Fukushima-derived Radionuclides Research Articles

Deciphering decadal observation of Fukushima-derived radiocesium in the most polluted port near the Fukushima Daiichi Nuclear Power Plant: from seawater to marine fish

The biological concentration effect of radionuclides in marine fish has exacerbated public anxiety about seafood security in the context of Fukushima nuclear-contaminated water discharged into the ocean. However, the most polluted port near the Fukushima Daiichi Nuclear Power Plant (FDNPP) has seldom been investigated, especially for radioactivity in marine fish. In this study, decadal observations of radiocesium in marine fish and seawater from the most polluted port were simultaneously established after the Fukushima Nuclear Accident. We found a generally decreasing trend of historical 137Cs activity in seawater, with seasonal variations modulated by precipitation. Seasonal variations were elucidated with finer detail and divided into exponential decline in the dry season and steady variation in the wet season. A novel method was proposed to estimate the continuing source term of 137Cs derived from the FDNPP, which was 3.9 PBq in 2011 and 19.3 TBq between 2012 and 2022 on the basis of historical 137Cs. The biological concentration effect of marine fish is quantitatively emphasized according to the higher ratio of over-standards for radiocesium in marine fish relative to that in seawater. Long-term observation and analysis of radiocesium in marine fish and seawater from the most polluted port would provide insights into the scientific evaluation of the effectiveness of the decommissioning of the FDNPP in the past and share lessons on the fate of Fukushima-derived radionuclides in the future.

Proteomic Biomarker Analysis of Serum from Japanese Field Mice (Apodemus Speciosus) Collected within the Fukushima Difficult-to-return Zone.

The environmental impact of the Fukushima Daiichi nuclear power plant accident is a source of ongoing concern as there is uncertainty regarding the effects of chronic radiation exposure on local plant and animal life from Fukushima-derived radionuclides. In the current study, changes in proteomic biomarker expression due to chronic environmentally-derived radiation exposures was examined in wild field mice. Serum from 10 wild field mice (Apodemus speciosus) native to the Fukushima difficult-to-return zone and from eight wild field mice native to the Soma area (control) were collected. External dose estimations were completed using measurements of ambient radiation levels and calculating 137Cs concentrations in soil. Internal dose was estimated by counting whole mice using an HPGe detector. Age of the mice was estimated using molar wear. Serum was screened using the aptamer-based SOMAscan proteomic assay technology for changes in expression of 1,310 protein analytes. A subset panel of protein biomarkers that demonstrated significant changes in expression between control and exposed mice was determined and analyzed using Ingenuity Pathway Analysis (IPA). Control animals had a calculated lifetime dose range from 0.001 to 0.007 Gy, and exposed animals had a calculated lifetime dose range from 0.01 to 0.64 Gy. No discernable effect of dose rate was seen as relative dose rate correlated with dose for all samples. Detectable values were obtained for all 1,310 proteins included in the SOMAscan assay. Subset panels of proteins demonstrating significant (p < 0.05) changes in expression with either an upregulated or downregulated 1.5-fold change over control were identified for both the sample cohort inclusive of all exposed samples and the sample cohort restricted to samples from animals receiving "low" dose exposures. These panels of proteins from exposed animals were analyzed using IPA, which highlighted changes in key biological pathways related to injury, respiratory, renal, urological, and gastrointestinal disease, and cancer. Significant changes in expression of proteomic biomarkers were seen in the serum of wild field mice that received environmental exposure to Fukushima-derived radionuclides. Our findings demonstrate novel biomarkers of radiation exposure in wildlife within the Fukushima difficult-to-return zone.

