FDNPP in 2013, would have received a total committed effective dose of approximately 0.95 mSv a(-1) from combined FDNPP and ambient radionuclides, of which 0.13 mSv a(-1) (14%) was solely from the FDNPP radionuclides and below the 1 mSv a(-1) benchmark for public exposure.

Determination of ¹³5Cs and ¹³5Cs/¹³7Cs atomic ratio in environmental samples by combining ammonium molybdophosphate (AMP)-selective Cs adsorption and ion-exchange chromatographic separation to triple-quadrupole inductively coupled plasma-mass spectrometry.

Since the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident in 2011, the activity ratio of (134)Cs/(137)Cs has been widely used as a tracer for contamination source identification. However, because of the short half-life of (134)Cs (2.06 y), this tracer will become unavailable in the near future. This article presents an analytical method for the determination of the long-lived (135)Cs (t(2/1) = 2 × 10(6) y) and the atomic ratio of (135)Cs/(137)Cs, as a promising geochemical tracer, in environmental samples. The analytical method involves ammonium molybdophosphate (AMP)-selective adsorption of Cs and subsequent two-stage ion-exchange chromatographic separation, followed by detection of isolated radiocesium isotopes via triple-quadrupole inductively coupled plasma-mass spectrometry (ICP-MS/MS). The AMP-selective adsorption of Cs and the chromatographic separation system showed high decontamination factors (10(4)-10(5)) for interfering elements, such as Ba, Mo, Sb, and Sn. Using ICP-MS/MS, only selected ions enter the collision/reaction cell to react with N2O, reducing the isobaric interferences ((135)Ba(+) and (137)Ba(+)) and polyatomic interferences ((95) Mo(40)Ar(+), (97) Mo(40)Ar(+), (119)Sn(16)O(+), and (121)Sb(16)O(+)) produced by sample matrix ions. The high abundance sensitivity (10(-9) for the (135)Cs/(133)Cs ratio) provided by ICP-MS/MS allowed reliable analysis of (135)Cs and (137)Cs isotopes with the lowest detection limits ever reported by mass counting methods (0.01 pg mL(-1) and 0.006 pg mL(-1), respectively). The developed analytical method was successfully applied to the determination of (135)Cs and (137)Cs isotopes in environmental samples (soil, litter, and lichen) collected after the FDNPP accident for contamination source identification.

Isotopic composition and distribution of plutonium in northern South China Sea sediments revealed continuous release and transport of Pu from the Marshall Islands.

The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios in sediments of the northern South China Sea and its adjacent Pearl River Estuary were determined to examine the spatial and temporal variations of Pu inputs. We clarified that Pu in the study area is sourced from a combination of global fallout and close-in fallout from the Pacific Proving Grounds in the Marshall Islands where above-ground nuclear weapons testing was carried out during the period of 1952-1958. The latter source dominated the Pu input in the 1950s, as evidenced by elevated (240)Pu/(239)Pu atom ratios (>0.30) in a dated sediment core. Even after the 1950s, the Pacific Proving Grounds was still a dominant Pu source due to continuous transport of remobilized Pu from the Marshall Islands, about 4500 km away, along the North Equatorial Current followed by the transport of the Kuroshio current and its extension into the South China Sea through the Luzon Strait. Using a simple two end-member mixing model, we have quantified the contributions of Pu from the Pacific Proving Grounds to the northern South China Sea shelf and the Pearl River Estuary are 68% ± 1% and 30% ± 5%, respectively. This study also confirmed that there were no clear signals of Pu from the Fukushima Daiichi Nuclear Power Plant accident impacting the South China Sea.

A method of measurement of (239)Pu, (240)Pu, (241)Pu in high U content marine sediments by sector field ICP-MS and its application to Fukushima sediment samples.

