Uptake and depuration of 131I from labelled diatoms (Skeletonema costatum) to the edible periwinkle (Littorina littorea)

Uptake and depuration of (131)I into winkles through consumption of the diatom Skeletonema costatum is described. The work follows on from previous studies that investigated the uptake of iodine into winkles from seawater and seaweed. Incorporation of (131)I in S. costatum from labelled seawater followed linear first-order kinetics with an uptake half-time of 0.40 days. Iodine uptake in winkles from labelled S. costatum also followed linear first-order kinetics, with a calculated equilibrium concentration (C(infinity)) of 42Bqkg(-1) and a transfer factor (TF) of 1.1x10(-4) with respect to labelled diatom food. This TF is lower than that observed for uptake of (131)I in winkles from labelled seaweed. For the depuration stage, a biphasic sequence with biological half-lives of 1.3 and 255 days was determined. The first phase is biokinetically important, given that winkles can lose two-thirds of their activity during that period. This study shows that, whilst winkles can obtain radioactive iodine from phytoplankton consumption, they do not retain the majority of that activity for very long. Hence, compared with other exposure pathways, such as uptake from seawater and macroalgae, incorporation from phytoplankton is a relatively minor exposure route.     

Uptake and depuration of 131I by the edible periwinkle Littorina littorea: uptake from labelled seaweed (Chondrus crispus)

Uptake and depuration experiments of (131)I from labelled seaweed (Chondrus crispus) by the edible periwinkle Littorina littorea have been performed. Radioiodine concentrations in winkles during uptake followed first-order kinetics with an uptake half-time of 1 day, and a calculated equilibrium concentration (C(infinity)) of 21 000 Bq kg(-1) resulting in a transfer factor of 0.07 with respect to the labelled seaweed used as food. For depuration, a biphasic sequence with biological half-lives of 1 and 24 days was determined. The results suggest that in general, iodine turnover in periwinkles is slower than observed for other molluscs (monophasic biological half-lives in the order of 2-3 days). Both environmental media, food and seawater, can be significant sources of radioiodine for the winkle.     

Experimental studies on the biokinetics of 134Cs and 24Am in mussels (Mytilus galloprovincialis).

The biokinetics of 134Cs and 241Am in mussel species contaminated through water pathway has been studied under laboratory conditions. At equilibrium, the concentration factors for 134Cs and 241Am in small and large mussels were 2.80 and 2.57 and 200 and 150, respectively. The concentration factor of 134Cs in soft parts of the mussels was significantly high than whole body and shell tissue. However, the concentration factors of 241Am in soft parts and shell tissue samples were found to have similar rates. The depuration kinetics of the radionuclides were described by two-component exponential models. The biological half-lives at slow components between small and large mussels did not change significant, and were found to be 46.8-46.5 and 72.2-75.3 days for 134Cs and 241Am. The depuration kinetics of 134Cs and 241Am in soft parts described a single-component exponential model and the biological half-lives were found to be 29.4 and 41.1 days, respectively.     

Chernobyl radionuclides in shellfish

Radionuclides from the Chernobyl accident arrived at Monaco on 30 April, 1986. A sample of Mytilus galloprovincialis collected six days later showed near-maximum levels of most radionuclides. Monitoring continued for seven months thereafter, peak concentrations being transiently as high as 480 Bq kg⁻¹ (all soft parts, wet weight) for ¹⁰³Ru. Other radionuclides detected included ¹³²Te, ^129mTe, ¹³¹I, ¹⁰⁶Ru, ¹³⁴Cs, ¹³⁷Cs, ^110mAg, ¹⁴⁰Ba, ¹²⁵Sb, ⁹⁵Nb and ¹⁴¹Ce. Biological half-lives for elimination in this environment were generally around 10 days or longer and most elimination curves contained a number of components. Radionuclide contents of the mussels were predicted quite accurately from concentrations observed on air filters collected simultaneously, but were not satisfactorily explained relative to total radionuclide concentrations in the seawater even three days after peak air filter activities. The use of concentration factors from the literature did not improve the latter predictions. This suggests that the radionuclides were absorbed very rapidly from the fallout particles, rather than from radionuclides first solubilised from particles. Patella lusitanica specimens contained activities about 20–50 times higher than those in the mussels.     

