Soil-to-plant transfer factors of fallout <Superscript>137</Superscript>Cs and native <Superscript>133</Superscript>Cs in various crops collected in Japan

In order to compare the soil-to-plant transfer factors (TFs) of fallout ¹³⁷Cs and those of native stable ¹³³Cs, concentrations of these isotopes were determined in various crops and the associated soils collected throughout Japan. The results showed that TF-¹³⁷Cs was 11 times higher than TF-native ¹³³Cs for brown rice, while those values were almost the same for leafy vegetables. Possibly, fallout ¹³⁷Cs would be more mobile and more easily adsorbed by plants than native ¹³³Cs in the soil because a part of the ¹³³Cs is in a soil structure where it is hard to replace with ¹³⁷Cs. However, ¹³⁷Cs and native ¹³³Cs have reached an approximately isotopic equilibrium in the bioavailable fraction in the soils, therefore, the TF-native ¹³³Cs can be used for long-term transfer of ¹³⁷Cs in the environment.     

Relationship between particle size and radiocesium in fluvial suspended sediment related to the Fukushima Daiichi Nuclear Power Plant accident

We collected fluvial suspended sediments in Fukushima after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident and analyzed the ¹³⁷Cs concentration in bulk and size-fractioned samples to investigate the particle-size-dependent distribution of radiocesium. The ¹³⁷Cs concentration in bulk suspended sediments decreased from August to December 2011, possibly reflecting a decrease of radiocesium concentration in its source materials. Smaller particles had higher radiocesium concentrations, reflecting larger specific surface areas. Silt- and sand-size fractions occupied more than 95 % of the total ¹³⁷Cs in the suspended sediments. The contribution of clay-size fractions, which had the highest ¹³⁷Cs concentration, was quite small because of their low frequency. A line of the data showed that the particle size distribution of radiocesium was essential to evaluate the migration and distribution of radiocesium in river systems where radiocesium is mainly present as particulate form after the FDNPP accident.     

Transfer of 137Cs and stable Cs in soil-grass-milk pathway in Aomori, Japan

The soil-to-grass transfer factors and grass-to-milk transfer coefficients were determined for ¹³⁷Cs and stable Cs in soil, grass and milk samples collected in Aomori Prefecture, Japan. The concentrations of ¹³⁷Cs in the soil and grass samples collected from 25 sampling sites were 13±12 Bq.kg^-1 and 2.0±2.1 Bq.kg^-1 dry wt., respectively. The geometric mean of soil-to-grass transfer factor of ¹³⁷Cs was 0.13 and its 95% confidence interval was 0.017-0.98. The transfer factor of ¹³⁷Cs was higher than that of stable Cs, and they had a positive correlation. The concentration of K in the soil affected both transfer factors. The concentration of ¹³⁷Cs in milk samples collected from 16 sites was 76±43 mBq.kg^-1 fresh wt. and had a good correlation with that of stable Cs. The geometric mean of grass-to-milk transfer coefficient of ¹³⁷Cs was 0.0027, assuming that a cow's total daily intake was 20 kg of dry grass. The transfer coefficient of ¹³⁷Cs was positively correlated with that of stable Cs.     

Relationships among <Superscript>137</Superscript>Cs, <Superscript>133</Superscript>Cs,and K in plant uptake observed in Japanese agricultural fields

Plant uptake of radiocesium (¹³⁷Cs) was investigated in consideration of the relationships with naturally existing ¹³³Cs and potassium (K). We first determined plant-unavailable fraction of ¹³⁷Cs in soil by batch sorption and sequential extraction methods with a radiotracer. Then, using the data obtained from the batch sorption and extraction methods, we clarified the relationships of plant-available and plant-unavailable fractions between ¹³⁷Cs, ¹³³Cs, and K in soil. Additionally, ¹³⁷Cs concentrations in crop were estimated using ¹³⁷Cs in soil and several factors, i.e. fixation ratio of ¹³⁷Cs in soil, cation exchange capacity, and K concentration in crop. The results implied that the fixation ratio of ¹³⁷Cs in soil was a very important key to understanding ¹³⁷Cs plant uptake.     

