Arrival time and magnitude of airborne fission products from the Fukushima, Japan, reactor incident as measured in Seattle, WA, USA

We report results of air monitoring started due to the recent natural catastrophe on 11 March 2011 in Japan and the severe ensuing damage to the Fukushima Dai-ichi nuclear reactor complex. On 17-18 March 2011, we registered the first arrival of the airborne fission products ¹³¹I, ¹³²I, ¹³²Te, ¹³⁴Cs, and ¹³⁷Cs in Seattle, WA, USA, by identifying their characteristic gamma rays using a germanium detector. We measured the evolution of the activities over a period of 23 days at the end of which the activities had mostly fallen below our detection limit. The highest detected activity from radionuclides attached to particulate matter amounted to 4.4 ± 1.3 mBq m⁻³ of ¹³¹I on 19-20 March.     

Determination of radioiodine species in rain water collected at Tsukuba near Tokyo

The distribution of radioiodine (¹³¹I) species in rain water collected at Tsukuba in May 1986 was studied using the isotopic exchange method. Organic-soluble forms of radioiodine were not observed. Iodide (I¹⁻) was the predominant species, and the concentration of iodate (I¹O₃⁻) was less than half of I¹⁻. The results were compared with those for ¹³¹I produced by neutron-irradiation of uranyl nitrate.     

Reconstruction of 131I radioactive contamination in Ukraine caused by the Chernobyl accident using atmospheric transport modelling

The evaluation of ¹³¹I air and ground contamination field formation in the territory of Ukraine was made using the model of atmospheric transport LEDI (Lagrangian–Eulerian DIffusion model). The ¹³¹I atmospheric transport over the territory of Ukraine was simulated during the first 12 days after the accident (from 26 April to 7 May 1986) using real aerological information and rain measurement network data. The airborne ¹³¹I concentration and ground deposition fields were calculated as the database for subsequent thyroid dose reconstruction for inhabitants of radioactive contaminated regions. The small-scale deposition field variability is assessed using data of ¹³⁷Cs detailed measurements in the territory of Ukraine. The obtained results are compared with available data of radioiodine daily deposition measurements made at the network of meteorological stations in Ukraine and data of the assessments of ¹³¹I soil contamination obtained from the ¹²⁹I measurements.     

Fallout in the New York metropolitan area following the chernobyl accident

In the metropolitan New York area, maximum concentrations in air of radioactive aerosol and gaseous debris from the Chernobyl accident of April 1986 were much lower than those measured in Europe. The observed maxima were: for gaseous ¹³¹I, 23mBq m⁻³; for aerosol samples, 20mBq m⁻³ of ¹³¹I and 9·mBq m⁻³ of ¹³⁷Cs. The data suggest that little gas-to-particle transformation of iodine occurred during transport of the radioactive cloud from the Ukraine to New York. The ratios of ¹⁰³Ru and other refractories to ¹³⁷Cs were low in the first debris sampled, debris which probably was emitted from Chernobyl in late April during the early stages of the accident. In subsequent samples these ratios were higher, presumably because debris from the later, hotter stages of the fire had reached our sampling sites. A significant fraction (25–40%) of the deposition of ¹³¹I and ¹³⁷Cs into our samplers and on grass was by dry deposition. The total deposition of Chernobyl ¹³⁷Cs in the area was <1% of that already present in the soil from fallout from past nuclear weapon tests. The highest concentration of ¹³¹I measured in fresh milk was about 1.5 B1 liter⁻¹, <0.1% of the US action level. The dose to the thyroid of a six-month-old infant who had fresh milk as a sole food source would be about 70 μGy (7 mrad).     

Fallout distribution in Padua and Northeast Italy after the chernobyl nuclear reactor accident

The radioactive cloud from the Chernobyl nuclear reactor accident arrived in northeast Italy on 30 April 1986. Ground-level air activities detected in Padua reached maximum values of 28·6, 19·2, 3·3, 1·7 and 7·5 Bq m⁻³ for ¹³¹I, ¹³²Te(¹³²I), ¹³⁷Cs and ¹⁰³Ru, respectively, on 1 May; about 10 days later, the activities had fallen to less than 1% of peak values. Considerations of cloud homogeneity are reported.The distribution of fallout radionuclides in Padua was evaluated on the basis of radioactivity detected on natural surfaces. The average committed dose equivalent to the thyroid for adult people in Padua through ¹³¹I inhalation was estimated at 0·37 mSv. Soil activity was monitored daily in samples collected in Padua during the first weeks of May 1986. Fallout deposition over northeast Italy was measured on 75 surface soil samples collected during June 1986 and long-lived radionuclide distribution maps were derived.     