Studies on the distribution of 210Po and 210Pb in the ecosystem of Point Calimere Coast (Palk Strait), India

A systematic study on the natural radionuclides such as 210Po and 210Pb in the environmental matrices of Point Calimere ecosystem has been undertaken to establish a baseline data on the radiation profile of Point Calimere environment. The environmental samples such as water, sediment and biota (seaweeds, crustaceans, molluscs and fish) have been subjected to analyses. It has been observed that the concentration of 210Po and 210Pb in the water samples of Point Calimere to be 0.5 mBq/l and 1.3 mBq/l, respectively. The soft tissues of the organisms accumulated higher 210Po content while shells and bones contained more 210Pb. The bivalve molluscs Meretrix casta have been identified to accumulate higher concentration of 210Po suggesting that they could serve as bio-indicator of radionuclides like 210Po in the Point Calimere ecosystem. The concentration factor of 210Po for the biotic components ranged from approximately 10(3) to 10(6) while for 210Pb it ranged from approximately 10(3) to 10(5).     

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.     

Bioavailability of sediment-associated and low-molecular-mass species of radionuclides/trace metals to the mussel Mytilus edulis

Sediments can act as a sink for contaminants in effluents from industrial and nuclear installations or when released from dumped waste. However, contaminated sediments may also act as a potential source of radionuclides and trace metals to the water phase due to remobilisation of metals as dissolved species and resuspension of particles. The marine mussel Mytilus edulis is a filter-feeding organism that via the gills is subjected to contaminants in dissolved form and from contaminants associated to suspended particles via the digestive system. In this paper the bioavailability of sediment-associated and seawater diluted Cs, Co, Cd and Zn radioactive tracers to the filtering bivalve M. edulis has been examined. The mussels were exposed to tracers diluted in ultrafiltered (<10 kDa) seawater (Low Molecular Mass form) or to tracers associated with sediment particles from the Stepovogo Fjord at Novaya Zemlya in short-term uptake experiments, followed by 1-month depuration experiments in flow-through tanks. A toxicokinetic model was fitted to the uptake and depuration data, and the obtained parameters were used to simulate the significance of the two uptake pathways at different suspended sediment loads and sediment-seawater distribution coefficients. The results of the model simulations, assuming steady state conditions, suggest that resuspended particles from contaminated sediments can be a highly significant pathway for mussels in the order ¹⁰⁹Cd ≌ ⁶⁵Zn < ¹³⁴Cs < ⁶⁰Co. The significance increases with higher suspended sediment load and with higher K_d. Furthermore, the experimental depuration data suggest that Cs is retained longer and Co, Cd and Zn shorter by the mussels when associated with ingested sediments, than if the metals are taken up from the low molecular mass (LMM) phase.     

Dynamic model for the assessment of radiological exposure to marine biota

A generic approach has been developed to simulate dynamically the uptake and turnover of radionuclides by marine biota. The approach incorporates a three-compartment biokinetic model based on first order linear kinetics, with interchange rates between the organism and its surrounding environment. Model rate constants are deduced as a function of known parameters: biological half-lives of elimination, concentration factors and a sample point of the retention curve, allowing for the representation of multi-component release. The new methodology has been tested and validated in respect of non-dynamic assessment models developed for regulatory purposes. The approach has also been successfully tested against research dynamic models developed to represent the uptake of technetium and radioiodine by lobsters and winkles. Assessments conducted on two realistic test scenarios demonstrated the importance of simulating time-dependency for ecosystems in which environmental levels of radionuclides are not in equilibrium.     

Characterization of ²⁴¹ Am and ¹³⁴Cs bioaccumulation in the king scallop Pecten maximus: investigation via three exposure pathways

In order to understand the bioaccumulation of ²⁴¹Am and ¹³⁴Cs in scallops living in sediments, the uptake and depuration kinetics of these two elements were investigated in the king scallop Pecten maximus exposed via seawater, food, or sediment under laboratory conditions. Generally, ²⁴¹Am accumulation was higher and its retention was stronger than ¹³⁴Cs. This was especially obvious when considering whole animals exposed through seawater with whole-body concentration factors (CF_7d) of 62 vs. 1, absorption efficiencies (A_0l) of 78 vs. 45 for seawater and biological half-lives (T_b½l) of 892 d vs. 22 d for ²⁴¹Am and ¹³⁴Cs, respectively. In contrast, following a single feeding with radiolabelled phytoplankton, the assimilation efficiency (AE) and T_b½l of ¹³⁴Cs were higher than those of ²⁴¹Am (AE: 28% vs. 20%; T_b½l: 14 d vs. 9 d). Among scallop tissues, the shells always contained the higher proportion of the total body burden of ²⁴¹Am whatever the exposure pathway. In contrast, the whole soft parts presented the major fraction of whole-body burden of ¹³⁴Cs, which was generally associated with muscular tissues. Our results showed that the two radionuclides have contrasting behaviors in scallops, in relation to their physico-chemical properties.     