An accurate and precise analytical method is highly needed for the determination of Pu isotopes in marine sediments for the long-term marine environment monitoring that is being done since the Fukushima Dai-ichi Nuclear Power Plant accident. The elimination of uranium from the sediment samples needs to be carefully checked. We established an analytical method based on anion-exchange chromatography and SF-ICP-MS in this work. A uranium decontamination factor of 2 × 10(6) was achieved, and the U concentrations in the final sample solutions were typically below 4 pg mL(-1), thus no extra correction of (238)U interferences from the Pu spectra was needed. The method was suitable for the analysis of (241)Pu in marine sediments using large sample amounts (>10 g). We validated the method by measuring marine sediment reference materials and our results agreed well with the certified and the literature values. Surface sediments and one sediment core sample collected after the nuclear accident were analyzed. The characterization of (241)Pu/(239)Pu atom ratios in the surface sediments and the vertical distribution of Pu isotopes showed that there was no detectable Pu contamination from the nuclear accident in the marine sediments collected 30 km off the plant site.

(135)Cs/(137)Cs isotopic ratio as a new tracer of radiocesium released from the Fukushima nuclear accident.

Since the Fukushima Daiichi nuclear power plant (FDNPP) accident in 2011, intensive studies of the distribution of released fission products, in particular (134)Cs and (137)Cs, in the environment have been conducted. However, the release sources, that is, the damaged reactors or the spent fuel pools, have not been identified, which resulted in great variation in the estimated amounts of (137)Cs released. Here, we investigated heavily contaminated environmental samples (litter, lichen, and soil) collected from Fukushima forests for the long-lived (135)Cs (half-life of 2 × 10(6) years), which is usually difficult to measure using decay-counting techniques. Using a newly developed triple-quadrupole inductively coupled plasma tandem mass spectrometry method, we analyzed the (135)Cs/(137)Cs isotopic ratio of the FDNPP-released radiocesium in environmental samples. We demonstrated that radiocesium was mainly released from the Unit 2 reactor. Considering the fact that the widely used tracer for the released Fukushima accident-sourced radiocesium in the environment, the (134)Cs/(137)Cs activity ratio, will become unavailable in the near future because of the short half-life of (134)Cs (2.06 years), the (135)Cs/(137)Cs isotopic ratio can be considered as a new tracer for source identification and long-term estimation of the mobility of released radiocesium in the environment.

Release of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant accident to the marine environment was negligible.

Atmospheric deposition of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has been observed in the terrestrial environment around the FDNPP site; however, their deposition in the marine environment has not been studied. The possible contamination of Pu in the marine environment has attracted great scientific and public concern. To fully understand this possible contamination of Pu isotopes from the FDNPP accident to the marine environment, we collected marine sediment core samples within the 30 km zone around the FDNPP site in the western North Pacific about two years after the accident. Pu isotopes ((239)Pu, (240)Pu, and (241)Pu) and radiocesium isotopes ((134)Cs and (137)Cs) in the samples were determined. The high activities of radiocesium and the (134)Cs/(137)Cs activity ratios with values around 1 (decay corrected to 15 March 2011) suggested that these samples were contaminated by the FDNPP accident-released radionuclides. However, the activities of (239+240)Pu and (241)Pu were low compared with the background level before the FDNPP accident. The Pu atom ratios ((240)Pu/(239)Pu and (241)Pu/(239)Pu) suggested that global fallout and the pacific proving ground (PPG) close-in fallout are the main sources for Pu contamination in the marine sediments. As Pu isotopes are particle-reactive and they can be easily incorporated with the marine sediments, we concluded that the release of Pu isotopes from the FDNPP accident to the marine environment was negligible.

Ecological half-lives of radiocesium in 16 species in marine biota after the TEPCO's Fukushima Daiichi nuclear power plant accident.

TEPCO's Fukushima Daiichi Nuclear Power Plant (FDNPP) accident of March 2011 caused the discharge of a considerable quantity of radionuclides, including (137)Cs. Because of its long half-life (30.17 years), the fate of (137)Cs in the marine biota is of great interest. This study aims to evaluate, using food monitoring data, ecological half-lives (Teco) of (137)Cs in marine biota caught offshore of Fukushima. The data were categorized into two regional groups (north and south) with respect to the FDNPP site, and the regional (137)Cs concentration trend and estimated Teco in the marine biota were appraised. Although the (137)Cs concentration in the seawater in the south was higher than that in the north, Teco values remained relatively consistent among common species of both regions. Teco was then compared to biological half-life (Tb) estimated in laboratory settings. The ratios of Teco/Tb were inconsistent among different groups of marine species. The ratios of Teco/Tb for brown seaweed and bivalves were approximately 1, and the ratios of Teco/Tb for demersal fish ranged from 4.4 to 16.1. The reasons for different ratios of Teco and Tb values may be attributed to environmental and ecological factors, such as different trophic levels.

