Experimental investigation and modelling of tritium washout by precipitation in the area of the nuclear power plant of Paks, Hungary

Tritium occurs in nature in trace amounts, but its concentration is changing due to natural and artificial sources. Studies focusing on natural tritium have to take into account the effect of artificial sources. Also, the impact of tritium is an important issue in environmental protection, e.g. in connection with the emissions from nuclear power plants. The present work focuses on the rain washout of tritium emitted from the Paks nuclear power plant in Hungary. Rainwater collectors were placed around the plant and after a period of precipitation, rainwater was collected and analysed for tritium content. Samples were analysed using low-level liquid scintillation counting, with some also subject to the more accurate ³He ingrowth method. The results clearly show the trace of the tritium plume emitted from the plant; however, values are only about one order of magnitude higher than environmental background levels. A washout model was devised to estimate the distribution of tritium around the plant. The model gives slightly higher concentrations than those measured in the field, but in general the agreement is satisfactory. The modelled values demonstrate that the effect of the plant on rainwater tritium levels is negligible over a distance of some kilometres.     

Studies of 131I, 137Cs and 103Ru in milk,meat and vegetables in North East Scotland following the Chernobyl accident

Uptake and clearance of radionuclides in foodstuffs have been studied in the neighbourhood of Aberdeen in North East Scotland following the Chernobyl accident. The level of¹³¹ I in goats' milk was 100–200 Bq litre⁻¹ in early May and declined with an effective half-life of 4sd3 days, but that in cows' milk was only a few Bq litre⁻¹ as most cattle were kept indoors. ¹³⁷Cs and ¹⁰³Ru activities in broccoli declined with effective half-lives of 11 and 6 days respectectively, while ¹³⁷Cs in grass decresed with a half-life of 22 days, the reduction appearing to show a relationship to weekly rainfall. Studies of tissues from groups of lambs initially grazed on contaminated pasture and later (a) fed indoors on concentrates or (b) continuing to graze outdoors, showed the ¹³⁷Cs concentrations to decline with half-lives of (a) 17 days and (b) 25 days, while the half-lives describing the reduction in total ¹³⁷Cs activity were (a) 20 days and (b) 35 days.     

Experimental studies of the transfer of neptunium from sea water to sediments and organisms (annelids and molluscs)

This paper deals with the physico-chemical behaviour of neptunium in sea water and with its capacity for transfer to coastal or deep-sea sediments and for uptake by two benthic species, Arenicola marina (L.) and Cerastoderma edule (L.). We used the ²³⁹Np isotope with mass concentrations in sea water of about 2·5 × 10⁻¹⁰−5·4×10⁻¹² g litre⁻¹, which are close to the concentrations observed in the environment for ²³⁷Np. The experimental results show that Np occurs in solution mainly as the neptunyl ion NpO₂⁺, but soluble anionic and neutral complexes and particulate forms were also detected. The distribution coefficients for the sediments varied from 350 to 6500. The carbonate phase plays a decisive role in neptunium transfer but other fixation processes are also possible. Concentration factors after 13 days were found to have values of 40 and 14 for the shells and soft parts of cockles, respectively, while polychaetes had a concentration factor of 2. Thus Np has a smaller probability of transfer to sediments and organisms than have plutonium and americium.     

Tritium concentrations in the atmospheric environment at Rokkasho, Japan before the final testing of the spent nuclear fuel reprocessing plant

This study aimed at obtaining background tritium concentrations in precipitation and air at Rokkasho where the first commercial spent nuclear fuel reprocessing plant in Japan has been under construction. Tritium concentration in monthly precipitation during fiscal years 2001-2005 had a seasonal variation pattern which was high in spring and low in summer. The tritium concentration was higher than that observed at Chiba City as a whole. The seasonal peak concentration at Rokkasho was generally higher than that at Chiba City, while the baseline concentrations of both were similar. The reason for the difference may be the effect of air mass from the Asian continent which is considered to have high tritium concentration. Atmospheric tritium was operationally separated into HTO, HT and hydrocarbon (CH₃T) fractions, and the samples collected every 3 d-14 d during fiscal year 2005 were analyzed for these fractions. The HTO concentration as radioactivity in water correlated well with that in the precipitation samples. The HT concentration was the highest among the chemical forms analyzed, followed by the HTO and CH₃T concentrations. The HT and CH₃T concentrations did not have clear seasonal variation patterns. The HT concentration followed the decline previously reported by Mason and Östlund with an apparent half-life of 4.8 y. The apparent and environmental half-lives of CH₃T were estimated as 9.2 y and 36.5 y, respectively, by combining the present data with literature data. The Intergovernmental Panel on Climate Change used the atmospheric lifetime of 12 y for CH₄ to estimate global warming in its 2007 report. The longer environmental half-life of CH₃T suggested its supply from other sources than past nuclear weapon testing in the atmosphere.     

