Trace metal partitioning in Thalassia testudinum and sediments in the Lower Laguna Madre, Texas

Seagrass communities dominate the Laguna Madre, which accounts for 25% of the coastal region of Texas. Seagrasses are essential to the health of the Laguna Madre (LM) and have experienced an overall decline in coverage in the Lower Laguna Madre (LLM) since 1967. Little is known on the existing environmental status of the LLM. This study focuses on the trace metal chemistry of four micronutrient metals, Fe, Mn, Cu, and Zn, and two non-essential metals, Pb and As, in the globally important seagrass Thalassia testudinum. Seasonal trends show that concentrations of most essential trace metals increase in the tissue during the summer months. With the exception of (1) Cu in the vertical shoot and root, and (2) Mn in the roots, no significant positive correlation exists between the rhizosphere sediment and T. testudinum tissue. Iron indicates a negative correlation between the morphological units and the rhizosphere sediments. No other significant relationship was found between the sediments and the T. testudinum tissue. Mn was enriched up to 10-fold in the leaf tissue relative to the other morphological units and also enriched relative to the rhizosphere sediments. Both Cu and Mn appear to be enriched in leaf tissue compared to other morphological units and also enriched relative to the Cu and Mn in the rhizoshpere sediments. Sediments cores taken in barren areas were slightly elevated in Zn relative to the rhizosphere sediments, whereas no other metals showed statistical differences between barren sediment cores and rhizosphere sediments. However, no correlation was measured in T. testudinum tissue and Zn in rhizosphere sediments. Previous studies suggested that Fe/Mn ratios could indicate differences between seagrass environments. Our results indicate that there is an influence from the Rio Grande in the Fe/Mn signature in sediments, and that ratio is not reflected in the T. testudinum tissue. The results from this study show that the LLM contains trace metal concentrations less than or equal to values for uncontaminated locations worldwide. In addition, there appears to be a complex partitioning in the trace metals in the morphological units of T. testudinum tissue and that analysis only of the leaf may not be indicative of the trace metal levels in this important seagrass species.     

Modelling radiocaesium transfer and long-term changes in reindeer

A dynamic model on (137)Cs in reindeer is presented, taking into consideration short- and long-term mechanisms, including the effect of ground deposition, transfer to vegetation, reindeer diet, feed intake, absorption and depletion of radiocaesium in the reindeer body. The model was optimised to fit measured activity concentrations in Swedish reindeer after the Chernobyl fallout. For comparison, regression analyses were made and aggregated transfer factors and effective ecological half-lives were estimated. The fit of the simulated model to observed activity concentrations was slightly better than the fit obtained by linear regressions. Improved knowledge about radiocaesium in vegetation would make the model more accurate for predictive purposes. Presently, the use of Tag and T(eff) is probably better for predictions, provided that their temporal and geographical limitations are taken into consideration. The dynamic model describes mechanisms better and may explain how changes in the system influence on activity concentrations of radiocaesium in the animal.     

Modelling the long-term dynamics of radiocaesium in closed lakes

During the years after the Chernobyl accident the radioceasium activity concentration in most contaminated aquatic ecosystems decreased markedly. Lakes with no permanent inflows and outflows (closed lakes), however, still present a radioecological problem which is expected to continue for some time. In this paper, a mechanistic model for the long-term prediction of radiocaesium behaviour in closed lakes is developed. The model of Prokhorov (Radiokhimiya (Radiochemistry) 11 (1969) 317) was modified to describe the effects of bottom sediment bioturbation, surface runoff from the catchment and suspended solids formation and sedimentation. The model input parameters are the effective diffusion coefficient in bottom sediments, depth of the completely mixed layer, the distribution coefficient in the sediment-water system, the runoff coefficient, sedimentation rate, and deposition density. Values of all these parameters can be independently estimated or measured in a short-term experiment. Given negligible runoff and sedimentation, the dynamics of radiocaesium in lake water is described by a simple equation with only one unknown parameter. This allows us to make long-term predictions on the basis of a series of measurements carried out during the relatively short period. The model was tested against 137Cs activity concentrations measured between 1993 and 1999 in Svyatoe lake in the Bryansk region of Russia. Calculated and measured activity concentrations are in good agreement.     