Concentrations of 131I in the urine of Japanese adults and children following the Chernobyl nuclear accident

Iodine-131 in urine samples from 15 Japanese subjects was determined during the period 4 to 29 May 1986. In a male adult, the peak concentration (3.3 Bq dm⁻³) was observed on 9 May, the levels decreasing thereafter to less than the detection limit by 29 May. The highest concentration observed was 7.6 Bq dm⁻³ in a female adult. The urinary concentrations in the 11 adult subjects appeared to correlate with consumption of green leafy vegetables and milk. In four children, 6 to 14 years old, ¹³¹I concentrations in urine were generally higher than those of the adults. The major source of ¹³¹I intake was confirmed to be from vegetables, not milk.     

Inorganic iodine incorporation into soil organic matter: evidence from iodine K-edge X-ray absorption near-edge structure

The transformation of inorganic iodine (I⁻ and IO₃⁻) incubated in soils with varying amounts of organic matter (Andosols from the surface layer of an upland field and forest, as well as Acrisols from surface and subsurface layers of an upland field) was investigated by using the iodine K-edge X-ray absorption near-edge structure (XANES). After 60 d of reaction, both I⁻ and IO₃⁻ were transformed into organoiodine in surface soils containing sufficient amounts of organic matter, whereas IO₃⁻ remained unchanged in the subsurface soil of Acrisols with low organic matter contents. Transformation of IO₃⁻ into organoiodine was not retarded when the microbial activity in soil was reduced by γ-ray irradiation, suggesting that microbial activity was not essential for the transformation of inorganic iodine into organoiodine. Soil organic matter has the ability to transform inorganic iodine into organoiodine.     

Radioactivity in surface air and precipitation in Japan after the Chernobyl accident

Radioactive plumes from the Chernobyl reactor accident first passed over Japan on 3 May 1986. Measurements of ¹⁰³Ru, ¹³¹I and ¹³⁷Cs in rainfall and airborne dust collected at Chiba near Tokyo show that, in fact, at least two or more kinds of plume arrived during May. Their altitudes were calculated to be about 1500 m in early May and 6300 m in late May.Radionuclides detected in 33 precipitation samples collected by the network of prefectural radiation monitoring stations from 1 to 22 May were ⁷Be, ⁸⁹Sr, ⁹⁵Sr, ⁹⁵Zr, ⁹⁵Nb, ¹⁰³Ru, ¹⁰⁶Ru, ^110mAg, ¹²⁵Sb, ^129mTe, ¹³¹I, ¹³²Te, ¹³²I, ¹³⁴Cs, ¹³⁶Cs, ¹³⁷Cs, ¹⁴⁰Ba, ¹⁴⁰La, ¹⁴¹Ce and ¹⁴⁴Ce, the measurements being made using germanium detectors and low-background GM counters after radiochemical separation. The radiation was characterized by higher levels of the volatile nuclides, such as ¹⁰³Ru (in the form of RuO₂), ¹³²Te, ¹³¹I and ¹³⁷Cs, than fallout levels in nuclear weapons testing, and by activity ratios of 0·48 and 14 for, respectively, ¹³⁴Cs/¹³⁷Cs and ⁸⁹Sr/⁹⁰Sr, as on 26 April. The fallout activity was higher in northwestern Japan, the average depositions of ⁹⁰Sr and ¹³⁷Cs in Japan from 1 May (or 30 April) to 22 May being 1·4 Bq m⁻² and 95 Bq m⁻², inventories which are 14 and 550 times higher than the pre-Chernobyl values.     