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).     

Radionuclide contamination of sediment deposits in the Ob and Yenisey estuaries and areas of the Kara Sea

The Ob and Yenisey rivers are major contributors to total riverine discharge to the Arctic Ocean. Several large nuclear facilities discharge into these rivers, which could affect actual and potential discharges of radionuclides to the Arctic region. This article presents new radionuclide concentration and grain-size data resulting from analyses of several sediment samples collected during research cruises in the Ob and Yenisey estuaries and adjacent areas during 2000 and 2001. Results indicate that discharges from the main nuclear facilities do not constitute a major contribution to the level of radioactive contamination in the marine areas studied, though Co-60 was detected at low concentrations in some sediment horizons. However, the aggregate contamination from different sources is not radioecologically significant in sediments within the study area, maximum Cs-137 levels being approximately 80 Bq kg(-1) dry weight.     

Environmental tritium (³H) and hydrochemical investigations to evaluate groundwater in Varahi and Markandeya river basins, Karnataka, India

The present study aimed at assessing the activity of natural radionuclides (³H) and hydrochemical parameters (viz., pH, EC, F⁻, NO₃⁻, Cl⁻, Ca²⁺, Mg²⁺) in the groundwater used for domestic and irrigation purposes in the Varahi and Markandeya river basins to understand the levels of hydrochemical parameters in terms of the relative age(s) of the groundwater contained within the study area. The recorded environmental ³H content in Varahi and Markandeya river basins varied from 1.95 ± 0.25 T.U. to 11.35 ± 0.44 T.U. and 1.49 ± 0.75 T.U. to 9.17 ± 1.13 T.U. respectively. Majority of the samples in Varahi (93.34%) and Markandeya (93.75%) river basins being pre-modern water with modern recharge, significantly influenced by precipitation and river inflowing/sea water intrusion. The EC-Tritium and Tritium-Fluoride plots confirmed the existence of higher total dissolved solids (SEC > 500 μS/cm) and high fluoride (MAC > 1.5 mg/L) in groundwater of Markandeya river basin, attributed to relatively longer residence time of groundwater interacting with rock formations and vice versa in case of Varahi river basin. The tritium-EC and tritium-chloride plots indicated shallow and deep circulating groundwater types in Markandeya river basin and only shallow circulating groundwater type in Varahi river basin. Increasing Mg relative to Ca with decreasing tritium indicated the influence of incongruent dissolution of a dolomite phase. The samples with high nitrate (MAC > 45 mg/L) are waters that are actually mixtures of fresh water (containing very high nitrate, possibly from agricultural fertilizers) and older ‘unpolluted’ waters (containing low nitrate levels), strongly influenced by surface source.     

Environmental radioactivity around tokai-works after the reactor accident at chernobyl

Following the reactor accident at Chernobyl, environmental samples of air, rain water and agricultural and marine products were collected and analyzed by gamma- and alpha-spectrometry. The highest concentrations of ¹³¹I in the environmental samples were as follows: 1·0×⁻¹ Bqm⁻³ (aerosol-associated in air); 3·0×10⁻¹ Bqm⁻³ (gaseous in air); 2·1×10² bq kg⁻¹ (plants); 1·4×10¹ Bq litre⁻¹ (milk). Other nuclides such as ⁹⁵Zr, ⁹⁵Nb, ¹⁰³Ru, ¹⁰⁶Ru, ¹²⁵Sb, ^129mTe, ¹³²I/¹³²Te, ¹³⁴Cs, ¹³⁷Cs, ¹⁴⁰Ba/¹⁴⁰La, ¹⁴¹Ce and ¹⁴⁴Ce were also observed in various environmental samples. ^110mAg was only detected in marine products such as cephalopoda and shellfish, ^239,240Pu and ²⁴¹Am originating from the accident were not identified.Based on the monitoring results at one dairy farm, we have derived an equation to model the transport of ¹³¹I from pasture grass to milk. This equation was then applied to the data from two other farms around Tokai-Works and the calculated ¹³¹I activities in milk were compared with those measured. The equation shows good predictive capabilities for quantification of the peak concentrations of ¹³¹I in milk but underestimates longer-term activities.     