Radiological impact assessment in the terrestrial environment of Greece using innovative tools – Adaptation of ERICA Tool to actual measurements

In the present study, the radioactivity levels in terrestrial non-human biota and the transfer pathways in the ecosystem are examined. Grass of Poaceae family and herbivore mammals (ruminants) of Bovidae family and soil samples were collected during the period of 2010 to 2014, from grasslands of the Greek rural territory where sheep and goats were free-range grazing. Natural background radionuclides (226Ra, 228Ra, 228Th) and artificial radionuclides (137Cs, 134Cs, 131I) were detected in the collected samples using gamma spectrometry. The actual measured activity concentrations and site- specific data of the studied organisms were imported in ERICA Assessment Tool (Version 1.2.1, February 2016) in order to provide an insight of the radiological dose rates. Natural radionuclides exhibited significantly higher contribution to the total dose rate than the artificial ones. The radiological exposure to Fukushima-derived radionuclides was quite low and owed to internal exposure, mainly derived through the ingestion pathway. According to the screening levels, the calculated dose rate to the studied non-human biota was below the threshold levels. However, the obtained results may be proved useful in further research regarding the possible impact of protracted low level ionising radiation to non-human biota on the various levels of life’s organization.

Pu isotopes in the seawater off Fukushima Daiichi Nuclear Power Plant site within two months after the severe nuclear accident

The marine environment is complex, and it is desirable to have measurements for seawater samples collected at the early stage after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident to determine the impact of Fukushima-derived radionuclides on this environment. Here Pu isotopes in seawater collected 33–163 km from the FDNPP site at the very early stage after the accident were determined (May 2011, within two months after the accident). The distribution and temporal variation of 239Pu and 240Pu were studied. The results indicated that both 239+240Pu activity concentrations (from 0.81 ± 0.16 to 11.18 ± 1.28 mBq/m3) and 240Pu/239Pu atom ratios (from 0.216 ± 0.032 to 0.308 ± 0.036) in these seawater samples were within the corresponding background ranges before the accident, and this suggested that Fukushima-derived Pu isotopes, if any, were in too limited amount to be distinguished from the background level in the seawater. The analysis of Pu isotopic composition indicated that the major sources of Pu in the seawater after the accident were still global fallout and the Pacific Proving Ground close-in fallout. The contribution analysis showed that the contributions of the Pacific Proving Ground close-in fallout in the water column of the study area ranged from 26% to 77% with the average being 48%.

Rapid ultra-trace determination of Fukushima-derived radionuclides in food

A selection of 35 food samples from Japan (plus one seawater sample and one mushroom sample from Russia) were analyzed by gamma spectrometry and liquid scintillation counting. The analytical protocol included concentration of the sample by lyophilization and/or thermal treatment, resulting in exceptionally low limits of detections (in the low mBq/kg range or even below) for the radionuclides 134Cs, 137Cs, 108mAg, and 110mAg, as well as low limits of detection for 90Sr (in the low Bq/kg range). Radiosilver was found in several mussels at low concentrations. Most samples exhibited detectable radiocesium concentrations (below the regulatory limit). An analytical protocol for 90Sr in food was developed and optimized, allowing detection limits in the sub-Bq/kg range. However, despite this high sensitivity, no Japanese food sample exceeded the limit of detection. Only one mushroom sample from Russia revealed detectable traces of 90Sr, but the lack of 134Cs in this sample proves that these radioactive traces did not originate from the Fukushima Daiichi accident. Several moderately time-consuming steps in the analysis of 90Sr increase the sensitivity so far that this radionuclide can be measured directly with high sensitivity, without having to wait for about 2 weeks for the ingrowth of its daughter nuclide 90Y. Our study supports previous studies, which also attested Japanese foods a high level of radiological safety.

Assessing Fukushima-Derived Radiocesium in Migratory Pacific Predators.