Distribution of 131I, 134Cs, 137Cs and 239,240Pu concentrations in Korean rainwater after the Fukushima nuclear power plant accident

Radionuclides such as ¹³¹I, ¹³⁴Cs, ¹³⁷Cs, and ^239,240Pu in Korean rainwater have been analyzed by Korea Research Institute of Standards and Science (KRISS) since the Fukushima nuclear power plant accident in March 2011 to investigate the activity level, distribution pattern, and temporal variation and to assess the radiation dose the public is exposed to. The concentration of ¹³¹I in the Korean rainwater samples varied between 0.033 (minimum detectable activity; MDA) and 1.30 Bq kg^?1 and the concentrations tended to decrease exponentially with time. The concentrations of ¹³⁴Cs and ¹³⁷Cs in rainwater ranged from 0.01 to 334 ± 74 and 0.29 ± 0.01 to 276 ± 1 mBq kg^?1, respectively. The mean activity ratio of ¹³⁷Cs/¹³⁴Cs in the rainwater samples collected from April 18 to May 12 was estimated to be 0.44 ± 0.21, and this value is lower than that (ca. 1) observed in Fukushima, Japan, when there was an escape from the nuclear reactors. When an attempt was made to analyze Pu isotopes in rainwater samples, no Pu isotopes were detected above the MDA in any of the rainwater samples. Although the locations investigated were different from Asia to Europe, the concentrations of ¹³¹I, ¹³⁴Cs and ¹³⁷Cs in the rainwater are comparable, which suggests a global contamination of ¹³¹I, ¹³⁴Cs, and ¹³⁷Cs occurred because of the Fukushima nuclear power plant accident.     

Fukushima-derived radionuclides in ground-level air of Central Europe: a comparison with simulated forward and backward trajectories

Results of forward and backward modeling of air mass transport from Fukushima Daiichi nuclear power plant to Slovakia were compared with aerosol radioactivity measurements. Several radionuclide maxima (¹³¹I, ¹³⁴Cs and ¹³⁷Cs) were observed in the Bratislava ground-level air in March–April 2011. The ¹³¹I/¹³⁷Cs activity ratio records showed the presence of two different fresh air masses in the Bratislava air, supported by simulations of forward and backward trajectories between Fukushima and Bratislava.     

Radionuclides from Fukushima accident in Thessaloniki, Greece (40°N) and Milano, Italy (45°)

¹³¹I, ¹³⁷Cs and ¹³⁴Cs were observed in environmental samples in Milano (40°N), Italy and Thessaloniki (45°N), Greece, soon after the nuclear accident in Fukushima, Japan. The radionuclide concentrations were determined and studied as a function of time. In Thessaloniki the ¹³¹I in air was observed for the first time on March 24, 2011. In Milano, the first evidence of Fukushima fallout has been confirmed with ¹³¹I and ¹³⁷Cs measured in wet precipitation collected 2 days later. The maximum ¹³¹I activity concentration in air of 467 ± 25 μBq m^?3, observed in Milano on April 3–4, 2011, was almost similar to the highest value of 497 ± 53 μBq m^?3 observed in Thessaloniki. The ¹³⁴Cs/¹³⁷Cs activity ratio values in air were around 1 in both regions. Soil, grass and milk samples were contaminated with ¹³¹I and ¹³⁷Cs at a low level. Finally, a dose assessment for these two areas showed clearly that the detected activities in all environmental samples were far below levels of concern.     

A complementary cesium coolant concentration ratio for localizing defective PWR fuel rods during reactor operation

Rough techniques for pinpointing defective fuel pins during actual reactor operation were developed for nuclear power plants. These techniques are based on various fission product concentration ratios. Here, a new cesium concentration ratio,¹³⁴Cs/¹³⁶Cs, was tested in combination with the more usual cesium ratio¹³⁴Cs/¹³⁷Cs. This new cesium ratio confirmed the conclusions drawn from the ratio¹³⁴Cs/¹³⁷Cs and provided some additional information on the location of the defective fuel rods. Application of this second cesium ratio improves the reliability of the rough localization method.     

