Analysis of the Contamination Process of the Extremely Contaminated Fat Greenling by Fukushima-Derived Radioactive Material
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Abstract
We analyzed the contamination process by which the fat greenling, which was caught in the area off the mouth of the Ota River of Fukushima prefecture on August 1, 2012, concentrated radiocesium (134Cs + 137Cs) to the level of 25,800 Bq/kg-wet. The radioactivity environment of the area was insufficient to maintain or increase the radiocesium concentration in the fish at the time. Distribution of the radioactive materials in the otolith of the fat greenling estimated by beta-ray emissions suggested that the fat greenling was in a highly contaminated environment during the period immediately following the Fukushima Dai-ichi Nuclear Power Plant (FNPP) accident. We used a biokinetic simulation of the 137Cs concentration to demonstrate that the fat greenling had to have been exposed to radioactivity from the FNPP to achieve such a high radiocesium concentration. Thus, the extremely contaminated fat greenling originated in the heavily contaminated environment of the FNPP port or the adjoining area in the period just after the accident.
Keywords
Fat greenling Contamination Radiocesium Autoradiography13.1 Introduction
Radioactive nuclides leaked from the Fukushima Dai-ichi Nuclear Power Plant (FNPP), operated by Tokyo Electric Power Company (TEPCO), when it was damaged by the tsunami following the Tohoku Earthquake on March 11, 2011. The United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR 2013) estimated the scale of the release of several radioactive nuclides: the range for radioactive iodine (131I) was from 100 to 500 petabecquerel (PBq) and the range for radiocesium (137Cs) was from 6 to 20 PBq. The committee noted that the amounts of released radioactive nuclides were much lower than that which occurred after the Chernobyl accident (the FNPP accident released 20 % of the 137Cs levels released after Chernobyl). The remarkable feature of the FNPP accident was the swift and direct release of highly polluted water to the ocean. Coastal area of Fukushima and adjacent prefectures were covered with seawater bearing high concentrations of 131I and radiocesium (134Cs and 137Cs) after the accident. The direct leakage of 137Cs was estimated as 3.5 PBq and the highest seawater concentration (>6 × 104 Bq/l) was observed at the coast near the FNPP (Tsumune et al. 2012). This value was seven orders of magnitude higher than the pre-accident levels.
The Ministry of Agriculture, Forestry and Fisheries (MAFF) and local government initiated emergency monitoring of radioactivity in marine products immediately after the accident to ensure food safety. Their findings were published on the websites of MAFF (2014) and of the Ministry of Health, Labor and Welfare (MHLW 2014). The Fisheries Research Agency (FRA) supported the measurement of radioactivity in marine products. In April 2011, extremely high levels of 131I and radiocesium (134Cs + 137Cs; >1.0 × 104 Bq/kg-wet) were reported in sand lance larvae. Such high contamination levels were confined to larvae of pelagic fish in the area south of the FNPP and were thought to result from the spread of contaminated water after the accident (Tateda et al. 2013). After that, 131I contamination levels decreased rapidly, consistent with its short half-life (about 8.02 days), and returned to the levels below the limit of detection (hereinafter referred to as ND) after August 2011 (Wada et al. 2013). The relatively longer half-life of 134Cs (about 2.07 years) and 137C (about 30.1 years) caused them to remain in the marine environment for much longer; monitoring of radiocesium in the marine environment and marine products has continued.
Cesium is an alkali metal that is metabolized by the same pathway that metabolizes potassium, which is an essential mineral (Kaneko et al. 2013). As are other alkali metals, radiocesium is exchanged between the environment and body of marine teleost fish by their osmoregulatory systems, which maintain electrolyte balance (Evans 2010). Thus, radiocesium concentrations in the fish depend on the concentrations in the surrounding seawater. Wada et al. (2013) showed continuous reduction in radiocesium concentrations in marine products obtained off the coast of Fukushima Prefecture; the ecological half-life of radiocesium is much shorter than the physical half-lives of 134Cs and 137Cs.