Plutonium in sheep faeces as an indicator of deposition on vegetation

In order to study the deposition on vegetation of plutonium arising from the testing of nuclear weapons and discharges from nuclear facilities, sheep faeces were collected from the South-west and North of England. The plutonium content of faeces has been shown to be a reproducible and sensitive indicator of deposition on herbage and, with this technique, plutonium discharged from the Sellafield Works of British Nuclear Fuels LImited can be detected 60 km from the site. On moorland pastures the concentration of ^239+240Pu in faeces, expressed as activity per gram of ash, is roughly equal numerically to the deposit of plutonium on 1 m² of vegetation.Some of the plutonium ingested by a grazing sheep is absorbed and the highest concentrations are found in liver. The liver of a sheep grazing on pasture where the ^239+240Pu concentration in faeces was about 2 pCi (74 mBq) g⁻¹ of ash, was found to contain <1% of the Generalised Derived Limit for mutton and offal, and the meat <0·001%.     

Biotic, temporal and spatial variability of tritium concentrations in transpirate samples collected in the vicinity of a near-surface low-level nuclear waste disposal site and nearby research reactor

The results of a 21 month sampling program measuring tritium in tree transpirate with respect to local sources are reported. The aim was to assess the potential of tree transpirate to indicate the presence of sub-surface seepage plumes.Transpirate gathered from trees near low-level nuclear waste disposal trenches contained activity concentrations of ³H that were significantly higher (up to ∼700 Bq L⁻¹) than local background levels (0-10 Bq L⁻¹). The effects of the waste source declined rapidly with distance to be at background levels within 10s of metres. A research reactor 1.6 km south of the site contributed significant (p < 0.01) local fallout ³H but its influence did not reach as far as the disposal trenches.The elevated ³H levels in transpirate were, however, substantially lower than groundwater concentrations measured across the site (ranging from 0 to 91% with a median of 2%). Temporal patterns of tree transpirate ³H, together with local meteorological observations, indicate that soil water within the active root zones comprised a mixture of seepage and rainfall infiltration. The degree of mixing was variable given that the soil water activity concentrations were heterogeneous at a scale equivalent to the effective rooting volume of the trees. In addition, water taken up by roots was not well mixed within the trees. Based on correlation modelling, net rainfall less evaporation (a surrogate for infiltration) over a period of from 2 to 3 weeks prior to sampling seems to be the optimum predictor of transpirate ³H variability for any sampled tree at this site.The results demonstrate successful use of ³H in transpirate from trees to indicate the presence and general extent of sub-surface contamination at a low-level nuclear waste site.     

Survey of gross beta radioactivity in surface waters of the Midland,Michigan area (lake Huron and the Chippewa,Pine, and Tittabawassee rivers)

Measurements of Lake Huron water as supplied to the Midland location of the Dow Chemical Company over the period 1970–1981 show that a mean concentration of ≈ 3 pCi/L gross beta activity held relatively constant with a range of yearly mean values from 2 to 4 pCi/L and a range of individual values from 1 to 7 pCi/L. This is comparable to observed values for other Great Lakes' waterways reported in the litarature. There was no apparent seasonal fluctuation. Midland area river water for 1967–1981 show median values of 3 to 4 pCi/L and a range of 2 to 11 pCi/L, comparable to those reported in the literature from througout the United States. The observed activity concentrations in the water are well below the limits of the EPA drinking water standards.     

Scavenging of 234Th in the Eastern Irish Sea

Measurements of the disequilibria of ²³⁴Th/²³⁸U in seawater and in suspended particulate and seabed sediment in the eastern Irish Sea reveal that the residence time of dissolved ²³⁴Th (0·5–7·7 days) is controlled by the concentration of particles in suspension (0·4–6·9 mg litre⁻¹, which reflects the rate of sediment resuspension (0·5–5·9 kg m⁻²y⁻¹). The residence time of ²³⁴Th with respect to removal to the seabed is longer (7–50 d) and is less dependent on variations in the suspended load. Anthropogenic sources of ²³⁸U contribute up to 8–15% of the water column production of ²³⁴Th. Enhanced scavenging occurs near the coast and there appears to be a net horizontal flux of ²³⁴Th within this region.     