Application of radiometric analysis in the study of provenance and transport processes of Brazilian coastal sediments

Natural gamma radiation of beach sand deposits was measured along the south coast of Rio de Janeiro State, Brazil, with the aim of studying the provenance and transport processes of sediments in this area. Concentrations of thorium, uranium and potassium were evaluated using γ-ray spectrometry and a behavioral study of eTh/eU and eTh/K cross plots was performed, reflecting the mineralogical properties of beach sands, as well as their history of transport and sorting processes. The results show that such technique can be efficiently used to map heavy mineral distributions and to distinguish the different origins of coastal sediments disclosing the influence of nearby rivers.     

The influence of clay mineralogy on the mobility of radiocaesium in upland soils of NW Italy

137Cs extraction experiments were performed on 14 contaminated soils from NW Italy with different characteristics and mineralogical composition. Solutions of HCl (pH = 0.5) and buffered EDTA/ammonium acetate (Lakanen solution) were used to assess bioavailability. The results show that less than 2% of 137Cs is available for leaching and/or root uptake. Even within a complex natural system it was possible to identify the amount of swelling clays (vermiculite + smectite) as the main control on Cs mobility under acidic conditions. The ammonium ion appears to be effective in desorbing Cs and its role is briefly discussed in terms of crystal chemistry. The relevance of mineralogy in assessing soil vulnerability is underlined.     

Distribution of 90Sr in coastal seawater, sediments and organisms off two atomic power stations in Korea

We have measured 90Sr activities in the marine environment (seawater, sediments and organisms) off the two Korean atomic power stations at Gori and Weolseong. The marine sampling sites were chosen in the vicinity of the power stations to investigate the dispersion of any local 90Sr sources. The 90Sr activities in seawater ranged from 1.3 to 1.9 mBq/l (mean: 1.4, n = 16) and 0.9 to 1.5 mBq/l (mean: 1.3, n = 29) at the Gori and Weolseong sites, respectively. These activities are comparable with those reported for the remote open ocean, suggesting that the 90Sr at these sites originated primarily from global fallout, which occurred during the 1960s, rather than from any local sources. The 90Sr activities in marine sediments ranged from 116 to 1,277 mBq/kg (mean: 565, n = 12) and from 304 to 1,799 mBq/kg (mean 933, n = 6) at the Gori and Weolseong sites, respectively. The horizontal distribution of 90Sr in surface sediments appears to be affected by grain size as well as local sedimentation rate. The enrichment of 90Sr in fish (5.5 +/- 2.6 mBq/kg, n = 5) and shellfish (7.1 +/- 1.2 mBq/kg, n = 2) was much lower than that in seaweed (57 +/- 33 mBq/kg, n = 5).     

Evaluating and reducing a model of radiocaesium soil-plant uptake

An existing model of radiocaesium transfer to grasses was extended to include wheat and barley and parameterised using data from a wide range of soils and contact times. The model structure was revised and evaluated using a subset of the available data which was not used for model parameterisation. The resulting model was then used as a basis for systematic model reduction to test the utility of the model components. This analysis suggested that the use of 4 model variables (relating to radiocaesium adsorption on organic matter and the pH sensitivity of soil solution potassium concentration) and 1 model input (pH) are not required. The results of this analysis were used to develop a reduced model which was further evaluated in terms of comparisons to observations. The reduced model had an improved empirical performance and fewer adjustable parameters and soil characteristic inputs.     

The true distribution and accumulation of radiocaesium in stem of Scots pine (Pinus sylvestris L.)