Contamination of terrestrial gastropods, Helix aspersa maxima, with 137Cs, 85Sr, 133Ba and 123mTe by direct, trophic and combined pathways

(137)Cs, (85)Sr, (133)Ba and (123m)Te contaminations of terrestrial gastropods, Helix aspersa maxima, by direct deposition, labelled food ingestion or combined (trophic and direct pathways) exposure were carried out under laboratory conditions. The aim of this study was to compare the three contamination pathways: direct, trophic and combined, in terms of individual mortality, radionuclide uptake, depuration and distribution in the tissues. An initial group of 30 snails (2 years old) was exposed to radioactive aerosols during a 20-h period. These aerosols were assumed to be representative of those that would be released during a nuclear accident occurring in a PWR. A second group of 50 snails (same age) was submitted to an ingestion of commercial food contaminated by the same aerosols, twice a week for 21 days (flour at a feeding rate of about 0.2g). A third group of 40 snails was submitted to a combined exposure: exposure to radioactive aerosols (20h), followed by ingestion of flour contaminated by the same aerosols, twice a week for 21 days. No significant difference between the three groups and a reference group of 10 snails was observed, neither in growth nor in mortality. Concerning the direct pathway, at the end of direct deposition (about 1 day after the beginning), cesium was the most bioavailable element, distributed rather homogeneously throughout the whole body (13% of the total Cs in all organs excepting the digestive system and 28% in the muscle). Strontium was measured in the shell (about 70%). Barium was found in the muscle (20%) and in the shell (65%). Tellurium was mainly present in the shell (70%) and in the digestive system (20%). After 21 days of depuration, the faeces eliminated 42% of the Te. As for contamination by ingestion, Te mainly accumulated in the digestive system (72% of Te present in the total body), Ba accumulated in the muscle (75%) and Sr in the shell (70%). Concerning contamination by combined pathways, at the end of the 21-day exposure, the 4 radionuclides had the same tendency as direct deposition. However, the effect of the trophic pathway was significant: it causes an 18% increase of Sr in the shell and an 7% increase of Cs in the digestive system in comparison to direct deposition, resulting in a final 86% in the shell and 27% in the digestive system.     

127I and 129I/127I isotopic ratio in marine alga Fucus virsoides from the North Adriatic Sea

The only stable iodine isotope is 127I and the natural 129I/127I ratio in the biosphere has increased from 10(-15)-10(-14) to 10(-10)-10(-9), mainly due to emissions from nuclear fuel reprocessing plants. In Europe they are located at La Hague (France) and Sellafield (England), where the ratio of 129I/127I is up to 10(-4). The marine environment, i.e. the oceans, is the major source of iodine with average concentrations of around 60 mirogL(-1) iodine in seawater. Brown algae accumulate iodine at high levels of up to 1.0% of dry weight, and therefore they are an ideal bioindicator for studying the levels of 127I and 129I in the marine environment. A radiochemical neutron activation analysis (RNAA) method, developed at our laboratory, was used for 129I determination in the brown alga Fucus virsoides (Donati) J. Agardh, and the same technique of RNAA was used for total 127I determination. The samples were collected along the coast of the Gulf of Trieste and the West coast of Istria in the North Adriatic Sea in the period from 2005 to 2006. Values of the 129I/127I ratio up to 10(-9) were found, which is in agreement with the present average global distribution of 129I. The levels of stable iodine found were in the range from 235 to 506 microg g(-1) and the levels of 129I from 1.7 to 7.3 x 10(-3)Bq kg(-1) (2.6-10.9 x 10(-7) microg g(-1)), on a dry matter basis.     