TEPCO began to monitor radioactivity in marine fishes within a 20-km radius of FNPP (hereinafter referred to as the 20-km area) in March 2012. Against the decreasing trend of radiocesium in marine products, extremely high radiocesium concentrations were detected in Hexagrammos otakii (fat greenling) in the summer of 2012. The fat greenlings were caught about 1 km offshore near the mouth of the Ota River on August 1, 2012 ( Chap. 12). The reported radiocesium (134Cs + 137Cs) level was 25,800 Bq/kg-wet (TEPCO 2012a), the highest radiocesium concentration found in marine fishes at the time. An additional survey of fat greenlings in the area was conducted by TEPCO from September to October 2012, during which time 57 samples were examined (TEPCO 2012b). Most of the surveyed greenlings showed radiocesium concentrations two orders of magnitude lower than that of the fat greenling caught in the area off the mouth of the Ota River on August 1, 2012. Radiocesium concentrations ranged from ND to 1,350 Bq/kg-wet (median, 77 Bq/kg-wet), equivalent to the levels found in samples taken outside the 20-km area. TEPCO’s research on marine fish in the port of FNPP beginning in October 2012 showed highly contaminated fish species, including fat greenlings, with radiocesium concentrations exceeding 10,000 Bq/kg-wet (TEPCO 2014a). Statistical analysis of the data from fat greenlings showed that the probability of finding fat greenlings with 137Cs concentrations exceeding 16,000 Bq/kg-wet was below 3.0 × 10−6, suggesting their radioactive exposure history was similar to that of the population in the port of FNPP (Shigenobu et al. 2014, Chap. 12).
The purpose of this study was to determine the contamination process of fat greenling by performing a quantitative analysis. We evaluated the radioactivity of the marine environment and the potential for generating highly contaminated fat greenlings. Analysis of fat greenling otoliths revealed the radioactive exposure history of the fish, the progress of which was examined by biokinetic model simulations.
13.2 137Cs Concentrations in Coastal Seawater and Marine Fish off the Coast of Fukushima Prefecture
Locations of radiocesium monitoring stations along the coast of Fukushima prefecture. Site-FP represents the station at the shallow draft quay in the Fukushima Dai-ichi Nuclear Power Plant (FNPP) port. Stations T-1, T-2, and T-2-1 are adjacent to the FNPP port and are referred to as site-F1. Stations T-3, T-4, T-4-1, and T-4-2 are located around the Fukushima Dai-ichi Nuclear Power Plant and southward, referred to as site-F2. Station T-S1 is the collection point for the extremely contaminated fat greenling exhibiting 25,800 Bq/kg-wet radiocesium (134Cs + 137Cs)
Data points of ND were interpolated to produce continuous daily data. ND data during several days at site-FP were interpolated by using the minimum values obtained in the 15 days around the target day; longer consecutive ND periods were filled with values calculated from data obtained at other station in the port by regression analysis. ND data in the site-F1 and site-F2 time-series were filled in the same way.
Combined time-series of observed and interpolated daily 137Cs concentration data at site-FP, site-F1, and site-F2 from March 21, 2011, to August 31, 2014
Temporal trends of observed 137Cs concentrations in fat greenlings caught in the coastal waters of Fukushima Prefecture, except the 20-km area and in the 20-km area with median values and 95th percentile values calculated from combined data of both for each 6-month period. The first term includes data from March 1, 2011 to August 31, 2011
13.3 The Marine Environment as a Source of Radioactive Contamination of the Fat Greenling
We sought to determine whether the observed radioactivity in the environment in the summer of 2012 could maintain radiocesium (134Cs + 137Cs) concentrations of 25,800 Bq/kg-wet in the fat greenling. Marine fish obtain radiocesium from the environment via uptake of food and water. 137Cs concentrations in marine fish directly correlate with the concentrations in seawater under stable conditions (Kasamatsu 1999; IAEA 2004), expressed as the concentration factor (CF). Kasamatsu (1999) summarized the CFs of 137Cs for 27 species of marine teleost fish around Japan. The CFs were calculated from data obtained between 1984 and 1996; the average CF value for each fish species ranged from 22 to 122. The IAEA-recommended CF value of 100 for marine fish lies within this range (IAEA 2004). We estimated the CF for fat greenling off the coast of Fukushima prefecture from 29 measures obtained in 1982–2010, archived, and published by the NRA (Nuclear Regulation Authority 2014). The average CF was 67 ± 29, also within the range described by Kasamatsu (1999).