The radial and vertical distributions of radiocaesium, potassium and calcium were determined in two Scots pine stands (17 and 58 yr old) similarly affected by the Chernobyl fallout. For both age classes, concentrations are always the lowest in the stemwood, highest in the inner bark and intermediary levels were observed for the outer bark. Due to the cumulative character of its biomass. however. stemwood is a long-term major reservoir of 137Cs. With tree development, changes in the 137Cs radial distribution are well described by variations in the sap ascent pattern and reveal an important transfer between tree rings. It is shown that. both the biomass evolution and knowledge of the evolution of the 137Cs radial gradient are important to predicting 137Cs accumulation in wood with time. According to the common transfer factor (TF) approach, one would expect a decrease in radiocaesium accumulation with time (from 0.0047 +/- 0.0013 to 0.0035 +/- 0.0008 m2kg(-1) for the 17 and 58 yr old trees, respectively). With the wood immobilisation potential (WIP) approach, it was, however, clearly shown that additional annual uptake was highest for the older stand (3.12 +/- 0.23 Bq cm(-3) yr(-1) for the 58-year-old stand compared to 1.99 +/- 0.30 Bq cm(-3) yr(-1) for the younger stand). Following the WIP approach, it was moreover possible to distinguish between the 137Cs incorporated via the root uptake process and a possible lasting effect of interception. It is shown that, whereas for the younger stand (5 yr old at the time of the accident) root uptake contributed exclusively to the wood contamination, the former process explained only 48% of the measured total 137Cs content in the wood of the older tree.     

Predictions of in situ solid/liquid distribution of radiocaesium in soils

Previous work has demonstrated that plant uptake of radiocaesium (RCs) is related to the activity concentration of RCs in soil solution, which is linked to the soil/soil solution distribution coefficient, K(D). The solid-liquid distribution of RCs is generally studied in soil suspensions in the laboratory and there are few reported measurements for in situ soil solutions. From a data set of 53 different soils (contaminated with either 134CsCl or 137CsCl) used in pot trials to investigate grass uptake of RCs, we analysed the variation of in situ K(D) with measured soil properties. The soils differed widely in % clay (0.5-58%), organic matter content (1.9-96%) and pH (2.4-7.0, CaCl2). The K(D) varied between 29 and 375,000 L kg-' (median 1460 L kg(-1)). Stepwise multiple regression analysis showed a significant correlation between the log K(D) and pH (p < 0.001), log %clay (p < 0.01) and log exchangeable K (p < 0.001) (overall R2 = 0.70). The in situ K(D) values were further compared to K(D)S predicted using an existing model, which assumes that RCs sorption occurs on specific sites and regular ion-exchange sites on the soil solid phase. Sorption of RCs on specific sites was quantified from the radiocaesium interception potential (RIP) measured for each soil and the soil solution concentrations of K+ and NH4+. The in situ log K(D) correlated well with the predicted K(D) (R2 = 0.85 before plant growth, R2 = 0.83 after plant growth). However, the observations were fivefold to eightfold higher than the predictions, particularly for the mineral soils. We attribute the under-prediction to the long contact times (minimum 4 weeks) between the RCs tracers and our experimental soils relative to the short (24 h) contact times used in RIP measurements. We conclude that our data confirmed the model but that ageing of RCs in soil is a factor that needs to be considered to better predict in situ KD values.     