Bioaccumulation of 137Cs in pelagic food webs in the Norwegian and Barents Seas

Knowledge and documentation of the levels of radioactive contamination in fish stocks important to Norwegian fisheries is of major importance to Norwegian consumers and fish export industry. In the present study, the bioaccumulation of caesium-137 ((137)Cs) has been investigated in marine food webs in the Barents and Norwegian Seas. The contents of (137)Cs in the different organisms were generally low (<1 Bq kg(-1) wet weight), but a marked bioaccumulation was apparent: The concentration of (137)Cs was about 10-fold higher in the harbour porpoise Phocoena phocoena, representing the upper level of the food web, than in the amphipod Themisto sp., representing the lower level of the food web. The Concentration Factors (CF=Bq kg(-1) wet weight/Bq l(-1) seawater) increased from 10+/-3 for a mixed sample of krill and amphipods to 165+/-5 for harbour porpoises.     

Uptake and distribution of 137Cs and 90Sr in salix viminalis plants

Agricultural areas in middle and northern parts of Sweden were contaminated with radionuclides after the Chernobyl accident in 1986. Alternative crops in these areas are biomass plantations with fast-growing Salix clones for energy purposes. The uptake and internal distribution of 137Cs and 90Sr in Salix viminalis were studied. Plants were grown in microplots under field conditions. The soils in the experimental site had been contaminated in 1961 with 35.7 and 13.4 MBq m(-2) of 137Cs and 90Sr, respectively. The experiment was carried out during three years. The plots were fertilised with 60 kg N ha(-1) and three treatments of K, consisting of 0, 80 and 240 kg K ha(-1) during the first two years. The activity concentration of 137Cs in the different plant parts varied between 140 and 20,000 Bq kg(-1) and was ranked in the following order: lowest in stems < cuttings < leaves < roots. The fine roots (0-1 mm) had the highest 137Cs activity concentration. One-year-old stems had higher 137Cs activity concentrations than two-year-old stems. The activity concentration of 137Cs in the plants was significantly affected by K-supply and was higher in the 0 kg K treatment than in the 80 or 240kg K treatment. Leaves contained more 90Sr than stems and cuttings.     

Radioactive contamination in the marine environment adjacent to the outfall of the radioactive waste treatment plant at ATOMFLOT,northern Russia

RTP "ATOMFLOT" is a civilian nuclear icebreaker base located on the Kola Bay of northwest Russia. The objectives of this study were to determine the distributions of man-made radionuclides in the marine environment adjacent to the base, to explain the form of the distributions in sediments and to derive information concerning the fate of radionuclides discharged from ATOMFLOT. Mean activity concentrations (d.w.) for surface sediment, of 63 Bq kg(-1 137Cs, 5.8 Bq kg(-1) 90Sr and 0.45 Bq kg(-1 239,240)Pu were measured. Filtered seawater activity levels were in the range of 3--6.9 Bq m(-3) 137Cs, 2.0-11.2 Bq m(-3) 90Sr, and 16-40 m Bq m(-3), 239,240Pu. Short-lived radionuclides were present at sediment depths in excess of 10cm indicating a high degree of sediment mixing. Correlations of radionuclide activity concentrations with grain-size appear to be absent; instead, the presence of relatively contaminated sediment appears to be related to the existence of radioactive particles.     

Level and origin of iodine-129 in the Baltic Sea

Environmental samples, such as seawater, seaweed, lake water, lake sediment and grass collected from the Baltic Sea area were analyzed for 129I and 127I by radiochemical neutron activation analysis. In 2000, the concentration of 129I in the seawater from Borholm and M?en in the Baltic Sea has reached 6.0 x 10(-13) and 16 x 10(-13) g/l, respectively, these are more than two orders of magnitude higher than the global fallout level. The highest value of 270 x 10(-13) g/l being found in the seawater from the Kattegat. By comparison of the level of 129I in the lake water and precipitation in this region, it is estimated that more than 95% of 129I in the Baltic Sea originates from reprocessing emissions, especially from the French nuclear fuel reprocessing plant at La Hague. More than 30% of 129I in the south Baltic and 93% in the Kattegat directly originates from the marine discharges of the European reprocessing plants.     

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.     