Release of plutonium isotopes into the environment from the Fukushima Daiichi Nuclear Power Plant accident: what is known and what needs to be known.

The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has caused serious contamination in the environment. The release of Pu isotopes renewed considerable public concern because they present a large risk for internal radiation exposure. In this Critical Review, we summarize and analyze published studies related to the release of Pu from the FDNPP accident based on environmental sample analyses and the ORIGEN model simulations. Our analysis emphasizes the environmental distribution of released Pu isotopes, information on Pu isotopic composition for source identification of Pu releases in the FDNPP-damaged reactors or spent fuel pools, and estimation of the amounts of Pu isotopes released from the FDNPP accident. Our analysis indicates that a trace amount of Pu isotopes (∼2 × 10(-5)% of core inventory) was released into the environment from the damaged reactors but not from the spent fuel pools located in the reactor buildings. Regarding the possible Pu contamination in the marine environment, limited studies suggest that no extra Pu input from the FDNPP accident could be detected in the western North Pacific 30 km off the Fukushima coast. Finally, we identified knowledge gaps remained on the release of Pu into the environment and recommended issues for future studies.

Estimation of Te-132 distribution in Fukushima Prefecture at the early stage of the Fukushima Daiichi Nuclear Power Plant reactor failures.

Tellurium-132 ((132)Te, half-life: 3.2 d) has been assessed as the radionuclide with the third largest release from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March 2011; thus it would have made some dose contribution during the early stage of the reactor failures. The available data for (132)Te are, however, limited. In this study, available reported values of other isotopes of Te were compiled to estimate (132)Te concentration (in MBq m(-2)). It was found that (132)Te and (129m)Te (half-life: 33.6 d) concentrations were well correlated (R = 0.99, p < 0.001) by t test. Thus, (132)Te concentrations on March 11, 2011 were estimated from (129m)Te using the concentration conversion factor ((132)Te /(129m)Te) of 14.5. It was also found that since deposited (129m)Te was well retained in the soil, the data collected in March-May of 2011 were applicable to (132)Te estimation. It was possible to obtain the first (132)Te concentration contour map for the eastern part of Fukushima Prefecture, including data from within the 20-km exclusion zone around the FDNPP, using these newly available estimated (132)Te data sets.

Distribution coefficients (K(d)) of stable iodine in estuarine and coastal regions, Japan, and their relationship to salinity and organic carbon in sediments.

The sediment-water distribution coefficient, (K(d)), is one of the most important parameters in radionuclide assessment models. In this study, we determined K ds of stable iodine (I) in estuarine and coastal regions. We studied 16 estuarine and coastal regions of Japan and obtained I data on water and sediments. Data on salinity, pH, dissolved organic carbon and dissolved oxygen in water, and organic carbon (OC) in sediments were also obtained as estuarine variables. Determined (K(d))S of I in the Sagami River estuary decreased along the salinity gradient (salinity range, 0.1-33.8), indicating that salinity is one of the important factors controlling the (K(d)) values; however, when the (K(d)) values were compared among all the estuaries, the difference between minimum and maximum (K(d)) values varied by about two orders of magnitude in a narrow salinity range of 30.0-34.4. A significant correlation between (K(d)) value and OC content in sediments was observed in all the stations with a salinity of ≥ 30 except for stations in the Ishikari and Onga River estuaries. The exceptions are probably due to different sources of the sediments, which are explained by the results of relatively low I/OC ratios in sediments in those two estuaries, compared to the other estuaries. Thus, OC in sediments as well as salinity may be responsible for the variation of (K(d))S of I in the estuarine and coastal regions.