Role of the fungal mycelium in the retention of radiocaesium in forest soils

The aim of this work was to study possible binding of 137Cs to various organic components in the soil and fungi, by using various sequential extraction procedures. The retention and binding of 137Cs has been studied in two horizons Of/Oh and Ah/B of a Ukrainian forest soil. The exchangeable fractions 137Cs from soil (sum of H2O and 1 M NH4OAc fraction) were found to be 12% in the organic-rich layer (range 11-14%) and 23% in the organic-poor (range 20-29%). The hydrolysis with 10% H2SO4 resulted in an additional release of 30% of 137Cs from the organic-rich soil (range 30-35%) and 38% from the organic-poor soil horizon (range 27-53%). Extraction with 30% H2O2 released 11 and 15% of the 137Cs activity from organic-rich and organic-poor soil horizons. The corresponding values for treatment with 98.8% NaOCl were about 27% in both types of soil. About 11% of the total 137Cs activity was found in the humic acid fraction, about 5% in the fulvic fraction and 46% in the residue fraction. Relatively high level of 137Cs activity in soil (ca. 50%) was thus still left unsolved in the residue fraction. About 29% of 137Cs activity concentration in fungal mycelia was found as water soluble with a range of 11 to 41%. Additionally 24% of the 137Cs activity from mycelia was released by 1 M ammonium acetate extraction. Together, water and 1 M ammonium acetate extraction released about 53% of the total 137Cs activity in the mycelia. In fruit bodies of mycorrhizal fungi, 68% of the total 137Cs inventory was found to be water soluble at room temperature and 93% at 80 degrees C.     

Soil-to-plant transfer of radiocaesium for selected tropical plant species in Bangladesh

Soil-to-plant transfer factors (TF) of radiocaesium (137Cs) were determined under field condition for grassy vegetation grown in Bangladesh at contaminated land in the Atomic Energy Research Establishment (AERE) campus. TF values for rice, grass and grassy/root vegetations grown in the same type of soil were also measured under pot condition. TF values of 137Cs for grassy vegetation (2.4 x 10(-2) -4.2 x 10(-2) with an average of 3.1 x 10(-2) +/-0.005) obtained under field condition were slightly lower than the values for grass and grassy/root vegetations (2.9 x 10(-2) -6.6 x 10(-2) with an average of 4.8 x 10(-2) +/-0.01 for grass and grassy vegetations and 2.3 x 10(-2) -5.6 x 10(-2) with an average of 4.0 x 10(-2) +/-0.009 for root vegetations, respectively) obtained under pot condition. However, TF values (9.0 x 10(-3) -2.6 x 10(-2) with an average of 1.9 x 10(-2) +/-0.004) obtained for rice were about a factor of 4 lower than the values obtained for grass and grassy/root vegetations. When the properties of the AERE soils as input parameters were used in the soil-plant transfer model of Absalom, the estimated TF values (4.5 x 10(-2) -6.7 x 10(-2) with an average of 5.3 x 10(-2) +/-0.006) were consistent with the measured values obtained for grass and grassy vegetations under pot condition, however, the model overestimates the TF values for rice.     

Solid partitioning and solid-liquid distribution of Po and Pb in marine anoxic sediments: roads of Cherbourg at the northwestern France

A sequential extraction protocol has been used to determine the solid-phase partition of ²¹⁰Po and ²¹⁰Pb in anoxic marine sediment from the roads of Cherbourg (France) in the central English Channel. Measurements were also obtained in pore waters, in which ²¹⁰Po activities range between 1 and 20 mBq L⁻¹ and ²¹⁰Pb activities between 2.4 and 3.8 mBq L⁻¹, with highest activities in the topmost layer. These activities are higher than in seawater, suggesting that sediment act as a source of both ²¹⁰Po and ²¹⁰Pb for overlying water. The ²¹⁰Po profile in the pore waters is apparently correlated with those obtained for Fe, Mn and SO₄²⁻, suggesting an influence of early diagenetic processes on the ²¹⁰Po solid-liquid distribution. In the sediment, ²¹⁰Po is predominantly bound to organic matter or chromium reducible sulphides, and residuals (clay minerals and refractory oxides). Our results indicate that ²¹⁰Po is not significantly bound to AVS, i.e. acid volatile sulphides: bioturbation could play a role by the early redistribution of ²¹⁰Po bound to acid volatile sulphides in the sediment. ²¹⁰Po, ²¹⁰Pb and Pb exhibit differences in terms of distribution, probably due to a different mode of penetration in the sediment. This work provides information on solid and liquid distribution of ²¹⁰Po and ²¹⁰Pb in marine sediment. These data are very scarce in the litterature.     