The 2011 release of Fukushima-derived radionuclides into the Pacific Ocean made migratory sharks, teleosts, and marine mammals a source of speculation and anxiety regarding radiocesium (134+137Cs) contamination, despite a lack of actual radiocesium measurements for these taxa. We measured radiocesium in a diverse suite of large predators from the North Pacific Ocean and report no detectable (i.e., ≥ 0.1 Bq kg-1 dry wt) Fukushima-derived 134Cs in all samples, except in one olive ridley sea turtle (Lepidochelys olivacea) with trace levels (0.1 Bq kg-1). Levels of 137Cs varied within and across taxa, but were generally consistent with pre-Fukushima levels and were lower than naturally occurring 40K by one to one to two orders of magnitude. Predator size had a weaker effect on 137Cs and 40K levels than tissue lipid content. Predator stable isotope values (δ13C and δ15N) were used to infer recent migration patterns, and showed that predators in the central, eastern, and western Pacific should not be assumed to accumulate detectable levels of radiocesium a priori. Nondetection of 134Cs and low levels of 137Cs in diverse marine megafauna far from Fukushima confirms negligible increases in radiocesium, with levels comparable to those prior to the release from Fukushima. Reported levels can inform recently developed models of cesium transport and bioaccumulation in marine species.

Lagrangian simulation and tracking of the mesoscale eddies contaminated by Fukushima-derived radionuclides

Abstract. A Lagrangian methodology is developed to simulate, track, document and analyze the origin and history of water masses in ocean mesoscale features. It aims to distinguish whether water masses inside the mesoscale eddies originated from the main currents in the Kuroshio–Oyashio confluence zone. By computing trajectories for a large number of synthetic Lagrangian particles advected by the AVISO velocity field after the Fukushima accident, we identify and track the mesoscale eddies which were sampled in the cruises in 2011 and 2012 and estimate their risk of being contaminated by Fukushima-derived radionuclides. The simulated results are compared with in situ measurements, showing a good qualitative correspondence.

Radiocarbon Releases from the 2011 Fukushima Nuclear Accident.

Radiocarbon activities were measured in annual tree rings for the years 2009 to 2015 from Japanese cedar trees (Cryptomeria japonica) collected at six sites ranging from 2.5–38 km northwest and north of the Fukushima Dai-ichi nuclear power plant. The 14C specific activity varied from 280.4 Bq kg−1 C in 2010 to 226.0 Bq kg−1 C in 2015. The elevated 14C activities in the 2009 and 2010 rings confirmed 14C discharges during routine reactor operations, whereas those activities that were indistinguishable from background in 2012–2015 coincided with the permanent shutdown of the reactors after the accident in 2011. High-resolution 14C analysis of the 2011 ring indicated 14C releases during the Fukushima accident. The resulted 14C activity decreased with increasing distance from the plant. The maximum 14C activity released during the period of the accident was measured 42.4 Bq kg−1 C above the natural ambient 14C background. Our findings indicate that, unlike other Fukushima-derived radionuclides, the 14C released during the accident is indistinguishable from ambient background beyond the local environment (~30 km from the plant). Furthermore, the resulting dose to the local population from the excess 14C activities is negligible compared to the dose from natural/nuclear weapons sources.

Predictability of the dispersion of Fukushima-derived radionuclides and their homogenization in the atmosphere

Long-range simulation of the dispersion of air pollutants in the atmosphere is one of the most challenging tasks in geosciences. Application of precise and fast numerical models in risk management and decision support can save human lives and can diminish consequences of an accidental release. Disaster at Fukushima Daiichi nuclear power plant has been the most serious event in the nuclear technology and industry in the recent years. We present and discuss the results of the numerical simulations on dispersion of Fukushima-derived particulate 131I and 137Cs using a global scale Lagrangian particle model. We compare concentrations and arrival times, using two emission scenarios, with the measured data obtained from 182 monitoring stations located all over the Northern Hemisphere. We also investigate the homogenization of isotopes in the atmosphere. Peak concentrations were predicted with typical accuracy of one order of magnitude showing a general underestimation in the case of 131I but not for 137Cs. Tropical and Arctic plumes, as well as the early detections in American and European midlatitudes were generally well predicted, however, the later regional-scale mixing could not be captured by the model. Our investigation highlights the importance of the parameterization of free atmospheric turbulence.