Chemical characteristics of precipitation and wet deposition of major ions in Liaozhong County of Liaoning Province,Northeast China

The chemical characteristics of precipitation were analyzed based on the chemical composition of principal ionic within acid rain（from February 2007 to January 2008）of Liaozhong Meteorological Station located in Malong Village in Liaozhong County of Northeast China,meteorological conditions on the corresponding period ground,and variation of several air pollutants concentration.The results indicated that:（1）The precipitation average pH value of all samples was4.76;the frequency of acid rain during the observation period was 70.7%;the frequency was 82.8%in summer and autumn.（2）In the chemical composition of precipitation,the primary anions were SO₄^2-and NO₃^-;the primary cations were NH₄⁺and Ca²⁺.（3）All concentration of anions was higher in summer and winter,but relatively low in spring and autumn.This showed that the relationship between regional rainfall acidification and pollution was not significant.（4）Rainwater acidity and nearly floor gaseous pollution concentration were different from each other,and pH and NO_x,CO,NO₂ and O₃concentrations showed significant negative correlation,but was not obvious with SO₂ concentration.However,the pH and alkaline pollutants,such as particulate,was positively correlative.     

Dose assessment for marine biota and humans from discharge of (131)I to the marine environment and uptake by algae in Sydney, Australia

Iodine-131 reaches the marine environment through its excretion to the sewer by nuclear medicine patients followed by discharge through coastal and deepwater outfalls. ¹³¹I has been detected in macroalgae, which bio-accumulate iodine, growing near the coastal outfall of Cronulla sewage treatment plant (STP) since 1995. During this study, ¹³¹I levels in liquid effluent and sludge from three Sydney STPs as well as in macroalgae (Ulva sp. and Ecklonia radiata) growing near their shoreline outfalls were measured. Concentration factors of 176 for Ulva sp. and 526 for E. radiata were derived. Radiation dose rates to marine biota from ¹³¹I discharged to coastal waters calculated using the ERICA dose assessment tool were below the ERICA screening level of 10 μGy/hr. Radiation dose rates to humans from immersion in seawater or consumption of Ulva sp. containing ¹³¹I were three and two orders of magnitude below the IAEA screening level of 10 μSv/year, respectively.     

Tropospheric and stratospheric distributions of radioactive iodine and cesium after the Chernobyl accident

Concentrations of ¹³¹I and ^134,136,137Cs in tropospheric and stratospheric air were determined over Poland during the first three weeks after the Chernobyl accident. Large amounts of activity were found at the higher levels of the troposphere up to 9 km. In the stratosphere, the activities at 15 km were usually about 1 to 6% of ground-level values.     

Evaluation and assessment of 25 years of environmental radioactivity monitoring data at Tarapur (India) nuclear site

The evaluation and assessment of monitoring data generated over a period of 1983-2007 (25 years) of a nuclear facility is presented. Time trends of particulate radioactivity, correlation between ¹³⁷Cs in discharge canal seawater and station discharged activity and correlation of ¹³⁷Cs, ⁶⁰Co, and ¹³¹I in marine species such as sponge and Nerita (gastropod) and corresponding discharged activity are discussed. The concentration of ¹³⁷Cs and ¹³¹I in seawater versus biota are discussed. A good correlation between ¹³⁷Cs in seawater and ¹³⁷Cs in liquid waste discharged was observed (R² = 0.8, p < 0.001). Similarly, correlation was good for Nerita and discharged concentration of ¹³⁷Cs, ¹³¹I and ⁶⁰Co (R² = 0.55-0.73 and p < 0.001). The measurements over the years indicated that there is no accumulation of radionuclides in either the terrestrial or aquatic environments. The mean ¹³⁷Cs decreased from the pre-operational levels: 7.0-3.6 Bq kg⁻¹ in soil, 0.91-0.016 Bq L⁻¹ in milk and 0.28-0.036 Bq kg⁻¹ in vegetation. Similarly, the mean ⁹⁰Sr in these matrixes decreased from 3.9 to 0.26 Bq kg⁻¹; 0.37-0.011 Bq L⁻¹ and 0.34-0.022 Bq kg⁻¹ respectively. Cesium-137 of about 700 μBq m⁻³ was measured in the air filter disks during 1986 and there was a decrease of three orders of magnitude in concentration over the 25 years. The evaluation of environmental data indicated that the radionuclide concentrations and potential impacts, in terms of effective dose to the members of public, have significantly reduced since 1969.     