Laboratory experiments to predict changes in radiocaesium root uptake after flooding events

Changes in soil solution composition after a flooding event were hypothesised to be one of the key factors in explaining changes in radiocaesium incorporation in the food chain in the areas affected by the Chernobyl accident. A laboratory methodology was set up to monitor changes in the soil solution composition after a sequence of flooding cycles. Experiments were performed using column and batch approaches on test soils with contrasting initial soil solution composition (high and low initial concentrations of K+). Results from column experiments indicated a potential increase in NH(4)(+) concentrations, a parameter which could lead to an increase in the radiocaesium root uptake. Batch results in the soil with high initial K+ concentration showed that after a number of flooding cycles, especially for high ratios of flooding solution/mass of soil, K+ concentration decreased sometimes below a threshold value (around 0.5-1 mmol l(-1)), a fact that could lead to an increase in radiocaesium transfer. For the soils with a low initial K+ concentration, the flooding solution increased K+ and NH(4)(+) values in the soil solution. The comparison of test soils with soils from Ukraine areas affected by flooding showed that the final stage in soil solution composition was similar in both cases, regardless of the initial composition of the soil solution. Moreover, the comparison with unflooded soils from the same area showed that potential changes in other soil parameters, such as (137)Cs activity concentration, clay content, and radiocaesium interception potential, RIP (a parameter that estimates the radiocaesium specific sorption capacity of a soil), should also be monitored for additional effects due to the flooding event. Therefore, the changes in the root uptake would depend on the resulting situation from changes in RIP, K+ and NH(4)(+) values in the soil solution.     

Modelling the long-term behaviour of radiocaesium and radiostrontium in two Italian lakes

The present paper describes the application of a state-of-the-art model to two lakes in central Italy (Trasimeno and Monterosi) for the assessment of migration parameters of (137)Cs and (90)Sr (migration velocity to sediment, transfer rates from sediment to water and to bottom sediment). Applications of a compartment model and a model based on the diffusion equation to predict the behaviour of pollutants in water and through bottom sediment are presented and discussed. The application of the diffusion equation shows some difficulties of a general nature and typical of such a modelling approach. Moreover, there is no evidence of significant improvements of the model performances when the diffusion equation is applied. Very low levels of sedimentation rate of suspended matter in Lake Monterosi were evaluated by the quantitative assessment of radiocaesium migrating to bottom sediment. This suggests that, in this lake, the removal of radionuclide from the water column is mainly due to the turbulent mixing of bottom sediment causing radionuclide burial.     

Analysis of radiocaesium in the Lebanese soil one decade after the Chernobyl accident

Fallout from the Chernobyl reactor accident due to the transport of a radioactive cloud over Lebanon in the beginning of May 1986 was studied 12 years after the accident for determining the level of (137)Cs concentration in soil. Gamma spectroscopy measurements were performed by using coaxial high sensitivity HPGe detectors. More than 90 soil samples were collected from points uniformly distributed throughout the land of Lebanon in order to evaluate their radioactivity. The data obtained showed a relatively high (137)Cs activity per surface area contamination, up to 6545Bqm(-2) in the top soil layer 0-3cm. The average activity of (137)Cs in the top soil layer 0-3cm in depth was 59.7Bqkg(-1) dry soil ranging from 15 to 119Bqkg(-1) dry soil. The horizontal variability was found to be about 45% between the sampling sites. The depth distribution of total (137)Cs activity in soil showed an exponential decrease. Estimation of the annual effective dose due to external radiation from (137)Cs contaminated soil for selected sites gave values ranging from 19.3 to 91.6 micro Svy(-1).     

Weathering of radiocaesium contamination on urban streets,walls and roofs

Recent investigations in Russia have emphasised the significance of dose contributions from contamination on urban streets and roof pavings, and, typically to a lesser extent, walls in the urban environment. The crucial factor determining the magnitude of these contributions is the retention of the contamination by the different types of urban surface. Since the Chernobyl accident, a series of long-term field studies has been carried out on urban streets, walls and roofs, to examine the weathering processes of 137Cs on the various surface types. The derived time-functions are applied to estimate resultant long-term doses to inhabitants of an urban centre. The paper highlights the effect on caesium retention of surface material characteristics.     