Comparison of thermal ionization mass spectrometry and Multiple Collector Inductively Coupled Plasma Mass Spectrometry for cesium isotope ratio measurements

In the nuclear domain, precise and accurate isotopic composition determination of elements in spent nuclear fuels is mandatory to validate neutron calculation codes and for nuclear waste disposal. The present study presents the results obtained on Cs isotope ratio by mass spectrometric measurements. Natural cesium is monoisotopic (¹³³Cs) whereas cesium in spent fuels has 4 isotopes (¹³³Cs, ¹³⁴Cs, ¹³⁵Cs, and ¹³⁷Cs). As no standard reference material is available to evaluate the accuracy of Cs isotopic measurements, a comparison of cesium isotopic composition in spent nuclear fuels has been performed between Thermal Ionization Mass Spectrometry (TIMS) and a new method involving Multiple Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICPMS) measurements. For TIMS measurements, isotopic fractionation has been evaluated by studying the behavior of cesium isotope ratios (¹³³Cs/¹³⁷Cs and ¹³⁵Cs/¹³⁷Cs) during the analyses. For MC-ICPMS measurements, the mass bias effects have been corrected with an external mass bias correction using elements (Eu and Sb) close to cesium masses. The results obtained by the two techniques show good agreement: relative difference on ¹³³Cs/¹³⁷Cs and ¹³⁵Cs/¹³⁷Cs ratios for two nuclear samples, analyzed after chemical separation, ranges from 0.2% to 0.5% depending on the choice of reference value for mass bias correction by MC-ICPMS. Finally the quantification of the ¹³⁵Cs/²³⁸U ratio by the isotope dilution technique is presented in the case of a MOx (mixed oxide) spent fuel sample. Evaluation of the global uncertainties shows that this ratio could be defined at an uncertainty of 0.5% (k = 2). The intercomparison between two independent mass spectrometric techniques is fundamental for the evaluation of uncertainty when no isotopic standard is available.     

Concentrations of 137Cs and 40K in wild mushrooms collected in a forest on Noto Peninsula,Japan

A variety of wild mushrooms were collected in a forest on the Noto Peninsula, Japan, to determine the concentration of ¹³⁷Cs and ⁴⁰K. The wild mushroom species belong to the orders Agaricales and Aphyllophorales. The concentration of ¹³⁷Cs varied widely (1.4–4,100 Bq/kg dry weight) in mushrooms growing in soil. On the contrary, ¹³⁷Cs concentration levels were relatively low (1.9–20 Bq/kg-dry weight) in mushrooms growing on wood. The concentration of ⁴⁰K varied widely (12–2,400 Bq/kg-dry weight) in contrast with several previous reports that suggest relatively constant ⁴⁰K levels in mushrooms. Unusually low concentrations of ⁴⁰K were observed in a few mushroom species that had very hard fruiting bodies with peculiar shapes. The mean and median of ¹³⁷Cs concentration in the present study were similar to those previously reported for Japanese mushrooms. Among the Agaricales mushrooms, Entolomataceae and Tricholomataceae families growing in soil had the highest concentration of ¹³⁷Cs. Among the Aphyllophorales mushrooms, Gomphaceae and Ramariaceae families growing in soil also had the highest ¹³⁷Cs concentrations. The concentrations of ¹³⁷Cs and stable Cs in mushroom samples were positively correlated. The concentration ratio of ¹³⁷Cs/Cs differed between Agaricales and Aphyllophorales mushrooms. The average ¹³⁷Cs/Cs ratio in mushrooms growing in soil was similar to that calculated for the top soil (<5 cm deep) alone because the mycelia of the mushrooms were mainly distributed near the surface of the soil.     

