Kinetics of trace element uptake and release by particles in estuarine waters: effects of pH,salinity, and particle loading

The uptake and release of 109Cd, 51Cr, 60Co, 59Fe, 54Mn, and 65Zn were studied using end-member waters and particles from Port Jackson estuary, Australia. The kinetics of adsorption and desorption were studied as a function of suspended particulate matter (SPM) loading and salinity. Batch experiments showed that the position and slope of the pH edges are dependent on the metal and on the salinity of the water (except for Mn). The general effect of salinity was to move the adsorption edge to higher pH values, with the greatest change being found for Cd. Most of the metals showed relatively simple kinetics with an increase in uptake as a function of time and suspended particle concentrations. The time dependence of Cd uptake was more complex, with an initial adsorption phase being followed by strong mobilization from the suspended sediments, explained by chlorocomplexation and competition with seawater major cations. The reversibility of the sorption decreased in the order Co>Mn>Zn>Cd>Fe>Cr. The percentage of adsorbed metal released in desorption experiments was greater in seawater than freshwater for Cd, Zn, and Co. These results are important in understanding the cycling of pollutants in response to pH, salinity, and particle concentrations in estuarine environments. In addition, they give valuable insight into the important mechanisms controlling the partitioning of heavy metals in the Port Jackson estuary.     

Erosion of atmospherically deposited radionuclides as affected by soil disaggregation mechanisms

The interactions of soil disaggregation with radionuclide erosion were studied under controlled conditions in the laboratory on samples from a loamy silty-sandy soil. The fate of 134Cs and 85Sr was monitored on soil aggregates and on small plots, with time resolution ranging from minutes to hours after contamination. Analytical experiments reproducing disaggregation mechanisms on aggregates showed that disaggregation controls both erosion and sorption. Compared to differential swelling, air explosion mobilized the most by producing finer particles and increasing five-fold sorption. For all the mechanisms studied, a significant part of the contamination was still unsorbed on the aggregates after an hour. Global experiments on contaminated sloping plots submitted to artificial rainfalls showed radionuclide erosion fluctuations and their origin. Wet radionuclide deposition increased short-term erosion by 50% compared to dry deposition. A developed soil crust when contaminated decreased radionuclide erosion by a factor 2 compared to other initial soil states. These erosion fluctuations were more significant for 134Cs than 85Sr, known to have better affinity to soil matrix. These findings confirm the role of disaggregation on radionuclide erosion. Our data support a conceptual model of radionuclide erosion at the small plot scale in two steps: (1) radionuclide non-equilibrium sorption on mobile particles, resulting from simultaneous sorption and disaggregation during wet deposition and (2) later radionuclide transport by runoff with suspended matter.     

Occurrence and behaviour of radionuclides in the Moselle River—Part III: Dispersion of radionuclides along the river course

Knowledge about propagation of radionuclides from nuclear power plants (NPPs) along the course of a river is of great interest in radioecological assessments. By use of a model previously applied in the cases of the Rhine and Weser Rivers, the distribution of various radionuclides released into the Moselle from the NPP Cattenom at normal operation is described with ⁵⁸Co, ⁶⁰Co and ^110mAg as tracers. A comparison of field measurements with calculated values revealed that the radionuclide concentrations in suspended matter and nuclide loads calculated from emission rates agreed with the measured data by a factor of less than two on average.Radionuclide concentrations and loads along the river course decrease mainly due to deposition of particulate radioactive matter in high-sedimentation areas and due to dilution with uncontaminated material from tributaries and other sources. The rate constants of both processes were evaluated, and the mean range of suspended radioactive particles in the Moselle was estimated. Moreover, this study showed anew that suspended matter has to be considered as the main carrier by which the radionuclides from NPPs may be transported over long distances.     

A modelling study on 137Cs and 239,240Pu behaviour in the Alborán Sea, western Mediterranean

A model for simulating the dispersion processes of 137Cs and 239,240Pu in the Alborán Sea is described. The model consists of two hydrodynamic models: a 2D depth-averaged model and a two-layer model which provide tidal and geostrophic currents, respectively; a sediment transport model which provides suspended particle concentrations and sedimentation rates over the domain; and the radionuclide dispersion model including interactions of dissolved radionuclides with suspended particles and bed sediments. These processes are formulated using kinetic transfer coefficients. The hydrodynamic and sediment models are run and validated in advance, and their results are then used to simulate the dispersion of 137Cs and 239,240Pu, which are introduced from atmospheric fallout. Radionuclide concentrations in the water column and distributions in bed sediments have been compared with measurements in the sea. Both set of data are, in general, in agreement. The model has also been applied to calculate radionuclide fluxes through the Strait of Gibraltar. These computed fluxes have been compared with previous estimations as well.     