Distribution of pre- and post-Chernobyl radiocaesium with particle size fractions of soils

The association of radiocaesium with particle size fractions separated by sieving and settling from soils sampled eight years after the Chernobyl accident has been determined. The three size fractions were: <2 microm, 2-63 microm and >63 microm. 137Cs in the soil samples was associated essentially with the finer size fractions, which generally showed specific activities 3-5 times higher than the bulk samples. Activity ratios of 134Cs/137Cs in the clay-sized fractions appear to be lower with respect to the corresponding values in bulk soil samples. This result indicates that some differences still exists in the particle size distribution between 137Cs originating from nuclear weapons, which has been in the soil for decades after fallout, and 137Cs coming from the Chernobyl accident, eight years after the deposition event. This behaviour could be related to "ageing" processes of radiocaesium in soils.     

Modelling the role of humic acid in radiocaesium distribution in a British upland peat soil

The significance of exchange sites on organic matter in the retention of radiocaesium in highly organic soils remains unclear. To quantify this retention, we measured the binding of 134Cs to a humic acid isolated from a British upland peat soil, under a range of chemical conditions. We interpreted our results using Humic Ion Binding Model V, a model of humic substance chemistry which simulates ion exchange by non-specific accumulation of cations adjacent to the humic molecules. Model V could simulate the humic acid-solution partitioning of Cs under all the solution conditions used. The model was used to estimate the contribution of organic matter to Cs sorption by the whole soil composite. An estimate of Cs sorption by illite frayed edge sites was also made. These simulations show that organic matter may play only a minor role in binding Cs. even in highly organic soils.     

Time-dependence of the radiocaesium contamination of roe deer: measurement and modelling

In spruce forest and peat bog, the migration of 137Cs from soil to plants, fungi, roe deer and consumers has been surveyed. In spruce forest the 137Cs activity concentration in roe deer decreases slowly with time and has superimposed periodic maxima in autumn which are correlated with the mushroom season. The decrease with time can be described by an effective half-life of 3.5 yr caused by a fraction of the 137Cs in the soil becoming unavailable for green grazing plants with time. The additional transfer of 137Cs into roe deer meat during the mushroom season depends on precipitation in July, August and September which also determines the yield of fungi in autumn. Our model confirms the assumption that fungi also have access to a fraction of the 137Cs in the soil which is unavailable for green plants. On peat bog the 137Cs activity concentration in roe deer is higher than in spruce forest and its effective half-life is about 17 yr, due to reversible binding of 137Cs to organic matter in the peat bog.     

Uptake and elimination of radiocaesium in fish and the "size effect."

A number of hypotheses have previously been developed concerning the rates of uptake and elimination of radiocaesium (137Cs) in fish. These include the influence of potassium and other water chemical parameters on both uptake and elimination, and the effect of fish size on accumulation. In order to test these hypotheses, we have assembled a data set comprising more than 1,000 measurements of radiocaesium (137Cs) in predatory fish (perch, pike and brown trout) in nine European lakes during the years after Chernobyl. These data have been analysed using simple models for uptake and excretion of 137Cs in fish, showing that: 1. Fish-water concentration factors (CF) were inversely proportional to potassium [K+] concentration of the different lakes, in agreement with previous studies. 2. The uptake rate of 137Cs in fish was negatively correlated with lake [K+], but excretion rate was independent of [K+]. 3. Lower than expected CF values were found in one lake, Iso Valkj?rvi, Finland. This is attributed to inhibition of the K+ (and therefore 137Cs) high affinity transport system in aquatic plants and fish by low pH and/or low Ca2+. 4. The inclusion of fish weight as a parameter in our dynamic model significantly improves the ability of the model to fit the observed measurements of 137Cs. 5. The model developed from the above hypotheses was able to fit the data from nine different lakes to within approximately a factor of 3 of the observed values.