常磐-三陸沖合，仙台湾および親潮域の海水および動物プランクトンにおける東京電力福島第一原子力発電所事故に伴う&lt;sup&gt;134&lt;/sup&gt;Csおよび&lt;sup&gt;137&lt;/sup&gt;Cs濃度の時系列変動

常磐-三陸沖合，仙台湾および親潮域の海水および動物プランクトンにおける東京電力福島第一原子力発電所事故に伴う&lt;sup&gt;134&lt;/sup&gt;Csおよび&lt;sup&gt;137&lt;/sup&gt;Cs濃度の時系列変動

Fukushima derived radiocesium in subsistence-consumed northern fur seal and wild celery

In July 2014, our investigative team traveled to St. Paul Island, Alaska to measure concentrations of radiocesium in wild-caught food products, primarily northern fur seal (Callorhinus ursinus). The 2011 Fukushima Daiichi Nuclear Power Plant accident released radiocesium into the atmosphere and into the western Pacific Ocean; other investigators have detected Fukushima-derived radionuclides in a variety of marine products harvested off the western coast of North America. We tested two subsistence-consumed food products from St. Paul Island, Alaska for Fukushima-derived radionuclides: 54 northern fur seal, and nine putchki (wild celery, Angelica lucida) plants. Individual northern fur seal samples were below minimum detectable activity concentrations of 137Cs and 134Cs, but when composited, northern fur seal tissues tested positive for trace quantities of both isotopes. Radiocesium was detected at an activity concentration of 37.2 mBq 134Cs kg−1 f.w. (95% CI: 35.9–38.5) and 141.2 mBq 137Cs kg−1 f.w. (95% CI: 135.5–146.8). The measured isotopic ratio, decay-corrected to the date of harvest, was 0.26 (95% CI: 0.25–0.28). The Fukushima nuclear accident released 134Cs and 137Cs in roughly equal quantities, but by the date of harvest in July 2014, this ratio was 0.2774, indicating that this population of seals has been exposed to small quantities of Fukushima-derived radiocesium. Activity concentrations of both 134Cs and 137Cs in putchki were below detection limits, even for composited samples. Northern fur seal is known to migrate between coastal Alaska and Japan and the trace 134Cs in northern fur seal tissue suggests that the population under study had been minimally exposed Fukushima-derived radionuclides. Despite this inference, the radionuclide quantities detected are small and no impact is expected as a result of the measured radiation exposure, either in northern fur seal or human populations consuming this species.

Fukushima-derived radionuclides in sediments of the Japanese Pacific Ocean coast and various Japanese water samples (seawater, tap water, and coolant water of Fukushima Daiichi reactor unit 5).

We investigated Ocean sediments and seawater from inside the Fukushima exclusion zone and found radiocesium (134Cs and 137Cs) up to 800 Bq kg−1 as well as 90Sr up to 5.6 Bq kg−1. This is one of the first reports on radiostrontium in sea sediments from the Fukushima exclusion zone. Seawater exhibited contamination levels up to 5.3 Bq kg−1 radiocesium. Tap water from Tokyo from weeks after the accident exhibited detectable but harmless activities of radiocesium (well below the regulatory limit). Analysis of the Unit 5 reactor coolant (finding only 3H and even low 129I) leads to the conclusion that the purification techniques for reactor coolant employed at Fukushima Daiichi are very effective.

Backward-in-time methods to simulate large-scale transport and mixing in the ocean

In oceanography and meteorology, it is important to know not only where water or air masses are headed for, but also where they came from as well. For example, it is important to find unknown sources of oil spills in the ocean and of dangerous substance plumes in the atmosphere. It is impossible with the help of conventional ocean and atmospheric numerical circulation models to extrapolate backward from the observed plumes to find the source because those models cannot be reversed in time. We review here recently elaborated backward-in-time numerical methods to identify and study mesoscale eddies in the ocean and to compute where those waters came from to a given area. The area under study is populated with a large number of artificial tracers that are advected backward in time in a given velocity field that is supposed to be known analytically or numerically, or from satellite and radar measurements. After integrating advection equations, one gets positions of each tracer on a fixed day in the past and can identify from known destinations a particle positions at earlier times. The results provided show that the method is efficient, for example, in estimating probabilities to find increased concentrations of radionuclides and other pollutants in oceanic mesoscale eddies. The backward-in-time methods are illustrated in this paper with a few examples. Backward-in-time Lagrangian maps are applied to identify eddies in satellite-derived and numerically generated velocity fields and to document the pathways by which they exchange water with their surroundings. Backward-in-time trapping maps are used to identify mesoscale eddies in the altimetric velocity field with a risk to be contaminated by Fukushima-derived radionuclides. The results of simulations are compared with in situ mesurement of caesium concentration in sea water samples collected in a recent research vessel cruise in the area to the east of Japan. Backward-in-time latitudinal maps and the corresponding material-line techniques are applied to document transport of water masses across strong currents. Backward-in-time drift maps are shown to be useful in identifying the Lagrangian fronts favorable for fishery.