Medical radioisotopes in the environment – following the pathway from patient to river sediment

Motivated by the detection of ¹³¹I in river sediment in routine long-term surveillance samples, a systematic short-term study of the wastewater treatment chain was planned and conducted. Inflow, effluent and primary sludge were collected on a daily basis during two weeks at a regional wastewater treatment plant. Samples were investigated by gamma spectroscopy. Four medically used isotopes could be identified (¹³¹I and ^99mTc regularly, ¹⁵³Sm and ¹²³I sporadically). The concentration levels coincide well with literature data for ¹³¹I, and with our own long-term data for ¹³¹I and ^99mTc for the same plant. Cosmogenic ⁷Be activity in primary sludge correlated well with rainfall intensity. Surface sediment was sampled at low tide at both shores of the river, up- and downstream of the plant. ¹³¹I was identified in all samples, with a sharp maximum (about 100 Bq kg⁻¹ d.m.) at the discharge point of the plant and lower levels elsewhere, decreasing monotonically in downstream direction. ⁷Be and ¹³⁷Cs showed the same behaviour, but no peak at the discharge point. Predictions from simple equilibrium models for the transport and sedimentation of ¹³¹I show good agreement with the experimental data and suggest that the wastewater treatment plant is the main source for this isotope.     

Transfer of Chernobyl-derived 134Cs, 137Cs, 131I and 103Ru from flowers to honey and pollen

The activity concentrations of ¹³⁷Cs, ¹³⁴Cs, ¹³¹I and ¹⁰³Ru were determined separately in honey and pollen samples collected from a single bee colony during several months after the deposition of Chernobyl fallout. The source of each honey and pollen sample was determined by pollen analysis. Although the activity concentrations in honey and pollen varied with time, the concentrations of ¹³⁷Cs and ¹³⁴Cs were, in general, higher in pollen than in honey. For ¹⁰³Ru and ¹³¹I, these differences were comparatively small. The mean ¹³¹ I/¹³⁷Cs and ¹⁰³Ru/¹³⁷Cs ratios were about one order of magnitude higher in honey than in pollen. The mean ¹³¹I/¹⁰³Ru ratio was about the same for honey and pollen. This observation, in the light of the corresponding nuclide ratios found in the deposition, suggests that ¹³⁷Cs, ¹³⁴Cs, ¹³¹I and ¹⁰³Ru were taken up by the plant leaves and transported to nectar and pollen. The higher activity concentrations of ¹³⁷Cs and ¹³⁴Cs in pollen, relative to honey, indicate that these radionuclides behave analogously to potassium, which is also found in higher quantities in pollen.     

Partition of iodine (¹²⁹I and ¹²⁷I) isotopes in soils and marine sediments

Natural organic matter, such as humic and fulvic acids and humin, plays a key role in determining the fate and mobility of radioiodine in soil and sediments. The radioisotope ¹²⁹I is continuously produced and released from nuclear fuel reprocessing plants, and as a biophilic element, its environmental mobility is strongly linked to organic matter.Due to its long half-life (15.7 million years), ¹²⁹I builds up in the environment and can be traced since the beginning of the nuclear era in reservoirs such as soils and marine sediments. Nevertheless, partition of the isotope between the different types of organic matter in soil and sediment is rarely explored. Here we present a sequential extraction of ¹²⁹I and ¹²⁷I chemical forms encountered in a Danish soil, a soil reference material (IAEA-375), an anoxic marine sediment from Southern Norway and an oxic sediment from the Barents Sea. The different forms of iodine are related to water soluble, exchangeable, carbonates, oxides as well as iodine bound to humic acid, fulvic acid and to humin and minerals. This is the first study to identify ¹²⁹I in humic and fulvic acid and humin. The results show that 30-56% of the total ¹²⁷I and 42-60% of the total ¹²⁹I are associated with organic matter in soil and sediment samples. At a soil/sediment pH below 5.0-5.5, ¹²⁷I and ¹²⁹I in the organic fraction associate primarily with the humic acid while at soil/sediment pH > 6 ¹²⁹I was mostly found to be bound to fulvic acid. Anoxic conditions seem to increase the mobility and availability of iodine compared to oxic, while subaerial conditions (soils) reduces the availability of water soluble fraction compared to subaqueous (marine) conditions.     