Elemental analysis of total suspended particulate matter in the ambient air of Baghdad

Samples of atmospheric particulate matter obtained from representative areas of the city of Baghdad were collected on glass fiber filters using a high-volume sampler. Atomic absorption techniques were used to analyze the total suspended particulates (TSP) for the following trace metals; Fe, Cu, Zn, Pb, Mn, Cr, Cd, Co, and Hg. Sulfates were measured by turbidemetric method. Ion-selective electrodes was used for chloride analysis. It is concluded that the major components of TSP in the ambient air of Baghdad consist of mineral dust. Pb and Cd gave high enrichment factor values, which implies enrichment of these two metals from anthropogenic sources. High enrichment factors were also obtained for Zn and Cu. It is also concluded that in this arid area, the black smoke reflectance method is not suitable for measuring total suspended matter gravimetrically.     

Distribution of organic carbon, selected stable elements and artificial radionuclides among dissolved, colloidal and particulate phases in the Rhône River (France): preliminary results

The behaviour of radionuclides discharged from nuclear facilities in the Rh?ne River depends on their distribution among the dissolved, colloidal and particulate phases. A large water sample was fractionated using sequential ultrafiltration. Size distributions of organic carbon, Fe, Al, Si, Ca, Mg, Cu, Zn, 137Cs, 60Co and 106Ru were obtained. Our results show that organic colloids account for 11% of the total organic carbon content. Approximately 20% of the dissolved (< 450 nm) Fe and Al are in colloidal classes. 137Cs is not significantly transferred by the colloidal phase while 25% of 60Co or 106Ru is associated with organic and inorganic colloids.     

Review of Russian-language studies on radionuclide behaviour in agricultural animals: part 4. Transfer to poultry

Data on radionuclide transfer to domestic chickens and ducks obtained from research performed in the former Soviet Union were reviewed to provide transfer coefficient values (Ff) to poultry and edible egg contents. The majority of the data are from experiments with ⁹⁰Sr and ¹³⁷Cs, reflecting the importance of these radionuclides after global fallout and major radiation accidents. Data for ³H, ⁵⁴Mn, ⁵⁹Fe, ⁶⁰Co, ²²Na ⁶⁵Zn, ¹³¹I and U are also given. The values derived have been compared with those in the current IAEA Handbook of parameter values for the prediction of radionuclide transfer in temperate environments (TRS 364) and the recent revision which incorporates the values from this paper. The Russian-language data give improved estimates for many radionuclides and the revised handbook is now based on the better quality data given for chronic administration.     

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.     

Suspended particle adhesion on aquatic plant surfaces: implications for 137Cs and 133Cs uptake rates and water-to-plant concentration ratios

Suspended particle adhesion on aquatic biota can significantly increase the apparent concentration of radionuclides above their endogenous value, leading to an overestimation of the uptake rate and concentration ratios. This study is an attempt to assess quantitatively the importance of suspended particle adhesion on periphyton samples (biological material coating submerged surfaces). The concentrations of 137Cs and stable Cs (133Cs) in periphyton, suspended particles and filtered water were measured to determine the net water-to-periphyton concentration ratios for 137Cs and stable Cs. The net amount of 133Cs (or 137Cs) taken up by periphyton was calculated by subtracting from the total amount of 133Cs (or 137Cs) on the collected material (periphyton + inorganic particles), the 133Cs (or 137Cs) due to the inorganic particles adhering to periphyton. The mass of suspended particles adhering to the periphyton surface was calculated using scandium as an indicator of the mineral fraction of the suspended particles. The relationship between the concentration ratios for 137Cs and stable Cs and suspended particle adhesion on periphyton external surfaces is discussed.     

A dynamic model for assessing radiological consequences of routine releases in the Loire river: parameterisation and uncertainty/sensitivity analysis

A dynamic model for assessing the transfer of several radionuclides ((58)Co, (60)Co, (110 m)Ag, (134)Cs, (137)Cs, (54)Mn and (131)I) in a food-chain was applied on the Loire river, where 14 nuclear power plants situated on five different sites operate. The model considers the following potential exposure pathways: (i) transfer of radionuclides through the aquatic food chain and the subsequent internal exposure of humans due to ingestion of contaminated water and/or fish; (ii) use of river water for agricultural purposes (irrigation), transfer of radionuclides through the terrestrial food chain and the subsequent internal exposure of humans due to ingestion of contaminated foodstuffs; (iii) internal exposure due to inhalation of dust originating from resuspension of contaminated soil particles; (iv) external exposure from radionuclides present in the river or deposited on the river sediments or the soil. For each of the parameters introduced in this model, a probability density function, allowing further uncertainty and sensitivity analysis, was proposed. Uncertainty/sensitivity analysis were performed to: (i) compare calculations to empirical data; (ii) determine a confidence interval for the mean annual dose to critical groups; and (iii) identify the parameters responsible for the uncertainty and subsequent research priorities.     