The CF value for fat greenling off the coast of Fukushima suggested that the surrounding seawater should contain 137Cs concentrations of 240 Bq/l to maintain a 137Cs concentration of 16,000 Bq/kg-wet (25,800 Bq/kg-wet for 134Cs + 137Cs) in the fish. In August 2012, the 137Cs concentration of seawater was less than 0.1 Bq/l off the coast of Fukushima Prefecture; the highest values observed in the FNPP port were also less than 100 Bq/l (TEPCO 2014b). TEPCO (2012b) also reported values much lower than 0.1 Bq/l in samples obtained around the Ota River.
We also considered the possibility that excretion of 137Cs from the fish was compensated for by ingestion of prey. Assuming a biological half-life of 100 days (World Health Organization and Food and Agriculture Organization of the United Nations 2011), the daily excretion rate was calculated as 0.0069 day−1 and the daily amount of 137Cs excreted from the fat greenling was 110 Bq/kg-wet. Assuming an ingestion rate of 0.03 day−1 and assimilation rate of 0.5 (Tateda 1997), the fat greenling would have to consume more than 7,300 Bq/kg-wet 137Cs daily to compensate for excretion. The 137Cs concentrations in the marine biota within the 20-km area were ND to 1,000 Bq/kg-wet (TEPCO 2014a), far below the required level.
Thus, the status of environmental 137Cs contamination in the area off the Ota River and in the 20-km area were insufficient to maintain the 16,000 Bq/kg-wet 137Cs concentration observed in the fat greenling, which were then assumed to be excreting excess radiocesium.
13.4 Radioactivity in the Otolith of Contaminated Fat Greenling
The fish otolith is a hard tissue that retains information on the age of the fish and the history of its environment, including temperature, salinity, and chemical composition (Campana 1999). The fish otolith consists mostly of calcium carbonate and other elements that indicate environmental exposure. For example, strontium is often used as an indicator of environmental salinity (Tsukamoto et al. 1998). Radioactive materials absorbed in the otolith are also used as indicators of environmental conditions. Baker and Wilson (2001) showed that the otolith core of red snapper from the Gulf of Mexico contains 14C produced by nuclear testing. We analyzed the radioactive nuclides contained in the otolith of the fat greenling to characterize its history of radioactive exposure.
Otolith of the fat greenling (a) and its slice (b). The otolith in this figure was extracted from the right side of the fat greenling’s head. The slice was cut from the left-hand otolith
Image of the otolith slice and distribution of cumulative strength of incident radiation on an imaging plate (IP). Dense (light) shading areas of the otolith slice correspond to the transparent (opaque) zone. Colors indicate the cumulative strength normalized to the highest value. The rectangle encloses the area of detailed analysis where the zonal patterns of the annulus were obvious and the one-dimensional analysis along the vertical direction could be applied
Comparison between the grey level of the otolith slice and the relative reaction strength of the IP for the enclosed area in Fig. 13.5. Thirty vertical rows of IP pixel data were included. Relative reaction strength data for each vertical row were reconstructed by using the peak position of the second transparent zone as the origin. The vertical distribution of the zonally averaged grey level of the otolith slice is shown by a solid thin line. Lower (higher) grey levels in the otolith slice correspond to the opaque (transparent) zone. The relative reaction strength of each pixel of the IP is shown with a full circle. The fitted curve for the IP pixel data in the area around the peak of the second transparent zone is shown by a sequence of large full circles. Upward arrow indicates the center of the second transparent zone
The opaque zone of the otolith was formed in the summer season (Sekigawa et al. 2002); the first transparent-opaque zone on the slice from the fat greenling caught in the summer of 2012 was thought to correspond to the period from autumn 2011 to summer 2012. Thus, the second zone containing the most beta ray-emitting radionuclides corresponded to the period from autumn 2010 to summer 2011. These results strongly suggested that the fat greenling was in an environment rich in beta ray-emitting nuclides between the spring and summer of 2011.
A possible candidate of beta ray-emitting radionuclide contained in the otolith was 90Sr. The beta-ray emissions from the otolith of several fish species collected in the FNPP port were associated with 90Sr concentration in the body, excluding the viscera, and were associated with 137Cs in the muscle tissue (Fujimoto et al. 2013). The amount of 90Sr leakage was estimated at about 3 % of 137Cs (Casacuberta et al. 2012), but it was thought that the 90Sr concentration in seawater rapidly increased, similar to 137Cs from late March to the beginning of April 2011. From these relationships, we hypothesized that the fat greenling absorbed a large amount of radioactive nuclides in the period just after the FNPP accident when contaminated seawater covered the coastal area of Fukushima Prefecture.