The comparison of generic model predictions with chernobyl fallout data on the transfer of radioiodine over the air-pasture-cow-milk pathway

Data have been collected on concentrations of ¹³¹I in air, vegetation and milk from numerous locations receiving Chernobyl fallout. Time-integrated concentrations derived from these data are used to compare predictions from generic models used for routine environmental radiological assessments. In general, the models markedly overestimated the transfer of ¹³¹I over the air-grass-cow-milk pathway. The reasons for this overestimate appear to be related to a combination of different factors, among which overestimation of the dry deposition velocity assumed for elemental ¹³¹I, overestimation of the interception and retention of wet-deposited ¹³¹I by pasture vegetation and overestimation of the cow's diet-to-milk transfer coefficient appear to be most important. The low transfer of Chernobyl ¹³¹I from air to milk indicates that the direct inhalation of contaminated air by humans may be more important in determining the ¹³¹I exposure to large populations than the consumption of contaminated cow's milk. Radiological assessments conducted prior to the Chernobyl accident have typically assumed that ¹³¹I exposure would be dominated by the consumption of milk. The consumption of milk, however, is still of dominant importance for the exposure of critical population subgroups composed of infants and small children.     

Use of 129I and 137Cs in soils for the estimation of 131I deposition in Belarus as a result of the Chernobyl accident

Using radioactivity measurements for 131I and 137Cs and nuclear activation analysis (NAA) or accelerator mass spectrometry (AMS) for 129I, ratios of 131I/137Cs and 129I/137Cs have been determined in soils from Belarus. We find that the pre-Chernobyl ratio of 129I/137Cs in Belarus is significantly larger than expected from nuclear weapons fallout. For the Chernobyl accident, our results support the hypothesis that there was relatively little fractionation of iodine and caesium during migration and deposition of the radioactive cloud. For sites having 137Cs > 300 Bq/kg, 129I can potentially give more reliable retroactive estimates of Chernobyl 131I deposition. However, our results suggest that 137Cs can also give reasonably good (+/-50%) estimates for 131I in Belarus.     

Transport of 131I through the grass-cow-milk pathway at a northeast US dairy following the chernobyl accident

Following the Chernobyl accident, samples of pasture grass and fresh farm milk were collected in northern New Jersey. The time-integrated activities of ¹³¹I were used to calculate a milk transfer coefficient of 0·001 d liter⁻¹. This value is at the lower range of those previously reported. No significant difference in the value of the transfer coefficient was seen when calculated based on the integrated ¹³¹I in the total grass as compared to only the upper portion of the grass. Therefore, for this event, the height of the vegetation grazed by the cows would not have influenced the concentration of ¹³¹I in fresh milk.     

Evidence of the radioactive fallout in the center of Asia (Russia) following the Fukushima Nuclear Accident

It was recently reported that radioactive fallout due to the Fukushima Nuclear Accident was detected in environmental samples collected in the USA and Greece, which are very far away from Japan. In April-May 2011, fallout radionuclides (¹³⁴Cs, ¹³⁷Cs, ¹³¹I) released in the Fukushima Nuclear Accident were detected in environmental samples at the city of Krasnoyarsk (Russia), situated in the center of Asia. Similar maximum levels of ¹³¹I and ¹³⁷Cs/¹³⁴Cs and ¹³¹I/¹³⁷Cs ratios in water samples collected in Russia and Greece suggest the high-velocity movement of the radioactive contamination from the Fukushima Nuclear Accident and the global effects of this accident, similar to those caused by the Chernobyl accident.     

Validation of I ecological transfer models and thyroid dose assessments using Chernobyl fallout data from the Plavsk district, Russia

Within the project “Environmental Modelling for Radiation Safety” (EMRAS) organized by the IAEA in 2003 experimental data of ¹³¹I measurements following the Chernobyl accident in the Plavsk district of Tula region, Russia were used to validate the calculations of some radioecological transfer models. Nine models participated in the inter-comparison. Levels of ¹³⁷Cs soil contamination in all the settlements and ¹³¹I/¹³⁷Cs isotopic ratios in the depositions in some locations were used as the main input information. 370 measurements of ¹³¹I content in thyroid of townspeople and villagers, and 90 measurements of ¹³¹I concentration in milk were used for validation of the model predictions.A remarkable improvement in models performance comparing with previous inter-comparison exercise was demonstrated. Predictions of the various models were within a factor of three relative to the observations, discrepancies between the estimates of average doses to thyroid produced by most participant not exceeded a factor of ten.