A general methodology for structuring models to predict the long-term migration of radionuclides from catchments

In the present paper a generic model for predicting the long-term migration of radionuclides and heavy metals from catchments is described. The model subdivides the catchment into a number of homogeneous, infinitesimal sub-catchments and integrates the radionuclide contributions from such sub-catchments to calculate the total flux of contaminant. It relates the radionuclide behaviour to the statistical distribution of the pollutant partition coefficient on the "ensemble" of sub-catchments. The methodology was validated for 90Sr and 137Cs by using data for water contamination in some European rivers. Values of migration parameters for Pu, Tc, I and Cd isotopes were obtained.     

Transfer factors of radioactive Cs,Sr, Mn,Co and Zn from Japanese soils to root and leaf of radish

Transfer factors (TFs) of some selected radionuclides from ten different Japanese soils to radish have been studied by radiotracer experiments. The geometric mean values of TFs (on a wet weight basis) of radioactive Cs, Sr, Co, Mn and Zn for edible parts of radish (tuber) were 0.0090. 0.029, 0.00094, 0.0034 and 0.067, respectively. TFs for leaf were higher than those for tuber. The geometric mean values of leaf/tuber ratios were 4.1 for Cs, 4.9 for Sr, 1.6 for Co, 11 for Mn and 1.9 for Zn. Most of the Cs TFs obtained for andosol, which is the most common arable soil in Japan, were higher than those for the other soils. This might be due to the high concentrations of organic matter and alophen in andosol. The obtained TFs were compared to reference values of IAEA Technical Report 364.     

The dispersion of 137Cs and 239,240Pu in the Rhone River plume: a numerical model

A numerical three dimensional model to simulate the transport of Cs and Pu by the Rhone River plume has been developed. The model solves the hydrodynamic equations, including baroclinic terms (that account for density variations) and a turbulence model, the suspended matter equations, including several particle classes simultaneously, settling, deposition and erosion of the sediment, and the radionuclide dispersion equations. Exchanges of radionuclides between the liquid and solid phases are described in terms of kinetic transfer coefficients. The dependence of these coefficients with water salinity is explicitly included in the model since it changes from freshwater to seawater values in the model domain. Computed activity levels in water, suspended matter and bed sediments are, in general, in agreement with measurements in the area. The model can also give a wide amount of information, as distribution coefficients for total suspended matter and sediments and for each particle class, fractions of radionuclides fixed to solid particles, and vertical profiles of radionuclides and distribution coefficients.     

Trace elements in fish from the Savannah river near Savannah river nuclear plant

A survey of trace element residues in fish from the Savannah River near Savannah River Nuclear Plant was undertaken in 1982. Fish muscle tissue was incubated by the wet digestion method. Fifteen trace elements were determined by flame atomic absorption spectrophotometry analysi of the digests. It was found that As, Se, Mg, Hg, Ca, Zn, and Fe levels were relatively higher than Pb, Cd, Ni, Co, Cr, and Mn in all fish species. In addition, in all fish species it seems that Pb, Cd, Ni, Co, Cr, and Mn levels were relatively higher than Cs and Cu. Cs and Cu levels were negligible in all fish species analyzed. Trace element levels found in these fish species were not high enough to render them dangerous for human consumption.     

An elemental rationing technique for assessing concentration data from a complex water system

Water samples have been collected at the surface and bottom layers at 51 locations throughout Chesapeake Bay. The suspended particulate and dissolved fractions of these samples have been analyzed for Cd, Ce, Co, Cu, Fe, Mn, Mo, Ni, Pb, Sc, Sn, Th, U, and Zn using neutron activation analysis and atomic absorption spectrometry. Special chemical procedures were used to preconcentrate the elements of interest in the dissolved samples and separate them from the salt water matrix. The elemental concentrations observed in the dissolved samples were evaluated by direct comparison to those found in coastal seawater; however, the elemental concentrations in the particulate samples (mass per volume of water) were strongly influenced by the total amount of particulate material suspended in the water at time of collection. A double normalization procedure was used to calculate crustal enrichment factors for each sample, and these enrichment factors provided both a means to observe sample-to-sample variations, and also allowed a crude comparison with the natural levels occurring in the earth's crust.     