Fukushima radionuclides in the NW Pacific, and assessment of doses for Japanese and world population from ingestion of seafood.

Variations of Fukushima-derived radionuclides (90Sr, 134Cs and 137Cs) in seawater and biota offshore Fukushima and in the NW Pacific Ocean were investigated and radiation doses to the Japanese and world population from ingestion of seafood contaminated by Fukushima radionuclides were estimated and compared with those from other sources of anthropogenic and natural radionuclides. The total effective dose commitment from ingestion of radionuclides in fish, shellfish and seaweed caught in coastal waters off Fukushima was estimated to be 0.6 ± 0.4 mSv/y. The individual effective dose commitment from consumption of radioactive-contaminated fish caught in the open Pacific Ocean was estimated to be 0.07 ± 0.05 mSv/y. These doses are comparable or much lower than doses delivered from the consumption of natural 210Po in fish and in shellfish (0.7 mSv/y). The estimated individual doses have been below the levels when any health damage of the Japanese and world population could be expected.

Chaotic Lagrangian transport and mixing in the ocean

Dynamical systems theory approach has been successfully used in physical oceanography for the last two decades to study mixing and transport of water masses in the ocean. The basic theoretical ideas have been borrowed from the phenomenon of chaotic advection in fluids, an analogue of dynamical Hamiltonian chaos in mechanics. The starting point for analysis is a velocity field obtained by this or that way. Being motivated by successful applications of that approach to simplified analytic models of geophysical fluid flows, researchers now work with satellite-derived velocity fields and outputs of sophisticated numerical models of ocean circulation. This review article gives an introduction to some of the basic concepts and methods used to study chaotic mixing and transport in the ocean and a brief overview of recent results with some practical applications of Lagrangian tools to monitor spreading of Fukushima-derived radionuclides in the ocean.

Fukushima-derived radionuclides 134Cs and 137Cs in zooplankton and seawater samples collected off the Joban-Sanriku coast, in Sendai Bay, and in the Oyashio region

The Fukushima Dai-ichi nuclear power plant (FNPP) accident that followed the Great East Japan Earthquake in 2011 resulted in the release of enormous quantities of anthropogenic radionuclides, especially radioactive cesium (134Cs and 137Cs) into the ocean off the east coast of Japan. FNPP-derived radioactive Cs may have consequently accumulated within marine food webs via seawater intake and predator–prey interactions. We provide evidence of the temporal variability in 134Cs and 137Cs concentrations in seawater and zooplankton samples collected in coastal waters off Joban-Sanriku, in Sendai Bay, and in the Oyashio region between June 2011 and December 2013. In Sendai Bay, seawater 134Cs and 137Cs concentrations exceeded 1 Bq/kg in June 2011 and rapidly decreased during the study period. 134Cs and 137Cs concentrations in zooplankton were also high in June 2011, up to 23 Bq/kg-wet and also decreased during the study period, although at a slower rate than seawater 134Cs and 137Cs concentrations. Regarding 137Cs concentrations, the difference in the rate of decrease between seawater and zooplankton resulted in a high apparent concentration ratio (aCR) for zooplankton. The observed relation between 137Cs in seawater and the aCR of zooplankton were good indicators of the progress of 137Cs contamination in zooplankton from the beginning of the FNPP accident to the restoration phase.