Vertical Profiles, Inventories, and Activity Ratios of 239+240Pu and 137Cs in Sediments from Sagami Bay, Western Northwest Pacific Margin

Marine sediment cores were taken from Sagami Bay of the western Northwest Pacific and analyzed for ^239+240Pu and ¹³⁷Cs activities. A significant correlation was observed between ^239+240Pu and ¹³⁷Cs activities in sediment cores, i.e., their vertical profiles. The measured activities which were used to obtain the inventories of ^239+240Pu and ¹³⁷Cs in the sediment column, showed large variations, ranging from 36 to 474 MBq/km² for ^239+240Pu and 49 to 652 MBq/km² for ¹³⁷Cs. ^239+240Pu inventories in the sediment from one region in the Bay, Sagami Nada were 5–10 times greater than those predicted from atmospheric global fallout 42 MBq/km² at the same latitude. On the other hand, ¹³⁷Cs inventories, with a mean value of 297±168 MBq/km², were much less than predicted, 2040 MBq/km². The activity ratios of ^239+240Pu/¹³⁷Cs obtained, with a mean of 0.65±0.17, were significantly greater than the ratio predicted from fallout, 0.021. Furthermore, there was a clear relationship between both ^239+240Pu and ¹³⁷Cs inventories and the water content, indicating that higher inventories may be attributed principally to concentration in, and scavenging by, fine-grained particles.     

Removal of226Ra(II) from uranium mining and processing effluents

The activity of¹³⁷Cs was determined in mosses and their surrounding soils in three Venezuelan cloud forests. The concentration of¹³⁷Cs in both the mosses and their respective soils were correlated with elevation (m.a.s.l.). This relationship was the result of the cloud forest effect, no direct deposition by condensation below the base of the clouds and increasing deposition of¹³⁷Cs with the density of the clouds. The ratio of the activity of¹³⁷Cs in the mosses to their surrounding soils was in general the same for sites near the top of the mountains, but the ratio at the Altos de pipe location was 3.5 times higher than that of the La Sierra mountain. This was explained by the difference in the water content of the surface and the top soil layer. It was concluded that the¹³⁷Cs measured in the mosses was from the soil effect rather than new deposition of¹³⁷Cs in the last three years.     

Combination of atomic lines and molecular bands for uranium optical isotopic analysis in laser induced plasma spectrometry

Radionuclide concentrations in wharf roaches inhabiting coastal areas of Honshu, Japan, were investigated in October 2011 and June 2012. Relative high concentrations of ^110mAg (2.1–127 Bq kg-wet^?1), ¹³⁴Cs (2.6–61 Bq kg-wet^?1), and ¹³⁷Cs (3.5–92 Bq kg-wet^?1) were detected in specimens from the eastern Honshu areas. Significantly lower ¹³⁷Cs concentrations (0.7–1.6 Bq kg-wet^?1) were detected in specimens from western and northern Honshu. The decay-corrected ¹³⁷Cs concentration was significantly inversely correlated with the distance from the Fukushima Dai-ichi Nuclear Power Plant. Thus, wharf roach may serve as a good bioindicator for monitoring radioactive contamination of its habitats.     

Rapid determination of Cs and precise Cs/Cs atomic ratio in environmental samples by single-column chromatography coupled to triple-quadrupole inductively coupled plasma-mass spectrometry

For source identification, measurement of ¹³⁵Cs/¹³⁷Cs atomic ratio not only provides information apart from the detection of ¹³⁴Cs and ¹³⁷Cs, but it can also overcome the application limit that measurement of the ¹³⁴Cs/¹³⁷Cs ratio has due to the short half-life of ¹³⁴Cs (2.06 y). With the recent advancement of ICP-MS, it is necessary to improve the corresponding separation method for rapid and precise ¹³⁵Cs/¹³⁷Cs atomic ratio analysis. A novel separation and purification technique was developed for the new generation of triple-quadrupole inductively coupled plasma-mass spectrometry (ICP-MS/MS). The simple chemical separation, incorporating ammonium molybdophosphate selective adsorption of Cs and subsequent single cation-exchange chromatography, removes the majority of isobaric and polyatomic interference elements. Subsequently, the ICP-MS/MS removes residual interference elements and eliminates the peak tailing effect of stable ¹³³Cs, at m/z 134, 135, and 137. The developed analytical method was successfully applied to measure ¹³⁵Cs/¹³⁷Cs atomic ratios and ¹³⁵Cs activities in environmental samples (soil and sediment) for radiocesium source identification.     