On the sensitivity of a marine dispersion model to parameters describing the transfers of radionuclides between the liquid and solid phases

The sensitivity of a marine dispersion model for non-conservative radionuclides, previously developed and validated for the English Channel, to parameters describing the exchanges between the liquid and solid phases (suspended matter and bottom sediments) has been studied using a Monte Carlo method. A probability distribution is assigned to each parameter. They are sampled to obtain a set of model parameters and a model run is carried out. This process is repeated to obtain a distribution of model outputs. Partial correlation coefficients are calculated to assess the relative influence of each parameter on model output. Errors are also assigned to model results. Three situations are studied: an instantaneous release of radionuclides, a continuous release and the case of a contaminated sediment behaving as a long-term source of radionuclides. Calculations have also been carried out for two radionuclides with different geochemical behaviour: (137)Cs and (239,240)Pu. The results indicate that all parameters are relevant, depending on the phase we are interested in obtaining the result and on the source term (instantaneous, continuous or due to sediments). However, parameters that are, in general, more influential are kinetic rates, mixing depth in the sediment and mean radius of suspended and sediment particles. This suggests that including several particle sizes in future radionuclide dispersion models could lead to an improvement in model results. Differences have also been found with respect to the relevance of some parameters depending on the geochemical behaviour of the radionuclide.     

Changes in plankton abundance, biomass, and chemical composition under the influence of the cooling system of the Beloyarsk Nuclear Power Plant

The abundance and biomass of phytoplankton and zooplankton proved to noticeably decrease after the water passed through the cooling system of the Beloyarsk Nuclear Power Plant: the phytoplankton perished by 38% (65 metric tons per day), and the zooplankton, by 55% (6 t/day). In the period between 1985 and 1991, the concentration of⁶⁰Co in the plankton of water intake and discharge canals varied from 120 to 1400 Bq/kg dry weight, and that of¹³⁷Cs, from 150 to 1040 Bq/kg dry weight, which is commensurable with the content of radionuclides in the plants and grounds of the Beloyarsk reservoir. In 1985, it was noted that the plankton passing through the cooling system of the nuclear power plant became enriched with Ca, Fe, Mg, Mn, Co, Cs, Cu, Mo, Ni, Pb, Si, Sn, Ti, V, and W.     

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.     

Heavy metals in water, sediments, plants and fish of Kali Nadi U.P. (India)

The distribution of heavy metals viz., Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb and Zn in the water, sediments, plants and fish samples collected from the Kali Nadi (India) have been determined. The studies have shown that there was considerable variation in the concentration of heavy metals from one sampling station to the other which may be due to the variation in the quality of industrial and sewage wastes being added to the river at different places. The orders of the concentration of heavy metals in water, sediments, plants (Eicchornia crassipes) and fish (Heteropnuestes fossilis) were Fe > Zn > Cu > Mn > Cr > Ni > Pb > Co > Cd; Fe > Zn > Mn > Ni > Cr > Co > Cu > Pb > Cd; Fe > Mn > Zn > Cu > Ni > Co > Pb > Cr > Cd and Fe > Zn > Mn > Ni > Pb > Co > Cr > Cu > Cd, respectively.     

Pre-assessment of the speciation of 60Co, 125Sb, 137Cs and 241Am in a contaminated aquifer

A sample of contaminated groundwater was analyzed using a combination of wet techniques to obtain geochemical information on the mobile species of 60Co, 125Sb, 137Cs and 241Am. The techniques were combined in a scheme to determine the predominant character of the radionuclides in negative or positive fractions, size separation by ultrafiltration, and their association with natural organic matter (NOM). The analyses indicated that the radionuclides of interest were predominantly in the negative fraction. Most of the 60Co and 125Sb were in the small size fraction (<5000 Da), and 137Cs and 241Am were found with the larger, colloidal-sized material. Antimony-125 and 60Co were predominantly in the hydrophilic fraction, while 137Cs and 241Am were found in hydrophobic fractions. Our analysis indicated that 137Cs is found in the same fraction as the large-sized colloidal (hydrophobic) material, suggesting an association with NOM. The results suggested that 60Co and 241Am were associated with NOM, in different size fractions, suggesting that these two nuclides are bound to different sites. Finally, the 125Sb results were inconclusive, whether this nuclide is associated with NOM, or it is inorganic.