Taxonomy of groundwater quality using multivariate and spatial analyses in the Tuticorin District,Tamil Nadu,India

A holistic appraisal of the quality of groundwater from the Tuticorin District has been conducted using multivariate statistical and spatial analyses. The objectives of the study were to delineate the spatial and temporal variabilities in groundwater quality and to understand its suitability for human uses. A total of 100 groundwater samples were collected and analyzed for major cations and anions during pre-monsoon and post-monsoon. Water quality index rating was calculated to quantify overall water quality for human consumption. The PRM samples exhibit poor quality in greater percentage when compared with POM due to the dilution after rainfall. Correlation, factor analysis, and plot of the factor scores reflect the seawater intrusion and weathering process. The mineral stability diagrams indicated that the groundwater is in equilibrium with kaolinite and Ca-montmorillonite, whereas Gibbs plot showed that the chemical composition of groundwater in both districts is controlled by the natural weathering processes irrespective of seasons. The major water type identified in this study is the Ca²⁺–Mg²⁺–HCO₃ ^? type, which degrades into predominantly Na⁺–Cl^?–SO₄ ^2? more saline groundwater toward the coast.     

Radioactivity in asbestos

²²⁶Ra has been measured in five asbestos group minerals. The activity levels are variable, are consistent with other forms of rock and range from 0.01–0.4 pCi ²²⁶Ra/g. Alpha particles from asbestos fibers immobilized in the lower lung near pleural surfaces and in the upper lung on bronchial surfaces may be implicated in initiating mesothelioma and bronchial carcinoma.     

A follow up of the decrease of non exchangeable organically bound tritium levels in the surroundings of a nuclear research center

In the past decades limited amounts of tritium were handled on the CEA site of Bruyères le Châtel with authorised atmospheric releases. A small fraction of the tritium released entered into environmental samples under three forms: (i) as part of free water (TFWT - Tissue Free Water Tritium), or associated with organic matter in two ways; either (ii) bound to the oxygen and nitrogen atoms of the material as exchangeable organically bound tritium (E-OBT), or (iii) bound to carbon atoms as non exchangeable organically bound tritium (NE-OBT). The first two components provide only a picture of atmospheric tritium concentrations at the sampling time as they are in equilibrium with atmospheric moisture and soil humidity. Unlike these exchangeable forms, however, NE-OBT is tightly bound to the organic matter and provides an integrated record of atmospheric tritium during the growing phase of the vegetation. We mapped NE-OBT in tree leaf samples in an area of about 25 × 30 km² around the centre of the CEA site and compared the results with those obtained during a previous sampling exercise in 1989. At this time, the activity levels were almost ten times higher than those observed presently in a similar area almost 20 years later which is consistent with the decrease of atmospheric releases issued from the centre. As the activity levels are now close to environmental background specific attention was also paid to the analytical procedure to ensure reliable low level NE-OBT detection.     

First report of pyrethroid bioaccumulation in wild river fish: A case study in Iberian river basins (Spain)

For the first time, this work described pyrethroid bioaccumulation in edible river fish samples. We analyzed 42 whole fish samples collected in 4 different Iberian rivers. All samples were positive to these insecticides. Levels of concentration ranged from 12 to 4938 ng g^− 1 lipid weight (lw). Moreover, isomeric characterization was carried out. Our results remarked a general preference of cis isomers in bioaccumulation. Finally, the enantiomeric evaluation showed that there was an enantioselective bioaccumulation of some pyrethroids, depending on the studied species. Pyrethroid concentrations were compared with levels obtained for other common pollutants, such as flame retardants, personal care products, hormones and pharmaceuticals. The highest values corresponded to pyrethroid insecticides, even though, pyrethroid levels are safe for human consumption taken into account the current regulations.     