Extraction of cesium in seawater off Japan using AMP-PAN resin and quantification via gamma spectroscopy and inductively coupled mass spectrometry

The March 2011 earthquake off the Japanese coast and subsequent tsunami that devastated the Fukushima Dai-Ichi nuclear power plant resulted in the largest accidental release of cesium 137 and 134 to the oceans. Seawater samples were collected in June 2011 from 30 to 600 km off the coast of Japan as part of initial mapping of the spread of contamination in the ocean. Cesium was extracted from unfiltered and filtered (<1.0 μm) seawater using an absorber based upon an organic polymer polyacrylonitrile (PAN) containing ammonium molybdophosphate (AMP) Sebesta and Stefula (J Radioanal Nucl Chem 140:15–21, 1990). The AMP-PAN resin can be counted directly using gamma spectroscopy for ¹³⁴Cs and ¹³⁷Cs. Stable ¹³³Cs was added to evaluate extraction efficiency and quantified by ICP-MS. Our 5 mL AMP-PAN resin column was on average 95 % efficient in the removal of cesium from 20 L samples at an average flow rate of 35 mL min^?1. Measured activities of ¹³⁴Cs and ¹³⁷Cs ranged from a few Bq m^?3 to >300 Bq m^?3. The extraction column can be adapted to different sample volumes and easily used in the field.     

Measurement of fallout with rain in Hiroshima and several sites in Japan from the Fukushima reactor accident

Fallout with rain from the Fukushima reactor accident was monitored for about two months in Higashi-Hiroshima City, Hiroshima, Japan, from March 20 to May 23, 2011. Gamma-ray (γ-ray) spectra measured using a low background HPGe spectrometer showed clear evidence of fission products—¹³¹I, ¹³⁷Cs, and ¹³⁴Cs. The ¹³¹I was observed on March 27 and April 8, while ¹³⁷Cs and ¹³⁴Cs were observed on March 27, April 18, and April 22. The ¹³¹I, ¹³⁷Cs, and ¹³⁴Cs activity concentrations in rainwater collected in Hiroshima reached 0.44 ± 0.09 on April 8, 0.17 ± 0.01 on April 18, and 0.15 ± 0.01 Bq/L on April 18, 2011, respectively. These activity levels were compared with global results collected from the Northern Hemisphere. Several samples of rainwater that were collected in Chiba (Kashiwa) on March 21, April 11, and May 12; Tokyo (Nerima) on March 21 and April 11; Osaka (Hirano) on April 8; Nara (Kitakatsuragi) on April 9; and Fukushima (Fukushima) on April 19, were also measured by our spectrometer and compared. Among these samples of rainwater collected at different locations in Japan, the one collected at Kashiwa City, Chiba Prefecture, on March 21 showed the highest activity concentrations of 6072 ± 1,   632 ± 4,   766 ± 3,   637 ± 1,   97.6 ± 0.8, and 752 ± 2 Bq/L for ¹³¹I,   ¹³²I,   ¹³²Te,   ¹³⁴Cs,   ¹³⁶Cs, and ¹³⁷Cs, respectively. The health risks due to these high activity levels were considered in terms of several regulations. The ratio of the activites for the isotopes ¹³¹I to ¹³⁷Cs and ¹³⁴Cs to ¹³⁷Cs were compared with the other measurements and discussed.     