Iodine uptake by spinach (Spinacia oleracea L.) plants grown in solution culture: effects of iodine species and solution concentrations

A hydroponic experiment was carried out to investigate the effects of iodine species and solution concentrations on iodine uptake by spinach (Spinacia oleracea L.). Five iodine concentrations (0, 1, 10, 50 and 100 microM) for iodate (IO(3)(-)) and iodide (I(-)) were used. Results show that higher concentrations of I(-) (> or =10 microM) had some detrimental effect on plant growth, while IO(3)(-) had little effect on the biomass production of spinach plants. Increases in iodine concentration in the growth solution significantly enhanced I concentrations in plant tissues. The detrimental effect of I(-) on plant growth was probably due to the excessively high accumulation of I in plant tissues. The solution-to-spinach leaf transfer factors (TF(leaf), fresh weight basis) for plants treated with iodide were between 14.2 and 20.7 at different solution concentrations of iodide; TF(leaf) for plants treated with iodate decreased gradually from 23.7 to 2.2 with increasing solution concentrations of iodate. The distribution coefficients (DCs) of I between leaves and roots were constantly higher for plants treated with iodate than those treated with iodide. DCs for plants treated with iodide increased with increasing solution concentrations of iodide, while DCs for plants treated with iodate (around 5.5) were similar across the range of solution concentrations of iodate used in this experiment. The implications of iodine accumulation in leafy vegetables in human iodine nutrition are also discussed.     

The geographic distribution of radionuclide deposition across the continental US from atmospheric nuclear testing

For the first time, calculations for the more than 3000 counties of the US have been completed that estimate the average deposition density (Bq m(-2)) of more than 40 radionuclides in fallout from atmospheric nuclear weapons tests conducted in the US (1951-1962) and 19 radionuclides from tests conducted elsewhere in the world (1952-1963). The geographic pattern of deposition across the US, as well as the amount of fallout deposited, varied significantly depending on whether the tests were conducted within or outside of the US. Fallout deposited from the Nevada Test Site (NTS) varied geographically as a result of dispersion and dilution in the atmosphere, the wind patterns following each test, and the occurrence of localized rainfall events. In general, states immediately east of the NTS received the highest deposition from tests conducted there. In contrast, the variation in deposition across the country from global fallout was less than for NTS fallout primarily reflecting variations in annual precipitation across larger regions. Hence, in the eastern and mid-western US, where rainfall is above the national average, higher levels of global fallout were deposited than in the more arid southwestern states. This paper presents a summary of the methods used and findings of our studies on fallout from NTS and global fallout, with emphasis on two of the most important radionuclides, (131)I and (137)Cs.     

Plutonium concentration and 240Pu/239Pu atomic ratio in liver of squid collected in the coastal sea areas of Japan

Plutonium isotopes, 239Pu and 240Pu, were measured in liver samples from Surume squid using a sector-field high resolution ICP-MS after radiochemical purification. Surume squid samples were obtained from nine landing ports in Japanese inshore during fishery season from September to December 2002. Concentrations of 239Pu and 240Pu ranged from 1.5 to 28 mBq kg(-1) and 1.1 to 24 mBq kg(-1), respectively. Plutonium (239,240Pu) concentrations in liver were several thousand times higher than levels found in seawater. The concentration factor (CF) compared to seawater for 239,240Pu and 13 other elements ranged from 10(0) to 10(7). The CF values for 239,240Pu, V and Th were 10(2)-10(4). Pu had an intermediate CF between conservative and scavenged elements. 240Pu/239Pu atomic ratios in the squid liver ranged from 0.177 to 0.237 which were slightly higher than 0.178+/-0.014 for global fallout. The variations of 240Pu/239Pu atomic ratios in ocean currents with different source functions are important for interpreting high 240Pu/239Pu atomic ratios in Surume squid liver. It seems likely that Pu with high 240Pu/239Pu atomic ratio is continuously transported through the solubilization and seawater transport from the North Equatorial Current to Kuroshio and its branch, Tsushima Current. By assuming that Pu found in Surume squid liver is a mixture of global fallout Pu (0.178) and close-in fallout Pu with high 240Pu/239Pu atomic ratio (0.30-0.36) around Bikini Atoll, Pu contribution from Bikini close-in fallout Pu accounts for close to 35% of the whole plutonium in Surume squid liver. These results highlight that Surume squid is a useful organism for evaluating environmental Pu levels of larger sea area and facilitate the development of models to understand oceanic transport of close-in fallout Pu from Bikini Atoll.     

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.