Study of the comparative dynamics of the incorporation of tissue free-water tritium (TFWT) in bulrushes (Typha latifolia) and carp (Cyprinus carpio) in the Almaraz nuclear power plant cooling reservoir

The Almaraz nuclear power plant (Spain) uses the water of Arrocampo reservoir for cooling, and consequently raises the radioactive levels of the aquatic ecosystem of this reservoir. From July 2002 to June 2005, monthly samples of surface water, bulrushes (Typha latifolia) and carp (Cyprinus carpio) were collected from this reservoir. They were analyzed to determine the temporal evolution of the levels of ³H in surface water and of its transfer from the surface water to free-water in the tissues (TFWT) of the aforementioned two organisms. The tritium levels in the surface water oscillate with a biannual period, with their values in the study period ranging between 53 and 433 Bq/L. The incorporation of tritium to bulrushes and carp was fairly similar, the respective mean concentration factors being 0.74 and 0.8 (unitless, as Bq/L tissue water per Bq/L reservoir water). The temporal evolution of the levels fairly closely followed that observed for the surface water tritium, although detailed analysis showed the dominant periodicity for the bulrushes to be annual. This difference reflects the influence on the incorporation of tritium to bulrushes of diverse environmental and metabolic factors, especially evapotranspiration and the seasonal growth of this plant.     

Activity concentrations of 226Ra, 228Ra, 210Pb, 40K and 7Be and their temporal variations in surface air

Activity concentrations of the long-lived natural radionuclides ²²⁶Ra, ²²⁸Ra, ²¹⁰Pb, ⁴⁰K and of ⁷Be in surface air were measured twice monthly at a semi-rural location 10 km north of Munich (FRG) for at least three years. For the time interval 1983–1985, all values were found to be distributed log-normally, with geometric means (in μBq m⁻³) of 1·2 for ²²⁶Ra, 0·5 for ²²⁸Ra, 580 for ²¹⁰Pb, 12 for ⁴⁰K and 3500 for ⁷Be. Reflecting their common origin, the activity concentrations of ²²⁶Ra and ⁴⁰K are correlated with surface air dust concentrations (geometric mean 59 μg m⁻³). Seasonal variations of ²¹⁰Pb and ⁷Be air activity concentrations are established for the time interval 1978–1985.The contribution of local soil activity to the air activity concentrations of these radionuclides and of natural uranium is discussed. Resuspension factors are found to be of the order of 10⁻⁹m⁻¹.     

Assessing field-scale migration of radionuclides at the Nevada Test Site: “mobile” species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides (³H, ¹⁴C, ³⁶Cl, ⁹⁹Tc and ¹²⁹I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and ³⁶Cl showed little evidence of retardation, while the transport of ¹⁴C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially ⁹⁹Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of ¹²⁹I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some “mobile” radionuclides (especially ⁹⁹Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

Priority and emerging flame retardants in rivers: Occurrence in water and sediment,Daphnia magna toxicity and risk assessment

The occurrence, partitioning and risk of eight polybrominated diphenyl ethers (PBDEs), nine new brominated (NBFRs) and ten organophosphorus flame retardants (OPFRs) were evaluated in three Spanish rivers suffering different anthropogenic pressures (Nalón, Arga and Besòs). OPFRs were ubiquitous contaminants in water (ΣOPFRs ranging from 0.0076 to 7.2 μg L^− 1) and sediments (ΣOPFRs ranging 3.8 to 824 μg kg^− 1). Brominated flame retardants were not detected in waters, whereas ΣPBDEs ranged from 88 to 812 μg kg^− 1 and decabromodiphenyl ethane (DBDPE) reached 435 μg kg^− 1 in sediments from the River Besòs, the most impacted river. The occurrence of flame retardants in river water and sediment was clearly associated with human activities, since the highest levels occurred near urban and industrial zones and after wastewater treatment plants discharge. Daphnia magna toxicity was carried out for OPFRs, the most ubiquitous flame retardants, considering individual compounds and mixtures. Toxicity of nine tested OPFRs differed largely among compounds, with EC₅₀ values ranging over three magnitude orders (0.31–381 mg L^− 1). Results evidenced that these compounds act by non-polar narcosis, since their toxicity was proportional to their lipophilicity (K_ow). Furthermore, their joint toxicity was additive, which means that single and joint toxicity can be predicted knowing their concentration levels in water using quantitative structure activity relationships (QSARs) and predictive mixture models. Based on these results, a risk assessment considering joint effect was performed calculating and summing risk quotients (RQs) for the water and sediment samples. No significant risk to D. magna (ΣRQs < 1) was observed for any of the monitored rivers.