Soil-to-plant transfer of 137Cs and 40K in an Atlantic blanket bog ecosystem

The transfer of ¹³⁷Cs and ⁴⁰K from soil to vegetation was studied in an Atlantic blanket bog ecosystem along the Atlantic coast of Ireland where the dominant vegetation is a mixture of Calluna vulgaris, Eriophorum vaginatum and Sphagnum mosses. The impact of soil chemistry and nutritional status of vegetation on the uptake of both radionuclides was also examined. Cesium-137 transfer factors values ranged from 1.9 to 9.6 and accumulation of ¹³⁷Cs was higher in the leaves of C. vulgaris than in the stems. Transfer factors values for ¹³⁷Cs in both C. vulgaris and E. vaginatum were similar indicating that for the vegetation studied, uptake is not dependent on plant species. The uptake of ¹³⁷Cs in bog vegetation was found to be positively correlated with the nutrient status of vegetation, in particular the secondary nutrients, calcium and magnesium. Potassium-40 transfer factors ranged from 0.9 to 13.8 and uptake was higher in E. vaginatum than in C. vulgaris, however, unlike ¹³⁷Cs, the concentrations of ⁴⁰K within the leaves and stems of C. vulgaris were similar. The concentration of both ¹³⁷Cs and ⁴⁰K found in moss samples were in general lower than those found in vascular plants.     

The study on radioactive contamination in foodstuffs imported from Japan after the Fukushima accident

During the Fukushima nuclear accident, a large number of radionuclides were released, causing direct radioactive contamination to the environment and the ecosystem, and eventually indirect contamination to the foodstuffs. The Radiation Monitoring Group, Office of Atoms for Peace (OAP) in cooperation with the Food and Drug Administration (FDA), has been monitoring the foodstuffs imported from Japan, especially the Fukushima and nearby areas. This monitoring program covered the potentially contaminated foodstuffs. The measurements were mainly conducted using Gamma spectroscopy systems in order to analyze the radioactive concentration of ¹³¹I, ¹³⁴Cs, and ¹³⁷Cs fission products. From 442 samples collected between after the nuclear accident to the end of September 2012, 28 of contaminated food products of fission isotopes have been found with the contamination ranges of 0.63–15.25 Bq/kg fresh, 1.45–44.70 Bq/kg fresh, and 0.45–51.10 Bq/kg fresh) for ¹³¹I, ¹³⁴Cs, and ¹³⁷Cs, respectively. However, the contamination levels are still well under the Thailand standard of food contaminated with radionuclide and the relevant international standards. Finally, the research also investigated the relationship between the times the samples were collected and the contamination levels.     

Radioactivity in the Exclusive Economic Zone of east coast Peninsular Malaysia: distribution trends of <Superscript>137</Superscript>Cs in surface seawater

Large volumes of surface seawater samples were collected from thirty locations in the Exclusive Economic Zone (EEZ) of the east coast Peninsular Malaysia on June 2008 to study the activity concentrations of ¹³⁷Cs. The results will serve as additional information to the existing baseline data and is very useful for monitoring fresh input of anthropogenic radionuclide into Malaysian marine environment. In this study, the activity concentrations of ¹³⁷Cs were determined using co-precipitation technique, followed by Gamma Spectrometry measurement. The mean activity concentration of ¹³⁷Cs ranged between 3.40 and 5.89 Bq/m³. Higher activity concentrations were observed at the coastal and towards the south of Peninsular Malaysia and were aligned with the high turbidity. These may due to the rapid diffusion of ¹³⁷Cs from suspended particulates and fine sediments into surface seawater. The activity concentrations of ¹³⁷Cs observed in this study were slightly higher than the concentrations reported in seawater at the Straits of Malacca, Vietnam and Philippines. This might be because the study area received more input of ¹³⁷Cs that originated from global fallout and then deposited on land which later being transported subsequently into the coastal zone due to siltation and erosion processes. It could also be attributed to the intrusion of river waters containing higher concentrations of ¹³⁷Cs.     

Source term estimation using air concentration measurements during nuclear accident

The focus of this paper is locating and quantifying the diffusion source of ¹³⁷Cs by using observation data collected from monitoring stations. The estimation method is firstly tested in synthetic experiments and then verified with real ¹³⁷Cs concentration data of Fukushima accident. An atmospheric dispersion simulation system is used to support particle diffusion model. Besides, ridge regression is applied to calculate release rate. In terms of location estimation, posterior function of the source location can be deduced according to Bayesian inference. particle swarm optimization (PSO) method is implemented to locate diffusion source.