Radioactivity impacts of the Fukushima Nuclear Accident on the atmosphere

The Fukushima Nuclear Accident (FNA) resulted in a large amount of radionuclides released into the atmosphere and dispersed globally, which has greatly raised public concerns. The state of the art for source terms of 19 kinds of radionuclides derived from the FNA was comprehensively collected and compared with levels of the global fallout and the Chernobyl Nuclear Accident (CNA). The atmospheric impacts of the FNA were evaluated from three aspects including radioactive baseline of the atmosphere, the concentration limits in standards and radiological protection. The FNA should not impose significant radiological risk on the public members in the countries excluding Japan. A conceptual scheme of Fukushima-derived radionuclides with physical and physicochemical insights on different temporal–spatial timescales was discussed and illustrated to understand their fates in the atmosphere.

Radioactive contamination of pine (Pinus sylvestris) in Krasnoyarsk (Russia) following fallout from the Fukushima accident

Following the Fukushima accident in March 2011, samples of pine trees (Pinus sylvestris) were collected from three sites near the city of Krasnoyarsk (Siberia, Russia) during 2011–2012 and analyzed for artificial radionuclides. Concentrations of Fukushima-derived radionuclides in the samples of pine needles in April 2011 reached 5.51 ± 0.52 Bq kg−1131I, 0.92 ± 0.04 Bq kg−1134Cs, and 1.51 ± 0.07 Bq kg−1137Cs. An important finding was the detection of 134Cs from the Fukushima accident not only in the pine needles and branches but also in the new shoots in 2012, which suggested a transfer of Fukushima cesium isotopes from branches to shoots. In 2011 and 2012, the 137Cs/134Cs ratio for pine needles and branches collected in sampling areas Krasnoyarsk-1 and Krasnoyarsk-2 was greater than 1 (varying within a range of 1.2–2.6), suggesting the presence of “older”, pre-Fukushima accident 137Cs. Calculations showed that for pine samples growing in areas of the Krasnoyarskii Krai unaffected by contamination from the nuclear facility, the activity of the Fukushima-derived cesium isotopes was two–three times higher than the activity of the pre-accident 137Cs.

Geochemical behavior and activity ratios of Fukushima-derived radionuclides in aerosols at the Geological Survey of Japan, Tsukuba, Japan

Aerosols from the Fukushima Dai-ichi Nuclear Power Plant accident were collected at the Geological Survey of Japan. The temporal patterns of the 134Cs/137Cs, 136Cs/137Cs, and 132Te/137Cs activity ratios were consistent with expectations based on their half-lives. Those for 131I and 129mTe decreased with some fluctuations. 110mAg/137Cs declined more rapidly than expected and 95Nb/137Cs increased with time. The results suggest that the temporal patterns depended not only on their half-lives but also on many factors such as chemical speciation, the diversity of sources, changes in the temperature and discharge rate from the reactors, and the processes of transport.

Lagrangian study of surface transport in the Kuroshio Extension area based on simulation of propagation of Fukushima-derived radionuclides

Abstract. Lagrangian approach is applied to study near-surface large-scale transport in the Kuroshio Extension area using a simulation with synthetic particles advected by AVISO altimetric velocity field. A material line technique is proposed and applied to find out the origin of water masses in cold-core cyclonic rings pinched off from the jet in summer 2011. Tracking and Lagrangian maps provide the evidence of cross-jet transport. Fukushima-derived caesium isotopes are used as Lagrangian tracers to study transport and mixing in the area a few months after the 11 March 2011 tsunami that caused heavy damage of the Fukushima Nuclear Power Plant (FNPP). Tracking maps are computed to trace the origin of water parcels with measured levels of 134Cs and 137Cs concentrations collected during two research vessel (R/V) cruises in June and July 2011 in the large area of the northwest Pacific (Kaeriyama et al., 2013; Buesseler et al., 2012). It is shown that Lagrangian simulations are useful for finding the surface areas that are potentially dangerous due to the risk of radioactive contamination. The results of simulation are supported by tracks of the surface drifters that were deployed in the area.