13.5 Simulation of 137Cs Concentrations in Fat Greenlings Using a Biokinetic Model
Variables and parameters in the biokinetic equation for a fat greenling
| Variable | Value | Unit | Explanation |
|---|---|---|---|
| C f | Bq/kg-wet | 137Cs concentration in fish body | |
| C pf | Bq/kg-wet | 137Cs concentration in prey fish body | |
| C w | Bq/l | 137Cs concentration of surrounding seawater | |
| C pi | Bq/kg-wet | 137Cs concentration of prey invertebrate | |
| k w | 0.10a | (kg/l) day−1 | Uptake rate of 137Cs activity from seawater |
| IR f | 0.030a | day−1 | Ingestion rate per unit mass of fish |
| AE f | 0.50a | No dimension | Assimilation efficiency for fish |
| k f | 0.0088a | day−1 | Excretion rate of 137Cs for fish |
| CF pi | 10b | No dimension | Concentration factor for prey invertebrate |
| k pi | 0.0087b | day−1 | Excretion rate of 137Cs for prey invertebrate |
| a | 0.36b | No dimension | Mixing ratio of prey fish |
Simulated 137Cs concentration of fat greenlings for site-FP, site-F1, and site-F2 with observed 137Cs concentrations in fat greenling caught in the coastal waters of Fukushima Prefecture, except the 20-km area, in the 20-km area, and in the FNPP port
Simulation results for site-F1 (dashed line) and site-FP (thin solid line) are also shown in Fig. 13.7. The same curve shape was observed, although at a different level. Maximum 137Cs concentration were observed in mid-July and correlated with the integrated values in seawater. The observed 137Cs concentration in fat greenling from the FNPP port was moderately simulated by the model. The 137Cs concentration in the highly contaminated fat greenling was in the range between simulations for site-FP in the FNPP port and site-F1. These model simulations support the hypothesis that the fat greenling collected in the summer of 2012 off the mouth of the Ota River had been exposed to the highly contaminated environment in the FNPP port or adjoining areas.
The range of 137Cs concentrations formed by the large difference between simulations for site-FP and site-F1 bracketed the majority of the distribution of 137Cs concentrations in fat greenlings in the FNPP port. The 137Cs concentration data at site-FP were within the intermediate range compared with other observation points at the initial stage of the radiation leak. Available seawater 137Cs concentration data from April 2011 showed that the averaged value for the observation point in the intake canal south of site-FP was several times higher than the value at site-FP. The minimum values of 137Cs concentrations in the port, where the concentrations were probably no lower than the level found outside the port (site-F1), where the concentration was about one order of magnitude lower than at site-FP. The large variability of observed 137Cs concentrations in fat greenling was partly attributed to the local spatial and temporal distribution of 137Cs in the FNPP port. In additional simulations of a fat greenling entering the FNPP port after the peak period of environmental contamination, highly contaminated fat greenlings were also generated, mainly by prey uptake. This process might also maintain the wider range in the group of highly contaminated fat greenlings in the FNPP port.
As for the extremely contaminated fat greenling caught in the area off the mouth of the Ota River, radioactivity in the otolith and the simulation suggested a generation scenario. The fat greenling were living in the FNPP port or in the adjoining area when contaminated water leaked to the sea and highly contaminated seawater covered the area. The 137Cs concentration of the fat greenling may have reached about 100,000 Bq/kg-wet. The relatively lower concentration compared with other fat greenlings in the FNPP port suggest the habitat was apart from the intake canal of the FNPP port and the fat greenling was able to avoid a direct encounter with the more highly contaminated seawater. After the direct leakage of highly contaminated water to the sea, the fat greenling eventually left the port.
Notes
Acknowledgments
The authors appreciate the members of the Research Center for Fisheries Oceanography and Marine Ecosystem of the National Research Institute of Fisheries Science for their support. The sliced sample of the otolith was processed by Japan NUS, and the autoradiographic measurement of the otolith slice was performed by BayBioImaging. This study was financially supported by the Fisheries Agency.
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